(Scottish Graduate Series) Adam S. Wyatt, Ian a. Walmsley (Auth.), Robert Thomson, Christopher Leburn, Derryck Reid (Eds.) - Ultrafast Nonlinear Optics-Springer International Publishing (2013)

Scottish Graduate Series
Robert Thomson
Christopher Leburn
Derryck Reid Editors
Ultrafast
Nonlinear
Optics
Ultrafast Nonlinear Optics
Scottish Graduate Series
The Scottish Graduate Series is a long-standing series of graduate level texts
proceeding from the Scottish Universities Summer Schools in Physics (SUSSP).
SUSSP was established in 1960 to contribute to the dissemination of advanced
knowledge in physics, and the formation of contacts among scientists from different
countries through the setting up of a series of annual summer schools of the highest
international standard. Each school is organized by its own committee which is
responsible for inviting lecturers of international standing to contribute an in-depth
lecture series on one aspect of the area being studied.
For further volumes:

http://www.springer.com/series/11662
Robert Thomson • Christopher Leburn
Derryck Reid
Editors
Ultrafast Nonlinear Optics
123
Editors
Dr. Robert Thomson Dr. Christopher Leburn
Heriot-Watt University Heriot-Watt University
Edinburgh, UK Edinburgh, UK
Prof. Derryck Reid

Heriot-Watt University
Edinburgh, UK
ISBN 978-3-319-00016-9 ISBN 978-3-319-00017-6 (eBook)

DOI 10.1007/978-3-319-00017-6
Springer Heidelberg New York Dordrecht London
Library of Congress Control Number: 2013933241
© Springer International Publishing Switzerland 2013

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Previous SUSSP Schools
1 1960 Dispersion Relations

2 1961 Fluctuation, Relaxation and Resonance in Magnetic Systems
3 1962 Polarons and Excitons
4 1963 Strong Interactions and High Energy Physics
5 1964 Nuclear Structure and Electromagnetic Interactions
6 1965 Phonons in Perfect Lattices and in Lattices with Point Imperfections
7 1966 Particles Interactions at High Energy
8 1967 Methods in Solid State and Superfluid Theory
9 1968 Physics of Hot Plasmas
10 1969 Quantum Optics
11 1970 Hadronic Interactions of Photons and Electrons
12 1971 Atoms and Molecules in Astrophysics
13 1972 Electronic and Structural Properties of Amorphous Semiconductors
14 1973 Phenomenology of Particles at High Energy
15 1974 The Helium Liquids
16 1975 Nonlinear Optics
17 1976 Fundamentals of Quark Models
18 1977 Nuclear Structure Physics
19 1978 Metal Non-metal Transitions in Disordered Solids
20 1979 Laser-Plasma Interactions: 1
21 1980 Gauge Theories and Experiments at High Energy
22 1981 Magnetism in Solids
23 1982 Lasers: Physics, Systems and Techniques
25 1983 Quantitative Electron Microscopy
26 1983 Statistical and Particle Physics
27 1984 Fundamental Forces
28 1985 Superstrings and Supergravity
v
vi Previous SUSSP Schools

30 1985 Synchrotron Radiation
31 1986 Localisation and Interaction
32 1987 Computational Physics
33 1987 Astrophysical and Laboratory Spectroscopy
34 1988 Optical Computing
36 1989 Physics of the Early Universe
37 1990 Pattern Recognition and Image Processing
38 1991 Physics of Nanostructures
39 1991 High Temperature Superconductivity
40 1992 Quantitative Microbeam Analysis
41 1992 Spatial Complexity in Optical Systems
42 1993 High Energy Phenomenology
43 1994 Determination of Geophysical Parameters from Space
44 1994 Simple Quantum Systems
45 1994 Laser-Plasma Interactions 5: Inertial Confinement Fusion
46 1995 General Relativity
47 1995 Laser Sources and Applications
48 1996 Generation and Application of High Power Microwaves
49 1997 Physical Processes in the Coastal Zone
50 1998 Semiconductor Quantum Opto-Electronics
51 1998 Muon Science
52 1998 Advances in Lasers and Applications
53 1999 Soft and Fragile Matter: Nonequilibrium Dynamics, Metastability and
Flow
54 2000 The Restless Universe: Applications of Gravitational N-body
Dynamics to Planetary, Stellar and Galactic Systems
55 2001 Heavy Flavour Physics
56 2002 Ultrafast Photonics
57 2003 Large Hadron Collider Phenomenology
58 2004 Hadron Physics
59 2004 Soft Condensed Matter in Molecular and Cell Biology
60 2005 Laser Plasma Interactions
61 2006 Neutrino Physics
62 2007 Extrasolar Planets
63 2008 High Pressure Physics
64 2008 Advanced Techniques in Electron Spin Resonance
65 2009 LHC Physics
66 2010 Ultrafast Nonlinear Optics
67 2011 Quantum Coherence and Quantum Information
68 2011 Laser Plasma Interactions and Inertial Confinement Fusion
Lecturers
Philip H. Bucksbaum Stanford University

Giulio Cerullo Politecnico di Milano
John M. Dudley University of Franche-Comté
Ajoy K. Kar Heriot-Watt University
Ursula Keller ETH Zurich
Ken W. D. Ledingham University of Strathclyde
Jon P. Marangos Imperial College London
Margaret M. Murnane JILA/University of Colorado at Boulder
Stefan Nolte Friedrich Schiller University of Jena
Jeff A. Squier Colorado School of Mines
Robert R. Thomson Heriot-Watt University
Thomas Udem Max-Planck-Institut für Quantenoptik
William Wadsworth University of Bath
Ian A. Walmsley University of Oxford
Guest Lecturers
Thomas M. Baer Stanford University
Chris Dorman Coherent Scotland
Allister Ferguson University of Strathclyde
Wilson Sibbett University of St Andrews
Executive Committee
Derryck T. Reid Heriot-Watt University Director and Co-Editor
David Townsend Heriot-Watt University Secretary
Henry T. Bookey Heriot-Watt University Treasurer
Robert R. Thomson Heriot-Watt University Editor
vii
viii Lecturers
International Advisory Committee

Prof. Jonathan Knight University of Bath – Bath – UK
Prof. Majid Ebrahim-Zadeh ICFO – Barcelona – Spain
Prof. Günter Steinmeyer Max Born Institute – Berlin – Germany
Dr Scott Diddams NIST – Boulder – USA
Prof. Uwe Morgner Gottfried Wilhelm Leibniz Universität – Hannover –
Germany
Dr Christophe Dorrer University of Rochester – Rochester – USA
Prof. Andreas Tünnermann Universität Jena – Jena – Germany
Prof. Wilson Sibbett University of St Andrews – St Andrews – UK
Dr Helen Margolis National Physical Laboratory – Teddington – UK
Preface
The Scottish Universities Summer Schools in Physics (SUSSP) was established in

1960, and since then there have been 68 schools (up to the end of 2011). A quick
glance at the list of past schools indicates just how wide ranging the SUSSP school
topics have been, and represents the breadth of research in Physics which continues
to be conducted in Scottish Universities.
The 66th school in the SUSSP series (SUSSP66) was held over 10 days at
Heriot-Watt University, Edinburgh, Scotland, between the 11 and 21 of August
2010. The topic of the school was the broad area of “Ultrafast Nonlinear Optics”,
and it consisted of lectures from 14 renowned international experts in this highly
research active area. This book consists of 13 contributed chapters, each of which is
either authored or co-authored by one or more of the SUSSP66 lecturers or executive
committee members.
The field of Ultrafast Nonlinear Optics is broad and multidisciplinary, and en-
compasses areas concerned with both the generation and measurement of ultrashort
pulses of light, as well as those concerned with the applications of such pulses.
Ultrashort pulses are extreme events – both in terms of their durations, and also
the high peak powers which their short durations can facilitate. These extreme
properties make them powerful experimental tools. On one hand, their ultrashort
durations facilitate the probing and manipulation of matter on incredibly short
timescales. On the other, their ultrashort durations can facilitate high peak powers
which can drive highly nonlinear light-matter interaction processes. The chapters
contained within this book cover a complete range of topics, both applied and
fundamental in nature, within the area of Ultrafast Nonlinear Optics.
ix
x Preface
Including lecturers, guest lec-

turers, organisers and students,
SUSSP66 attracted 133 participants
from 28 countries. This included 14
lecturers, 4 guest lecturers and 115
students. Over the 10 working days
of the school, there were 42 lec-
tures, 1 computer laboratory based
tutorial session, 2 panel discussions
(1 industry focused, and 1 on future
directions) and 2 lively poster ses-
sions where students presented 82 posters.
In addition to the academic-related activities, the packed social programme also
formed an important and highly enjoyable part of the school. Students were invited
to take part in various activities, such as a trip to the Edinburgh Military Tattoo,
a coach tour to the Scottish Highlands, a guided scientific history walk round
Edinburgh which culminated in a well-deserved dram at the top of Arthur’s seat,
hiking in the Pentland hills, a Scottish Ceilidh and a banquet to finish the school.
The students also organised a number of social events themselves – including
a commendable attempt by a small band of enthusiastic students to reenact the
first observation of a soliton – made by John Scott Russell on the Union Canal
nearby the Heriot-Watt University Riccarton Campus (see picture above). The
SUSSP66 executive committee sincerely thank Ruth Livingstone and Tobi Lamour
for coordinating the social programme – their considerable effort was a key to its
success. The executive committee also thank the numerous post-graduate students
from the Physics Department at Heriot-Watt University for helping with the social
events.
The executive committee are also extremely grateful to the SUSSP66 spon-
sors: the Scottish Universities Physics Alliance (SUPA), the UK Engineering and
Physical Sciences Research Council (EPSRC), the European Physical Society
(EPS), the Institute of Physics (IOP) – Quantum Information, Quantum Optics
and Quantum Control group, the IOP – Quantum Electronics and Photonics group,
the Atomic Weapons Establishment (AWE), Innolume, Venteon, Toptica, Thorlabs,
Philips, Coherent, Molecular Machines and Industry (MMI), the James Watt
Institute for High Value Manufacturing, Elliot Scientific, Stratton Technologies,
Time-Bandwidth, M-Squared Lasers, the Royal Society of Edinburgh, Newport,
Spectra-Physics, the European Office of Aerospace Research and Development,
the Air Force Office of Scientific Research, the United States Air Force Research
Laboratory, the Scotland-Stanford Universities Partnership (SU2P), the Scottish
Universities Summer Schools in Physics (SUSSP), the Scottish chapter of the IEEE
Photonics Society, Selex-Galileo, Taylor and Francis, Fastlite, Laser Quantum, the
Optical Society of America (OSA), Fast-Dot and Alcatel-Thales.
Preface xi
The executive committee hope that this book will act as part of a lasting legacy of
an extremely interesting and fulfilling school, where participants not only expanded
their knowledge, but also formed lasting friendships and networks.
Edinburgh, January 2012 Robert R. Thomson

Editors’ Note
The chapters contained in the book are based on the lectures given by the lecturers
at SUSSP66. The chapters are aimed at graduate-student level and are intended to
provide the student with an accessible, self-contained and comprehensive gateway
into each subject. Chapters 1, 2, 3, and 4 are concerned with the generation
and measurement of ultrashort pulses. Chapters 5, 6, and 7 are concerned with
fundamental applications of ultrashort pulses in metrology and quantum control.
Chapters 8 and 9 are concerned with ultrafast nonlinear optics in optical fibres.
Chapters 10, 11, 12, and 13 are concerned with the applications of ultrashort pulses
in areas such as particle acceleration, microscopy and micromachining. The editors
sincerely thank the authors for their excellent and timely contributions. Matthew
Edmonds is acknowledged and thanked by the editors for his help in proofreading a
number of chapters.
xiii
Contents
1 Measuring Ultrashort Optical Pulses. . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 1

Adam S. Wyatt and Ian A. Walmsley
2 Ultra-Broadband Optical Parametric Amplifiers . . .. . . . . . . . . . . . . . . . . . . . 23
Giulio Cerullo and Daniele Brida
3 Attosecond Generation and High Field Physics . . . . .. . . . . . . . . . . . . . . . . . . . 45
Jon P. Marangos and Malte Oppermann
4 Advances in Solid-State Ultrafast Laser Oscillators .. . . . . . . . . . . . . . . . . . . 73
Christopher G. Leburn and Derryck T. Reid
5 Ultrafast Quantum Control in Atoms and Molecules . . . . . . . . . . . . . . . . . . 105
Philip H. Bucksbaum
6 Femtosecond Optical Frequency Combs . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 129
Thomas Udem, Ronald Holzwarth, and Theodor Hänsch
7 Ultrafast Material Science Probed Using Coherent X-ray
Pulses from High-Harmonic Generation.. . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 149
Stefan Mathias, Henry C. Kapteyn, and Margaret M. Murnane
8 Ultrafast Nonlinear Fibre Optics and Supercontinuum Generation.. 177
John M. Dudley, Rim Cherif, Stephane Coen,
and Goery Genty
9 Nonlinear Wavelength Conversion and Pulse Propagation
in Optical Fibres . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 195
William J. Wadsworth
10 Applications of Ultra-Intense, Short Laser Pulses . .. . . . . . . . . . . . . . . . . . . . 227
Ken W.D. Ledingham
xv
xvi Contents
11 Utilising Ultrafast Lasers for Multiphoton Biomedical Imaging .. . . . . 251

Erich E. Hoover, Eric V. Chandler, Jeffrey J. Field,
Dawn N. Vitek, Michael D. Young, and Jeff A. Squier
12 Femtosecond Laser Micromachining .. . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 287
Loren Cerami, Eric Mazur, Stefan Nolte,
and Chris B. Schaffer
13 Ultrafast Laser Inscription of Photonic Devices in Bulk Dielectrics .. 323
Robert R. Thomson and Giulio Cerullo
Poster Sessions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 351
Participants .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 357
Index . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 367
Chapter 1
Measuring Ultrashort Optical Pulses
Adam S. Wyatt and Ian A. Walmsley
1.1 Introduction
Modern laser and laser-driven sources can generate light pulses of unprecedented
brevity, with durations in the range of picoseconds to attoseconds. Such durations
are significantly shorter than any photodetector response time. Further, there is
a need for more information about the pulse than the temporal intensity profile
obtained from a simple photodetector. Sophisticated applications, such as coherent
control of atomic and molecular dynamics demand a detailed knowledge of the
electric field of the pulse, and not merely its duration [1].
The need for metrology has increased along with the development of new sources
and their application in a wide range of new fields. Of course, the need to determine
the pulse duration remains a primary application, both because this parameter is an
important specification of the laser output needed for other applications, and because
it acts as a diagnostic of the system operation.
Modern mode-locked lasers, for example, generate pulses with spectral band-
widths exceeding one octave and with durations below 10 fs, well beyond anything
that can be characterized by means of fast photodetectors. The operation of such
lasers relies on a complex combination of linear pulse propagation, influenced
by the chromatic dispersion of the laser material, the mirrors and the intra-cavity
dispersion compensating devices, together with nonlinear effects, such as self-phase
modulation of the pulse in the laser material or by saturation of an intracavity
absorption, such as in a semiconductor saturable absorber mirror (SESAM), as
well as, in some cases, space-time coupling. The optimization of a mode-locked
laser is made practicable by means of a diagnostic providing the electric field as a
A.S. Wyatt () • I.A. Walmsley

Clarendon Laboratory, Department of Physics, University of Oxford,
Parks Rd, Oxford OX3 0BU, UK
e-mail: a.wyatt1@physics.ox.ac.uk
R. Thomson et al. (eds.), Ultrafast Nonlinear Optics, Scottish 1

Graduate Series, DOI 10.1007/978-3-319-00017-6 1,
2 A.S. Wyatt and I.A. Walmsley
function of time or frequency, or at least providing some temporal information such

as the second order intensity autocorrelation. One of the primary limits at present
to the generation of few-cycle pulses directly from a laser is the dispersion of the
intracavity mirrors and other optical elements. Historically, detailed measurements
of the laser output were able to identify this as a major obstacle to generating shorter
pulses [2].
Chirped pulse amplification (CPA) operates by lowering the peak power of the
pulses in the amplifier gain medium, which would otherwise induce non-linear
phase distortion of the pulse [3, 4]. To achieve this, the pulses are stretched in
time by means of a dispersive delay line, often based on angular dispersion from
diffraction gratings or prisms. After amplification, the pulse is temporally recom-
pressed using an “inverse” dispersive delay line, or compressor, that compensates
the dispersion introduced by the stretcher and the propagation through the other
amplifier elements. Obtaining peak performance from such a scheme requires a
reliable and rapid method to characterize the output. Accurate characterization of
the output pulses enables the optimization of the parameters of the system, such as
the distance between the two gratings of a compressor and the angle of incidence
of the input beam on the gratings. The usual optimization parameters in such an
application are the duration of the recompressed pulses, since the peak power scales
like the ratio of the energy per pulse to the duration, and the temporal contrast,
since pre-pulses can hinder the control or observation of the physical processes of
interest, for example the ionisation of a target. Some examples of this application
can be found in [5, 6]. The spectral phase of the output pulse from a Ti:sapphire CPA
system can be used directly as the basis for a controller to optimize the compressor to
minimize the pulse duration, for example. The compressor optimization consists of
adjusting the angle of diffraction gratings relative to the input beam and the relative
distance between the two gratings. A large cubic spectral phase, for example, gives
rise to significant pre-pulses, and the compressor optimization leads to a better pulse
shape with a higher intensity.
The bandwidth of an optical pulse can be increased while maintaining a
deterministic phase relation between different spectral components by means of
various nonlinear optical processes such as self-phase modulation and harmonic
generation. All of these require careful compensation of the spectral phase in order
to lead to an output pulse with a shorter duration than the input. Further, these
processes are dynamically complicated and sensitive to the details of the input pulse
shape. Therefore, even characterizing the raw output pulse before recompression
can be a difficult task.
Shaped pulses, sometimes of a quite complex temporal structure, are now
commonly used to both probe and manipulate fundamental processes in atoms
and molecules (see Chap. 5 by Bucksbaum). For instance, the study of primary
processes in biologically-relevant systems via ultrafast microscopy is now quite
common. The details of the pulse shapes usually contain important information
about the dynamical process under study, and this information, residing in both the
temporal amplitude and the temporal phase of the field, can only be extracted using
modern techniques of metrology. For example, the important phenomenon of the
1 Measuring Ultrashort Optical Pulses 3
self-action of intense optical pulses in nonlinear media gives rise to a complicated

set of dynamics that has analogues in many branches of physics. The study of the
changes in the shapes of pulses propagating through such media provides access to
these dynamics.
1.2 General Considerations
An electromagnetic pulse may be specified by its electric field alone, at least below
intensities that give rise to fields that will accelerate electrons to relativistic energies.
Thus a useful notation is that of the analytic signal, whose amplitude and phase we
seek to determine via measurement. The (real) electric field of the pulse is given in
terms of the analytic signal by Eq. (1.1).
E.t/ D ".t/ C " .t/ (1.1)
where ".t/ is an analytic function of time (and space, although we suppress other
arguments here for clarity). The signal ".t/ is taken to have compact support in the
domain .T; T /, and we shall refer to it henceforth as the “field of the ultrashort
pulse”.
The spectrum of the pulse is then defined by the Fourier transform (Eq. (1.2))
ZT
"Q .!/ D dt ".t/ e i !t; (1.2)
T
so that EQ .!/ D "Q .!/ C "Q .!/. Note that "Q .!/ contains only positive frequency
R1
components, since ".t/ D dt "Q.!/e i !t . This is therefore a reasonable descrip-
0
tion for the fields of pulses propagating in charge-free regions of space, for which
RT
the pulse area, ‚.T / D dt ".t/ D ".!
Q D 0/ must be zero.
T
A single pulse is said to be completely characterized if the function ".t/ is
known on the domain .T; T /. In practice one usually adopts the approximation
that the pulse is also characterized by the function "Q .!/ on the domain .; /,
where >> 1 = with the rms pulse duration. The sampling theorem prevents a
function from having compact support in both domains, but it is usually a reasonable
approximation to truncate the spectral function at large frequencies, where the
spectral energy falls below the noise level of the detector.
The analytic signal is complex and therefore can be expressed uniquely in terms
of an amplitude and phase
E.t/ D jE.t/j exp Œi t .t/ exp.i 0 / exp.i !o t/; (1.3)

Where jE.t/j is referred to as the time-dependent envelope, !0 is the carrier

frequency (usually chosen near the centre of the pulse spectrum), t .t/ is the
time-dependent phase, and 0 a constant, known as the carrier-envelope offset
(CEO) phase. The square of the envelope, I.t/ D jE.t/j2 , is the time-dependent
instantaneous power of the pulse which can be measured if a detector of sufficient
electronic bandwidth is available. The derivative of the time-dependent phase
accounts for the occurrence of different frequencies at different times, i.e. .t/ D
@t
is the instantaneous frequency of the pulse that describes the oscillations
@t
of the electric field around that time. The frequency representation of the analytic
signal
ZT
ˇ ˇ
Q
E.!/ D ˇE.!/
Q ˇ exp Œi ! .!/ D dt E.t/ e i !t ; (1.4)
T
ˇ ˇ
can be decomposed similarly, so that ˇE.!/ Q ˇ is the spectral amplitude and ! .!/
ˇ ˇ2
is the spectral phase. The square of the spectral amplitude, IQ.!/ D ˇE.!/ Q ˇ , is
the spectral intensity (strictly speaking this quantity is the spectral density – the
quantity measured in the familiar way by means of a spectrometer followed by
a photodetector). The spectral phase describes the relative phases of the optical
@!
frequencies composing the pulse, and its derivative is the group delay T .!/ at
@!
the corresponding frequency, i.e. the time of arrival of a subset of optical frequencies
of the pulse around ¨.
The necessary and sufficient conditions that must be satisfied by any method
that provides a complete specification of an ultrashort pulses field can be found
quite generally from a theory based on manipulating the pulses by means of linear
filters. The fact that this is possible already implies that apparati based entirely on
linear optical elements are capable of pulse characterization, something that was not
appreciated until relatively recently [7]. In practice, many of the popular methods
make use of nonlinear optical processes, but this is because it has proven difficult to
construct linear filters of the correct character or response time, rather than for any
fundamental reason.
The inversion protocols for extracting the pulse shape from measured data are
also made clear by working with linear transformations, and allows a categorization
of different methods, and the development of a catalogue of what is possible in
principle. An important feature introduced by the use of nonlinear optics is that
the inversion algorithms become more complicated. In some cases they remain
deterministic, but in others an iterative search for a solution satisfying the twin
constraints of the signal form and the data must be implemented. Thus the two
major considerations in pulse characterization are the physical arrangement of the
linear and nonlinear components and the inversion procedure [8].
The basic elements required for the complete characterization of optical pulses
are quite simple: at least one fast shutter or phase modulator, a spectrometer or an
element to temporally stretch the pulse via dispersion, and one or two beamsplitters.
One can think of all elements, except the beamsplitters, as two-port devices: a pulse
enters at one port and exits at another. There may be ancillary ports for control
signals, such as the timing signal for the shutter opening, for example, but these are
essentially linear systems, in that the output pulse field scales linearly with the input
pulse field. Thus the input/output relations for these devices are all of the kind
ZT

"o .t/ D dt 0 H t; t 0 "i t 0 ; (1.5)
T
Where ".t/ is the analytic signal (with subscripts i and o representing the input and
output fields respectively), and H .t; t 0 / is the (linear, causal) response function of
the device. We will specify the functional forms of the common linear filters given
above in subsequent paragraphs.
The beamsplitter is a four-port device, having two input and two output ports. The
input-output relations for this device are well known, and the main utility in pulse
measurement applications is either in providing a means to generated a replica of a
pulse (one input and two outputs) or to combine the unknown pulse with a reference
pulse (two inputs and two outputs), or as elements of a interferometer in which
phase to amplitude conversion takes place.
We take it that all detectors available have a response that is slow compared to the
pulse itself, though they need not be integrating. For pulses with temporal structure
of duration less than 100 fs or so, this is usually the case. The measured signal from
an integrating detector is related to the incident field, for our purposes, via
ZTR
ˇ ˇ2
S.f / D dt 0 ˇ"f t 0 ˇ ; (1.6)
TR
where TR is the integration time of the detector apparatus.

Combining Eqs. (1.5) and (1.6) implies that the detector signal depends on the
two-time correlation function of the field:

C t; t 00 D " .t/" t 00 : (1.7)
In general, the signal will be averaged over a train of pulses. If each pulse in the
train is not identical then the root quantity characterizing the ensemble of pulses is
˝ ˛
C t; t 00 D " .t/" t 00 : (1.8)
where the brackets indicate either a time average over the pulse train, or an
ensemble average over repeated experiments. Eqs. (1.7) and (1.8) are identical
only if each pulse in the train is identical with all others. Note that C .t; t 00 / is
not the same as the correlation function that is derived from the pulse spectral
intensity jQ" .!/j2 . In that case, the Fourier transform yields the reduced correlation
R1
C 0 ./ D dt C .t; t C /. This obviously contains no more information than the
1
spectrum itself, in contrast to C .t; t 00 /.
A key issue for all methods of pulse characterization is that it is assumed that
Eq. (1.7) is the correct form of the correlation function. All inversion algorithms
assume this. Of course, for single shot measurements, based on just one pulse from
an ensemble, the assumption is necessarily valid. Further, single-shot methods can
be used to determine whether the ensemble consists of identical pulses by repeated
measurements on single realizations of the ensemble on individual pulses drawn
from the train.
It is frequently productive to work with a variation of the correlation function
that uses a two dimensional space of time and frequency – the chronocyclic phase
space [9]. The intuitive concept of chirp (that is, time-dependent frequency in the
pulse) can be most easily seen within this space. A particularly useful function in
this regard is the chronocyclic Wigner function, defined as;
ZT
t0 t0 0
W .!; t/ D dt 0 C t C ; t e i !t (1.9)
2 2
T
A particular feature of the Wigner representation is that the marginals of the

distribution are the temporal and spectral intensities respectively
Z
2
I.t/ D j".t/j D d! W .!; t/ ; (1.10)
Z
IQ .!/ D jQ".!/j2 D dt W .!; t / : (1.11)
Note also that the Wigner function is sufficient to characterize both individual
pulses and partially coherent pulse ensembles. However, the function is not in
general positive definite, and cannot therefore be considered a probability distri-
bution of the pulse field. Indeed negative Wigner functions characterize many of
the complicated pulse shapes that are in current use in, say, quantum control. For
example, a pair of phase-locked Gaussian pulses has a significant region of phase
space where its Wigner function is negative. The restrictions on the pulse duration
and bandwidth required by Fourier’s theorem are inherent in the Wigner function,
and there is a minimum area of the chronocyclic phase space that it may occupy.
Example Wigner functions for a number of simple pulse shapes are shown in
Fig. 1.1. The concept of a time-dependent frequency or chirp is clearly visible in
Figs. 1.1b, d, and the coherence between two separate pulses, that is a well-defined
relative phase, is shown in Fig. 1.1c.
This representation sheds some light on the general form of measurements, since
Eq. (1.5) may be written in terms of the Wigner representation of the pulse field and
that of the measurement apparatus as an overlap integral
Fig. 1.1 Wigner functions of (a) a Fourier-transform limited Gaussian pulse, (b) a pulse with
Gaussian spectrum and quadratic spectral phase, (c) a pair of identical Fourier-transform-limited
Gaussian pulses, and (d) a pulse with Gaussian spectrum and third-order spectral phase. In each
case, the temporal and spectral marginals are plotted
Z1 Z1
S .; T / D dt d!W .!; t/ WS .!; tI ; T / : (1.12)
1 1
Where WS .!; tI ; T / is the Wigner chronocyclic representation of the apparatus

response function, with ˝ and T representing parameters associated with the
settings of the apparatus. For example, ˝ might be the passband of a spectrometer,
and T the time shift introduced by a delay line.
More generally, considering an apparatus characterized by a set of parameters
fpi g, with phase-space representation WS .!; tI fpi g/ then this function should be
able, by suitable choices of the pi , to explore all of the phase space occupied
by the pulse. In this case the data S .fpi g/ contains sufficient information to
reconstruct the pulse field. Indeed, this is both a necessary and sufficient condition
for characterizing the pulse. The apparatus function can be considered a “window”
onto the chronocyclic phase space, through which the pulse itself can be seen.
The chronocyclic phase space may be explored in a number of ways. The three
main approaches are: spectrography/sonography, tomography, and interferometry.
In the first, the window function is a band-limited function whose representation
is similar to that of the pulse shown in Fig. 1.1a. The parameters describing this
function are W and T noted in the previous paragraph. The window function moves
around the phase space as these parameters are adjusted: parallel to the time axis
as T changes, and parallel to the frequency axis as W changes. At each location a
“sample” of the field Wigner function is taken. The overlap integral in this case is
a convolution, and the inversion algorithm is a deconvolution in two dimensions.
Because these dimensions are complementary variables, the inversion is unique.
The second approach makes use of a window function that approximates a line
in the phase space. The orientation of this line is adjusted by one parameter and
the offset with respect to the origin by another. For example, the window function
may be oriented parallel to the time axis, intersecting the frequency axis at ˝.
The overlap integral determining the signal is therefore a projection of a “slice”
of the pulse Wigner function W .!; t/ onto the frequency axis. As the orientation is
changed about the intersection frequency, a different section of W .!; t / is projected
onto this frequency, thereby building up a set of spectra parameterised by the
window function orientation, so fSi g S .I fi g/. This is called phase-space
tomography, by analogy to the process used in medical diagnostics to assemble a
3-dimensional representation of an organ from a set of 2-dimensional projections.
The third approach makes use of an apparatus that shifts the pulse Wigner
function in time or frequency (or some combination of the two) and then mixes
it with the original, unshifted, version. As can be imagined from Fig. 1.1c, this
gives rise to fringes that reveal the relative phase between different components
of the pulse. The spectral or temporal phase can be read off from the position of
these fringes, and this, together with the direct measurement of the pulse spectral
or temporal intensity (the marginals of W .!; t/) gives the pulse field directly. This
approach has the simplifying feature that the shifted pulse replica need not be moved
around the phase space, since the interference property of Wigner representations
enables the important phase information to be mapped into the amplitude domain.
These operations need to be implemented in laboratory apparatus. We may use
the linear filter model to help delineate the necessary and sufficient conditions for
such an apparatus. Linear filters are those for which the output field scales linearly
with the input field. These filters modulate the pulse being measured and possess a
characteristic response time of the order of the pulse itself, though not significantly
shorter than it. They change the pulse in a way that is prescribed by an external
signal, say the voltage applied to an electroabsorption modulator. Linear filters
may be separated into two classes: those with time-stationary response functions
and those with time-nonstationary responses. For the former class, which includes
the spectrometer and dispersive delay line, the shape of the output pulse does not
depend on which time the input pulse arrives. For the latter class, which includes
the modulator and the shutter, the output pulse shape clearly depends on the timing
of the input pulse with respect to the shutter opening or the modulator drive signal.
Time stationary filters are characterized by response functions of the form
H .t; t 0 / D S .t t 0 /, and non-stationary filters by H .t; t 0 / D N.t/ı.t t 0 /.
Equivalently in the frequency domain, stationary filters take the general form
HQQ .!; ! 0 / D SQ .!/ ı .! ! 0 /, and nonstationary the form HQQ .!; ! 0 / D NQ .!! 0 /,
where the tilde represents a Fourier transform.
Representative response functions for the various common elements that facili-
tate analysis of all pulse measurement apparatuses, are:
2
Shutter W N A .t/ D e .t / =g2 ; (1.13a)
2
Modulator W N P .t/ D e i'.t / ; (1.13b)
Dispersive line W SQ P .!/ D e i'

00 .!! /2
R ; (1.13c)
Spectrometer W SQ A .!/ D e .!/ = ;

2 2
(1.13d)
Spectrographic techniques make use of two sequential filters, one time-stationary

(spectral filter) and one time-nonstationary (time gate) followed by a square-law
detector. The recorded signal is either a measure of the spectrum of a series of time
slices or a measure of the time of arrival of a series of spectral slices depending
upon the ordering of the filters. There is no difference in principle between the
two possible filter orderings and thus this type of apparatus should be thought of
as one that makes simultaneous measurements of the conjugate variables rather
than sequential measurements. The success of this approach has been extensively
demonstrated in the technique of frequency resolved optical gating (FROG) [10].
Tomographic techniques require in-series time-stationary and time-nonstationary
filters so that the entire phase-space can be explored. However, unlike spectro-
graphic techniques, the first filter in a tomographic apparatus is a phase-only
filter (either a quadratic temporal phase modulator or a quadratic spectral phase
modulator). The inclusion of a quadratic phase-only filter results in a distinctly
different interpretation of the measurement, leading to a fundamentally different
inversion algorithm. To see this, notice that a phase-only filter does not provide any
information on the frequency or the arrival time of a pulse ensemble and hence
does not constitute a measurement of either frequency or time. So, a tomographic
apparatus does not make a simultaneous measurement of these incompatible
variables. Rather, the quadratic phase modulation acts to rotate the phase-space.
The square-law detector in combination with the amplitude-only filter records the
resulting intensity distribution. A sufficiently large number of phase-space rotations
between =2 and =2 allows in principle reconstruction of the Wigner function
via the inverse Radon transform or of the ambiguity function via a set of inverse
Fourier transforms, but such task has not been performed experimentally. However,
the assumption that the pulse train is coherent reduces the requirements on the
modulator considerably. In that case, a complete rotation of the phase space density
is not necessary, and one can use two rotations with small angle (with one of them
possibly being zero) to reconstruct the amplitude and phase of the field.
Interferometric techniques require only one slice of the correlation function
(or equivalently, the Wigner function) to obtain the electric field amplitude and
phase. Roughly speaking, if one wishes to reconstruct the field at N time points,
then at least 2N independent data points are required. While interferometric
techniques are capable of reconstructing the field by recording only the necessary
2N points, spectrography and tomography require the measurement of N2 points.
The acquisition of excess data is necessary to obtain a reliable estimate of the pulse
shape. Of course, an overcomplete data set is available from direct measurement of
the entire correlation function as well.
1.3 A Catalogue of Methods
1.3.1 Intensity Autocorrelation
The simplest technique for gathering at least moderate quantitative information

about the temporal structure of an ultrashort pulse is the intensity autocorrelation.
In a conventional autocorrelator, two pulse replicas are mixed in a nonlinear
material, and the average power of a generated beam (measured with an integrating
detector) is recorded as a function of the relative delay between the two test pulse
replicas. By assuming a functional form for the temporal shape of the test pulse, one
can estimate its duration from the autocorrelation trace. Because of its simplicity,
autocorrelation is by far the most common method of “measuring” ultrashort optical
pulses. However, the autocorrelation trace by itself provides little more than an
estimate of the pulse duration.
The data consist of a one-dimensional array of numbers representing the output
pulse energy as a function of the delay, represented here by the function S2 ./. This
is related to the input field by
ZT
1
S2 ./ D dt j".t/" .t C /j2 : (1.14)
T
T
The autocorrelation yields directly a measure of the root-mean-square (rms)

pulse duration through the relation:
R
max
d 2 S2 ./
max
rms D R
max
: (1.15)
d S2 ./
max
However, the autocorrelation provides very little information about the temporal
phase structure of the pulse, so from it alone, there is no way to determine
whether all the frequencies of the pulse arrive at the same time or not. If they
do, then the pulse is said to be “transform-limited”, and has the shortest possible
duration consistent with a given spectrum. The pulse duration obtained from the
Fig. 1.2 Implementation of a

spectrogram
autocorrelation combined with the bandwidth obtained from a measurement of the

spectrum thus determines the proximity of the pulse to transform-limited duration.
If the pulse is not transform-limited, then these measurements are insufficient to
characterize the way in which the pulse is distorted. Thus there are two difficulties
with inferring the pulse shape from autocorrelation-related measurements: the
temporal intensity profile is not unique and the chirp cannot be determined [11].
1.3.2 Spectrograms
Spectrography is based on the sequential action of a time-stationary and time-

nonstationary filter (Fig. 1.2). Under experimentally accessible conditions, the
measured trace is exactly a spectrogram or a sonogram of the electric field under
test, as can be calculated for signal representation in many other domains [12].
A typical implementation of spectrography uses a temporal gate for the signal under
test (for example, the action of the pulse under test with one or several other pulses
in a nonlinear optical medium [13], or a “shutter” function provided by a temporal
modulator) and a device capable of measuring the optical spectrum (for example,
an optical spectrum analyser based on a diffraction grating and imaging optics, or
a scanning Fabry-Perot etalon, together with a photodiode whose time response is
longer than the inverse bandwidth of the spectrometer itself). The spectrogram of
the electric field of the test pulse is obtained by measuring the optical spectrum of
the pulse after temporal gating for various relative delays between the pulse and the
gate. The experimental trace is therefore:
ˇZ ˇ2
ˇ ˇ
S.!; / D ˇ E.t/R.t / exp.i !t/dt ˇˇ
ˇ (1.16)
Where ! is the optical frequency and the relative delay between the gate and the
test pulse. It is important that the resolution of the spectral filter is very high in order
to ensure that the measured trace is effectively the spectrogram of the test pulse.
A sonogram can be measured by reverting the order of the temporal and spectral
gate [13, 14].
The spectrogram is the double convolution of the Wigner function of the pulse
with the Wigner function of the gate with a change of sign on the frequency
variable [12]:
“
S.!; / D WE .t; ! 00 /WR .t ; ! ! 00 /dtd! 00 (1.17)
Thus, the pulse field may be estimated from a spectrogram by means of phase
retrieval that implements a deconvolution [15]. In fact, this is the only option if the
gate is unknown. The spectrogram of Eq. (1.16) is the modulus square of the short-
time Fourier transform of the pulse. The trick in phase retrieval is to estimate the
phase of the transform, since then, a Fourier transform would directly lead to the
recovery of the pulse under test and additionally the gating function.
Phase retrieval is usually ambiguous in one dimension, but is usually unique
in two dimensions. The excess data available in the spectrogram enables iterative
reconstruction of N complex numbers specifying the field from the N2 data points,
and this can also lead to the simultaneous reconstruction of the gate [16, 17]. Fur-
thermore, in the case of the nonlinear spectrogram, there is often a known functional
relation between the pulse and the gate, since the gate is often implemented as a
nonlinear interaction with replicas of the pulse under test. Also, other information
might be available, such as the spectrum of the pulse or the transfer function of the
gate. The recovery can be performed by means of several algorithms. A very robust
approach is based on the Principal Component Generalised Projections Algorithm
[18]. The protocol works as follows: from sampled representations of the field En
and gate Rn , one calculates the complex “square root” spectrogram. The modulus
of the calculated “square-root” spectrogram is replaced by the measured signal,
while the reconstructed phase is kept. A new set of representations (EnC1 , RnC1 )
is calculated by decomposing this constructed function into its singular values.
The pair of vectors corresponding to the largest singular value is taken as the set
(EnC1 , RnC1 ). The convergence of the algorithm can be monitored by examining
the difference between the measured spectrogram and the calculated one using, for
example, the rms difference. Also, the consistency of the decomposition into an
outer product can be quantified by considering the eigenvalues of the decomposition
since, for a perfect decomposition, there is only one non-zero singular value.
Moreover, the precision of the estimate of the field can be obtained from the
distribution of the eigenvalues [19].
1.3.3 Interferograms
Interferometry is a well-known approach to the characterization of optical fields

in the spatial domain. It is a simple method for converting phase information into
amplitude information that can then be read using square-law detectors. A similar
approach can be taken for the characterization of temporal fields. There are two
general classes: test-plus-reference and self-referencing. The former requires a well-
characterized reference pulse with spectral support across the entire bandwidth
of the test pulse, and with similar temporal support. On the other hand, self-
referencing interferometers can do without such an ancilla [20]. This is important,
since possessing a well-characterized reference pulse suggests that the problem of
measurement has already been solved.
A common means for characterizing spatial wavefronts is by spatial shearing
interferometry, in which the spatial phase profile of a beam is determined by
Fig. 1.3 A spectral shearing

interferometer
interfering it with a laterally shifted (or sheared) replica. The resulting intensity
interferogram can be measured with a square-law detector, and the phase simply
extracted. The spectral analogue, in which two spectrally sheared pulses are
interfered also allows direct reconstruction of the electric field in the spectral domain
using the measured spectral phase and a pulse spectrum [21].
We will focus here on techniques that use the two-frequency correlation
Q
function E.!/ EQ .! /, the phase '.!/'.! / of which can be concatenated
or integrated to get the spectral phase of the initial pulse (note that the spectral
intensity can be measured directly with an optical spectrum analyser). The spectral
shear is set by the sampling theorem, and it is typically a few percent of the total
bandwidth of the pulse under test. Too large a shear would lead to undersampling
of the pulse spectrum, while too small a shear could lead to increased sensitivity
to noise, and thus reduced precision and in some circumstances reduced accuracy
of the reconstruction. The spectral intensity can be obtained either from a separate
measurement using the spectrometer, or can be extracted from the correlation
function directly.
The quantity E.!/Q EQ .! / can be obtained by measuring the interference
of the pulse under test with its sheared replica with an optical spectrum analyser
(Fig. 1.3) The frequency shear can be implemented for example using a linear
temporal phase modulation exp.i t/. The spectral intensity of the two interfering
ˇ ˇ2 ˇ ˇ
pulses is ˇE.!/
Q ˇ C ˇE.!Q /ˇ2 C E.!/Q EQ .! / C EQ .!/E.! Q /. The
interferometric component of interest can be extracted from several measurements
of the spectral density for various relative phases between the two interfering
pulses. However, if a delay is introduced between the non-shifted and the shifted
replica, this leads to spectral fringes with small spacing, by virtue of the phase
'.!/ '.! / C !. In this case, the interferometric component can be directly
extracted using Fourier processing of a single interferogram [22].
1.3.4 Tomograms
The spectrum of a light source is easy to measure experimentally. Mathematically

it is the spectral projection of the Wigner function on the frequency axis. This is
the key to understanding tomography. If the pulse Wigner function can be rotated in
phase space, then a series of spectra measured for different rotation angles consti-
tutes the complete data set needed for tomographic inversion of the pulse itself.
Fig. 1.4 Simplified

chronocyclic tomography
It can be shown that an arbitrary rotation of the Wigner function can be imple-
mented using a combination of a quadratic temporal and spectral phase modulation.
Therefore, the chronocyclic tomography approach to the characterization of the
electric field consists in rotating the Wigner function by various angles using a
combination of quadratic temporal and spectral phase modulation and measuring
the spectrum of the field after manipulation, as shown in Fig. 1.4. From the set
of spectra, the Wigner function can be reconstructed using algorithms used in
tomography, such as the back-projection algorithm. This leads to the reconstruction
of the Wigner function of the source. Complete phase space rotations are hard,
however, so it is often preferred to use a simplified approach.
The simplified version of chronocyclic tomography uses a particular relation
between the frequency marginal of the rotated Wigner function and the electric field
[23, 24]. The fractional power spectrum of the pulse is obtained from the rotated
Wigner function:
Z
I˛ .!/ D W Œt cos.˛/ C ! sin.˛/; ! cos.˛/ t sin.˛/ dt (1.18)
The derivative of this function with respect to the angle of rotation ’ at ’ D 0

leads to:
Z Z
@I˛ @W @W @
D ! t dt D tW dt; (1.19)
@˛ @t @! @!
and therefore to

@I˛ @ @'
D I ; (1.20)
@˛ @! @!
A rotation of the phase space of the pulse requires a combination of a quadratic

temporal and spectral phase modulations. However, the relation in Eq. (1.17) also
holds for a shear of the phase space, in which ¨ is transformed into ¨ C §t, and
the temporal coordinate is unchanged. This can be accomplished by means of a
parabolic temporal phase modulation 12 t 2 alone. In this case one finds:
Z
@I0 @ @ @'
D W .! C t; t/dt D I : (1.21)
@ @ @! @!
This is the form most amenable to experiment, since the bandwidth required to
generate a small shear using a phase modulator is modest.
1.4 Case Study: SPIDER
Spectral phase interferometry for direct electric-field reconstruction (SPIDER) is a

particular implementation of spectral shearing. In its conventional form (as depicted
in Fig. 1.5), the spectral shear is created by upconverting two test pulses separated
in time by £ with a highly stretched copy of the test pulse (known as the ancilla)
by focusing into a .2/ nonlinear crystal. If the group delay dispersion (GDD) is
sufficiently large, then the frequency of the chirped pulse will remain approximately
constant over the duration of the individual test pulses. Since the test pulses are
delayed in time, they will interact with different frequencies from the chirped pulse,
whereby the difference is the spectral shear and is given by D =' 00 . Type-II
upconversion is used, since we require the phasematching function of the crystal
to support the full bandwidth of the test pulse replicas, but only a small bandwidth
from the ancilla. The pulses resulting from sum frequency generation between the
time delayed test pulses and the highly stretched pulses are spatially and spectrally
filtered from the second harmonic and fundamental pulses and then imaged onto the
entrance slit of a spectrometer.
After extracting the SPIDER phase .!/ D 'TP .! / 'TP .!/ via Fourier
processing and removal of the calibration phase ¨£, the spectral phase of the test
pulse can be reconstructed via concatenation:
8 P
< NnD1 .! C n/ if > 0
'TP .!0 C N / D .!0 / C P (1.22)
: N 1 .! C n jj/ if < 0:
nD0
Thus the spectral phase is reconstructed on a grid with spectral resolution . This
procedure is exact, but of course may undersample the spectral phase if the shear is
too large. An alternative method of reconstructing the spectral phase is via trapezium
integration as follows
XN
!n !n1
'TP !N D '.!0 / .!n /: (1.23)
2 nD1

Fig. 1.5 Conventional SPIDER concept

This method is exact for reconstructing the global GDD and third order dispersion
(TOD), which are normally of primary interest, and exact for the group delay locally.
Thus higher order phase can be reconstructed with sufficient accuracy if the shear
is suitably small such that the spectral phase can be approximated linearly over a
spectral range equal to the shear.
1.4.1 Optimal Design
When designing a new SPIDER or any other device, or using an existing setup, it
is necessary to consider the gross properties of the optical pulses that one wants to
be able to measure, and the range of values that these properties take on. Any given
device is designed for a particular range of parameters, such that the reconstructed
pulse will be accurate and within a specified precision [25]. When utilizing the
device outside this range, it may still be possible to obtain some information on the
pulse, but in general the accuracy of this information will diminish the further away
from this ideal range the test pulse becomes. Such considerations are a necessary
design prerequisite for every measurement device. Here, we concentrate on the first-
order design for a SPIDER instrument.
The primary parameters of importance in the design include the spectral range,
the amount of chirp, and the pulse complexity. Clearly the optics must be suitable
for the pulse spectrum and that of the frequency shifted pulses and the detector must
also be sensitive to the full spectral range spanned by both the fundamental and
frequency shifted pulses. However, the pulse bandwidth also determines the amount
of dispersion that must be applied to the ancilla to ensure upconversion with a quasi-
monochromatic frequency. Additionally, the ancilla dispersion, test pulse bandwidth
and test pulse dispersion are constrained for the same reason. The accuracy of the
reconstruction can also depend on the pulse complexity; unfortunately this can
be difficult or even impossible to quantify in general. However, there are some
important features that can be considered.
1.4.1.1 Spectral Shear
The most important parameter in any SPIDER device is setting the shear to the
correct value. According to the sampling theorem, for a given pulse with compact
support T, the spectral resolution and therefore the shear is constrained to:
2
D (1.24)
T:
This upper bound may not be attainable. Since the spectral phase is reconstructed
by concatenation of the SPIDER phase, the precision of the reconstruction is
proportional to the square root of the number of sampling points, which is itself
inversely proportional to the shear. Therefore it is best to set the shear close to the
sampling limit to optimize the precision.
In the case of a spectral phase that varies smoothly, it is possible to use a
shear larger than determined by the sampling limit, although it is still necessary
to reconstruct on a sampling grid with better resolution than the shear. This can be
achieved by using an integration scheme generalising Eq. (1.23). However, if the
GDD of the test pulse becomes too large, then the SPIDER phase will be aliased
(i.e. it will vary by more than ˙ between pixels). This increases the maximum
acceptable shear to:

; (1.25)
' 00 TP ı!max
where ı!max is the maximum spectral resolution of the spectrometer within the
spectral region covered by SPIDER interferogram.
1.4.1.2 Ancilla Chirp Rate
Another important aspect of a standard SPIDER (i.e. one that uses sum/difference
frequency generation to create the spectrally sheared pulses) is the chirp rate of the
ancilla. This is important since to be able to create spectrally sheared replicas of the
test pulse, one needs to ensure that the instantaneous frequency of the ancilla does
not vary significantly over the duration of the test pulse. However, increasing the
chirp rate also reduces the efficiency of the nonlinear process, and thus reducing the
sensitivity of the SPIDER apparatus. Therefore there is a balance between efficiency
and precision.
Calculating the optimal chirp rate would require exact knowledge of the test
pulse. However, it is possible to place some bounds on the chirp by considering
that the frequency sweep during the nonlinear interaction must be much smaller
than the spectral shear, i.e. >> ı!CP Š T =' 00 CP . Combining this relationship
with Eq. (1.24) allows one to determine the maximum temporal support of the test
pulse that can be accurately reconstructed, given the ancilla chirp rate:
T 2' 00 CP (1.26)
Note that in practice, this does not place a strict limit on the temporal window/chirp
rate because the frequency sweep is applied across the whole temporal window and
so the error in the spectral phase at a given frequency will still remain small. In
addition, the error will depend on the exact pulse shape. As an example, in [26],
a glass block is used to stretch the ancilla, introducing a GDD of 2 104 fs2 /rad;
this will enable accurate reconstruction of pulses up to at least 300 fs in duration.
Simulation has shown that a temporal window larger than a picosecond is required
before the reconstruction becomes unacceptably inaccurate.
It is also necessary to ensure that the stretcher used to chirp the ancilla applies
enough GDD to significantly stretch the pulse, and thus requires that the test pulse
has a minimum bandwidth. In the highly chirped limit, the pulse duration is given by
tchirp Š ' 00 !. This is valid when the chirped pulse duration is much larger than
the Fourier transform limited (FTL) pulse duration, i.e. tchirp >> tFTL ˛= !,
where ’ is a scaling factor that depends on the shape of the spectral intensity. Thus:
r
˛
! >>
' 00 CP
p
tFTL << ˛' 00 CP (1.27)
For a Gaussian spectral intensity and defining the pulse duration/bandwidth over
the full width at half maximum (FWHM), ’ D 4ln2. Eq. (1.27) is a stringent limit,
therefore the much greater (less) than symbols should be read as at least (most) 10
(.1) times the right hand side. To illustrate, a spectral bandwidth of at least 0.1 rad/fs
( œ 30 nm @ œ0 D 800 nm) or FTL pulse duration of at most 30 fs is required for
the device in [26].
It should be noted that Eqs. (1.26) and (1.27) place sufficient bounds on the pulse
duration that can be measured for a given ancilla chirp (or equivalently the ancilla
chirp required to measure a particular pulse). This can be understood more clearly if
one asks the following questions: (1) what is the minimal spectral bandwidth of the
pulses and (2) what is the maximum dispersion (and hence maximum time window)
that one can measure with any given device.
1.4.1.3 Test Pulse Separation (£)
Another design parameter is that of the temporal separation between the test pulse
replicas. This parameter is constrained by the resolution of the spectrometer, such
that it must be necessary to resolve the fringes; and it is also constrained by the need
to be able to isolate the sidebands from the DC term during Fourier filtering. The
sidebands are located at pseudo times tQ Š ˙, and the width of the DC term and
the sidebands are given by at most 2T, the limits are given by:

2T < < (1.28)
ı!max
1.4.1.4 Crystal Thickness
The final design parameter is the crystal thickness. If the crystal is too thin, then
the signal may be too weak to measure. However, if the crystal is too thick, then
phasematching can restrict the bandwidth of the upconverted pulses to less than
the fundamental. It should be noted that the effect of the phasematching function
of the crystal is to reduce the signal in the wings of the interferogram, and thus
reduce the precision at those locations and not the precision overall. By considering
longitudinal phase matching, the length of the crystal is given by
2
L< ; (1.29)
k .!0 ; !/
where:
k .!0 ; !/ Š .2!0 ˙ !/ n .2!0 ˙ !/ =c .!0 ˙ !/

n .!0 ˙ !/ =c !0 n .!0 / =c
is the momentum mismatch between the ancilla, test pulse and signal pulse. In [26],
a 30 m crystal was used, which can support upconversion of pulses spanning 550–
1200 nm when upconverting with 750 nm. The wavelength range can be extended
by angle tuning (dithering) the crystal.
1.4.1.5 Pulse Complexity
One final note should be made about SPIDER’s ability to measure complex pulses.
Provided the pulse being measured is within the bounds specified by the parameters
noted above, one can in principle measure a pulse of any shape and therefore any
complexity. This is true except for one caveat: the interferometric term extracted
from the SPIDER interferogram must have sufficient intensity at every sampling
point of the reconstruction grid to enable accurate determination of the SPIDER
phase at those points. If the intensity falls below the noise floor, then the SPIDER
phase at that point becomes undetermined, and therefore the relative phase of the
spectral regions either side of that point is also undetermined. This can have quite
significant consequences for the temporal reconstruction. Such a problem can be
alleviated by making the spectral shear large enough to span any spectral holes.
This of course will reduce the sampling of the spectral phase within the separated
spectral regions. In the case that this needs to be sampled with a fine resolution,
one may take multiple measurements with different sized shears, such that the small
shear measurement can be used to accurately reconstruct the individual spectral
regions, and the larger shear measurement to obtain the relative phase between the
separated regions, as demonstrated in [27, 28].
1.5 Conclusions
The establishment of general principles of pulse characterization, and the instanti-

ation of these principles in several different techniques, suggests that the field of
ultrafast pulse characterization is a mature one. Indeed, some of the methods have
proven commercially viable, so that they have passed from being laboratory tools to
being workaday devices.
The concepts of spectrography, tomography and interferometry serve as the
major classifications for pulse shape characterization, and each may be implemented
using appropriate linear optical elements. The use of linear temporal modulators as
time-nonstationary filters in these classes of measurement has been detailed and
experimental implementations for characterization presented. As research in both
signal analysis and ultrafast optics is in continual development, it can be expected
that further exciting discoveries will be made in the near future.
The field of ultrashort pulse measurement at present is moving a number of
different directions. Now that the basic principles are well established, and the most
simple and reliable apparatuses have been demonstrated, the application to more
complex fields is underway. This includes determining the space-time structure of a
pulse, rather than simply its temporal structure, as well as identifying the fields of
pulses that are not close to the transform limit, or which may have highly structured
spectra. In another direction, the techniques developed for the optical domain are
finding application in the characterization of pulses in quite different spectral and
temporal domains, including that of attosecond duration XUV pulses generated via
high harmonic radiation from atoms.
Underlying all of this, however, is fundamental notion, well exemplified in
optics, that the development of new tools underpins scientific discovery, so that
as new methods arise, and old ones evolve, we can be sure there will emerge new
phenomena. Conversely, new science underpins the development of new technology,
so we can also be sure that there will be new techniques and applications arising
from new discovery. The symbiosis between science and technology is clear: the
generation, amplification and measurement of short electromagnetic pulses has
opened new vistas in physics, chemistry and materials science, as well as in
applications such as biomedicine and telecommunications. It should be anticipated
that accurate and precise measurement methods will continue to play a key role in
discovery and innovation.
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Chapter 2
Ultra-Broadband Optical Parametric Amplifiers
Giulio Cerullo and Daniele Brida
2.1 Introduction
Many modern studies of light-matter interaction require optical pulses with short
durations as well as broad frequency tuneability. Both properties are of utmost
importance for time-resolved optical spectroscopy and high-field physics. In fem-
tosecond pump-probe spectroscopy, the system under study (atom, molecule or
solid) is resonantly excited by a “pump” pulse and its subsequent evolution is
monitored by measuring the pump-induced transmission change of a delayed
“probe” pulse [1]. To be able to probe elementary photophysical and photochemical
relaxation processes, it is necessary to push the temporal resolution towards the
limit set by the oscillation period of the carrier wave. The need to excite a system
on resonance and probe optical transitions occurring at different photon energies
requires broad frequency tuneability of both pump and probe pulses [2]. On the
other hand, by focusing high-intensity ultrashort pulses in a noble gas jet, it
is possible to produce coherent bursts of XUV radiation by the so-called High
Harmonic Generation (HHG) process [3] (See Chap. 3 by Marangos et al. and
Chap. 7 by Mathias et al.). Also for the HHG process, wavelength tuneability of
the driver pulses is important, since it influences both the frequency extension and
the phase-matching conditions of the XUV pulses. In view of the above mentioned
applications, the generation of tuneable few-optical-cycle light pulses is one of the
major challenges of ultrafast optics [4].
Nowadays, several reliable sources of femtosecond pulses exist, based for
example on Ti:sapphire or Ytterbium technologies; however they emit only at fixed
frequencies. Despite this limitation, the very high peak power of these sources
enables exploiting the second order nonlinear optical effect known as Optical
G. Cerullo () • D. Brida

Dipartimento di Fisica, Politecnico di Milano, Piazza L. da Vinci 32, 20133 Milan, Italy
e-mail: giulio.cerullo@fisi.polimi.it

24 G. Cerullo and D. Brida
Fig. 2.1 (a) Optical

Parametric Amplification in a
non-centrosymmetric
nonlinear crystal (b)
corpuscular interpretation of
the OPA process
Parametric Amplification (OPA) [5, 6] to extend their tuning range. The principle of
OPA is quite simple (Fig. 2.1a): in a suitable nonlinear crystal, energy is transferred
from a high frequency and high intensity beam (the pump beam, at frequency ! 3 ) to
a lower frequency, lower intensity beam (the signal beam, at frequency ! 1 ) which
is thus amplified; in addition a third beam (the idler beam, at frequency ! 2 ) is
generated. The OPA process can be given a simple corpuscular interpretation (see
Fig. 2.1b): a photon at frequency ! 3 is absorbed by a virtual level of the material
and a photon at frequency ! 1 stimulates the emission of two photons at frequencies
! 1 and ! 2 . In this interaction energy conservation:
„!3 D „!1 C „!2 (2.1)
is fulfilled. The signal frequency to be amplified can vary in principle from ! 3 /2

(the so-called degeneracy condition, with ! 1 D ! 2 ) to ! 3 , and correspondingly the
idler varies from ! 3 /2 to 0 (as a matter of the fact the lowest frequency is limited by
absorption of the nonlinear crystal).
In summary, the OPA process transfers energy from a high-power, fixed fre-
quency pump beam to a low-power, variable frequency signal beam, generating an
idler beam to satisfy energy conservation. The OPA process thus provides an optical
amplifier with continuously variable centre frequency and represents an easy way
of tuning over a broad range the frequency of an otherwise fixed femtosecond laser
system. On the other hand, if suitably designed, an OPA can have a very broad
amplification bandwidth and thus efficiently transfer energy from a narrowband
pump pulse to a broadband signal pulse; it can therefore be used to dramatically
shorten, by more than an order of magnitude, the duration of the pump pulse. The
concept of broadband OPA is very flexible and can be applied to produce few-
optical-cycle pulses over a very wide frequency range, provided that a broadband
yet weak seed is available and the proper phase-matching conditions are identified.
This chapter reviews the principles of ultrashort pulse OPAs, focusing in
particular on the generation of few-optical-cycle pulses. It is organized as follows:
Section 2.2 discusses the propagation of an ultrashort pulse in a nonlinear medium;
Sect. 2.3 reviews the theory of parametric amplification for the case of monochro-
matic waves; Sect. 2.4 extends it to the case of ultrashort pulses; Sect. 2.5 discusses
the architecture of ultrafast OPAs and gives a relevant example; Sect. 2.6 reviews
ultra-broadband OPAs; Sect. 2.7 explains how OPAs can be used to stabilize the
carrier-envelope phase of ultrashort pulses; finally, Sect. 2.8 introduces the concept
of optical parametric chirped pulse amplification, the most promising approach for
energy scaling of ultrashort pulses.
2 Ultra-Broadband Optical Parametric Amplifiers 25
2.2 Ultrashort Pulse Propagation in a Nonlinear Medium
In this section we briefly derive the equation for the propagation of an ultrashort
pulse in a dispersive nonlinear medium, that will be used in the remainder of the
chapter [6–8]. We start from Maxwell’s propagation equation for the electric field E
of a scalar plane wave:
@2 E 1 @2 E @2 P
D 0 (2.2)
@z2 c02 @t 2 @t 2
where c0 is the speed of light in vacuum and P is the polarisation describing the
medium response. We write the electric field as:
1
E.z; t / D RefA .z; t/ expŒi .!0 t k0 z/ g D fA .z; t / expŒi .!0 t k0 z/ C c:c:g
2
(2.3)
where A(z,t) is the complex field envelope. In the following we will for simplicity
drop the notation Re f: : :g. The polarisation can be decomposed in the sum of a
linear (PL ) and a non-linear (PNL ) component:
P .z; t / D PL .z; t/ C PNL .z; t / (2.4)
Let us initially consider only the linear component of the polarisation:
PL .z; t / D pL .z; t / expŒi .!0 t k0 z/ (2.5)
and solve the equation:
@2 E 1 @2 E @2 PL
D 0 (2.6)
@z2 c02 @t 2 @t 2
Equation (2.6) is more easily solved in the frequency domain, by introducing the
Fourier transforms:
EQ .z; !/ D AQ .z; ! !0 /exp.i k0 z/ (2.7a)
PQL .z; !/ D pQL .z; ! !0 /exp.i k0 z/ (2.7b)
and becomes:
@2 EQ !2
2
C 2 EQ D 0!
2
PQL (2.8)
@z c0
which, with the help of (2.7), can be rewritten as:
@2 AQ @AQ 2 Q !2 Q
2i k0 k0 A C AD 0!
2
pQL (2.9)
@z2 @z c02
We now make the Slowly Varying Envelope Approximation (SVEA), which consists
@2 AQ @AQ
in assuming that 2
k0 ; this corresponds to neglecting variations of
@z @z
the envelope over propagation lengths of the order of the wavelength. With this
assumption we obtain:
@AQ !2
2i k0 k02 AQ C 2 AQ D 0!
2
pQL (2.10)
@z c0
From the definition of refractive index n(!), we can write:

pQL .!/ D "0 n2 .!/ 1 AQ .!/ (2.11)
and obtain:
@AQ
2i k0 D k 2 .!/ k02 AQ (2.12)
@z
!
with k .!/ D n .!/. In a dispersive medium, the refractive index is a function
c0
of frequency, and the wavenumber thus becomes a nonlinear function of !. We can
further approximate:
k 2 .!/ k02 Š 2k0 Œk .!/ k0 (2.13)
We now perform a Taylor expansion of k(!) around ! 0 :
1
k .!/ D k0 C k 00 .! !0 / C k 000 .! !0 /2 C : : : (2.14)
2

dk 1
where k 00 D D , vg0 being the group velocity of the carrier frequency
d! !0 vg0
2
d k
and k 000 D the Group Velocity Dispersion (GVD). Usually an expansion
d ! 2 !0
up to the second order is sufficient, with the third order required only for very broad
pulse bandwidths. Equation (2.12) then becomes:
@AQ .! !0 / 1 1
i Š .! !0 / AQ C k 000 .! !0 /2 AQ (2.15)
@z vg0 2
We can transform (2.15) back to the time domain, obtaining:
@A .z; t / 1 @A i 00 @2 A
C k0 2 D0 (2.16)
@z vg0 @t 2 @t
Equation (2.16) describes the linear propagation of a pulse in a dispersive medium.

We now introduce the nonlinear polarisation, which can be written as:

PNL .z; t / D pNL .z; t /exp i !0 t kp z (2.17)
We have emphasized that the wavenumber kp of the nonlinear polarisation at ! 0

is different from that of the electric field. Matching of the wave-vectors kp D k0
(phase matching) is the key for an efficient nonlinear interaction. If we make the
approximation that the envelope pNL varies slowly over the timescale of an optical
@2 pNL @pNL
cycle, so that ; !0 << !02 pNL , we can write:
@t 2 @t
@2 PNL
2
Š !02 pNL exp i !0 t kp z (2.18)
@t
and finally obtain the equation:
@A 1 @A i 00 @2 A 0 !0 c
C k 0 2 D i pNL exp Œi kz (2.19)
@z vg0 @t 2 @t 2n0
where k D kp k0 is the so-called “wave-vector mismatch” between the nonlinear

polarisation and the field. This equation will be used in the next section to derive the
coupled nonlinear equations for second-order parametric interaction.
2.3 Theory of Optical Parametric Amplification
Let us consider an optical field, consisting of the superposition of three waves, at

frequencies ! 1 , ! 2 and ! 3 :
1 A1 .z; t / exp Œi .!1 t k1 z/ C A2 .z; t / exp Œi .!2 t k2 z/ C

E .z; t / D (2.20)
2 A3 .z; t / exp Œi .!3 t k3 z/ C c:c:
satisfying the condition ! 1 C ! 2 D ! 3 , impinging on a medium with a second order

nonlinear response:
PNL .z; t / D "0 .2/

E 2 .z; t/ (2.21)
Such a situation is known as “nonlinear second-order parametric interaction” and

corresponds to an exchange of energy between the three fields mediated by the
second order nonlinearity. The nonlinear polarisation will contain three components
at frequencies ! 1 , ! 2 and ! 3 , given by:
.2/
"0
P1NL .z; t / D A2 A3 exp fi Œ!1 t .k3 k2 / z C c:c:g (2.22a)
2
.2/
"0
P2NL .z; t/ D A1 A3 exp fi Œ!2 t .k3 k1 / z C c:c:g (2.22b)
2
.2/
"0
P3NL .z; t / D A1 A2 exp fi Œ!3 t .k1 C k2 / z C c:c:g (2.22c)
2
Obviously there are other terms on PNL at different frequencies, such as for example
2! 1 , 2! 2 , ! 1 –! 2 : : : Here we consider only the terms at ! 1 , ! 2 and ! 3 because
we assume that only the interaction between these three fields is efficient, due to the
phase-matching condition. We can then derive the following three equations for the
fields at ! 1 , ! 2 and ! 3 :
@A1 1 @A1 i @2 A1
C k 001 2 D i 1 A2 A3 exp Œi kz (2.23a)
@z vg1 @t 2 @t
@A2 1 @A2 i @2 A2
C k 002 2 D i 2 A1 A3 exp Œi kz (2.23b)
@z vg2 @t 2 @t
@A3 1 @A3 i @2 A3
C k 003 2 D i 3 A1 A2 exp Œi kz (2.23c)
@z vg3 @t 2 @t
!i .2/
where we have defined the nonlinear coupling coefficients: i D and the
4cni
“wave-vector mismatch” as: k D k3 k1 k2 . The three equations are coupled
nonlinear partial differential equations, are in general not amenable to an analytic
solution and must be treated numerically. A first simplification, that captures the
main physics of second order parametric interaction, consists in neglecting the GVD
terms, i.e. putting k 00i D 0. This is justified by considering that the three interacting
pulses are propagating with very different group velocities vgi . Unless one considers
ultrashort pulses, the effects of this group velocity mismatch (GVM) are much more
relevant than those of GVD between the different frequency components of a single
pulse. The coupled equations can be further simplified by moving to a frame of
z
reference translating with the group velocity of the pump pulse D t , and
vg3
become:
@A1 @A1
C ı13 D i 1 A2 A3 exp Œi kz (2.24a)
@z @
@A2 @A2
C ı23 D i 2 A1 A3 exp Œi kz (2.24b)
@z @
@A3
D i 3 A1 A2 exp Œi kz (2.24c)
@z
where ıi 3 D v1gi v1g3 i D 1; 2 is the GVM between signal/idler and pump

waves. These are nonlinear coupled partial differential equations that can be solved
numerically. To get some physical insight, we can start by considering quasi-
@
monochromatic waves, which allows us to set D 0. A further approximation
@
can be made by assuming that the conversion efficiencies are so low that pump
depletion can be neglected, i.e. A3 Š A30 D constant. We thus obtain the nonlinear
coupled equations for the signal and idler waves:
d A1
D i 1 A3 A2 exp Œi kz (2.25a)
dz
d A2
D i 2 A3 A1 exp Œi kz (2.25b)
dz
Equation (2.25a) can be easily rewritten as:
d 2 A1 d A1
D i k C 2 A1 (2.26)
d z2 dz
2deff 2 !1 !2
where 2 D I3 and I3 D 12 n3 c"0 jA3 j2 is the pump beam intensity. The
c03 "0 n1 n2 n3
nonlinear coefficient deff is proportional to the element of the (2) tensor that keeps
trace of the polarisation of the beams and their propagation directions within the
nonlinear crystal lattice.
In the hypothesis of an initial signal field amplitude A1 .0/ D A10 (the “seed
beam”) and no initial idler (A2 .0/ D 0), the solutions of Eqs. (2.25) are:
( 2 )

I1 .z/ D I10 1C sinh .gz/ (2.27a)
g
2
!2
I2 .z/ D I10 sinh .gz/ (2.27b)
!1 g
q
k 2
where g D 2 2
. For the case of large gain (gz >> 1) Eqs. (2.27) further
simplify to:

I10 2
I1 .z/ D exp .2gz/ (2.28a)
4 g
!2
I2 .z/ D I1 .z/ (2.28b)
!1
giving an exponential growth of both signal and idler intensities with crystal length,
characteristic of an optical amplifier. It should also be noted, that, in the large gain
limit, signal and idler intensities are related by energy conservation, since for each
annihilated pump photon a signal and an idler photon are simultaneously generated.
The parametric gain for the signal beam, in the large gain limit, can be written as:

I1 .z/ 1 2
GD D exp .2gz/ (2.29)
Is0 4 g
Let us now discuss the factors influencing this gain:
1. G / exp(g) exponentially depends on the parameter g, which is maximum when
k D 0 (phase-matching condition). G rapidly decreases for non-zero values of
k, suggesting that phase-matching is a key condition to be fulfilled in order to
get significant amplification from the non-linear material.
2. G / exp(deff ) depends exponentially on the second order nonlinear optical
coefficient of the crystal deff ; one should therefore select the crystal with the
largest nonlinear response. There are however other considerations leading to the
choice of the crystal, such as phase matching range, dispersive properties, and
optical damage threshold.
3. G scales as the exponential of the square root of the pump intensity. This indicates
the suitability of ultrashort pulses for OPAs, due to their high peak powers. One
should try to use the highest possible pump intensity before the onset of other
nonlinear optical phenomena such as self-focusing, self-phase modulation and
beam breakup. In order to be able to use high pump intensities, it is however
important to have a spatially clean beam profile, without hot spots.
4. G scales as the exponential of the crystal length, as in an optical amplifier. With
ultra-short light pulses, however, the optimum crystal length has to be chosen
considering the durations and group velocities of the interacting pulses.
5. G scales as the exponential of the square root of the product of signal and idler
frequencies. This seems to indicate an advantage to use higher pump frequencies.
However we will see that with ultrashort pulses this advantage is often offset by
the larger difference in group velocities of the interacting pulses.
The gain of an OPA is similar to that of a classical optical amplifier based on
population inversion, but with some important differences;
1. an OPA does not have any energy storage capability, i.e. the gain is present only
during the pump pulse;
2. the gain centre frequency is not fixed, but can be continuously adjusted by
varying the phase-matching condition;
3. the gain bandwidth is not limited by the linewidth of the transition, as in an
amplifier based on population inversion, but rather by the possibility of satisfying
the phase-matching condition over a broad range of frequencies.
2.4 Parametric Amplification with Ultrashort Pulses
So far we have considered the theory of OPAs with monochromatic waves. When
dealing with ultrashort pulses, one should in principle perform a full numerical
solution of Eqs. (2.23). However, considerable physical insight can already be
derived from the simpler Eqs. (2.24), showing that the efficiency of the process
is governed by the GVM between the interacting pulses. In particular, GVM
between the pump and the signal/idler pulses limits the interaction length over
which parametric amplification takes place, while GVM between the signal and
the idler beams limits the phase matching bandwidth [9]. Given a pump pulse with
duration £, one can define a pulse splitting length Lsp as the propagation length
after which the signal (or the idler) pulse temporally separates from the pump pulse
in the absence of gain, which can be expressed as:

Lspj3 D ˇ ˇ j D 1; 2 (2.30)
ˇı j 3 ˇ
Note that the pulse splitting length becomes shorter for decreasing pulse duration
and for increasing values of GVM, depending on the crystal type, pump wavelength
and type of phase matching. There is a qualitatively significant difference between
the cases in which •13 and •23 have the same or different signs. When •13 •23 > 0,
both the signal and the idler pulses walk away from the pump in the same direction
so that the gain rapidly decreases for propagation distances longer than the pulse
splitting length and eventually saturates. On the other hand, when •13 •23 < 0, signal
and idler pulses move in opposite direction with respect to the pump; in this way
the signal and idler pulses tend to stay localized under the pump pulse and the gain
grows exponentially even for crystal lengths well in excess of the pulse splitting
length. This situation is illustrated in Fig. 2.2, showing simulations of the evolution
of the temporal intensity profiles inside the gain medium, obtained by numerical
solution of Eqs. (2.24).
Figure 2.2a shows a simulation for the case •13 •23 > 0; one can see that,
for propagation lengths greater than the pulse splitting length, the parametric
amplification process stops as the signal and idler pulses linearly walk away from
the pump. Figure 2.2b shows a simulation for the case •13 •23 < 0. Here we see that
the signal growth stays exponential for propagation distances well exceeding the
pulse splitting length and that the signal pulse tends to stay localized under the
pump. To understand this effect we can consider the situation in which the signal
pulse has moved slightly to the left and the idler pulse to the right of the pump
pulse. During the parametric amplification process, the signal pulse generates idler
photons, which move to the right, i.e. towards the peak of the pump; in turn, the
idler pulse generates signal photons which move to the left, again towards the peak
of the pump. This concentration of photons under the peak of the pump explains the
exponential gain growth overcoming GVM effects.
Fig. 2.2 Simulated signal intensity profiles of OPAs in a frame of reference moving with the pump
pulse: (a) for the case •13 > 0, •23 > 0: signal and idler are slower than the pump and the effective
crystal length is equal to the pulse splitting length between pump and signal, after which both
pulses walk away from the pump; (b) for the case •13 > 0, •23 < 0: signal and idler walk in different
directions with respect to the pump, as a result they stay trapped under the pump, increasing the
interaction length
Let us now discuss which conditions determine the gain bandwidth of an OPA.
Ideally one would like to have a broadband amplifier, i.e. an amplifier which, for a
fixed pump frequency !N 3 , provides a more or less constant gain over an as broad
as possible range of signal frequencies. To this end, one needs to keep the phase
mismatch k as small as possible over a large bandwidth. Practically, however,
the phase-matching condition can be satisfied only for a given set of frequencies
(!N 1 ; !N 2 ; !N 3 ), such that:
k D k .!N 3 / k .!N 1 / k .!N 2 / D 0 (2.31)
If the pump frequency is fixed at !N 3 and the signal frequency changes to !N 1 C !,

then by energy conservation the idler frequency changes to !N 2 !. The ensuing
wave vector mismatch becomes:
k D k .!N 3 / Œk .!N 1 / C k1 Œk .!N 2 / C k2 D k1 k2 (2.32)
which can be approximated to the first order as:
@k1 @k2
kD !C ! D ı12 ! (2.33)
@!1 @!2
1 1
where ı12 D is the GVM between signal and idler pulses. The full
vg2 vg1
width at half maximum parametric gain bandwidth for a crystal of length L can
then be calculated from Eq. (2.29), within the large gain and low pump-depletion
approximations, as:

4 log .2/1=2 1=2 1
!D (2.34)
L jı12 j
Equation (2.34) shows that the gain bandwidth is inversely proportional to the GVM
between signal and idler and has only a square root dependence on small-signal gain
and crystal length. For the case when vg1 D vg2 (group velocity matched OPA), Eq.
(2.34) loses validity and (2.33) must be expanded to the second order in !, giving:

4 log .2/1=4 1=4 1
!D ˇ 00 ˇ (2.35)
L ˇk1 C k2 00 ˇ1=2
In this case the gain bandwidth is inversely proportional to the square root of the sum
of the GVDs of signal and idler pulses. The conditions for achieving group-velocity
matched OPAs will be discussed in Sect. 2.6.
2.5 Ultrafast OPA Architecture
A general scheme of an ultrafast OPA is presented in Fig. 2.3. The system is

powered by energetic femtosecond pulses, such as those produced by an amplified
Ti:sapphire laser at 800 nm or by an Ytterbium laser at 1 m. A fraction of the beam
is split and used to generate the seed beam. Then the pump beam (which may be
optionally frequency doubled) and the seed, after their timing has been adjusted by
a delay line, interact in a first amplification stage. It is possible to further amplify
the signal in a second stage (power amplifier), using a previously split fraction
of the pump beam. The two-stage approach has two advantages: (i) it allows one
to compensate for the GVM arising between pump and signal pulses in the first
stage; (ii) it enables one to adjust the pump intensity, and thus the parametric gain,
separately in the two stages. In particular the power amplifier requires a much lower
gain. At the OPA output, after the pump has been spectrally filtered, both signal
and idler beams are available. In some cases, it may be necessary to use a pulse
compressor to restore the transform-limited (TL) duration of the pulses.
The first stage of any OPA is the seed generator, i.e. a stage producing the
initial photons at the signal wavelength. Since the seed beam is at a different
wavelength with respect to the pump beam, a nonlinear process is required for its
production. The two main techniques employed for seed generation are white-light
continuum (WLC) generation and parametric superfluorescence. The WLC seed has
the advantages of much higher stability and nearly diffraction-limited spatial beam
quality, and is thus the most widely used.
As an example, we show in Fig. 2.4 a typical setup for a near-IR OPA [10]: it is
pumped by an amplified Ti:sapphire laser generating 500- J, 50-fs pulses at 1 kHz
repetition rate. A small fraction of the pump (2 J) is used to generate a WLC
seed in a 2-mm-thick sapphire plate. 50 J are used to pump a pre-amplifier stage
Fig. 2.3 Scheme of an ultrafast optical parametric amplifier. BS beam splitter, OPA optical
parametric amplification stage
Fig. 2.4 Scheme of a near-IR OPA. BS beam splitter, DM dichroic mirror, LPF long-pass filter,
VA variable attenuator
consisting of a 3-mm-thick “-barium borate (BBO) crystal cut for type II phase
matching (™ D 26ı , ® D 0ı ). Wavelength tuning is achieved by tilting the crystal,
thus changing the phase-matching condition. Typical signal energies after the pre-
amplifier are up to 6 J. The power amplifier stage consists of an identical BBO
crystal pumped by 450 J; in this case amplified pulse energies up to 200 J are
generated. The signal beam is tuneable from 1.1 to 1.6 m and the idler up to
2.8 m, limited by absorption in the BBO crystal; pulsewidth ranges from 30 to
50 fs according to wavelength.
2.6 Ultra-Broadband OPAs
Equation (2.34) makes it clear that, in order to obtain broad phase matching
bandwidths, one must achieve, for a given signal frequency !N 1 , •12 D 0, i.e. group
velocity matching between signal and idler pulses. It will then become possible
to amplify a broad bandwidth centred around !N 1 . We will show in the following
that, by using suitable non-linear crystals, pump frequencies and phase-matching
configurations !N 1 can be varied over a very broad range, spanning from the visible
to the mid-infrared, enabling the generation of widely tuneable few-optical-cycle
light pulses from OPAs.
In an OPA using a collinear interaction geometry, the propagation direction
inside the nonlinear crystal is selected to satisfy the phase-matching condition
(k D 0) for a given signal wavelength. In this configuration the signal and
idler group velocities are in general not matched. Group velocity matching can
be obtained in a type I (or type 0 in a periodically poled crystal) degenerate
configuration, in which signal and idler have the same frequency (! 1 D ! 2 D ! 3 /2)
and the same polarisation.
If the signal wavelength is tuned away from degeneracy, then the •12 D 0
condition is generally not fulfilled in a collinear configuration, leading to narrow
phase-matching bandwidths. An additional degree of freedom can be introduced
using a non-collinear geometry [11], in which pump and signal wave-vectors form
an angle ’ (independent of signal wavelength) and the idler is emitted at an angle
with respect to the signal. In this case the phase matching condition is a vector
equation, k3 D k1 C k2 that, when projected on directions parallel and perpendicular
to the signal wave-vector, becomes:
k3 cos ˛ D k1 C k2 cos (2.36a)

k3 sin ˛ D k2 sin (2.36b)
Note that the angle is not fixed, but it depends on the idler frequency according to
Eq. (2.36b). If the signal frequency increases by !, the idler frequency decreases
by ! and the wave-vector mismatches along the two directions parallel and
perpendicular to the signal wavevector can be approximated, to the first order, as:
@k1 @k2 @
kpar Š !C cos ! k2 sin ! (2.37a)
@!1 @!2 @!2
@k2 @
kperp Š sin ! C k2 cos ! (2.37b)
@!2 @!2
To achieve broadband phase matching, both kpar and kperp must vanish. Upon
multiplying (2.37a) by cos and (2.37b) by sin and adding the results, we get
@k2 @k1
cos D0 (2.38)
@!2 @!1
Fig. 2.5 Scheme of a BBO based NOPA pumped at 400 nm. BS beam splitter, SPF shortpass filter
which is equivalent to:
vg1 D vg2 cos (2.39)
Equation (2.39) lends itself to a very simple geometrical interpretation [12]: in a

non-collinear configuration, broadband phase matching can be achieved for a signal-
idler angle such that the signal group velocity equals the projection of the idler
group velocity along the signal direction. The so-called non-collinear OPA (NOPA),
is a widely used device for the generation of few-optical-cycle pulses in the visible
range [13–18]. In a practical situation the pump-signal angle ’ is determined by the
propagation direction of the seed beam, while the signal-idler angle adjusts itself,
according to (2.36b), to satisfy the phase-matching condition. For this reason, the
idler is emitted at a different angle for each wavelength, i.e., it is angularly dispersed
and not easily usable.
In the following we will describe a typical visible NOPA design [19], the
schematic of which is shown in Fig. 2.5. The system is pumped by an amplified
Ti:sapphire laser generating 150-fs, 800-nm pulses at 1 kHz with energy up to
500 J. The energy is sufficient for simultaneously pumping several independent
NOPAs. A fraction of the beam is used to generate the pump pulses at 400 nm
by second-harmonic generation in a 1-mm-thick BBO crystal; pulse energies up
to 30 J are used to pump the first stage. Another small fraction of the beam,
with energy of approximately 2 J, is focused into a 1-mm-thick sapphire plate
to generate the WLC seed; by carefully controlling the energy incident on the plate
(using a variable-optical-density attenuator) and the position of the plate around the
focus, a highly stable single-filament WLC is generated. The chirp of the visible
portion of the white light is small and fairly linear with frequency. To avoid the
introduction of additional chirp, only reflective optics are employed to guide the
WLC to the amplification stage. Parametric gain is achieved in a 1-mm-thick BBO
crystal, cut for type I phase matching (™ D 32ı ), using a single-pass configuration to
increase the gain bandwidth. The chosen crystal length is close to the pulse-splitting
length Lsp13 for signal and pump in the visible wavelength range. To minimize the
effects of self-focusing, the BBO crystal is beyond the focus of the pump beam. The
WLC seed is imaged by a spherical mirror in the BBO crystal, with a 100- m spot
size matching that of the pump beam. A thin short-pass filter removes the strong
residual 800-nm component from the WLC, preventing its parasitic amplification.
When the BBO crystal is illuminated by the pump pulse and aligned perpendic-
ularly to the pump beam, it emits a strong off-axis parametric superfluorescence in
the visible in the form of a cone with apex angle of 6.2ı (corresponding to an
angle of 3.82ı inside the crystal); this is the direction for which the group velocities
of signal and idler are matched and therefore the gain bandwidth is maximized.
The visible cone gives a visual aid to the identification of the optimum condition
for broadband generation, which is found when the pump-signal angle matches the
cone apex angle. In this condition, for optimum pump–seed delay, an ultrabroad
gain bandwidth that extends over most of the visible (500–750 nm) is observed.
The amplified pulses from a single stage have energy of approximately 2 J; much
higher energies, up to 300 J [20], can be extracted by a second amplification
stage. After the gain stage the amplified pulses are collimated by a spherical mirror
and sent to the compressor.
Several compressor schemes have been implemented for the visible NOPA.
Simple prism pairs can correct the second but not third-order dispersion and thus
can only compress the pulses down to 10–15 fs; sub-10-fs pulses can be achieved
by using either prism-grating [17] or prism-chirped mirrors combinations, as well as
adaptive compressors based on deformable mirrors [20–22]. It is also possible to use
exclusively chirped mirrors [19, 23], greatly simplifying the system design, allowing
for compactness, insensitivity to misalignment and high day-to-day reproducibility,
which are of great importance in practical applications.
2.7 Carrier-Envelope Phase Stabilization in an OPA
The previous paragraphs illustrated ultra-broadband OPA configurations capable

of producing widely tuneable few-optical-cycle pulses. Here we will show how
these schemes can be extended to the synthesis of pulses with controlled carrier-
envelope phase (CEP), i.e. with an electric field profile reproducible from shot to
shot. Mathematically, the electric field of an ultrashort pulse can be written as:
E.t/ D A.t/ cos .!c t C / (2.40)
where A(t) is the pulse envelope with its maximum at t D 0, ! c is the carrier
frequency and is the CEP. If D 0, a maximum of the electric field corresponds
to the peak of the pulse envelope (cosine pulse), while if D /2 the electric
field at the peak of the pulse envelope is zero (sine pulse). Control of the CEP
Fig. 2.6 Frequency and phase summation rules for (a) sum-frequency generation (SFG), (b)
difference-frequency generation (DFG), equivalent to the generation of the idler wave in an OPA,
and (c) a four-wave mixing process (FWM)
becomes important for few-optical-cycle light pulses and for extreme nonlinear
optics experiments, which are sensitive to the electric field rather than the intensity
of the pulse.
Typical femtosecond laser sources generate a pulse train in which the CEP is not
stabilized, so that varies randomly from shot to shot. CEP can be stabilized using
either active or passive methods. Active control starts by measuring the pulse-to-
pulse CEP slip in a mode-locked oscillator and stabilizing it by active electronic
feedback [24]; by picking pulses at a fraction of the laser repetition rate, it is possible
to obtain a train of pulses with a constant absolute phase, which can be further
amplified. A completely different approach is passive CEP stabilization, which
exploits nonlinear optical effects to generate a pulse train with stable CEP [25].
To understand passive CEP stabilization, let us review the effect of different non-
linear processes on the CEPs of the interacting pulses. For the second-order process
of Sum-Frequency Generation (SFG), in which two pulses at frequencies ! 1 and ! 2 ,
with CEPs 1 and 2 , generate the sum frequency ! 3 D ! 1 C ! 2 , the CEP of the
resulting pulse is 3 D 1 C 2 /2 (Fig. 2.6a). For the particular case of second
harmonic generation (SHG) starting from a pulse with frequency ! 0 and CEP , one
obtains a pulse with frequency ! SH D 2! 0 and CEP SH D 2 /2. In the second-
order process of Difference-Frequency Generation (DFG) between two pulses at
frequencies ! 1 and ! 3 , with CEPs 1 and 3 , the resulting difference-frequency
pulse has frequency ! 1 D ! 3 ! 2 and CEP 1 D 3 2 /2 (Fig. 2.6b). In
the third order non-linear process of Four-Wave Mixing (FWM), four waves at
frequencies ! 1 , ! 2 , ! 3 and ! 4 , with ! 4 D ! 1 ! 2 C ! 3 , are coupled in a (3)
nonlinear medium. In this case, the CEPs of the waves are linked by the relationship:
4 D 1 2 C 3 /2 (Fig. 2.6c). Self-Phase Modulation (SPM), i.e. spectral
broadening due to the instantaneous intensity-dependent variations of index of
refraction in a Kerr medium, can be regarded as a special case of FWM, in
which a new frequency ! SPM is generated starting from three frequencies ! 1 ,
! 2 and ! 3 , all belonging to the pulse spectrum, according to the FWM process:
! SPM D ! 1 C ! 2 ! 3 . These new frequencies in turn contribute to subsequent

FWM processes, causing a progressive broadening of the pulse spectrum as it
propagates through the nonlinear medium. If we now consider that the mixing
pulses share the same CEP 1 D 2 D 3 D , then the SPM pulse will have
the CEP SPM D 1 2 C 3 /2 D /2. Thus the newly added frequency
components of the broadened SPM spectrum inherit the original value of the CEP
of the driving pulse. The SPM/FWM process is the dominant nonlinear interaction
behind WLC generation.
Having clarified the effects of nonlinear optical processes on the CEPs of the
interacting pulses, we are now in a position to understand the passive CEP stabi-
lization method. If a DFG process ! DF D ! 2 ! 1 occurs between two pulses with
the same shot-to-shot CEP fluctuations ( 1 D C c1 , 2 D C c2 ), then DF D c2 –
c1 /2 D const., i.e., the fluctuations of are automatically cancelled [25]. Passive
CEP stabilization has some clear advantages with respect to the active one: (i) it is
an all-optical technique and does not require any electronic feedback circuits; (ii) it
directly produces a train of CEP-stable pulses, avoiding the need to pick pulses.
Let us now discuss how CEP stable pulses can be generated from an OPA. We
start by recalling that the idler pulse is generated through a DFG process between
pump and signal, so that its CEP, according to the previous discussion, is given by
2 D 3 1 /2. Let us now consider an OPA that is pumped by pulses at the
fundamental frequency (FF) ! 0 , with CEP 3 D which is generally fluctuating
from shot to shot. If the seed pulse is produced via WLC generation starting from
the FF pulse, then its CEP is linked to that of the pump by 1 D /2 (see
Fig. 2.7c); in this case the idler has CEP 2 D 0, which is stable from shot to shot
(Fig. 2.7b). When the OPA is pumped by the second harmonic (SH) of the driving
pulse, then 3 D 2 /2; if the WLC seed is generated from the SH of the driver,
then 1 D 2 and 2 D 0 (Fig. 2.7). We can thus conclude that an OPA generates
a CEP stable idler when the seed is generated with the same pulse used as the pump,
either the FF or the SH of the driving laser.
If, on the other hand, the OPA is pumped by the SH but the seed is generated
from the FF, we have 3 D 2 /2 and 1 D /2. In this case, we obtain
2 D /2, so that the idler is not CEP stabilized, but rather reproduces, from
shot to shot, the CEP fluctuations of the driving pulse [26].
2.8 Optical Parametric Chirped Pulse Amplification
In a broadband OPA both the pump and the seed are femtosecond pulses, typically
generated by a Ti:sapphire system. It is generally difficult and expensive to scale
the energy of femtosecond pump lasers; on the other hand, it is easier to generate
energetic picosecond pulses (5–50 ps duration) exploiting well-established gain
media such as Nd: or Yb:doped crystals. With a long pump pulse, in order to achieve
efficient energy extraction, it is necessary to temporally overlap the seed pulse
with the pump by first stretching the seed pulse and then, after the amplification
Fig. 2.7 Schematics of three OPA configurations. For clarity, the seed and the pump beams are
shown to intersect non-collinearly in the crystal. However, the conclusions are also valid for the
collinear beam arrangement
step, recompressing it back to nearly TL durations. This scheme, which is very

similar to the Chirped Pulse Amplification (CPA) [27] occurring in a real gain
medium, is known as OPCPA [28, 29] and is considered as the most promising
route for energy scaling of few-optical-cycle pulses [30]. The key technical hurdle
in OPCPAs is the synchronization of the pump and seed pulses; it can be achieved
either electronically, using suitable circuitry, or optically, by using a part of the seed
pulse spectrum to injection seed the pump laser. The optical approach allows a much
lower pump-seed timing jitter but it is more challenging, since pump and seed are
at different frequencies.
The OPA/OPCPA approaches offer some distinct advantages with respect to CPA
for the generation of high peak power few-optical-cycle pulses:
1. the OPA/OPCPA has the capability of providing a high gain in a relatively short
path, allowing a compact, tabletop amplifier setup, minimizing the linear and
nonlinear phase distortions and ensuring an excellent temporal and spatial quality
of the pulses.
2. with suitable selection of the phase-matching conditions (see Sect. 2.6), the OPA
process can provide gain bandwidths well in excess of those achievable with
conventional amplifiers and can sustain pulse spectra corresponding to a TL
duration of just a few cycles of the carrier frequency.
3. in an OPCPA, amplification occurs only during the pump pulse, so that amplified
spontaneous emission and the consequent pre-pulse pedestal are greatly reduced.
4. since the OPA/OPCPA is an instantaneous process of energy exchange between
the interacting beams, no fraction of the pump photon energy is deposited in the
medium; thus, if parasitic pump absorption can be neglected, thermal loading
effects are absent, greatly reducing spatial aberrations of the beams. This allows
much higher repetition rates to be achieved while avoiding the heat removal
problems that limit the frequency scaling of CPA systems.
In addition to these clear advantages, the OPA/OPCPA concept also has some
drawbacks:
1. an OPA/OPCPA requires pump pulses with short duration (hundreds of femtosec-
onds to tens of picoseconds), which are technologically challenging to generate,
especially at high energy and/or high repetition rate; on the other hand the CPA,
thanks to energy storage in the excited state, can use much longer nanosecond
pump pulses (or even continuous wave pumping for materials with long excited
state lifetime like Yb-doped crystals);
2. an OPA/OPCPA is very sensitive to the spatial and temporal quality of the pump,
again putting a severe technological constraint on the pump laser.
2.9 Conclusions
This chapter has provided a brief review of the principles of ultrashort pulse OPAs,
focusing in particular on the generation of few-optical-cycle pulses. After discussing
the propagation of an ultrashort pulse in a nonlinear medium and reviewing the
theory of parametric amplification, we considered the typical architecture of an
ultrafast OPA. This chapter went on to discuss non-collinear OPAs, which are
widely used for the generation of few-optical-cycle pulses in the visible range and
capable of producing pulses with energies of 2 J, which can be further amplified to
300 J. These schemes can be extended for the synthesis of pulses with controlled
carrier-envelope phase. Indeed, the last section of this chapter introduces the concept
of optical parametric chirped pulse amplification, which is considered the most
promising approach for energy scaling of few-optical-cycle pulses.
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Chapter 3
Attosecond Generation and High Field Physics
Jon P. Marangos and Malte Oppermann
3.1 Introduction: Why Make Attosecond Measurements?
This chapter is intended as a general introduction and overview of some of the

key aspects of attosecond measurement technology and of the strong field laser
physics that underlies much of it. For more comprehensive and detailed material
the reader should refer to the original research papers and reviews cited within the
text. Other chapters in this volume deal with related subjects: phase stabilised few
cycle laser pulses, metrology of attosecond pulses, free electron lasers and High
Harmonic Generation (HHG) sources for imaging.
An attosecond is 1018 s or 1,000th of a femtosecond and we will loosely
(and perhaps optimistically) refer to the “attosecond time domain” whenever we
are targeting sub-femtosecond processes. As things stand, most of the action so
far in attosecond science is involved in resolving processes with timescales from
a few femtoseconds down to just under 100 attoseconds. Future sources may
well reach the 10 attosecond to few attosecond range. Zeptosecond domain pulses
(1 zeptosecond D 1021 s) may eventually be available, certainly HHG is capable
of generating the 1 keV bandwidths required to create such pulses, but we will not
touch on that science here.
The femtosecond domain is a timescale of great importance to physical processes
because it is the natural timescale for vibrational modes of motion in molecular and
condensed phase systems (phonons). So for instance the fastest vibration (in H2 ) has
a period of just 8 fs whilst large molecule vibrational modes may have periods of
many picoseconds. This sets the timescale for what we would conventionally view
as chemical change, which involves the motion of an atom or group of atoms from
one location to another within a molecule. Indeed “femtochemistry” has been an
J.P. Marangos () • M. Oppermann

Blackett Laboratory, Imperial College, London, South Kensington SW7 2AZ, UK
e-mail: j.marangos@imperial.ac.uk

46 J.P. Marangos and M. Oppermann
area of great activity over the last two decades (note the award of the 1999 Nobel
prize in Chemistry to Ahmed Zewail for his development of that subject) covering
investigation from diatomic molecules to large biomolecules. The principal tool
for femtosecond chemistry is the mode-locked laser that typically provides pulses
of duration as short as 20 fs which through various non-linear optical processes
can routinely span the range of wavelengths from 200 nm to 5 m. These pulses
comprise multiple cycles of the carrier frequency of the optical domain laser field.
Typically, a pump-probe methodology is adopted where a pump interaction is used
to “start” the event and then it is probed after a short delay t. This allows us to
capture the state of the system at a time t after the event starts. To build up the full
dynamics it is necessary to repeat the measurement over the desired range of t.
One reason for needing measurements with just a few femtosecond resolution
is that some chemical events are very fast (such as proton transfer) and if we
wish to capture them with sufficient resolution for a full understanding, pulses
significantly shorter than the event are needed. This certainly justifies the progress
in generating optical domain pulses to the few femtosecond (few optical cycle)
limit. There is, however, a more profound reason for seeking a sub-femtosecond
temporal resolution and that is to target electron dynamics within matter. The recent
development of new tools enables these measurements and a far more sophisticated
understanding of the fast dynamics in matter after electronic excitation can be
obtained. Electrons move very quickly within matter, often on timescales measured
in 10’s of attoseconds. Moreover, in almost all matter the electrons are bound in
very close proximity to other electrons and so their dynamics are highly correlated
through both the Coulomb interaction and quantum mechanical exchange effects.
Although this may not be apparent in our everyday perception of matter, it is of cru-
cial importance if we are to understand or control the microscopic states of matter,
goals which are at the core of many emerging twenty-first century technologies [1].
Through attosecond science we are developing the tools required to measure these
ultra-fast correlated electron processes (for a detailed review see [2]).
For instance in the last 5 years advanced quantum chemistry calculations by the
groups of Cederbaum in Heidelberg [3] and Levine in USA/Israel [4] have revealed
that sudden photo-excitation in polyatomic molecules leads to large amplitude
charge migration (rapid motion of the hole through the molecular structure) driven
by the electron correlations (See Fig. 3.1). This occurs on timescales of just a few
femtoseconds down to less than 100 attoseconds, and crucially before any nuclear
motion has begun. The universality of this charge migration phenomenon is just
beginning to be recognised and the coupling to subsequent physical and chemical
changes due to the nuclear motion that it drives is an open question. There is,
therefore, a target to understand such processes in gas and condensed phase systems
and this motivates further advances in attosecond sources. Other areas that are the
target of attosecond science include: ultrafast (few fs) nanoplasmonics, ultrafast
x-ray spectroscopy and chemical processes at surfaces (see Chap. 7 by Mathias
et al.). A summary of current approaches to making ultrafast structural dynamics
methods can be found in Altucci et al. [6].
3 Attosecond Generation and High Field Physics 47
Fig. 3.1 Charge migration as an example for electron dynamics in molecular systems. The figure
shows a numerical simulation of the 3D-charge density evolution after initial ionisation of the
molecule 2-phenylethyl-N,N-dimethylamine (PENNA) at three different time steps. The hole
density is shaded in light grey, whereas the electron density is depicted in dark grey. The left
panel shows the evolution for the ground-state geometry of the molecule, whereas the right panel
shows the process for the C–C bond between the benzene ring and the N-atom elongated by 20 pm
[5] (Reproduced with permission from Ref. [5])
The resolution of a measurement with a light pulse (e.g. in a pump-probe scheme)

is clearly limited by the pulse duration, which in turn is limited by the transform
limit, i.e. for an optical pulse of duration , the spectral bandwidth required to sup-
port it is constrained (for a Gaussian waveform) by the relationship > 0.44.
So a 5 fs pulse requires a bandwidth of 88 THz, which for a carrier of 800 nm is a
spectral bandwidth of 300 nm and 2 optical cycles (cycle period 2.7 fs). Pulses
of 5 fs duration are now possible to create in dispersion managed mode locked
oscillators and for higher power applications via a number of non-linear optical
strategies (see Chap. 2 by Cerullo et al.). For a pulse of 1 fs duration a bandwidth of
440 THz is required which clearly requires a higher frequency carrier (into the deep
UV) and for 0.1 fs a 4,400 THz bandwidth (that is a photon energy spread of 18 eV)
requiring a carrier at least into the extreme ultraviolet spectral range. The creation of
these pulses relies upon the high order non-linear interaction of an optical domain
laser pulse and we will see that it is in fact the carrier wave of the optical field that
plays the crucial role in determining the attosecond resolution. It is necessary to
use the carrier-wave frequency rather than the pulse envelope duration to provide
the temporal resolution. To do this requires high order nonlinearity from an intense
field and a stable carrier waveform (a so called carrier envelope phase (CEP) stable
pulse). See Chap. 6 by Udem et al. for a discussion of CEP stabilisation.
A high order non-linearity permits access to timescales that are only a fraction of
the optical cycle time of the laser field. We shall see later there are other potential
methods for creating sub-femtosecond pulses: broadband Raman generation, pulse
shaping of free electron laser emission and relativistic high order harmonic genera-
tion. Nevertheless, all of these also rely in one way or the other on the interaction of
free or bound electrons with few cycle phase stabilized high intensity optical pulses.
Therefore our next task is to gain an understanding of the salient physics of the
interaction of a strong field with matter.
3.2 The Physics of High Harmonic Generation
3.2.1 Free Electron in a Strong Field
Consider the motion of a free classical electron interacting with a laser electric field
of peak amplitude E0 and angular frequency !. Assuming a linearly polarised field
in the x-direction of the cosinusoidal form (i.e. ignoring the spatial and suppressing
the polarisation properties):
E.t/ D E0 cos.!t/ (3.1)
The typical wavelength of optical light (2 107 to 5 106 m) is much larger than
the size of atoms, or even the excursions electrons make in a moderately intense
field, which justifies the suppression of the spatial dependence. We confine our
discussion to lower intensities (<<1017 Wcm2 ) so no relativistic effects arise. The
field will of course exert an oscillatory force on the electron (charge e and mass m)
and thus a time-dependent acceleration of magnitude:
d2 x e
2
D E0 cos.!t/ (3.2)
dt m
The equation of motion can be solved to yield the time dependent oscillatory
velocity and displacement of the electron, taking into account any initial conditions
for velocity or position. The amplitude of the electron oscillation is given by:
eE0
x0 D (3.3)
m! 2
We can see that the displacement depends linearly upon the electric field and
inversely to the frequency squared (i.e. quadratically with the wavelength). For
example, in a field of wavelength 1 m at an intensity of 1014 Wcm2 the oscillation
amplitude is 1 nm (109 m), which is 10 atomic radii. This illustrates that in a
strong field the excursion of the field driven electron can cause it to be far removed
from the influence of the atomic core (which is the basis of the strong field limit
discussed below).
The cycle averaged kinetic energy of the electron is called the ponderomotive
energy Up and is given by:
e 2 E02
Up D (3.4)
4m! 2
For the example just discussed (wavelength 1 m at an intensity of 1014 Wcm2 )

the ponderomotive energy will be 10 eV. This will scale with the square of the
electric field (i.e. linearly with the laser intensity) and with the inverse square
of the frequency (i.e. with the square of the laser wavelength). Thus we can
increase the ponderomotive energy by a factor of 4 by doubling the wavelength
(e.g. from 10 to 40 eV by changing the laser wavelength from 1 to 2 m at fixed
intensity).
3.2.2 Interaction with Matter – Ionisation in a Strong Field
In general we are most interested in what happens when the strong field interacts not
with an initially free electron but with an electron bound in an atom or molecule. The
interaction of a strong laser field with matter is in general a very complex problem
(see Cohen Tanoudji [7]). As a simplification we will assume that the field is non-
resonant (far detuned from any single photon transition frequency in the system),
low frequency (photon energy much less than the ionisation potential) and that the
field is very strong so that (a) it can be regarded as a classical field and (b) the
binding potential can start to be considered as weak with respect to the interaction
with the interaction with the laser field.
It is important to note that within the multiphoton picture a strong field can give
rise to very high order processes that include absorption of multiple photons into
excited states. Typically multiphoton ionisation starts to appear at intensities in the
range from 1011 to 1013 Wcm2 (depending on the atomic ionisation potential and
possible existence of multiphoton resonances). Transitions between laser dressed
states of the continuum can become probable in a strong field giving rise to high
orders of photoelectron absorption (called above threshold ionisation, ATI). These
excited states can radiate back to the ground state if parity is satisfied (odd number of
photons absorbed) giving rise to the phenomenon termed high harmonic generation
(HHG).
Unfortunately the usual quantum theoretical approaches are either very difficult
to implement accurately (such as high order perturbation theory) or don’t provide
much physical insight into the process (numerical solution of the time-dependent
Schrödinger equation) at these high field strengths. Fortunately the strong field in
the problem gives rise to a great conceptual simplification that has an accompanying
powerful theoretical and simple physical insight for the calculation of HHG: the
Strong Field Limit first developed by Corkum [8] and Schafer et al. [9]. The so
called “simple man’s” or “3 step” model for HHG and other strong field processes
Fig. 3.2 Illustration of the three step model, with the driving laser electric field E(t) displayed in
the lower part of the figure. Directly above, the two ground state electrons in the atom’s Coulomb
potential are displayed, where Ip is illustrated as the energy required to transfer one of them to the
continuum. Their time-evolution in the laser field is described by the three step model, where in
the last step the electron recombines with the parent ion, releasing a photon of energy -h!
is as follows (see Fig. 3.2). In this limit we can view the effect of the strong field as
a strong periodic distortion of the binding potential due to the interaction with the
combined Coulomb and laser fields.
Ze 2 1
V .x/ D C .e/E.t/x (3.5)
4"0 r
Where r is the radial distance from the nucleus and x the coordinate in the laser field
direction, Z the ion charge (Z D 1 for the singly ionised atom).
The distortion can be so great that the resulting potential barrier is instan-
taneously suppressed below the bound state energy – leading to the classical
freeing of the electron. Yet it is more likely that the potential barrier is lowered
but still higher than the bound state energy. In this case there is a probability
for quantum mechanical tunnelling to occur. If tunnelling has a high probability
of occurring within an optical cycle, then tunnel ionisation will dominate over
multiphoton ionisation. The ionisation rate then becomes strongly time dependent,
with significant magnitude only around the peaks of the laser field jE.t/j [10]. We
now introduce the Keldysh parameter [11]. The case where < 1 corresponds to the
strong field limit, where tunnelling ionisation starts to dominate:
s
Ip
D (3.6)
2Up
The Keldysh parameter decreases as the square root of the laser intensity and as
the inverse of the laser wavelength. It is therefore much easier to reach the tunnelling
regime with near IR lasers than visible-UV, the fact that titanium sapphire lasers at
800 nm is thus advantageous although increasingly longer wavelength fields derived

from optical parametric conversion are being employed in strong field research.
The three step picture of HHG follows from tunnel ionisation in the strong
field. So the first step is that the IR field ionises the atom or molecule via optical
tunnelling. Ionisation occurs near the peaks of the oscillating electric field. The
tunnelling rate is exponentially sensitive to the area under the barrier which is
determined by the bound state energy and the laser field strength:
" 2=3 #
2 2Ip
exp (3.7)
3E.t/
The ionisation rate also depends upon the “shape” of the atomic or molecular
wavefunction in the region of the barrier, this can be critically important in
determining the ionisation dynamics of a specific state. The formula for tunnelling
derived for atoms by Ammosov, Delone and Krainov (ADK) theory [12–15] is a
useful guide that captures these features:

.2l C 1/ .l C jmj/Š 3E.t/ 1=2 2F0 2n jmj1 2F0
w.t/ D Cn2 Ip exp
2jmj jmjŠ .l jmj/Š F0 E.t/ 3E.t/
(3.8)
The above ADK tunnelling rate w(t) is given for an initial state characterized by its
effective principal quantum number n* D Z(2 F0 )1/2 , its principal quantum number
n, orbital angular momentum l and magnetic quantum number m. Furthermore Z is
the ionic charge state, Ip the ionisation potential in atomic units (au), F0 D (2Ip )3/2
the intra-atomic field strength (au) and E(t) the linearly polarised time dependent
electric field amplitude (au). Progress is being made to extending durable theoretical
treatments to the ionisation of molecular systems [16, 17].
If the electron is released after the field peak, the classical trajectory it takes can
lead to it returning to the ion from which it was ionised within an optical cycle.
Of course the electron is not a simple classical particle, instead it is most correctly
described as being in a wavepacket of many continuum states consistent with the
initial localisation at the moment after tunnelling. The initial wavepacket is related
to the boundstate wavefunction but with a transverse Gaussian filter applied from
the tunnelling process [18]. The wavepacket state inevitably undergoes quantum
diffusion (wavepacket spreading) due to the non-zero momentum components that
comprise it. For the fullest description, the continuum electron states must be
regarded as in a laser dressed state continuum state (Volkov state). An important
property is that the continuum wave-packet position expectation value hri is
oscillatory as we can anticipate for the classical free electron case just discussed.
The tunnelling process will result in an amplitude for ionisation and an amplitude
for the electron to remain bound, so the wavefunction of the electron should be
viewed as a superposition of these two components. The consequence of this is that
there is the possibility for the continuum part of the electron wavefunction to return
and re-interact with ion at a slightly later time (determined by the optical cycle)
and this has big role in control of light emission and other strong field processes.
The recolliding continuum wavepacket interferes with the remaining bound state,
resulting in high frequency oscillations in the electron’s dipole moment, radiation
from which leads to high-order harmonic generation (HHG) (corresponding to the
recombination process).
3.2.3 Recollision Processes
The nature of the HHG process in a strong laser field, and the importance of
this process to attosecond measurement, is encapsulated in the “three-step” picture
described in the previous section. In the first step the laser field ionises the atom
or molecule through field ionisation (predominately quantum tunnelling through
the field suppressed potential barrier) which occurs with high probability when the
electric field amplitude is near a peak. The exponential dependence of the tunnelling
rate ensures that the ionisation is confined in time to ˙200 attosecond (for an
800 nm laser field) around the cycle peak. In the next step, the liberated electron
wavepacket moves in response to the laser field: first being accelerated away
from the parent ion, and then returning at some later time on the order of half
an optical cycle period (typically 0.5–1.5 fs for a laser field at 800 nm) as the
laser field reverses direction. During this process the electron wavepacket gains
energy from the laser field. The third step is a recombination process in which
the energy gained is emitted as a high energy photon with the electron returning
to the ground state of the parent system. The spectrum extends up to a cut-off
energy set by the maximum possible electron return energy which from classical
considerations is 3.17Up C Ip . The recombination is inherently confined in time to a
period of a few hundred attoseconds, which will be discussed later. The discovery,
elucidation and application of this process to attosecond measurement are very
important developments that have paved the way to attosecond science.
The theoretical description of this process is captured in essence by the so called
Strong Field Approximation (SFA) theory of Lewenstein et al. [19]. A development
from SFA casts the strong field process in terms of all the possible quantum paths
that an electron may follow. Only a few of these turn out to make a significant
contribution to the HHG process, those that satisfy the correct conditions for the
momentum and position at the time of birth (zero initial momentum, initially
located at the exit of the quantum tunnel) and return (returning to atomic centre).
Mathematically these “saddle point” conditions greatly reduce the computation of
all the quantum path integrals. Moreover the concept of quantum paths essentially
allows us to make direct contact with the classical trajectories and in fact the
classical motion of electrons in the combined Coulomb and laser field thus gives
a powerful insight into the process.
The electron interacts with the ionic core if it approaches close enough on its
return to the parent ion. A number of processes can occur during this re-encounter
Fig. 3.3 Schematic representation of recollision induced processes
(see Fig. 3.3). These processes include inelastic excitation of the ion during
the collision that may result in excitation or further ionisation. Elastic collision
will also occur and has recently proved to contain useful information on the
molecular structure encoded through the diffraction effect from multiple centres in
the molecule [18], a process termed laser induced electron diffraction. The electron
may also recombine back into the state it left resulting in the molecule returning to
the initial state of energy and, if the resulting harmonic photon is forward scattered
in the direction of the laser field, the momentum is also the same as before. In
this case the molecule is equivalent to all others in the sample. Provided there is a
degree of macroscopic phase matching preserved the emitted harmonics can be a
strong signal, albeit with an overall energy conversion efficiency typically <<106 .
This is the reason for the coherent addition of the electric field signals that is at the
heart of all optical parametric processes and results in a N2 scaling of the intensity of
emitted radiation (N number of atoms/molecules in the interaction region), and the
fact that the emission is confined into a narrow low divergence beam in the forward
scattering direction. We will describe this process in more detail below, particularly
how it can lead to the generation of isolated attosecond duration soft X-ray pulses
that can be used in subsequent measurements.
3.3 Attosecond Pulses from HHG
3.3.1 Temporal Qualities of HHG Emission
The quantum orbit model uses the saddle point method to select a finite number of
orbits which can be summed up to approximate the entire integral. This approach
allows individual or groups of trajectories to be studied in isolation. Thus we can
continue to use our purely classical picture of the electron trajectories to gain deep
insight into the process. To account for quantum contributions to the trajectories we
must also account for the ionisation process and the action S(t,t0 ) accumulated by
the electron during the trajectory which determines the phase:
0ˇ ˇ2 1
ˇ* ˇ
ˇ ˇ
*
0
Z t B ˇp.t; t / C A./ˇ C
B C
S.t; t 0 / D d B C Ip C (3.9)
t0 @ 2 A
The correct summing of these trajectories must include the phase which clearly
depends upon the time spent in the continuum for the trajectory D t t0 . The birth
time t0 also determines the momentum gained by the electron upon its return.
After tunnelling, the electron position x(t) and velocity v(t) are determined by the
field according to the equations [8]:
eE0
x.t/ D Œ cos.!t/ C v0x t C x0x (3.10)
m! 2
eE0
vx .t/ D sin.!t/ C v0x (3.11)
m!
Here, the x-axis corresponds to the polarisation direction of the field and x0x and v0x
are the initial conditions at the time of tunnelling, which are set to 0 in the simplest
approximation.
The solution to these equations shows that half the electrons (those born after the
peak in each half cycle) will return to the origin (x D 0) at least once. Electrons born
before a cycle peak will never return and instead will undergo displaced oscillatory
motion in the field that drifts away from the atom. Further, these equations show that
it is the electrons born at 0.047 of an optical cycle after the peak of the field (i.e. at a
phase of 170 ) that return at the maximum energy of 3.17Up. We shall refer to these
as the maximum return energy electrons. These electrons return after D 0.6 T of
an optical cycle (that is 1.6 fs for an 800 nm field).
Electrons born either immediately before or after the maximum return energy
electrons also return to the atom, but with reduced energy and a different return
time . Those born after the maximum return energy electrons return sooner than
the maximum return energy electrons and so are referred to as having “short trajec-
tories”. Short trajectory electrons have a definite dependence of increasing return
energy with increasing return time, they show a “positively chirped” behaviour (see
Fig. 3.4). Electrons born before the maximum return energy electrons will return
after longer times and have a return energy that decreases with return time (they are
negatively chirped) and this group are referred to as “long trajectories”.
To quantify the relationship between the return energy Er and return time for
the short trajectories, Lein [20] has made a good fit to the exact classical result for
driving field of angular frequency ¨ and ponderomotive energy Up using the form:
Fig. 3.4 Time dependent properties of the trajectories describing the free electron motion in a
strong laser field. The top panel shows the excursion distance x(t) as a function of time within an
optical laser cycle for electrons born at different times after the peak of the field. The trajectory with
maximum return energy is highlighted. The bottom panel shows the return energy as a function of
the electron’s return time and thereby illustrates which photon energies and hence frequencies are
emitted at which point in time. This contains information about the chirp of the harmonic emission
1:207 0:492
Er Er
! D 0:786 f C 3:304 f (3.12)
Up Up
Where the function f (x) is defined as f(x) D arccos(1 x/1.5866)/. How close
these results are to the real situation where quantum effects and the full molecular
potential are also present has been the subject of recent research that has so far
concluded that these approximations are fairly reliable for plateau harmonics up to
the cut-off (up to a shift of less than 100 attoseconds), although the results may be
less reliable for harmonics close to threshold.
In the discussion so far we have not considered phase matching of the harmonic
emission from the macroscopic sample. In general this is a complicated subject
as several contributions to the wavevector mismatch k must be considered that
originate from geometrical (Guoy) phase as the fields propagate through the focus,
material dispersion, intensity dependent dipole phase (related to the action integral)
and dependent upon the local intensity I(r,t), dispersion of free electrons (also time-
space dependent). Accurate computation of phase matching must take into account
the real temporal and spatial distribution of the laser field and typically one-
dimensional calculations are not sufficient for anything other than indicative results.
Nevertheless, by reasonable choices of gas density, gas path length (typically kept
small relative to the laser Rayleigh range), laser focusing and position of the sample
a robust trajectory selection can be achieved e.g. so only short trajectory harmonics
are observed and the emitted spectral amplitude can be a faithful reflection of the
single molecule emission.
At first glance it might appear that the existence of these ranges of return times
and return energies will simply “smear out” the HHG emission so that it is not useful
for attosecond pulse production. In fact this is not so if isolation of short (or long)
trajectories is achieved via phase matching in the sample. Details can be found in
the literature [21], but in essence the action leads to different accumulated phases in
short and long trajectories that can be balanced against the geometrical phase. Short
trajectories are strongly favoured if the gas sample is confined to a location around
a Rayleigh range downstream of the laser focus. Further the mapping of return
energy to time have been experimentally confirmed [22] by the use of the RABBITT
technique that characterises the relative phases between neighbouring harmonics
and so allows the reconstruction of the time history of emission of different
harmonic orders. This work confirms that the harmonics emitted from each half-
cycle of the field will have a chirp on the attosecond timescales. Various methods to
correct for this are being actively considered, including carefully prepared optical
fields to compress the recollision times of the highest energy returning electrons
and use of soft-X-ray optical filters with the appropriate dispersion to correct for the
chirp in the field.
3.3.2 Attosecond Pulse Production
We now turn to the experimental state-of-the-art for HHG based attosecond sources.
From the description of the temporal dependence of HHG emission it is clear that
each half-cycle of an intense optical field will give rise to ionisation events that
lead to electron trajectories that can return and result in emission of HHG radiation.
This radiation will be emitted in a burst with a duration spanning several hundred
attoseconds. For a multi-cycle laser pulse where the optical field strength varies little
over several cycles there will therefore be two attosecond bursts per cycle. These
are for electrons colliding from opposites sides each cycle and the interference
between these events leads to the odd order harmonic emission within this picture.
The resulting attosecond pulse train (APT), with oppositely phased fields emitted
every half-cycle, will be radiated in this multi-cycle limit.
It is clear that an attosecond pulse train will accompany all HHG generation
although it was only in the last decade or so that the sub-cycle temporal structure
was fully characterized and explained. Accessing this temporal structure is not
trivial and requires considerable precautions to deliver the distinct pulses in the
train to an experiment and utilise them. Work in this direction followed the first
characterization of an APT by the RABBITT technique and was pursued by
groups in France and in particular in Sweden (Lund) [23]. The approach being
pursued in Lund is to reconstruct the photoelectron wavepacket generated by the
attosecond pulses in the train, which is done by utilising the IR field (synchronised
to the APT but with a controllable relative delay) to shift the momentum of the
electron wavepacket by an amount that depends upon the IR field phase at the
time of photoionisation by the attosecond XUV pulse (see below in the description
of streaking) [24]. The momentum distribution of the generated electron wave
packets is recorded using a velocity map imaging detector. Consecutive electron
wavepackets will thus overlap and interfere at the detector and from the interference
the spectral phase of the wavepacket can be reconstructed. It is hoped that the
photoelectron wavepacket can then be related back with sufficient fidelity to the
original electronic ground state dynamics.
The challenge of producing isolated attosecond pulses has been met by two
successful approaches so far. The first, and most direct, of these is to generate
HHG from very short pulses comprising only a few optical cycles. In such a short
pulse, the variation in field strength from one half cycle to the next is substantial and
only a single cycle generates the highest energy harmonics which will be emitted
only once in the laser pulse. These harmonic orders, near the cut-off, are isolated
by spectral filtering of lower photon energies which forms an isolated pulse. Our
discussion below will concentrate upon this approach. The other approach, suitable
for somewhat longer pulses, applies an idea first proposed some years ago [25]
where the laser polarisation is controlled so that it varies from circular through
linear and back to circular through the pulse, with pure linear polarisation only
achieved for a period less than a single cycle. This technique relies upon the fact that
the efficiency of high-harmonic generation decreases rapidly with increasing laser
field ellipticity due to a suppression of electron returns in the recollision model.
Due to this strong polarisation dependence of the HHG efficiency this “polarisation
gating” method leads to isolated attosecond pulses. By using two counter-rotating
circularly polarised pulses, with an appropriate short mutual time delay there is a
small time window (or gate) when the combined field becomes linear. It can be
contrived for this gate to be smaller than a half-optical cycle, then there will only be
one burst of XUV emission during the gate resulting in the production of an isolated
attosecond XUV pulse. Pulses as short as 130 attosecond have been reported by this
method [26].
The approach that has resulted in the shortest isolated pulses so far reported is,
however, the direct approach requiring a laser pulse comprising just a few optical
cycles. This is described by Goulielmakis et al. [27]. It requires several key technical
features to be fully controlled; (a) the pulse must be very short with a FWHM of
fewer than 2 optical cycles, (b) the CEP must be tightly locked so that within this few
cycle pulse only a single dominant recollision accounts for the cut-off harmonics,
(c) the HHG spectrum must be efficiently spectrally filtered so that the cut-off can
be isolated. In general (a) requires the use of either focussing the laser through a
gas filled hollow core fibre to ensure self-phase modulation (SPM) causes sufficient
broadening to support a short pulse [28] or a similar broadening mechanism arising
through self-guided filamentation in a gas filled cell. Typically a factor of 4 increase
in spectral width can be achieved with around 50 % transmission. The next step is to
compensate all orders of phase to produce the very short, high power, pulse which
is done through using high order phase compensating stacks of chirped mirrors
and additional thin glass matched wedges for fine adjustment. The technology of
CEP stabilisation of chirp pulsed amplified titanium sapphire lasers [29] is now
well established and such lasers are commercially available, although it is often
challenging to achieve the degree and duration of phase stability required for
the purposes of attosecond pulse production. A range of transmission filters and
reflective dielectric mirror coatings are now available for selection of a number
of XUV spectral ranges, for example, Al (bandpass 20–75 eV), Zr (bandpass
70–120 eV), MoSi (reflective 85–95 eV). Figure 3.5 presents the results of a
numerical simulation under the conditions of the experiment by Goulielmakis et al.
[27, 30], leading to the required XUV emission for the creation of an isolated
attosecond pulse.
Future developments are promising to extend the photon energy range to both
deeper into the X-ray [31] and to lower VUV photon energies [32] which, providing
the appropriate VUV – soft X-ray optics are available, will allow the techniques
of attosecond measurement to be extended to a wider range of systems. Increased
photon flux is also being achieved, for instance by limiting the HHG generation to
a single optical cycle so reducing the effect of ionisation saturation.
3.3.3 Streaking Measurements
An essential step in the development of the current attosecond technology is the

capability to characterise an attosecond XUV pulse. Not only does this confirm that
isolated attosecond pulses are really being generated, but also their characterisation
is an important part of any optimisation of these sources (e.g. of pulse duration,
contrast, pulse energy etc.). The formation of a continuous spectrum in the HHG cut-
off region is of course indicative of an isolated attosecond pulse but because this only
provides the spectral intensity information and not the spectral phase it is impossible
to fully retrieve the pulse. The method that is used for full pulse characterisation is
to perform photoionisation by the XUV pulse in the presence of the IR generating
Fig. 3.5 Numerical simulation illustrating the creation of isolated attosecond pulses from a sub-
1.5 cycle, linearly polarised, 720 nm driving laser pulse in Neon atoms. The top panel shows the
maximum energy electron trajectories generated near the peaks of the laser field EL (t). The number
next to those trajectories denotes their ionisation probability. The bottom panel shows the resulting
XUV emission spectra from the set of trajectories emitted close to the laser field peaks, with the
line formatting corresponding to the trajectories displayed in the top panel. The spectrum resulting
from the solid line trajectory in the top panel is not visible due to its low ionisation probability and
hence intensity. The dash-dotted line in the bottom panel shows the bandpass filter, which filters
out the harmonic emission for the isolated XUV pulse (Reproduced and adapted with permission
from Ref. [30])
field which is locked to the XUV pulse in phase, but with the possibility to vary
the phase of the arrival of the XUV pulse. The measured photoelectron energies
correspond to a mapping of the XUV pulse spectrum. The “streaking effect” of the
IR field on the photoelectrons shifts the momentum by an amount that depends upon
its electric field amplitude and the phase at which ionisation occurred and therefore
provides the spectral phase information of the XUV pulse.
The momentum of the electron observed in the laser polarisation direction at
some time t following ionisation by the XUV pulse at time t0 is given by the
expression [33]:
eE0
p.t; t0 / D O
Œcos.!t0 /Oy cos.!t/Oy C ı u (3.13)
!
Where the momentum imparted by the undressed XUV pulse is given by:
q
ıD .Exuv Ip /=2Up (3.14)
where e is the electron charge, E0 and ! the IR field amplitude and carrier frequency,
respectively, Exuv and Ip being the XUV photon energy and atomic ionisation
potential, respectively, Up D e 2 E0 2 =4m! 2 the quiver energy of the released
electron of mass m in the IR pulse, yO and uO are the IR field polarisation and initial
direction of the outgoing electron, respectively. The final electron momentum at the
end of the pulse, i.e. that measured at the detector, is given by:
eE0
pf .t0 / D O
Œcos.!t0 /Oy C ı u (3.15)
!
Note the final momentum depends on a term E0 ı which for modest IR field
strength and moderate initial photo-electron energy (a few 10’s of eV) leads to a
significant momentum shift that is then modulated by the oscillating term depending
on the field. The momentum that is observed therefore encodes the time t0 of
ionisation by the XUV.
Streaking measurements can be analysed by composing a spectrogram from a
series of streaked electron spectra recorded for different delays (i.e. different t0 )
between the laser and the attosecond pulse. Such a data set contains both temporal
and spectral information about the physical process under study. Measurement
of the “streaked” photoelectron spectrum thus provides information on when the
XUV pulse arrives within the IR pulse and (from the spread in final measured
photoelectron energies) a mapping of the XUV pulse. In the limit of a single XUV
pulse shorter than the optical cycle time a delay scan of the XUV pulse through the
(attenuated) IR few-cycle pulse provides sufficient information to retrieve both the
IR field history and the XUV pulse duration (from algorithms such as FROG-CRAB
[34]). (See Chap. 1 by Wyatt et al. for a discussion of ultrashort pulse measuring
techniques).
3.4 HHG Spectroscopy
A related application of HHG has recently been exploited to carry out a new class
of attosecond measurements. The approach is to characterise very carefully the
harmonic radiation emitted from a molecule. It has been found that the spectrum,
phase and polarisation of this radiation can encode information of molecular
structure and internal dynamics. The recombination step of HHG depends upon
the matrix element between the continuum state ((k) with returning electron
momentum k) and the bound state for a particular molecular ion intermediate state:
D E
Aj D '0 jkj.k/'jC (3.16)
The amplitude for harmonic emission from an individual atom/molecule is deter-

mined by the amplitudes for ionisation, the phase accumulated during propagation
in the field and the recombination amplitude [19]:
X
D.!/ D Aj recombination Œt.!/Aj i propagation Œt.!/; t 0 .!/Ai ionization Œt 0 .!/ (3.17)
ij
where, reading from right to left, are the amplitudes for ionisation at t’, propagation
between t’ and t, and recombination at t; the summation is over different ‘quantum
trajectories’ that result in the same return energy. Crucially, different phase-
matching properties of the radiation associated with different trajectories allow
one to effectively select a single term from the sum in the measurements. This
simplification makes the analysis of the connection between the harmonic spectrum
and the underlying physics practical and feasible.
The possibility to extract molecular orbitals from this approach has been widely
discussed and the reader is recommended to read several original research papers
and reviews on this topic (for example Ref. [35]), although there is not space here
to review this further in depth.
An intriguing side of HHG spectroscopy is the ability to probe the dynamics that
the parent molecular ion undergoes while the “probe” electron is away. Note that
these dynamics are only launched upon ionisation and curtailed by recombination.
For time resolution it is the inherent chirp of the harmonic emission that is the
crucial aspect. Clearly, D(t) encodes attosecond dynamics taking place between
ionisation and recombination and the presence of the strong laser field allows one
to dramatically simplify the formal expression, making such recovery possible.
High harmonic spectroscopy can probe such dynamics with time-resolution
better than 100 asec. First steps in using HHG for attosecond probing have been
made in [36]. In a molecule, ionisation simultaneously launches an electronic
wavepacket into the continuum and a nuclear wavepacket onto the groundstate
electronic potential energy surface of the molecular ion. As the nuclei move between
ionisation and return, recombination to the initial state requires an overlap between
the evolving nuclear wavepacket (R, t(¨), t0 (¨)] in the ion and the original
nuclear wavefunction 0 (R) in the neutral (R labels the nuclear coordinates, e.g.
the internuclear distance for a diatomic). With the corresponding modification of
the recombination amplitude, the harmonic emission becomes [20]:
Z

D.!/ D 0 .R/ R; t.!/; t 0 .!/ D0 .R; !/dR (3.18)
where D0 (R,!) characterizes emission in the absence of nuclear motion.

Thus, the HHG signal becomes relatively weaker, the further the nuclei have
moved away from their original positions. To gain quantitative information, it is then
necessary to measure the overlap between 0 (R) and (R, t(¨), t0 (¨)] at a range of
ionisation-recollision time delays . In the technique PACER (Probing Attosecond
dynamics using Chirp Encoded Recollisions), this is achieved within a single laser
shot by exploiting the chirped nature of the returning electron wavepacket i.e. the
strong dependence of its energy on time, Fig. 3.4.
If ‘short’ trajectories are isolated, leaving only a single set of terms in the sum in
Eq. (3.17), then each harmonic frequency is emitted at a different time according
Fig. 3.6 Illustration of the impact of nuclear dynamics on the observed high harmonic emission as
described in the text. Three electron trajectories are displayed at different ionisation and recollision
times. The recollision time and hence time delay t is encoded in the emitted harmonic frequency,
whereas the corresponding intensity depends on the internuclear stretching during that time. Here,
a lower intensity is suggested by a thinner linewidth of the harmonic emission (Reproduced and
adapted with permission from Ref. [36])
to a known relationship (see Eq. (3.12)) The emission of each harmonic order
therefore probes the molecular ion at a different time delay. The strength of the
harmonic signal at different frequencies therefore has encoded within it the position
of the molecular nuclei at a range of ionisation-recollision time delays. In this
way a remarkable temporal resolution is achieved, since the emission of successive
harmonic orders is typically separated in time by less than 100 as.
The strength of the harmonic signal at different frequencies also depends on
ionisation and propagation steps contributing to D0 (R, t). In the first PACER
measurement, the effect of the nuclear motion was isolated from any effects of the
electronic parts of Eq. (3.18) by comparing the harmonic emission in two isotopes
of the same species. This procedure circumvents the need to consider details of the
electronic contributions such as the recombination and ionisation amplitudes for a
given R – these are similar for the two isotopes. The same applies to the impact of the
macroscopic propagation of the emitted light. The PACER technique is described
in detail in [36, 37]. In essence it is simply necessary to compare high harmonic
generation in protonated and deuterated samples of a molecule at the same laser
intensity and gas density. As an example, the harmonic signals in both H2 and D2
as well as CH4 and CD4 were recorded, and any difference in the spectra could be
attributed largely to the different nuclear dynamics in the two species. This principle
is illustrated in Fig. 3.6 for H2 and D2 .
More recently the concept of PACER has begun to be applied to studying
the electronic dynamics that are initiated when the HHG ionisation event simul-
taneously excites a superposition of two ionic electronic states [38, 39]. In the
case of CO2 , interference between these channels has been obseved in addition
to the structural interference. It is anticipated that this method can be extended
to investigate a wide range of molecular hole dynamics. To achieve this it is
necessary to decouple the structural dependence of the HHG signal from the
temporal dependence. There are several possible strategies to do this, the isotope
comparison of the original PACER measurement being an example. The HHG
spectrum at a given photon energy is of course emitted at different times if the laser
wavelength and/or intensity is changed [38, 39] opening the way to make these
separations without a reference molecule or atom.
3.5 Other Routes to Attosecond Science
HHG remains very promising and is currently the only demonstrated path for
making attosecond measurements. There are, nevertheless, several potential short-
comings in HHG based routes coming principally from the limited photon energy
range of the sources (confined to the VUV (>20 eV) to very soft X-ray range
<100 eV) and so presently not capable of accessing inner shell processes. Also the
low pulse energy of the sources demonstrated so far (nJ) is still not sufficient for
many potential applications. We now turn to other routes for generating attosecond
pulses that may overcome these limits within the next few years.
3.5.1 Raman Based Sub-fs Sources
As is well known in non-linear optics, for example in acousto-optical and electro-

optical modulators, a medium with a time modulated refractive index will modulate
the frequency of a light field passing through it. The effect is to add sidebands to
the carrier frequency ! at the modulation frequency ˝. Strong modulation will
result in side-bands appearing at a finite number of integer multiples of ˝, and
these will be phase locked to the carrier frequency. The modulation frequency of
these conventional devices is typically <10 GHz so they are not useful as ultrafast
optical devices. Oscillations at much higher frequencies (up to 100 THz) are found
in the vibrations and rotations of molecules. Faster modulations of refractive index
result from vibrational modulation, the fastest of all being the 8 fs period of the H2
molecule that will cause a 125 THz refractive index modulation. A strong refractive
index modulation will produce multiple side-bands and thus create the >450 THz
spectrum needed to support sub-fs pulses.
Since the late 1990s a family of schemes for sub-fs pulse generation based upon
Stimulated Raman Scattering (SRS) has been under development which exploits
this fast varying refractive index to modulate incident laser fields. In these schemes
the efficiency of SRS is increased by first preparing the scattering medium so
that a high proportion of the component molecules oscillate in phase and so act
as an efficient high frequency modulator. High order Raman sidebands of a field

propagating through this medium are thereby generated with high efficiency, leading
to energetic pulses with sufficient bandwidth to support sub-femtosecond duration
pulses. Pioneering work by Harris and Sokolov showed how adiabatic preparation of
the molecular medium using a pair of fields detuned slightly from Raman resonance
to ensure the adiabatic condition can lead to a maximal coherence (vibrational
amplitude) which gives rise to very strong modulation of any laser field propagating
through the medium resulting in near 100 % transfer of the optical field energy into
a spectrum of sidebands that spans an octave or more. In the first experiments on
adiabatic preparation of cooled D2 gas [40, 41] and solid H2 [42] the modulation of
the visible/NIR input fields with high efficiency and generating a large bandwidth
(sufficient to support a 1 fs pulse) was shown. The fields required for adiabatic
preparation of a vibrational or rotational coherence must be single mode (transform
limited) and are usually the nanosecond range, the result is that the short pulses are
produced in a train, repeated at the vibrational/rotational period, with the energy
converted into the fields divided between 106 repetitions in the train. It has been
shown that short pulses (130 fs) can be modulated in a medium first adiabatically
prepared with nanosecond fields [43]. The generation of isolated short pulses that
are reproducible from shot to shot requires still shorter pulses to be modulated
and phase-locking of the field to be modulated with the coherence generated in
the medium. This requires some significant steps in optical engineering with the
technique of coherence amplification of a weak seed using multi-mode nanosecond
pulses as one promising route [44].
Progress has also been reported in excitation of strong vibrational coherence in
the impulsive regime, i.e. using a pulse shorter than the molecular vibration period
and so containing frequency components sufficient to drive the Raman transition
[45]. To prepare a strong coherence requires an intense drive field that is subject
to additional nonlinearities, e.g. SPM, and so the strategy identified to develop this
impulsive Raman method is again to use a second “probe” pulse (also shorter than
the modulation period) that is efficiently modulated by the medium following the
preparation of the medium coherence by the first pulse. Phase locking is achieved
by controlling the delay between the pulses.
The attraction of the Raman based methods is that although they are unlikely
to compete with HHG in pulse duration, they are well suited to generated 1 fs
pulses with a UV carrier (e.g. 5–10 eV) and pulse energies of 1 J or more. The
UV frequency is particularly relevant to excitation of ultrafast chemical dynamics
as many biomolecules have strong electronic absorption in the UV range. The reader
is advised to consult a recent review for more detail on this topic [46].
3.5.2 Relativistic HHG
Relativistic High Harmonic Generation (RHHG) is based on the relativistic Doppler

upshift of optical laser light from a surface oscillating with a maximum velocity
close to the vacuum speed of light c. This mechanism has been termed the relativistic
oscillating mirror and along with the coherent wakefield emission mechanism that
is observed at somewhat lower laser intensities gives rise to a very broad spectrum
of efficient harmonics (for details see [47]). Such surface oscillations are driven
when a high intensity laser is reflected from either a solid or liquid surface. Here,
the electric field direction is into the surface. The maximum upshift that can be
observed scales with laser intensity and allows the up-conversion of NIR lasers to
100 eV for 5 1019 Wcm2 increasing to multiple keV for intensities exceeding
1020 Wcm2 . At high intensities the RHHG conversion efficiency is independent of
laser intensity (i.e. it becomes a linear process) with a conversion efficiency into the
nth harmonic scaling as n2.6 [48].
RHHG intrinsically produces attosecond pulses (or trains) with one pulse emitted
per laser cycle and it is currently believed to be the brightest known source of
attosecond pulses [49] (see Table 3.1). Scaling to higher drive energies and higher
photon fluxes is currently an area of active research but there is already a clear
advantage over gas target HHG in terms of efficiency and photon flux. Currently
the laser sources used to drive RHHG have been relatively low repetition rate
(10 Hz or less) and this makes the application of the attosecond pulses so far
produced challenging. Future sources based upon RHHG will require high intensity
(>>1019 Wcm2 ) laser source to drive attosecond pulse train sources, with a need
for kHz and higher repetition rates.
Moreover to drive an isolated attosecond source at full efficiency requires a high
intensity (>1019 Wcm2 ) few cycle (sub 10 fs) laser source or a demonstration of
polarisation gating (as in gas HHG) is needed. A high pulse contrast (>1011) is
essential as the surface must not be disrupted prior to exposure to the high intensity
laser. This is required either from the laser itself or as so far shown by use of plasma
mirrors. Work on optical parametric amplification (OPCPA) lasers may be able to
remove the need for plasma mirrors [50] by delivering high contrast, few-cycle drive
pulses of the required intensity. To match the future high repetition rate lasers high
repetition rate target sources must be developed e.g. by use of liquid jets or tape
targets (for details see [51] and references therein).
3.5.3 FELs and Attosecond Pulse Production
In the last few years the first true X-ray lasers have become available for scientific
applications. These free-electron sources are based upon high charge, low emittance,
bunches of electrons accelerated to relativistic energies which emit copious amounts
of coherent radiation if they pass through a sufficiently long magnetic undulator
structure. An undulator consists of a periodic lattice of permanent magnets that
creates a strong alternating transverse magnetic field. This forces the electron
bunch to oscillate and emit electromagnetic radiation at a fundamental radiation
wavelength which co-propagates with the electrons. The fundamental wavelength
66
Table 3.1 Comparison of ultra-short XUV pulse sources and related techniques. Material collated for NLS project (www.newlightsource.org)
Accelerator based
HHG based sources Free Electron Lasers
HHG RHHG Slicing Current Energy Chirp Single Spike Mode-Locking
Pulse Length <100 as <100 as 250 as <200 as 3 fs–300 as 400 as–23 as pulse train
Photon energy 100 eV–1 keV 1–10 keV 12 keV 12 keV 300 eV–12 keV 100 eV–8.6 keV
Photons per 106 –104 1011 (1 keV) 109 1010 1010 –108 1010 –108
pulse
Peak Power 200 W (1 keV) 1 GW 10 GW 100 GW 250 MW–5 GW 1–5 GW
Contrast Good Good Poor Good Excellent Good
Rep-rate Laser <10 kHz Laser 10 Hz Laser seed Laser seed LINAC Laser seed
Synchronisation Yes Yes Yes Yes No Yes
(with laser)
J.P. Marangos and M. Oppermann

is given by 1 D u 1 C aN u2 =2ƒ2 ; where u is the period of the undulator, ƒ
is the energy of the electrons in units of their rest-mass and aN u2 is the undulator
parameter, proportional to the root means square (RMS) magnetic field strength
between its poles. The continued oscillation of the electrons in the presence of this
radiation results in an exponential instability that forces the electrons to bunch at the
fundamental radiation wavelength and to emit coherently at that wavelength – the
so called Self-Amplified Spontaneous Emission process (SASE).
At the time of writing, three such facilities are operational: XUV machines
at DESY, Hamburg (FLASH) and SPring-8 Japan and the world’s first X-ray
FEL the LCLS (Linac Coherent Light Source) at SLAC, Stanford, USA. They
are based upon SASE [52] that generates radiation pulses of limited temporal
coherence consisting of a series of phase uncorrelated spikes. Pulse durations as
short as a few femtoseconds are present in a single emission “spike” but typically
contain many such spikes within a pulse of 30–200 fs duration. The radiation
is thus multimode, and because SASE is triggered by spontaneous processes, is
inherently stochastic with a significant temporal jitter (typically larger than the pulse
duration). Nevertheless the lasing bandwidth in a FEL is sufficient to support sub
100 attosecond pulses and so ways to control the emission are now being sought to
permit the intrinsic attosecond capability to be harnessed.
One of the simplest methods to reduce the poor temporal coherence of the
SASE output is to seed the FEL amplifier with a resonant seed source of power
significantly greater than that of the intrinsic spontaneous noise from which SASE
starts. Successful seeding of the Japanese VUV FEL by a HHG source was
demonstrated at 160 nm [53] and it is anticipated that HHG seeding up to 100 eV
photon energies will be possible (10 nm). Where seed sources have insufficient
power to dominate initial noise towards shorter wavelengths, currently .10 nm
for HHG sources, it is possible to use an Harmonic Optical Klystron [54] (HOK) or
High Gain Harmonic Generation [55] (HGHG) configuration of the high-gain FEL
to reach shorter wavelengths while retaining good temporal coherence.
Several techniques have been identified that may shorten the pulse durations of
<20 fs possible from seeding yet further into the attosecond regime. A conceptually
simple method has been suggested [56] that ‘spoils’ all but a short region of
the electron bunch. Only this region subsequently lases in the FEL which could
potentially operate under either SASE or seeded mode to generate a short radiation
pulse of duration <1 fs.
A wide range of proposals have been made to pre-modulate the electron bunch
energy with a carrier envelope phase-locked high power laser before the bunch
enters the radiator undulator. The resonant FEL wavelength is correlated to this
energy modulation, and it may be possible to selectively filter [57] or amplify [58] a
restricted wavelength band to generate short pulses with widths of a fraction of the
modulation period. Another approach, called E-SASE [59], uses laser modulation
of the electron bunch energy at an intermediate acceleration stage. Regions of
enhanced current are created that subsequently generate short pulses in a final
radiator undulator. The above techniques might generate single attosecond pulses
(there may be smaller satellite pulses about the main pulse) of typical duration
100–300 as at a target wavelength of 1 1 Å.
Two different methods from those discussed above are viable candidates for short
pulse X-ray generation. The first employs a relatively low charge, short electron
bunch of length of a few cooperation lengths [60]. Such electron pulses emit only
one or two spikes in the SASE mode (see above). This mode has been successfully
employed at LCLS [61] where the short pulse has been utilised, e.g. for studies
of double core hole formation as the pulse is shorter than the characteristic Auger
decay times in most atoms [62]. The second method has not been demonstrated
experimentally yet. It uses techniques familiar from mode-locking in conventional
cavity lasers to generate an attosecond pulse train [63]. A cavity-like longitudinal
mode structure can be synthesised in a FEL amplifier by applying a series of
spatiotemporal shifts between the radiation and copropagating electron bunch.
These shifts are achieved by repeatedly delaying the electron bunch using magnetic
chicanes between undulator modules. By introducing an interaction modulation
at the synthesized mode spacing the modes may become phase locked to give a
temporal train of short, equally spaced, high-power pulses. At 12 nm a train of
400 as pulses, evenly spaced at 2.5 fs, of peak power 1 GW are predicted for
typical FEL parameters for this wavelength range. For operation at 1.5 Å, again
using typical parameters, a pulse train consists of 23 as pulses separated by 150 as
with peak powers up to 6 GW are predicted.
3.6 Future Prospects for Attosecond Measurement
The methods for attosecond measurement that arise from attosecond generation in
strong laser fields have been summarised in this chapter. The possible alternatives
to gas phase HHG have been discussed, the majority of these also relying on strong
field interactions e.g. RHHG and most of the viable FEL based methods. Despite
the potential of the alternatives, gas phase HHG remains the dominant technique
for attosecond measurement since it is the only route that has demonstrated actual
attosecond measurement applications. This is partly because HHG is now a rather
well understood process both theoretically and technically. Moreover, although
state-of-the-art few cycle lasers are required, these are based upon commercially
available and relatively small scale laser systems that offer access to “attosecond
science” to any motivated university laboratory (i.e. do not require the resources
of large national laboratories and research institutes). Moreover a critical fact of
many attosecond experiments where the measurement process dictates low count
rates per laser shot (e.g. the need to avoid space charge effects in photoelectron
studies or to make correlated or coincidence measurements) is access to high
repetition rates (kHz or greater). RHHG and FEL based methods are therefore
still requiring technical breakthroughs in lasers technology and superconducting
accelerator technology before these sources can be as versatile and high rep-rate
despite their potential advantages.
Moreover there are prospects for considerable enhancements to HHG technology

with recent progress towards accessing the water window (>285 eV) at high
efficiency [31], reports of production of much higher attosecond pulse energy using
very short pulses and ionisation gating methods [64]. It is therefore likely that at
least for the next 5 years or perhaps considerably longer HHG based attosecond
measurement will continue to dominate the field of attoscience.
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Chapter 4
Advances in Solid-State Ultrafast Laser
Oscillators
Christopher G. Leburn and Derryck T. Reid
4.1 Introduction
Ultrafast laser oscillators remain an area of constant technological development and

a key driver of new commercial and scientific applications of ultrashort optical
pulses. New, high-quality broadband gain materials with absorption profiles com-
patible with direct diode-pumping are increasingly offering a practical alternative to
Ti:sapphire. The greater reliability and availability of semiconductor quantum-well
and quantum-dot saturable absorbers have also driven research into ultrafast lasers
capable of operating at new wavelengths within broader regimes of repetition-rate
and output power.
This chapter is organised into three remaining sections. The principles of
generating ultrashort laser pulses are introduced in Sect. 4.2, which deals with the
fundamentals of modelocking and dispersion control. Section 4.3 concentrates on
the specific technology of semiconductor saturable absorbers and their implemen-
tation in modelocked lasers. Finally, Sect. 4.4 presents a selection of representative
modern ultrafast lasers, which serve as examples of how the techniques discussed
in the preceding sections may be implemented in real systems.
C.G. Leburn () • D.T. Reid

Scottish Universities Physics Alliance (SUPA), Institute of Photonics and Quantum
Sciences, Heriot-Watt University, Edinburgh, Scotland EH14 4AS, UK
e-mail: c.g.leburn@hw.ac.uk; d.t.reid@hw.ac.uk

74 C.G. Leburn and D.T. Reid
4.2 Fundamentals of Ultrashort Pulse Generation
4.2.1 Passive Modelocking
Nearly all modern ultrashort-pulse lasers rely on the process known as passive
modelocking to generate and sustain femtosecond pulses. In an inhomogeneously-
broadened laser, different frequencies in the emission bandwidth experience gain
simultaneously when they correspond to the frequencies of the longitudinal modes
of the resonator. The frequency separation between adjacent longitudinal resonator
modes can be expressed as:
! D 2 c= l (4.1)
where l is the optical roundtrip length of the resonator and c is the speed of light.
When these modes are coupled by a fixed phase relationship – the modelocked
condition – a periodic sequence of ultrashort optical pulses is generated. If the nth
longitudinal mode has an amplitude En , then the total optical field can be denoted as:
X
E.t/ D En exp i Œ.!0 C n !/t C n ' (4.2)
n
Figure 4.1 illustrates how the coherent superposition of such resonator modes
generates a wavepacket whose extent in the time-domain is inversely propor-
tional to its frequency-domain bandwidth. Practical femtosecond lasers require
frequency bandwidths in excess of 1 THz, typically corresponding to the coherent
superposition of around 100,000 resonator modes. This requirement places a
demanding constraint on which laser gain materials can be used for femtosecond-
pulse generation, ruling out gas lasers and focusing attention on media with
broadband fluorescence spectra, such as dyes, vibronic crystals and doped amor-
phous materials.
From the discussion above, it is clear that practical modelocking requires both
! and ' to be constants; ! is a constant when the resonator length is fixed,
however ' must be stabilized by using a modelocking mechanism – any effect
which introduces a periodic modulation of either the amplitude or phase of the field
in the resonator. It can be shown (see Box 4.1) that an amplitude or phase modulation
of a monochromatic field of frequency !0 leads to the creation of coherent sidebands
at frequencies of !0 ˙ , where is the modulation frequency. If we consider
a single longitudinal resonator mode oscillating with frequency !0 , then when
exactly matches the frequency separation between adjacent resonator modes,
!, the generated sidebands experience low-loss propagation in the laser cavity
and can themselves be amplified in the laser gain medium. Furthermore, because
these sidebands are generated coherently, they have a constant phase relationship
to the original mode and so can combine coherently to form a modelocked pulse.
This process repeats over many cavity roundtrips, with the periodic modulation
4 Advances in Solid-State Ultrafast Laser Oscillators 75
Fig. 4.1 (a) Time-domain and (b) frequency-domain representations of a modelocked pulse
synthesised by the coherent superposition of (top to bottom) 3, 5, 7 and 9 resonator modes
creating sidebands on each of the resonant cavity modes, broadening the frequency
bandwidth of the oscillating field and shortening the pulse duration, until a steady-
state condition is reached which results from the finite bandwidth of the gain
medium, or the dispersion characteristics of the cavity.
The requirement for the amplitude or phase modulation frequency, , to exactly
match the frequency separation between adjacent resonator modes, !, means that
the laser field must be modulated with a period equal to roundtrip cavity time, l/c.
In a passively modelocked laser, the periodic modulation of the pulse amplitude
is obtained by using a saturable absorber, an optical element whose loss decreases
as the incident light intensity increases. Incorporating a saturable absorber inside a
laser resonator allows a resonant pulse to modulate its own amplitude – a process
known as self-amplitude modulation (SAM) – and this effect automatically satisfies
the modelocking requirement that D !.
Many different saturable absorption effects and devices have been successfully
used to obtain modelocking at pulse durations below 1 ps, and include: organic
dyes [1]; semiconductor saturable absorber mirrors (SESAMs) [2]; Kerr-effect self-
focusing [3]; Kerr-effect nonlinear polarisation rotation [4]; Kerr-effect self-phase
modulation [5–9]; and carbon nanotubes [10].
The dynamics of the modelocking process depend critically on the speed of the
SAM effect and its recovery time after the loss of the absorber has been saturated
by an intense pulse. Two characteristic timescales are particularly relevant, namely
the pulse roundtrip time of the laser cavity (typically around 10 ns) and the pulse
duration (typically a few hundred fs or less). Slow saturable absorbers (for example,
organic dyes) exhibit a typical recovery time of many ns which is comparable
with the pulse roundtrip time of the laser. In contrast, fast saturable absorbers (for
example, effects which exploit a Kerr nonlinearity) have a recovery time which is
either instantaneous or comparable to the pulse duration. Many practical saturable
absorbers, such as SESAMs and carbon nanotubes, possess recovery times of
the order of several ps, several times the pulse duration, but much shorter than the
pulse roundtrip time. These saturable absorbers can still be used for femtosecond
pulse generation when the dispersion of the laser resonator is properly controlled.
Box 4.1
The field of a laser cavity mode n can be represented as:
En exp.i !n t/
Modulating the amplitude of the field with a modulation depth m and at a

frequency leads to the modified field:
E D En exp.i !n t/ .1 C m cos t/
By using the identity cos t D Œexp.i t/ C exp.i t/=2, this field may
be rewritten as:
m m
E D En exp.i !n t/ C En exp.i.!n C /t/ C En exp.i.!n /t/
2 2
Phase modulation may be analysed in a similar way, and the phase-
modulated field may be written as:
E D En exp.i !n t/ exp.im sin t/
For small modulation depths (m << 1), the Taylor-series approximation

exp.im sin t/ 1 C i m sin t allows the field to be expressed as:
m m
E D En exp.i !n t/ C En exp.i.!n C /t/ En exp.i.!n /t/
2 2
Consequently, both amplitude and phase modulation lead to the generation
of phase-coherent sidebands positioned at a frequency offset of ˙ from the
original carrier.
4.2.2 Dynamics of Ultrafast Pulse Generation
4.2.2.1 Analytic Description of an Ultrafast Laser Pulse
A pulse with a centre frequency of !0 can be represented by a complex envelope

function A(t) so that the real electric field can be written as:
E.t/ / Re fA.t/ exp.i !0 tg (4.3)
In this notation, A(t) is expressed in units normalized so that jA.t/j2 represents the
instantaneous optical power. It is often useful to express the pulse in the optical
frequency domain, corresponding to a Fourier transform of the complex temporal
amplitude:
Z1
1
A.!/ D p A.t/ exp.i !t/dt (4.4)
2
1
The quantity jA.!/j2 is the power spectrum of the pulse, which is readily measured
in the laboratory by an optical spectrum analyser.
The duration-bandwidth product describes the relationship between the width of
a pulse in time and its spectral bandwidth. Table 4.1 lists the minimum duration-
bandwidth products resulting from pulses with particular temporal profiles. The
duration, p , and the spectral bandwidth, p , are measured at the full-width at
half-maximum (FWHM) points. It can be seen from Table 4.1 that the duration-
bandwidth product increases as the energy content in the wings of the pulse
decreases. This effect arises from the FWHM-definition of the pulse duration.
Chirping of the pulse due to dispersion increases the duration-bandwidth product
to above the minimum values listed in Table 4.1.
With the exception of propagation in a vacuum, a pulse always experiences
dispersive effects as it travels through optical materials and systems. These effects
can be treated generally as an additional frequency-dependent phase, '(!), written
onto the pulse:
A.!/0 D A.!/ exp.i'.!// (4.5)
The resulting pulse in time is described by the inverse Fourier transform:
Z1
0 1
A.t/ D p A.!/0 exp.i !t/d! (4.6)
2
1
Table 4.1 Common field envelope profiles of ultrashort pulses and their minimum duration-
bandwidth products
Pulse A.t / vp p
Hyperbolic secant
sech.1:763t = p / 0.315
Gaussian
exp.2 ln 2t 2 = p2 / 0.441
Parabolic s
2t 2 0.728
1
p2
Rectangle
p 0.886
1; jt j
2
p
0; jt j >
2
The local variation of the spectral phase due to an optical medium can be represented
by the Taylor expansion:
ˇ ˇ
@' ˇˇ 1 2 ˇ
2@ 'ˇ
'.!/ D '.!0 / C .! !0 / ˇ C .! !0 /
@! !0 2 @! 2 ˇ!0
3 ˇ
ˇ n ˇ
ˇ
1 3@ 'ˇ 1 n@ 'ˇ
C .! !0 / C C .! !0 / (4.7)
6 @! 3 ˇ!0 nŠ @! n ˇ!0
The first term in Eq. (4.7) is the change in carrier phase after passing through the
medium and has no effect on the shape of the pulse. In the second term we can
observe a linear phase ramp in frequency which corresponds, through the Fourier
Fig. 4.2 (a) Unchirped pulse; (b) chirped pulse showing the variation of instantaneous frequency
shift theorem, to a delay of the pulse in time. A quantity known as the group delay
has units of fs and corresponds to the time spent by the pulse inside the medium is
given by:
ˇ
@' ˇˇ
g D (4.8)
@! ˇ!0
For a medium of physical length z, the group delay can be related directly to the
group velocity, vg , of the pulse in the medium by using the definition:
ˇ
@k ˇˇ
vg D 1= (4.9)
@! ˇ!0
Since the phase change due to propagation is simply kz, we obtain:

z
g D (4.10)
vg
The quadratic and higher-order terms describe the variation of the group delay with
frequency (or wavelength), and have a direct influence on the shape of the pulse
in time. The .! !0 /2 term is responsible for adding linear chirp which refers to
a time-varying uniform increase or decrease in the instantaneous optical frequency
across the pulse. Figure 4.2 compares chirped and unchirped pulses, showing the
variation in instantaneous frequency of a chirped pulse. The pulse shown has
positive linear chirp, meaning the instantaneous frequency increases linearly with
time across the pulse.
Formally, group delay dispersion (GDD) has units of fs2 and is described by the
quantity:
ˇ
@g @2 ' ˇˇ
GDD D D (4.11)
@! @! 2 ˇ!0
Table 4.2 Dispersion formulae for light propagating a distance z in a dielectric medium
Expressed in phase/ Expressed in index
Quantity wavevector and frequency and wavelength
! c
Phase velocity vp D
k n
1
@k dn
Group velocity vg D 1= c n
@! d

@' z dn
First-order dispersion (group delay) g D n
@! c d
@g @2 ' 3 z d 2 n
Second-order dispersion (GDD) D
@! @! 2 2 c 2 d 2
2
@3 ' 4 z d n d 3n
Third-order dispersion (TOD) 3 C
@! 3 4 2 c 3 d 2 d 3
Cubic spectral phase variations associated with the .! !0 /3 term lead to

sharpening of one edge of the pulse and broadening of the other, ultimately resulting
in pulse break-up. The quantity known as third-order dispersion (TOD) has units of
fs3 and is given by:
ˇ
@3 ' ˇˇ
TOD D (4.12)
@! 3 ˇ!0
Strategies for generating the shortest pulses from ultrafast lasers rely on control-
ling the net intracavity dispersion so that the quadratic and higher-order spectral
phase terms associated with one cavity roundtrip are negligible across the entire
spectral bandwidth of the pulse. Contributions to the cavity dispersion may originate
from a number of sources:
Material dispersion is associated with the wavelength-dependent refractive index
of a dielectric medium. In solid-state lasers this is limited mainly to the gain
medium, but in fibre lasers may be distributed throughout the entire cavity.
For propagation in bulk dielectric media, the material dispersion is commonly
represented in terms of the wavelength-dependent refractive index, n(). It is
therefore often convenient to express the quantities in Eqs. (4.9), (4.10), (4.11),
and (4.12) in a form that can allow them to be evaluated directly from n(), and
Table 4.2 lists the formulae used for this conversion.
Geometrical dispersion arises from the wavelength-dependent path lengths that
can be observed in optical systems exhibiting angular dispersion, such as prism
or diffraction-grating sequences. The GDD and TOD of such systems may be
highly controllable by careful choice of the materials and geometrical layout of the
elements.
Table 4.3 lists the second and third-order dispersion formula for double-passed
prism [11–13] and grating pairs [14, 15], the two most common optical systems used
to obtain geometrical dispersion. The formulae listed can be combined with those
Table 4.3 Expressions for the second and third-order dispersion of common optical systems
Double-pass prism-pair, apex separation l, d 2' 3 d 2 P
angular deviation within ray of “ 2
D
d! 2c 2 d 2
2
d 3' 4 d P d 3P
D 3 C
d !3 4 2 c 3 d 2 d 3
" 2#
d 2P d 2n dn
D 4l sin ˇ C.2n1=n /3
d 2 d 2 d
2
dn
8l cos ˇ
d
"
d 3P ı 3 dn 3 d n d 2n
D l cos ˇ 24 n 48n 24
d 3 d d d 2
" 3
dn ı 6 ı ı ı
C l sin ˇ 12 n C 12 n4 C 8 n3 16 n2 C 32n
d

ı dn d 2 n d 3n
C 24n 12 n3 C 4
d d 2 d 3
" 2 #3=2
Double-pass grating-pair, separation l, angle
d 2' 3
of incidence ” , line spacing d. Dl 2 2 1 sin
d !2 c d d

d 3' 4
D 6l 1 C sin sin2

d !3 c3d 2 d
" 2 #5=2

1 sin
d
in Table 4.2 to identify a suitable geometrical arrangement (e.g. prism separation)

whose GDD and TOD have approximately equal magnitudes but opposite signs to
those of a bulk material such as a laser crystal. In this way, systems such as prism
pairs may be used to implement dispersion compensation in a laser resonator, which
for many lasers is a prerequisite for stable modelocking.
Mirror dispersion results from interference effects in dielectric Bragg mirror
coatings and its application to dispersion control in femtosecond laser systems was
first reported in [16]. All Bragg mirrors exhibit GDD, as illustrated by Fig. 4.3,
which shows the reflectivity and GDD curves for a 10-pair Bragg mirror comprised
Fig. 4.3 Simulated reflectivity and group-delay dispersion of a Bragg mirror comprising 10 equal
pairs of quarter-wave layers with alternating refractive indices of 1.35 and 2.35
of alternating n D 1.35 and n D 2.35 index quarter-wave layers. Chirping the Bragg
period [17] allows the mirror dispersion to be engineered to achieve a specific
(typically negative) GDD over a certain wavelength range. Unavoidable modulation
in the GDD characteristics of chirped mirror coatings can be addressed by designing
matched pairs of coatings, in which the GDD modulations of one mirror are
cancelled by those of the other mirror [18]. Gires-Tournois interferometer (GTI)
mirrors [19] offer an alternative means of introducing substantial GDD via a Bragg
mirror coating containing an embedded etalon-like structure, and typically offer
several times the GDD of a chirped-mirror coating but over a narrower reflectivity
bandwidth.
Waveguide dispersion is unique to lasers incorporating a waveguide such as an
optical fibre, and may be a significant contributor to net cavity dispersion. Normally
waveguide dispersion is only practical to exploit in fibre lasers [20] or fibre optical
parametric oscillators [21].
4.2.2.2 Ultrafast Pulse Propagation Modelling in a Laser Resonator
Ultrashort pulses propagating inside a laser resonator are subject to a variety of

linear and nonlinear effects, which act to reshape the pulse intensity and phase
in both the time and frequency domains. These effects include material and
geometrical dispersion, frequency-dependent gain and loss, saturable absorption (in
certain laser media, also saturable gain) and self-phase-modulation. For the purposes
of modelling the pulse evolution, we can consider each effect to act separately inside
a laser resonator, as illustrated in Fig. 4.4.
The extended nonlinear Schrödinger equation (ENLSE) describes these effects
in a single nonlinear differential equation:
@A X ˇk @k A
D Œg l q.t/A C i kC1 C i jAj2 A (4.13)
@z kŠ @t k
k1
Fig. 4.4 Schematic of a ring resonator showing consecutive operation of dispersion, self-phase-
modulation, gain/loss and saturable absorption operators. A linear resonator may be modelled in a
similar way
In Eq. (4.13), g is the roundtrip amplitude gain coefficient, which may be

a function of frequency, propagation distance and pulse energy (in the case of
saturable gain); l is the roundtrip amplitude loss coefficient (from parasitic losses
or from output coupling); q(t) is the time-dependent saturable loss coefficient; ˇ k is
the kth derivative of the cavity propagation constant with respect to !; and is the
nonlinear coefficient. The ENLSE can be solved numerically by using a split-step
Fourier approach [22].
Gain saturation can be treated by allowing the gain to depend on the pulse energy
according to:
g0 .z; !/
g.z; !/ D (4.14)
TR
R =2
2
1C jA.t/j dt=EL
TR =2
where TR is cavity roundtrip time and EL is the saturation energy of the laser gain
medium, which can be related to the saturation fluence of the gain medium and the
laser mode area [23]. The dependence of the gain on the propagation coordinate z
may be important in gain media in which the population inversion varies along their
length, e.g. fibre amplifiers. A parabolic approximation to the gain dispersion can
be treated explicitly by the addition of another term to the ENLSE [24], or it can be
handled implicitly by including g(!) in the numerical model [23].
The saturable absorber action can be treated in a similar way to the gain, but here
the time-dependence of the absorber must be included. For slow saturable absorbers
the dynamic loss coefficient can be described by [25]:
2 3
Zt ˇ ˇ
6 1 ˇ 0 2 0 ˇ7
q.t/ D q0 exp 4 ˇA.t / dt ˇ5 (4.15)
EA
TR =2
where EA is the saturation energy of the absorber, and the integral term describes
the total pulse energy incident on the absorber until a time t. This expression is
valid when the duration of the pulse is much shorter than the recovery time of the
absorber, which itself is assumed to be shorter than the cavity roundtrip time, TR .
Fast saturable absorbers operate in a regime where the duration of the pulse is
much longer than the recovery time of the absorber. Consequently, such absorbers
respond to the peak power of the pulse, not the integrated energy, and are described
by [24]:
q0
q.t/ D (4.16)
1 C jA.t/j2 =PA
where PA is the saturation power of the absorber.
Both analytical and numerical solutions to the ENLSE have been studied in a
variety of contexts, and for further details the reader is referred to papers dealing
with specific cases [26–29].
4.3 Passive Modelocking with Saturable Absorbers
We now know that modelocking is achieved by introducing a modulation to the

system, usually in the form of an amplitude or frequency modulation within the
cavity. There are many ways of generating this necessary modulation and much
literature has been written on each different technique. However, in most modern
femtosecond laser systems, just two techniques are used to generate femtosecond
pulses. These are passive modelocking by use of a saturable absorber in the form
of a semiconductor saturable absorber or Kerr-lens mode-locking. Both of these
techniques are classed as passive modelocking techniques that rely on an amplitude
modulation.
In passive modelocking, a non-linear intracavity element, which exhibits an
intensity dependent loss, is present in the system to allow the circulating radiation
to modulate and subsequently modelock itself in a process known as self-amplitude
modulation (SAM) [30–32] (defined in Sect. 4.2.1). The phases of the modes in the
cavity self-adjust to produce a field that exhibits the least loss as it propagates round
the cavity. This is known as the maximum emission principle [33] and ensures that
given the suitable circumstances, a pulsed laser field will build up from amplitude
noise.
Fig. 4.5 Passively mode-locked pulse shaping mechanisms due to gain and loss dynamics of:
(a) a slow saturable absorber, (b) a fast saturable absorber and, (c) solitonic modelocking with a
slow saturable absorber
The modulation required for modelocking can be thought of as a shutter, which

has been placed close to one of the end mirrors of the laser cavity. When the shutter
is closed there is a loss in the system and there is no laser output. If the shutter is
opened briefly every nl/c seconds the phase relationships of the oscillating modes
become fixed and a train of pulses are generated. This periodic ‘shutter’ modulation
of the gain (or loss) is created by an intracavity element, which has some appropriate
non-linear intensity-dependent characteristic and is known as a saturable absorber.
Saturable absorber systems, be it a dye, SESAM or other kind, such as colloidal
quantum dots embedded in glass [34] or carbon nanotube based saturable absorbers
[35], have several different pulse shaping capabilities. A mathematical description
of passive mode-locking with both slow [36] and fast [24] saturable absorbers
systems has been successfully formulated and has been able to describe the action of
a pulse on an absorber (and gain dynamics in the cavity) in the time domain. It is also
possible to derive steady-state solutions for the pulse duration, which occur after
many round trips of a pulse within the cavity. The effect of the saturable absorption
on a laser pulse can be most easily understood in the time domain (e.g. by solving
the ENLSE introduced in Sect. 4.2.2.2), and although a rigorous derivation of the
dynamics of passive mode-locking is beyond the scope of this chapter, a qualitative
understanding of the effects is very useful.
4.3.1 Pulse Shaping Mechanisms
Figure 4.5 illustrates the three main pulse-shaping mechanisms responsible for
the generation of ultra-short pulses using saturable absorbers. In the case where
the recovery time of the saturable absorber is not much faster than the pulse
duration, and the upper-state lifetime of the gain medium is short, then the
pulse shaping mechanism cannot shape the trailing edge of the pulse, as the
absorber remains strongly bleached for a duration much longer than the pulse
duration. If the bleaching of the saturable absorber means there is net gain, then
the trailing edge of the pulse is amplified along with any noise, and the pulse
soon becomes unstable. However, if the saturation fluence of the gain medium is
sufficiently low and the upper-state lifetime sufficiently fast, the gain saturates very
quickly after the absorption is bleached. This has become known as dynamic gain
saturation [37]. It allows for a short net-gain window to be formed (as illustrated in
Fig. 4.5a). Due to the long upper state lifetime in gain media such as glass-based or
crystalline solid-state media, dynamic gain saturation cannot be realised. Therefore,
this mechanism is limited to short-lifetime gain media such as semiconductors
or dyes.
The second pulse shaping mechanism (Fig. 4.5b) is known as fast saturable
absorber (FSA) modelocking and requires a saturable absorber with a fast recovery
time so that a suitable short net gain window can be created. For solid-state laser
systems, the most successful FSA-based mode-locking mechanism has been Kerr-
lens modelocking (KLM), whereby the laser crystal itself is encouraged to act like
a fast saturable absorber. In the case of a fast saturable absorber, any spikes in
the random temporal output will suffer low attenuation in the saturable absorber,
whereas low intensity noise will be attenuated to a far greater extent. As a result, it
is possible for a single noise spike to be promoted by a succession of many round
trips into a short, intense pulse. When the intensity of the pulse is large enough to
sufficiently bleach the absorber, then a short window of net gain appears for the
intense central maximum of the pulse and the low intensity wings experience net
loss, and this acts as the pulse shaping mechanism. This makes the assumption that
there is no appreciable variation in the gain during the passage of the pulse, which
requires the upper-state lifetime of the gain medium to be significantly longer than
the absorber recovery time, such as in glass-based solid state lasers where the upper
state lifetime is typically hundreds of microseconds [38]. Of course, there is a limit
to how short the pulse can be, limited by the recovery time of the absorber and the
finite extent of the gain bandwidth.
The third important pulse shaping mechanism in mode-locked lasers is soliton
mode-locking [28, 38, 39]. In this regime, a saturable absorber is responsible for
starting and stabilising mode-locking, however the pulse duration is controlled by
a cancellation of non-linear phase changes and anomalous dispersion contributions
within the cavity. In media that exhibit the nonlinear optical Kerr effect, which is
an intensity dependent modification to the refractive index of the material, high-
intensity pulses produce time dependent phase changes in the material as they
propagate, known as self-phase modulation (SPM). The modulation of the phase
produces a linear frequency chirp of the pulse carrier frequency, which increases
with time, and is therefore identical in effect to normal dispersion. This acts as
a pulse broadening mechanism, and large amounts of SPM can lead to severe
instabilities. However, the effect can be compensated by a suitable amount of
anomalous dispersion, allowing the pulse to propagate without broadening from
either mechanism. In this case the pulse is a stable solution to a wave equation with
non-linear terms arising from the SPM and anomalous dispersion, which is known
as a soliton solution.
In solitonic modelocking an additional loss mechanism (typically a saturable
absorber) is required to initiate the formation of solitonic pulses from background
noise spikes, and to stabilise the solitonic pulses once they are formed. The short net-
gain windows that are achieved through dynamic gain saturation and FSA are not
necessary for solitonic modelocking because the soliton formation is the dominant
pulse shaping mechanism. This de-couples the saturable absorber from the cavity
and relaxes the constraints of the saturable absorber, thus allowing for a much longer
net-gain window than its dynamic gain saturation and FSA counterparts (Fig. 4.5c).
This greatly relaxes the limitations of the saturable absorber used to initiate the
modelocking. The pulse duration of the soliton solution is comparable for fast and
slow absorbers [28]. The relaxation time of the saturable absorber can be up to
10 times longer than the pulse duration of the laser. This makes semiconductor
saturable absorbers ideal candidates as mode-locking devices.
4.3.2 Important SESAM Properties
A semiconductor saturable absorber has five important macroscopic properties that

determine its performance within a laser system. These are: the impulse recovery
time (£A ), the modulation depth ( R), the non-saturable loss (RNS ), the saturation
fluence (Fsat ) and the spectral bandwidth ( œ).
The first of these properties is the impulse recovery time of the device. Essen-
tially, this is the time it takes for the device to recover after a suitably intense pulse
has bleached the absorber. When FSA modelocking is the dominant mechanism
within the cavity, the recovery time needs to be very fast (around that of the pulse
being generated). When solitonic modelocking is the dominant mechanism then the
recovery time can be up to 10 times larger than the pulse duration.
The modulation depth, R, is the maximum nonlinear change in reflectivity
between a low intensity pulse and a high intensity pulse, which will bleach the
absorber. Figure 4.6 shows the saturable reflectivity of a typical SESAM device.
If the modulation depth is too small, then the pulse shaping mechanisms may be
inefficient. A large value for this property will allow the generation of very short
pulses and increase the chances of self-starting operation, however it also increases
the potential for unwanted Q-switching instabilities within solid-state lasers, or
may lead to cavity losses which are too large to sustain laser operation, therefore
a balance must be found. Furthermore, in femtosecond lasers or soliton mode-
locking, careful attention must be paid to the dispersive characteristics of the device.
Typically, R is in the range of 1–2%. This value can be altered by changing the
reflectivity of the front surface of the absorber or by changing the absorber thickness.
Once an intense pulse has bleached the absorber, any remaining loss of the
device is defined as the non-saturable loss, RNS . These losses include reflectivity
Fig. 4.6 A sketch of the saturable reflectivity of a typical SESAM under cw illumination, showing
the important parameters of modulation depth, saturation intensity and non-saturable loss
of the Bragg stack (which will be <100%), scattering losses within the material
and excited state absorption. The design and growth characteristics of the device
strongly affect this parameter. For low gain laser systems it is imperative to have
intracavity losses that are as low as possible.
The saturation fluence is defined as the pulse fluence (energy density per unit
area) required to saturate the absorption of a device. The value for the saturation
fluence should be kept relatively small so that the incident fluence needed to saturate
the device does not damage the structure.
The shortest pulse durations that can be generated from a SESAM modelocked
laser system are limited by two factors. One is the bandwidth of the gain material
and the other is the spectral bandwidth of the Bragg mirror of the device. The
bandwidth of SESAM devices is determined by the index contrast of the layers
and the thickness of the layers in the Bragg stack.
In laser systems with long upper-state lifetimes, which are passively mode-
locked with a slow saturable absorber, there is a tendency for instabilities, usually
in the form of Q-switched modelocking [25, 40] (QML). In QML the mode-locked
pulse train output of the laser is modulated within a broader, Q-switched envelope,
typically with kHz frequencies, as opposed to the hundreds of MHz repetition
frequencies of the pulse train. For applications which require constant pulse energies
at high repetition rates, QML is a serious drawback. However, QML has found some
applications in laser machining, as the modulated pulse train has higher peak power
than the continuous wave mode-locking regime.
Honninger et al. [40] showed that the criterion for stability against QML is
given by:
ˇ
dR.EP / ˇˇ TR TR EP
EP < rD C (4.17)
dEP ˇE P L L ESAT;L
where EP is the energy of a modelocked pulse in the cavity, R(EP ) is the nonlinear
reflectivity, TR is the cavity round trip time, L is the upper-state lifetime of the
laser medium. ESAT,L is the saturation energy of the gain, which is defined as the
product of saturation fluence (FSAT,L D h /(m L )) and the effective laser mode area
in the gain medium. r is the pump parameter, defined as r D 1 C P/PSAT,L where
PSAT,L is the saturation power, given by ESAT,L / L A and describes the number of times
over threshold at which the laser is operating. Eq. (4.17) shows that modelocking
can be achieved when EP Esat , when the laser is operated far beyond threshold,
r 1, or the cavity round trip time is long. These constraints are very significant
for the choice of saturable absorber, especially in the case of SESAMs, for use with
a particular laser system. For example, in a passively mode-locked system using
an intracavity SESAM, a high repetition-rate laser with low intracavity power will
require a SESAM with low saturation fluence in order to minimise the LHS of Eq.
(4.17). However, in the case of lasers with very high intracavity pulse energies,
the saturation fluence needs to be large enough to avoid over-saturation of the
SESAM, which may lead to multiple pulsing, where the mode-locking dynamics
result in two lower power, longer duration pulses [41]. The SESAM also needs
to be resistant to intensity related effects, such as non-linear optical effects like
two-photon absorption. A simple way of correctly matching the intracavity pulse
energy, EP , to the saturation fluence of the SESAM, Fsat , is by controlling the spot-
size of the intracavity beam on the absorber. However, there is obviously a limit to
the parameter range using the spot-size alone. The absorption recovery time of the
absorptive transition is also important, requiring consideration of the mode-locking
mechanism for the particular gain medium as to whether the saturable absorber is
required to be fast or slow.
4.3.3 SESAM Material Systems
Several researchers have been able to develop a recipe for the design and production
of tailor-made SESAMs for insertion into specific systems. It should be noted that
semiconductor saturable absorber mirrors (SESAMs) and saturable Bragg reflectors
(SBRs) both have an intensity-dependent reflectivity. Although SBRs and SESAMs
could be classed as separate devices, they are in fact very similar in structure and
in the way they operate. Differences between the two types of devices are usually
attributable to the way they are grown and processed.
The first semiconductor saturable absorber devices used to modelock solid-
state lasers date back to 1992 [2]. Since then, they have become very popular
intracavity devices that can be exploited in lasers to generate picosecond and
femtosecond pulses. Epitaxial growth techniques such as molecular beam epitaxy
(MBE) and metal-organic chemical vapour deposition (MOCVD) can be used to
produce devices with very well defined parameters. Being able to grow devices
that have specific and pre-determined properties makes them very attractive as
modelocking elements. These devices consist typically of alternate layers of high
Fig. 4.7 Schematic diagram of a typical SESAM structure. The device consists of a substrate onto
which a Bragg stack is grown. AlAs and GaAs have a sufficient refractive index contrast and almost
identical lattice constant to produce very high quality DBR structures. The last few layers contain a
quantum well or quantum dot absorber. Material type and placement of the absorber layer is crucial
and strongly determines the performance and losses of the device
and low index semiconductor materials, which act as a Bragg reflector with a thin
saturable absorber layer near the top of the device (Fig. 4.7). As already discussed,
the modulation that is necessary for modelocking is brought about via bleaching of
the absorber layer when sufficiently intense intracavity pulses are incident on the
device.
The absorber layer consists of either quantum-well or quantum-dot material,
depending on the type of laser that is being modelocked and its wavelength of
operation. The first semiconductor device to be used as a modelocking element was
a GaAs/GaAlAs device that had 75 GaAs quantum wells embedded in the absorber
layer. This device was used in a Ti:sapphire laser and assisted in the formation
and stabilisation of picosecond pulses [42]. This semiconductor approach was then
transferred to a Nd:YLF laser with similar results [2]. This new technique was
termed resonant passive modelocking but was the basis of SESAM modelocking
as we know it today.
Quantum-dot systems have atom-like density of states, which allows for the
growth of devices that have tuneable optical properties, depending on the size and
density of the quantum dots within the absorber layer. Although QD technology
is less well established than its QW counterpart, it has been recognised that QDs
have several advantages over QWs for use in SESAMs operating in the near-
IR. They have ultrafast absorption recovery times [43] and large inhomogeneous
line-widths relative to QWs. This makes them ideal candidates for laser systems
where large absorption bandwidths are required. Typically quantum-dot devices
also exhibit lower saturation fluences when compared with quantum-well devices
that have a similar modulation depth. In 1999, the first quantum-dot devices were
used to modelock semiconductor edge emitter devices [44]. Following on from this
result, Garnach et al. demonstrated the first QD-SESAM in 2001 [45]. Rafailov
et al. then went onto demonstrate the fast recovery dynamics of QD-devices [46]
and pulse durations of 86 fs have been demonstrated at 1.3 m with QD-SESAMs
[47]. A recent review of ultrashort-pulse laser modelocked by QD-based saturable
absorbers can be found in [48].
Different III–V semiconductor systems have since been investigated to find

different wavelength regions of operation. The lattice match between AlAs and
GaAs is good enough that it is possible to produce high quality DBR structures with
low losses. To create a SESAM with a QW or QD absorber that operates at a specific
wavelength it is necessary to introduce other elements to shift the band gap of the
device to a particular wavelength. This introduces strain between the boundaries of
the different layers of the SEAM and leads to increased losses.
The first SESAM structures for solid-state lasers were based on QW In-
GaAs/GaAs materials, where the bandgap of the absorber allowed modelocked
operation of a Nd:YLF laser at 1,047 nm. A wide range of passively modelocked
near-infrared solid-state lasers operating in the 1,200–1,600 nm region have also
used SESAMs based on InGaAs quantum wells on GaAs based Bragg mirrors
or InGaAsP quantum wells on InP based Bragg mirrors [41, 49, 50], both of
which have recognized shortcomings [51]. The indium concentration required for
longer wavelength operation (>1 m) of an InGaAs device results in a lattice
constant differential that is beyond the critical level for a coherently strained
InGaAs:AlAs/GaAs Bragg mirror structure. Strain relaxation occurs with the
inevitability of high non-saturable losses and low damage thresholds, which makes
these devices unusable in near-infrared solid state lasers. The alternative scheme of
growing an InGaAsP absorber on an InP-based mirror structure offers narrow band-
width Bragg mirror reflectivity, due to the small refractive index contrast achievable
with materials that are lattice matched to InP, but this restricts significantly the pulse
durations that can be generated.
A significant new route in the design and development of more suitable SESAM
devices for ultrashort pulse lasers has been demonstrated [52–54]. In 2002, Sun
et al. [52] reported the first demonstration of passive modelocking using a GaInNAs
SBR incorporated within a high power picosecond Nd-based laser operating near
1,300 nm, thus demonstrating the high damage threshold of GaInNAs based
saturable devices. The key to this demonstration involved the use of GaAs-based
SBRs that incorporate GaInNAs quantum wells for saturable absorption. Inclusion
of small percentages of nitrogen not only reduces the strain, but also shifts the
absorption edge very effectively into the 1,200–1600 nm region. This has allowed
for reliable femtosecond operation of modelocked laser at wavelengths >1 m with
devices that have suitably low non-saturable losses.
The low-loss nature of GaInNAs SESAMs is crucial for the development of effi-
cient and reliable Cr4C :forsterite lasers. The active forsterite medium has relatively
low gain so its lasing efficiency suffers when lossy intracavity elements are inserted
into the system. This means that Cr4C :forserite lasers that incorporate InGaAs on
GaAs SBRs [51, 55, 56] have inferior performance characteristics compared to their
cw or Kerr-lens modelocked counterparts. Work done by McWilliam et al. [57]
demonstrated that GaInNAs SESAMs can generate sub-100 fs pulses in the near-
IR. Current research is now looking to extend SESAM technology to even longer
wavelength regions. This will be discussed in the final section of this chapter as
we look at a few examples of state of the art SESAM devices in solid-state laser
systems.
4.4 Selected Highlights of Solid-State SESAM

Modelocked Lasers
This last section will briefly look at a small selection of SESAM modelocked solid-
state laser sources. This is by no means an exhaustive list of the most recent research
in the field of ultrafast laser science. In fact we have restricted this section in order to
highlight advances in: high power systems, high pulse repetition rate laser systems,
2 m laser sources, and SESAMs that are now bringing added functionality to the
systems they are incorporated into.
4.4.1 High Power Systems Incorporating SESAMs
SESAM technology is now allowing researchers to develop laser oscillators that

can generate pulse energies to the 10 J level without the need for amplification
[58]. The current state of the art with Yb:YAG thin-disk lasers can generate pulse
energies of up to 11.3 J with the thin-disk gain element in a single folding mirror
configuration [59] and up to 25.9 J in a multi-pass cavity [60] that produces
700 fs pulses at a few MHz pulse repetition rates.
It is also possible to generate average output powers beyond the 100 W level
for the first time with a SESAM-modelocked Yb:Lu2 O3 thin-disk laser oscillator
generating 141 W, with 738 fs pulses, at 60 MHz repetition rate, with a pulse energy
of 2.4 J with an optical-to-optical efficiency of more than 40% [61].
4.4.2 High Pulse-Repetition Frequency SESAM Based Systems
High pulse-repetition-frequency (PRF) femtosecond lasers are attractive sources for

a wide range of applications including optical communications, biophotonics and
metrology (through frequency comb generation – see Chap. 6 by Udem et al.).
However, obtaining femtosecond operation at high PRFs in bulk mode-locked
lasers is challenging because cavity size reduction tends to promote the onset of
Q-switched modelocking and makes dispersion management more complicated
given that the commonly-used prism pair compensation scheme is no longer
practical.
SESAM modelocking has also helped push the frontier in gigahertz pulse repeti-
tion rates from diode-pumped solid-state lasers. In 2002 Krainer et al. demonstrated
a PRF of 160 GHz at 1 m [62] and more recently Oehler et al. demonstrated
PRF 100 GHz at 1.5 m [63, 64], although these systems are not capable of
generating pulse durations below 1 ps. This is due to the narrow bandwidth of the
laser materials that were used and also the lack of dispersion management that could
be incorporated into such a small cavity.
To reach femtosecond pulse generation at GHz PRFs we have to look towards

larger bandwidth materials and suitable dispersion management. A number of
sources directly generating femtosecond pulses at GHz repetition rates have been
demonstrated experimentally including a 10 GHz Ti:sapphire laser [65], a 3.6 GHz
Cr4C :YAG laser [66], a 1 GHz Cr3C :LiSAF [67, 68], and 1 GHz Yb:KYW [69]
and Yb:KGW lasers [70]. Liu et al. have also demonstrated a Cr4C :forsterite laser
incorporating a low-reflectivity intracavity flat-surface element to harmonically
multiply the PRF to 1.24 GHz [71]. All of these systems rely on the Kerr-lens
modelocking technique. There is also a significant level of interest for the generation
of high PRF ultrashort pulses with self-starting operation with SESAM modelocked
systems.
Laser cavities incorporating anti-resonant (SESAMs) assist in forming and
sustaining the pulse within the cavity, thus relaxing the constraints that are necessary
in KLM lasers. Indeed, there are several recent pieces of work that incorporate anti-
resonant SESAMs to help generate pulses above 1 GHz. In all of these systems
dispersion is managed by using either a single prism or by exploiting chirped-mirror
designs.
Pekarek et al. recently demonstrated a diode-pumped Yb:KGW laser with a
repetition rate of 1 GHz capable of generating a pulse duration of 281 fs at a
wavelength of 1,041 nm [70]. This work incorporated a standard anti-resonant
quantum well SESAM with a saturation fluence of 40 J/cm2 , a modulation depth
of 0.5%, and low non-saturable losses (<0.1%). Mode-locked lasers operating
at GHz repetition rates often use SESAMs with low saturation fluence to over-
come the QML threshold. With harmonic modelocking they were also able to
increase the pulse repetition rate up to 4 GHz with an average power of 900 mW
and a pulse duration of 290 fs. They used a specially designed GTI mirror within
the cavity to perform the dispersion compensation of the system.
Work on SESAM design [47, 72] has shown how resonant dispersionless
SESAMs with large modulation depths and low saturation fluences can be in-
corporated into solid-state lasers. These ideas have been taken further to show
how a near-resonant GaInNAs-based SESAM can be incorporated to provide
the required modulation and dispersion compensation within a Cr4C :forsterite
cavity for the generation of 150 fs pulses at a PRF in excess of 0.6 GHz with
average output powers of 270 mW at the technologically relevant wavelength of
1.3 m [73].
This resonant-like GaInNAs SESAM was grown by solid-source molecular
beam epitaxy and consisted of a 30-pair AlAs/GaAs distributed Bragg reflector.
The top-most GaAs layer of the stack was extended to be a half-wave layer to
produce a resonant device at 1,342 nm. The 10-nm GaInNAs absorber layer was
positioned 5 nm from the surface to be (a) at the antinode of field i.e. to obtain
a low saturation fluence and (b) close to the surface to obtain fast recovery by
recombination of excited carriers through surface-defect states. The stop-band of
the Bragg stack extended over 110 nm, centred around 1,325 nm, and the quantum-
well luminescence peaks at 1,330 nm. Room temperature reflectivity measurements
Fig. 4.8 Reflectivity and GVD characteristics for the resonant-like GaInNAs QW structure
confirmed that the resonant nature of the device led to a modulation depth of 7%
at 1,330 nm. This would typically make the device unsuitable for operation in
a Cr4C :forsterite laser system, but the low insertion losses of the device and its
high reflectivity characteristics at shorter wavelengths (around 1,270 nm) allowed
continuous-wave output powers of 1.1 W to be generated by the laser when the
device was inserted into the laser cavity.
Figure 4.8 illustrates the group velocity dispersion characteristics of the SESAM.
This is a typical plot for a resonant-like device compared against the anti-resonant
case, illustrated in Fig. 4.3, where the GVD is flat across a large proportion of the
bandwidth of the device. From Fig. 4.8 it can be seen that GVD values between
0 and 1,100 fs2 per bounce can be generated by the device when operating at
wavelengths between 1,260 and 1,310 nm respectively. The positive dispersion
generated from the Cr4C :forsterite crystal used in this experimental assessment was
estimated to be 1,050 fs2 per round trip [74].
Given the relatively large modulation depth of the SESAM, the laser was
operated away from its higher gain region (1,270 nm) to ensure the initiation of
modelocking. This was achieved by inserting a fused silica prism into the cavity
to force the laser to operate at a wavelength were modelocking was self-starting.
When modelocked with the 1% output coupler in place, output powers of 270 mW
could be extracted from the system. The laser supported an optical spectrum
of œFWHM D 12 nm and the autocorrelation data implied near-transform-limited
pulses of 150 fs. An RF spectrum analyser was used to confirm the pulse repetition
frequency of 652 MHz. This piece of work illustrates how SESAM devices are now
becoming multi-functional components within solid-state laser systems. Not only
can they start and maintain the formation of modelocked pulses, they can also relax
the need for GTIs or chirped mirrors.
4.4.3 Electrical and Optical Control of SESAMs
Researchers have gone a step further to look at ways of disturbing the modelocking
dynamics of the SESAM to force the laser between cw and cw-modelocked
regimes. Zolotovskaya et al. [75] developed a passively mode-locked Cr:forsterite
laser incorporating a dc-voltage-controlled p-n junction quantum-dot semiconductor
saturable absorber mirror. With this system output pulse durations could be varied
from 17.4 ps to 6.4 ps by applying a dc voltage between 0 and 4.5 V across
the SESAM. In this work the QD SESAM structure comprised of a 300-nm Si-
doped GaAs buffer layer deposited on an n-type GaAs (100) substrate, an n-doped
distributed Bragg reflector (DBR), and a long GaAs microcavity, with a design
wavelength of 1,250 nm incorporating a p-doped GaAs cap layer. Metal contacts
were deposited on the p- and n-side of the device. The DBR stack consisted of 33
pairs of Si-doped GaAs–AlGaAs layers, with a stop band centred at a wavelength of
1,260 nm. The QD saturable absorber region was formed in seven groups consisting
of three layers of InAs–InGaAs QDs, with 32-nm-thick GaAs spacer layers in
between. The groups of QDs were positioned at the antinodes of the electric field
standing wave using GaAs spacers. Stable modelocked operation of the Cr:forsterite
laser was attained across the whole bias range with pronounced pulse shortening
observed with increasing applied reverse voltage. These workers were able to infer
that the reduction in the modelocked pulse duration was attributed to a decrease in
the saturable absorber recovery time under reverse biasing.
Several researchers have also looked at ways of disturbing the modelocking
dynamics of the SESAM to force the laser between cw and cw-modelocked regimes
[76–78] by optically disturbing the SESAM. Currently, femtosecond laser systems
operate in a fixed pulsed regime. There are several applications, particularly in
the area of biophotonics, that would profit from a system that provided more
flexible characteristics. These include experiments involving optical transfection
of trapped cells [79] and optical tweezing [80] where the laser system can be
simply and effectively switched between the continuous wave (cw) state and the
cw mode-locked state to enable different functionalities at specific times. Actively
modelocked lasers have demonstrated this type of regime change, but the electronic
modulators required for this complicate the system and add cost to the overall
setup. Mechanical methods have been implemented to switch between cw and
femtosecond operation of passively modelocked systems however switching times
have been relatively long (ms to s) [81, 82]. Savitski et al. [76] demonstrated a
picosecond Nd:YVO4 system that could switch between the cw and cw mode-
locked state, with a switching time 50 s, however picosecond pulses are not
suitable for most biological applications [83]. Savitski et al. have also demonstrated
this switching technique using a SBR device within a femtosecond Ti:sapphire laser
[77], and performed a detailed study of the changes in the nonlinear optical response
of the saturable absorber in the presence of a continuous-wave optical pump source.
They also went on to develop a model of the heating dynamics within the device
under optical pumping and show that fast optically induced heating could be used
Fig. 4.9 Schematic diagram of the set-up used to switch the Cr:forsterite laser between the cw and
cw-modelocked regime
to externally control the behaviour of the SBR. This external optical pumping of
the SBR allowed for rapid (75 s) switching between CW and femtosecond pulse
operation of a passively mode-locked Ti:sapphire laser.
Work has also been carried out at the biologically relevant wavelength region of
1,300 nm [84] with a Cr4C :forsterite laser system which contained a SESAM that
was optically pumped from outside the cavity, in order to switch the laser from a
state where the laser produced sub-300 fs pulses to a state where the laser operated
in the cw regime. Figure 4.9 illustrates the set up that was used for this experiment.
A standard 4-mirror asymmetric, astigmatically compensated Z-fold cavity was
constructed and a Yb:fibre laser was used as the pump source. This pump beam
passed through a telescope and focusing lens into the Cr4C :forsterite crystal (pump
spot radius, wp 25 m). The 11.6-mm-long Brewster-cut Cr4C :forsterite rod had a
small-signal pump absorption coefficient of 1.3 cm1 , and was mounted in a water-
cooled copper jacket that was maintained at a temperature of 12 ı C. The two curved
folding mirrors in the cavity had radii of curvature of 100 mm and 75 mm for the
long and short arms respectively, high-reflectivity (HR) coatings for wavelengths in
the 1,250–1,370 nm range and high transmission at the pump laser wavelength. A
wedged 0.5% output coupler was located at the end of the long arm of the cavity
and either a HR mirror or SBR structure terminated the short arm of the cavity (spot
size 110 m radius). Two silica prisms were incorporated into the long arm of the
laser resonator to compensate for the positive GVD.
The GaInNAs anti-resonant quantum well SESAM reflectivity characteristics
exhibited a >110 nm-stop-band Bragg reflectivity centred at 1,320 nm and a
photoluminescence peak at 1,340 nm, as detailed in [57]. To control the mode
of operation of the laser, a commercially available external diode laser (EDL)
Fig. 4.10 Typical temporal response of rapid state-switching of the Cr4C :forsterite laser when
(a) the EDL is activated and (b) deactivated
delivering an incident power of up to 1 W at a wavelength of 808 nm was collimated

and subsequently focused through an f D 9 mm lens to generate a spot that could be
overlapped with the intracavity spot incident on the SESAM. The EDL spot size
was comparable to the intracavity spot on the SESAM.
With the prisms inserted in the long arm of the cavity at a tip-to-tip separation
of 340 mm, it was possible to support a spectral bandwidth of 6.3 nm at a
centre wavelength of 1,296 nm with a FWHM pulse duration of 290 fs, assuming
sech2 pulses. The output characteristics of the mode-locked laser are illustrated in
Fig. 4.10. Typical modelocked output powers were measured to be 50 mW.
Figure 4.10 shows how the femtosecond pulse train diminished to a cw state
when the EDL was switched on. Using a fast oscilloscope it was possible to measure
the switching time to be less than 25 s when the EDL was activated. An EDL
power >600 mW was required to initiate the switching effect. As stated by [76]
the main mechanism responsible for quenching cw modelocked operation when
optically pumping the SESAM, is due to a reduction of the QW transition energy
due to heating. When the EDL is turned off it takes 100 s to generate the fs pulse
train. This longer time frame is largely related to the number of round trips required
to establish the stable cw modelocked state, which, for solid state lasers is taken
as >1,500 round trips [40]. Unlike the system discussed in [76] no Q-switching
or relaxation-oscillation-induced spiking was observed during these assessments,
which makes this Cr4C :forsterite system suitable for optical transfection and optical
tweezing experiments at 1,300 nm. These pieces of work again illustrate how
SESAM can be manipulated to add functionality to femtosecond laser sources.
4.4.4 SESAMS for Longer Wavelength Operation
There is now a push to extend the wavelengths of operation for SESAM devices.
As already been discussed, pushing towards longer wavelengths requires thicker
layers within the SESAM structure, which leads to increased strain and losses.
To remove the strain within longer wavelength devices researchers have investi-
gated several different schemes (including carbon nanotubes and InGaAsSb-based
saturable absorbers, which produced 9.7 ps and 3.3 ps pulses near 1,950 nm
and 2,060 nm, respectively), but the most promising technique has involved ion-
bombardment of the SESAM devices.
As an example, Lagatsky et al. [85] have used a GaSb/AlAsSb SESAM structure
for the initiation and stabilization of passive modelocking in a Tm,Ho:KYW laser
at 2 m. The distributed Bragg reflector had a high reflectivity at 1,930–2,150 nm
and two InGaAsSb quantum wells as the absorber. In their original work Lagatsky
et al. demonstrated 3.3 ps pulses centred on 2,057 nm from a Tm,Ho:KYW
laser using this as-grown SESAM [86]. They later discovered that no significant
variations in pulse durations or spectral widths were observed for different values of
intracavity pulse energy or net cavity group-velocity dispersion, and they attributed
this restrictive mode-locking regime to the relatively long recovery time (100 ps)
and low self-amplitude modulation in the as-grown SESAM. To decrease the carrier
recombination time [87, 88], the SESAM samples were irradiated with 4 MeV AsC
ions at doses ranging from 5 1010 cm2 to 5 1011 cm2 . As the implantation dose
increased, a damage-induced reduction of the overall reflectivity was observed.
With this ion-bombarded SESAM, stable modelocking was realised at 2,055 nm
with a maximum average output of 130 mW and a pulse repetition frequency of
118 MHz. The pulse durations varied from 2.64 ps at the modelocking threshold to
570 fs at the maximum output power of 130 mW.
These workers are concentrating on the development of diode- pumped Tm,Ho-
codoped femtosecond lasers using SESAMs having better optimized macroparame-
ters for efficient femtosecond modelocking in the 2 m spectral region and illustrate
how the detailed design of SESAM devices are still yielding significant advances in
ultrashort pulse solid-state laser sources.
4.5 Conclusions
The examples of modern ultrafast oscillators discussed here illustrate how higher
repetition rate multi-GHz laser systems have a requirement for SESAMs with faster
recovery times and lower saturation fluences. The longer upper-state lifetime of
contemporary gain media like Yb:KYW also makes it harder to satisfy the stability
criterion for SESAM modelocking (Eq. 4.17). Consequently, the role of both QW
and QD SESAMs will become ever more important as the need for achieving
broader bandwidth and faster recovery times gets stronger. The push towards mid-IR
ultrafast operation through new gain materials will only be possible with the advent
of new SESAM material systems too. Application-led development will also play a
role in determining the path of ultrafast science. This will include, for example, areas
like low-repetition-rate, high-energy mid-IR lasers for high harmonic generation,
and high-repetition-rate, high-peak-power, short-duration pulses for GHz frequency
combs.
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Chapter 5
Ultrafast Quantum Control in Atoms
and Molecules
Philip H. Bucksbaum
5.1 Introduction
The interaction of short wavelength and strong field lasers with atoms and small
molecules can be described in the language of a control problem: That is, the
electromagnetic field produced by the laser exerts control over the quantum
evolution of the system under study. By exerting this control in a predetermined
way, the system will evolve to some desired final state, such as dissociative products
or photoelectrons in a particular direction. This chapter uses this point of view to
introduce the subject of ultrafast short wavelength strong field interactions. This
subject is quite broad and deep, and this chapter can only discuss a few interesting
aspects of it. Readers who wish to learn more should consult some of the review
papers and textbooks on this subject [1].
To place this in its simplest context, consider the Schrödinger equation for
a molecule in an open environment, and in the presence of a laser field. The
Hamiltonian can be considered as the sum of three parts:
E t/ D i P .x;
.Hmol C Henv C Hlaser / .x; E t/ (5.1)
(Note that this is written using atomic units, in which „ D me D jej D 1). The
first term Hmol is the single isolated molecule Hamiltonian in all its glory, including
all kinetic energy terms, coulomb interactions among electrons and ions, spin-orbit
interactions, and hyperfine interactions. This Hamiltonian has a ground state as
well as bound and continuum excited states with eigenenergies En which satisfy
Schrödinger’s time-independent equation Hmol n .x; E t/ D En n .x; E t/: The second
and third terms describe “everything else,” and here we must adopt a particular
P.H. Bucksbaum ()

SLAC National Accelerator Laboratory, Stanford PULSE Institute,
Menlo Park, CA 94025, USA
e-mail: phbuck@stanford.edu

106 P.H. Bucksbaum
point of view in order to separate this into two parts, due to the laser, and due to the
“environment.” For the purposes of this discussion the laser term Hlaser will be taken
to include both the laser energy itself as well as its interaction with the molecule.
Control is exerted on the quantum system by means of this term.
In order to utilize Hlaser to control the system, we therefore require that it possess
two criteria:
• Hlaser > Henv , i.e. the forces on the system due to the laser must exceed the forces
of the environment, or other forces within the molecule that lead to dephasing or
quantum diffusion of the wave packet away from the optimal path.
• laser < „= E, i.e. the time of the interactions must be less than the natural
dynamical timescale for the system, given by the energy splitting. This timescale
depends on the context. For example, in many molecular problems the relevant
timescale is set by the relative motion of the atoms in the molecule, which
is typically on the order of hundreds of femtoseconds. In other problems, the
relative timescale may be due to the motion of molecular electrons, which can
have dynamics on the few femtosecond or sub-femtosecond scale.
Thus control requires both ultrafast pulses and strong fields, to beat the tendency
towards decoherence and to overcome natural dephasing. Some general protocol is
required to generate a laser pulse corresponding to Hlaser that is optimal for a given
problem.
5.2 Control Schemes
There are two different types of proposals for quantum control, that are known
generally by the names of their inventors, the “Tannor-Rice” scheme and the
“Brumer-Shapiro” scheme. Tannor, Rice, and the team of Brumer and Shapiro have
each written textbooks or monographs including descriptions of control from their
points of view, and these are excellent introductions [2–4]. Here we will merely
summarize the essential features of these schemes.
5.2.1 Born-Oppenheimer Surfaces
Many readers of this chapter may already be completely familiar with the Born-
Oppenheimer approximation in molecules, but since this chapter is intended for a
broader group of laser scientists, we include a “one-page course” on the essential
physics of this powerful idea. A very readable and more complete treatment is given
in a review paper by Worth and Cederbaum [5]. Consider a molecule with N atoms
and many electrons. The quantum Hamiltonian of this molecule can be separated
5 Ultrafast Quantum Control in Atoms and Molecules 107
into a kinetic energy part Tn for the atoms, whose relative positions are described by
a 3N-6 dimensional vector R, (3N-5 for a diatomic molecule); plus all of the terms
describing the kinetic energies of the electrons at their different positions r and the
electrostatic potential energies between all of the pairs of charged particles. It can
be written in a schematic way like this:
H.R; r/ D Tn .R/ C Hel .R; r/ (5.2)
The Born-Oppenheimer approximation is motivated by the insight that the atoms

usually move much more slowly than the lighter electrons, so that the electronic
structure can be calculated assuming that the atomic positions are frozen. Thus the
Tn terms may be neglected in first approximation. R becomes parameters describing
the positions of the atomic nuclei in a simpler eigenvalue equation involving the
electrons:
Hel i .rI R/ D Vi .R/i .rI R/ (5.3)
The electronic energy eigenvalues Vi .R/ are the potential energy surfaces of
the Born-Oppenheimer approximation. Although they are often depicted as one-
dimensional potential wells or two-dimensional “elastic sheets,” they are really high
dimensional manifolds spanning all of the different relative positions of all of the
atoms in the molecule.
The i .R/ form a real orthonormal basis on which the full solution to the
molecular wave function may be expanded:
X
j .R; r/ D i .R/i .r/ (5.4)
i
Combining this expression for with the molecular Hamiltonian, we can express
the full Schrödinger’s equation H D i „ P . Then we employ the familiar algebraic
procedure to find the coefficients .R/, i.e. multiply on the left by each of the i
and integrate. This yields a set of coupled equations that look almost like a series
of Schrödinger’s equations for the atoms moving on the potential energy surfaces
Vi .Ri /, with wave functions that are the expansion functions i:
X
ŒTn C Vi i C ƒij j D i „ Pi (5.5)
j
The different i ’s are coupled together by the non-adiabatic coupling

operatorsƒij , but in regions of nuclear coordinate space where this can be neglected,
the nuclear wave functions may be considered as standing or traveling waves
on separate potential energy surfaces V. This is the picture of intramolecular
structure and dynamics that guides much of the thinking about control in
molecules.
108 P.H. Bucksbaum
5.2.2 Limits to Adiabaticity, and Conical Intersections
The Born-Oppenheimer approximation breaks down when the non-adiabatic cou-

pling operators ƒij cannot be ignored or treated as a small perturbation. These
couplings come about because the wave function is not a simple product state
i .R/i .r/ for a single potential energy surface, and they become large when two
different potential energy surfaces are nearly degenerate.
The usual procedure for treating two degenerate eigenvalues in stationary state
perturbation theory can be employed in this case: We consider a subspace that
contains only the two degenerate i states, and diagonalise the Hamiltonian
including the off-diagonal couplings, but restricted to that subspace. For degeneracy
between two potential energy surfaces, which is the usual case, this is a 2-state
problem. The Hamiltonian takes on the following form in the Born-Oppenheimer
basis: For R such that jV1 .R/ V2 .R/j jƒ12 j,

V1 ƒ12 V1 h2 j r1 i
H12 .R/ D (5.6)
ƒ21 V2 h1 j r2 i V2
In simple one-dimensional problems the eigenvalues of this matrix break the

degeneracy so the energies display an “avoided crossing.” True degeneracy requires
two independent conditions for H: V1 .R/ D V2 .R/; and ƒ12 .R/ D 0. So if R is
just a single degree of freedom, there is usually no value for R that will satisfy both
conditions.
In molecules, however, R spans 3N-6 degrees of freedom corresponding to all
of the relative positions of all the atoms. A single crossing between two potential
surfaces only provides two constraints. Specifically, the locus of degenerate points
in between these two surfaces in the 3N-6-dimensional -basis must fill a subspace
with one dimension less, i.e. 3N-7-dimensions. On each position R in this subspace,
H12 takes on the simple form:

E h2 j r1 i
H12 .R/ D (5.7)
h1 j r2 i E
where E is the degenerate energy.

The off-diagonal terms can now break the degeneracy, but not everywhere in the
remaining space, rather only where h1 j r2 i is non-zero. The gradient coupling
defines a direction where the degeneracy is lifted. In all 3N-8 orthogonal directions
that are still in the V1 .R/ D V2 .R/ subspace the degeneracy is maintained. Thus
crossings of potential energy surfaces are not avoided in molecules with three or
more atoms; in fact, degeneracies are common. This dimensional argument was
first made by Wigner, von Neumann and Teller [6, 7]. The degeneracies are called
Conical Intersections. In the two-dimensional space where the degeneracies are
lifted, the potentials appear as two cones with a common vertex as shown in Fig. 5.1,
which gives this feature its name.
Fig. 5.1 Conical Intersection

between two potential energy
surfaces
Fig. 5.2 Model ground state

potential energy surface for a
triatomic molecule ABC with
two bond lengths: R1 is the
AB bond, and R2 is the BC
bond
5.2.3 Tannor-Rice
David Tannor and Stuart Rice have introduced an intuitive concept for control
based on the motion of coherent wave packet states in laser-excited molecules. This
is often referred to as “pump-dump” control [8]. The essence of this scheme is
demonstrated by considering two Born-Oppenheimer potential energy surfaces in
a molecule. We consider a model molecule consisting of three atoms, A, B, and
C, which have a ground state in which the three are bound together in the order
ABC. There are 3N-6 D 3 dimensions in the Born Oppenheimer potential energy
surfaces, which could, for example, be designated as the AB bond length (R1 ); the
BC bond length (R2 ), and the ABC bend angle (R3 ). The coherent control problem
is to photoexcite the molecule in such a way to control whether A or C dissociates
from the other two atoms. The Born-Oppenheimer surface for the ground state in
the R1 -R2 plane might look like Fig. 5.2.
Note that there are two low places in the energy landscape, where A may
dissociate from BC (along R1 ), or C may dissociate from AB (along R2 ). The initial
state of the molecule is presumed to be the ground vibrational state, which is well-
localized in the region of the potential minimum at (R1 , R2 ) D (2,2). The control
task is to guide the system toward one dissociation channel using coherent light.
110 P.H. Bucksbaum
Fig. 5.3 Model excited state

potential for the molecule
ABC whose ground state is
shown in Fig. 5.2
Fig. 5.4 The path of the pump-dump control scheme is shown above. The molecule is initially at
location 1. It is pumped to 2, and then evolves on the excited surface to 3, where it is dumped to
4 and dissociates. The output channel is selected by controlling the time between the pump and
dump pulses
The Tannor-Rice scheme employs an excited electronic state to facilitate control.

This has a different potential energy surface, such as the one shown in Fig. 5.3.
Tannor-Rice starts with an initial ultrafast photoexcitation pulse, which transfers
some of the probability amplitude residing in the ground state to the excited
state, with the atoms in the same position, i.e. near (2,2). Note that this does not
correspond to the bottom of the excited potential well. Therefore the probability
distribution that had been a stationary state in the ground potential is still localized
but no longer stationary in the excited state potential. The wave packet then evolves
under the forces that are indicated by the potential gradient, and is de-excited back
to the ground state at a later time T. Control of the exit channel depends on T:
As shown in Fig. 5.4 above, dissociation is accomplished by excitation by a short
pulse at t D 0 (1 ! 2 above), followed by evolution on the excited state surface
(2 ! 3), followed by de-excitation at a later time T (3 ! 4). Control is through the
choice of dump time T. The simple premise of pump-dump control is that the initial
molecular state can be selectively transferred to a target state simply by choosing
the coherence properties (in this example, the time of arrival) of an interacting
laser field.
Fig. 5.5 In this model

illustrating Brumer-Shapiro
control, an initial state A may
evolve to either B or C
depending on the properties
of the applied laser fields.
The final state is selected
by controlling interfering
pathways in the quantum
evolution of the system
5.2.4 Brumer-Shapiro
In the alternative Brumer-Shapiro route to quantum control, the final state specificity
comes from the interference between multiple pathways in multiphoton transitions
from the initial state to the final state. This method emphasizes the role of
phase coherence in the control mechanism. Brumer-Shapiro control is multimode
interference between stationary states, whereas Tannor-Rice control is wave packet
evolution of nonstationary states. At first glance it might appear that the control
mechanisms are totally different, since Tannor and Rice emphasize ultrafast pump
and dump pulses to create wave packets that consist of many different eigenstates,
whereas Brumer and Shapiro seem to deal with narrowband resonant processes
with good phase control and excitation in two competing pathways that interfere.
In fact, in many respects these are just two different views, time and spectral, of
the same process. A simple example of how the Brumer and Shapiro idea can
be connected to ultrafast excitation is the two-photon process depicted below in
Fig. 5.5.
We assume that the bandwidth of the pulses is sufficiently broad that A ! B and
A ! C can both occur, and the control problem is whether we can use multipath
interference to select only one of these alternatives. The answer is that we can
control the outcome without changing the power spectrum of the laser pulse, and we
do this by controlling the spectral phase of the light. (Spectral phase is an important
control feature of ultrafast light pulses, and is covered in some detail in other
chapters of this volume, such as Chap. 1 by Wyatt and Professor Walmsley, so I will
assume the reader has some familiarity with it.) The use of phase is seen clearly
by considering the two-photon process within the formalism of time-dependent
perturbation theory, where a non-resonant two-photon excitation is driven by an
operator proportional to E 2 .t/. The Fermi’s Golden Rule transition probability
between the ground state and any excited state is then proportional to the spectral
power of E 2 .t/, i.e. by the square of its Fourier transform. Let’s take a simple
pictorial example: Consider a short pulse E.t/, with a real Fourier transform and
a power spectrum as shown in Fig. 5.6.
112 P.H. Bucksbaum
Fig. 5.6 The four panels show the electric field of a transform-limited ultrafast pulse; the spectrum
of the pulse; the squared field; and the spectrum of the squared field
Fig. 5.7 These panels show the same progression as in Fig. 5.6., but for a phase-shaped pulse. The
spectrum of the squared field displays phase-dependent features that affect two-photon absorption
The spectrum of a transform-limited (TL) pulse is a smooth bell-shaped function

centred on the central wavelength, and so is the power spectrum. The power
spectrum of E 2 is also shown in the last panel on the right of Fig. 5.6, overlapped
with the level diagram to show how both transitions lie within the two-photon
bandwidth.
Spectral phase shaping changes the situation dramatically, as shown in Fig. 5.7
above. Here we display the same spectral content, but the frequencies above the
median are reversed in sign, i.e. advanced in phase by . The power spectrum,
which only depends on the magnitude of the spectral components, is unchanged.
However, the nonlinear spectrum of E 2 is substantially altered, so that the spectral
power for a two photon transition to one of the two transitions is enhanced while
the other transition nearly vanishes. The multipath interference responsible for this
consists of not just two paths, but the continuum of different paths with two photons
from the pulse which sum to the required transition frequency.
Pulse shaping control of this sort has been seen in laboratory experiments, and
as the simple example above suggests, the effects can be quite large.
To conclude, these examples show that ultrafast pulse shaping can be an
effective means to control quantum processes. Both Tannor-Rice and Brumer-
Shapiro provide ways of thinking about quantum control, but neither comes to terms
with the problem of how to find the optimal pulse sequence or phase shape to effect
control. For that we seek some search protocol or algorithm that can be used to
model general systems, to examine their controllability and to find the best control
parameters.
5.3 Optimal Control Theory
One such protocol is Optimal Control Theory. We begin with a general statement of
the problem: Given i .t/ and H D H0 C H 0 Œ".t/, we want to adjust ".t/ to create
a desired target state f .T /. Furthermore, we want to find the “best” path, i.e. the
path that minimizes some cost, such as the total energy consumed. How do we do it?
This is a deep subject, and there are many deep thinkers who have influenced it.
An excellent introduction is the textbook by Tannor [9]. The best we can do here is to
provide some basic information. We will start with some simplifying assumptions:
Two potential energy surfaces in the Born-Oppenheimer approximation; and pure
states (i.e. no decoherence or thermal averaging) so that we can use the Schrödinger
equation without modifications.
The “pump-dump” picture and the “two-path interference” picture both suggest
that a perturbative approach taken to second order (for two interactions with the
laser field) should suffice to describe the process of control. However, following
Tannor, we will take a more general approach that allows for strong fields and any
number of photons.
Our objective can be quantified as the overlap integral, or projection, of the
system .T / on the target state f , i.e.
ˇ˝ ˇ ˛ˇ2
J D lim ˇ f ˇ .T / ˇ D lim h .T /j Pf j .T /i (5.8)
T !1 T !1
ˇ ˛˝ ˇ
where Pf D ˇf f ˇ is the projection operator for channel f, e.g. a particular final
state channel. J is called the “objective functional” for the optimal control problem.
The system state function .t/ is evolving according to some H.t/ that depends
explicitly on the history of the applied laser field ".t/ at all times t < T:
h Œ".t/ .T /j Pf j Œ".t/ .T /i (5.9)
There may also be some constraints. For example, perhaps we need to do this
RT
job with finite total laser pulse energy dtj".t/j2 . To implement this constraint, we
0
modify the objective functional by decreasing its value in proportion to the pulse
energy, as a penalty:
ZT
J lim h .T /j Pf j .T /i dtj".t/j2 (5.10)
T !1
0
where is a Lagrange multiplier.

114 P.H. Bucksbaum
The wave function must obey Schrödinger’s equation, but this may also be
enforced as a constraint, following Kosloff [3], so that we have:
J lim h .T /j Pf j .T /i
T!1
2 T 3
Z ZT
4 @ H.".t// 5
C 2 Re dt h .t/j C j .t/i dtj".t/j2 (5.11)
@t i„
0 0
The “dual” wave function .t/ plays the role of the Lagrange multiplier. Clearly
the second term vanishes for any .t/ which satisfies Schrödinger’s equation,
independent of .t/. Notice by the way, that the opposite is also true: If .t/
obeys Schrödinger’s equation, then the second term vanishes. A convenient physical
interpretation for .t/ is the projection of .T / on the target state, i.e.
.T / D Pf .T / (5.12)
We can use transitions between two states of the system, the ground state (“g”) and
an excited state (“e”), just as in the Tannor-Rice example. The Hamiltonian takes on
a simple 2 2 form:

Hg " .t/ g g
H ; with D ; D (5.13)
".t/ He e e
The job now is to find the extremum value for J by varying its parameters .t/,
.T /, ".t/, and " .t/. The first two variational equations simply direct us to require
that .t/ satisfies Schrödinger’s equation and .T / is the projection of .T / on the
target state, as we supposed from inspection of the form of J. The field variationals
are more interesting. They lead to the principal equation of optimal control:
i ˝ ˇ ˝ ˇ
".t/ D g .t/
ˇ j e .t/i g .t/
ˇ j e .t/i (5.14)
„
This equation states a relationship between the field, the wave function, and the
“dual” function at every time during the quantum evolution of the state. The target
state appears implicitly because of its connection to the dual function .T /, and this
provides a clue about how to solve this equation iteratively:
1. Start with the initial state .t D 0/ and a simple guess for the field ".t/.
2. Propagate the wave function using H Œ".t/ from t D 0 to t D T.
3. Invoke .T / D Pf .T /.
4. Now propagate .t/ backwards in time from T to 0 using H Œ" .t/.
5. Now armed with both .t/ and .t/, we may calculate a new ".t/. This will
generally be different from the first field that was chosen. But this new field can
now be employed in steps 1–5, repeating the iterations until convergence.
Does this work? Often, but not always. The issue of “controllability” is beyond the
scope of this introduction, except to state that not all simple quantum systems are
obviously controllable. A classic example of a “problem” potential is the harmonic
oscillator. Since all energy levels are equally spaced, any transition between two
is potentially a transition among all, which makes control more challenging, if not
impossible.
The ABC dissociation problem that we discussed earlier as an example was
considered by Kosloff et al. for the specific case of mass ratios of 1:1:2 (such as
HHD), as a test of the optimal control algorithm discussed above. The results are
quite instructive regarding the connection to the Tannor-Rice ansatz. They do indeed
find that the best laser field transfers population from g to e in a “pump-dump”
sequence, but the optimal field sometimes requires several pump-dump cycles.
The conclusions of this section are quite powerful. We find that it is possible
to define a protocol for quantum control in many general situations! That is, given
an initial molecule and a more than one possible target product, we can use the
coherence properties of a laser field to selectively direct a transition. The next
question is, so what?! We take up this issue next.
5.4 Deriving Insight from Control Calculations
This section has a grand title that it probably doesn’t deserve, because there is no
general prescription for deriving physical insight from the results of optimal control
theory. Nonetheless, that is a primary motivation for the field. We desire to know the
optimal field, but immediately after that to also know why that field works. What is
the underlying physical mechanism? To illustrate the problem, we consider a recent
theoretical study by Artamonov on the isomerization of ozone [1]. The normally
bent O3 molecule has a metastable triangular form. Optimal control theory was used
to find the optimal field for the transition, as shown in Fig. 5.8. The optimal field,
taken by itself, is rather uninformative.
Perhaps one can glean that the field starts out at a lower frequency, then has a
period of near darkness, before resuming a higher frequency. The spectrum shows
that these two features are quite separate:
The correlation between time and frequency is an important feature of any
control pulse, but that correlation is sometimes difficult to pick out of the temporal
representation ".t/, and the information is totally lacking from the power spectrum.
There are representations that contain both time and frequency information in an
easy to read form. One example from audio waves is a musical score. Sheet music
is a form of audio spectrogram, where each note on the page displays spectral
information through its vertical placement on the musical staff, and temporal
information through its shape and its placement order along the horizontal. This
suggests that a two-dimensional representation could also be employed for light,
and there are several different examples in common use.
116 P.H. Bucksbaum
Fig. 5.8 Left: Optimal field for the ozone isomerization transition [1]. Right: Spectrum of the field
shown on left of the figure (Reproduced and adapted with permission from Ref. [1])
Fig. 5.9 Left: Potential energy vs. opening angle for ozone. Right: WFT spectrogram for the
optimal photoisomerisation pulse (Reproduced and adapted with permission from Ref. [1])
A simple example is the windowed Fourier transform (WFT). A WFT uses a

moving time gate function to restrict the electric waveform to a narrow window in
time. The Fourier transform of the field within this gate as a function of gate position
is then displayed on a two-dimensional plot. The WFT for the optical field found
for the ozone isomerization is shown below in Fig. 5.9, next to the potential energy
curve showing the ground state well (bent form around 112ı ) and metastable well
(triangle form at 60ı ).
The spectrogram shows that two pulses are needed. The first is centred on the
energy differences of levels residing in the stable initial well, and suggest a series
of transitions upwards in the potential well at greater amplitudes, until the molecule
can pass across to the metastable well. Then a positive chirped higher frequency
pulse induces de-excitation to the final state. This pulse has a transfer efficiency of
an impressive 94 %. This simple explanation may not be correct, though, because if
the optimal pulse is replaced by a simple combination of two chirped pulses with the
same shape, but without the low amplitude parts that appear to be a noisy pedestal,
then the transfer efficiency goes down to less than 10 %. Evidently, even the small
bumps and wiggles are very important to the success of the experiment, and the
simple view of chirped pulse ladder climbing is not the whole story, nor even the
biggest part of the story! [1].
One missing element in the simple one-dimensional wave packet interpretation of
this calculation is the three-dimensional structure of the potential energy surfaces for
ozone. The other two dimensions are associated with bond stretching. Although they
are hidden from view in the one-dimensional picture, their presence survives in the
energy level splitting, and the optimal field is affected by this as it tries to steer the
molecule away from unnecessary vibrations excited by sub-optimal control fields.
Two-dimensional representation of control fields: This example demonstrates
the value of good visualization of the control field using two-dimensional spectro-
grams. Optical spectrograms can be constructed in different ways, and the analogy
to music only describes them partially. We would like a spectrogram that retains all
of the same information as the temporal representation, E.t/, which is a complete
description of the field. The WFT does not do this, since it convolves the field with
a gate function of finite width and shape. The gate can smear out sudden field
changes, or attenuate rapid fluctuations. One transformation that retains complete
information is the Wigner distribution, which is the inverse Fourier transform of the
autocorrelation of the complex spectrum (Fig. 5.10):
Z
0
S.; t/ D E. C 0 /E . 0 /e 4i t d 0 (5.15)
Like the field itself, the Wigner distribution is a real function. It resembles a
spectral-temporal probability distribution, but differs in two important ways from
this simple interpretation. First, the Wigner distribution can take on both positive and
negative values, so it can’t simply represent a probability. Second, it has features that
appear in locations in space and time where there is no field at all! These are regions
between optical field pulses, and they represent the relative coherence properties
between sub-pulses that are not temporally connected. Still, like the FROG traces
discussed in Chap. 1 of this book, the Wigner distribution does provide a fairly
simple connection to the real pulse after a little practice. The Wigner distribution is
“overcomplete.” This simply means that that if I divide an electric field waveform
into N pieces, for example in order to plot it in Matlab, then the Wigner distribution
I calculate from this has N N D N 2 pixels, even though only N pieces of
information went into its construction. A different
p transformation
p was developed
that contains the same features but with only N N D N pixels, called the
von Neumann distribution [10].
118 P.H. Bucksbaum
Fig. 5.10 Displays of a two-pulse optical field. Top: The spectrum and the intensity vs. time.
Left: Intensity and power spectrum. Left: Wigner time-frequency distribution, showing coherence
features between the two separated spectral peaks. Right: A Husimi distribution eliminates the
spectral interference features but still shows the spectral separation of the two peaks
Finally, for those who wonder if all two-dimensional optical distributions are
named after Princeton faculty, here is a counterexample: A very useful spectrogram
called a Husimi distribution is a two-dimensional convolution of the Wigner
distribution with a minimum uncertainty Gaussian. This procedure removes rapid
oscillating coherence features from the Wigner distribution, leaving something
that much more closely resembles the temporal-spectral probability. Although this
destroys coherence information contained in the complete description of the field, it
shows clearly how the optical energy is distributed in both time and frequency.
5.5 Producing Shaped Ultrafast Optical Fields
Pulse shaping for ultrafast optical fields can be performed in various ways. There
is an excellent pedagogical review by one of the pioneers in the field, Andrew
Weiner [11]. Here I summarize some of the basic ideas and methods.
Fig. 5.11 A Fourier filter pulse shaper
At its root, pulse shaping is wave filtering. A pulse shaper receives an input wave
form with a complex Fourier transform Ein .!/, transforms it by combining it with
some mask or mixing wave M.!/, and outputs a final waveform Eout .!/, as in the
example in Sect. 5.2 of this chapter. If the mixer is a frequency modulator then we
describe this using the language of nonlinear optics:
Eout .!/ D .2/

Ein .!in /M.!M / (5.16)
where Eout .!/ is nonzero for frequencies ! D !i n ˙ !M .

In this case the main function of the pulse shaping is to add spectral content
to the light field in the form of spectral sidebands spaced apart from the input
frequency by ˙!M . Other examples of pulse shaping that add to the spectrum
of the input field include nonlinear self-phase modulation, including white light
generation (see Chaps. 8 and 9 by Dudley et al. and Wadsworth respectively); and
frequency multiplication, including high harmonic generation (see Chaps. 3 and 7
by Marangos et al. and Mathias et al. respectively).
At the other extreme is a simple grating monochromator with a very narrow slit
M.!/ for ! D !M . We use a different language to describe what the slit does:
0 for ! ¤ !M
Eout .!/ D Ein .!/M.!/ (5.17)
Ein for ! D !M
This kind of mask appears purely subtractive, meaning that it cannot add new
frequencies to Eout .!/, but only filter frequencies that are already present in the
input field. This is an example of a linear filter, whereas the wave mixing modulator
is a nonlinear filter. Most programmable pulse shapers used in quantum control
experiments use a linear frequency filter to shape pulses. Filters used include
grating-mask combinations employing patterned stationary masks, liquid crystal
programmable masks, acousto-optic Bragg cells, and programmable dispersive
filters, such as the “Dazzler.”
The basic configuration of a linear frequency filter, as shown in Fig. 5.11, is
similar to a spectrometer combined with its mirror image:
120 P.H. Bucksbaum
This is sometimes called a “4f ” configuration, because the distance between the
mirrors is chosen to be twice their focal length f. The distance from the gratings to
the mirrors is f, so that the first mirror collimates the expanding fan of wavelengths at
the same time as it focuses each separate wavelength. Such an arrangement does not
change the size of the laser beam from the input to the output. Also, to lowest order
the optical path for each wavelength is the same, so that a short pulse is not dispersed
at the output. The mask is at the image plane of the first spectrometer, which is the
point where the different wavelengths are most cleanly separated. The mask can
then transmit some wavelengths and block others, or apply pre-programmed phase
shifts to different regions of the spectrum. The second half of the device performs
an inverse Fourier transform on the amplitude- and phase-altered spectrum that
emerges from the mask. If the mask is programmable, then this device functions
as an arbitrary waveform generator for light.
There are a few important constraints on the waveform that can be produced by a
Fourier filter pulse shaper. First, if the mask is a static and a linear element as I have
described it, then this device can only attenuate and shift frequencies that are already
present in the input beam. Second, global phase cannot be controlled by this device.
This is sometimes called the “carrier envelope” phase. For any optical field pulse
longer than a few tens of femtoseconds, this phase has no significance, because it
only represents a trivial overall time shift of less than one optical cycle. But for very
short pulses that are only a few cycles long, the carrier phase can determine the
details of the interactions of the light with matter.
Fourier filter pulse shapers can be constructed using several different kinds of
spectral selection, some of which have been commercialized. The simple 4f system
shown in Fig. 5.11 requires a mask-type filter, which can be implemented with
programmable liquid crystals, acousto-optic Bragg-type reflectors, or static masks.
All of these methods are subtractive, and in addition they have various efficiencies.
I have already described how nonlinear processes can be controlled by adjusting the
phase alone, and indeed phase shaping can accomplish many tasks, including the
production of series of short pulses with variable delays. For this purpose, phase-
only shapers are sufficient, such as deformable mirrors that adjust the phase of
different spectral components by introducing sub-micron delays. The “Dazzler” is
a commercial acousto-optic pulse shaper that relies on the spectral selectivity of a
programmable periodic Bragg reflector, and therefore does not require dispersing
gratings [12, 13].
Another property that influences the selection of an appropriate pulse shaper is
the refresh rate. Acousto-optic gratings are transient but can only be refreshed at the
speed of sound, and therefore inappropriate for continuous wave or high repetition
rate applications. On the other hand, they are ideal for applications where a different
pulse shape must be selected on each pulse, up to repetition rates of several kilohertz.
Liquid crystals and deformable mirrors refresh much more slowly, but they make
good static programmable masks, which can therefore be used for continuous wave
applications.
5.6 Learning Feedback Algorithms
An experimental protocol analogous to Optimal Control Theory is called “learning

feedback.” The explicit suggestion for this was, not surprisingly, made in a theory
paper, by Judson and Rabitz [14]. In learning feedback, a target observable is
selected for optimization. For example, one might desire that the pulse shaper be
adjusted to take an unknown input pulse and readjust the phases to produce the
shortest possible output pulse, subject only to the bandwidth limitation imposed
by Fourier’s theorem. Alternatively, one might want to discover the optimal pulse
shape to optimize a complex task in molecular or chemical physics such as a
specific dissociation or isomerization. We may or may not have some idea from
theory or previous experiments about the optimal pulse, but the point of learning
feedback is that such prior knowledge is not needed. The quantum system under
investigation can solve Schrödinger’s equation for us, if we give it the right pulse for
its interaction Hamiltonian. We therefore need an efficient search protocol. Several
have been proposed, such as searches using parameterisations of the pulse shape in
the time and frequency domain. Parameterisation by one or two parameters, such
as an expansion in order of dispersion, or simple use of overall amplitude, central
frequency and chirp, have limited ability for the discovery of new insights. On the
other hand, a large parameter space is almost impossible to search systematically.
To see just how seemingly hopeless the task is, consider the number of degrees of
freedom in a typical pulse shaper, with 256 different spectral amplitudes and phases.
If each phase can be adjusted with eight bits of precision, then there are 256256
different pulse shapes. That’s more than the number of protons in the universe.
The search could be streamlined by selecting an initial pulse and following the
fitness gradient. But with so many dimensions, even determining the gradient is
a challenge. Technical noise and other experimental limitations come into play.
Furthermore, there is no particular reason to think the problem is necessarily convex,
i.e. one where the optimal pulse can be found by following the gradient. This is
where evolutionary algorithms become useful.
A number of successful learning feedback protocols employ variations on evolu-
tionary algorithms. Such schemes are based on a map that contains the information
needed to construct the pulse. This “pulse DNA” is called the “genome” for the
pulse, and its individual pieces, the “genes” can be anything that is convenient for
the experimenter. For example, the pulse spectrum could be divided into N pieces,
and each piece assigned an amplitude and phase. These 2N pieces of information
compose the genome for that pulse. The specific encoding is relatively unimportant,
but it is necessary that any arrangement of genes within the 2N dimensional pulse
shape space corresponds to a pulse that can be produced in the lab and used to
perform a test on the physical system. Shown below, and in Fig. 5.12, are the steps
of the learning search:
1. Select a population of starting genomes. This is usually done at random, and this
step is only performed once. This population of genomes creates a population
of pulse shapes, which are the individual members of an initial pulse shape
population, Generation 0.
122 P.H. Bucksbaum
Fig. 5.12 Flow chart

showing a learning
feedback loop
2. Perform the experiment with each member of the generation, and record the
relative amount of the desired target state following each experiment. This
successful fraction is called the “fitness” of the corresponding pulse, since it
indicates its relative suitability.
3. Rank the genomes according to their fitness.
4. Now form the next generation in the learning feedback loop, by combining the
best traits of the previous generation. This step is one where all the improvement
in fitness occurs, and I will have more to say about it below.
5. Go back to step 2, and repeat steps 2–5 until the fitness is optimized.
The fact is that such a fitness directed search works extremely well. Much of the
success, however, comes from clever innovations in step 4 above, i.e. the selection
of a new generation base on the fitness ranking of the previous generation. The
selection method is called an “operator.”
5.6.1 Operators in Genetic Algorithms
The operator in a genetic algorithm converts a parent population into offspring

based on some kind of mathematical manipulation of the individual genomes. The
most common operators employed are crossovers and mutation, which generate new
pulse shapes using rules based on random statistics. Crossover operators create
offspring by sharing the genetic material of two (or more) parents. In a typical
implementation, one parent’s genome is cut in n-places (n-point crossover), creating
(n C 1) or more segments, often at a randomly selected point in the genome string.
Then a second parent’s genes are substituted for one or more of the segments.
A similar type of operator is the “average crossover,” which creates offspring whose
genes are the arithmetic average of the two parent genes in the same position
along the genome. One important difference between normal crossover and average
crossover is that the latter introduces new gene values to the population.
Mutation is also generally considered to be very beneficial in genetic learning al-

gorithms, because it introduces new genetic material, i.e. different values of spectral
amplitude and phase. This may either be insertion of a completely alien individual
into the population, or the replacement of some of the genes in parent genomes.
Operators could also be based on some physical knowledge of the system.
Examples include time-domain crossover, where the genome is a discretization
of E.t/ rather than E.!/. This can be more efficient in cases where the optimal
solution consists of discrete pulses, which are easy to describe in the time domain
but depend on more complicated phase functions in the frequency domain.
There are as many different operators as imagination can provide. Another
example is polynomial phase mutation, where the spectral phase is decomposed
into a polynomial expansion, and one order (cubic, for example) is replaced with a
mutated value.
The large number and variety of operators suggests that learning feedback is as
much an art as a science, but note that all of these variations are simply means to
arrive at an optimization more rapidly. Operators are “inside the feedback loop”
in the sense that a poor choice of operator may impede the progress to a solution,
but will generally not prevent that optimization. Nonetheless, an efficient algorithm
should find a way to utilize this variety.
5.6.1.1 Adaptive Operators
The learning feedback used to select individual pulses with high fitness can also be
used during the algorithm to select the most efficient operators. This technique is
called “adaptive operators.” In a typical implementation, several different operators
are used to create offspring. The particular operator for each individual is chosen
at random, but recorded by associating a genealogy with each individual. After
three generations, the genealogy of the most fitted individuals is a record of the
most efficient operators. The ensuing generations use this information to weight the
probability for using these more effective operators. The genealogy is examined in
every subsequent generation, and the probability for selecting operators is adjusted
to ensure that the most effective operators are used a higher fraction of the time
(Fig. 5.13).
5.6.1.2 Principal Control Analysis
One of the great strengths of learning feedback control is that it achieves a solution
without any prior knowledge of the Hamiltonian. Its efficiency does not depend on
this, nor to any great extent on the size of the control space. It is hardly more effort
to search a large space than a small one, since the search is fitness-directed, and
therefore tends away from unproductive regions or degrees of freedom. The number
of possible solutions in the control space may be huge, but the number of solutions
included in the search is not huge [16].
124 P.H. Bucksbaum
Fig. 5.13 The fitness for multiple operators plotted as a function of generation for a single
run of the learning algorithm while maximizing the fitness for a particular learning feedback
algorithm. This was a search to optimize the peak intensity of a pulse by adjusting its spectral
phase (Reproduced and adapted with permission from Ref. [15])
The price paid for this luxuriously large search space is that the solution may be
difficult to intuit, and it may be nearly impossible to discern the underlying physics
by examining the features of the optimal pulse. The fitness function maximum
may only depend on a few “essential” features of the control field, even though
these are not obvious in the spectral basis used for most control experiments. Other
unimportant features are just ornaments, so long as they do no harm.
This problem has been addressed by adapting a control analysis protocol bor-
rowed from the analysis of large statistical data sets, known as Principal Component
Analysis (PCA). The version adapted to control problems has been named Principal
Control Analysis [17]. PCA is based on the notion that all solutions with high fitness
should share common traits which can be found by examining details of the search
process itself.
The basic idea is that the control Hamiltonian for any particular pulse shape
H ŒE.xi / depends on a vector of control parameter settings xi that produce that
pulse shape. It should be possible to rewrite the Hamiltonian using a new basis
where the most important linear combinations of parameters are basis vectors. In
the old bases, the set of most important control directions forms a lower-dimensional
subspace, like a surface embedded in a cube (see Fig. 5.14). Each essential control
direction is a linear combination of the much larger basis of the control experiment.
Since the trial pulse shapes in the experiment were chosen specifically because
Fig. 5.14 Geometric model of the control Hamiltonian. The space of all pulse shapes is depicted as
a cube on the left. The optimal pulses lie on a lower dimensional space within the cube, here shown
as a surface. All pulse shapes on this surface are equally fit. The same Hamiltonian control space
is shown on the right, but now transformed to the essential control basis. Now the unimportant
degrees of freedom are no longer present, so that the optimal pulses all lie at a point. PCA is a
method to find these essential degrees of freedom (From Ref. [17])
they had the highest fitness, we can get a good sense of these control directions
by examining the control values in the learning search [18].
Principal Control Analysis investigates the covariance of the values of pairs of
genes in the set of pulse shapes used in the search. In other words, how much do
pairs of values vary together in a fitness directed search. The variance of ith gene in
the control parameter genome xi is:
!1=2
X
hxi i D xi2 n (5.18)
n
and the covariance is a square matrix:

2 3
c11 : : : c1m
6 7
cij D hxi xj i hxi ihxj i D 4 ::: : : : ::: 5: (5.19)
cm1 cmm
We want to find a new basis in which the variance of each control direction is
independent of the others. Clearly this is just the basis in which cij is diagonal:
2 3 2 3
c11 : : : c1m 1 0 0
6 :: : : : 7 6 7
4 : : :: 5 ! 4 0 2 0 5 : (5.20)
:
cm1 cmm 0 0 ::
126 P.H. Bucksbaum
The largest eigenvalues correspond to directions in the control space with the largest
variance. Since the search is directed by fitness, these are the directions of greatest
fitness improvement, and therefore correspond to the most important features of
the pulse for control. The eigenvectors of these eigenvalues then form the essential
control basis. Often there are only two or three large eigenvalues, indicating that
control can be established with only a few independent controls.
5.6.1.3 Most Correlated Feature Analysis
A closely related technique to PCA is Most Correlated Feature Analysis (MCFA).

In MCFA, we directly determine the features (directions) in the search space that
correlate best with fitness. Here we define a feature as any vector in the control
space that can have some fitness associated with it. The correlation of fitness f with
any projection of the searched pulse shapes onto an arbitrary feature a is:
haf i haihf i
RD
a f
P
N P
N
˛k k f ˛k k hf i
kD1 kD1
D (5.21)
a f
The feature with the highest fitness correlation has a particularly simple form in
the PCA eigenvector basis: Its components are given by:
hk f i hk ihf i

˛k D (5.22)
k
This is powerful, because it allows us to compute the pulse shape with the highest
correlation to fitness even though this specific pulse shape may never have been
produced in the search. Furthermore, since we know that only a few directions in
the PCA basis have high eigenvalues and therefore high sensitivity to the search
objective, therefore only the first few ˛ k are important.
A basis of most correlated features may be calculated iteratively by Schwartz
decomposition, i.e. subtracting the projection of the data onto the most correlated
feature from the data and repeating the MCF analysis. This basis can be used to
produce a simplified “essential” cut in the fitness landscape.
5.6.1.4 Multi-dimensional Data for Control
The fitness measurement in a learning control experiment is at least as important

as the pulse shaper. There is considerable flexibility in choice of a fitness criterion,
since the feedback loop process will move in the right direction for any measurement
that has a monotonic relationship to the target functional. However, the connection
between the raw signal and the fitness can be exploited to learn more about the
dynamics initiated by the control fields, and recent work in quantum control has
begun to focus on this.
5.7 Conclusion and Outlook
This chapter has introduced some of the basic concepts in the subject of quantum
control of small molecules. The original impetus for quantum control was to learn
how to use the coherent properties of lasers to accomplish arbitrary and selective
bond rearrangements in molecules, despite the fact that the molecular Hamiltonian is
far too complicated to solve directly, and the number of coupled degrees of freedom
means that any solution will be nearly impossible to implement anyway.
The theory problem has been approached through optimal control methods,
which are essentially computational feedback protocols to iteratively solve complex
problems. On the experimental side, the learning feedback method overcomes
this complexity by using the molecule itself as an analogue computer, where the
experimental apparatus supplies the input and output registers, and the experimenter
is merely the programmer [14]. The ansatz here is that the molecule will solve the
problem for us, if we supply the right experimental protocol, and if we are persistent.
The current state of the field is far from the original goal of bond-selective
manipulation, but quantum control has had an important impact in several areas,
for example in ultrafast and strong-field physics, and ultracold atom physics. This
brief introduction has not gone into these applications, but now we mention a few
of them to provide an outlook for future work.
The theory of quantum control is extremely active. Fundamental issues such as
the dependence of controllability on the nature of the state space, or the topology
of the control landscape, are quite current [19]. Control in open systems, where
there is dissipation, is important to many applications. A particularly active area of
theoretical interest in this regard is quantum information.
Many of the concepts of quantum coherent control are closely related or
even derived from the far more established field of nuclear magnetic resonance.
Very sophisticated pulse shapes and feedback protocols are employed in magnetic
resonance experiments to obtain structure information on the atomic
0
scale [20].
The new field of attosecond science relies on strong (V/Å) laser field, which
can field ionise and subsequently re-scatter a molecular electron, producing high
harmonics (HHG). Control of these quantum processes could been used for
detecting atomic-scale structure and transient processes in small molecules [21].
Finally, quantum control concepts are also beginning to have an impact in the new
x-ray free electron lasers. Control schemes are needed there to prepare molecules
for interrogation by intense x-rays [22].
128 P.H. Bucksbaum
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Chapter 6
Femtosecond Optical Frequency Combs
Thomas Udem, Ronald Holzwarth, and Theodor Hänsch
6.1 Introduction
Frequency can be measured with by far the highest precision of all physical
quantities. In the radio frequency (rf) domain (! < 2 100 GHz), frequency
counters have existed for a long time. Almost all of the most precise measurements
in physics have been performed with a counter that uses an atomic clock as a time
base. To extend this accurate technique to higher frequencies, so called harmonic
frequency chains have been constructed since the late 1960s [1, 2]. In such a chain
nonlinear elements produce frequency multiples (harmonics) of a given oscillator to
which a subsequent oscillator is phase stabilized. Repeating this procedure several
times makes it possible to multiply a reference radio frequency to much higher
frequencies. Electronic phase locked loops [3] can be used to stabilize the relative
phase of any kind of oscillator, even lasers, provided their intrinsic stability is
sufficient so that there is no need for very rapid frequency corrections. It was not
until 1996 that visible laser light was first referenced phase coherently to a cesium
atomic clock using this method [4].
The disadvantage of these harmonic frequency chains was not only that these
set-ups could fill several large laser laboratories at once, but that they could only
measure a single optical frequency. A new solution to that problem emerged at the
end of the 1990s through the use of a mode locked laser that is capable of producing
pulses of light in the femtosecond domain. Such a laser emits a very broad spectrum,
comparable in width to the optical carrier frequency. The laser stores this light pulse
inside its resonator for an almost unlimited duration emitting a copy of the stored
pulse after each round trip time T that typically lasts between 1 and 100 ns.
In the frequency domain, a train of short pulses from a mode locked laser is the
result of a phase coherent superposition of many continuous wave (cw) longitudinal
T. Udem () • R. Holzwarth • T. Hänsch

Max-Planck Institute fur Quantenoptik, Hans-Kopfermann Straße 1, Garching 85748, Germany
e-mail: thu@mpq.mpg.de

130 T. Udem et al.
cavity modes. These modes form a series of frequency spikes that is referred to as
a frequency comb. The individual modes can be selected by phase locking other
cw lasers to them. The modes are remarkably uniform, i.e. the frequency difference
between adjacent modes is constant across the comb. This strictly regular arrange-
ment is the most important and defining feature of a frequency comb and was first
demonstrated in [5]. The optical frequencies ! n of the comb may be expressed as:
!n D n!r C !CE (6.1)
Because a periodic signal in the time domain corresponds to a periodic structure in

the frequency domain with inverse spacing, the modes are separated by ! r D 2/T.
They are enumerated by the mode number n 105 : : : 107 with a zero mode that
is arbitrarily chosen in Eq. 6.1 such that the frequency offset ! CE lies in between 0
and ! r . The latter is due to the difference of the phase and group velocity inside the
laser cavity and shifts the modes from being simple harmonics of the repetition rate
as will be shown in the next section.
6.2 The Optical Frequency Comb
To derive the frequency comb properties as detailed by Eq. 6.1, it is useful to

consider the electric field E(t) of the emitted pulse train [6–8]. If the pulses were
exact time shifted copies, E(t) D E(tT), a simple Fourier transformation would
yield a strictly periodic spectrum with a mode separation of ! r and a vanishing comb
offset ! CE D 0. However, this is not what is expected in a real laser. Due to intra-
cavity dispersion the group and phase velocities of each pulse do not match. This
causes the carrier wave to continuously shift with respect to the pulse envelope. This
is illustrated in Fig. 6.1. The copies of the pulses that exit the laser cavity through the
output coupling mirror after each round trip show a discrete pulse-to-pulse carrier
envelope phase shift of '.
The difference between phase and group velocity is determined by the dispersion
properties of the cavity as a whole. The remarkable property of Kerr-lens mode
locked lasers is that this difference is the only effect of intra-cavity dispersion
on the pulse train. Higher order dispersive terms that would continuously deform
the pulse are strongly suppressed so that the pulse can circulate undistorted for a
virtually unlimited time. This long-term coherence is the intrinsic reason for the
very precise uniformity of the mode spacing expressed by Eq. 6.1. In fact, as of
today no deviation from this expression has been detected [9, 10].
To analyse this situation, the pulse train is most conveniently written as an optical
carrier wave propagating with its phase velocity at ! c modulated by the pulse
envelope functionA(t) that propagates with its group velocity. The observed strict
periodicity of the latter is expressed by demanding A(t) D A(tT) with the pulse
repetition time T D 2/! r . To obtain the spectrum of the pulse train the envelope
can be re-expressed through a Fourier series:
6 Femtosecond Optical Frequency Combs 131
Fig. 6.1 Three consecutive pulses of the pulse train emitted by a mode locked laser and the
corresponding spectrum. There is a pulse-to-pulse phase shift of ' between pulses because
the pulse envelope propagates at the group velocity and the optical carrier wave at ! c moves with
the phase velocity. In the frequency domain this corresponds to an offset frequency ! CE D '/T
that shifts the comb as a whole from the strict harmonics of ! r
X
E.t/ D A.t/e i !c t C c:c: D Aq e i.!c Cq!r /t C c:c:; (6.2)
q
where Aq are Fourier components of A(t). This equation represents a comb of laser
frequencies with spacing ! r that is shifted as a whole from the harmonics of ! r , just
as in Eq. 6.1. The only difference being the numbering of modes which clearly is a
matter of convention.
In a real laser the pulses may be chirped, i.e. their carrier frequency varies across
the pulse. Such a chirp from a laser is periodic with the repetition rate otherwise the
carrier wave would increase/decrease indefinitely. For this reason the chirp can be
accounted for by allowing a complex envelope function A(t) leaving all of the above
arguments valid.
Another obvious difference of the above model to a real laser is that neither
the carrier wave nor the pulse train will be free of noise. To take this into account
the Fourier series in Eq. 6.2 has to be replaced by a convolution of the carrier
wave spectrum with the spectrum of the pulse envelope [11]. Provided the carrier
wave possesses a suitably narrow line width and the noise in the repetition rate is
low enough (to maintain the comb structure), individual modes can be separated.
This condition is easily satisfied, even with a free running mode locked laser. The
noise of the frequency comb will be taken out by phase locked loops that stabilize
both frequencies in Eq. 6.1 relative to a precisely known radio frequency reference.
132 T. Udem et al.
Usually only slow fluctuations of the repetition rate have to be compensated

with a small servo bandwidth (100 Hz) while more bandwidth is required to
phase lock the carrier-envelope frequency. In the phase locked condition the above
derivation remains valid when averaging over timescales much longer than the
inverse bandwidths of the phase locked loops.
It is easy to show that a grating with sufficient resolution to resolve the frequency
comb would be at least as large as the laser cavity, which appears unrealistic for
most mode locked lasers. Fortunately for frequency metrology applications it is not
necessary to resolve individual modes in the optical domain as detailed below.
The spectral width of femtosecond light pulses produced by a mode locked laser
can be significantly broadened by virtue of self-phase modulation in optical fibres.
This process, whose origin stems from an intensity dependent refractive index, is
described in the time domain by the optical Kerr effect (the same effect used to
operate a Kerr lens mode locked laser). After propagating a length l, the intensity
dependent refractive index n(t) D no C n2 I(t) leads to a self-induced phase shift of:
ˆ.t/ D n2 I.t/!c l=c; with I.t/ D jA.t/j2 : (6.3)
This time dependent phase shift leads to a frequency modulation that is pro-
portional to the time derivative of the self-induced phase shift ˚(t). Self-phase
modulation modifies the envelope function according to:
A.t/ ! A.t/e i ˆ.t / (6.4)
Because ˚(t) has the same periodicity as A(t), the comb structure of the spectrum,
as previously derived, is not affected.
In an optical fibre this process is more efficient than in bulk material, even though
the nonlinear coefficient in fused silica is comparatively small. This is because the
fibre core carries a high intensity over an extended length. However, dispersion
causes the pulse to broaden temporally so that the large peak intensity required for
this process can diminish significantly after only a few cm of propagation length.
Optical fibres that partially compensate that effect can be much more effective
in terms of spectral broadening. In the near infrared one can use the zero group
velocity dispersion of silica around 1.3 m, but the zero dispersion wavelength
can also be shifted in fibres by properly designing the refractive index profile
of the waveguide. In addition, doping can be used to increase the non-linearity.
This approach is generally used with fibre based mode locked lasers that operate
in this spectral region. For wavelengths around 800 nm, where titanium sapphire
mode locked lasers operate, photonic crystal fibres (or micro structured fibres)
may be used. Such a fibre uses an array of air holes that surround the fibre core
and run the length of a silica fibre to change its effective dispersion [12]. Some
lasers can reach an octave spanning spectrum even without using external self-
phase modulation. This became possible with intra-cavity self-phase modulation
[13] and/or by using extremely broad band intra-cavity mirrors [14]. These titanium
sapphire lasers are an advantage because they avoid problems associated with
mechanical stability when coupling into the tiny core of a photonic crystal fibre.
(For a more comprehensive discussion of nonlinear effects in optical fibres, see the
Chaps. 8 and 9 by Dudley et al. and Wadsworth respectively).
6.3 Self-Referencing
To stabilize the frequency comb it is first of all necessary to generate the two radio
frequencies ! r and ! CE that make up the frequency comb in order to stabilize them
relative to some radio frequency reference. Whereas the pulse repetition frequency
may be detected anywhere in the laser beam, the generation of the carrier envelope
frequency is more involved. In fact, generating ! CE became possible only in 1999
by beating different harmonics (3.5th and 4th) of different components of the
comb [15]. This first demonstration involved considerable effort to generate the
required harmonics, but the task simplified dramatically with the availability of
octave spanning frequency combs [9, 16, 17].
The so called f-to-2f self-referencing technique uses a group of modes
from the low frequency end of the comb around nL ! r C ! CE that is frequency
doubled in a nonlinear crystal and super imposed with another group of
modes around nH at the high frequency end of the comb. This generates
signals at the difference frequency of two optical waves on a photo detector:
2(nL ! r C ! CE )nH ! r C ! CE D (2nL nH )! r C ! CE .
These beat frequencies are created for all possible combinations of nL and nH
that lie within the bandwidth of the photo detector. One can restrict the number
of signals to precisely one by using an rf low pass filter. If this filter has a cut off
frequency of ! r /2, only the beat note at ! CE , belonging to all combinations with
2nL nH D 0, remains. The octave spanning comb ensures that these combinations
exist, i.e. that the modes nL and nH with nH D 2nL are active modes of the comb
with non-vanishing power. A typical set-up for f-to-2f self-referencing sketched
in Fig. 6.2. Knowing both, ! CE and ! r , means that frequencies of all modes are
known using Eq. 6.1 and may be used for optical frequency measurements. This is
accomplished by creating another beat note ! b between an unknown laser at ! l and
a nearby mode of the comb. The frequency of that laser can then be determined
by ! l D n! r C ! CE C ! b . The mode number n may be determined by a coarse
measurement of ! l , say with a wavelength meter or by repeating the measurement
with slight variations in ! r [18].
By adjusting the resonator length, through a piezo-electric transducer, the
repetition rate can be adjusted. For a typical laser the intrinsic stability of the
repetition rate is good enough such that the attainable bandwidth of the transducer
is by far sufficient to keep it in phase with a reasonable rf reference. The other comb
parameter (! CE ) is determined by both the phase and group velocity of the stored
pulse. It was shown that for a soliton like laser such as the Ti:sapphire Kerr-lens
mode locked laser, that the group and phase velocity depend on the peak intensity
of the stored pulse [19]. Therefore, one can adjust the pulse-to-pulse slippage of
134 T. Udem et al.
Fig. 6.2 The carrier envelope offset frequency ! CE that displaces the modes of an octave spanning
frequency comb from being exact harmonics of the repetition rate ¨r is measured by frequency
doubling some modes at the “red” side of the comb and beat them with modes at the “blue” side.
The top figure sketches one possible implementation of this f-to-2f self-referencing method while
the bottom part shows what happens in the frequency domain
the carrier envelope phase, and thereby ! CE , by controlling the average laser power.
For titanium sapphire and fibre mode locked lasers this can be done by controlling
the power of the pump laser. The two controls are not completely independent.
However, any modification of the frequency that maintains the comb properties
can be characterized by a fix-point corresponding to the unaffected mode [20]
(which possibly lies outside the active frequency comb). It turns out that the fix-
point with respect to pump laser modulation is usually located close to the centre of
the frequency comb [20, 21]. For this reason using the pump power and the cavity
length always changes both degrees of freedom of the frequency comb. Keeping the
servo bandwidths for ! r as low as possible and for ! CE as high as possible usually
de-couples the two servo systems. Having the two phase servo systems operational
ensures that, by virtue of Eq. 6.1 and the large integer n, the radio frequencies ! r
and ! CE are phase coherently up-converted to the optical region.
To investigate the integrity of the frequency comb and to check for possible sys-
tematic deviations several tests have been performed. Two independent frequency
combs have been found to agree at a level of 5.1 1016 [9] and 1.3 1017 [10].
Even though Doppler shifts due to mirror motions caused by thermal expansion set
in at this level, no systematic shifts have been found yet.
6.4 Applications
By virtue of Eq. 6.1 a frequency comb can be used to phase coherently connect the
radio frequency domain with the optical domain. This is enabled by the large integer
n ( 105 : : : 106 ) that the pulse repetition frequency is multiplied with. As sketched
in Fig. 6.3, three interesting frequency conversions are possible with the frequency
comb. Locking the radio frequencies ! r and ! CE to a Cs clock references the
optical modes to the SI second in order to determine optical transition frequencies of
interest with the utmost precision. Using the repetition rate as a reference to stabilize
the carrier envelope frequency allows the division of an optical frequency down to
the radio frequency domain or to directly measure optical frequency ratios [22].
Fig. 6.3 Frequency

conversions possible with the
frequency comb. (Top) by
locking to radio frequencies
! r and ! CE of the comb to a
Cs atomic clock the optical
modes ! n may be used to
determine atomic transition
frequencies in units of Hz.
(Middle) In reverse operation
the comb is referenced to an
optical transition extracting a
pre-scaled radio frequency
copy. (Bottom) Phase
coherent optical-optical
frequency ratios are also
measured
136 T. Udem et al.
6.4.1 Optical Clocks
An optical clock consists, like any other clock, of an oscillator that defines the ticks
in time and a counter that keeps track of these cycles. In a cesium clock for example
the ground state hyperfine splitting of the 133 Cs atom is used. An electronic counter
advances the second hand every time the counter has completed 9,192,631,770
oscillations. This number was chosen when the SI second was redefined in 1967
to match with the previous definition. If we look at the history of time keeping,
and compare clocks as different as sun dials, pendulum clocks and quartz clocks,
it is obvious that they become more accurate as the oscillation frequency increases.
This is simply because a higher oscillation frequency slices time into smaller pieces.
Since the end of the 1950s the cesium 9.192 : : : GHz oscillator has been used. With
the frequency comb one has a simple tool to count up 5 orders of magnitude faster.
In fact, it can be shown that any clock limited by quantum noise will possess an
instability that decreases with the inverse of the averaging time and is proportional
to the observed line width divided by the transition frequency [23]. For practical
reasons one cannot simply pick a transition with an arbitrary small line width,
because this will at the same time increase the required observation time. For this
reason optical oscillators have been envisioned to be used in clocks for a long time.
For a well-chosen transition the systematic uncertainties may be as low as 1018 .
After tremendous advances in laser spectroscopy in the 1980s and 1990s that
ultimately resulted in trapped atom and ion standards (see for example [24, 25]),
a reliable optical clockwork mechanism was the missing piece for completion of
the all-optical atomic clock. The best of these new clocks are now surpassing the
accuracy of even the best Cs fountain clocks. To demonstrate such a performance a
comparison with another optical clock is required. Recently T. Rosenband and co-
workers at NIST have succeeded with such a measurement that shows the stability
of two optical clocks based on single trapped Hg and Al ions. The frequency ratio
measured as sketched at the right hand side of Fig. 6.3 has been found to be
reproducible within 5.2 1017 [26].
An overview of the evolution of radio frequency (cesium) clocks versus optical
standards over the last decades is presented in Fig. 6.4. Whereas the cesium atomic
clocks have steadily improved by an order of magnitude per decade, the optical
frequency standards have significantly gained in pace since the introduction of
frequency combs. Because existing optical clocks are still quite complicated devices
and different atoms and ions are still being investigated it will be some time before
a particular transition is chosen to re-define the SI second.
6.4.2 Basic Research
The possibility to readily count optical frequencies has opened up new experimental
possibilities. High precision measurements on hydrogen have allowed for improved
Fig. 6.4 Evolution of radio frequency (rf) and optical frequency standards. The rf standards gain
quite steadily an order of magnitude per decade (straight line). The optical measurements are on a
different slope since they can be conducted with frequency combs. Now the best optical clocks are
outperforming even the best cesium atomic clocks [26]
tests of the predictions of Quantum Electrodynamics (QED) and the determination

of the Rydberg constant [27]. As the simplest of all stable atomic systems, the
hydrogen atom provides the unique possibility to confront theoretical predictions
with experimental results. The narrowest line starting from the 1S ground state in
hydrogen is the 1S-2S two-photon transition with a natural line width of 1.3 Hz at a
transition frequency of 2,466 THz. To explore the full capacity of this transition, a
frequency measurement is imperative. In fact this task motivated the construction
of the first self-referenced frequency comb [15, 17]. At that time the frequency
comb was referenced to a transportable cesium fountain clock from BNM-LPTF
(now LNE-SYRTE), Paris [28]. Through the introduction of the frequency comb,
the uncertainty of this measurement became limited by the spectrometer to about
two parts in 1014 . Lacking a suitable laser cooling method is a particular problem
for the light hydrogen atom so that the limits are currently set by how well the
velocity and angular distribution of the 6 K atomic beam is understood.
A new measurement in 2003 did not yield an improvement but was useful to set
an upper limit on a possible small variation of the fine structure constant as well
as the strong interaction constant [29]. The question of slowly drifting fundamental
constants was first raised in 1937 by P.A.M. Dirac, where he speculated that such a
drift would be synchronized with the expansion of the universe [30]. The traditional
way to search for such a phenomenon is to determine the value of say the fine
structure constant as it was effective billions of years ago by astronomical or
geological observations. With frequency combs it is now possible to compete with
138 T. Udem et al.
these observations with laboratory measurements, even though the look back time
is typically about 9 orders of magnitude smaller.
In the first round of these experiments the hydrogen 1S-2S [29], and transitions in
single trapped Hg [31] and Yb ions [32] were used by comparing them with the best
cesium atomic clocks. Since the 133 Cs ground state hyper-fine splitting is determined
by the nuclear structure, the strong interaction mainly scales the reference frequency.
It is therefore impossible to distinguish variations of the fine structure constant
from the strong coupling constant using a single atomic system. If such a variation
actually takes place, grand unified theories predict a synchronization of the various
coupling constants [33] such that it may cancel out from the observation of a
single system. Fortunately H, YbC and HgC possess different dependences on the
fine structure constant so that the contributions of the coupling constants can be
separated [34].
An even better way to detect a drifting fine structure constant is to observe optical
frequency ratios as discussed in Sect. 6.3. The above mentioned comparison of the
HgC and AlC optical clocks provides this unique possibility. After only 1 year
of observation this frequency ratio puts the smallest limit of 5.2 1017 year1
on the drift of the fine structure constant [26]. Remarkably, the precision of these
laboratory measurements makes it possible to reach the same sensitivity within
a few years of monitoring, that astronomical and geological observations require
billions of years of look back time. In the laboratory, systematics can be investigated
or challenged, and if in doubt, experiments may be repeated given the relative short
time intervals. So far none of the laboratory tests have been able to detect a temporal
variation of the fine structure constant. Geological and astronomical observations
may be affected by systematic uncertainties that lead to partially contradicting
results (see Refs. [35–37] for results on quasar absorption and [38, 39] geological
data). It should however be pointed out that laboratory tests operate on a different
epoch than astronomical and geological observations so that the data may not be
directly comparable.
A very important application for improved atomic clocks in basic research could
be to test or refine general relativity which still poses one of the major problems
in physics as it refuses proper quantization. It is possible that small, yet undetected,
deviations from the classical theory of gravity give valuable hints on how to proceed
with quantization.
6.4.3 High Harmonics and HeC
Laser-like pulsed emission of very short wavelength can be produced with a method
generally referred to as high harmonic generation (HHG) [40]. For this purpose one
focuses infrared femtosecond pulses in a gas target employing its extreme nonlinear
response when subject to intensities exceeding 5 1012 Wcm2 . In most HHG
experiments a nozzle emitting a jet of noble gas atoms is placed near the focus of an
amplified femtosecond pulse train to produce up to the 1,000th harmonic [41] in a

nearly diffraction limited laser like beam that travels co-linearly with the generating
pulse train.
We expect that each of these harmonics is made up of a frequency comb so that
direct frequency comb spectroscopy [42–45] should be possible in the extreme ultra
violet. It can be shown that for a two-photon transition driven with the modes of a
frequency comb, the modes will add up pair-wise to the same transition energy. In
this case, the effective laser line width corresponds to the line width of a single mode
while the transition probability is calculated from the power of all modes [46]. There
are several conditions for the HHG radiation to be useful for this type of high res-
olution spectroscopy: (i) the HHG process must be coherent in order to support the
mode structure of a frequency comb; (ii) the mode spacing (repetition rate) must be
sufficiently large so that the ion or atom can separate out individual modes. (iii) the
power of the HHG radiation has to be sufficient to obtain a detectable transition rate.
Even though there is significant evidence to suggest the process of HHG is fully
coherent [47], the existence of a frequency comb has been verified only up to the 7th
harmonic at 153 nm [48]. The second condition states that the pulse repetition rate
must be much larger than the observed line width. This requirement is contradicting
the requirement for high peak intensities necessary to drive HHG. A large pulse
repetition rate distributes the limited average power on many pulses per second.
A promising route to solve this issue is to generate HHG’s inside an enhancement
resonator. Harmonics with up to 110 MHz repetition rate have been generated this
way [49, 50]. In the first generation of these setups the extracted extreme ultraviolet
(XUV) power was not sufficient to be useful for high resolution laser spectroscopy.
Thanks to the highly non-linear character of the process, moderate improvements
have already led to orders of magnitude more power, which is now getting into a
regime with a useful excitation rate say at the 1S-2S transition in HeC [51, 52].
This very sharp transition takes place with two 60 nm photons. Since HeC is iso-
electronic with the hydrogen atom, its energy levels can be calculated with the same
accuracy by using QED. Besides demonstrating an all new spectroscopy tool, HeC
can solve several experimental and theoretical problems currently encountered with
hydrogen. Because of the very unfavourable laser wavelengths, hydrogen has never
been laser cooled. Due to its small mass even at a temperature of a few Kelvin,
it is difficult to keep the hydrogen atoms inside the laser beam for more than one
millisecond. This gives rise to a set of systematic problems. Since HeC is charged
it may be held in a trap extending to virtually unlimited interaction times. Trapped
He ions can further be sympathetically cooled through interactions with other ions
such as MgC for which cooling lasers are readily available.
On the theoretical side, contributions to the energy levels with higher powers
of the nuclear charge Z will generally allow a more sensitive test of QED. The
Lamb shift corrections scales in lowest order as Z4 with the Z6 terms currently
under consideration. For this reason the same interesting physics is investigated at
significantly lower resolution by going from hydrogen to HeC [53].
140 T. Udem et al.
6.4.4 Astronomical Frequency Combs
In connection with the search for a variation of fundamental constants, optical

frequency measurements are useful for comparing the properties of celestial objects
with samples on Earth. To detect extra-solar planets a powerful method has been to
measure the periodic Doppler shift modulation due to the recoiling motion of the
orbited star [54–56]. These recoil velocities are rather small unless a massive planet
in close orbit around a light-weighted star is considered. This is the reason why
mostly “hot Jupiters” are among the roughly 500 extra-solar planets detected so far.
The lightest of those planets possesses about two Earth masses in a very close orbit
of only 3.1 days period [57].
To find an Earth-Sun like system, i.e. a habitable planet, one needs to measure a
velocity amplitude of only vE D 9 cm.s1 with a period of 1 year. This corresponds
to a Doppler shift modulation of vE /c D 3 1010 . Converted to visible radiation of
say 500 THz, this requires a resolution of 150 kHz and the same reproducibility
after half the orbital time.
Spectral lines from atoms and ions from interstellar clouds, and the Fraunhofer
lines of stars, are subject to strong line broadening of the order of several GHz due
to collisions and their thermal motion. These lines can be measured with telescopes
like the 3.6 m telescope of the European Southern Observatory that is equipped with
a very stable spectrometer (HARPS) [58]. Given the rather broad lines, the required
spectral or velocity resolution can be obtained by using the statistics of many lines
observed simultaneously. For calibration, the rather irregular line spectrum of Th-
Ar lamps have been used so far. Using a frequency comb instead for this purpose
appears to be the optimum tool, both in terms of providing an equidistant dense
calibration and for allowing long-term reproducibility that goes well beyond the
typical lifetime of an individual spectrometer [54]. The latter property derives from
the possibility to reference to a precise clock. In this case even a simple GPS
disciplined rubidium clock suffices for the required 3 1010 reproducibility to
detect Earth-like extrasolar planets.
The main challenge for this frequency comb application has been to reach a
sufficient mode spacing of about 10–20 GHz such that the individual modes can
be resolved by a precision astronomical spectrometer. Increasing the resolution
of the latter would involve more spectral bins or photo detectors (pixels) such
that corresponding increase of the total dark current prevents the observation of
faint objects. As this is not a workable option for the astronomers, methods for
generating combs with a large mode spacing are required. However, increasing the
pulse repetition rate reduces the achievable peak power which then makes it difficult
to spectrally broaden the comb. Filtering the frequency comb with external cavities
with a free spectral range that is a harmonic of the pulse repetition rate has been
proposed and used for this purpose [54, 59–61]. Residual dispersion of these filter
cavities lead to non-equidistant mode spacing, that again limit the spectral coverage
of the filtered comb. Advanced Yb doped fibre based systems are now reaching the
position to combine all this [62].
An alternative route might be to use a miniature Ti:sapphire laser that is capable

of generating 10 GHz pulse trains. Recently, such a laser has been demonstrated
by A. Bartles and co-workers [63], and even though the peak power of this laser
was somewhat low, the authors where able to broaden it spectrally beyond an
octave. While this is an important achievement, fibre lasers may be more suitable
when continuous unattended operation is required [64]. However, currently it is
challenging to obtain the very large repetition rates with fibre lasers.
In the long term, precision astronomical spectroscopy might help to resolve
one of the biggest puzzles of our times. So far the cosmic expansion is only
derived from snap shots of red shift distributions among the galaxies – assuming
the validity of general relativity for its interpretation. In this way, accelerated
expansion rather than a slowing down, as expected from attractive gravity, has
been proclaimed. A mysterious form of invisible energy with repelling gravity has
been devised as the cause. This so called dark energy does not yet show up in any
other context, so independent verification of the accelerated expansion rate would
be of great importance. Frequency comb calibrated spectrometers could become
accurate enough to measure the proposed variation of the expansion rate in real
time. However, centimetre per second Doppler resolution that can be tracked over a
decade would be required [56].
6.4.5 Direct Frequency Comb Spectroscopy
Employing individual modes of a frequency comb for direct excitation of a narrow

band transition is possible [65] but shows no practical advantage as compared to
the use of a single mode laser. However, there seem to be two exemptions where
direct frequency comb spectroscopy does have practical relevance. As detailed
above, frequency combs may be converted to the XUV where no single mode laser
exist. Another useful application of direct frequency comb spectroscopy is to record
rich spectra, say of molecules, with all modes at once. There are several ways to
achieve this.
The multi-heterodyne method uses two frequency combs with a slightly differ-
ent mode spacing ' r [66, 67]. Superimposing the two combs generates radio
frequency beat notes at n ' r where n counts the modes relative to a stitching
frequency at which both combs coincide. In this way the combs spectra are
multiplied and compressed by a factor ' r /! r . The radio frequency component
uniquely identifies the modes and therefore the optical frequency. Using selective
absorption by transmitting one of the combs through a sample and comparing the
radio frequency signal with and without it yields the optical spectrum of the sample.
Besides the built-in calibration, the dual comb method offers another advantage
over conventional absorption spectroscopy with incoherent white light illumination.
A frequency comb is the only “white light source” than can be coupled into a cavity
of proper length in order to resonantly enhance the intensity. This feature can be
142 T. Udem et al.
Fig. 6.5 Very short pulses driving a very non-linear process such as high harmonic generation
close to the short wavelength cut-off. If the intensity and/or the non-linearity is well chosen such
that it sets in at a certain threshold, a “cos” pulse will produce a spectrum that is periodic with the
infrared carrier frequency because the threshold is reached twice per pulse (left). In contrast the
“sine” pulse (right) produces a single isolated harmonic pulse that is much shorter than an optical
cycle of the infrared driving pulse [73]
used to increase the sensitivity for trace gas analysis by coupling the probing comb
into the sample holding cavity and applying the multi-heterodyne method with the
transmitted light [68].
Non-resonant intra-cavity ring down spectroscopy has been used for a long time
to enhance sensitivity. With the introduction of the frequency comb this method has
been extended to operate simultaneously on many optical frequencies at once [69].
Adjusting the mode spacing of the enhancing cavity to be an integer ratio
(say 100:101) of the combs mode spacing, allows pre-selection of every 100th
mode from the comb. This means that a simple low resolution grating is capable
of resolving the transmitted modes. By scanning the cavity length this cavity
successively resonates with sub groups of modes very much like a Vernier calliper
in the frequency domain [70]. This method combines a simple set-up with only one
frequency comb, the possibility to (sequentially) resolve individual modes of the
comb and the high sensitivity of cavity enhanced sensing.
6.4.6 Carrier Envelope Phase
The application of frequency combs has also enabled advances in another field as
it allows the possibility for stabilizing the carrier envelope phase [71]. According
to Fig. 6.1 a pulse train with a vanishing ! CE has a fixed phase of the carrier with
respect to the envelope. This means that all the pulses have the same electric field.
With the technique of self-referencing this can be readily accomplished. However,
even though the electric field transients of the pulses are identical in this case, it is
unknown what value the carrier envelope phase actually assumes upon stopping its
pulse to pulse slippage.
To detect the value of the carrier envelope phase, very short pulses that drive
processes which depend on the electric field in high order are used. Figure 6.5 shows
two extreme values of the carrier envelope phase that correspond to a “cos” and a
“sine” pulse. Close observation of the field transients reveals that the peak electric
field slightly depends on the carrier envelope phase. In addition the duration of the
optical carrier cycle changes slightly due to the steep pulse envelope when measured
say between two field maxima. These effects are largely enhanced if the pulses are
short and can be detected using HHG’s or above threshold ionisation [72].
Two important aspects are realized from this: For “cos” driving pulse, the high
harmonic pulse is much shorter than one cycle of the generating field. So by
stabilizing the carrier envelope phase to the proper value (“cos” drive pulses), single
isolated attoseconds could be produced for the first time [74]. Secondly the high
harmonic spectrum reveals whether the carrier envelope phase has been fixed at the
proper value or not. A “sine” drive pulse creates two high harmonic pulses per laser
pulse, that have almost, but not quite the same, time separation given by the carrier
frequency. For this reason the spectrum shows well separated harmonic peaks even
at the shortest wavelength that are generated. In contrast to that, a “cos” produces a
shifted harmonic spectrum that loses its periodicity in this region. This is because it
belongs to a single isolated attosecond pulse [73].
Not only that the detection and stabilization of the carrier envelope phase allowed
the production of attosecond pulses, it also allowed to completely recover the
electric field transients of ultra-short pulses. The work in that direction relied
on measuring the pulses autocorrelation which, together with the determination
of the carrier envelope phase via spectral analysis of high harmonics, allows the
calculation of the field transient [74]. A more direct measurement uses cross
correlation between attosecond pulses generated the way described above with the
driving pulses. In this way the field transient of the latter can be sampled with a
temporal resolution significantly shorter than one optical cycle [75].
6.5 Conclusions
Optical frequency combs provide a phase coherent link between the radio frequency
domain and the frequency domain of lasers. This possibility enabled precise
determination of atomic and molecular transition frequencies. In addition, optical
atomic clocks are realized by using a frequency comb as a clock work mechanism.
Optical frequency combs have also found numerous other applications as described
in this contribution.
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Chapter 7
Ultrafast Material Science Probed Using
Coherent X-ray Pulses from High-Harmonic
Generation
Stefan Mathias, Henry C. Kapteyn, and Margaret M. Murnane
7.1 Introduction
X-rays represent one of the most powerful tools for understanding molecules and
materials at the nanoscale, uncovering important information related to magnetism,
photochemistry, materials, biology, nanoscience and many other areas of science
and technology.
To date, research in x-ray science has predominantly been carried out using
synchrotron light sources, with great success due to the power of x-rays as probes
of matter. Their short wavelengths provide access to elemental absorption edges, to
site-specific chemical and magnetic states of matter, as well as ultrahigh spatial
resolution imaging capabilities. In recent years, advances in laser science have
made it possible to generate x-ray pulses at the femto- and attosecond frontiers
using either free-electron laser facilities (“4th generation” synchrotron) or high-
harmonic up-conversion of femtosecond lasers (also see Chap. 3 by Marangos
and Malte Oppermann). The availability of such ultrashort x-ray pulses paves the
way for a completely new generation of experiments that can capture the coupled
dynamics of elementary excitations in materials. Ultrashort x-ray pulses can access
the fundamental interactions between charge, lattice, orbital, and spin dynamics in
real time, which eventually determine the intrinsic physical limits at which, for
example, a phase-transition in a correlated-electron material occurs, the magnetic
state of a material can be switched, or a chemical reaction on a surface evolves.
In biology, these new ultrafast x-ray light sources promise to capture the most basic
processes, such as charge transfer, photosynthesis or cell death, on their fundamental
time- and length-scales, using the “diffraction before destruction” concept.
S. Mathias () • H.C. Kapteyn • M.M. Murnane

JILA, University of Colorado and NIST, Department of Physics, 440 UCB, Boulder,
CO 80309, USA
e-mail: smathias@physik.uni-kl.de

150 S. Mathias et al.
The promise of ultrafast x-ray science has fuelled the impressive free-electron
laser facilities that are coming online worldwide, which deliver high energy bursts
of femtosecond x-rays to capture an image in a single shot. Recent breakthroughs
in coherent x-ray generation using high-harmonic up-conversion provide a com-
plementary small-scale light source that is ideal for the study of ultrafast material
science [1–3]. The key enabling advance for generating bright compact ultrafast
x-ray sources was the extension of phase-matching techniques from the extreme
ultraviolet region (XUV) to the soft x-ray region to photon energies >1 keV.
The goal of this chapter is to give a short introduction to high-harmonic
generation (HHG) (Sect. 7.2), followed by a summary of recent breakthroughs in
using HHG for the study of ultrafast material science (Sect. 7.3). The experiments
discussed in this book chapter were all carried out using photon energies in the
40–100 eV photon energy range, where high flux HHG beams are readily available
at high (> kHz) repetition rates. In the near future, however, equally high photon flux
table-top high-harmonic beamlines will be available at photon energies up to 1 keV,
which will have great potential impact on material science research, as discussed in
Sect. 7.4 “Conclusions and Outlook”.
7.2 Ultrashort Coherent Soft X-ray Beams

from High-Harmonic Generation
High-harmonic generation (HHG) is the most extreme nonlinear process observed

to date, where atoms driven by a strong laser field can emit high harmonics of
the fundamental driving light, up to some cutoff photon energy. Using intense
visible or infrared femtosecond light pulses to drive the process, a broad spectrum
of harmonics spanning the water window and even keV photon energies can be
generated [4–6].
An intuitive and physical picture of HHG was developed in quantum simulations
by Kulander et al. [7, 8], and then formulated in a classical trajectory picture by
Corkum [9]. In this picture, high harmonic emission results as a consequence of
a three-step electron rescattering process (Fig. 7.1) that occurs when an atom is
ionised in a strong laser field. In the first step, the Coulomb barrier binding the
electron to the atom is suppressed by the strong laser field, resulting in a quantum
tunnel ionisation process. Once free, during the second step the electron accelerates
in the laser field, gaining kinetic energy. Finally, the third step occurs after the laser
field reverses, when the electron recollides with the parent ion. If the electron was
ionised at the correct time (phase), there is a finite probability that it will recombine
with that ion and emit any excess kinetic energy gained in the field as a high-energy
photon.
To calculate the average kinetic energy of the electron driven by the laser field,
one can simply estimate the energy of a free-electron oscillating in a laser field of
wavelength œ (or frequency ¨) and intensity IL , which is given by the ponderomotive
potential Up IL œ2 . Depending on the exact time (phase) of the laser field when
7 Ultrafast Material Science Probed Using Coherent X-ray Pulses. . . 151
Fig. 7.1 Illustration of the three-step model for high-harmonic generation. (Top) An electron
tunnels from the atom in the presence of a strong laser field that suppresses the Coulomb potential
binding the electron to the atom. The free electron is then accelerated by the laser field and can
recombine with the parent ion, emitting a high-energy photon. (Bottom) Quantum representation
of the recolliding electron wavepacket in HHG (Reproduced and adapted with permission from
Ref. [1])
the electron tunnel ionises, the energy it gains can range between 0 and 3.17 Up –
the latter representing the maximum kinetic energy that the electron can gain if it
ionises just after the peak of the laser field. As a result, when the electron recombines
with its parent ion, the energy of the highest cutoff harmonic that can be emitted is
given by:
„!cut off D Ip C 3:17Up (7.1)
where Ip is the ionisation potential of the atom.

Fig. 7.2 Phase-matched HHG spectrum generated in 20 Torr of Ar using a waveguide geometry
(Reproduced and adapted with permission from Ref. [14])
Ionisation of the medium occurs as a sequence of bursts near the peaks of the
field, and occurs twice per cycle. This leads to harmonic emission that occurs as a
series of short attosecond bursts in time, corresponding to a series of odd harmonics
of the fundamental laser (¨, 3¨, 5¨ etc.) in frequency space, up to the cutoff photon
energy „!cut off . Furthermore, harmonics are emitted only during a fraction of the
laser pulse when the atom is ionising and very rapid changes in the time-dependent
dipole moment are present. As a result, the total HHG pulse duration is considerably
shorter than the driving laser pulse [10, 11]. For sufficiently short driving pulse
duration, the highest harmonics can be confined primarily to a single attosecond
burst [11, 12]. Moreover, when phase matching is taken into account, that specifies
the time interval during which emission from a large number of atoms is coherently
combined, bright harmonic bursts as short as 200 attoseconds can be generated in
the XUV region of the spectrum, even using 15 fs lasers at a wavelength of 0.8 m
[13]. Even shorter HHG pulses, below 10 attoseconds, can be generated in the soft
x-ray region of the spectrum using mid-infrared driving lasers with pulse durations
of tens of femtoseconds (Fig. 7.2) [1].
The development of sub-30 fs solid-state lasers based on Ti:sapphire was
instrumental to the first practical applications of HHG [15–17]. The efficiency of
HHG increases as the driving laser pulse duration is reduced, because the required
laser pulse energy is less in order to reach ionising intensities of 1014 Wcm2 . In
addition, as explained below, phase-matching conditions are dramatically improved
by using 20 fs laser pulses, resulting in efficient generation of harmonics with
efficiency 105 per harmonic per pulse in the XUV region of the spectrum.
For phase matched frequency upconversion, the driving laser and the generated
harmonics must travel with the same phase velocity, to ensure constructive addition
of the generated HHG field from a macroscopic number of atoms over an extended
propagation distance. In the XUV, the real part of the refractive index is close
to unity, and thus high harmonics travel at phase velocities close to c (the speed
of light in vacuum). In the case of the laser field, the refractive index of neutral
atoms is greater than unity, corresponding to a phase velocity less than c for the
laser. However, the gas medium is being ionised by the laser as it propagates.
Since the index of refraction of a plasma is less than unity, the phase velocity
of the driving laser is dynamically changing, from less than c on the leading
edge of the pulse to greater than c once significant ionisation of the medium
occurs. In general, there will be a finite time interval during which phase matching
of HHG can occur, provided that the required HHG photon energy (i.e. laser
intensity) is reached while the medium is still only weakly ionised (<5 % for
Argon gas).
A very successful approach to phase matching of HHG that scales to keV photon
energies and that results in perfectly spatially coherent beams, uses a gas-filled
waveguide as the generation medium [1, 2, 18–21]. Laser beams well above the
ionising intensity can be reliably guided in a gas-filled hollow waveguide without
damage to the structure. In this case, phase matching occurs when the phase
velocities of the laser and HHG are equal, or equivalently, the difference in their
k-vectors of propagation is zero:
k.t/ D qk! kqw

2
u11 L 2
q P Œ1 .t/ ın .t/N r
at m e L C kquant um .t/;
4 a2 L
(7.2)
In Eq. (7.2), q is the harmonic order, u11 is the lowest-order waveguide mode
factor, L is the centre wavelength of the driving laser, a is the inner radius of the
hollow waveguide, P is the pressure, is the ionisation fraction, re is the classical
electron radius, Natm is the number density of atoms at 1 atm, ın is the difference
between the indices of refraction at the fundamental and harmonic wavelengths,
and kquantum , often negligible in a waveguide geometry, accounts for any Gouy or
other phase shifts in the focus. The gas-filled hollow waveguide ensures that a well-
defined spatial mode builds up over an extended propagation distance and allows for
careful control to engineer the phase-matched conditions including the wavelength,
gas pressure, gas species and waveguide size. To achieve phase matching, the gas
pressure is tuned so that the neutral and plasma index of the gas balances the
waveguide dispersion. The waveguide geometry thus makes it possible to obtain
optimal conversion efficiency in a wide range of conditions in a compact geometry
(i.e., 1 m beamline) using pulse energies readily obtainable using kHz and higher
repetition-rate lasers. The waveguide geometry has been used in all experiments
following in Sect. 7.3 of this book chapter.
Expanding the useful range of photon energies that can be generated using HHG
depends on continued progress in understanding how to phase match the process.
Dramatic progress has been achieved in this area in the past 2 years, with the
demonstration of mid-infrared phase matching in the keV region [1, 2, 22]. Other
approaches include new techniques for quasi phase matching using periodic struc-
tures [23–25] or counter-propagating light pulses [26] that periodically modulate
the emission and can thus facilitate coherent signal build-up at higher energies
than is possible through simple phase matching. The most successful approach
to date is to generate HHG using longer wavelengths which allows for full phase
matching of the HHG process at very high multi-atmosphere pressures, enabling
conversion efficiencies into the water window and keV region of the spectrum
predicted to be comparable to those currently obtained in the XUV [1, 2]. These
future developments will continue to expand the capabilities of HHG based ultrafast
material science research.
7.3 Recent Material Science Experiments with Coherent

High-Harmonic Radiation in the XUV Regime
7.3.1 Correlated-Electron Materials
Correlated-electron materials exhibit many-body interactions that are key to under-

standing macroscopic effects such as superconductivity. Their specific properties
are determined by the interactions between electronic charges, electronic spins,
atomic orbitals, and the crystal lattice. In a series of pioneering experiments that
have just been possible in recent years, ultrafast spectroscopies have helped separate
the different timescales involved in the different interactions, and as a result, uncover
a more fundamental understanding of correlated-electron materials [27–36].
One of the most powerful static techniques for the study of correlated-electron
materials has been angle-resolved photoemission spectroscopy (ARPES) using
synchrotron radiation in the XUV regime. ARPES can directly map the electronic
structure and Fermi surface topology of a material. Also, many-body effects can be
extracted from photoemission data, since the photoemission intensity is proportional
to the single-particle spectral function.
Consequently, combining ultrahigh time-resolution with ARPES [33, 37–41]
opens up many new frontiers in materials science. A pioneering experiment showing
the potential of time-resolved ARPES for the study of correlated-electron materials
was carried out by Schmitt et al. [33], who measured the photo-induced charge-
density wave phase transition in TbTe3 in real-time. Until recently, however, such
time-resolved ARPES experiments used ultrafast laser-pulses in the visible and UV
regime (up to 6 eV). In order to take full advantage of the power of the ARPES
technique in a time-resolved experiment, higher energy photons in the XUV spectral
region are needed [14, 38, 40–42].
Figure 7.3 shows a schematic of the photoemission and angle-resolved pho-
toemission technique. An electron in the initial state Ei absorbs a photon of the
Fig. 7.3 Photoemission and conservation of the k-vector component parallel to the surface
energy h and is promoted into the final state Ef . The final kinetic energy Ekin of the
photoelectron is measured with the electron energy analyser and is given by:
Ekin D h W jEb j (7.3)
where W is the work function of the material, and Eb the binding energy of the initial
state with respect to the Fermi-level EF (Fig. 7.3a). Because of the 2D translational
symmetry parallel to the surface, the wave-vector component parallel to the surface
is conserved (see Fig. 7.3b):
kEjjex D kEjji n C G
E jj (7.4)
Where kEjjex and kEjji n are the parallel wave-vector components of the electron outside
and inside the crystal, respectively, and G E jj a reciprocal lattice vector of the crystal.
The kE? component normal to the surface is not conserved during transmission
through the surface. The wave-vector component parallel to the surface outside the
crystal, which is determined from known experimental parameters,
r r
2me p 2me
kEjjex D h jEb j W sin.‚/ D Ekin sin.‚/ (7.5)
„2 „2
therefore directly yields the internal wave-vector component kEjji n for a kinetic energy
Ekin and emission angle of the photoemitted electron. Modern electron analysers
measure the photoelectron energy and emission angle in parallel, and thus directly
map the electronic structure E(kjj ). Figure 7.3c depicts the dependence of the
photoelectron emission angle on the wave-vector component kEjjex parallel to the
surface for three different photon energies and a typical workfunction of W D 5 eV.
For the lowest photon energy, h D 6 eV (and Ekin D h W D 1 eV), which can
conveniently be reached by frequency quadrupling the output of a Ti:sapphire
ultrafast laser system in two beta-barium-borate crystals, the maximum kEjjex wave
vector that can be measured (for a theoretical emission angle of 90ı ) is about
0.5 Å1 . In order to reach typical Brillouin-zone boundaries at about 1.5 Å1 , which
is crucial for the study of ultrafast correlated-electron physics in materials, higher
photon energies and therefore XUV and soft x-ray pulses from HHG or free-electron
laser (FEL) sources are needed.
The first experiment that implemented and used the capabilities of time-resolved
ARPES with HHG XUV light for the study of correlated-electron materials was
recently carried out by Rohwer et al. [40]. Here, the charge-density wave state
in the potential excitonic insulator 1 T-TiSe2 was disrupted on a timescale as
short as 20 fs. The photo-induced phase transition was monitored using ARPES,
enabling real-time stroboscopic imaging of the electronic band dispersions E(kjj ) at
large momentum, in the vicinity of the first Brillouin zone. The transition metal
dichalcogenide 1 T-TiSe2 undergoes a (2 2 2) charge-density wave (CDW)
phase transition below a temperature of 200 K. The transition is accompanied
by a periodic lattice distortion, where the real-space unit cell doubles its size in
all three directions. In momentum space, the dimensions of the Brillouin zone
are correspondingly halved, and this effect is most prominently resolved using
conventional APRES, by monitoring the consequent backfolding of the Se 4p bands
at the Brillouin zone boundary (M -point). Figure 7.4 (from Ref. [40]), top left,
shows the ARPES intensity map of 1 T-TiSe2 recorded with HHG XUV pulses in
the charge-density wave phase. The photoemission intensity in the vicinity of the
M -point is due to the backfolded Se 4p bands (“Folded Se 4p”) in the CDW phase,
and it is this signature that is used to track the ultrafast photo-induced vaporization of
the charge-density long-range order in the material. Figure 7.4b–e shows snapshots
of the electronic structure as a function of delay between the 32 fs infrared pump-
pulses, and the sub 10 fs XUV probe pulses. When pump and probe pulses overlap
(b), the Ti 3d band is filled with hot electrons. These transiently generated free
Fig. 7.4 Tracking the photoinduced transition by femtosecond time-resolved ARPES [40]. (a)
ARPES intensity map of 1T-TiSe2 recorded with high- harmonic XUV pulses in the CDW phase
(temperature T D 125 K). (b–e) Time-resolved ARPES snapshots at increasing pump (infrared)–
probe (XUV) temporal delays (pump-pulse fluence, 5 mJ/cm2 ). (f) Photoemission transients of the
folded Se 4p band for different infrared excitation fluences close to time zero. The infrared–XUV
cross-correlation signal, which has been determined from the laser assisted photoemission [40]
(LAPE) signal, is added. Inset, transients up to temporal delays of 3.5 ps (Reproduced and adapted
with permission from Ref. [40])
carriers then screen the Coulomb potential on femtosecond timescales, destroying

the charge-density periodic long-range order. The characteristic build-up time for
carrier screening in response to an ultrashort
ıp laser excitation is the plasma oscillation
period, £pl , which scales with 1 n , with n the number of free carriers. In
the experiment, the number of generated free carriers, and thereby the speed of
the elimination of the charge-density wave state, was controlled by the pump-
pulse fluence (Fig. 7.4f). The fastest phase change occurred for a pump-fluence of
5 mJ/cm2 , on timescales as fast as 20 fs. This ultrafast phase change is much faster
than the material-characteristic oscillations of collective modes that are commonly
thought to limit the response times in photoinduced processes.
Very often electron states with large momenta govern fundamental electronic
properties in correlated-electron materials. The extension of time-resolved ARPES
into the XUV and soft X-ray regime by the use of HHG represents a major
breakthrough for future studies of ultrafast condensed matter physics in a wide range
of materials.
7.3.2 Ultrafast Magnetism
Magnetization dynamics on the femtosecond timescale, termed “femtomagnetism”,

was pioneered in 1996 by the work of Beaurepaire et al. who demonstrated that
the ferromagnetic phase of Ni can be destroyed by a femtosecond pump light pulse
on a sub-picosecond timescale [43]. Since then, studies of magnetism at ultrafast
timescales have addressed the important question of how fast magnetization can be
modified in a material, and what physical processes present fundamental limits to
this speed. Technically, the methods of choice for studying femtomagnetism are
spin- and time-resolved photoemission spectroscopy, as well as magneto-optical
studies. In the past, magneto-optical studies made use of either ultrafast lasers,
or x-rays from large-scale synchrotron x-ray facilities. Ultrafast lasers produce
short pulses (20 fs), making possible femtosecond time resolution [43]. However,
these studies lack element specificity, because light can only interact with the
electrons near the Fermi energy. X-rays from synchrotrons, on the other hand,
enable element-specific probes using photons with energy at the absorption edges
of ferromagnetic materials. However, the time resolution in these studies has to-
date been too slow (ps) to resolve the fastest magnetization dynamics. Due to this
limitation, significant efforts have been devoted to using laser pulses to ‘slice’ short
burst (<100 fs) of x-rays from a synchrotron light source [44], and some pioneering
femtomagnetism experiments have been carried out in recent years [45, 46]. A
complementary method to sliced x-rays from a synchrotron light source and ultrafast
x-ray pulses from FEL has recently been presented by La-o-vorakiat et al. who
combined coherent ultrafast XUV pulses from HHG with a transverse magneto-
optical geometry [47].
Magneto-optical effects lead to a magnetization dependent modification (polar-
isation, ellipticity, intensity) of transmitted and reflected light from the magnetic
material. The physical origin of the magneto-optical effect lies in the influence of
exchange interaction and spin-orbit interaction on the transition probability between
initial and final states for the electrons that are excited by the incoming light. In
the so-called longitudinal and polar geometries (in-plane magnetization parallel to
plane of incidence, and out-of-plane magnetization parallel to plane of incidence,
respectively), linearly polarised light that is reflected from the magnetic material
shows a rotation of the polarisation plane (Kerr angle) and it becomes elliptically
polarised. In the transversal geometry (in-plane magnetization perpendicular to
plane of incidence), as used by La-o-vorakiat et al. the M-edge magneto-optical
effect results predominantly from spin-orbit splitting and the unfilled d-band spin
polarisation [48]. In this geometry, the reflected light shows a modulation of the
intensity depending on the magnetization direction of the material. Therefore, no
polarisation analysis and no circular polarised light is needed, which considerably
relaxes experimental requirements.
Taking the two reflection coefficients for the two magnetization directions for
p-polarised modes from [49], the normalized difference for the T-MOKE signal
is [50]:
" #
2"0 "2 sin 2i
A D Re 2 (7.6)
"1 cos i "0 "1 C "20 sin2
2
"1 and "2 are the diagonal and off-diagonal elements of the dielectric tensor,
respectively, and i the angle of incidence with respect to the surface normal.
Therefore, the T-MOKE is directly related to the off-diagonal permittivity tensor.
Figure 7.5 shows the measured T-MOKE asymmetry signal of a Permalloy
sample (using synchrotron light), which contains Fe and Ni atoms, in grey scale
as a function of energy and angle of incidence [51]. The asymmetry signal as given
by Eq. (7.6) shows highest asymmetry values for angles of incidence around 45
degrees. The Fe magnetic asymmetry signal is visible below energies of 60 eV,
while the Ni magnetic asymmetry signal appears above 60 eV, as expected since
the elemental M absorption edges are around 54 eV for Fe and 67 eV for Ni. In the
experiment by La-o-vorakiat et al. which was carried out using coherent XUV pulses
from HHG, the magnetism of a grating structure made of Permalloy (Ni80 Fe20 )
was investigated (where the grating structure was used to spectrally resolve the
harmonics) [47].
The recorded HHG spectrum with this setup is shown in Fig. 7.6, illustrating the
discrete harmonics diffracted from the Permalloy grating. The strong absorption at
72 eV is due to aluminium filters that are used to block the fundamental laser light
that is co-propagating with the harmonics. From this spectrum, it is clear that the
magnetic asymmetry can be mapped over the entire M-edge region of Ni ( 67 eV)
and Fe ( 54 eV).
After the sample was excited by an intense infrared pump pulse, the very short
(<10 fs) duration HHG light was used to probe the ultrafast demagnetization
processes – with element specificity for the first time. Initially, the ultrafast intense
Fig. 7.5 Variations of T-MOKE signal from a Permalloy film consisting of Fe and Ni as a function
of photon energy E and angle of incidence ™ [51] (Data courtesy P. Grychtol, R. Adam and C.M.
Schneider, Forschungszentrum Jülich, Germany)
Fig. 7.6 Experimental data showing the HHG spectrum (bottom, right axis) and measured
magnetic asymmetry (top, left axis) for different incidence angles. No asymmetry is measured
with s-polarised light. (Left to right) The vertical lines denote Fe, Ni and Al M-shell absorption
edge (Reproduced and adapted with permission from Ref. [47])
Fig. 7.7 Time-resolved measurement of the femtosecond laser-pulse induced demagnetization of

the Permalloy film by high-harmonic photons around the Fe (open square), Ni (full circle) M-edge
pump pulse coherently interacts with the electron and spin systems during the time
the laser pulse is incident on the material [52]. Thermalisation of the electron and
spin systems then takes place through incoherent scattering processes, resulting in a
subsequent reduction/re-orientation in the magnetization [43, 53–55]. The change
in asymmetry as a function of time after the IR pump pulse can then be used
to follow the demagnetization dynamics (see Figs. 7.6 and 7.7). As expected, the
Permalloy sample demagnetizes on a femtosecond timescale, with an exponential
decay time-constant of below 400 fs for both Fe and Ni in Permalloy. The time
resolution of this first proof-of-principle experiment was about 55 fs, limited by
the experimental geometry. In the future, by using a more-collinear pump probe
geometry and a shorter HHG pulse, unprecedented time-resolution for ultrafast
magnetic studies will be available, which may, e.g., enable the direct investigation
of ultrafast coherent magnetization dynamics [52].
The experiment by La-o-vorakiat et al. clearly demonstrates that T-MOKE with
XUV light from HHG provides an ultrafast, element-specific probe of the magnetic
state. Furthermore, the use of coherent HHG for probing magnetic materials
promises to combine ultrafast, element-specific magnetism with nanometre spatial
resolution (see Sect. 7.3.5), making it possible to answer important fundamental
and technologically relevant questions in ultrafast magnetism. Furthermore, the new
experimental capability presented by La-o-vorakiat et al. is useful in the context of
correlated-electron materials, where ferromagnetic and antiferromagnetic order are
parts of the rich phase diagrams of these materials.
7.3.3 Ultrafast Surface Dynamics
Understanding electron dynamics at surfaces is critical to optimizing catalysis,

electrochemical processes, molecular electronics, and solar energy conversion.
Because charge transfer happens on femtosecond timescales, and between specific
atomic sites in a molecular complex or on a surface, this research requires an
ultrafast and element-specific probe of the electronic state. Ultrafast x-ray pulses
from synchrotron slicing, free-electron lasers, and HHG can be used for these
experiments. The first pioneering work done with HHG in the XUV energy range
probed dynamics on surfaces [14, 56–62]. For a survey, see Ref. [14].
Here we discuss a recent ultrafast and site-specific measurement by Miaja-Avila
et al. that captured dynamics in Xe atoms absorbed on a Pt(111) surface [63]. In
this experiment, XUV light from HHG was used to excite a 4d core-hole in the Xe
adsorbate, and the direct photoelectrons and Auger electrons were monitored. In
the presence of an additional laser field, sidebands appear on the photoelectron and
Auger peaks due to the laser-assisted photoelectric effect (LAPE) [64]. By varying
the time delay between the XUV and laser pulses, the 4d core-hole lifetime of the
Xe adsorbate was extracted.
LAPE was first reported in gas-phase photoemission [65, 66], but for a long time
it was not understood that LAPE also occurred when a material was simultaneous
irradiated by XUV and laser fields [64, 67]. In LAPE, an atom is simultaneously
irradiated by XUV and an intense infrared light field. The presence of the infrared
laser modifies the normal XUV photoelectron spectrum. The effect can be described
as the simultaneous absorption or stimulated emission of one (or several) infrared
photons with the XUV photon. For many-cycle infrared pulses, the LAPE process
leads to discrete sidebands in the XUV photoelectron spectrum at energies corre-
sponding to multiples of the infrared photon energy. Few-cycle infrared pulses give
rise to the streaking of the electrons photoemitted by the XUV pulse by the electric
field of the laser light [68, 69]. Because of the instantaneous character of LAPE, this
effect is particularly useful for temporal characterization of XUV pulses. Figure 7.8
shows the characteristic d-states peak-like structure of the photoemission signal of a
Pt(111) single crystal in the vicinity of the Fermi-edge. In the presence of an intense
laser field, sidebands appeared in the Pt(111) photoemission spectrum that could
unambiguously be assigned to a LAPE process.
From a model fit to the photoelectron spectrum, it was possible to reconstruct the
LAPE response function, which is shown in the inset of Fig. 7.8. In comparison to
LAPE in the gas phase, surface LAPE benefits from the high density of target atoms
on a surface and can therefore be used to characterize lower-flux and higher-energy
XUV sources.
In a similar manner, the emission of an Auger electron from an atom can be
modified by an intense infrared laser pulse [63, 66]. In this process, an Auger
electron is first generated by the decay of a core hole created by the absorption
of an XUV photon (see Fig. 7.9). Subsequent absorption of an infrared photon
by this electron gives rise to sidebands, this time located next to the Auger peak
Fig. 7.8 Experimental observation of laser-assisted photoemission from a Pt(111) surface using
HHG light. The XUVCIR spectrum (solid line) shows a strong distortion around the Fermi
edge compared to the XUV-only spectrum (dotted line). This change is due to the appearance of
sidebands in the spectrum. The dashed line shows the fit of the XUVCIR spectrum by convolving
a LAPE response function with the XUV-only spectrum. The inset shows the LAPE response
function associated with the fit. The energy separation between the sidebands is equal to the IR
photon energy, as expected for surface LAPE [64, 67] (Reproduced and adapted with permission
from Ref. [64])
characteristic for the probed-atom species. By comparing the time evolution of the
LAPE response from the Pt substrate with the LAAD signal from the adsorbed
Xe, Miaja-Avila and co-workers measured the lifetime of the 4d core hole initially
created by the XUV pulse (see Fig. 7.10). This measurement was possible despite
the many complexities that result from using the metallic substrate such as above-
threshold photoemission, hot electrons, and space-charge effects. The extracted
lifetime of 7 ˙ 1 fs for the Xe/Pt 4d core hole was consistent with high-resolution
linewidth measurements of Xe in the gas phase [70], clearly validating the success
of this experimental approach. Although carried out in a simple model system of a
noble-gas atom physisorbed on a surface, this experiment paves the way to more
complex charge-transfer processes in surface-adsorbate systems, where complex
electron relaxation processes, which depend on the chemical environment, are
expected.
7.3.4 Thermal Transport from Nanoscale Interfaces
Understanding heat flow away from a nanoscale hotspot is important for our
fundamental understanding of phonon transport as well as for many areas of
nanotechnology. Applications include thermal management in integrated circuits
or in heat-assisted magnetic recording techniques for future hard-disk devices,
thermoelectrics or thermally-enabled cancer therapies. An optimal method for
Fig. 7.9 Ultrafast XUV and IR pulses are focused onto a Xe/ Pt(111) surface, where the kinetic
energy of the photoemitted electrons is measured by a time-of-flight detector. An electron from
the Xe N4 (4d) shell is ejected by the XUV, followed by filling of the core hole by an O2,3 (5p)
shell electron and ejection of a secondary (Auger) electron from the O2,3 shell. In the presence of
the IR beam, sidebands appear in the photoelectron spectrum of both Xe and Pt. By comparing the
sideband amplitude vs. time delay for the Pt and the Xe Auger photoelectron peaks, the lifetime of
the Xe 4d core hole can be extracted [63] (Reproduced and adapted with permission from Ref [63])
investigating nanoscale heat transport should be non-contact, non-destructive, and

employ better than picosecond temporal with nanometre-scale spatial resolution.
Ultrashort pump-probe measurements are therefore the method of choice, and the
use of short wavelength beams allows access to the required nanometre spatial
resolution.
Using XUV light pulses from HHG, a pioneering work on quasi-ballistic thermal
transport from nanoscale interfaces was recently carried out by Siemens et al.
[71]. The authors demonstrated experimentally how Fourier theory, which describes
heat transport as a diffusive process, breaks down and heat transport becomes
quasi ballistic as the size of a nanoscale thermal hotspots shrinks to a dimension
comparable to the phonon mean free path in the heat sink. As a consequence,
as compared with Fourier-law predictions, the energy transport away from the
heat source decreases significantly for nanoscale thermal hot-spots compared with
diffusive heat flow.
In the experiment by Siemens et al. an infrared pump pulse was used to heat
nickel grating structures with 20 nm height and linewidths varying between 65 and
2,000 nm. The heat flow dynamics was then probed by diffracting HHG beams
from the nanogratings. Figure 7.11 shows the measured changes in XUV diffraction
Fig. 7.10 (a) Photoemission spectra from Xe/Pt(111) as a function of the time delay between the
IR and the XUV pulse. The time evolution of the redistribution of electrons due to the IR dressing
at the Pt d-band and at the Xe Auger photoelectron peaks can be observed. (b) The sideband height
for the Pt d-band (grey curve) corresponds to a cross correlation between the XUV and the IR
pulses. The Auger sideband height (black curve) is shifted and broadened with respect to the Pt
d-band curve. A value of 7.1 ˙ 1.1 fs for the Xe 4d core-hole lifetime was extracted using these
data [63] (Reproduced and adapted with permission from Ref. [63])
as a function of time delay between the infrared laser pulse and the XUV probe
(solid black line). Upon cooling of the nanostructure as heat flows into the substrate,
the diffracted signal decays on picosecond-to-nanosecond timescales. Additionally,
Fig. 7.11 Normalized dynamic XUV diffraction signal for Ni lines on sapphire. The signal (solid
line) consists of a sharp rise owing to impulsive laser heating, a thermal decay owing to interfacial
thermal transport and an oscillation owing to surface acoustic wave propagation. The dashed and
dotted lines show the fit using the Fourier law for thermal transport in the substrate and either large-
scale interfacial resistance (dotted line) or a modified effective interfacial resistance (rEffective , units
of 109 K m2 W1 ), which accounts for ballistic effects from a nanoscale heat source (dashed
line) (Reproduced and adapted with permission from Ref. [71])
the signal shows rapid oscillations on a picosecond timescale because of surface

acoustic wave propagation in the nanostructure. The surface acoustic waves are
generated by the surface strain that is caused by the periodic heating process.
To analyse and interpret their results, Siemens et al. used a multiphysics model
including thermal transport, thermomechanics and Fresnel optical propagation (for
details see Ref. [71]). They parameterise the results of their model in terms of
the effective resistivity rEffective , which they fit to the time-resolved thermal decay
data, and which includes both conventional thermal boundary resistivity and size-
dependent ballistic effects in the substrate owing to the confined heat source.
Qualitatively, Siemens et al. show by modifying the model by Chen in [72], that
the quasi-ballistic heat transport term is expected to depend on the inverse of the
Knudsen number L/ƒ, with L the linewidth of the nickel stripes, and ƒ the phonon
mean free path in the substrate. For linewidths larger than the mean free path, the
resistivity predicted by the Fourier law dominates (Fig. 7.12, case for fused-silica).
For linewidths comparable or smaller than the mean free path, the Fourier Law
considerably under-predicts the resistivity, and quasi-ballistic heat transport must
be taken into account (Fig. 7.12, case for sapphire).
In this manner, Siemens and co-workers modified the extracted effective resis-
tivity by rEffective D rTBR C rBC , with rBC the ballistic correction being proportional
to /L. rTBR , the thermal boundary resistivity, is measured for very large linewidths
of the Ni nanostructures, where the Fourier law dominates. The deviation from rTBR
for smaller sized nanostructures, with L in the region of the mean free path of the
substrate, then shows deviations as rBC . Figure 7.11 shows this behaviour, where
the dotted line is the expected diffraction signal curve for Fourier law heat transport
only, and the dashed line is the best fit taking the modified rEffective into account.
Fig. 7.12 Measured effective thermal resistivity for nickel nanostructures of width L deposited on
fused-silica and sapphire substrates. The dotted horizontal lines show the large-scale resistivity
rTBR for data from the fused-silica and sapphire substrates. The dashed curves show model
predictions for the ballistic resistivity correction rBC ƒ/L, with ƒFS D 2 nm and ƒSa D 120 nm,
respectively (Reproduced and adapted with permission from Ref. [71])
Figure 7.12 summarizes the systematic measurement and analysis of different sized
gratings on different substrates. Siemens et al. could experimentally show and
reproduce the expected dependence of rBC on /L.
The experiment by Siemens and co-workers is the first direct and systematic mea-
surement of quasi-ballistic thermal transport effects from a nanoscale heated region,
an effect of very high importance for material science research and applications,
e.g., in nanoscale thermal transport in circuits, for heat-assisted magnetic recording,
and for other structures in nanotechnology. The key to this type of measurement
was the use of coherent XUV light from HHG, which enabled for the first time heat
transport measurements with the necessary temporal and spatial resolution.
7.3.5 Coherent Diffractive (Lensless) Imaging
Coherent lensless imaging with x-rays is currently one of the most promising
techniques for ultrahigh resolution imaging with broad applications in biology,
nanoscience, and materials science. In combination with a HHG light source,

lensless imaging further provides tabletop applications and the potential to study
ultrafast processes in atoms, molecules, and materials on their fundamental length
and timescales. The use of x-rays as a light source for microscopy enables a
general full-field nano-scale resolution imaging capability by the virtue of their short
wavelengths. Moreover, because of the presence of x-ray absorption edges in the soft
x-ray region, x-rays allow for elemental and chemical specificity, without the need
to label or section a sample. Previously, full field high spatial resolution imaging,
without labelling or sectioning a sample, was possible only using very large-scale
synchrotron or free electron laser sources.
Lensless imaging in combination with a coherent tabletop HHG light source
with a wavelength of 29 nm was first demonstrated in 2007 by Sandberg et al. who
initially achieved a resolution of about 200 nm [73]. Since then, spatial resolutions
down to 50 nm were achieved by the same authors by increasing the numerical
aperture of the microscope imaging system [73]. Ravisio et al. also demonstrated
single-shot imaging with a HHG light source in 2009 [74], while Raines et al.
have shown a three-dimensional reconstruction (“ankylography”) of the illuminated
object from two-dimensional diffraction data that was collected with an x-ray table-
top laser source [75].
In lensless imaging, x-rays illuminate the object and only the diffracted light
from the sample is collected with an x-ray CCD camera [76]. The imaging
elements in the optical systems are then replaced by a computerized phase retrieval
algorithm, which reconstructs the image of the object from the diffraction pattern.
Three preconditions must be met in lensless imaging: (i) the object must be
illuminated by a coherent wavefront; (ii) the object must be isolated; and (iii) the
scattered light must be collected with sufficient spatial resolution to oversample
the diffraction pattern so that it is recorded at a frequency higher than the Nyquist
frequency [77].
Figure 7.13 shows the experimental setup for lensless imaging using an ultrafast
coherent XUV HHG lightsource, from Sandberg et al. [73]. As described before,
HHG is generated in a phase-matched HHG lightsource, and residual longer
wavelength light is blocked with Al filters. A pair of multilayer mirrors is used
to monochromise the HHG light at a wavelength of D 29 nm. The samples are
held on a two-axis piezo stage, placed 2–4 cm from the camera, to optimally sample
the diffraction pattern and to capture the highest possible angle of diffraction for the
available flux. Furthermore, beam blocks of varying sizes are used to block out the
most intensive portions of the diffraction pattern to increase the dynamic range of
the recorded pattern beyond the dynamic range of the CCD camera. Figure 7.14b
shows the coherent XUV diffraction pattern (after curvature correction) from a 7 m
“waving stick girl” etched into a 100-nm-thick silicon nitride window, covered
with a 200 nm gold film electroplated on the sample. Figure 7.14c shows the
reconstructed image using the phase retrieval computer algorithm. A lineout of the
image (Fig. 7.14c) along the legs of the stick-figure demonstrates a resolution of
94 nm.
Fig. 7.13 Setup of the tabletop soft x-ray diffraction microscope. A coherent XUV beam is
produced by high-harmonic generation or by spatially filtering the emission from a capillary
discharge laser in an Ar-filled hollow waveguide. The beam is gently focused by a multilayer
mirror pair onto the sample, and the diffraction pattern is collected on an x-ray CCD. A moveable
beam block allows for brighter portions of the diffraction pattern to be blocked to avoid saturating
the CCD when acquiring the highest angle diffracted light. ROC, radius of curvature (Reproduced
and adapted with permission from Ref. [78])
In other work by Sandberg and co-workers, this oversampling phase retrieval

technique was combined with multiple reference Fourier transform (FT) holography
to demonstrate an ultimate resolution of 53 nm [79]. In FT holography (Fig. 7.15),
a coherent beam is focused onto a multiple reference FT holography sample, and
the coherent diffraction pattern, or the hologram, is detected in the far field on the
CCD. The spatial autocorrelation of the object is then retrieved by taking the squared
magnitude of the FT of the hologram. For the sample in Fig. 7.14, Sandberg et al.
achieved a resolution of 89 nm, very near to the theoretical limit 88 nm (which
is given by 70 % of the diameter of the 125 nm reference holes). However, in
combination with oversampling phase retrieval, the resolution of the retrieved image
could be significantly increased down to about 53 nm.
Most importantly, because the light source used is based on high harmonic gen-
eration, many applications are possible because bright (phase matched) harmonics
have now been demonstrated throughout the extreme ultraviolet into the keV region
of the spectrum. This will enable the same setup to be used to capture 3D images of
whole cells, for understanding dynamics and function in advanced materials, and for
magnetic domain or plasma dynamic imaging with unprecedented combined spatial
(<10 nm) and temporal resolution (<10 fs).
7.4 Conclusions and Outlook
The presented series of ultrafast x-ray condensed matter physics experiments with
HHG demonstrates the potential of these table-top phase-matched high-flux light
sources in material science research. In future, the combination and extension of
Fig. 7.14 Lensless imaging by using coherent high-harmonic beams at 29 nm. (a) Reflection
image of the sample using an SEM. (Scale bar, 1 m.) (b) Coherent soft x-ray diffraction pattern (in
transmission) after curvature correction (maximum momentum transfer of 0.134 nm at the edge of
the CCD). (c) Reconstructed image. (d) Lineout of the image along the legs (Inset), demonstrating
a resolution of 94 nm (Reproduced and adapted with permission from Ref. [78])
such experiments, e.g. to nano-ARPES, time-resolved ESCA (electron spectroscopy

for chemical analysis), x-ray absorption spectroscopy [80], and ultrafast magnetic
imaging, will comprise a powerful toolset for all areas of ultrafast condensed matter
physics.
Most important, while so far efficient high-flux phase-matched creation of
HHG was limited to the XUV regime, recent progress in HHG upconversion
technology promises ultrafast high-flux and high-energy x-ray sources even into
the water window and above [1, 2, 81]. Clearly, the most compelling aspects about
this development are the possibility to build low-cost (compared to synchrotron
facilities) and table-top x-ray beamlines all around the world. Furthermore, high-
energy, high-flux HHG beamlines are a perfect complement to the recent build-up
of large-scale free-electron laser (FEL) facilities.
Fig. 7.15 Multiple reference FT holography. A coherent high-harmonic beam with œ D 29 nm

illuminates a test pattern surrounded by five reference holes. The scattered light interferes and is
recorded on a CCD camera in the far field as a hologram (log scale). The spatial autocorrelation
of the object can be retrieved by taking the squared magnitude of the Fourier transform of the
hologram. A single subimage from the autocorrelation is shown (Reproduced and adapted with
permission from Ref. [79])
Acknowledgements We thank M. Aeschlimann, M. Bauer, C. La-o-vorakiat, A.V. Carr, L. Miaja-

Avila, M. Siemens, M. Seaberg, D. Adams, and T. Popmintchev for support and discussion. We
gratefully acknowledge support from the National Science Foundation, from the Department of
Energy and from the DOD NSSEFF program. S.M. acknowledges support from the European
Community’s FP7 under Marie Curie International Outgoing Fellowship GA 253316.
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Chapter 8
Ultrafast Nonlinear Fibre Optics
and Supercontinuum Generation
John M. Dudley, Rim Cherif, Stephane Coen, and Goery Genty
8.1 Introduction
Nonlinear fibre optics is a very mature field of research, and nonlinear propagation
effects have been studied under a wide range of conditions. Very good general
textbook treatments of the whole field as well as specialised monographs treating
particular aspects of the field exist and it is not the purpose of this chapter to fully
reproduce material that is covered more fully in other places. Rather the aim here is
to present a focussed treatment of the subject, concisely covering the most essential
aspects of the field in a self-contained way. A particular feature of the chapter will
be a brief review of the physics of supercontinuum (SC) generation in optical fibre
under different conditions. The term SC generation is generally used to describe
the case where (relatively) narrow-band incident pulses undergo extreme nonlinear
spectral broadening to yield a broadband spectrally continuous output.
SC generation in bulk media and fibres has been studied since the earliest work
in nonlinear optics and nonlinear fibre optics. The broadband spectral output of
SC generation has found numerous applications in many diverse fields including
spectroscopy and the design of tuneable ultrafast femtosecond laser sources. The
dramatic observation of SC generation in photonic crystal fibre in 1999–2000 led to
J.M. Dudley ()

Département d’Optique P. M. Duffieux, Institut FEMTO-ST, CNRS UMR 6174,
Université de Franche-Comté, Besançon 25030, France
e-mail: john.dudley@univ-fcomte.fr
R. Cherif
Cirta’Com laboratory, Engineering School of Communication of Tunis (Sup’Com),
University of 7th November at Carthage, Technopark El Ghazala, Ariana 2088, Tunisia
S. Coen
Department of Physics, University of Auckland, Private Bag, Auckland 92019, New Zealand
G. Genty
Department of Physics, Tampere University of Technology, Tampere 33101, Finland

178 J.M. Dudley et al.
a revolution in the field of optical frequency metrology, a story that has been well-
told elsewhere. In a telecommunications context, the spectral slicing of broadband
SC spectra has also been proposed as a simple way to create multi-wavelength
optical sources for dense wavelength division multiplexing applications.
There is clearly wide interest in understanding the complex process of SC
generation, but it seems at first sight very difficult because of the complex way in
which the different linear and nonlinear propagation effects can combine. But in fact
the essential features of the spectral broadening can be broken down into a number
of different contributing mechanisms and it is possible to present a reasonably
clear physical interpretation of the major spectral and temporal features observed.
A key element, however, relates to understanding the fundamental principles of
nonlinear fibre optics, and thus we must begin our description of SC generation with
a summary of the nonlinear and dispersive interactions that can occur when a light
pulse is injected in a dielectric waveguide. Our approach follows that in Ref. [1].
Note that this chapter represents a synthetic summary of a number of our previous
publications in this area, prepared with the specific aim of covering the content of
the lectures given by one of us (JMD) at the 66th Scottish Universities Summer
School in Physics, which was held at Heriot-Watt University in August 2010.
8.2 The Propagation Equation
The aim here is to summarise the theory that underlies the description of a
guided wave propagating in an optical fibre. We suppose firstly, that the transverse
component of the guided wave field can be decoupled from the time-varying
component along the propagation direction. Then if the electric field is written as:
E.r; t/ D 1=2 x ŒE.r; t/ exp.i¨0 t/ C c:c; (8.1)
(where x is a unit polarisation vector), the complex envelope E(r, t) can be expressed
as:
E.r; t/ D F.x; y/ A.z; t/ exp.i“0 z/; (8.2)
where A(z, t) is the envelope describing the evolution of the field, F(x, y) represents
the transverse field profile, and “0 D “(¨0 ) is the wavevector. Note that we are of
course neglecting (vectorial) polarisation effects here. On the other hand, recent
work has begun to develop a comprehensive treatment of this important problem
but this is outside the scope of this chapter. In any case, polarisation effects can be
neglected over quite a large range of experimental parameters. Also, the bandwidths
of ultrashort light pulses are generally sufficiently large that chromatic dispersion in
the material must be described with minimal approximation. The effect of dispersion
can be conveniently examined using a Taylor series expansion:
“.¨/ D “0 C “1 .¨ ¨0 / C 1=2 “2 .¨ ¨0 /2 C 1=nŠ “n .¨ ¨0 /n C (8.3)

8 Ultrafast Nonlinear Fibre Optics and Supercontinuum Generation 179
where “n D dn “/d¨n . The coefficient “1 D 1/vg , where vg is the group velocity of

the pulse and “2 D 1/vg 2 dvg /d¨ is the group velocity dispersion (GVD). Under
some special situations considering dispersion only up to “2 can be adequate, but in
general this is not the case and higher-order coefficients must also be included. An
important point to realise here is that if the light is propagating in a bulk material,
the group velocity dispersion can simply be calculated from the material Sellmeier
equation. However, if the light is propagating in a waveguide, the confinement
can significantly modify the dispersion away from the material value. It is this
possibility of “dispersion engineering” in optical fibres that makes them such a
useful platform to study a wide variety of propagation effects. As might be expected
on physical grounds, the contribution of waveguide dispersion is greater for cases
where the waveguide introduces tighter confinement, and it is this fact that has been
responsible for so much of the interest in dispersion control using photonic crystal
fibres (PCFs) as discussed in Chap. 9 by Wadsworth [2].
Due to the high transverse confinement of the guided mode, the field intensity
in a fibre can easily attain values of MW.cm2 and this leads to a range of
different nonlinear effects. In fibres, the most important effect is the third-order
Kerr nonlinearity that yields an intensity-dependent refractive index:
n D n0 C n2 I .t/; (8.4)
where n0 is the usual linear index, the intensity I(t) is expressed in W.m2 and n2 is
the material nonlinear refractive index.
There is some debate over what value of n2 should be used for optical fibres,
but for fused silica good agreement with many experiments is obtained using
n2 D 3.2 1020 m2 .W1 [1]. There is a need for further clarification here, however,
and it is to be hoped that as experimental techniques improve, some of the ambiguity
associated with the correct value of nonlinear parameter to use in fibres can be lifted.
The combined effects of dispersion and nonlinearity on a pulse with bandwidth
¨ << ¨0 are described in the absence of loss by the nonlinear Schrödinger
equation (NLSE):
@A ˇ2 @2 A
i C jAj2 A D 0: (8.5)
@z 2 @T 2
Here A(z, T) is the pulse envelope where T D t “1 z is time expressed in a

frame moving at the pulse group velocity (described as a co-moving frame) and
” D n2 ¨0 /cAeff is a nonlinear coefficient that depends on n2 as above but also on the
modal effective area in the fibre (Aeff ). Thus fibres that confine light more tightly in
the core exhibit a higher nonlinear coefficient. This particular form of the NLSE is
dimensional in that the normalisation of the amplitude (A) in the NLSE is such that
jAj2 gives instantaneous power in W (watts). This dimensional form of the NLSE is
often preferred by workers in nonlinear fibre optics as it allows characteristic powers
and length scales to be conveniently derived. Of course for analytic or mathematical
studies, a dimensionless form of Eq. (8.5) would be preferred. The relative effects
of dispersion and nonlinearity on propagation are often quantified in terms of
characteristic dispersion and nonlinear lengths LD and LNL defined as LD D T0 2 /j“2 j

and LNL D 1/”P0 where P0 and T0 are peak power and duration (at 1/e2 intensity
maximum) of the input pulse. Note the definition of T0 here; the pulse width is not
the full width at half maximum; a scaling factor must be used to relate the 1/e2 width
to the FWHM.
Analysing the solutions of the NLSE is the subject of a book itself, and even
interpreting numerical solutions can require quite sophisticated insights. Still, some
simple analytical solutions can be obtained with minimal effort. For example,
when the distance of propagation satisfies z LD and z << LNL , dispersive effects
dominate and the NLSE becomes:
@A ˇ2 @2 A
i D 0; (8.6)
@z 2 @T 2
which has the solution in the frequency domain associated with the development of
a quadratic spectral phase across the field spectrum.

Q Q i
A.z; / D A.0; / exp 2
ˇ2 .2v/ z ; (8.7)
2
Here is the frequency, the reciprocal Fourier variable of T. Note that the solution
(8.7) in fact describes a temporal equivalent of linear diffraction in space, and there
are many important equivalents between temporal propagation in fibres and spatial
diffractive effects (e.g. the imposition of a quadratic spectral phase by a modulator
is often referred to as a “time lens”.)
When the distance of propagation is such that z LNL and z << LD , nonlinear
effects dominate and Eq. (8.5) becomes:
@A
i C AjAj2 D 0; (8.8)
@z
with the solution now in the time domain associated with a nonlinear phase
modulation:

A.z; T / D A.0; T / exp i jAj2 z : (8.9)
It is important to fully understand the implications of the solutions (8.7) and (8.9).
A pulse propagating in the presence of only dispersion is associated with a spectral
intensity that remains invariant during propagation, whereas a pulse propagating in
the presence of only nonlinearity is associated with a temporal intensity profile that
remains invariant during propagation. But in general, both effects occur together,
and numerical techniques must be used to solve (8.5). A very straightforward
technique to achieve this is the split-step Fourier technique, where propagation
is considered in terms of multiple small increments that allow the separation of
dispersive and nonlinear effects. In this case, the analytic solutions we derived above
in (8.7) and (8.9) can be applied iteratively to propagate forward from some initial
condition to follow the evolution of an initial field.
Fig. 8.1 Numerical solution of the NLSE showing top: (a) fundamental soliton evolution and
bottom: (b) N D 2 soliton evolution.
Figure 8.1 presents the results of this technique used to study soliton solutions
of the NLSE. Stable fundamental soliton solutions exist when “2 < 0, and under
conditions such that the linear and dispersive effects are exactly balanced. This
is often termed the p
focussing regime of the NLSE. The form of the fundamental
soliton is: A(0,T) D P0 sech(T/T0 ) with the pulse parameters matched to the fibre
parameters through:
LD jˇ2 j
D N 2 D 1 thus P0 D (8.10)
LNL T02
The results shown in Fig. 8.1 use fibre parameters of dispersion “2 D

12.75 ps2 .km1 and nonlinearity ” D 0.10 W1 .m1 , typical of highly nonlinear
PCF at wavelengths in the operating regime of modelocked Ti:sapphire lasers [2].
For T0 D 30 fs and with the fibre parameters above, the corresponding peak power is
P0 D 142 W, and Fig. 8.1a shows the stable propagation of the fundamental soliton
solution where N D 1. Results are plotted in both the time and frequency domains.
Solutions for higher integral order N D 2, 3, 4, : : : describe higher-order solitons
that propagate periodically with period zsol D /2 LD (D 0.11 m for our case) and
Fig. 8.1b shows the periodic evolution for the case N D 2 using our parameters.
Note that the study of the periodic recurrence of higher-order soliton evolution can
be used as a convenient test to verify the fidelity of any numerical scheme used in
solving the NLSE.
8.3 From Solitons to Supercontinuum – Modelling

Considerations
The generation of spectrally continuous radiation arising from nonlinear propaga-

tion in fibres has been known since the 1970s. Fibre SC generation can occur under
a range of conditions and has been reported in standard silica fibre, highly nonlinear
Germanium-doped fibre and of course PCF. It is the latter case that we consider in
most detail here as it that which has attracted most attention because of the seminal
role that PCF SC generation played in the development of frequency metrology and
the award of the 2005 Nobel Prize. Of course, nonlinear optics in PCF continues
to attract attention because of new applications and the ever-increasing demand for
broadband sources in specific wavelength regimes [3].
SC generation in photonic crystal fibre has been reported under a variety of
experimental conditions – different pulse durations, peak powers and different
wavelengths of the pump relative to the fibre zero dispersion wavelength [4–6].
In many of these experiments, the spectral characteristics at the fibre output
appear at first sight quite similar, yet a more detailed analysis shows that the
characteristics of the temporal electric field can vary significantly as a function of
the particular choice of parameters. It is clear that the systematic optimization of
SC generation sources requires a more careful case-by-case consideration of the
underlying spectral broadening mechanisms. We present a brief overview of these
effects below.
It is useful in the first instance to broadly distinguish different regimes of
SC generation by contrasting “short” (femtosecond) versus “long” (picosecond,
nanosecond and continuous wave) pump pulses. We consider both these cases
here and illustrate the underlying dynamics by using numerical simulations in the
following sections of the chapter. In this case, however, the numerical modelling
must use a more sophisticated propagation equation to include both higher-order
dispersion and nonlinearity. To highlight its fundamental link with the classic
NLSE, this generalised NLSE (GNLSE) is often expressed in a time-domain form
as follows:
@A X k ˇk @k A
i C i
@z kŠ @T k
k2
0 1
Z1
i @ @
C 1 C A.z; T / R.T 0 /jA.z; T T 0 /j2 d T 0 A D 0 (8.11)
!0 @T
1
Here, the “k ’s are the higher-order coefficients of the propagation constant as

described above in Sect. 8.2 and the function R(T) is a time-domain operator
that describes the material nonlinearity. The @/@T derivative operator describes
the dispersion of the nonlinear response itself, an effect which is neglected with
the standard NLSE. Together with the inclusion of an appropriate number of
higher-order dispersion coefficients, this results in the GNLSE being valid over
very broad bandwidths and even down to pulses of one or two cycles [7]. But
here it is important to realise that just because the GNLSE describes the evolution
of an envelope, it does not mean that the envelope has to be “slowly-varying”. In
fact when one revisits the derivation of the GNLSE from Maxwell’s equations, one
realises that the transformation from the usual second-order differential propagation
equations of electromagnetism to a first order partial differential equation such as the
GNLSE is actually associated with a factorisation step that is equivalent to assuming
that the propagation is purely unidirectional. This is an important point that deserves
careful reflection [7].
Also of importance to fully understand is the form of the nonlinear operator:
R.T / D .1 fr /ı.T / C fr hr .T / (8.12)
The delta-function term here describes an instantaneous nonlinear response,

whereas the function hr (T) is the Raman response function of the silica core
that originates from the delayed reaction of the nonlinear polarisation to the applied
field (physically arising from nuclear motion). The fraction fr D 0.18 and the Raman
response for fused silica can be conveniently described by the following function:
12 C 22
hr .T / D exp.T =2 / sin.T =1 / (8.13)
1 22
with £1 D 12.2 fs, £2 D 32 fs [1]. Note that there are some subtle aspects of
normalisation in the way in which the Raman effect is included in the GNLSE; for
example the function hr (T) is normalised to have unity integral, yet the dimensional
Raman gain at the pump wavelength is included through the terms ” and fr , and
its wavelength dependence is included through the time-derivative term. (Recall in
this context that the Fourier transform of a time-derivative term is equivalent to
multiplication by a frequency operator, and thus we can see how a ¨/¨0 scaling can
multiply the strength of the nonlinear response term in the frequency domain form
of the GNLSE.)
8.4 Illustrating Supercontinuum Evolution
In this section, we consider the general features of SC generation with the aim of
discussing the general physical mechanisms involved and illustrating the different
features that can be observed in both the time and frequency domains. The cases
considered are SC generated by femtosecond pump pulses, SC generated by pump
pulses longer than several picoseconds, and SC generated in a particular class of
fibre with a convex dispersion profile where the flat spectral characteristics are
especially useful for telecommunications applications.
8.4.1 Femtosecond Pump Pulses
SC generation when using femtosecond pump pulses is dominated by soliton

dynamics. A straightforward way to understand the main features of SC gener-
ation in this regime is to first consider the case of pumping in the anomalous
dispersion regime, but close to the wavelength where the fibre GVD is zero.
Because of the low dispersion parameter, even modest pump powers under typical
conditions means that the input pulses are “seen” by the fibre as solitons of order
N D [LD /LNL ]1/2 >> 1, where LD D T0 2 /j“2 j and LNL D (” P0 )1 . The pulses upon
injection initially undergo the expected higher-order soliton evolution dynamics of
spectral broadening and temporal compression (seen in Fig. 8.1) but because the
real environment of a fibre is not the ideal soliton-supporting NLSE, the subsequent
evolution becomes perturbed [8]. Specifically, noise, higher-order dispersion and/or
stimulated Raman scattering all contribute such that the dynamics departs from the
recurrent behaviour expected of ideal high-order solitons and the pulses break up
through a process which is now generally referred to as “soliton fission”.
Using the inverse scattering transform of nonlinear differential equation theory,
it is possible to treat this problem analytically and show that each higher order
soliton pulse separates into N distinct fundamental soliton components. Although
some special cases can be constructed to see this ideal fission scenario occur,
in experiments it is generally the case that the same perturbations that induce
the breakup in the first place also modify the evolution of the ejected solitons
such that other processes develop and lead to the generation of additional spectral
and temporal structure on the propagating field. For example, the presence of
higher-order dispersion results in the ejected solitons shedding energy via the
generation of dispersive wave spectral components in the normal dispersion regime,
whilst the Raman effect with continued propagation leads to a continuous shift to
longer wavelengths through the Raman soliton self-frequency shift. In the most
classic regime, the former process generates the shorter wavelengths and the
latter process generates the longer wavelengths in the spectrum. Despite the large
wavelength shifts between the extreme edges of the spectrum, however, under some
circumstances, the group and/or phase velocities of the spectral components across
the SC can be the same. This opens up additional possibilities for interactions such
as the well-known trapping process between solitons and dispersive waves [6].
These processes of SC generation can appear at first sight very complex (indeed
intimidating) to understand. Things are not made any easier in experiments because
the rich dynamical evolution is certainly not apparent by simply measuring the spec-
trum at the fibre output. This is where numerical simulations can be so convenient
in unravelling or deconstructing the complicated dynamics of propagation.
The simulations below in Fig. 8.2 correspond to the case of pumping in the
anomalous dispersion regime of a PCF with the following parameters: sech2 pulses
of 50 fs duration (FWHM) and 10 kW peak power at 835 nm in a PCF with
zero dispersion wavelength around 780 nm. Further simulation details are given
in Ref. [6]. The figure contains a greyscale representation of the SC development,
Fig. 8.2 Greyscale representation of SC generation in the femtosecond regime
and highlights in particular the point of soliton fission, the generation of dispersive
wave (DW) radiation, and the continual spectral and temporal shifting of an ejected
soliton undergoing the Raman self-frequency shift (RS).
The initial phase of nonlinear evolution contributes very significantly to the
overall spectral bandwidth. It is often the case that it is the spectral extension
during this phase that results in the injected higher-order soliton “experiencing” the
perturbation of dispersion across its bandwidth. This perturbation ultimately leads
to its breakup. Cutting the fibre before the breakup point has been applied usefully
for applications in pulse compression, and we can apply insights obtained in this
previous work to aid in the practical study of SC generation. In particular, motivated
by studies aiming to optimise compression [9], we introduce a characteristic length
scale to describe the fission point, based on the distance at which the spectral width
of the initial soliton reaches it maximum value. This has been termed the fission
length and can be written approximately as Lfiss LD /N D (LD LNL )1/2 . Simulations,
such as those shown in Fig. 8.2, can be readily extended over a wider parameter
range, allowing the study of femtosecond propagation where the pump pulse is
in the normal GVD regime. In this case, results show that the initial spectral
broadening arises primarily from self-phase modulation (SPM) and can lead to a
spectrum that is significantly less structured than that associated with anomalous
GVD pumping. However, power levels generally required to achieve the same
bandwidth are lower when soliton dynamics are exploited. When pumping in the
normal GVD regime, but approaching closer to the zero dispersion wavelength, the
initial spectral broadening due to SPM transfers spectral content into the vicinity
of the zero dispersion wavelength and across into the anomalous dispersion regime.
Once this occurs, soliton dynamics as described above can also begin to contribute
significantly to the spectral and temporal features of the generated SC.
At this point when discussing SC characteristics in different wavelength regimes,
we should also make an obvious but necessary remark. Although we often plot
spectral characteristics using axes scales in nanometres, meaningful physical com-
parisons of spectral widths generated across different wavelength ranges should be
made in frequency units of GHz or THz because “the number of nanometres/THz”
varies significantly with wavelength. For small bandwidths, some useful conversion
factors to remember (using j œ/ j D œ2 /c) are 1 THz/nm at 550 nm; 0.5 THz/nm
at 780 nm; 0.3 THz/nm at 1,000 nm; 125 GHz/nm at 1,550 nm. A 100 nm SC around
1,550 nm using a fibre laser for example is associated with a photon energy spread
equivalent to a 25 nm SC from a Ti:sapphire laser at 780 nm.
8.4.2 Picosecond Pulses and Longer
Shortly after the initial experiments by Ranka et al. in 2000 [4] reporting SC
generation using femtosecond pulses, several groups reported broadband SC in
PCF using nanosecond and picosecond sources (See Ref. [6] for a full historical
review). Subsequent research has also extended this “long pulse” regime to include
continuous wave sources. For the long pulse regime, soliton effects do not pay
an important role in the initial dynamics, but it is rather the spontaneous growth
of new frequency components outside the pump bandwidth that dominates the
initial spectral broadening. The mechanisms involved in this regime are based on
spontaneous four wave mixing (FWM) or, as it is referred to in the time domain,
modulation instability (MI). To emphasise the fact that these terms are different
ways of discussing the same physics, we refer to this as FWM/MI in what follows.
The relative importance of soliton effects and spontaneous FWM/MI is in fact
quite easy to quantify. If we consider anomalous dispersion regime pumping, as
the soliton order becomes very large ( N >> 10), higher-order soliton evolution (as
described above) become progressively less important because the characteristic
length scale over which soliton fission occurs increases with the pump pulse
duration, so the effect of spontaneous MI/FWM sideband growth dominates. In
such cases, initial MI/FWM dynamics leads to the temporal break-up of the pump
pulse into a large number of sub-pulses. Interestingly, recent work has provided new
insight into this pulse breakup by showing that they can be interpreted in terms of
a particular class of analytic solution to the NLSE known as Akhmediev breathers
[10]. The subsequent evolution of these sub-pulses then leads to additional spectral
broadening and SC formation through a variety of mechanisms, notably the same
soliton dynamical effects such as dispersive wave generation and the Raman soliton
self-frequency shift as seen above. However, the transition regime between breather
structures and solitons remains somewhat lacking of a clear physical picture, but
some insights are being obtained and links with instability processes of turbulence
and convection in other areas of physics are providing new insights. Still, a simple
Fig. 8.3 Left: Single-shot simulation results showing spectral evolution of a 500 W peak power
20 ps pulse at 800 nm over 2 m. Right: Similar single-shot results for pulse durations as shown
unified picture of this process would be very welcome if indeed mathematically it

is possible. In this regard, it is perhaps worth pointing out that the rational solutions
of MI/FWM described by the Akhmediev breather existed in the literature for over
25 years before their significance in describing MI/FWM processes became widely
appreciated and confirmed by experiment!
For picosecond pulse excitation, the simulation results in the left panel of Fig. 8.3
illustrate some characteristic features of the spectra that are observed. Using a fibre
with 780 nm zero dispersion wavelength, and for a 20 ps input pulse at 800 nm with
500 W peak power, the results show spectral evolution as a function of distance.
The left panel clearly illustrates the spontaneous growth of sidebands from noise,
followed by further spectral broadening and the appearance of soliton structure after
2 m. Note that the noise model used here was a uniform one photon per mode
spectral density with random phase, but essentially identical results are obtained
with other low level noise sources provided the noise is present over the frequency
range of MI/FWM gain (which will generally always be the case experimentally).
The results in the right panel of the Fig. 8.3 show simulations for different pulse
durations, but showing the output spectra only. The significance here is that these
results illustrate the broad similarity in characteristics observed once the “long
pulse” regime is entered. It is very important to note that the simulation results here
are single-shot realisations, but in simulations that are performed over an ensemble
using different noise seeds, there is significant shot-to-shot variation that washes
out/averages much of the fine spectral and temporal structure seen in the figure
[11, 12]. Understanding the mechanisms of these instabilities and developing new
techniques for their measurement is forming the basis of the emerging field of
“optical rogue wave” research – the description here refers to a possible analogy
between fibre instabilities and oceanic instabilities that lead to the formation of giant
high amplitude waves of great destructive power [13]. We consider this below.
8.4.3 Telecommunication Supercontinuum

with Convex Dispersion
Much of the studies of nonlinear propagation in optical fibres in the 1980s were
performed in the context of optical telecommunications, focussing extensively on
applications such as soliton transmission, Raman amplification and wavelength
conversion [1]. Possible applications of SC generation to telecommunications have
also been considered, motivated by the need to develop broadband sources suitable
for spectral slicing in wavelength-division multiplexing. The idea here is that it
is generally easier to increase data rates by using more channels of different
wavelength carrying data at a low bit rate rather than one single channel at a greatly
enhanced bit rate. The spectral slicing approach is based on using one primary
source to generate a broad spectrum that is subsequently filtered into the desired
number of separate wavelength channels. This is an attractive alternative to using an
independent source for each channel.
For such multi-wavelength applications, a crucial practical requirement is spec-
tral uniformity across as wide a wavelength range as possible, centred at around the
telecommunications wavelength range of 1,550 nm. Generating SC spectra across
this range has been pioneered by Japanese groups [14–16]. The optical fibres used
for SC generation at around 1,550 nm generally possess dispersion characteristics
that are very different from the fibres used for SC generation with Ti:sapphire laser
sources. As a result the propagation dynamics and the output spectral characteristics
are also qualitatively very different from the results seen in Figs. 8.2 and 8.3. The
mechanisms of SC generation in this regime have been considered in a number of
publications, notably [16] for standard fibre and, more recently [17] for PCF.
A case of particular interest is when the fibre possesses a convex dispersion
profile such that two zero dispersion wavelengths bracket the pump wavelength.
Although this is a class of fibre design that has seen some recent interest for photonic
crystal fibre, it has existed within the highly nonlinear fibre technology for some
time. One consequence of this class of fibre is that propagating pulses can see a
slope of dispersion that changes sign on either side of the point where the dispersion
reaches its extremum. Propagation in this regime leads to interesting new effects in
the SC spectrum.
When a convex profile is combined with a dispersion at the pump wavelength
that varies longitudinally from anomalous at the fibre input to normal at the
fibre output, spectra are obtained that are simultaneously uniform, symmetric, and
Fig. 8.4 A “telecommunications supercontinuum” showing (a) longitudinal evolution and (b) the
corresponding output spectrum after 1 km of propagation. Note the significant qualitative
difference in the spectral shape when compared to supercontinuum generation with soliton or
MI/FWM dynamics
stable. Of course this requires appropriate matching of fibre and source parameters.
Figure 8.4 above shows results from simulations that illustrate the features observed.
Here we show (a) the longitudinal evolution in greyscale as well as (b) the output
spectrum after 1 km of propagation in a convex profile dispersion decreasing fibre
(see Ref. [17]). In this case, the uniform spectrum at the output develops from
a combination of initial compression followed by dispersive wave generation as
the expanding pulse spectrum penetrates into regimes of normal dispersion on
both the short wavelength and long wavelength side of the central wavelength.
This symmetric dispersive wave generation appears to be the primary mechanism
underlying the smooth spectra observed. Note that the spectral asymmetry seen in
Fig. 8.4b arises from Raman gain on the long wavelength edge.
8.5 Supercontinuum Stability
The “stability” of a SC refers to how the properties of the output spectrum and
temporal intensity vary with time. Stability issues are most readily understood when
considering SC generation using pulsed sources [6]. In this case, we consider the
variation in the SC characteristics from shot-to-shot, as each pulse in a mode-locked
laser pulse train excites an independent spectrum. Because there will always be
some level of technical and/or quantum noise, each input pulse will be slightly
different; thus in regimes where the spectral broadening is highly sensitive to noise,
this can lead to significant shot-to-shot variation.
One important consequence here is that the SC characteristics measured using

integrating detectors such as scanning optical spectrum analysers may yield a
smooth spectrum, but this may be artificial, not reflecting the fine structure that
would be observed if shot-to-shot diagnostics were available. In this regard an
appropriate choice of spectral resolution is also necessary to resolve the structure
of the spectrum.
Issues of SC stability were considered in early work studying SC generation
in a telecommunications context, and extended significantly motivated by optical
frequency metrology applications. Interestingly, the work in frequency metrology
established practical guidelines to stabilise the octave spanning SC well before
the reasons underlying the spectral instability were fully understood. As with the
underlying spectral broadening mechanisms, the stability of fibre SC generation
depends on the combination of particular fibre and source parameters.
For the common case of near zero dispersion wavelength pumping, a simplified
but conceptually useful way to understand the sensitivity to noise is to consider the
growth rate of two specific nonlinear processes: (i) the intrinsic spectral broadening
of the input pulse envelope due to the initial phase of soliton fission and (ii) the
spontaneous growth of spectral components due to MI/FWM. When seeded from
noise, the latter process introduces a noise source that can compete with and/or drive
the otherwise coherent spectral broadening processes involving soliton dynamics.
However, when soliton fission dominates the initial dynamics (e.g. with broadband
femtosecond pulses), the input pulses get temporally compressed so quickly that the
spectral extent of the emerging SC can overlap with the frequencies of maximum
MI gain before significant incoherent amplification has taken place. This results in a
coherent seeding of the SC that is generated. On the other hand, when the dynamics
of MI dominate (e.g. with narrowband picosecond pulses) then the SC generated
can exhibit spectral and temporal instabilities from pulse-to-pulse.
A number of rules of thumb concerning stability have been proposed, and it
appears that for typical experiments employing PCFs of several 10’s of cm, input
pulses where N < 20 possess high coherence, and input pulses where N > 40 possess
low coherence. More precise matching of fibre length and input soliton number can
be determined for specific conditions using numerical simulations. Of course, as MI
is not present in the normal GVD regime, SC spectra with normal dispersion regime
pumping are, in principle, always highly coherent. However, the drawback is that
the spectral width (at the same peak power) is comparatively much smaller due to
the initial dispersion of the pump pulses.
8.6 Conclusions
The objective of this short chapter was not to present a complete overview of
every possible scenario of SC generation in optical fibres, but rather to discuss
a selection of specific results that are of particular interest in understanding the
underlying physics. SC generation is a fascinating optical phenomenon that provides
a unique testbed to examine numerous areas of nonlinear fibre optics. If there is one
absolutely critical thing to stress in closing, however, it is that one should not be
overly simplistic in trying to explain the dynamics of SC broadening.
Appendix
This MATLAB code using the split-step Fourier technique is a very simple
implementation to show the correspondence between the description in the text and
Fig. 8.1 concerning the basic soliton solutions of the NLSE.
% - - - - - - - - - - - - - - - - - - - - WARNING- - - - - - - - - - - - - - - - - - - - - - - - -
% This code is written in simple dimensional form with no
% effort to be particularly robust numerically.
% Higher order effects are neglected with this implementation
clear,close all
lambda0 D 850e-9; % input wavelength [m]
c D 299792458; % speed of light [m/s]
F0 D c/lambda0;
% Time and Frequency Arrays
Npts D 256;
Tmax D 0.5e-12;
dT D 2*Tmax/(Npts-1);
TT D [Npts/2:(Npts/2)-1]*dT; % [ps]
FF D [Npts/2:(Npts/2)-1] ./(2*Tmax); % [THz]
WW D 2*pi*FF;
% Fibre parameters
beta2 D 1.275e-026;
gamma D 0.10; %nonlinear length
% Soliton order and other parameters
N D 1;
T0 D 30e-15; %nonlinear length
P0 D Nˆ2*abs(beta2)/(T0ˆ2*gamma); %nonlinear length
% Length scales
L D D T0ˆ2/abs(beta2); %dispersion length
L NL D 1/(gamma*P0); %nonlinear length
L sol D pi/2*L D;
% Input pulse
A0 D sqrt(P0)*sech(TT/T0);
% - - - - - - - - - - - - - - - - - - - - - Propagation - - - - - - - - - - - - - - - - - - - - - - -
Nz D 1,000; % number of steps

Lz D 2*L sol; % propagation length
dz D Lz/Nz % steps length
Nplots D 11; % number of plots
% Operators
D op D beta2/2*WW.ˆ2*dz;
N op D gamma*dz;
sel D round(Nz/(Nplots-1));
pik D linspace(0,Lz,Nplots)';
Ip D zeros(Nplots,Npts);
Ip TF D zeros(Nplots,Npts);
Ip(1,:) D abs(A0).ˆ2;
Ip TF(1,:) D abs(fftshift(ifft(A0))).ˆ2;
disp(['Courbe No. 1 de ' num2str(Nplots)])
A1 D A0;
for ii D 2:Nz
A TF D fftshift(ifft(fftshift(A1))).*exp(i*D op);
A1 D fftshift(fft(fftshift(A TF)));
A1 D A1.*exp(i*N op*abs(A1).ˆ2);
if (ii/sel) DD round(ii/sel)
disp(['Courbe No. ' num2str(1 C ii/sel) ' de ' num2str(Nplots)])
Ip(1 C (ii/sel),:) D abs(A1).ˆ2;
Ip TF(1 C (ii/sel),:) D abs(A TF).ˆ2;
end
end
% - - - - - - - - - - - - - - - - - - - - - - Display - - - - - - - - - - - - - - - - - - - - - - - - -
figure(1)
a D waterfall(1e-12*FF,pik/L sol,Ip TF);
xl D xlabel('Frequency(THz)'),set(xl,'Rotation',32,'fontsize',16)
yl D ylabel('Distance z/L fsolg'),set(yl,'Rotation',-30,'fontsize',16)
zl D zlabel('Spectrum (arb.)','fontsize',16)
set(gcf,'colormap',[0 0 0])
set(gca,'Xgrid','off','Ygrid','off','Zgrid','off','fontsize',16, : : :
'Linewidth',1)
view(135,50)
axis([150 150 0 2 0 max(max(Ip TF))])
figure(2)
b D waterfall(1e12*TT,pik/L sol,Ip);
xl D xlabel('Time (ps)'),set(xl,'Rotation',32,'fontsize',16)
yl D ylabel('Distance z/L fsolg'),set(yl,'Rotation',-30,'fontsize',16)
zl D zlabel('Intensity (W)','fontsize',16)
set(gcf,'colormap',[0 0 0])
set(gca,'Xgrid','off','Ygrid','off','Zgrid','off','fontsize',16, : : :
'Linewidth',1)
view(135,50)
axis([0.5 0.5 0 2 0 max(max(Ip))])
References
1. G.P. Agrawal, Nonlinear Fiber Optics, 4th edn. (Academic, San Diego, 2007)
2. P.S.J. Russell, Photonic-crystal fibers. J. Lightwave Technol. 24, 4729–4749 (2006)
3. J.M. Dudley, J.R. Taylor, Ten years of nonlinear optics in photonic crystal fibre. Nat. Photonics
3, 85–90 (2009)
4. J.K. Ranka, R.S. Windeler, A.J. Stentz, Visible continuum generation in air-silica microstruc-
ture optical fibers with anomalous dispersion at 800 nm. Opt. Lett. 25, 25–27 (2000)
5. J.M. Dudley, L. Provino, N. Grossard, H. Maillotte, R.S. Windeler, B.J. Eggleton, S. Coen,
Supercontinuum generation in air–silica microstructured fibers with nanosecond and femtosec-
ond pulse pumping. J. Opt. Soc. Am. B 19, 765–771 (2002)
6. J.M. Dudley, G. Genty, S. Coen, Supercontinuum generation in photonic crystal fiber. Rev.
Mod. Phys. 78, 1135–1184 (2006)
7. G. Genty, P. Kinsler, B. Kibler, J.M. Dudley, Nonlinear envelope equation modeling of sub-
cycle dynamics and harmonic generation in nonlinear waveguides. Opt. Express 15, 5382–5387
(2007)
8. E.M. Dianov, A.Y. Karasik, P.V. Mamyshev, A.M. Prokhorov, V.N. Serkin, M.F. Stel’makh,
A.A. Fomichev, Stimulated-Raman conversion of multisoliton pulses in quartz optical fibers.
JETP Lett. 41, 294–297 (1985)
9. C.M. Chen, P.L. Kelley, Nonlinear pulse compression in optical fibers: scaling laws and
numerical analysis. J. Opt. Soc. Am. B 19, 1961–1967 (2002)
10. J.M. Dudley, G. Genty, F. Dias, B. Kibler, N. Akhmediev, Modulation instability, Akhmediev
Breathers and continuous wave supercontinuum generation. Opt. Express 17, 21497–21508
(2009)
11. J.M. Dudley, S. Coen, Coherence properties of supercontinuum spectra generated in photonic
crystal and tapered optical fibers. Opt. Lett. 27, 1180–1182 (2002)
12. K.L. Corwin, N.R. Newbury, J.M. Dudley, S. Coen, S.A. Diddams, K. Weber, R.S. Windeler,
Fundamental noise limitations to supercontinuum generation in microstructure fiber. Phys. Rev.
Lett. 90, 113904 (2003)
13. D.R. Solli, C. Ropers, P. Koonath, B. Jalali, Optical rogue waves. Nature 450, 1054–1057
(2007)
14. T. Morioka, K. Mori, M. Saruwatari, More than 100-wavelength-channel picosecond optical
pulse generation from single laser source using supercontinuum in optical fibres. Electron.
Lett. 29, 862–864 (1993)
15. K.R. Tamura, H. Kuhota, M. Nakazawa, Fundamentals of stable continuum generation at high
repetition rates. IEEE J. Quantum Electron 36, 773–779 (2000)
16. K. Mori, H. Takara, S. Kawanishi, Analysis and design of supercontinuum pulse generation in
a single-mode optical fiber. J. Opt. Soc. Am. B 18, 1780–1792 (2001)
17. G. Genty, S. Coen, J.M. Dudley, Fiber supercontinuum sources (Invited). J. Opt. Soc. Am.
B 24, 1771–1785 (2007)
Chapter 9
Nonlinear Wavelength Conversion and Pulse
Propagation in Optical Fibres
William J. Wadsworth
9.1 Introduction
The subject of nonlinear optics in optical fibres has a long history, and has developed
in parallel with, and as a spur to, developments in fibre design and laser sources.
Chapter 8 in this book covers in some detail the physics of nonlinear pulse
propagation in optical fibres in terms of the nonlinear Schrödinger equation (Eq. 8.5)
and its application to understanding the mechanisms of supercontinuum generation.
This chapter approaches many of the same issues, but from the perspective of
the engineering and capabilities of real fibres. One external reference that it is
impossible to ignore in this field is Agrawal’s book ‘Nonlinear Fiber Optics’ [1]
which, in any of its four editions to date, will guide the reader through the theory
of pulse propagation and nonlinear wavelength conversion in optical fibres with a
wide range of practical examples from the academic literature. Many phenomena
can only be touched on here, and Ref. [1] will help to lead the reader to a deeper
understanding of the nonlinear optics.
9.2 Nonlinearity
In optics, the term nonlinearity refers to the relationship between the electric
displacement, D, and the electric field, E, which may be expressed either as
D D "0 "r E; (9.1)
W.J. Wadsworth ()

Centre for Photonics and Photonic Materials, Department of Physics, University of Bath,
Bath BA2 7AY, UK
e-mail: w.j.wadsworth@bath.ac.uk

196 W.J. Wadsworth
or
D D "0 E C P : (9.2)
Normally the relative permittivity, "r , is considered to be a scalar constant,

or equivalently the electric polarisation, P, is linearly proportional to the electric
field E. In general this is not the case, and to take account of the nonlinear
relationship between P and E one can make a Taylor expansion of P in powers
of E

P D "0 .1/
EC .2/
E2 C .3/
E3 C : : : ; (9.3)
assuming for the moment that vectors P and E are in the same direction and so
may be treated as scalars. One must, however, bear in mind that in principle the
coefficients (n) are tensors with elements linking each possible component of E
with each component of P. If the electric field oscillates as ei!t , then terms in
E2 contain components at twice the frequency, e2i!t . If the electric field contains
components at frequencies ! 1 and ! 2 , then terms in E2 contain components at
! 1 C ! 2 and ! 1 ! 2 , with similar effects for the terms in E3 . An oscillating induced
polarisation will re-radiate electromagnetic waves, which will now contain new
frequencies or wavelengths of light. This is the basis for nonlinear wavelength
conversion. In this chapter we shall only consider optical fibres, which are made
from glasses. As glasses are centrosymmetric materials, symmetry forbids a non-
zero (2) so the lowest order nonlinearity is (3) . Furthermore, of the 81 elements of
the (3) tensor only five are non-zero
.3/
xxxx D .3/
yyyy D .3/
xxyy C .3/
xyyx C .3/
xyxy ; (9.4)
for electric fields polarised in the (x,y) plane. The cross terms mean that an induced
polarisation, P, and hence an output field, can be generated perpendicular to the
polarisation direction of the input field. In order to achieve a macroscopic conversion
of energy into the new frequencies one obviously needs large nonlinear coefficients
(n)
, but one also needs to ensure that the fields at new frequencies radiated
from different points in the medium add up in phase at the output. This requires
phasematching, which will be discussed later in Sect. 9.6.1.
Another useful way of expressing the optical nonlinearity is in terms of an
intensity dependent refractive index, as in Eq. (8.4). Putting Eq. (9.3) into (9.2)
and re-formulating the result into the form of (9.1) gives (again assuming a scalar
relationship between the fields)

D D "0 E C "0 .1/ E C .2/ E 2 C .3/ E 3 C : : :

D "0 1 C .1/ C .2/ E C .3/ E 2 C : : : E (9.5)
9 Nonlinear Wavelength Conversion and Pulse Propagation in Optical Fibres 197
(2)
Using the fact that is zero in glasses and that the refractive index is defined
by n2 D "r we obtain:
q
nD 1C .1/ C .3/ E 2 C :::
q
1
1C .1/ C p .3/
E2
2 1C .1/
1
D n0 C .3/
E2
2n0 (9.6)
This expression is now of the form of a nonlinear refractive index, n D n0 C n2 E2 .

Further details may be found in Section 2.3.1 of Ref. [1]. For completeness we
should note that the (3) coefficient in this time averaged scalar approximation is
related to the co-polarised component of the tensor by [1]:
˚
.3/
D 3
4 Re .3/
xxxx : (9.7)
To convert to the intensity units used in Eq. (8.4) one can relate the optical intensity,
I, to the electric field, E, by [2, 3]:
c"0 n 2
I D E : (9.8)
2
Several nonlinear processes may be explained from the induced polarisation
picture or the nonlinear refractive index picture. The (3) component of the induced
polarisation gives an output wave at a frequency
!4 D !1 C !2 ˙ !3 ; (9.9)
corresponding to third harmonic generation (! 1 D ! 2 D ! 3 D ! 4 /3) or four-wave

mixing (FWM). The most common effect studied in optical fibres is partially
degenerate FWM with a single pump field providing ! 1 D ! 2 , generating signal
and idler output waves ! 3 and ! 4 . This is discussed further in Sect. 9.6. In the time
domain, output waves ! 3 and ! 4 generated equally spaced at either side of the pump
by a frequency shift, , will beat with the pump wave and hence cause an amplitude
modulation at the frequency . As the intensity of the generated signal and idler
fields grows, the depth of this modulation will increase, so the FWM process can be
referred to as modulation instability (MI) in the time domain. One should note that
one of the output waves, ! 3 , appears on the pump side of Eq. (9.9), a result of the
form of Eq. (9.3). This means that a seed is required for FWM or MI to take place.
If a macroscopic seed is not supplied then the process proceeds by amplification
of quantum noise, which has certain implications for the stability of these processes
(Sects. 9.7 and 8.5). The nonlinear refractive index, n2 , with a time varying intensity,
I(t), also gives rise to the processes of self phase modulation (SPM) and cross phase
modulation (XPM), as has already been shown in Chap. 8.
198 W.J. Wadsworth
The processes of FWM, MI, XPM and SPM all arise from the electronic
nonlinearity. The inelastic processes of Raman scattering or Brillouin scattering are
not considered in detail here.
9.3 Optical Fibre Modes
In order to understand the capabilities and limitations of optical fibres as nonlinear

optical devices, it is necessary to understand the basic properties of guided modes
in waveguides. Given that most of this book deals with bulk lasers and free-space
Gaussian beams, we start from the simple picture of guidance in a high-index
medium by total internal reflection at a boundary with a low-index medium,
Fig. 9.1a. The fibre geometry is defined by the core radius, , the index step, ın, and
the core and cladding indices, ncore and nclad respectively (Fig. 9.1b). This simple ray
picture is extremely restrictive, however it does give the trivial information that the
core index must be higher than the cladding index in order to allow the total internal
reflection. It also gives an indication of the maximum angle at which an input ray
can enter the end of the fibre and be guided. The idea of a ray propagating inside
a fibre core is, however, clearly unphysical for small core dimensions – a beam
can only be described as a ray with a defined position and propagation direction
when the propagation distance is much less than the Rayleigh range of the beam.
For Fig. 9.1a to be a good representation of a typical fibre with a core diameter of
10 m, a micron-diameter beam would be needed. From Gaussian beam optics the
Rayleigh range of such a beam at 1,064 nm is just 0.75 m, and so such a beam
cannot exist on the scale of Fig 9.1a.
In order to get any meaningful insight into guidance in an optical fibre we must
instead make a more rigorous calculation of the electromagnetic field in the structure
shown in Fig. 9.1b.
Maxwell’s equations governing the electromagnetic field are simple and com-
plete and are the starting point for all analysis of guided wave optics. One generally
makes the approximation of a linear, isotropic and homogeneous medium in order
to derive a wave equation for plane waves in free space. However a circular
a b
nclad r
ncore
dn
n nclad
ncore
r
nclad 0
Fig. 9.1 (a) simple (though incorrect) ray picture of guidance in an optical fibre, (b) terms defining
a step-index fibre geometry
waveguide, whilst it is still piece-wise homogeneous, yields extra terms because of

the vector boundary conditions for the electric field at the core-cladding index step.
The definition of a waveguide mode is an electromagnetic field which propagates
without change (except for a phase) as it propagates along the waveguide. Assuming
the mode propagates in the z-direction this gives an electric field of the form
E.x; y; z; t/ D E.x; y/e i.ˇ z!t / (9.10)
and Maxwell’s equations may be manipulated into the vector wave equation

rt2 E C k 2 n2 ˇ 2 E D rt C iˇOz E:rt ln n2 : (9.11)
Here, E and n are functions of x and y only (the transverse mode field profile and
transverse index profile of the fibre or waveguide), ˇ is the propagation constant, k
the free-space wavevector (! /c), and rt is the transverse gradient operator
@ @
rt D xO C yO C 0Oz: (9.12)
@x @y
The x-component of the left hand side of Eq. (9.11) contains only the
x-component of the field, however the x-component of the right-hand side of Eq.
(9.11) contains terms which contain both the x and y components of the electric field
E. The equation is generally intractable and solutions require numerical methods.
However one can often make approximations for which this reduces back to a
tractable scalar equation. If n(x,y) does not vary very much (weak guiding), then
the term on the RHS of Eq. (9.11) may be neglected:

rt2 C k 2 n2 ˇ 2 D 0; (9.13)
with the electric field vector, E(x,y), related to the scalar field, (x,y), by a spatially
invariant direction vector, eO W E

.x; y/ D eO .x; y/: Note that the polarisation
described by eO is not necessarily linear, however the polarisation is constant
across the (x,y) plane. It can be useful to note that this scalar wave equation is
mathematically identical to the Schrödinger equation for the wavefunction, ‰, of a
particle, mass m, in a 2D potential, V,

2m 2m
rt2 ‰.x; y/ V .x; y/ E ‰.x; y/ D 0: (9.14)
„2 „2
Note that here E is the energy of the state, not the electric field. We can identify
the potential, V, (note the sign change) with the fibre index profile, n2 , and the
energy eigenvalue, E, with the fibre mode propagation constant, ˇ. This analogy is
useful because many students study solutions of the Schrödinger equation, so have
some intuition for the form of these solutions which can then be transferred to give
a basic understanding of the modes of optical fibres.
200 W.J. Wadsworth
a ∞ ∞
p
b c ncore
4 dn nmode
3
dV dV
V 2 V
n
1 nclad
x x r
0 a 0 a -
Fig. 9.2 Schematic representations of: (a) solutions to the Schrödinger equation in a 1-D infinite
potential well, (b) the same for a finite potential well, (c) solutions to the scalar wave for a step-
index optical fibre
Table 9.1 Wavefunctions ‰ p (x) Ep

and energy eigenvalues for a
State p sin (p x / a) p2 h2 / 8 m a2
particle in the infinite square
potential well shown in State 2 sin (2 x / a) 4 h2 / 8 m a2
Fig. 9.2a State 1 sin ( x / a) h2 / 8 m a2
The integer p is used to denote the state number
rather than the more usual n or m to avoid ambi-
guity with the refractive index or particle mass
The first problem which we often solve for the Schrödinger equation is a particle
in an infinite square potential well. There are sin(p x/a) solutions as shown in
Fig. 9.2a with defined spatial profiles and energies as in Table 9.1. These eigen
solutions are wavefunctions which do not change in time (except for a phase),
analogous to the modes of a fibre which do not change with propagation distance
along the fibre (except for a phase). The solution for a finite potential well is similar
to the solution for an infinite potential well, but with the addition of evanescent tails
of the wavefunction extending into the classically forbidden region outside the well
(Fig. 9.2b). There are then a finite number of bound states with energies below the
potential of the boundaries of the well.
A step-index optical fibre bears a close resemblance to a finite potential well as
shown in Fig. 9.2c. The potential well becomes a positive index step (because of
the sign change between Eqs. 9.13 and 9.14), the energy eigenvalue becomes the
modal propagation constant, the tails of the particle wavefunction in the classically
forbidden regions outside the well become the evanescent tails of the optical field in
the low-index cladding medium. Also, in Eqs. 9.10, 9.11 and 9.13 the propagation
constant ˇ appears where one would normally expect the wavevector in a medium,
kn D n ! /c. We can therefore define a modal index
ˇ
nmode D ; (9.15)
k
where k is the free-space wavevector.
By analogy with the bound energy eigenvalues in a finite potential well, there will
be a finite number of guided modes in a step index fibre, with modal indices lying
between the core and cladding indices for the fibre, as shown in Fig. 9.2c. There
will also be a continuum of unbound states, the cladding modes, with modal indices
below the cladding index. From further inspection of Eqs. 9.13 and 9.14, with the
definition of modal index in Eq. (9.15), it is clear that the free-space wavevector, k,
is analogous to the particle mass, m. It is not usual to consider particles of different
mass in a box, but it is very common in optics to consider light of widely differing
wavelengths, and hence of differing wavevectors. The overall effect on the modal
index of changing wavelength may be easily seen from the basic ideas of optical
diffraction. Light of a long wavelength will be more difficult to confine in the small
spatial dimension of an optical fibre core. The evanescent tails in the cladding will
be stronger, and the modal effective index will become closer to the index of the
cladding. Conversely a shorter wavelength will have smaller evanescent tails and a
modal index closer to the index of the core. This will be considered further in the
discussion of dispersion in Sect. 9.4.2.
Looking at the order of the modal indices of the fundamental mode and higher
order modes shown schematically in Fig. 9.2c, there appears to be a contradiction
with the ray picture of Fig. 9.1a. Intuitively, one would expect that the fundamental
mode would be the one with the straightest path in the ray picture, which would
also have the shortest path and travel faster down the fibre. However in the modal
indices given in Fig. 9.2c the fundamental mode has the highest index, which implies
a slower velocity. The resolution of this apparent contradiction comes from the
difference between phase and group velocity. The modal index is a phase index,
implying that the fundamental mode has a slow phase velocity. However pulses or
information travel at the group velocity, d! / dˇ, and the fundamental mode does
indeed have the expected low group index and high group velocity.
The number of guided modes is an important consideration in fibre optics, and
it is often convenient or required for a fibre to support only one guided mode – a
single-mode fibre (SMF). We define a fibre parameter
q
2
V D n2core n2clad ; (9.16)

which normalises all the important parameters of the fibre given in Fig. 9.2c into
a single dimensionless number which describes the size of the ‘box’ available for
the modes. It is bigger for a larger index step or a larger core diameter, and bigger
for a shorter wavelength: in other words, when the box is larger compared to the
wavelength. For V < 2.405 there is only one guided mode, for 2.405 < V < 3.832
the second mode is guided as well. For highly multimode fibres with V >> 1 the
number of spatial modes, N, varies as N V2 /4, with each spatial mode having
twofold polarisation degeneracy.
202 W.J. Wadsworth
9.4 Design of Optical Fibres for Dispersion Control
All of the nonlinear processes discussed in Sect. 9.2 require control of chromatic
dispersion – the relative refractive indices for different wavelengths of light. For
SPM and XPM we have seen in Chap. 8 that the sign of dispersion, normal or
anomalous, has a fundamental impact in the formation of optical solitons (Eq. 8.10).
For FWM/MI phasematching is required, which also is controlled by the dispersion
of the medium. An optical fibre will always have a small core and long length,
so that the intensity length product is extremely large, and fibres with particularly
small cores are often termed ‘highly nonlinear fibres’. However, one can only take
advantage of the nonlinearity induced at this high intensity if the dispersion is
correct for the intended nonlinear process. The dispersion must be the first design
factor, this may result in several possible designs with different fibre nonlinearities.
Only if the correct dispersion is obtained can the high nonlinearity of a small core
fibre be useful. This is the case for supercontinuum generation in photonic crystal
fibres pumped at 800 nm, and is one of the reasons that the phenomenon was so
pronounced at such low energies when first demonstrated by Ranka et al. in 1999
[4, 5]. The exceptions to this rule are Brillouin and Raman scattering which do not
require specific dispersion or phasematching.
9.4.1 Group Velocity Dispersion
Before entering into a full discussion of optical fibre dispersion it is necessary

to discuss the two common variables used to define the dispersion. In Chap. 8,
chromatic dispersion was characterised in terms of a Taylor expansion of the
propagation constant, ˇ, with respect to the angular optical frequency, ! (Eq. 8.3).
This is the natural approach in numerical simulations where ˇ and ! are the
variables used in the nonlinear Schrödinger equation (Eq. 8.5). The important
term is the second derivative, ˇ 2 D d2 ˇ / d! 2 , with units of ps2 .km1 . However,
in experiments, we usually consider the free-space optical wavelength rather than
the frequency, and the group velocity dispersion is easily understood from an
engineering point of view as the time delay (in ps) for two optical pulses with
a particular separation in wavelength (in nm) propagating over a certain distance
(in km). This is written as
@1=vg
DD (9.17)
@
where vg is the group velocity and D has units of ps.nm1 .km1 . The two variables
D and ˇ 2 are related simply by a coefficient, but unfortunately this coefficient
contains a minus sign
2
ˇ2 D D : (9.18)
2c
D (ps / nm km)
anomalous
β2 (ps2 / km)
normal
0 0
λ ω
normal
anomalous
λ
ZDW
Fig. 9.3 Sketch of the dispersion of a fibre expressed in terms of D() or ˇ 2 (!), showing the
regions of normal and anomalous dispersion. The zero dispersion wavelength, ZDW , is marked
a b
ps / nm km)
Mode effective index nmode
ncore
0
(µm
· D (µ
(
nclad
0 l/ 8 0 l/ 8
Fig. 9.4 Dispersion of a waveguide mode: (a) Variation of modal index with normalised wave-
length for fixed core and cladding indices. (b) The resultant normalised dispersion. The horizontal
scale applies for ncore D 1.45, nclad D 1.0, and in that case the vertical scale in (b) is 800 to
400 m.ps.nm1 .km1
It is therefore not possible to talk about ‘positive’ or ‘negative’ dispersion without

ambiguity. The terms ‘normal’ and ‘anomalous’ dispersion are unambiguous and
refer to regions of negative D (positive ˇ 2 ) and positive D (negative ˇ 2 ) respectively
(Fig. 9.3). The wavelength (or optical frequency) at which the dispersion is zero is
known as the zero dispersion wavelength, ZDW , and is also clearly important as the
dividing point between normal and anomalous dispersion. This is obviously (and
fortunately) the same in both representations.
9.4.2 Optical Fibre Dispersion
Optical fibres are made out of a particular material, usually silica glass, which
will have a material dispersion of its own, however this will be modified by the
dispersion arising from the optical waveguiding. The variation of the modal index
with wavelength was considered in Sect. 9.3: at long wavelengths the modal index
will become close to the index of the cladding and at short wavelengths the modal
index will become close to the index of the core. This effect and the consequent
waveguide group velocity dispersion are illustrated in Fig. 9.4.
204 W.J. Wadsworth
20 Step index
Dispersion D(ps/nm km) Dispersion shifted

10
0
1.1 1.2 1.3 1.4 1.6 1.7
Wavelength (μm) m)
Dis
-10 per
sio
n fl
atte
ned
-20
Fig. 9.5 Dispersion of various fibres in the telecommunications wavelength range together with
example radial refractive index profiles
Generally the material dispersion is normal at short wavelengths and anomalous

at long wavelengths (most materials have normal dispersion in the visible, which
is how the term arises). The waveguide dispersion shows the opposite trend, being
anomalous at short wavelengths and normal at longer wavelengths. In Fig. 9.4, the
wavelength scale is normalised to the fibre core radius, which indicates that the
actual wavelength spread of the waveguide dispersion may be altered by changing
the fibre design. The magnitude of the waveguide dispersion is also obviously a
function of the magnitude of the core-cladding index step.
In conventional step-index silica optical fibres with germanium doped cores the
index step is small, <3 %, resulting in low waveguide dispersion. The waveguide
dispersion then only has a noticeable effect in the spectral region where silica itself
has low dispersion, close to the material ZDW at 1,270 nm. Index profiles which
are more complicated than the simple step index considered in Sect. 9.3 can give
flattened or shifted dispersion in the telecommunications windows near 1,310 and
1,550 nm, as shown in Fig. 9.5 [6 (pp. 132–140), 7]. In these fibres, extra guidance
structures are included in the refractive index profile, which have the effect of
modifying the wavelength range over which the modal index varies, giving sharper
transitions in modal index and hence higher waveguide dispersion.
Very large core-cladding index steps can result in a dispersion which is compa-
rable to the material dispersion over a wide wavelength range. Large index steps
are attainable using structures containing silica glass and air [5, 8–10], Fig. 9.6. The
simplest structure is a strand of silica glass in air, a silica microwire or nanowire
[10–12], which also gives the largest index step. This type of structure is at the heart
of fused fibre couplers and wavelength multiplexers used for telecommunications,
and is often also referred to as a fibre taper because it is usually made by heating
and pulling a standard optical fibre [10]. A controlled index step is achievable using
a microstructure containing air and silica as an engineered cladding material in
a photonic crystal fibre (PCF) [8, 9, 13, 14]. Such fibres are also referred to as
microstructured fibres or holey fibres.
Fig. 9.6 Scanning electron microscope images of silica – air fibre structures. In all images,
black areas are air, grey/white areas are silica glass. (a) Free silica micro/nanowire (a tapered
optical fibre). The structure is suspended from the ends by standard fibre and input and output
tapered transition regions. Useful diameter range <0.5–5 m, fabricated length 1–25 cm. (b)
Silica micro/nanowire suspended from the sides by 100 nm wide silica webs in a high air filling
fraction PCF structure (overall fibre and close-up of the core region). Useful core diameter range
0.8–4 m, fabricated length 100s–1,000s m. (c) Low air filling fraction PCF for further dispersion
control. Useful core diameter range 1–20 m, fabricated length 100s–1,000s m. (d) Hollow-core
PCF. Core diameter 7 m at 800 nm, fabricated length 100s–1,000s m
9.4.3 Silica Micro/Nanowires
Taking the extreme case of a silica microwire in air first, the material and waveguide
dispersion are plotted in Fig. 9.7a. It is clear that the dispersion of the waveguide
can now dominate the material dispersion in the visible and near infrared, opening
up the possibility of fibres with anomalous dispersion at wavelengths shorter than
1,270 nm (ZDW for silica glass). Separating the fibre dispersion into a waveguide
part (assuming a constant material index) and the bulk material dispersion gives
insight into the factors affecting the dispersion, but will not give an accurate
dispersion curve. A full calculation of the guided modes of a silica nanowire,
including the material dispersion, yields the dispersion curves shown in Fig. 9.7b.
The dispersion curves for 1.5, 2.0 and 2.5 m diameter strands look qualitatively
similar to the dispersion of silica (Fig. 9.7a solid line) or conventional step-
index fibres (Fig. 9.5) i.e. there is large normal dispersion at short wavelengths,
a zero dispersion (ZDW ) in the red or near infrared and anomalous dispersion at
longer wavelengths. There will be little difference in the fundamental linear and
nonlinear physics observed. However the change of ZDW from 1,270 nm to the
600–800 nm region is technologically important for nonlinear optics. To achieve
206 W.J. Wadsworth
a b
800
d=0
532 nm 780 nm 1064 nm
.5 μm
400
Dispersion D(ps/nm km)
600 0.9 μm 1.1 μm

1.5 μm
Dispersion D(ps/nm km)

400 200 2.0 μm
d=2 2.5 μm
200 μ m 0
0.7 μm
0
-
-200
0.5 μm
d=1
- 200
-
-400
μm
- 400
400 600 800 1000
1000 2000 3000 Wavelength (nm)
Wavelength (nm)
Fig. 9.7 (a) Material dispersion of silica (solid line) and waveguide dispersion for different
diameters of silica microwires in air; 0.5 m (dotted), 1.0 m (dashed), 2.0 m (dash-dot); (b)
Total dispersion of silica microwires in air with diameters from 0.5 to 2.5 m. The common laser
wavelengths of 532, 780 and 1,064 nm are marked
high nonlinearity one needs a high power laser, and this usually means a high
peak power pulsed laser. The Ti:sapphire laser, which is the established laboratory
workhorse, typically operates at 780 nm. Silica microwires in the form of small
core PCFs were the starting point for visible continuum generation in fibres at low
power because of the match of ZDW to the operating wavelength of modelocked
Ti:sapphire lasers [4, 5, 10, 15]. Frequency doubled pulsed Nd3C and Yb3C lasers
at around 532 nm are also very common, and a ZDW in this region is achievable
with sub-micron silica nanowires (Fig. 9.7b). Nonlinearity and supercontinuum
generation has been observed in these structures [12, 16], although the small size
brings further problems.
9.4.4 Low Air Filling Fraction Photonic Crystal Fibres
Taking next the case of a PCF with a relatively low air filling fraction, gives further
options for selecting appropriate waveguide dispersion. Here one may not only
select the core diameter, but also the core – cladding index step. This would be
useful even with a naive assumption that the index of the silica – air cladding
is simply given by the averaged index, taking into account the area of glass and
air in the cladding. However the reality is somewhat more complex, and luckily
also more effective in dispersion design. A PCF cladding of the type shown in
Fig. 9.6c has a scale that is large or comparable to the wavelength of light. This
means that the modes of the cladding (which define the effective cladding index
[17, 18]) will actually be well confined to the silica regions in the cladding, giving
a high effective index at short wavelengths. At longer wavelengths, or at smaller
Fig. 9.8 (a) Wavelength dependence of the effective index of a silica – air PCF cladding with
d/ƒ D 0.4, for different values of pitch: ƒ D 10 m (dot), ƒ D 5 m (dash), ƒ D 2 m (dash-
dot), compared to uniform bulk silica (solid), inset: representation of the structure (b) Measured
dispersion of three PCFs with pitch ƒ D 3 m and different air hole diameters close to d/ƒ D 0.4,
compared to uniform bulk silica (solid), inset: Scanning electron microscope image of core region
of one of the fibres (Part (b) reproduced and adapted with permission from Ref. [19])
cladding scale, the modes will spread out into the air (just as the fundamental mode
spreads from the core of a fibre at long wavelengths) and the effective index will be
low. The calculated effective index for an infinite cladding material for a particular
structure is shown in Fig. 9.8a for a range of wavelengths at different structural
scales. Thus a PCF cladding not only has an effective index which is controllable
over a wide range – from 1 to 1.45 – but the cladding index is also highly wavelength
dependent, adding another dimension to the waveguide dispersion. An example of
the application of this type of fibre for nonlinear optics is shown in Fig. 9.8b, where
a set of fibres has been fabricated with ZDW close to the wavelength of common
pulsed Nd3C and Yb3C lasers [19]. Again this is of technological importance
because the lowest cost high power pulsed lasers available are in the 1,030–1,080 nm
spectral range. These fibres serendipitously have one further useful property; they
are endlessly single mode (ESM), that is, they support only one guided mode at all
wavelengths [17, 18]. The variation of the cladding effective index exactly cancels
the term 1/ in the fibre parameter, V, (Eq. 9.16) at short wavelengths so that when
d/ƒ < 0.4 the effective V never rises above 2.4 (using an appropriate scaling factor
to define V for a PCF [17]). ESM fibre is reassuring for supercontinuum systems
discussed in Sect. 9.7, which may generate light over the range from less than
350 nm to beyond 2,400 nm.
Calculation of the propagation constants and dispersion of modes in PCFs is
generally a complex numerical task. However some commercial finite element codes
(such as Comsol) offer techniques for PCF modelling, and a mode solver using
the multipole method is currently available from the University of Sydney [20].
An empirical model provided by Saitoh and Koshiba [21] is an invaluable simple
tool for initial estimates of fibre design. One must always bear in mind the stated
validity limits for this model and also that as it separates out the contribution of
208 W.J. Wadsworth
material and waveguide dispersion it has a certain built-in inaccuracy. However it is

remarkably effective and provides an extremely quick and easy way to examine a
wide range of structures in order to select a promising region for detailed modelling
or experimental investigation.
9.4.5 Hollow-Core Photonic Crystal Fibres
Hollow-core photonic crystal fibres (HC-PCFs) (Fig. 9.6d) exploit the photonic
bandgaps that can be achieved in periodic dielectric structures – light of a certain
range of frequencies and propagation constant can be excluded from such a structure
[13, 14]. If we imagine an elongated doughnut of a photonic crystal then if light
at a frequency within the bandgap is launched into the central hole it cannot
escape through the photonic crystal and therefore must be guided along the hole.
In the usual implementations of photonic crystals, light propagates in the plane
of periodicity, whereas in a PCF the light travels perpendicular to the plane of
periodicity. For a HC-PCF one also requires that light is in a guided mode in
the hollow core region, which means that at any particular frequency the bandgap
only needs to cover the well-defined propagation constant for that mode. This is a
considerably simpler criterion to fulfil than the full 2-D bandgap required for in-
plane photonic crystal waveguides [22] and means that HC-PCFs can be fabricated
from silica-air structures and do not need high index materials like silicon.
Figure 9.9 shows the relatively narrow guiding band of a HC-PCF, which
may extend to 20 % of the central frequency. Attenuation and dispersion are
fundamentally linked by the Kramers – Kronig relations [23]. With a narrow guiding
band and sharp transitions to extremely high loss, the dispersion of HC-PCF is
determined primarily by the Kramers – Kronig relations and the position of the
guiding band. The dispersion imposed by the bandgap guidance is zero at the centre
of the bandgap and diverges to large normal dispersion at the short wavelength
edge and to large anomalous dispersion at the long wavelength edge. There is also
a contribution from waveguide dispersion, which is anomalous across the whole
guiding band, so the overall ZDW is shifted closer to the short wavelength edge, and
the dispersion is anomalous over much of the guiding band, as shown in Fig. 9.9.
This anomalous dispersion allows propagation of solitons at any wavelength where
HC-PCF can be fabricated, which has been demonstrated at 532, 800, 1,064 and
1,550 nm [24–27].
9.5 Pulse Delivery and Compression in Fibres
Propagation of optical solitons was introduced in Chap. 8 (Eq. 8.10). Solitons

were predicted as solutions of the nonlinear Schrödinger equation, which propagate
unchanged in a nonlinear medium. At first sight this may appear to be too good to
Fig. 9.9 The attenuation

spectrum and dispersion of a
HC-PCF guiding around
1,550 nm (Reproduced and
adapted with permission from
Ref. [28])
be true; the solitons occur for a particular pulse shape with defined energy (related
to the pulse duration) in a nonlinear Schrödinger equation that does not include the
Raman effect, fibre attenuation or a slope of the GVD curve (third-order dispersion).
Surely a real pulse of non-ideal pulse shape, with too much or too little energy and
launched into a real fibre with attenuation and higher order dispersive and nonlinear
terms will never be able to excite these magic unchanging pulses. The fact that
solitons are actually readily observable [27, 29] may be seen more easily from the
simple phenomenological description of a soliton, as follows. In a nonlinear medium
the leading edge of a pulse experiences a red-shift from self phase modulation.
With anomalous dispersion red-shifted frequencies have a slower group velocity
and so will tend to move back into the body of the pulse. Similarly the trailing edge
experiences a blue shift from self phase modulation, and the blue-shifted frequencies
travel forward into the pulse under anomalous dispersion. When the nonlinear SPM
and the linear dispersion are balanced then the pulse will propagate unchanged along
the fibre as a soliton. In this picture it is apparent that a soliton is not an impossible
stationary solution (like a pencil balanced on its point) but can be a self-building and
self-healing solution. In fact, solitons are extremely robust; solitons can form from
most input pulse shapes at energies far from the exact soliton energies, and solitons
will react to gradual changes as they propagate (such as reduction in energy through
fibre attenuation or changes in fibre dispersion) by adjusting temporal duration and
spectral bandwidth to suit the new conditions (Sect. 9.5.2).
9.5.1 Pulse Delivery
A soliton will propagate unchanged along a fibre, so seems to be an ideal way to

transmit short pulses without mirrors or alignment – from bench to bench in a
210 W.J. Wadsworth
Table 9.2 Soliton parameters for femtosecond pulses propagating in hollow-core PCF
Wavelength (nm) Pulse duration (fs) Soliton energy (nJ) Fibre length (m) Ref.
1,550 300 500 3 [27]
1,064 500 170 5 [26]
800 300 65 5 [25]
532 100 25 1 [24]
laboratory or from the laser to the work piece in a laser machining rig. However,
the energy transmitted as a soliton cannot be selected arbitrarily but must satisfy the
relation
3 DAeff
Esoliton D 1:76 2 ; (9.19)
2 cn2 0
where Esoliton is the soliton energy, is the wavelength of the light, 0 is the FWHM
pulse duration, D is the group velocity dispersion, Aeff is the modal effective area
in the fibre, c is the speed of light and n2 is the nonlinear refractive index. This
is the same condition as Eq. (8.10) and the explanation in Sect. 8.2, but with the
nonlinearity, , written out explicitly and the pulse duration expressed as FWHM
rather than 1/e2 width. If one uses typical values for fibre and pulse parameters
of 0 D 100 fs, D D 20 ps.nm1 .km1 , Aeff D 80 m2 and n2 D 2 1020 m2 W1
then Esoliton D 0.07 nJ at a wavelength of 800 nm or 0.5 nJ at 1,550 nm. The first
solitons demonstrated were 7 ps in duration at energies of just 8.4 pJ [29]. These
are extremely low energies. In order for soliton propagation to be useful the pulse
energy delivered by the fibre must be sufficient for the application: energies of
<1 nJ are in the range of telecommunications pulses (although solitons have not
proved greatly successful in this application because of the interactions of adjacent
solitons), and they may be enough for seeding amplifiers. For most of the other
applications covered in this book, energies of at least 10s or 100s nJ are required,
and often much more.
The energy in Eq. (9.19) is governed by the dispersion and the nonlinearity of the
fibre. In particular, if the nonlinearity of the fibre, n2 , can be reduced, then the soliton
energy is increased. Hollow-core PCF gives an excellent way of greatly reducing the
nonlinearity by replacing the guiding medium with air, or even a vacuum. There is
still some overlap of the guided mode with the silica glass in the cladding which
contributes to the nonlinearity, but the overall effect of changes in D, Aeff and n2
is an increase in the soliton energy by a factor of 100–1,000 more than the figures
calculated above for solid core fibres. This was first demonstrated at 1,550 nm with
a soliton energy of 500 nJ for 300 fs pulses propagated over 3 m of fibre [27]. Such
an energy is sufficient for micromachining applications (see Chaps. 12 and 13).
Subsequently, soliton propagation has been demonstrated at shorter wavelengths
as shown in Table 9.2. The pulse durations are output pulse durations, rounded to
the nearest 100 fs and the soliton energies are the minimum energy given in the
references for propagation of a soliton. The soliton energy scales with wavelength,
roughly as 3 , even though D and Aeff in Eq. (9.19) also change with wavelength.
9.5.2 Pulse Compression
The pulse durations for pulse delivery listed in Table 9.2 are the output pulse
duration, and are longer than the input pulse duration in all but the 532 nm case.
This is partly as a result of the formation of a soliton from an input pulse which may
not be transform limited or may not have the required sech2 pulse shape, partly as
a result of third-order dispersion, and partly as a result of attenuation in the fibre.
Eq. (9.19) is formulated to calculate the input energy required to launch a soliton,
however, once a soliton exists inside a fibre the free parameter is not the energy but
the pulse duration, so it is appropriate to reformulate Eq. (9.19) as
3 DAeff
0 D 1:76 : (9.20)
2 2 cn2 Esoliton
From this it is clear that a soliton experiencing attenuation in a fibre will adjust
to have a longer pulse duration. However, if the dispersion or effective area is
reduced along the length of the fibre, then the soliton will adjust to have a shorter
pulse duration. The length scales for any changes in fibre parameters must be long
compared with the characteristic soliton length (LD D LNL in Sect. 8.2 and [1]) in
order for these transformations to be adiabatic. Adiabatic pulse compression has
been observed in dispersion-decreasing conventional fibres [30, 31], and also for
high energy solitons in HC-PCFs [28, 32–34]. As the dispersion of HC-PCF is
defined by the position of the bandgap (Fig. 9.9), which in turn is defined by the
scale of the cladding structure, it is relatively simple to produce a HC-PCF with
decreasing dispersion by drawing a section of fibre with increasing outer diameter.
This shifts the bandgap and the ZDW to longer wavelengths, which reduces the
dispersion at any given wavelength. As an example, adiabatic soliton compression
has been achieved in a non-uniform HC-PCF at 800 nm [32]. The output pulse
duration was half the input pulse duration, whereas, with a uniform fibre, the
output pulse duration was nearly three times longer than the input. The longer pulse
duration in the uniform fibre is not simply due to chirp, the spectral bandwidth is
simultaneously reduced to maintain soliton pulses close to the transform limit. The
minimum pulse duration achievable in this way is limited by third order dispersion.
The small Raman gain shift in air can also impose a limit in air-filled fibres [35].
Adiabatic soliton compression has also been proposed by varying the nonlinearity
of a fibre using a pressure gradient of the gas in the core [33].
Higher order solitons, which may be launched at higher energies, experience
spectral broadening and pulse compression in the first stage of propagation [1]. With
appropriate pulse energy and fibre length this may be employed for high energy
pulse compression in HC-PCF [24, 36].
Linear compression of chirped pulses is also possible in HC-PCF. This is of
particular use for amplified modelocked fibre lasers, where SPM in the amplifier
can yield an output pulse with a broadened spectrum and linear normal chirp. The
chirp can be compensated for by a grating pair to give short, high energy pulses.
212 W.J. Wadsworth
Fig. 9.10 (a) Normalized experimental output pulse width and (b) spectrum as a function of the
propagation distance in HC-PCF for 5 ps SPM-broadened pulses at 320 nJ laser pulse energy
The same chirp compensation can also be achieved by the anomalous dispersion
of a HC-PCF, but there is also the benefit that the HC-PCF does have some
small nonlinearity. For an appropriate pulse energy, the pulse formed by linear
compression can undergo spectral re-shaping from SPM and the Raman effect to
form a transform limited soliton. This has been demonstrated for compression of
5 ps pulses to 300 fs [26] where the two stages of compression are clearly visible
from a cut-back measurement (Fig. 9.10). For the first 4.5 m of fibre the pulse
duration reduces because of the linear dispersion. In this stage the spectrum remains
almost unchanged as the peak power is insufficient to initiate nonlinear effects in the
HC-PCF. When the pulse is compressed to 500 fs after 4.5 m (approximately the
transform limit of the structured 12 nm input spectrum), the peak intensity is then
high enough for nonlinearity to re-shape the spectrum and after a total propagation
of 6 m a soliton is formed with a nearly transform limited smooth spectral bandwidth
< 3 nm, containing nearly 70 % of the total output energy [26].
9.6 Four-Wave Mixing
The process of FWM/MI introduced in Sect. 9.2 allows for conversion of a laser at a
particular wavelength to another arbitrary wavelength, governed by phasematching
in a fibre. This is similar to bulk optical parametric generators and oscillators but
with two important differences: firstly the phasematching is provided by a guided
fibre mode, so there is no need for angle tuning and no possibility of spatial walk-
off, secondly the nonlinearity used is (3) rather than (2) and so the generated signal
and idler wavelengths are equally spaced around the pump rather than both being
longer than the pump wavelength. Conversion of, for example, 1,064–700 nm can
then be made in one step, rather than requiring frequency doubling to 532 nm and
subsequent (2) parametric conversion to 700 nm.
9.6.1 Phasematching for Four-Wave Mixing
The energy conservation and phasematching conditions for the frequency, !, and
propagation constant, ˇ, for partially degenerate FWM in an optical fibre are
2!p D !s C !i (9.21)
and
2ˇp ˇs ˇi 2P D 0 (9.22)
where subscripts p, s and i refer to the pump, signal and idler waves respectively,
is the nonlinear parameter defined below Eq. (8.5) and P is the power in the
pump wave. FWM does not rely on a time varying intensity (unlike SPM), so these
relations are valid for CW or pulsed lasers, with P being the peak power for pulsed
lasers. Using Eq. (9.21) one can see that the signal and idler waves are shifted up
and down by equal frequency offset, , from the pump. One may then make a
Taylor expansion of the propagation constant ˇ(!) as in Eq. (8.3) so that Eq. (9.22)
becomes
2ˇ.!p / ˇ.!p C / ˇ.!p / 2P D 0 (9.23)

2ˇ.!p / ˇ.!p / C ˇ1 C 12 ˇ2 2 C 16 ˇ3 3 C 1
ˇ 4
24 4
(9.24)
ˇ.!p / ˇ1 C 12 ˇ2 2 16 ˇ3 3 C 1
24 ˇ4
4
2P D 0
ˇ2 2 1
ˇ 4
12 4
2P D 0 (9.25)
with further terms if the Taylor expansion is carried beyond 4th order [37]. As
the pump power P is always positive and is positive in silica glass, this has
solutions for negative ˇ 2 (anomalous dispersion), or for sufficiently large negative
ˇ 4 even when ˇ 2 is positive (normal dispersion, close to ZDW ). An example of the
phasematching curve for a particular fibre is shown in Fig. 9.11a.
In the case of anomalous dispersion at the pump wavelength (right hand side
of Fig. 9.11a), the phasematched sidebands are relatively close to the pump and
the FWM gain extends over a relatively broad bandwidth (and is strongly power
dependent). Wavelength conversion has been extensively investigated for telecoms
applications in this regime, with an emphasis on dispersion flattened fibres with
small and constant ˇ 2 < 0 (ˇ 3 0, ˇ 4 0) to maximise the bandwidth [39].
Dispersion control in PCF offers the potential to improve the bandwidth greatly
with fibres with extremely small and flat anomalous dispersion. There are very many
proposed designs in the literature, but very few have been made [37, 40] owing to
the very tight dimensional tolerances. These arise because in order to achieve a
low fibre dispersion one needs to exactly cancel the material dispersion with the
waveguide dispersion. A very small percentage error in the waveguide dispersion
214 W.J. Wadsworth
Fig. 9.11 (a) Calculated phasematching curve for FWM in a particular birefringent PCF when
pumped close to its zero dispersion wavelength on each of the two principal polarisation axes,
ZDW D 655 and 662 nm. (b) Observed output spectra for pumping at 647 nm with different
polarisations (Reproduced and adapted with permission from Ref. [38])
leads to a large deviation from zero in the resultant fibre dispersion. An example
of a dispersion flattened PCF used for signal conversion in the telecommunications
band is shown by Anderson et al. [40] where signal and idler gain bandwidths of
30 nm were demonstrated (compared to 15 nm in [39]). Fibre optical parametric
oscillators in small-core PCF pumped at 750 nm have also been demonstrated based
on this parametric gain [41].
In the case of normal dispersion at the pump wavelength (left hand side of
Fig. 9.11a, the phasematched sidebands are far from the pump and the FWM gain
extends over only a narrow bandwidth. This only occurs for relatively large ˇ 4 ,
which is a curvature in the spectral variation of the group velocity dispersion.
It is clear from Fig. 9.7 that the large waveguide dispersion required to bring
the zero dispersion wavelength down to the visible and near-infrared in a PCF
usually imparts a large curvature to the dispersion, so this region of phasematching
is particularly common in PCFs at short wavelengths, and less pronounced in
conventional fibres at telecommunications wavelengths. Figure 9.11b shows an
example of this type of phasematching used to produce signal and idler sidebands
close to 500 and 1,000 nm when pumped with 60 ps pulses at 647 nm [38].
Using PCFs with ZDW close to 1,064 nm (Fig. 9.8b) replicates these results in
both normal and anomalous regimes [19, 42]. At this pump wavelength there are
many pump laser options, from nanosecond and sub-nanosecond Q-switched lasers
(in particular compact microchip lasers [19, 43, 44]) to fs or picosecond modelocked
bulk or fibre lasers [45, 46]. The FWM process is efficient even without a feedback
cavity. A single pass of fibre has been shown to give more than 30 % conversion
to signal wavelengths around 700 nm for a variety of laser configurations using
0.5–4 m fibre lengths [19, 43–46]. The range of signal wavelengths observed from
a 1,064 nm pump spans 650–950 nm with corresponding idler wavelengths from
1,200 nm to nearly 3 m, Fig. 9.12. With high power, high repetition rate pump
sources, 2.16 W has been generated at 20 MHz at 740 nm [45, 46] and 450 mW
at 1 MHz at 2,539 nm [43, 44]. The steepness of the phasematching curve on
the left hand side of Fig. 9.11a indicates that for a relatively small pump tuning
range there will be a wide signal and idler tuning range, the potential of which is
discussed extensively in [43–46]. However this also points to a bandwidth constraint
on the pump laser: if the pump bandwidth is too broad then different wavelength
components of the pump will be phasematched for generation of different FWM
wavelengths and the process is not efficient and eventually becomes swamped by
non-phasematched Raman scattering.
9.6.2 Single and Pair Photon Generation by Four Wave Mixing
In Sects. 9.2 and 9.6.1 the FWM process has been treated in a classical manner.
However it is clear that in a quantised electromagnetic field the FWM process, Eq.
(9.21), corresponds to the annihilation of two pump photons and the creation of a
signal and idler photon with the same total energy, and Eq. (9.22) corresponds to
conservation of photon momentum. This means that the signal and idler field must
contain the same number of photons: FWM cannot generate a signal photon without
an idler photon (or vice versa). If one then imagines turning the pump power down
sufficiently so that there is on average less than one FWM event per pulse, then the
few pulses where anything happens contain exactly one signal photon and one idler
photon. This is the basis of a heralded single photon source: the two photons are
216 W.J. Wadsworth
Fig. 9.12 (a) Output spectra for FWM (658 and 667 nm) in two different PCFs pumped with
30 ps pulses at 1,064 nm [45], (b) Output spectra and signal and idler efficiency for FWM in
PCF pumped with 200 ps pulses at 1,064 nm [43] (Parts (a) and (b) reproduced and adapted with
permission from Refs. [45] and [43] respectively)
separated (they are at different wavelengths) and one (e.g. the signal) is detected.
Detection of a single signal photon from particular pulse determines (heralds) that
there must be an idler photon from that pulse in the experiment. This idler photon
(together with others from similar sources) can then be used as the basic resource of
quantum bits (qbits) in quantum interference and quantum information experiments.

Such sources can also be realised by (2) parametric down conversion (PDC) in
which a single pump photon, instead of two, is split into two output photons. PDC
in bulk crystals has been the mainstay of single photon research for many years [47].
FWM in a fibre geometry is attractive mainly because it offers automatic selection
of a single spatial mode, and it offers relatively simple integration into fibre or
waveguide based quantum processing circuits. Pair photon generation by FWM in
the anomalous dispersion regime in conventional solid fibres has been demonstrated
around 1,550 nm [48], but there is also much research in PCF-based sources where
the pump can be at 800 nm [49–52] or 1,064 nm [53, 54], and one or both of the
generated photons can be in the 500–900 nm region where single photon detectors
are efficient, low noise and low cost. Fibre sources of single photons are potentially
subject to background photons generated by spontaneous Raman scattering. This is
avoided either by placing the generated photons very close to the pump where the
Raman cross-section is relatively small (using FWM in the anomalous dispersion
regime [48]), or by placing the idler wavelength well beyond the main Raman band
(using FWM in the normal dispersion regime [51, 53]).
9.7 Supercontinuum Generation
Supercontinuum generation takes wavelength conversion to an extreme, producing

light of an extremely broad range of wavelengths on either side of the pump
wavelength. The theoretical basis of supercontinuum generation (SCG) has been
covered in Chap. 8 and will not be repeated here. Instead this section will cover
the practical aspects of realizing some of the design goals which are indicated
from that theoretical understanding. As with pulse propagation and FWM, the
key parameter is the fibre dispersion. Usually SCG experiments use fibres with
anomalous dispersion at the pump wavelength. The discussion in Sects. 8.4.1 and
8.4.2 have already shown that this leads to the formation and subsequent fission
of ultrashort optical solitons. Remarkably, this is also the case for long input
pulses or even continuous wave SCG [55]. In these cases the FWM/MI causes
the optical intensity to be deeply modulated, and then SPM and dispersion build
solitons of different pulse duration from the peaks of the modulated intensity.
Enhancing the formation of solitons from MI-induced modulation by using an
appropriate fibre has been used to form a high peak power, long wavelength source
from a modulated diode laser seed which was then used to generate 10.5 W mid-
infrared supercontinuum spanning 0.8–4 m in a ZBLAN (fluoride glass) fibre [56].
Here the ZBLAN fibre provides transparency in the mid-infrared, and appropriate
dispersion for pumping at wavelengths close to 2 m.
218 W.J. Wadsworth
9.7.1 Simple Supercontinuum Sources
Most SCG sources employ a fs or ps modelocked laser and a fibre with a zero
dispersion wavelength, ZDW , slightly shorter than the pump wavelength giving
small anomalous dispersion at the pump wavelength. For pumping at 1,550 nm,
conventional step-index fibres are appropriate (Fig. 9.5), in particular those with
highly Ge-doped cores giving a small core diameter and relatively high nonlinearity
[57]. For pumping at 1,064 nm, PCFs provide appropriate dispersion (Fig. 9.8b) and
generate broad, flat supercontinua that extend into the visible [19, 42]. Pumping at
800 nm requires small core, high index contrast structures (Fig. 9.7b) either as PCFs
[4, 5, 9] or tapered optical fibres [10]. Figure 9.7b shows that this same approach
applies in the visible, down to pump wavelengths at 532 nm [12].
All of these sources will provide a broad spectrum at the output of the fibre,
in a single spatial mode. This is an extremely bright source in terms of mW per
nanometre spectral bandwidth per unit solid angle per unit area of the source.
Indeed, the spectral coverage is similar to the output of an incandescent lightbulb,
but because it is a directed beam, an SCG source is more than 10,000 times brighter
even for just 100 mW of total power. Such sources have obvious applications; in
photonic testing (measuring the attenuation of a single mode optical fibre over a
large spectral range requires a source with a large spectral range and sufficient power
in a single mode); spectroscopy; confocal microscopy and a range of nonlinear
spectroscopic and microscopic techniques. However not all SCG sources are good
for all applications. The details of the different processes involved in SCG require
SCG sources to be application specific for demanding applications.
The biggest issue in SCG is the fundamental pulse-to-pulse fluctuations inherent
in SCG when it arises from soliton breakup or from MI based spectral broadening.
In this context it is useful to consider FWM in the time domain as MI to emphasise
the instability. Both soliton breakup and MI are seeded from noise (Sect. 8.5) which
is necessarily random and different from pulse to pulse. This can lead to pulse-to-
pulse fluctuations in intensity of >10 % over most of a supercontinuum spectrum
(e.g. when pumped with ps to ns pulses at 1,064 nm), with fluctuations rising to
>50 % towards the edges of the continuum spectrum.
Perhaps surprisingly, this fluctuation actually imparts some useful properties
to an SCG source for some applications. As the fluctuations are caused by truly
random noise rather than systematic effects, they will average out over time with
p
the usual 1/ N dependence for N pulses (except for the very edges of the SCG
spectrum with extreme statistics [58]). This, together with the picture of an MI
based SCG containing many individual solitons at different wavelengths, suggests
that with each pulse giving a randomly different spectral structure, the average
spectrum will be smooth. This is indeed the case; long pump pulses (e.g. >1 ps)
which can be expected to produce SCG through MI, usually do give very smooth
and flat averaged spectra. With modelocked pump sources operating at 10 MHz,
the fluctuations average out rapidly, even 50 % pulse-to-pulse variation averages
to 0.5 % in 1 ms (10,000 pulses). These sources are then excellent for almost any
single point spectroscopic measurement even at high sample rates, but start to show
problems if used for 2-D high speed imaging. A 2-D image even at a relatively
low resolution contains hundreds of thousands of pixels. With a video frame rate
there are now only a few laser pulses available for each pixel and the fundamental
SCG fluctuation will begin to show up. This is potentially an issue for confocal and
other point-by-point microscopes and also for optical coherence tomography (OCT)
which aims towards one pulse per voxel data rates. Other technologies are even more
demanding, for example optical frequency metrology requires the pulse-to-pulse
phase of the laser to be carried through into the continuum ([59, 60], Chap. 6).
9.7.2 Continuum from Self Phase Modulation
Of all the processes involved in SCG, only SPM will allow deterministic, and
therefore stable, transformation of the input pulse into a continuum (see also
Sect. 8.5). SPM requires a large dI/dt so will be particularly prevalent for short pump
pulses. This was recognised experimentally in the context of frequency metrology
(early experiments with 100 fs pulsed lasers simply did not work, and shorter pulses
provided a solution) and then explained through numerical modelling [61]. In these
studies, fibres with anomalous dispersion were considered, so MI will compete with
SPM. However, in the normal dispersion regime the widely separated FWM/MI
bands are a much weaker competitor to SPM. Furthermore, it is possible to fabricate
fibres where the dispersion is always normal, there is no anomalous dispersion, so
there is no zero dispersion wavelength and hence no phasematching for FWM/MI
(Eq. 9.25). In this case only SPM broadening can occur [62]. The spectral bandwidth
may be easily estimated (Section 4.1.2 of Ref. [1]) and is usually relatively narrow.
By designing a fibre with a sufficiently low value of the normal dispersion, the pump
pulse will retain its peak intensity for a long fibre length and the SPM broadening
may extend to several hundred nanometres. It is, of course, imperative that there is
no anomalous dispersion or ZDW over the generated bandwidth and that the low
normal dispersion is maintained [62, 63].
9.7.3 Extended Wavelength Coverage in Supercontinuum
Section 8.4.1 provides a picture of SCG as a process where high order solitons break
up into multiple fundamental solitons, each of which shifts to longer wavelength
under the soliton self frequency shift (SSFS). It can also be shown that short
wavelength radiation, in the normal dispersion regime, becomes trapped by these
solitons and is shifted to even shorter wavelengths [64]. The actual short wavelength
which is trapped is determined by group velocity matching to the long wavelength
soliton. The wavelength coverage of an SCG spectrum is then defined by how far the
SSFS can take a soliton into the infrared, and how the group velocity of this soliton
220 W.J. Wadsworth
is matched to the group velocity at short wavelengths [64, 65]. At short wavelengths
the index of the guided mode is close to the core index, and also the dispersion of
silica becomes increasingly strong and is dominant over the waveguide dispersion,
so that in practice it is not possible to make large changes to the group velocity of a
fibre mode for wavelengths below 500 nm. Extension of SCG to both long and short
wavelength then relies solely on the wavelength and the group velocity of the long
wavelength SSFS shifting solitons [56, 65, 66].
Extension of the SSFS to longer wavelength is determined by attenuation and
dispersion in the fibre. Equation (9.20) shows that if a soliton loses energy, then
the soliton duration increases. The peak power suffers doubly because less energy
is then spread over a longer time. Eventually there is insufficient peak power for
the SSFS to continue. As the SSFS is based on the Raman effect, photon number
is conserved and energy is lost to vibrations of the silica matrix as the wavelength
increases. This, however, is not generally seen to be the main practical limit for
long wavelength generation. Usually the SSFS is limited by absorption in the fibre,
with rising dispersion at long wavelengths sometimes also playing a role. In silica
glass the intrinsic absorption rises to 10 dB/m at 2.7 m and 100 dB/m at
3.5 m, and the extrinsic absorption from OH impurities (usually below the ppm
level) adds absorption bands at 1.38, 2.2 and 2.76 m with strength increasing with
wavelength [67]. The long wavelength of a supercontinuum is then usually limited
to 2.4–2.6 m, but SCG in fibres with high OH content can be limited by the
2.2 or even 1.38 m OH absorption bands. Very high peak power pump pulses and
short fibre lengths mean that even the very high absorption of silicate glasses can be
overcome to produce spectra extending to beyond 3 m [68]. Other glasses, such as
fluorides, tellurites or chalcogenides, with lower intrinsic infrared absorption, have
also been used [56, 69–71] allowing extension to beyond 4 m and even as far as
4.8 m in particularly short fibres [70].
Stone and Knight [65] designed fibres to match the group index of 2.6 m
solitons to the shortest wavelengths possible and achieved short SCG wavelengths
in the 400 nm region from a 1,064 nm pump. A further constraint is that there
must be some short wavelength radiation generated initially, which is group velocity
matched to wavelengths near the pump, in order for it to be able to be swept down
to shorter wavelength by the SSFS solitons. This usually means that the pump
wavelength must be close to the ZDW of the fibre. The ideal PCF for group velocity
matching to very short wavelength would be a silica microwire type PCF (Fig. 9.6b)
with a core diameter of around 2 m. This has a ZDW close to 715 nm and is
therefore not suitable for pumping at 1,064 nm. However, it is simple to generate
715 nm by FWM or SCG from pulses at 1,064 nm, so multistage approaches have
been demonstrated to achieve visible wavelengths, either using a FWM stage to
generate 740 nm followed by SCG using the 740 nm pump [72], or using a series
of concatenated PCFs with different core diameters [73]. The limit of concatenated
fibres is, of course, a continuously varying fibre, which was demonstrated to yield
375 nm from a pump at 1,064 nm [66] and, more recently, wavelengths well below
350 nm have been generated [74].
Another technique for achieving high power at short wavelength from an infrared
source is to use dual wavelength pumping with both wavelengths far from the ZDW
that lies between them [75]. The short wavelength may be generated as the second
harmonic of the pump in a nonlinear crystal [75], or by FWM in an all-fibre device
[76]. These techniques also allow extension to below 400 nm.
9.8 Conclusion
In a single chapter it has only been possible to provide a brief introduction to

the subject of nonlinearity in optical fibres. The intention has been to provide the
reader with an understanding of the underlying principles together with a wide
ranging reference list for further information on the various topics. The nonlinear
principles themselves will be recognised by researchers familiar with nonlinearity
in bulk crystals, although there are some important changes when using the (3)
nonlinearity. Dispersion is key to nonlinearity in any system, so the majority of this
chapter has been devoted to the discussion of dispersion in optical fibres, and how
it may be changed in particular fibres.
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Chapter 10
Applications of Ultra-Intense, Short
Laser Pulses
Ken W.D. Ledingham
10.1 Introduction
Outstanding progress has been made in high power laser technology over the last
10 years, with laser powers reaching petawatt levels. At present there are 15 petawatt
lasers built or being built around the world and plans are afoot for new even higher
power lasers reaching values of exawatt or even zetawatt levels. Petawatt lasers
generate electric fields of 1012 V m1 with a large fraction of the total pulse energy
being converted to relativistic electrons with energies in excess of 1 GeV. In turn
these electrons result in the generation of beams of protons, heavy ions, neutrons
and high-energy photons. These laser driven particle beams have encouraged many
to think of carrying out experiments normally associated with conventional nuclear
accelerators and reactors. It must be acknowledged right from the outset that to
date laser driven particle beams have yet to compete favourably with conventional
nuclear accelerator generated beams in any way but in principle have the potential
of providing compact accelerators with much reduced shielding.
In this chapter there will be three sections: high intensity laser production
of electrons, protons, ions and photons, applications of ultra-high intensity laser
physics and the future of the field particularly the Extreme Light Infrastructure
(ELI), and the Photo Nuclear Pillar in Romania.
K.W.D. Ledingham ()

Department of Physics, Scottish Universities Physics Alliance (SUPA), University of Strathclyde,
Glasgow G4 0NG, UK
AWE plc, Aldermaston, Reading GG7 4PR, UK
e-mail: k.ledingham@phys.strath.ac.uk

228 K.W.D. Ledingham
10.2 High Intensity Laser Production of Electrons, Protons,

Ions and Photons
‘Is the future of conventional RF accelerators limited?’ This is the first question
one might ask, motivated by the observation that the size of such accelerators
is becoming prohibitive and the huge electric fields necessary to provide even
higher particle energies is likely to cause breakdown in the accelerator structures.
In his retiral address, Enrico Fermi suggested that a PeV accelerator would have
a circumference that would encircle the earth. Scientists are presently seeking
solutions to these problems to provide more compact accelerators. One of the
possible solutions is to use high power laser acceleration. After the invention
of the laser in 1960, the laser powers have increased dramatically and indeed
recent advances in laser technology have led to the development of compact multi-
terawatt and petawatt pulsed laser systems in many laboratories worldwide. When
focused to an area of a few tens of square microns or less, this laser radiation
can reach intensities close to 1021 W cm2 . Figure 10.1a illustrates the increase
in achievable laser intensity since 1960. Arguably the greatest advance was made
in the mid-1980s with the introduction of ‘chirped pulse amplification’ (CPA) [1].
In CPA a laser pulse of the order of femtoseconds or picoseconds is temporally
stretched by 3–4 orders of magnitude using dispersive gratings, thus preventing
damage to the laser amplifying medium resulting from non-linear processes at
high intensities. After amplification, these laser pulses are recompressed to deliver
103 –106 PW cm2 on target. Proposed techniques, including optical parametric
chirped pulse amplification, (OPCPA) (See Chap. 2 by Cerullo and Brida), [2, 3]
promise to continue to extend the boundaries of laser science in the foreseeable
future and powers of exawatts (1018 W) and zetawatts (1021 W) are being discussed.
High intensity laser radiation may now be applied in many traditional areas
of science usually reserved to nuclear accelerators and reactors. As the laser
intensity and associated electric field is increased, so does the electron quiver
energy, the energy a free electron has in the laser field – this is illustrated in
Fig. 10.1b. When laser radiation is focused onto solid and gaseous targets at
intensities >1018 W cm2 , electrons quiver with energies greater than their rest
mass (0.511 MeV) creating relativistic plasmas [4].
It is very useful to compare laser accelerators (Fig. 10.1a) with conventional
accelerators driven by alternating radio frequency electric fields (Fig. 10.1b) in the
so called Livingstone plot [6]. It should be noted that the electron beam energy of
conventional accelerators has increased by a factor of 10 every 6 years over the
last 70 years while the peak power of the laser has increased on average by an
order of magnitude every 3 years. Moreover there is a widely held view that the
Livingstone plot for conventional accelerators will flatten off above 1 TeV whereas
there is no apparent limitation for laser accelerators. It is perhaps a little naı̈ve to
compare the maximum energy of laser driven electron beams with conventional
accelerators since the existing properties of laser accelerators are still a long way
from being of interest to particle physicists. However, the present completion date
10 Applications of Ultra-Intense, Short Laser Pulses 229
Fig. 10.1 (a) Focussed laser intensity as a function of time [5]. The electron quiver energies are
indicated and as of 2006 have reached energies of 1 GeV. (b) So called Livingstone plot showing
how conventional accelerator energies have increased over the last 70 years. There is a widely held
view that the Livingstone plot will flatten off above 1 TeV – a fate not shared by laser accelerators
of the international linear collider is somewhere between 2020 and 2030 and there
is the potential for laser accelerators to play a part in the final design.
It is clear that the high power laser has emerged as a new tool for investigating
advanced physics under extreme conditions. Laser-plasma based accelerators have
the potential to deliver accelerating gradients more than 1,000 times higher than
conventional accelerator technology and on a table-top scale. When laser and
conventional accelerators are compared, one of the main differences between the
two technologies is the one of scale. This large increase in accelerating gradient for
laser technology is the key to reducing the size and associated cost over conventional
accelerators and in addition the shielding requirements are much reduced. Through
acceleration of a range of energetic particles and photons, intense laser-matter inter-
actions may induce nuclear and particle processes. This will be covered in Sect. 10.3
of this chapter. It should be emphasised that many of the applications that have been
demonstrated on very large lasers as a “proof of principle”, will soon be carried
out on the new generation of compact scale high intensity, high repetition rate lasers
being developed. Both types of lasers are necessary to advance this field of research.
10.2.1 Laser–Plasma Interaction to Produce Electrons Beams
The mechanisms involved in the interaction of charged particles with intense

electromagnetic fields have been considered for 60 years. This was one of the first
explanations suggested by the early workers to explain the origin and the energies
of cosmic rays e.g. [7]. Simply, the idea is as follows: A charged particle in an
intense electromagnetic (EM) field is accelerated initially along the direction of the
electric field. The v B force causes the particle’s path to be bent in the direction
of the travelling wave. In large fields, the particle’s velocity rapidly approaches the
velocity of light and the particle travels with the EM wave, gaining energy from it.
In astrophysical situations, the solar corona is thought to be one of the sources of
the electromagnetic waves. Charged particles that are known to exist throughout the
universe also become entrained in a long wavelength wave and galactic particles
could be accelerated to energies as high as 1019 eV. These astrophysical phenomena
were the counterparts of the terrestrial RF machines, cyclotrons, synchrotrons and
linacs, built later to accelerate particles to high energies.
In 1971 the possibility of accelerating electrons in focused laser fields was first
proposed, e.g. [8]. They showed theoretically that an electron could gain energies
as high as 30 MeV after a single pass through the focus of a diffraction limited
laser beam of power 1012 W and wavelength 1 m. The problem with this and other
early schemes is that it was not possible to maintain the required intensities over
large distances in vacuum, even with the highest energy laser systems that are in
existence today.
In the late 1970s, this problem was overcome by the seminal work of Tajima
and Dawson [9] who realized that by focusing laser light into a plasma medium,
much higher accelerating electric fields could be generated than by focusing into a
vacuum alone. They proposed the construction of a laser-electron accelerator based

on an intense laser pulse producing a wake of plasma oscillations (localised volumes
of low and high densities of electrons). Similar to a boat creating a bow wave or
wake as it moves through water, a bunch of high velocity electrons creates a wake
of plasma waves as it passes through the plasma. They demonstrated with computer
simulations that existing glass lasers, illuminating plasmas densities 1018 cm3 with
irradiances of 1018 Wcm2 could yield electrons energies of GeV energy per cm
of acceleration length. It is known that conventional accelerators are limited by
electrical breakdown to fields of about 20 MV m1 ; since at these fields the electrons
are torn from the atoms in the accelerator’s support structure. In contrast, plasmas
are already ionised gases and hence are impervious to electrical break down. Thus,
laser driven plasma particle accelerators promise fields more than a 1,000 times
greater than the most powerful conventional accelerators.
Laser light, like all electromagnetic waves, has associated with it perpendicular
electric and magnetic fields with the direction of propagation being the vector
cross product of these. For a powerful laser pulse, producing a focussed in-
tensity of I D 1020 W cm2 , the associated electric field (E) is very large and
E? D 2.7 1011 V cm1 (I D 1/2 "o cE? 2 with "o and c being the permittivity of
free space and the velocity of light respectively). This is a factor of 400 greater
than the field experienced by the electron of the hydrogen atom in its K-shell. At
the same time, the varying magnetic field (B) is also very large being close to
109 G (I D 1/2 cB2 / o , where o is the permeability of free space). This is only
a factor of 1,000 smaller than the magnetic field of a typical black hole with 2–3
solar masses. The electric field is perpendicular to the direction of propagation, and
hence no significant charged particle acceleration can take place in this direction.
However, the Lorentz force e(v B) due to the laser interacting with charged
particles, produces a longitudinal force and electrons can be accelerated in the
direction of laser propagation. It can be shown that the ponderomotive force along
the direction of the laser propagation is proportional to the gradient of E? 2 and is
equal in magnitude to the v B force. Electrons readily oscillate in the electric field
of a laser with a velocity known as the quiver velocity. For I2 > 1018 W cm2 . m
(where I is the laser intensity in W cm2 and is the laser wavelength in m) these
velocities become relativistic. The characteristic parameter (a) of this quiver motion
is the normalised momentum (p) defined by a D posc /mo c, where mo is the rest mass
of the electron [10],
p 2ı
a D posc =mo c D vosc =c D eE =mo c¨o D Iœ 1:37 1018 (10.1)
is the relativistic factor 1/[1(v/c)2]1/2 , ¨ is the laser angular frequency, I is

the laser intensity in units of W cm2 and is the laser wavelength in m. The
relativistic expression for the ponderomotive potential (Up ) using (10.1) is:
p˚
Up D mo c 2 . 1/ D mo c 2 1 C a2 1
p˚ ı
D 0:511 1 C I 2 1:37 1018 1 ŒMeV (10.2)
Assuming the electron energy distribution can be described by the relativistic

equation E2 exp(E/kT), where k is the Boltzmann constant and T is the electron
temperature, the average value of kT is found to be Up [11] and for a laser intensity
of 1020 Wcm2 using Eq. 10.2 is found to be Up 4 MeV. Wakefield acceleration
in plasmas can in fact cause the electrons to be accelerated to many times the value
of the ponderomotive potential. In early experiments, the electron spectra were
exponential in shape and up to several hundred MeV. In 2004 Nature published
three papers under the title Dream Beams where the electron spectra were quasi
monoenergetic when certain plasma conditions were met [12–14]. The highest
energy reached for electron beams with present lasers is about 1.5 GeV [15]. This
is shown in Fig. 10.2.
10.2.2 Laser Production of Proton and Ion Beams
Measurements of proton emission from laser-solid interactions have been made as

early as the 1980s using nanosecond CO2 lasers. In more recent experiments with
I2 up to 1020 W cm2 . m2 e.g. [16, 17], multi-MeV protons have been observed. In
the simple picture, at the front side of the target the laser ponderomotive force, as has
been described above, forces the electrons created by the laser-solid interaction into
the target. The ions are merely spectators at this stage but electric fields are created
by the charge separation, which then drag the ions through the target. However, the
main mechanism thought to be responsible for the generation of proton beams is the
production of electrostatic fields due to space charge effects when the fast electrons
exit the target. These fields cause surface molecules to be ionised by field emission.
The details of the interaction physics are not yet fully understood, although probably
Wilks et al. [18], have offered the most viable model to date called Target Normal
Sheath Acceleration (TNSA). Proton beams have been observed both in front of
the target (the “blow-off direction”) and behind the target (the “straight through”
direction). The hydrogen atoms responsible for the proton production are either from
the bulk hydrocarbon molecules or from water vapour and hydrocarbon impurities
on the target surfaces when solid targets are used [19]. Like the electron beams,
the energy spectra of the proton beams were exponential in shape with energies up
to 60 MeV.
As has previously been described in Sect. 10.2.1, the recent publication of the
three high profile reports (Dream Beams) on the use of laser-based accelerators
stimulated the production of high-energy quasi-monoenergetic electron beams of
good quality and heralded a new age of laser applications particularly in nuclear
and high energy physics. The logical next step in the development of laser and
target technology involved the generation of similar quality beams of other species
such as protons and heavy ions. In 2006 two papers were published [20, 21] on the
generation of mono-energetic protons.
Schwoerer and his team produced quasi-monoenergetic protons from micro-
structured targets, an idea which had been suggested earlier [22]. These authors
Fig. 10.2 (a) A laser is injected into a plasma in a 3 cm capillary tube to generate energetic
electron beams which are analysed by a magnet. (b) A graph of an electron beam reaching energies
of 1 GeV (Reproduced and adapted with permission from Ref. [15])
Fig. 10.3 (a) A laser with intensity 3 1019 W cm2 is directed onto a proton rich dot deposited
on a titanium substrate. (b) The peaked proton distribution (black dots) and a particle in cell (PIC)
simulation (black curve). The inset shows the peaked proton spectrum expected at 1021 W cm2
pointed out that the resulting proton spectrum has a strong correlation with the
spatial distribution of the protons on the target surface, as shown in Fig. 10.3a.
A terawatt laser beam is focused on the front side of a metal target generating
Fig. 10.4 An ultra-fast laser

driven microlens to focus and
energy select MeV protons.
This technique is in principal
scalable to high energy
protons [21] (a) Shows a
schematic of the microlens
device (b) The CPA2 laser
injects electrons within the
cylinder (c) These electrons
expand and induce a plasma
resulting in a radial electric
field (Reproduced and
adapted with permission
from Ref. [21])
electrons which set up a Debye sheath on the back surface – as described earlier.
Applying a small hydrogen rich dot on the back surface enhances the proton yield in
the central part of the accelerating field which is nearly homogeneous. This produces
a quasi monoenergetic bunch of protons. Figure 10.3b indicates the mono-energetic
bunch and also the PIC simulation for the laser and target conditions used in the
experiment. The inset in Fig. 10.3b estimates the proton peak energy when the laser
intensity is increased to 1021 W cm2 .
A completely different approach was adopted by Toncian et al. [21]. As shown in
Fig. 10.4, two CPA lasers were used; CPA1 produced a broad spectrum of protons
from the target which were directed through a hollow metal cylinder irradiated by a
second CPA2 laser beam.
The second laser beam causes transient focusing electric fields to be set up
in the hollow cylinder which enabled a range of proton energies to be selected from
the broad spectrum generated by the first laser beam, depending on the timing of
the two lasers and on the flight time of the ions through the cylinder. This technique
addresses two of the current drawbacks of laser accelerated proton beams: namely
their broad energy spectrum and the source divergence. A similar outcome could
more easily be achieved using small quadrupole or solenoid magnets, an approach
that is being developed by several groups including the author of this chapter.
10.3 Applications of Ultra High Intensity Laser Physics
10.3.1 Laser Induced Proton and Heavy Ion Cancer Therapy
The contributions to cancer cure from surgery, radiation therapy and chemotherapy
are about 49, 40 and 11 % respectively and the role of X-ray radiotherapy is assured
for many years in the future. However it has been known for some time that some
Fig. 10.5 This graph shows the relative radiation doses as a function of depth of tissue given by
conventional radiation treatments as well as the Bragg peak for protons
patients (as many as 10 %) would be better treated with proton and ion therapy
rather than X-rays. Hadrontherapy is a form of radiotherapy that uses protons,
carbon and other heavy ions to irradiate cancerous tumours. The use of protons
and carbon ions in radiotherapy has several advantages to the more widely used
X-ray radiotherapy. Firstly, the proton beam scattering from the atomic electrons is
greatly reduced, and thus, there is less irradiation of healthy tissues in the vicinity
of the tumour. Secondly the well-known Bragg peak for ions, where the energy loss
dE/dx increases dramatically near the end of its path, can be used to good effect to
coincide with the location of the tumour causing the deposition of the largest fraction
of energy inside the tumour. The Bragg peak results in very little radiation being
deposited after the tumour (spatially) and the oxygen enhancement ratio (OER), as
well as the radiation toxicity, are also reduced compared to X-ray radiotherapy. This
is precisely what is required when passing through healthy tissue. This is shown in
Fig. 10.5 below.
In recent years a number of papers discussing the potential for laser hadron
therapy have been published e.g. [23–27]. These authors point out that proton
beams with the required parameters can already be obtained using conventional
accelerators of charged particles (synchrotrons, cyclotrons and linacs). There are
a number of conventional accelerators being built for hadrontherapy in Europe,
America and Japan and two in particular at Heidelberg and in Italy will treat
several thousand patients per annum. Alternatively the potential use of a laser-
based accelerator is attractive for three reasons: it is compact, requires less radiation
shielding and a large expensive positioning gantry is no longer required. Very

recently it has been realized that the simultaneous production of imaging beams
is easier to achieve with laser technology than with conventional accelerator
technology.
A possible way of using a laser accelerator can be envisaged as follows. The
laser interacts with a target, generating energetic ions which irradiate the tumour.
Simultaneously produced electrons and energetic photons must be eliminated. This
laser accelerator will produce broad energetic ion beams which may be used to
some advantage since, with conventional accelerators, the monoenergetic beams
must be broadened to match the size of the tumour, before being used in therapy. It
is expected that monochromatic beams with energies up to 250 MeV with a width
of a few MeV will be produced by future lasers with intensities of up to 109–10
protons per second. At the time of writing, the highest proton energies that had been
generated by high intensity lasers is about 60 MeV. These energies are sufficient for
treating tumours in the eye. Proton therapy for deep-sited tumours requires proton
beams of about 200 MeV.
“What will it take for laser driven proton accelerators to be applied to tumor
therapy”, has recently been discussed [28]. These authors recognize that after
many years of development using conventional accelerators, clinicians are gradually
accepting proton and ion-beam therapy. They acknowledge that the considerable
costs involved are used to explain the slow market penetration and possible savings
might occur if laser technology is used. At the time of writing, these authors point to
the necessary improvements facing the laser community: (i) verifying scaling laws
for proton energy with laser power (ii) improving proton flux by at least an order
of magnitude (iii) improving shot to shot reproducibility to the few percent level
(iv) development of accurate dose control and (v) addressing quality assurance and
patient safety.
Recently, estimates have been made of the costs involved in laser driven hadron
therapy as opposed to conventional accelerator hadron therapy. It must be pointed
out that these figures are only tentative and do not include very important costs e.g.
costs of medical staff [29].
The following list gives an idea of the relative costs of each facility:
1 Laser accelerator proton and ion facility $5–10 Million

2 Conventional RF proton and ion facility $50–100 Million
3 Conventional medical x-ray facility $3–5 Million
In addition, the building for a conventional cyclotron system would cost about
$40 million with no large costs for housing a laser accelerator facility.
Although we are still a long way from generating laser protons for hadron
therapy, a number of groups are experimenting with low energy laser proton sources
up to a few MeV for biological studies e.g. the demonstration of DNA double-strand
breaking in cancer cells was recently demonstrated [30].
Fig. 10.6 Accuracy of PET

in detecting lung cancer
compared with X-ray CT
scanning
10.3.2 Laser Induced Positron Emission Tomography

Isotope Production
Laser driven ion, neutron and photon beams can produce radioactive isotopes similar
to reactors and cyclotrons, but the arguments for pursuing this line are similar to
those described in Sect. 10.3.1 – namely a laser accelerator is potentially more
compact, requires less radiation shielding and perhaps less expensive to construct.
Positron Emission Tomography (PET) is a powerful medical diagnostic/imaging
technique requiring the production of short-lived (2 min ! 2 h) positron emit-
ting isotopes. The PET process involves the patient receiving an injection of a
pharmaceutical, labelled with a short-lived “C emitting source which collects in
‘active’ areas of the body such as tumours. The principal tracers used in the PET
technique are 11 C, 13 N, 15 O and 18 F. Many chemical compounds can be labelled
with positron emitting isotopes and their bio-distribution can be determined by
PET imaging as a function of time. The most commonly used radiopharmaceutical
is 2-fluoro-2-deoxyglucose, 2-[18 F]FDG. Over the last few years, the value of
PET-FDG in the management of cancer patients has been widely demonstrated.
Figure 10.6 highlights the success rate of PET in diagnosing lung cancer compared
with conventional X-ray computed tomography (CT) scanning.
One of the main factors limiting the wider use of FDG-PET imaging is the
requirement for expensive infrastructure at the heart of which lies the cyclotron and
the associated extensive radiation shielding. As was described earlier, a simplified
approach to isotope production would be to develop a miniaturised, on site resource
with capabilities similar to that of a cyclotron. Recent results show when an intense
laser beam (I >1019 W cm2 ) interacts with solid targets, beams of MeV protons
capable of producing PET isotopes are generated. A number of recent reports have
been published using the high power laser VULCAN both as a 100 terawatt laser and
a petawatt laser [31, 32]. In addition some preliminary work has also been carried
out at the 10 Hz table–top “Salle Jaune” laser at the Laboratory of Applied Optics
LOA [33], which has been calculating the strength of PET isotopes which could be
Fig. 10.7 The total activity

(front and back) generated by
a single laser pulse for both
11
C (circles) and 18 F
(triangle) as a function of
laser irradiance with pulse
energies from 15 to 300 J.
The upper and lower hatched
areas refer to typical patient
doses for C11 and F18
respectively
generated on a compact laser. The PET isotope 18 F is generated by a (p, n) reaction

on 18 O enriched (96.5 %) targets. The enriched 18 O targets were irradiated in the
form of 1.5 mL of [18 O]-H2 O placed in a 20 mm diameter stainless steel target
holder. For the production of 11 C, boron samples were used. After irradiation, the
boron targets were removed from the vacuum chamber and the 11 C activity produced
in the (p,n) reaction on 11 B was measured in the coincidence system about 2 h after
the laser shot, a safety precaution because of the high activity.
In order to determine the thickness of the primary target which generated the
highest activity sources from a (p,n) reaction, the 11 C activity generated in the
secondary 11 B targets is measured as a function of thickness. It was shown that
thin targets (1 m) provide the highest activity sources when the total activity
produced per laser shot is taken to be the sum of the back and front activities.
Figure 10.7 summarises the measurements to date in this research programme into
11
C and 18 F PET isotope production on VULCAN. By inspection of Fig 10.7 it
can be seen that if total activity scales linearly with laser intensity then radioactive
sources of clinical significance will be produced when laser intensities above
1021 Wcm2 are reached.
The results obtained at LOA [33] are arguably the more important ones to discuss
since they represent what can be done using a compact laser, which is more likely
to be the laser of choice for hospitals. Using 6 m foil targets (both plastic and
aluminium), a proton spectrum with energies of up to 10 MeV can be generated
with the laser intensity of 6 1019 Wcm2 as is shown in Fig. 10.8.
The pulse energy on target was approximately 1 J in 40 fs. This spectrum was
used to calculate the expected activities of 11 C and 18 F. This indicated that activities
between 2 and 12 Bq could be generated per shot. Thus the LOA laser at pulse
repetition rates of 1 kHz could generate between 300 and 1,300 MBq in 30 min.
This is sufficient for in-situ production since the typical patient dose is 200 MBq.
One interesting fact that can be tentatively drawn from a comparison between the
activities gained on VULCAN and LOA is the scaling between large and compact
Fig. 10.8 The black dots are data obtained from a plastic target and the open dots from an
aluminium target. The curve represents a two dimensional PIC simulation (Reproduced and
adapted with permission from Ref. [33])
lasers at roughly the same laser intensity. For a pulse of about 300 J, the 11 C activity
per shot on VULCAN was a few 106 Bq. At LOA, for a pulse of typically 1 J, the
activity was about 10 Bq. The ratio of the activities is about 105 , with the ratio of
the energies being 300. Thus at roughly the same laser intensity, the activity scales
approximately with the square of the pulse energy.
10.3.3 Laser Driven Transmutation Studies
One of the major problems of the nuclear power industry today is the management
and disposal of high-level radioactive waste with a long half-life. Vitrified high-level
waste can be stored for about 50 years before ultimate geological disposal. However,
in many countries around the world much research effort is being expended in
the possibility of partitioning and transmuting radioactive waste, which can reduce
its toxicity by a factor of 100 e.g. [34]. Recently a number of roadmaps for
nuclear waste transmutation using GeV energy light particle beams have been
produced [35].
Although the most frequently discussed methods involve transmutation by bom-
bardment with neutrons from a reactor, there have been other suggested approaches
to this problem, for example, laser-driven high-brightness gamma generation for
photo-transmutation. It is possible to generate monochromatic gamma rays by back
scattering laser light from conventional GeV linacs or indeed laser driven GeV
electron beams (to be described later). The energy of the photons should coincide
Fig. 10.9 The laser enters

from the left interacting with
an Au target to produce
gamma rays which irradiated
the two iodine samples shown
in the right hand side of the
picture
with the maximum of the giant dipole resonance cross section for (”,n) reactions.
Initial studies have been encouraging and the experiments using the nuclear waste
isotopes 129 I and 137 Cs will be carried out in the future [36].
Transmutation studies have also been carried out at two high power laser centres,
the large single pulse laser centre at the Rutherford Laboratory and compact high
repetition rate laser centre at the University of Jena. Firstly, the experiment carried
out on VULCAN at the Rutherford Appleton Laboratory will be discussed [37]. This
involved using the petawatt laser to drive the photo-transmutation of long-lived 129 I
with a half-life of 15.7 million years to 128 I with a half-life of 25 min. A laser-
generated gamma ray is absorbed by the 129 I nucleus, which releases a neutron to
undergo transmutation to 128 I. This giant dipole resonance (”,n) reaction is observed
in 129 I and 127 I, and the absolute activities of the reaction products 128 I and 126 I were
used for the first time to determine the integrated cross-section for 129 I(”,n)128 I from
the known 127 I(”,n)126 I cross-section. The laser produced relativistic electrons then
interacted with a 4 mm thick Au target to produce high energy gamma rays. These
photons irradiated iodine samples of 85 % 129 I and 15 % 127 I as shown in Fig. 10.9.
The iodine samples were analysed using germanium detectors before and after
laser irradiation of the gold target. The background spectrum in Fig. 10.10 was
measured for 3 h and the principal lines observed resulting from the decay include
125
Sb. The background activity from the samples was of the order of 2.4 108 Bq.
Figure 10.10 shows clear peaks at 443.3 and 527.1 keV, characteristic of the decay
of 128 I. The decay rate of 128 I was determined by measuring the integrated area
under the peaks over successive time intervals. The half-lives of the 443.3 and
527.1 keV peaks were 25.8 ˙ 1.0 and 25.5 ˙ 1.5 min respectively, which agree well
with the literature value of 25.0 min. In addition, the measured ratio of the area
under the 443.3 and 527.1 keV peaks averaged over all of the measured spectra is
10.9, which is in good agreement with the literature value of 10.4. From the data,
the total activity of 128 I produced at the time of the laser shot was deduced to be
1,323 Bq. This corresponds to the production of 2.9 106 nuclei of 128 I for the
360 J laser shot.
600
128
500 I
443.3keV
400
Counts
300
200 125
Sb 128
125
428keV Sb I
100 463keV 527.1keV
128
I
0
Background
-100
400 420 440 460 480 500 520 540 560 580
Energy(keV)
Fig. 10.10 Gamma emission spectra from one of the iodine samples measured before (back-
ground) and after laser irradiation of the gold target. Characteristic emission lines of 128 I at 443.3
and 527.1 keV are clearly observed
Fig. 10.11 The laser is

directed at a helium gas jet
and the fast electrons
generated interacted with a
thick high Z bremsstrahlung
target and then into the iodine
target. This arrangement was
more efficient for nuclear
reaction production than
aiming the laser directly on
the solid target (Reproduced
and adapted with permission
from Ref. [38])
A transmutation experiment was also carried out at the compact high repetition
laser JETI at the University of Jena using the same iodine sources [38]. The Jena
multi TW laser system generates pulses with an energy of 1 J, <80 fs pulse width,
at a repetition rate of 10 Hz with a centre wavelength of 800 nm. The laser pulses
facilitate the intensities of up to 1020 W cm2 within a focal area of 5 m2 . This
is directed onto a helium gas jet to produce an electron beam and then directed at a
high Z target to produce a bremsstrahlung beam as shown in Fig. 10.11. The nuclear
reaction rate in 129 I was increased by two orders of magnitude by striking a helium
gas jet in front of the thick high Z bremsstrahlung target, compared against striking
the high Z target directly with the laser beam [38].
By comparing the two experiments at VULCAN (300 J) and Jena (1 J) with

similar laser intensities but with very different laser pulse energies (EL ) there
appears to be an EL 2 energy dependence of the nuclear reaction rate. It has been
realised that such a comparison is naı̈ve since the pulse widths and focal radii are
very different, however, it does indicate that in order to obtain similar reaction rates
with a compact laser many laser shots must be integrated.
10.4 The Future of Ultra High Intensity Laser Physics

Particularly ELI and the Photo Nuclear Pillar
in Romania
10.4.1 The Production of Laser Induced High Energy Photons
In this section we shall develop laser acceleration a stage further and investigate
what happens when conventional RF accelerators or laser driven electron accel-
erators are coupled with high power lasers. This is likely to be a very important
development for ELI- Nuclear Physics.
The interaction of optical photon and electron beams is a process called Thomson
scattering when the photons have energies much smaller than the rest energy of the
electron (mo c2 ), or Compton scattering if the photon’s energy is mo c2 .
Figure 10.12 illustrates how backscattered photons are produced. To get the
maximum energy of scattered X-rays, the electron and photon beams are directed
towards each other head on. The photons scatter off the electrons at 180ı with energy
(! max ) given by the following simple equation if the laser beam is only moderately
intense – in other words linear Thomson scattering:
ı
!max D !laser 4 2 1 C 2 2 (10.3)
where is (Ee /mc2 C 1) with Ee being the electron energy, ! laser is the laser photon
energy, is the usually small angle between the electron beam direction and the
angle of observation. The photons are thus backscattered and are Doppler shifted
into the X-ray or gamma-ray part of the spectrum.
At the FZD facility in Dresden there exists all the instrumentation for carrying
out this type of experimentation. The linac Elbe at 40 MeV, is 40/0.511 C 1 D 79.
Elaser is 800 nm D 1.6 eV and hence the back scattered photons have energies
38 keV. The arrangement of the electron and photon beams interacting in the
newly constructed high vacuum target chamber in the Elbe beam vault is shown
in Fig. 10.13.
If the laser beam is sufficiently intense then a more complicated nonlinear process
takes place described by the equation ! sc D n! laser 2 2 (1cos')/(1 C ao 2 /2 C 2 2 ),
where n is the number of laser photon absorbed by the electron. The term ao is a
dimensionless quantity indicating the strength of the laser intensity. n can take
Fig. 10.12 A typical arrangement for detecting back scattered X-rays. The electron and photon
beams interact (180ı ) as shown and the X-rays continue through a pinhole in a focusing
parabola and are detected by a germanium detector (Reproduced and adapted with permission
from Ref. [39])
Fig. 10.13 Photograph showing how the Elbe electron beam couples to the photons from the
DRACO laser in the backscattering chamber
any integral value to produce a series of harmonics, although the ao term in the
denominator reduces the maximum X-ray energy (red-shift) for n D 1. This is
shown in Fig 10.14.
The most important application for backscattered monochromatic x-rays in the
range of 20–50 keV is in phase contrast imaging particularly for medical purposes.
Fig. 10.14 This diagram

shows the number of
backscattered photons from
the 40 MeV Elbe linac
interaction with a laser beam
of about 1018 W/cm2 at
œ D 800 nm. The nonlinear
harmonic peaks occur at
twice and three times the
original energy [40]
The Thomson back scattered photons scale as the square of the electron beam
energy and so if we have GeV electrons with a 2 value of about 4 106 , the
energy of the back scattered photons is about 20 MeV. Thus we are getting into the
MeV monochromatic photon regime where applications to nuclear physics become
important. These GeV electrons can be produced by a laser wakefield accelerator.
10.4.2 Description of the ELI Project
ELI at present is the only funded European and International Centre for high-
level research on ultra-high intensity laser, laser-matter interaction and secondary
sources with unparalleled possibilities. Its pulse peak power and ultra-short pulses
will go beyond the current state-of-the-art by several orders of magnitude. Because
of its unique properties, this multidisciplinary facility will provide outstanding
new opportunities to study the fundamental processes unfolded during light-matter
interaction.
The ELI project, which is being co-ordinated by Gerard Mourou, is a collabora-
tion between 13 European countries and will consist of four pillars:
1. High Energy Beam Science devoted to the development and usage of dedicated
beam lines with ultra-short pulses of high energy radiation and particles reaching
almost the speed of light (100 GeV). This part of ELI will be realized in Prague
(Czech Republic).
2. Attosecond Laser Science designed to conduct temporal investigation of elec-
tron dynamics in atoms, molecules, plasmas and solids on the attosecond scale
(10 18 s). Szeged (Hungary) will host the short pulse pillar of ELI.
3. Laser-based Nuclear Physics: The third site in Magurele (near Bucharest/
Romania) will focus on laser-based nuclear physics. While atomic processes
are well suited to the visible or near visible laser radiation, as a third pillar
ELI-NP will generate radiation and particle beams with much higher energies
and brilliances suited to studies of nuclear and fundamental processes.
4. Ultra High Field Science will explore relativistic laser-matter interaction in an
energy range where totally new phenomena, like radiation dominated interac-
tions, become dominant. The decision on the location of the technologically most
challenging pillar will be taken in 2012 after validation of the technology.
10.4.3 The Scientific Case for ELI-Nuclear Physics
The ELI-NP pillar will be the only laser facility in the world that will be solely
dedicated to the study of laser driven nuclear processes both at a fundamental level
but also with applications in mind. For ELI-NP two new central instruments are
planned:
1. A very high intensity laser, where three 10 PW Apollon lasers are coher-
ently added to yield a high intensity of 1,024 W/cm2 or electrical fields of
2 1,015 V/m. This is close to four orders more powerful than any existing laser.
2. A very intense, brilliant ” beam (E” 19 MeV), which is obtained by incoherent
Compton back scattering of direct laser light or laser light from a super cavity off
a very brilliant, intense, classical electron beam of GeV energy or laser driven
electron beam.
The ” beam will have unique properties in world-wide comparison and opens
new possibilities for high resolution spectroscopy at higher nuclear excitation
energies. They will lead to a better understanding of nuclear structure at higher
excitation energies with many doorway states, their damping widths, and chaotic
behaviour, but also new fluctuating properties in the time and energy domain. The
detailed investigation of the pygmy dipole resonance above and below the particle
threshold is very essential for nucleosynthesis in astrophysics. In ion acceleration
the high power laser permits the production of 1015 times higher density ion beams
than is achievable with classical RF accelerators. This will permit for the first time,
a possible fission-fusion reaction mechanism that can then be used to produce very
neutron-rich heavy nuclei. These nuclei will permit the investigation of the N D 126
waiting point of the r-process in nucleosynthesis. With this type of new laser acceler-
ation mechanism, very significant contributions to one of the fundamental problems
of astrophysics, the production of the heavy elements beyond iron in the universe,
can be addressed. According to a recent report by the National Research Council
of the National Academy of Science (USA), the origin of the heaviest elements
remains one of the 11 greatest unanswered questions of modern physics [41].
The ” beam also opens many new possibilities for applications. The ” beam
itself can be used to map the isotope distributions of radioactive waste remotely
via Nuclear Resonance Fluorescence (NRF) of radioactive waste [42]. At lower
energies around 100 keV the high resolution of the beam is very important for
protein structural analysis. In addition we want to produce low energy, brilliant,
intense neutron beams and low energy, brilliant, intense positron beams, which open
new fields in material science and life sciences. The possibility of studying the same
target with these very different brilliant beams will be unique and advance science
much faster.
The high power laser allows for intensities of up to 1024 W cm2 . Here very
interesting synergies are achievable with the ” beam and the brilliant high energy
electron beam, which will allow the study of new fundamental processes in high
field QED. When the ” beam is injected into the focus of the high intensity laser,
which in this special case consists of a standing electric-field of two focused lasers,
the most recent non-perturbative QED calculations predict that one can observe
already, at 1024 W cm2 , the catalytic pair creation from the vacuum [43]. If
confirmed, this would constitute a very basic non-perturbative textbook QED result.
Also, the radiation damping theory could be tested very accurately with the very
brilliant electron beam injected into the laser focus. Here reflected high-energy ”
quanta and cascades of e C e pairs could be studied as a function of the ” factor
of the electron beam and the laser field strength. While the predictions for radiation
damping will probably be correct in the perturbative regime, the different theoretical
approximations can be tested very sensitively for nonlinear radiation damping. On
the other hand, the central questions of high-field QED for the ultra-relativistic laser-
plasma interaction with I > 1024 W cm2 will be the subject covered by the fourth
pillar of ELI.
10.5 Conclusions
In this chapter some of the emerging applications of ultra-intense, short laser

pulses were reviewed. In particular, the use of high power lasers for producing
beams of particles such as electrons, protons and ions were discussed. Potential
applications for such beams, particularly in the areas of cancer therapy and PET
isotope production were outlined. Finally, a brief outline of the European ELI
project was given – a European project which brings together 13 European countries
working in areas such as high energy beam science, attosecond laser science, laser-
based nuclear physics and ultra-high field science.
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Chapter 11
Utilising Ultrafast Lasers for Multiphoton
Biomedical Imaging
Erich E. Hoover, Eric V. Chandler, Jeffrey J. Field, Dawn N. Vitek,

Michael D. Young, and Jeff A. Squier
11.1 Introduction
Laser scanning multiphoton microscopy is a powerful tool for producing high-

resolution (<1 m laterally and axially), three-dimensional images of biological
specimens. The utility of the multiphoton approach is derived from several key
advantages that include, but are by no means limited to, these specific facts:
1. The excitation is confined to the focal plane, limiting out-of-focus bleaching.
2. Near-infrared wavelengths are used for excitation, and these wavelengths tend to
be less damaging and deeper penetrating in biological systems.
3. No detection pinhole is required, meaning that scattered signal photons can still
contribute to the image contrast in a meaningful way.
4. Endogenous non-bleaching contrast mechanisms, such as second harmonic
generation (SHG) and third harmonic generation (THG), can be readily accessed.
These aspects of multiphoton imaging (and others) have made this technique the
tool of choice for the biological research community. As such, there has been a
tremendous amount of development in terms of the ultrafast optical technology that
is employed in the biological microscope. The intent of this chapter is not to provide
a review of the field (there are presently multiple review articles in the literature
that provide a comprehensive overview [1–6]); but rather we highlight some of the
very pragmatic aspects needed to design a laser scanning multiphoton microscope
(e.g. scan and collection optics and the effects of bleaching), discuss a novel
method for improving the sectioning in the limit of wide-fields (spatio-temporal
focusing), and finally, explore how to optimise detection in the limit of weak signals
(single molecule multiphoton spectroscopy and photon counting). This last point is
E.E. Hoover () • E.V. Chandler • J.J. Field • D.N. Vitek • M.D. Young • J.A. Squier ()
Center for Microintegrated Optics for Advanced Bioimaging and Control, Department of Physics,
Colorado School of Mines, Golden, CO 80401, USA
e-mail: ehoover@mines.edu; jsquier@mines.edu

252 E.E. Hoover et al.
particularly exciting. By moving to a photon counting detection scheme, new design

degrees of freedom have been created. This freedom has made it possible to simul-
taneously image multiple focal planes within scattering specimens for the first time.
11.2 The Basic Microscope
11.2.1 System Architecture
The basic multiphoton imaging system is quite straight forward and essentially
consists of four components: (1) the laser source, (2) the scanning system, (3) the
microscope platform, and (4) the detection system. Starting with the first com-
ponent, the laser, the most common ultrafast source for this application is the
Ti:sapphire laser, owing to its broad wavelength range (700–1,100 nm) and high
average power capability (>1 W). The tuning range is particularly desirable from
the point-of-view of being able to selectively excite different fluorophores when
performing two-photon excitation fluorescence (TPEF) imaging. In addition, the
average power capability can be usefully exploited in several ways. Given the
average repetition rates of these lasers, which is typically on the order of tens of
megahertz (MHz), the per pulse energy translates into tens of nanojoules (nJ). This
energy makes it possible to image deeply (up to about a millimetre) into scattering
specimens, or quickly (30 frames per second and higher) – the energy can be
distributed over multiple focal points decreasing the scan time needed to complete
a field-of-view.
In terms of scanning (the second component), multiple strategies are used –
the exact choice being dependent upon the system being studied. The beam can
be rastered across the specimen (beam scanning); the specimen can be scanned
about the excitation beam (specimen scanning); or, in the case of non-scattering
specimens, a wide-field approach can be employed – which eliminates or requires
minimal beam scanning. Sometimes several of these approaches are combined
together to create the most optimal exposure conditions possible for exploring and
studying the biological system under consideration. Basic beam scanning for single
and multiple beam geometries is discussed in Sect. 11.3, while a wide-field approach
using spatio-temporal focusing is detailed in Sect. 11.6.1.
The scanning system couples the ultrafast laser source to the microscope
platform – the third component. The platform can be a commercially available
microscope or a home-built unit. It provides delivery of the excitation light to the
specimen and simultaneously collects and routes the signal photons to the detection
system. Often a pathway for separately viewing the specimen with a white light
source either through an eyepiece, a camera, or both is incorporated. In the next
section, we will explore the characteristics of the objective – the most important
component in the microscope platform.
The fourth and final component of the multiphoton imaging system is the
detector, which is used to capture precious signal photons with the highest possible
11 Utilising Ultrafast Lasers for Multiphoton Biomedical Imaging 253
Fig. 11.1 A 1.2 NA, 40X water immersion objective with correction collar (left) for use with a
cover slip, and a 0.80 NA, 40X water immersion objective that requires no cover slip (right)
efficiency. Normally, a single element detector is employed such as a photomulti-

plier tube (PMT). The PMT has the desirable characteristics of good efficiency, high
gain, and low noise. In Sect. 11.6.2 we discuss a relative newcomer to single element
detection now being used in multiphoton microscopy, namely photon-counting.
This modality is particularly applicable for low signal-light levels and, thanks
to inexpensive technologies such as field programmable gate arrays, is becoming
increasingly straightforward to implement.
11.2.2 How to Read a Microscope Objective
A good starting point in the design of a multiphoton imaging system is the objective
lens, and as such it is important to be able to read and understand the characteristics
of the optic.
Figure 11.1 depicts two different objectives for use under different imaging
conditions. First, note the band about the barrel of both objectives. The colour
denotes the rough magnification, the exact magnification being imprinted directly on
the side of the objective. Different coloured bands denote different magnifications
and serve as a simple way of quickly identifying the degree of magnification. The
objective on the right has an additional white band denoting that this objective can
be used in water, and in this case, without a cover slip. The marking located on the
side of the barrel is used to indicate that no cover slip is necessary. The ‘0’ indicates
that the objective requires a zero thickness cover slip, while the infinity sign denotes
that this is an infinity-corrected objective. In other words, the lens will produce the
least abberated image when the image is at infinity. A second lens, known as a tube
lens, must therefore be used in conjunction with an infinity-corrected lens to create
a real image.
The objective on the left has a similar marking on the side of the barrel:
1 D 0.14 0.18. Again, the infinity sign denotes it is an infinity-corrected objec-
tive, but in this case, a cover slip must be used in conjunction with the objective.
For this objective the cover slip size can range from 0.14 to 0.18 m in thickness.
The grooved correction collar must be adjusted accordingly to match the desired
thickness. Finally, the numerical aperture (NA) is always recorded on the side of the
objective. For the objective shown on the left, the NA is 1.2, and for the objective
on the right the NA is 0.80. The NA describes how tightly the excitation beam
will be focused and is key to determining the resolution that can be achieved with
the objective – the higher the NA, the better the resolution. Specifically, the NA is
defined as:
NA D n sin .˛/
where n is the index of refraction of the medium in which the beam is focused, and
˛ is the half angle of the cone of light (semi-aperture angle) produced at focus.
11.2.3 Focusing of Ultrashort Pulses with High NA Optics
As the contrast mechanisms in multiphoton microscopy all scale with the excitation
intensity to the power of two or greater, it is important to ensure a short pulse is
created at the focus of the objective to obtain efficient high-resolution imaging.
Optimally, at focus the pulse should be diffraction-limited in space and transform-
limited in time in order to produce the highest intensity. Complications often occur
with refractive optics which prevent either one or both of these conditions from
being satisfied. For example, multi-element objectives (and the scan optics) are
sufficiently long, from an optical path length point-of-view, that there is significant
dispersion. This dispersion causes the pulse to be stretched in time (“chirped”) and
become no longer transform-limited. This dispersion lowers the excitation intensity
and hence also the efficiency at which a particular nonlinearity is driven. There
are multiple strategies for addressing dispersion, all of which involve simply “pre-
chirping” the pulse. When pre-chirping, the pulse is pre-stretched with the opposite
sign of chirp compared to what is produced by the imaging system. The result of
this is that at focus, the system dispersion is effectively cancelled and a transform-
limited pulse is produced. Strategies for effective dispersion compensation and
measuring the pulse-width at the focal plane of the objective are well documented
[4, 6] and will not be covered any further within the context of this chapter.
They are however an important consideration for the end-user of any multiphoton
imaging system, and as such should not be neglected in the final system design and
implementation.
11.3 Scan Optics
11.3.1 Design of a Basic Single Beam Scan System
The key principle behind the construction of a scan system for a laser scanning
microscope is the concept of the telecentric plane. A telecentric plane occurs when
the back of the objective is image relayed in the beam path (any location where the
marginal rays and the chief ray are parallel for all scan parameters). It is relatively
easy to design such a telecentric scan system by working backwards (from the
objective toward the laser) with an off-axis beam. Anywhere where the chief ray of
this off-axis beam crosses the origin is where the telecentric planes exist. All of the
beam-modifying elements should be located at these positions in order to produce a
good scan system. The majority of scan systems utilise galvanometric scan mirrors,
due to their high optical throughput, but a variety of other technologies exist and
follow the same principle.
Figure 11.2 shows the two most common telecentric scanning systems, though
many other valid configurations exist. While the majority of scanning systems put
the true telecentric plane between the scan mirrors, such a system does not provide
for the best performance. In a scan system where the telecentric plane is located
between the two mirrors (Fig. 11.2a) a situation results where the centre of the
beam does not perfectly hit the centre of the mirror closest to the objective. This
problem is exacerbated when a large tilt is applied to the mirror further from the
objective. An ideal scan system places a telecentric plane at each mirror [7], relaying
the plane from one mirror to the other, but comes at the cost of two additional lenses
(Fig. 11.2b). This sacrifice is important for multifocal systems and systems with
axial beam scanning, since these techniques have beams that are not perfectly on-
axis going into the first scan mirror.
11.3.2 Design of a Multifocal Scan System
In a multifocal scan system, the multiple beams need to be overlapped on the back
of the objective, which results in laterally separated beams at the focus. To produce
such a system, it is necessary to image relay the back of the objective through the
scan mirror system, thereby placing a telecentric plane at each scan mirror. With this
configuration (Fig. 11.3) it is possible to produce overlapped beams at the back of
the objective by overlapping the beams on the first scan mirror. While it is possible
to build a multifocal scan system using a single telecentric plane placed between the
two scan mirrors, such a system will not scan exactly the same size region for each
beam and is consequently less desirable.
It is important to note that not all multifocal systems are combined with an
external scan system. A rotating disk microlens array [8, 9] is a good example of
such an alternative system. In such a system the microlenses are placed so that
Fig. 11.2 Beam scanning

system configuration – most
scan setups put the telecentric
plane between the two scan
mirrors and try to place the
mirrors as close together as
possible (a), an ideal scan
system has a telecentric plane
at each scan mirror (b)
Fig. 11.3 A simple two-beam ideal multifocal scan system
rotation of the disk is designed to reach the different regions of the focal plane,
requiring fewer optics to produce the scan system. However, this type of scan
system does not produce a traditional square uniformly-illuminated scan region and
is therefore non-ideal for many imaging applications [9].
Fig. 11.4 A remote focusing system for adjusting the axial focal plane position
11.3.3 Moving the Beam Axially
Moving the axial position of the focal plane is another important issue to consider
when constructing a scan system. Traditional systems accomplish this task by either
moving the sample or the objective, which can be disruptive to the sample and
does not permit rapid scanning. These challenges can be overcome by utilising the
remote focusing technique [10], which relays the telecentric plane at the back of the
objective to a secondary objective focused onto a piezoelectric mirror (Fig. 11.4).
This technique permits the rapid movement of the axial position of the focal plane
by adjusting the divergence of the beam at the back of the objective through moving
the piezo mirror back and forth.
Since the beam divergence can vary drastically depending on the piezo position,
it is important when constructing such a scan system to take into account the
potentially large size of the beam at all of the optics between the two objectives.
Most optical systems are designed to operate with collimated beams over the
majority of the scan system, where a remote focusing system only has a collimated
beam when the piezo mirror is exactly at the focus of the matched objective. This
situation places significant restrictions on the distance between the different optical
elements – a system with too much space between elements will cause the beam to
be clipped for some piezo positions.
11.4 Pragmatic Collection Optics
Since the 1960s, with the advent of computers, the task of lens design has greatly
shifted. A cursory examination of lens design books prior to the 1960s [11, 12] will
show the laborious process involved in calculating the aberrations introduced by
an optical system. Now, computers can quickly and accurately calculate the Seidel
coefficients and even other higher order terms. Despite the great advantages which
computers afford the design process, the design of a custom optical element or
system cannot simply be left to a computer. In the computer’s attempt to optimise
a set of variables on the target parameters, the design may settle into local minima
(of the merit function), which are not ideal and often non-physical.
It is still the role of the lens designer or optical engineer to find an appropriate
and promising initial optical configuration. In this section we will walk through the
design of a simple non-imaging optical component and demonstrate some of the
key general principles of optical design and also the advantage of custom optics for
specific applications [13]. For our design we wish to create a simple optical system
that will collect endogenously produced light from a sample and relay it to the active
area of a point detector, such as a PMT.
11.4.1 Target Specifications
Our first-order system properties are:

• Object-space NA is 0.95 or greater,
• Field of view is 0.707 mm (0.5 mm 0.5 mm square),
• Wavelength range is from 350 to 600 nm,
• Front focal length is at least 0.5 mm, so as to collect through a cover slip
(170 mm) and still have at least a 150 mm working distance, and
• The total track (the distance from the focal plane to the detector) of the system is
less than 75 mm, in order to be comparable to a commercial objective.
Our imaging requirements are:
• The image-space spot-size is less than 4 mm for the geometric radius.
Other special considerations are:
• This system must include as few optical elements as possible, ideally three
elements or less,
• At some point along the optical path the rays must be collimated to allow for
interference filters, and
• Only off-the-shelf lenses should be used.
11.4.2 Design Process
Optics literature, such as text books [14–17] and scholarly articles [18, 19], may
provide a good starting point that meets some of our design requirements [13].
One example of such a system is called the substage condenser, which is used to
relay light from a source in such a way that it uniformly illuminates the sample and
matches the cone of light defined by the objective’s NA. The simplest condenser
Fig. 11.5 Schematic diagram

of an Abbe two-lens
condenser
systems involve no lenses and instead utilise only a concave mirror to illuminate
the sample plane. Such a system can fill objectives of small numerical aperture
(about 0.25).
Substage condensers may contain any number of lenses, but one of the simplest
demonstrated designs is the Abbe two-lens condenser (Fig. 11.5), which can
accommodate an objective with a numerical aperture up to 1.2 [15]. By reversing
the design of the Abbe condenser, so that it collects light generated at the specimen
rather than focusing light into the specimen, we have a good starting place for our
initial design. In some ways we may consider this configuration to be a two-lens
infinity-corrected objective. In order to focus this collimated light onto the detection
surface of a point detector, we require an additional singlet to function as a tube lens.
11.4.2.1 Lens Selection
Since we are not interested in designing custom lenses, it is important to have a

suitable set of lenses with which to experiment. We can narrow the number of
possible lenses greatly by eliminating those which are not suitable for ultraviolet
wavelengths. Also, we wish to a have a short total track, as defined in the target
specifications, so that the resulting custom optic will fit in the same space as a
commercial objective. In order to achieve these requirements all of our optics must
have a focal length of about an inch or less. In this case we are going to use two
plano-convex sapphire lenses with an inch focal length, one for the second lens in
the condenser and the other as the tube lens.
Choosing the first lens for our system is actually the most difficult. We want to
balance many of the properties of that first optic to achieve the highest possible NA,
obtain a long working distance, and be able to relay the light to the subsequent optic.
The short focal length would imply a small radius of curvature at least on one side
of the optic. This limits the overall diameter of the optic, even though a large optical
diameter helps to accommodate a long working distance. If the NA is too high, rays
that emanate from our sample at the most extreme angles may reflect off the surface
Fig. 11.6 Common oil

immersion objective
of our first optic. A solution to this would be using a meniscus lens. However, a
meniscus lens may not have a sufficiently short focal length to relay the light to our
next optic. Normally this is remedied by a series of meniscus lenses which slowly
bend the rays into a desired configuration, but we wish to avoid using more than
three lenses total. In this case we are going to use a bi-convex aspheric lens made
from B270 glass with a 12 mm focal length and an 18 mm diameter. This by no
means represents an exhaustive search of available lenses; however, such a setup
will be shown to be suitable for our design. Examining basic designs for objectives
also provides us with a better understanding and familiarity for what designs do and
do not work. Many of these considerations may be identified in Fig. 11.6. In this
figure an initial optic with a small radius of curvature is followed by a meniscus
lens in order to gradually bend the light onto a pair of achromats, providing good
performance across a broad range of colours [15].
If a lens is found to be ultimately unsuitable, then we return to this step and
try another option, such as favouring something with a smaller diameter but a
shorter focal length. It is important to understand which parameters are going to
be most important to meeting the target specifications and which can be adjusted
or sacrificed. Often the best way to gain a familiarity with what works is to try a
variety of lenses and options. Fortunately, computer aided design programs often
contain lens catalogues from typical providers and make it easy and straightforward
to substitute different lenses into a simulated design.
11.4.2.2 Paraxial Design
As an initial attempt at the design, we can use the paraxial ray tracing equations
for thin lenses first and then try thick lenses. It is worth mentioning that there
are obvious and significant problems with this approach. Since we are designing
a relatively small optic in terms of total length relative to optic diameter, the thin
lens approximation is poor. Due to our requirement for a very high NA, the paraxial
Fig. 11.7 Paraxial designs for (a) A thin lens system and (b) A thick lens system
approximations for small angles (sin() ) are also quite poor [20]. Despite these
bad assumptions we can still proceed, since we simply wish to create a rough initial
configuration that can be entered into a computer design program. Once we have a
rough configuration, we can adjust by eye and then allow the software to create a
more optimised configuration.
After plugging the numbers, the thin lens calculations give us a very simple
design (Fig. 11.7a). Unfortunately, it is obvious that the thin lens approximation
does not give us a clear picture of how the system should be constructed. However,
the thick lens paraxial approximation gives us a much more reasonable starting
point, since we can start to see some physically realisable distances between
elements (Fig. 11.7b).
11.4.2.3 Computer Aided Design
Starting from the estimates produced from the thick lens paraxial design, we can
now enter the design into a computer aided program. Once these parameters are
entered, we can ray trace the system utilising real lenses (Fig. 11.8).
11.4.2.4 Optimisation
Now that our initial design is entered into the software we can optimise further
by giving the software some variables to adjust. The lens spacings and total track
length are our only variables that we can attempt to optimise. Optimising on
these parameters, we can find a good solution (Fig. 11.9a) by requesting that the
software minimise the final spot size (Fig. 11.9b) and collimate the rays between
the condenser and tube lenses. Considering all of the approximations made in our
first order paraxial design, it is quite remarkable that this design implemented with
real lenses (Fig. 11.8) comes so close to our optimised design (Fig. 11.9a).
Before we finish we can attempt to push the limits of this design to see how
much of the light we can really capture. We can explore this limit by increasing
the numerical aperture until the point just before the software starts to lose rays
(Fig. 11.10a). It is also informative to take a look at water immersion of the objective
Fig. 11.8 Initial computer aided design
(Fig. 11.10b), which demonstrates an even better collimation than the air-immersion
objective.
Finally, as a last check, we can test our design to ensure that it can handle the
requisite wavelength range and field of view. Figure 11.11a shows that the rays still
hit our target for all desired wavelengths, even at the edge of our field of view,
where Fig. 11.11b demonstrates that we retain all the rays on the detector even at
this extremum.
11.4.3 Design Results
In review, Table 11.1 shows how we met or exceeded all of our target specifications.
This design is not really a condenser or a traditional objective; rather it may be
considered a measurement objective, since it is just designed to collect light and
relay it to a PMT. Whatever the case may be, it is a good example of pragmatic
optics. Pragmatic optics allow us to sacrifice many of the qualities of expensive
optical components by realising what is important to our specific design and only
focusing on those attributes. Such an attitude can potentially translate into a less
expensive optic that offers a substantial gain in performance.
Fig. 11.9 (a) Optimised computer design at 0.95 NA (b) Optimised spot size
Fig. 11.10 Computer aided design at 0.97 NA (a) Air immersion. (b) Water immersion
Fig. 11.11 Final design with full spectrum and at extreme point on field of view. (a) Worst case
layout. (b) Spot diagram for worst case layout
Table 11.1 Specification Target value Design value

target and actual values
Object space NA 0.95 0.97
Field of view 0.707 mm 0.707 mm
Wavelength range 350–600 nm 350–600 nm
Front focal length 0.50 mm 1.20 mm
Total track <75 mm 70 mm
Image spot size <4 mm 1.75 mm
Number of optical elements 3 3
Collimation Needed Provided
Stock lenses Needed Provided
11.5 Optimising Fluorescence Yield in the Presence

of Bleaching
Photobleaching of fluorescent markers, a reduction in the flux of photons emitted

by a fluorophore during continual or repeated excitation, is an undesirable yet
unavoidable phenomenon in all forms of fluorescence imaging. Aside from the
obvious disadvantage that specimens, especially biological systems, cannot be
viewed for arbitrary lengths of time, photobleaching causes a reduction in the overall
signal-to-noise ratio (SNR) in acquired images. This reduction in SNR is responsible
for a loss in spatial resolution as well, due to the Poisson-statistical nature of
photons [21]. Therefore, while photobleaching can be useful in determining several
parameters of a specimen, such as diffusion rates in fluorescence recovery after
photobleaching (FRAP) [22]; it is, in general, a limitation to most fluorescence
microscopy assays.
As we have already seen, two photon absorption (TPA) is limited to only the
focal plane of the excitation objective. Unlike confocal microscopy, in which linear
fluorescence occurs over the entire volume of the laser beam within the specimen,
this limits the region of photobleaching to only the volume in which TPA occurs.
The advantage of this localisation of photobleaching is that areas in a three-
dimensional specimen that are not under excitation experience no photobleaching
prior to data collection (i.e., there is no out-of-focus photobleaching). In contrast,
confocal microscopes suffer from photobleaching in regions of the specimen in
which data is not being taken, resulting in significantly degraded images when
scanning a three-dimensional specimen. Unfortunately, this advantage of two-
photon laser scanning microscopy (TPLSM) does not come without a cost –
several studies have shown that rates of photobleaching in TPLSM are significantly
increased as compared to confocal microscopy [23, 24]. The result of this situation
is that, although photobleaching is less damaging from a three-dimensional imaging
standpoint in TPLSM, the number of images that may be acquired at a given axial
plane is reduced in TPEF as compared to confocal microscopy.
Despite the increased rate of photobleaching occurring under TPA, the numerous
advantages of TPLSM (e.g., whole-field detection, increased penetration, etc.) make
it an extremely useful tool for studying a myriad of systems, especially biological
Fig. 11.12 A simplified

Jablonski diagram illustrating
the singlet (Sn ) and triplet
(Tn ) states of a hypothetical
fluorophore, as well as
photokinetic pathways. Here
the variables ki represent
transition rates for
two-photon excitation (TPE),
fluorescence (f ),
phosphorescence (p), and
inter-system crossing (ISC).
Dashed arrows represent
photobleaching pathways
from the various energy
manifolds within the
fluorophore
samples. As such, a large body of research has been accumulated in the past decade
aimed at reducing rates of photobleaching under TPLSM. While some studies aim
to improve the photostability of certain fluorophores, a more global approach is to
manipulate the excitation source in the hope that any improvement in photobleach-
ing rates will apply to many fluorescent tags. Photostability in TPLSM has been
studied by manipulation of the femtosecond pulse trains in terms of their energy
[24–26], repetition rate [25, 27], and shape [26, 28, 29]. In order to understand what
parameters of a femtosecond pulse train are relevant to photobleaching rates and
fluorescence yield, it is useful to examine the mathematical form of TPEF.
11.5.1 The Mathematics of Two-Photon Excited Fluorescence
Two-photon excitation occurs by the nearly simultaneous (within 1016 s; [30])

absorption of two photons to promote a fluorophore from its ground singlet state,
S0 , to the first excited singlet state, S1 . This transition is represented schematically
in a Jablonski diagram shown in Fig. 11.12, which displays several energy levels of
a hypothetical fluorophore and some of the photokinetic pathways available to the
molecule. Both the spatial and temporal coherence of the excitation source play a
large part in TPA rates for a fluorophore. Assuming a spatially homogeneous and
unchanging concentration of fluorophores, as well as spatio-temporal decoupling
of the femtosecond pulse, the time-averaged fluorescence measured in TPEF
in the absence of stimulated emission and self-quenching can be expressed as
Eq. (11.1) [31]:
Z
1
hF .t/i D 2 C 2 ghI0 .t/i2 dr S 2 .r/; (11.1)
2
V
where is the fluorescence collection efficiency, 2 is the fluorescence quantum

efficiency of the dye, C is the concentration of the dye, 2 is the two-photon
absorption cross section, I0 (t) is the temporal intensity envelope of the pulse, S(r) is
the spatial intensity of the excitation pulse, and V is the illuminated sample volume.
The quantity g, which is a measure of the second-order temporal coherence of the
excitation source, is defined as shown in Eq. (11.2):
R1
˝ 2 ˛ dt f I02 .t/
I0 .t/ 1 gp
g D 2 D ; (11.2)
hI0 .t/i 2
R1 f
dt f I0 .t/
1
where f is the repetition rate of the laser oscillator, I0 (t) is the temporal intensity
envelope, is the full-width at half-maximum (FWHM) of the temporal intensity
envelope, and gp is the shape factor, a unitless quantity that is only dependent upon
the shape of the laser pulse. Equation (11.2) clearly shows that the temporal intensity
envelope is of critical importance to the TPEF signal through the so-called gain
factor, g, also referred to as the TPEF efficiency [32].
To visualise the effect that g has on the strength of TPA in a fluorophore, let
us assume a Gaussian-intensity pulse in the temporal domain. It is well known
that spectral dispersion acquired from linear optics (e.g. lenses, dichroics, and
objectives) causes distortions away from transform-limited (TL) pulse shapes in
the focal plane and can stretch the duration of the excitation pulse significantly. By
applying various amounts of spectral phase, one can calculate g for different orders
of spectral dispersion. Figure 11.13 shows how g varies as a function of bandwidth
as well as second-order dispersion, also called group-delay dispersion (GDD), for a
Gaussian pulse centred at 800 nm. As one can clearly see, the shorter the pulse is in
time, the better the TPA efficiency is and therefore the more fluorescence photons
one can measure.
It is interesting to compare g and gp as spectral dispersion is added to the
pulse. In this case, we will assume a constant bandwidth of 25 nm and a repetition
rate of 21.7 MHz, typical for an extended-cavity Ti:sapphire (Ti:Al2 O3 ) oscillator.
Figure 11.14 shows , g, and gp for a Gaussian pulse as GDD and third-order
dispersion (TOD) are varied. It is interesting to note that for both cases g is maximal
when the pulse is shortest, i.e. when GDD and TOD are zero, while gp is maximal
when GDD D 0 but not when TOD D 0. Since gp is only a measure of how good
the pulse shape is, ignoring temporal duration, one can conclude that a Gaussian
pulse with approximately 20,000 fs3 of TOD is better at exciting TPA than a TL
Gaussian pulse, but that the concomitant increase in temporal duration offsets this
improvement in shape.
The best shape factor is clearly unity, which is possible only when I0 2 (t) D I0 (t).
An example of such a pulse is the square pulse (Eq. 11.3):
Fig. 11.13 Second order temporal coherence, or TPA efficiency, for a Gaussian pulse centred on
800 nm with varying amounts of GDD and spectral bandwidth. Note that the shortest pulse (largest
bandwidth and TL) produces the largest value for g, and that spectral dispersion of the excitation
pulse causes a significant reduction in TPEF efficiency
8
<0 t < =2
Isq .t/ D 1 =2 t =2 ; (11.3)
:
0 t > =2
implying that the greater the slope of the pulse, the better the shape factor will
be. Clearly, by minimising the duration of the square pulse to be infinitesimal, we
qualitatively arrive at a Dirac-delta function, ı(t), for the optimal pulse shape, a
pulse that is not realisable in practice due to its infinite peak intensity. Clearly then,
the closest one can get to realising a Dirac-delta pulse in practice is to produce a
TL pulse, which optimises the efficiency of TPEF. Put simply, a TL pulse is optimal
for TPA efficiency because the peak intensity of such a pulse is higher than that of
a stretched pulse of the same bandwidth. The ramifications of this scenario are that
the probability for the fluorophore to absorb two photons simultaneously is higher
for the TL pulse, boosting the TPEF signal.
A more qualitative picture can be used to understand this principle. Intensity is
typically measured in units of W/cm2 . However, using the expression for the energy
of a photon, E D „!, where „ is Planck’s constant divided by 2, and ! is the
angular frequency of the photon, one finds the result in Eq. (11.4) [3]:
1 mW D 5 1012 photons nm1 s1 : (11.4)
This result means that it is physically correct to think of intensity as a mea-

surement of the flux of photons through a given cross-sectional area. If we now
Fig. 11.14 Variation in g & gp for a Gaussian pulse as a function of TOD and GDD. The effect of
GDD is shown in (a) and (b), while TOD is shown in (c) and (d). Note that the noise in these
simulations is due to quantisation noise in the numerical determination of the temporal pulse
duration
consider two pulses that have the same spectrum, but differ in that one is TL and the
other is stretched, we know from Parseval’s theorem that both pulses must have
the same energy, and thus the same number of photons per pulse. What differs
between the pulses is the peak flux of these excitation photons. Because the TL
pulse has all fluorescence photons arriving in the shortest possible duration, the
photon flux is greater, and thus there is a higher probability that the fluorophore will
simultaneously absorb two photons as compared to the stretched pulse. This leads
to an increased fluorescence yield in a non-bleaching sample as the pulse duration
is decreased. Mathematically, we see that this qualitative argument is verified by
the inverse relationship between the average fluorescence and the pulse duration
(cf. Eqs. 11.1 and 11.2).
11.5.2 Fluorescence Yield and Photobleaching
In a bleaching specimen, increased intensity also leads to increased photobleaching

rates [24]. This situation results since additional channels for photobleaching are
available when fluorescent molecules are in the various excited singlet and triplet
states (cf. Fig. 11.12). Thus as a fluorophore is more efficiently excited to a higher
energy state, the probability that the molecule will undergo photobleaching is
increased due to the various mechanisms for photobleaching that become available,
such as two-step photolysis [33].
In light of both these facts, what is the optimal pulse shape for exciting a sample
that will undergo photobleaching? Importantly, one must consider the operating
regime in which the imaging is to be carried out. In the case where thin preparations
are to be imaged, it is possible to reduce the excitation power and still achieve an
acceptable SNR. This approach has been shown to result in significant decreases
in the rate of photobleaching at the expense of fluorescence yield [24, 26]. In
deep-tissue imaging, however, one is often power-limited [34], meaning that no
reduction in excitation power is possible without sacrificing penetration depth into
the specimen. In such a case, the optimal pulse shape for achieving fluorescence
yield is TL [29], which offsets the concurrent increase in bleaching rates. Recently,
we investigated photobleaching rates and fluorescence yield as a function of spectral
dispersion compensation for several fluorophores commonly used in TPLSM [29].
Our results indicated that the instantaneous TPEF achieved with TL pulses was
always greater than that of un-optimised pulses, despite their increased bleaching
rates, causing the SNR and thereby the spatial resolution to be better with TL pulses.
11.6 Novel Techniques
11.6.1 Temporally Focused Optics for Wide-Field Imaging
Multiphoton imaging is traditionally performed with beam scanning or by using

a multifocal system covering the sample area. In addition to these techniques, it
is also possible to utilise a novel spatio-temporal pulse shaping technique called
simultaneous spatial and temporal focusing (SSTF) to obtain wide-field multiphoton
images [35, 36], making scanning or multiplexing the laser beam unnecessary.
Instead, the pulses are weakly focused in space to illuminate a large area and
modification to the temporal profile is used to achieve a good focus. It is important
to note that with traditional non-spatio-temporal focusing, the depth resolution
would be compromised. This limitation to the sectioning capability is overcome
by simultaneous temporal focusing as the pulses propagate to the focal plane.
In practise, SSTF is attained by spatially chirping the femtosecond laser pulses.
A grating is used to spatially separate the component frequencies of the pulse,
resulting in an increase to the pulse duration everywhere the frequencies no longer
overlap in space. This grating is imaged onto the sample such that all of the
frequency components converge at a focal plane and, by Fermat’s principle, the
original pulse duration is re-established. Using SSTF, Oron et al. monitored two
photon excitation fluorescence over an area of 100 m2 with 4.5 m FWHM
depth resolution [35]. In this experiment the lateral image resolution was 0.25 m
giving approximately 100,000 effective pixels per image. Thus, an equivalent image
obtained with a multifocal or scanning beam system would need to cover roughly
100,000 positions.
More complex focusing arrangements in SSTF may be achieved by shaping the
phase and amplitude of the pulses. For example, the position of the temporal focus
may be offset by adding second order phase or group velocity dispersion (GVD)
to the spatially chirped pulses [37–39]. This dispersion can be achieved by several
means – including a prism pair, a dispersive optical fibre, or a liquid crystal array
pulse shaper. Within a certain range, the pulses remain transform-limited in time,
and the temporal focal plane is linearly dependent on the GVD. Such an SSTF
system with an adjustable axial focal position has been demonstrated with a range
of over 200 m, or 17 times greater than the beam’s Rayleigh length of 11.5 m
[37]. A potential application of this capability is remote axial scanning in a fibre
endoscope. While GVD controls the axial focal position, it has also been shown that
the lateral position of the SSTF focus is dependent upon the pulse’s linear phase
[38]. In addition, the shape of the illumination pattern on the sample may be adjusted
by amplitude shaping at the grating [40]. For example, illuminating the grating
with a line-shaped beam produces a line focus on the sample and illumination with
an array of lines produces an array of line-shaped foci on the sample. Amplitude
patterning combined with phase shaping has also been employed in order to generate
multiple foci with independent axial and lateral focal positioning [38].
11.6.1.1 Temporally Focused Optics for Micromachining

Biological Samples
In addition to wide-field multiphoton imaging applications, SSTF improves the

rate of femtosecond laser micromachining, another multiphoton process. Many
micromachining applications require a geometry where the beam must focus in the
bulk or through a transparent material; however, out-of-focus nonlinear interactions
deplete the energy of the pulses and may prematurely damage the material.
Typically, this problem is overcome by increasing the strength of the geometric
focusing by using high NA optics. SSTF improves the machining rate by axially
confining a larger interaction area, allowing machining at low NA. For example,
SSTF can be applied to performing a craniotomy [41]. In a craniotomy a portion of
the skull is removed and the viability of the sample is retained through continuous
immersion in a saline solution. Without SSTF, nonlinear interaction with the water
layer prohibits machining at low NA. With SSTF, we ablated a rat skull through
6 mm water at 0.03 NA – a numerical aperture with an interaction volume
orders of magnitude larger than that achieved at 0.50 NA, a common choice for
Fig. 11.15 (a) Craniotomy

in an excised rat skull
performed using femtosecond
laser ablation with SSTF.
For comparison, we show a
traditional craniotomy
performed with a hand-held
dental drill (Zoomed-out
view). (b) Top and (c)
tilted-forward enlarged views
of the femtosecond laser
craniotomy
ablation through transparent materials without SSTF. The 0.5 mm 1 mm 1 mm

craniotomy is shown in Fig. 11.15 and was ablated in 10 min with a 1 kHz
laser. Another application of SSTF to femtosecond laser micromachining is to
employ amplitude shaping in order to vary the diameter of subsurface channels for
microfluidic devices [42]. In summary, while SSTF began as a technique for wide-
field multiphoton imaging, it has since proved its flexibility for creative application
to many other areas.
11.6.2 Photon Counting
11.6.2.1 Why Photon Counting?
In multiphoton microscopy it is traditional to utilise a PMT along with a pulse

amplifier to produce a strong analogue signal corresponding to the occurrence of
incident photons on the PMT. Since these photons come in very rapidly, on the
order of nanoseconds between photons, the resulting analogue signal requires an
extremely fast analog to digital converter in order to electronically capture all of the
photons. As a result of the difficulty of accomplishing this task, a different approach
has been taken by the majority of researchers working with point detectors. In these
systems the analogue signal is averaged, instead of attempting to capture enough of
the waveform to count all of the photons directly.
Averaging the signal from the PMT is virtually identical to conditioning a pulse
width modulation signal. By filtering the high frequency pulses from the PMT, a
data acquisition card will read a higher voltage the more pulses per unit time that
are produced by the PMT. However, since the pulses from the PMT are not always
the same width or amplitude, this leads to an imperfect representation of the original
signal, as some photons will increase the average more than others. In addition,
when utilising photon counting, any counts that occur when the light is turned off
(dark counts) can be thresholded out, dramatically improving the signal to noise
ratio [43, 44]. While the averaging technique is elegant in its simplicity, and much
less expensive than traditional photon counting systems, this simplicity comes at the
cost of the integrity of the collected data.
Data integrity is not always necessary in biological imaging, but for some
applications it is of crucial importance. For example, in photon counting it is
possible to calibrate the number of photons measured by the detector to the exact
concentration of a fluorophore. This kind of calibration is not possible when
averaging is performed, as the shot-to-shot instability of the PMT signal means that
there is no longer a direct connection between the measured quantity and the number
of photons incident on the detector [45]. So, provided that an experiment is operating
in the photon counting regime, it is always better to use photon counting as opposed
to averaged detection, since photon counting is valid for a broader set of techniques.
However, if the probability is large for more than one photon to be excited per
laser pulse (if the experiment is not in the photon counting regime), then it is not
possible to accurately count the photons excited from the sample – due to photon
pile up. In many biological imaging applications we are in the weak fluorescence
limit, and photon counting is therefore the optimum detection modality. For an
excellent discussion into when analog integration or photon counting is appropriate
in multiphoton imaging, see the paper by Driscoll et al. [46].
11.6.2.2 History of Photon Counting in Multiphoton Microscopy
Photon counting has a long history in microscopy, evolving into a variety of different
methods with various advantages and disadvantages. Since photon counting requires
extremely fast electronics, early photon counting used analogue techniques, such as
the time to amplitude converter (TAC). A TAC is used in time-correlated single pho-
ton counting (TCSPC) to measure the time between the incident pulse and the arrival
of the emitted photon. Later, the gated photon counting technique was introduced,
permitting the digital differentiation of photons arriving at different times after the
incident sample pulse. This technique was then extended to produce the photon
counting histogram (PCH), which performs virtually the same measurement as
TCSPC by utilising digital techniques rather than a time to amplitude converter [47].
Due to the complexity involved in photon counting, an innovative technique for
“fixing” averaging the signal from the PMT was developed. By utilising a discrim-
inator and a pulse shaper on a traditional averaging system, the resulting pulses
are conditioned to have virtually identical width and amplitude [45]. Performing
averaging on this modified system is therefore not as detrimental. Since the number
of photons can be accurately extracted from the averaged value on such a system,
the appropriate fluorophore concentration can be inferred from the averaged value.
However, this technique does not permit for any of the photon timing information
to be extracted, limiting the technique for many applications.
Combining these techniques with synchronised scan mirrors (or other beam
deflecting techniques) opened the door to performing laser scanning microscopy
with a point detector. Early systems designed to perform these measurements
involved a great deal of custom electronics [43], but these systems were eventually
commercialised and turned into more manageable, but expensive, turn-key systems.
However, with the advent of field programmable gate array (FPGA) technology and
complex programmable logic devices (CPLD) these systems are becoming inexpen-
sive enough that laboratory researchers can build on their own. These programmable
logic device technologies also permit novel customisation of the photon counting
system, allowing for unique techniques, such as spectral photon counting [44] and
demultiplexing photon counts from a single detector corresponding to multiple input
beams [48].
11.6.2.3 Novel Geometries and Capabilities Enabled by Photon Counting
One of the major disadvantages of imaging detection is that it is necessary to descan

or spatially filter the photons from the sample before placing them on the detector
[49]. By switching to a point (non-imaging) detector, such as a PMT or an avalanche
photodiode, it is no-longer necessary to descan the returning photons (Fig. 11.16).
This change can be incredibly useful for imaging with low light levels, as the path
back through the scan system introduces significant additional losses. Additionally,
imaging back through the scan system assumes that all of the returned photons are
from the focal volume. This situation is not the case when imaging within highly
Fig. 11.16 Geometric difference between imaging detection and point detection. (a) Imaging
detection. (b) Point detection. CCD charge-coupled device camera, D dichroic, SM scan mirror,
SL scan lens, TL tube lens, OBJ objective, PMT photomultiplier tube
scattering media, resulting in significant background fog when deeper imaging is

performed within the media.
While point detection can still be implemented with averaging the signal from a
PMT, there are several capabilities that are unique to photon counting. For example,
in TCSPC the delay between an incident pulse and the emitted photon is measured
so there is no way to perform this measurement without photon counting. Among
other things, TCSPC allows researchers to measure the fluorescence lifetime of
different dyes, permitting the differentiation of dyes even when their emission
wavelengths are indistinguishable. The PCH technique can be used to perform a
similar measurement. PCH just takes a slightly different approach by using a clock
to divide up the time after the incident pulse into histogram bins for storing the
photon counts, rather than collecting all of the precise measurements of the time
between the incident pulse and the emitted photons and post processing that data.
Another technique unique to photon counting is the ability to electronically
demultiplex the information from optically multiplexed beams. This differential
multiphoton microscopy technique works by utilising beams with a time separation
greater than the fluorescence lifetime of typical dyes (several nanoseconds) and
electronically distinguishing the beam corresponding to the emitted photons. This
technique has unique utility in that it permits the nearly simultaneous acquisition
of photons from different beams, allowing for measurements from multiple layers,
multiple polarisations, multiple lateral locations, or multiple beam shapes.
11.6.2.4 Photon Counting Architecture Basics
Photon counting is not very complicated, at least in principle. The general principle
of a photon counting system is to detect the edges of a PMT signal corresponding
to single photons and increment a counter every time such an edge is detected.
In practice, photon counting data signals are extremely rapid (up to a couple
hundred megahertz for multiphoton microscopes); and therefore require a great
deal of care to handle properly. A commonly overlooked issue with signals at these
frequencies is that every cable between the photon counting components operates as
an antenna. Due to this problem, it is necessary to use well shielded cable (at least
double shielded) to keep environmental signals from causing extraneous noise to be
interpreted as signal photons. One might suppose that this shielding is only critical
before the pulse amplifier; however, experience shows that due to the combination
of high frequencies and high amplitudes, it is necessary to shield all of the PMT and
photodiode signals prior to the photon counting electronics.
The general architecture of a photon counting system is shown in Fig. 11.17.
This figure shows both the components necessary to construct a basic photon
counting system and the extra components required for an advanced demultiplexing
system. Both systems require a good PMT designed for photon counting; however,
a Geiger-mode PMT is not ideal for such systems, as these PMTs have a long
dead time between pulses. A much better performing system consists of a non-
Geiger-mode photon counting PMT chained with a pulse amplifier and a high-speed
comparator (HSC). Such a PMT does not output enough current for the pulses to be
discriminated directly, hence the need for a pulse amplifier, but provides much better
pulse-pair resolution than a Geiger-mode PMT. In addition to the pulse amplifier,
a HSC is necessary to threshold the pulses and provide a clean logic signal to
the photon counting electronics. Together with these signal electronics, it is also
necessary to synchronise the photon counting system with the scan electronics
(usually scan mirrors), so that a two-dimensional image can be formed from the
intensity readings. It is not strictly necessary to integrate this step with the photon
counting system (this task can be performed by a computer), but properly integrating
this step onto the photon counter means there will be no dead-time between pixels.
Fig. 11.17 Photon counting system architecture. PMT photomultiplier tube, PD photodiode,
PA pulse amplifier, HSC high-speed comparator (discriminator), SMC scan mirror controller,
LN line clock signal, PXL pixel clock signal, PhC photon counter. Star (*): Only required for
demultiplexing photon counting systems
A more advanced demultiplexing photon counting system also requires timing

signals indicating when the different beams of the laser arrive at the sample. In order
to consistently pick out the same beams, two timing signals are necessary: a “start
of burst” signal and a “laser clock” signal. The start of burst signal indicates which
of the laser clock pulses occurs “first,” and the laser clock signal indicates when
the counter should move on to the next beam. It is important to note that without
the start of burst signal, any interruption in the laser clock signal would have a
high probability of resulting in a re-ordering of the beams from the perspective of
the demultiplexing electronics. It is worth noting that for many photon counting
systems, the output of the photodiode can be tied directly to the photon counting
electronics; but for photodiodes with poor conversion, or photon counting systems
requiring a strong trigger signal, it becomes necessary to utilise additional HSCs to
provide the electronics with the appropriate trigger.
11.6.3 Spectrally Resolved Multiphoton Microscopy
The multiphoton microscopy methods presented to this point have focused on

either gathering volumetric information from a sample or improving signal-to-noise
and/or spatial resolution. This section details the importance of spectrally resolved
multiphoton microscopy, as well as various techniques of collecting spectra and
spectral imaging. Practical design issues are stressed.
11.6.3.1 Spectroscopy
Spectroscopy, as applied to microscopy, involves examining the different colours

emitted from an excited sample. A simple example illustrates the utility of
Fig. 11.18 Simplified energy level diagrams. (a) Indicates the Stokes shift, the difference in
energy between excitation and emission wavelengths for linear excitation. (b) Relaxation from
different vibrational levels within excited states contributes to broadening of the output spectrum
spectroscopy – the spectrum of an atomic gas lamp enables mapping specific energy
level transitions to given spectral lines. The same is true for any fluorophore – an
emission wavelength directly maps to a transition from an excited state to the ground
state or another, lower-energy excited state. Unfortunately, complications abound in
real systems, stemming from both the method of excitation and the physical system
of the sample.
Practical considerations for spectroscopy include the following points. In linear
excitation, there is a slight difference between the emission and excitation energies,
as shown in Fig. 11.18a, known as the Stokes shift. The proximity of the source
and emission wavelengths often limits observation of the emission spectrum at
shorter wavelengths. Multiphoton spectroscopy circumvents the issue by pushing
the excitation wavelength far from the emission wavelength, enabling capture of
the entire emission spectrum. In either case, filtering out the source wavelength is
critical, though certainly simpler in the multiphoton excitation method. Dichroics,
absorptive glass, or edge filters are the most common methods of separating source
light from excitation light.
The physical process of optical excitation and relaxation further complicate spec-
troscopy. Each energy level possesses sub-levels generated by different vibrational
and rotational modes, as in Fig. 11.18b. The small contributions to the transition
energy from these sub-levels broaden the emission wavelength well beyond the
near-infinitesimal width from atomic gas lamps. Broadening limits the efficacy of
spectroscopy in two ways. Nearby transitions can overlap, making it difficult or
impossible to discern which transition is responsible for the fluorescence. More
relevant to biological systems, broadening also increases the difficulty of detecting
small spectral shifts (shifts on the order of several nanometres). A fluorophore
will undergo a small spectral shift, if the nearby chemical environment (electron
density) changes. As an example, the fluorophore may be attached to a larger
molecule that has undergone a conformational shift, and the new electron densities
force a slight alteration in the excited state energy. An understanding of the
fluorescence shift often provides insight into the physical process responsible for the
chemical change. Thus, a practical consideration for any spectrometer is spectral

resolution– the minimum difference in wavelengths that can be resolved in a
spectrograph.
11.6.3.2 Spectrometers
No single definitive technique or spectrometer dominates the field – each method

possesses strengths suited for different situations. Spectral resolution is considered
the most critical, and the factors that determine it vary with each technique. Spectral
range is often significant and is linked to spectral resolution for systems employing
imaging detection (given the set number of pixels available for detection). As
with any optical detector, further considerations are acquisition time, sensitivity,
mechanical stability, and polarisation sensitivity. Throughput, spectral resolution,
and spectral range are often linked, so even within a single spectrometer design,
there is no single optimal solution.
Spectrometer calibration consists of two tasks. The first requires ensuring that
when a spectrum is taken, there is an accurate relationship between the pixel
number and wavelength. The second involves calibrating the wavelength dependent
throughput of the device. Wavelength calibration is best performed with an atomic
gas lamp with well-defined and narrow peaks. When a spectrograph is taken on an
imaging detector, each pixel is assigned a wavelength. When wavelength scanning
is performed, a wavelength vs. position (or voltage) mapping is obtained. The
throughput of a spectrometer is often calibrated using a blackbody lamp. These
lamps have a broadband output in the visible, as well as a convenient analytical
expression for the output as a function of wavelength. Amplitude calibration ac-
counts for any wavelength dependent losses in the system, including dichroic/filter
transmission, detector sensitivity, and any wavelength sensitivity of the dispersing
element.
Grating-based spectrometers are the most familiar, and the simplest to under-
stand. As illustrated in Fig. 11.19, light enters the spectrometer through a small
slit typically between 50 and 100 m wide. The light is directed onto a grating,
dispersed, and passed to a detector. One key feature of this design is that the entrance
slit is imaged to the detector; thus, the entrance slit width is directly responsible for
the spectral resolution. In the case of a scanning spectrometer, an exit slit selects
which small band of wavelengths pass to the detector (typically a high-gain, single
element detector), and rotating the grating scans the different wavelengths across
the detector. The portion of the spectrometer without the camera is often referred to
as a monochromator. In the case of an imaging spectrometer, there is no exit slit,
and all wavelengths are dispersed onto a multi-element detector such as a CCD or
multi-anode PMT, and a spectrograph is obtained in a single exposure.
Practical design considerations for grating-based spectrometers include the fol-
lowing points. Grating-based spectrometers are convenient for visible wavelengths,
since gratings are widely available in multiple blazes, groove densities, and sizes.
Gratings are also advantageous, since they disperse light linearly; that is, the
distance between different colours separated from the central wavelength is directly
Fig. 11.19 A simplified grating spectrometer. The entrance slit is imaged to the detector by the
curved mirror. The grating and focusing mirror together determine the spectral resolution. Optional
grating turret is shown for grating substitution. In the case of a scanning spectrometer, the grating
rotates causing a different colour to be passed through the spectrometer’s exit slit to a non-imaging
detector
proportional to the wavelength, unlike with prisms. However, care must be taken
in selecting the proper grating. The blaze angle tilts the rulings with respect to
the surface normal, forcing more energy into a particular order (typically the
first order). Blazed gratings are most efficient when angled to satisfy the Littrow
condition, where both the incident and diffracted light are normal to the grooves.
Unfortunately, gratings exhibit strongly wavelength-dependent and polarisation-
dependent efficiencies.
If a wide wavelength range is to be observed, grating substitution may be
necessary to maintain sufficient throughput. This is often achieved with multiple
gratings on a rotating turret in commercial systems. Groove density determines
how much dispersion is applied; for example, a grating with 1,200 lines/mm will
introduce twice as much dispersion as a 600 lines/mm grating. Additional dispersion
improves spectral resolution for a set entrance slit width but also limits the spectral
range on an imaging detector. For a set number of pixels on an imaging detector,
twice the dispersion halves the wavelength range but doubles the resolution. Less
dispersive gratings improve spectral range but suffer from mode overlap, where
shorter wavelengths of higher orders can overlap with longer wavelengths of lesser
orders. As an example, 300 nm light from the second-order of a grating will overlap
with the 600 nm light from the first-order [50].
Further, one might consider dialling down the entrance slit width to maximise
spectral resolution. However, the smaller the entrance slit width, the fewer signal
photons reach the detector. This is a significant concern for two-photon induced
processes, where the cross-section is already quite small and photon production is
limited. Increasing the exposure time is the obvious solution, but it is not feasible
in mobile biological systems. High-gain and high quantum efficiency detectors,
such as PMTs for grating scanning spectrometers and electron-multiplying CCDs
(EMCCDs), help mitigate this problem.
11.6.3.3 Spectral Imaging
Spectral imaging adds an additional dimension to traditional confocal or multipho-

ton imaging – each point in the sample is not only mapped, but a spectrum is also
acquired. This technique is often referred to as multi-spectral imaging. Spectral
imaging typically falls into one of two categories: wavelength scanning and spatial
scanning. In the former, full images are obtained for multiple narrow spectral ranges.
In the latter, all wavelengths are detected simultaneously, and the sample or beam
is scanned [51]. A brief overview of the most common techniques applicable to
multiphoton microscopy and their advantages and disadvantages follows.
The most recognisable wavelength scanning technique makes use of Fourier
transforms, the most commonly encountered variety being the Fourier transform
infrared (FTIR) spectrometer. In multiphoton microscopy, the output of the micro-
scope is directed through an interferometer into a CCD detector. The interference
pattern intensity is recorded as a function of path length, resulting in an inter-
ferogram [52, 53]. The transform of this interferogram results in the spectrum.
Spectral resolution falls with increasing wavelength and is typically 1 % of the
excitation wavelength [54]. Fourier transform imaging spectroscopy (FTIS) requires
high mechanical stability and algorithmic modifications for phase correction and
apodisation [52–54].
Use of a liquid crystal tuneable filter (LCTF) also enables rapid wavelength
scanning. A LCTF is a multistage Lyot polarisation interference filter, consisting
of multiple polarisers, each separated by a liquid crystal layer. The entire array is
bounded by birefringent crystals. The resulting apparatus acts as an electronically
tuneable interference filter for the output of the microscope [51]. The key advantage
is rapid wavelength selection; but limited spectral range, low transmission, and
sensitivity to temperature and polarisation limit the application base [55].
To improve throughput, yet maintain electronic tuneability, acousto-optic tune-
able filters (AOTF) provide an alternative to other techniques. An acoustic wave
sent into a medium results in a periodic modulation of its index of refraction,
acting as a three-dimensional sinusoidal phase grating. Light exiting the crystal
at particular wavelengths is deflected at an angle, and adjusting the acoustic wave
frequency changes the grating frequency, selecting which wavelengths are deflected
[51]. Unfortunately, out of band rejection ratios of only 103 and post-processing
(to improve image quality) reduce the efficacy of this technique [56, 57].
Most spatial scanning techniques – whether the beam is rastered across the
sample, or the sample itself is translated – use a grating-based spectrometer to
obtain spectral images. A minor variant of the grating-based spectrometer involves
employing a multiple slit mask and deconvolving the resulting image to obtain
the spectrum [58]. The multi-slit approach improves throughput over single-slit
techniques. The spectral image itself must be assembled in post-processing from
individual spectra obtained from each spatial location.
11.7 Conclusion
The immense versatility of multiphoton microscopy has led to an increasing number

of biological researchers turning to multiphoton techniques. Particularly, the ability
to image deep within scattering tissue without causing out-of-focus bleaching has
carved a significant niche for multiphoton microscopes. In addition, the nature of
multiphoton imaging permits unique detection mechanisms that require less optics
and no detection pinhole; thereby, reducing the number of precious photons that are
lost prior to the detector. These distinctive characteristics also allow for the design
of custom collection optics, further increasing detection efficiency and dramatically
improving image contrast.
Multiphoton microscopy also benefits from a variety of novel imaging
techniques, placing an even more powerful tool in the hands of the biologist.
Among these techniques is the unconventional ability to construct a non-multifocal
wide-field multiphoton microscope, realised through the use of spatio-temporal
focusing. Additionally, the unrivalled capability to implement a variety of different
photon counting technologies gives multiphoton researchers new avenues to explore
previously inaccessible specimens. Furthermore, spectrally resolved multiphoton
microscopy furnishes researchers with the ability to explore the relaxation of
different vibrational levels in an excited state, providing a unique spectral map of
the specimen.
Acknowledgments This work was funded by the National Institute of Biomedical Imaging and
Bioengineering, Grant EB-003832.
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Chapter 12
Femtosecond Laser Micromachining
Loren Cerami, Eric Mazur, Stefan Nolte, and Chris B. Schaffer
12.1 Introduction
12.1.1 What Is Femtosecond Laser Micromachining?
Femtosecond laser micromachining is a process by which pulses from a femtosec-

ond laser are used to induce micrometre-sized structures on the surface or in the
bulk of solid materials. The most common laser system used for micromachining
is the Ti:sapphire laser. This type of laser uses a titanium-doped sapphire crystal
as the gain medium, and has a centre wavelength near 800 nm. Recently, high-
power fibre-based and other solid-state femtosecond lasers have been developed
that are very interesting for micromachining [1, 2]. The study of the interaction
of femtosecond pulses from a Ti:sapphire laser with absorptive materials and
transparent materials has been extensive. Ablation has been demonstrated in both
absorptive and transparent materials, and bulk modification, manifesting itself
primarily as a refractive index change, has been widely shown in transparent
materials.
Micromachining in absorptive materials has been applied to hole drilling,
removal of surface defects, and photolithographic mask repair [3–7]. Bulk refractive
index modifications in transparent materials have been utilized primarily for the
L. Cerami • E. Mazur
Division of Engineering and Applied Sciences, Harvard University, Cambridge,
MA 02138, USA
S. Nolte ()
Institute of Applied Physics, Friedrich-Schiller-University Jena, Max-Wien-Platz 1,
07743 Jena, Germany
e-mail: stefan.nolte@uni-jena.de
C.B. Schaffer
Department of Biomedical Engineering, Cornell University, Ithaca, NY 14853, USA

288 L. Cerami et al.
fabrication of optical waveguides and waveguide-based photonic devices [8–14].

In addition, micromachining in transparent materials has found applications in the
fabrication of microfluidic channels [15–22].
12.1.2 Brief History
Optical breakdown is a process by which energy is transferred from an optical

field to a material, causing ionisation of a large number of electrons. In solids,
the electrons transfer energy to the lattice and permanent structural damage results.
Laser-induced optical breakdown has been studied since the first demonstration of
the laser. In 1962, researchers at Ford Motor Company discovered that light from
a Q-switched ruby laser could ionise air, creating a very bright spark [23]. Several
years later laser damage in glass was observed [24] – a discovery with practical
implications for laser experiments, as optical components are typically made from
glass. These discoveries prompted investigations into how laser light interacts with
gases and solid materials, a research field that remains active to this day.
As lasers capable of generating pulses of shorter and shorter duration were
developed, it became necessary to improve the understanding of light-matter
interactions. Pulsed lasers achieve much higher peak intensities than continuous
wave lasers and therefore their interactions with materials are very different in
nature. The unique interaction of femtosecond lasers pulses with materials, in
particular, has given rise to an extensive and productive research area over the last
15–20 years.
The first demonstrations of microstructuring in bulk glass using femtosecond
laser pulses occurred in 1996 by two separate research groups [8, 25]. One group
reported the fabrication of waveguides inside of a piece of glass using a 120 fs,
200 kHz Ti:sapphire laser system. The other group demonstrated the ability to
modify the refractive index of submicrometre-sized volumes inside a variety of
transparent materials using a similar laser system. Soon after, it was shown that
a ‘micro-explosion’ caused by the high-intensity of the laser can create small
voids in the bulk of transparent samples [26]. The early experiments all used
amplified femtosecond laser systems with pulse energies on the order of microjoules
to achieve the required high intensity. In 2001, however, micromachining using
only nanojoules of energy was demonstrated, presenting new opportunities for
microstructuring in glass [27]. More recently, micromachining in bulk polymers has
gained interest. The first writing of waveguides in polymers using a Ti:sapphire laser
system was shown in poly(methyl methacrylate) (PMMA) in 2004 [28]. Around the
same time that bulk damage was first demonstrated in glass, the effect of amplified
femtosecond laser pulses on absorptive materials, especially on metals, was already
being studied [3, 29–31]. Longer pulses had been previously used to ablate metal
surfaces, but with different results.
12 Femtosecond Laser Micromachining 289
Fig. 12.1 Schematic diagram of typical micromachining setup. A femtosecond duration laser
pulse is tightly focused by a microscope objective or lens onto the surface of an absorbing or
transparent material for ablation or into the inside of a transparent sample for bulk micromachining.
The sample is mounted on a three-axis translation stage and its position is scanned relative to the
laser focus to produce the desired microstructure
12.1.3 General Laser Requirements/Setup
Femtosecond micromachining has primarily been performed with laser systems

using titanium-doped sapphire crystals as the lasing medium. Typical Ti:sapphire
laser oscillators have megahertz repetition rates and output pulses on the order of
50–100 fs, with pulse energies of tens of nanojoules. Higher energy laser oscillators
are becoming available, but in order to achieve pulse energies in the microjoule
range, it is typically necessary to amplify the output from the laser oscillator. The
amplification reduces the repetition rate to the kilohertz range, which affects the
laser interaction with materials, as we will see in Sect. 12.2.3.3.
Micromachining in transparent materials is performed using both amplified
lasers and oscillator-only systems. In both cases, the laser beam is focused into the
sample using a microscope objective. For laser oscillator micromachining, with only
nanojoules of energy per pulse, a higher numerical aperture microscope objective is
required to ensure intensities that are high enough to microstructure the sample.
Amplified systems output much higher energies than oscillators, meaning tight
focusing is not as crucial to reach the same intensity. Therefore, lower numerical
aperture objectives can be used for micromachining with amplified lasers. The
microscope objective is held fixed, while the sample is placed on a movable three-
axis stage. The stage is translated with respect to the laser beam to create continuous
structures on the surface or in the bulk of the sample. Figure 12.1 shows a schematic
of a typical micromachining setup.
The micromachining setup for absorptive materials is very similar, typically
employing a microscope objective for focusing the laser beam onto the sample
surface. This ensures the fabrication of small features. For applications that require
larger features, like hole drilling, long focal length lenses are often used. Although
many aspects of the laser/material interaction may differ, the setups for transparent
material microstructuring and absorptive material ablation are essentially the same.
Laser parameters and material properties have a significant effect on the inter-
action and therefore on the results of the micromachining process. Pulse energy,
repetition rate, wavelength, and pulse duration are several laser properties that
play a role in the absorption of laser pulses by solid materials. Specific properties
of materials, such as bandgap and thermal properties determine whether micro-
machining with femtosecond pulses is possible and how the resulting structures
look and behave. The processes by which energy from the laser is absorbed
by a material and the mechanisms by which the material responds are the key
to understanding the micromachining process. Section 12.2 will illuminate these
processes and give the reader an understanding of the capabilities of femtosecond
laser micromachining. In Sect. 12.3, several applications of micromachining in both
absorptive and transparent materials will be discussed.
12.2 Interaction of Femtosecond Pulses with Solids
12.2.1 Absorption and Ionisation
The interaction of femtosecond laser pulses with materials differs from the inter-
action of longer pulses or continuous wave light in two ways. First, the energy
deposition occurs on a timescale that is short compared to any relaxation process.
The laser energy is absorbed by the electrons, leaving the ions cold, and only after
the laser pulse has left the focal region does thermalisation take place. Second, the
intensity of a femtosecond pulse, even with very moderate energy, is high enough to
drive highly nonlinear absorption processes in materials that do not normally absorb
at the laser wavelength.
12.2.1.1 Linear Absorption
Overall, linear absorption of femtosecond pulses does not differ from the linear
absorption of any other light field. In non-metallic materials, the highest energy
level occupied by an electron (in the valence band) is separated by an energy gap
(the bandgap) from the lowest energy level that is unoccupied (in the conduction
band). If the photon energy exceeds the bandgap energy, light can be absorbed by
the material, promoting electrons from the valence band to the conduction band
(Fig. 12.2, left panel) [32]. In metals, the conduction band is partially occupied,
providing unoccupied energy levels at only slightly higher energy than occupied
ones. In this case, photons can be absorbed through free-carrier absorption, a three-
body interaction where an electron gains energy by absorbing a photon, and gains
momentum through an interaction with a phonon (a lattice vibration) to move to
a higher-lying level in the conduction band [33]. In addition, there remains the
possibility for interband transitions between the conduction band and higher-lying
bands, as in insulating materials. If sufficient laser energy is deposited into the
surface of a material through linear absorption, material ablation can occur.
Fig. 12.2 Schematic diagram of absorption mechanisms that play a role in femtosecond laser
micromachining. Linear absorption (left panel) dominates for materials with a bandgap that is
less than the photon energy. In transparent materials optical processes such as multiphoton (centre
panel) and avalanche (right panel) ionisation are required to deposit energy, where the photon
energy is less than the material bandgap
12.2.1.2 Nonlinear Absorption
In samples that are transparent to the laser wavelength, a single photon of light does
not have enough energy to excite an electron from the valence to the conduction
band, and absorption of laser energy can occur only through nonlinear processes.
If enough laser energy is deposited into the material by this nonlinear absorption,
ablation or permanent structural changes can occur. Because the absorption is
nonlinear, i.e. the absorption probability is a nonlinear function of the laser intensity,
the absorption can be confined to the bulk of a transparent sample by tightly focusing
the laser beam inside the sample, producing a much higher laser intensity in the focal
volume than at the surface.
There are two classes of excitation mechanisms that play a role in absorption in
transparent samples: photoionisation and avalanche ionisation [34]. In photoionisa-
tion, electrons are directly excited from the valence to the conduction band by the
laser field. Depending on the laser frequency and intensity, there are two different
regimes of photoionisation: the multiphoton ionisation regime and the tunnelling
ionisation regime, shown to be two limits of the same process by Keldysh [35], yet
retaining very distinct conceptual pictures.
In tunnelling ionisation, the electric field of the laser suppresses the potential
that binds a valence electron to its parent atom, allowing the electron to tunnel out
and become a free electron. This type of nonlinear ionisation dominates for strong
laser fields and low laser frequency. At higher laser frequencies (but still below
that required for linear absorption) nonlinear photoionisation occurs due to the
simultaneous absorption of multiple photons by an electron (Fig. 12.2, centre panel).
The sum of the energy of all the photons absorbed must exceed the bandgap energy,
i.e. n„! Eg , where Eg is equal to the bandgap energy, ! to the laser frequency,
and „ to the reduced Planck constant, and n is the minimum number of required
photons. Multiphoton absorption requires n photons to interact simultaneously with
a single electron, so the probability for absorption will scale as the density of the
photons raised to the power n. Because photon density is proportional to laser
intensity, I, the probability for multiphoton absorption scales as In .
Avalanche ionisation involves free carrier absorption by an electron already in the
conduction band of the material followed by impact ionisation. An electron in the
conduction band sequentially absorbs several laser photons until its energy exceeds
the conduction band minimum by more than the bandgap energy, then collisionally
ionises another electron, leaving two electrons at the conduction band minimum
(Fig. 12.2, right panel) [34]. As long as the laser field is present this process repeats,
and the electron density in the conduction band grows exponentially.
Note that avalanche ionisation requires some “seed” electrons in the conduction
band of the material. For femtosecond duration laser pulses, photoionisation during
the leading edge of the laser pulse provides these seed electrons for avalanche
ionisation during the rest of the pulse [36]. The electron density grows through
avalanche ionisation until the plasma frequency of the electrons in the conduction
band approaches the frequency of the incident laser radiation (the “critical” plasma
density). This high density plasma strongly absorbs laser energy by free-carrier
absorption [36]. For ultrashort pulse durations, the absorption described above
occurs on a timescale that is short compared to the timescale for energy transfer
to the lattice, decoupling the absorption and lattice heating processes. At the end of
the laser pulse, we are essentially left with “hot” electrons and a “cold” lattice.
12.2.2 Energy Relaxation
As discussed before, the laser radiation interacts primarily with the electronic states
of the valence and the conduction bands. The time to deposit the energy within
these states is determined by the laser pulse duration. For very short laser pulses the
resulting energy distribution of the electrons at the end of the laser pulse may be
non-thermal. Within a fraction of a picosecond this non-thermal energy distribution
will relax to a Fermi-Dirac distribution, which can be properly characterized by a
temperature. Later on, the deposited energy is redistributed over the various energy
states of the system, i.e. energy is transferred from the electrons to the lattice. In
order to understand the difference in the interaction of ultrashort and long laser
pulses with matter, it is instructive to consider the characteristic timescales involved.
This will be done in the following for the interaction with metals. However, similar
derivations can be obtained for other materials as well.
12.2.2.1 Long Pulse Interaction
Let us first consider laser material interactions for a long laser pulse. In this case
“long” means that the pulse duration is much longer than any time-scale concerning
the energy relaxation within the system. This is true for pulses of nanosecond
duration and longer. (Note that in some cases nanosecond pulses are considered to
be short; it is thus obvious that these attributes can only be interpreted in the proper
context!) Since all relaxation processes occur much faster than the pulse duration,
the whole system will be in equilibrium during the interaction process.
Let us consider energy conservation in this system. Since any change in the
internal energy U within a volume V must be either due to the absorption of laser
light within this volume (S V) or due to energy diffusion out of the volume (Ej being
the energy flux), the change in energy can be described by
@U
D r.Ej V / C S V (12.1)
@t
This change in internal energy can be connected to a change in temper-
ature T using the specific heat capacity Ci of the material per unit volume
(@U/@t D Ci V @T/@t). The heat source S can be calculated taking the energy loss
of the laser radiation (S D (1 R) @I/@z) into account (R denotes the surface
reflectivity and I the laser intensity). Using Beer’s law: I.t; z/ D I.t/ exp.˛z/,
this can be simply derived to
S D I.t/ A ˛ exp.˛z/; (12.2)
where A D 1 R is the surface absorptivity and ˛ is the material absorption

coefficient. In most cases the energy loss will be due to heat diffusion, which can be
written as [32]
Ej D k rT: (12.3)
Here, k denotes the thermal conductivity. We can now rewrite Eq. (12.1) as:
@T
Ci D r.k rT / C S: (12.4)
@t
This is the so-called parabolic heat equation. The temperature dependence of the
thermophysical parameters (Ci , k) and of the optical parameters (A, ˛) makes Eq.
(12.4) non-linear, so that its analytical solution can be obtained only in a few cases
(see Ref. [37]). In general, it has to be solved numerically.
We will restrict ourselves here to only a brief discussion of the heat transport,
in order to obtain an intuitive feeling for the typical temporal and spatial scales
involved. Assuming constant thermophysical parameters (Ci , k) one can derive from
Eq. (12.4) that the resulting heat wave after laser absorption will propagate for
about [37]:
p
lt h D t: (12.5)
lt h is called the heat diffusion length, and D D k/Ci is the thermal diffusivity. For
most metals the thermal diffusivity is typically in the range of 0.1–1 cm2 s1 [37],
which means that the heat wave will travel about 0.1–1 m within the pulse duration
for a 10 ns pulse. Note that this is much longer than the optical penetration depth
’1 , which is on the order of 10 nm for metals. Thus, it is appropriate to speak of
the laser as a surface source of heat. Since typical laser spot sizes are much larger
than the heat diffusion length, heat diffusion will be mainly a one-dimensional heat
flow directed normal to the surface in this case.
12.2.2.2 Short Pulse Interaction
It is easy to see from Eq. (12.5) that the heat diffusion length will become equal or
even smaller than the optical penetration depth for pulse durations in the picosecond
or femtosecond range. In addition, there is an even more dramatic change in the
interaction for these short pulse durations. Now, the laser pulse duration is shorter
than the energy relaxation within the system, i.e. the time it takes for the electrons
to transfer their energy to the lattice. As a consequence, heating with ultrashort laser
pulses results in strong non-equilibrium conditions. Thus, electrons and lattice have
to be described by their own temperatures separately. Such a description, called the
two-temperature model (TTM), has been proposed by Anisimov et al. [38],
@Te @Q.z/
Ce D .Te Ti / C S; (12.6)
@t @z
@Ti
Ci D .Te Ti /: (12.7)
@t
Note that a similar two-temperature model had already been used 20 years earlier
to describe the energy relaxation between the electrons and the lattice in order to
explain deviations from Ohm’s law at high currents [39].
In Eqs. (12.6 and 12.7) Te and Ti , denote the electron and lattice temperatures,
z is the direction perpendicular to the target surface, and Ce and Ci are the heat
capacities (per unit volume) of the electron and lattice subsystems, respectively.
The parameter characterizes the electron-lattice coupling, i.e. the energy exchange
between the two systems. Expressions for the coupling constant ” can be found in
[39–41]. Measurements revealed values in the range of D 1016 –1017 Wm3 K1
[42–44]. Q.z/ D ke .Te /@Te =@z is the heat flux, and S D I.t/A˛ exp.˛z/ is the
laser heating source term. A and ˛ are the surface absorptivity and the material
absorption coefficient, I(t) is the laser intensity, and ke is the electron thermal
conductivity. In the above equations, thermal conductivity in the lattice subsystem
(phonon component) is neglected because this heat transport is typically negligible
compared to the electronic contribution for metals.
The strong non-equilibrium conditions associated with ultrashort pulse laser
interaction with solids makes a detailed theoretical analysis difficult. In principle,
the fast and significantly varying properties, including heat capacity, thermal
conductivity, relaxation time, reflectivity, and absorption coefficient have to be taken
into account by using quantum treatments [41]. Instead, we will discuss here a
simplified analytical solution, which is more instructive for the reader.
By dividing Eqs. (12.6 and 12.7) by the corresponding heat capacities Ce and
Ci , respectively, it can be easily seen that these equations have two characteristic
timescales e D Ce / and i D Ci / , where e is the electron cooling time, and i is
the lattice heating time. Due to the differences in the heat capacities, it is always true
that e i . Typical values are of the order of 1 ps for e and 0.01–1 ns for i . These
timescales define three different regimes of interaction: the laser pulse duration is
shorter than e , longer than i or in between the two values. Below, we will discuss
the differences.
Long (Nanosecond) Pulses If the laser pulse duration L is much longer than the
lattice heating time, thermalisation between the electron subsystem and the lattice
takes place during the laser pulse. In this case the electrons and the lattice can
be characterized by a common temperature T D Te D Ti and Eqs. (12.6 and 12.7)
reduce to the parabolic heat diffusion equation (Eq. 12.4) as discussed above.
Picosecond Pulses For picosecond laser pulses the condition e L i is
fulfilled. For times t e , Eq. (12.6) for the electron temperature becomes qua-
sistationary, i.e., the energy loss due to heat transport and energy exchange with
the lattice is compensated by the energy deposited due to the laser radiation.
Accordingly, Eq. (12.6) can be simplified, because @Te /@t D 0. For times t i it
is also possible to simplify the equation for the lattice temperature. Due to the
quasistationary character of the electron temperature, the lattice temperature will
exponentially approach the electron temperature and can thus be expressed as [29]:

t t
Ti Te 1 exp Te : (12.8)
i i
Here, an initial lattice temperature has been neglected. It can be seen from this
expression that in the picosecond regime, the lattice temperature remains much
lower than the electron temperature during the pulse duration. Equilibrium is
obtained only after the pulse is over.
However, a detailed analysis of this interaction regime depends on the actual ma-
terial properties. Since these parameters will strongly change during the interaction
process, such an analysis is beyond the scope of this chapter.
Femtosecond Pulses For pulse durations much shorter than the electron cooling
time ( L e ), i.e. femtosecond pulses or pulses of a few picosecond duration,
the coupling between the electrons and the lattice can be neglected in a first
approximation for times t e . In this case, the differential Eq. (12.6) can be pretty
easily solved, since it is identical with the parabolic heat Eq. (12.4), except that the
electron heat capacity has a specific temperature dependence.
An even simpler solution can be obtained when electronic heat transport is

neglected, i.e. when the heat diffusion length lth D (D e )1/2 ˛ 1 is much shorter
than the optical penetration depth. Note that the electron cooling time (not the
pulse duration) has been used here for calculating the heat diffusion length, since
the electrons have this time to transport heat before they give their energy to the
lattice.
When the electron temperature remains smaller than the Fermi temperature
TF D EF /kB (EF is the Fermi energy, and kB is Boltzmann’s constant), the electron
heat capacity is given by [29, 42, 45, 46]
2 ne kB 2
Ce D Ce0 Te D Te ; (12.9)
2 EF
where ne is the electron density. Within these approximations, the differential

equation for the electron temperature (Eq. 12.6) reduces to:
@Te 2
Ce0 D 2I.t/A˛ exp.˛z/: (12.10)
@t
Assuming a constant intensity I(t) D I0 , Eq. (12.10) can be directly integrated,
yielding
s
2Ia ˛
Te .t/ D t exp.˛z/: (12.11)
Ce0
Here, we have neglected any initial electron temperature T0 D Te (t D 0), and

Ia D I0 A is the absorbed intensity. At the end of the laser pulse the electron
temperature is given by
s
2Fa ˛
Te .L / D exp.˛z/; (12.12)
Ce0
where Fa D Ia L is the absorbed laser fluence.

The evolution of the electron and lattice temperatures after the laser pulse is
described by Eqs. (12.6) and (12.7) with S D 0. After the laser pulse the electrons
are rapidly cooled due to the energy transfer to the lattice. Since this cooling time is
very short, Eq. (12.7) can be approximated by (compare Eq. 12.8) [29]:
t
Ti Te .L / : (12.13)
i
The attainable lattice temperature is determined by the average cooling time of the
electrons ea Ce0 Te .L / =2 [29] and is given by:
Ce0 Fa ˛
Ti Te 2 .L / D exp.˛z/: (12.14)
2Ci Ci
This lattice temperature distribution is a direct consequence of Beer’s law, since

heat conduction has been neglected so far. However, if the heat diffusion length
lth D (D e )1/2 ˛ 1 is much longer than the optical penetration depth, a similar
calculation of the resulting lattice temperature is possible. In this case, Eq. (12.14)
can still be used, provided that we substitute the reciprocal heat diffusion length
lth 1 for the optical penetration depth ˛ [47]:
Fa
Ti exp.z=lt h /: (12.15)
Ci lt h
12.2.2.3 Heat Transport
Heat transport in dielectrics and semiconductors is comparably low compared to

metals, since the electrons are not able to escape due to the charge separation force
keeping the material neutral. In general, metals show much stronger heat diffusion,
since the hot electrons moving into the target can be replaced by cold electrons from
the adjacent region. However, as will be shown below, even in the case of metals
heat diffusion can be significantly reduced when ultrashort pulses are used, due to
the strong non-equilibrium interactions between electrons and the lattice [48].
When the energy of the electrons kB Te remains lower than the Fermi energy
EF D mvF 2 /2, the electron thermal conductivity is given by (see Ref. [32]) ke D
Ce vF 2 =3 D Ce0 Te vF 2 =3. is the electron relaxation time, which is determined
by electron-phonon and electron-electron collisions 1= D 1=e ph C 1=e e . When
the lattice temperature is larger than the Debye temperature, Ti ‚ D „!D =kB ,
where ! D is the Debye frequency (the maximum phonon frequency), all oscillation
modes of the lattice are excited, and a good approximation for the electron-phonon
collision frequency is given by [32, 49] 1=e ph kB Ti =„. The electron-electron
collision frequency can be estimated by 1=e e .kB Te /2 =„EF [49].
While the electrons and the lattice are in equilibrium, Te D Ti , during the
interaction of long laser pulses with the metal, the condition e ph < e e is
fulfilled, resulting in e ph . However, ultrashort laser pulses produce strong
non-equilibrium conditions with electron temperatures much higher than the lattice
temperature Te Ti . Thus, e ph > e e , and therefore e e becomes possible.
In contrast to the well-known behavior at equilibrium, the electron relaxation time
is now determined by the electron-electron collisions. Thus, heat diffusion might be
even less for the interaction with ultrashort laser pulses than described by Eq. (12.5),
where the equilibrium values for the thermal diffusivity are used.
12.2.3 Material Modification
12.2.3.1 Ablation
The non-equilibrium physics associated with ultrashort pulse laser ablation makes a
detailed theoretical analysis difficult. Thermodynamically metastable states such as
superheated liquids are likely to play a role under these highly transient conditions.
Recent experiments revealed that ultrashort laser pulse ablation is a process with
emission of particles up to several hundred nanoseconds after the laser pulse in at
least two steps [50]. In the first step a thin surface layer on the order of the optical
penetration depth is ablated by electron emission, sublimation and transition to the
plasma state. These ablation processes proceed on a nanosecond timescale or faster.
The remaining heat diffuses into the sample and leads to the emission of particles
and droplets after several 10 ns due to a thermal boiling process. Note that the
material ejected in the initial ablation step can carry away much of the deposited
laser energy, especially when working very close to the ablation threshold, thereby
minimizing the amount of thermal energy that later diffuses into the sample. Only
for femtosecond pulses is this true, and it leads to greatly reduced collateral damage
to material surrounding the ablation zone. A full treatment of the ablation process is
thus complex. While numerical approaches including plasma hydrodynamics yield
good agreement with experimental results (see, Ref. [51]), we will present a very
simplified analytical solution below. First we will discuss the scenario of metal
ablation.
In this simplified model, we assume that the energy of the lattice Ci Ti (per
unit volume) has to exceed a certain threshold value in order to obtain significant
ablation. For the following discussion, it will be sufficient to estimate this threshold
value as the heat of evaporation ˝, where is the density and ˝ is the specific heat
of evaporation per unit mass [29]. The condition for significant ablation, Ci Ti ˝,
can be written based on Eq. (12.14) as:

Fa exp.˛z/: (12.16)
˛
If, however, the heat diffusion length for the electrons before they transfer
their energy to the lattice, lth D (D e )1/2 ˛ 1 , is much longer than the optical
penetration depth, Eq. (12.16) has to be changed to
Fa lt h exp.z=lt h /; (12.17)
according to Eq. (12.15). The corresponding thresholds for the absorbed laser
fluences are Ft h =˛ and Ft h lt h , respectively. Note that these thresholds
are independent of the pulse duration. This is in contrast to longer pulses ( L > i ),
where the heat diffusion length and therefore the corresponding threshold value
scale with the square root of the pulse duration [52].
The ablation depths can be easily derived from Eqs. (12.16) to (12.17), giving:
L ˛ 1 ln .Fa =Ft h / .˛ 1 > lt h I Ft h D =˛/; (12.18)
L lt h ln .Fa =Ft h / .˛ 1 < lt h I Ft h D lt h /: (12.19)
This logarithmic dependence of the ablation depth on the laser pulse fluence has
been demonstrated in several experiments (see, Ref. [30]). However, it is interesting
to note, that as the laser fluence increases, the ablation behaviour will change from
being limited by the absorption depth (Eq. 12.18) to being limited by the diffusion
length (Eq. 12.19). This is due to faster diffusion for the highly energetic electrons
that are produced only in the high fluence regime [47, 53].
For semiconductors and transparent materials the physics of ultrashort pulse
laser ablation is basically the same as for metals as described above. The main
difference is that in metals the electron density can be considered constant during
the interaction with an ultrashort laser pulse, while the electron density changes
in transparent materials and semiconductors due to interband transitions, as well
as nonlinear field and avalanche ionisation (see Sect. 12.2.1.2). In transparent
materials, free electrons are first generated by nonlinear field ionisation, which serve
as seed electrons for the avalanche process. The ablation process thus does not rely
on the presence of free electrons due to defects. As a consequence, the ablation
threshold for femtosecond pulses is much better defined than for long laser pulses,
where initial electrons are required resulting from defects [54].
Concerning the ablation threshold, transparent materials and semiconductors do
not exhibit a constant value as a function of pulse duration (in the short pulse regime)
like metals (see above). This is a direct consequence of the strongly nonlinear
absorption process. Since the absorption increases with increasing intensity, i.e.,
decreasing pulse duration, the threshold fluence also decreases with pulse dura-
tion [52].
The high potential for ultrashort pulse laser micromachining arises from the
fact that heat diffusion can be minimized and the interaction process is mainly
determined by the optical penetration depth. In the regime of low laser fluences,
high precision processing is thus possible with negligible heat affected zones and
practically no burr formation. Moreover, the laser fluence threshold is much lower
than for longer pulses due to the reduced thermal losses and, for transparent
materials, higher intensities to drive nonlinear processes. Therefore, lower pulse
energies can be used for processing, resulting in significantly reduced mechanical
damage around the processed area.
In contrast, the absorption of laser radiation at very high fluences results in the
creation of a dense, high-temperature plasma. In this regime, the material is removed
in plasma, liquid and vapour phases, and the heat penetrates deep into the target. The
plasma expansion and the vaporisation process create a strong recoil pressure that
expels molten material. This results in the formation of droplets and debris on the
target surface. Expelled liquid material, which resolidifies at the edges of the hole,
results in the formation of burr. Moreover, the high ablation pressure causes strong
mechanical deformations and even cracks in the surrounding material [55].
While using ultrashort laser pulses in this processing regime provides no
advantage regarding the achievable machining precision, it should be noted that
relatively high ablation rates can be achieved [56]. This is due to the fact that the so-
called plasma-shielding (the laser pulse is absorbed and reflected by the expanding
plasma and does not reach the target; see, Ref. [57]) which limits the achievable
ablation rate for long laser pulses, does not exist for ultrashort pulses due to the
temporal separation between energy deposition and ablation process (the plasma
expansion occurs mainly after the laser pulse).
12.2.3.2 Bulk Damage in Transparent Materials
When sufficient energy is deposited into the bulk of a transparent material through
nonlinear absorption of tightly-focused femtosecond laser pulses, structural changes
can be produced inside the sample without affecting the surface, allowing three-
dimensional patterns to be fabricated by translating the laser focus throughout the
sample. In contrast to the surface ablation discussed above, no energy deposited by
the laser can be carried away from the sample through material ablation, resulting
in somewhat different regimes of material damage. To date, three qualitatively
different kinds of structural changes have been induced in the bulk of transparent
materials with femtosecond laser pulses: an isotropic refractive index change
[12, 58]; a birefringent refractive index change [59, 60]; and a void [25, 26, 61].
The structure produced depends on laser parameters (pulse duration, wavelength,
energy, repetition rate), material parameters (bandgap, thermal properties), and the
numerical aperture (NA) of the focusing objective. In the case of tightly-focused
(NA > 0.65), 100-fs, 800-nm pulses in fused silica, each of the three morphologies
can be produced by varying only the incident laser energy, with isotropic refractive
index changes produced from the threshold energy of about 40 nJ to about 150 nJ,
birefringent refractive index changes produced from about 150 nJ to about 500 nJ,
and voids formed above about 500 nJ. Figure 12.3 illustrates these three types of
modification.
The isotropic refractive index changes are likely due to localized melting and
rapid resolidification of the glass (Fig. 12.3, left panel) [62–64]. In fused silica, the
density increases if the glass is quenched from a high temperature [65, 66], partially
explaining the higher refractive index observed in femtosecond laser irradiated fused
silica [8, 67, 68]. Glasses with a more typical thermal behaviour show a lower
refractive index and density in the irradiated region [64, 69]. From this evidence,
it seems likely that the energy deposited in the focal volume by near-threshold
femtosecond laser irradiation leads to heating and melting of the glass in the focal
volume. Subsequently this glass rapidly cools, leading to density and refractive
index changes.
Fig. 12.3 Schematic diagram of the morphology of femtosecond laser-induced structural modifi-
cations in bulk transparent materials. Three different energy regimes, low, intermediate, and high,
are represented from left to right, with examples of the damage morphology produced in glass in
the lower panels. On the left is an optical image of a refractive index change. Centre is an SEM
image of a nanograting. Right is an SEM image of a void (The left, centre and right hand images
are reproduced and adapted with permission from Refs. [61], [70] and [25] respectively)
The birefringent refractive index changes [59, 60] appear to be caused by

periodic, nanometre-scale stripes with varying material composition that are formed
in the irradiated volume (Fig. 12.3, middle panel) [70]. In fused silica the stripes
consist of alternating layers of material with slightly increased and decreased
density. The stripes are oriented perpendicular to both the polarisation vector and
incident direction of the laser beam and give rise to form birefringence [71].
Currently, the origin of these structures is still under discussion. It has been proposed
that these “nanogratings” form as a result of interference phenomena that lead to
periodic modulations in the electron plasma density and therefore to modulations in
the nature of the structural change [70]. Another possible explanation is based on the
formation of small nanoplasmas which grow on successive pulses asymmetrically
due to field enhancement effects and merge into nanoplasma planes. Finally, these
nanoplasma planes evolve into planar nanocracks [72].
The voids produced at high energy have been attributed to an explosive expansion
of material out of the focal volume and into the surrounding material, termed
a “microexplosion” (Fig. 12.3, right panel) [25, 26, 73]. Because this expansion
occurs within the bulk of the material, the microexplosion leaves a less dense or
hollow core (the void) surrounded by a densified shell of material [61, 74].
Other processes, such as colour centre formation [8, 64] and migration of
components in the glass [75] are also known to occur as a result of femtosecond
laser irradiation of transparent samples. The role of these, and other mechanisms,
requires further study. The colour centres, however, do not produce the majority of
the refractive index change because eliminating them by annealing does not recover
the original refractive index [68, 76].
12.2.3.3 Repetitive Versus Cumulative Micromachining

of Transparent Materials
As discussed earlier, laser oscillators and amplified systems have very different
repetition rates. As a result, oscillator-only micromachining is fundamentally
different from micromachining with amplified laser systems. Because the average
output power is limited by the pump source, there is a trade-off between the
pulse energy and pulse repetition rate of femtosecond lasers. The time interval
between the pulses emitted by a femtosecond laser oscillator is on the order of tens
of nanoseconds, which is significantly shorter than the 1- s heat diffusion time
characteristic of the micrometre-sized focal volume of the high numerical aperture
objectives used for bulk micromachining. Consequently there is not enough time
between successive pulses for the energy deposited by one laser pulse to diffuse
out of the focal volume before the next pulse arrives. Over time, the energy from
successive pulses accumulates in and around the focal volume, producing damage.
The train of oscillator pulses constitutes a “point source of heat” located at the focal
volume within the bulk of the material. The longer the material is exposed to the
train of pulses from an oscillator, the higher the temperature at the focus and the
larger the region that is heated. If the temperature exceeds the material’s melting
point, structural changes can occur. The pulses from an amplified femtosecond laser
system, on the other hand, typically are separated by milliseconds, which far exceeds
the time required for heat to diffuse out of the focal volume. The focal volume
thus returns to room temperature before the next pulse arrives. Consequently, the
structural change caused by an amplified laser is confined to the focal volume,
regardless of the number of pulses that strike the sample. This means that the
shape and volume of the modified area depends on the volume of the focus. For
low numerical aperture (NA) objectives, the confocal parameter is much larger than
the radius of the focal spot, leading to an elliptical focal volume. Only with very
high NA objectives or special beam shaping techniques [16, 77, 78] does the focal
volume become more symmetric. On the other hand, when micromachining with a
femtosecond oscillator, heat causes melting outside of the focal volume, leading to
a more spherically shaped modified region. The shape of the focal volume becomes
a factor when choosing a waveguide writing geometry, which will be discussed in
Sect. 12.3.
12.2.4 Experimental Considerations
12.2.4.1 Role of Focusing and Aberrations
The intensity of femtosecond laser pulses is a determining factor in governing

the laser/material interaction in transparent materials. As intensity is defined as
the power within a set area, it will depend on the spot size of the laser beam. In
micromachining experiments, a lens is used to focus the laser beam down to a spot
size that ensures intensities above the damage threshold. For micromachining in
glass, microscope objectives are typically used for this purpose to achieve a very
tight focus.
When dealing with a focused femtosecond laser beam in a transparent material,
one must consider two issues that can arise: self-focusing and aberrations. Self-
focusing is a process by which the spatial variation in intensity across a laser beam
leads to a spatial variation in the refractive index (through the nonlinear Kerr index
n D n0 C n2 I ), which acts as a lens and causes the beam to focus itself [79]. This
process leads to a more intense laser beam and can cause catastrophic collateral
damage when micromachining precise structures. Fortunately, there are ways to
minimize self-focusing when micromachining with femtosecond laser pulses. Self-
focusing depends on the peak power of the laser, whereas microstructuring in glass
is intensity-dependent. By keeping the peak power below the threshold for self-
focusing, while keeping the intensity above the threshold for damage, one can ensure
precise micromachining. This is done by using high NA focusing optics.
Aberrations arise as distortions to the laser beam at or near the focus and
are a result of the focusing process. Spherical and chromatic aberrations are two
types that should be considered for micromachining, though chromatic aberrations
may be neglected if the bandwidth of the laser is narrow enough. As mentioned
above, microscope objectives are typically used for micromachining in transparent
materials. These complex lens systems are often corrected for aberrations when
used with a glass cover slip of a specific thickness. When using different materials
(different refractive index) or different thicknesses of material, the aberrations
may become noticeable and degrade the focus. The change in the focus affects
the threshold energy above which modification occurs. Higher numerical aperture
objectives exhibit more significant spherical aberration than lower NA objectives.
For surface micromachining, focusing should be aberration free to achieve the
finest feature size, by using, for example, a microscope objective that is designed
to form a sharp focus without a glass coverslip. Only when using very high pulse
energies does self-focusing in the air in front of the sample become a problem. Such
high-energy machining is usually associated with the use of projection masks to
ablate a large, patterned area at once, rather than with the point-scanning systems
discussed here. The self-focusing can be avoided by placing the sample in a vacuum
chamber.
12.2.4.2 Role of Pulse Duration and Dispersion
Micromachining in transparent materials is an intensity dependent process. When

pulses are above the intensity threshold, damage will occur. Otherwise, no mod-
ification will occur. The laser intensity is equal to the pulse energy divided by the
pulse duration and the area of the focal spot. Pulse duration is limited by the spectral
width of a laser pulse, with a wider spectrum implying a shorter attainable pulse
duration. Dispersion is a process whereby different frequencies of light travel at
different speeds inside of a material. Dispersion separates frequency components
of a femtosecond pulse temporally, therefore increasing the pulse duration. When

using multi-element focusing optics such as a microscope objective large amounts
of dispersion can be induced. Because the pulse duration is lengthened by this
dispersion, there is a risk that the threshold intensity cannot be reached at the
focus, and microstructures will not be created. In order to avoid this, measures
must be taken to compensate dispersion. A micromachining setup may include a
compression scheme whereby the pulses can be pre-chirped to compensate for the
dispersion induced by the focusing lens and other optics to ensure that dispersion
does not affect the laser writing process.
12.3 Applications of Micromachining
12.3.1 Absorbing Materials
Precise micromachining using long laser pulses is often limited due to thermally
or mechanically induced damage (melting, stress, formation of microcracks) of the
surrounding area. These problems are especially severe for brittle materials, like
semiconductors, or for materials with a high thermal conductivity, like metals. The
collateral damage can be significantly larger than the desired structures in this case.
Moreover, the process efficiency is reduced due to the extensive thermal losses.
In contrast, thermal or mechanical damage can be minimized or almost avoided
as discussed in Sect. 12.2.3.1 when ultrashort laser pulses are used for processing.
Since the heating of surrounding material through thermal diffusion is minimal in
this case, the processing efficiency is much higher compared with the long pulse
case. Moreover, the processing area can be precisely defined by the laser beam
geometry, i.e., by the diffraction limit of the optical system. Thus, structure sizes
within the nanometre range can be obtained.
12.3.1.1 Mask Repair
One application example for nanometre scale structuring is the repair of photolitho-
graphic masks. Photolithographic masks typically consist of a fused silica substrate
coated by a 100-nm thick chrome layer. The chrome layer is patterned using either
electron beam lithography or ultraviolet light. This pattern is then imaged onto the
semiconductor wafer to expose the photoresist by an appropriate lens system which
reduces the pattern size by a factor of 4 [7].
Unfortunately, many masks exhibit defects, which in turn result in failures in the
produced integrated circuits. Due to the high costs of the masks, a reliable defect
removal method is indispensable. In most cases the defects consist of excess chrome
in undesired places, which has to be removed with minimal collateral damage.
Fig. 12.4 Atomic force microscope images of a chromium layer on top of a fused silica substrate
structured with (a) 270-nJ, 10-ns and (b) 225-nJ, 150-fs pulses using 780-nm laser radiation [6].
Note the different height scaling in the images
Such a defect repair can be achieved using focused ion beams. However, their use
is limited due to damage of the substrate [5], which results in reduced transmission
or phase shifts of the transmitted light.
These drawbacks can be overcome if the defects are removed using laser
radiation. However, long-pulse laser processing suffers from the large thermal
damage created. To illustrate this, Fig. 12.4 shows a comparison of the ablation of a
100-nm thick chrome film on top of a fused silica substrate by 10-ns (Fig. 12.4) and
150-fs pulses (Fig. 12.4) [6]. In both cases the 780-nm radiation has been focused
onto the sample and scanned across it along two different paths. The pulse energies
were chosen to be close to the ablation threshold. In the case of nanosecond pulses
Fig. 12.5 Microscope images (transmission mode at 248 nm) of a photomask before (left) and
after (right) repair. At two sites the chrome has been fully ablated and the transmission was
recovered (Reproduced and adapted with permission from Ref. [7])
the metal film is melted and then resolidifies at the edge of the trench creating a
large burr. It is thus obvious that such an approach is impractical for the defined
chrome removal on a nanometre scale.
In contrast, processing with femtosecond pulses results in clean ablation with
sharp edges, and no metal splatter or debris is evident. Since the fused silica sub-
strate has an ablation threshold significantly higher than the chrome layer selective
ablation is possible without damaging the substrate. Thus, a high transmission at
the repaired site can be recovered. Typical transmission of repaired sites in excess
of 95 % of similar areas requiring no repair have been achieved on photolithographic
masks [5].
As feature sizes of the photolithographic masks decrease, the resolution demands
on the repair tool increase. In principle, the minimum achievable structure size
is determined by the diffraction limit of the optical system and is of the order of
the laser wavelength. Thus, using short laser wavelengths improves the resolution
[80]. A further increase in resolution can be obtained by taking advantage of the
well-defined ablation threshold associated with ultrashort laser pulses. By choosing
the peak of the Gaussian intensity distribution only slightly above the threshold
value, sub-diffraction sized holes can be produced [3]. Combining both approaches,
researchers at IBM were able to achieve a resolution of 75–80 nm by tightly focusing
ultrashort pulses at a wavelength of 266 nm (frequency tripled Ti:sapphire laser)
onto the photomasks [7]. This corresponds to a resolution of /3, i.e., substantially
below the diffraction limit.
An example of the application of this technique is given in Fig. 12.5, where
two regions of chrome in the left image are removed. The transmission image on
the right impressively demonstrates the accuracy of the process as well as the high
transparency obtained after repair [7].
12.3.1.2 Hole Drilling
High quality materials processing without visible thermal and mechanical damage
can be achieved using ultrashort laser pulses at low fluences close to the ablation
threshold as detailed in Sect. 12.2.3.1. However, several applications like the drilling
of deep holes, as required for fuel injection nozzles, spinnerets and extrusion dies,
rely on the use of much higher fluences significantly above the ablation threshold
[4]. Apart from the fact that a high processing speed is necessary in order to
drill the hole in a reasonable time, the high fluences are mainly necessary due to
the following two reasons. On one hand, material expulsion occurs deep within a
typically small hole. Therefore, the ejected particles need to have a high kinetic
energy in order to be able to escape from the drilled hole. On the other hand, laser
drilled holes typically exhibit a conical shape, which is due to the Gaussian intensity
profile of the beam and due to enhanced thermal losses at the walls of the hole. As
a consequence, the laser radiation is interacting at grazing incidence with the walls
increasing the interaction area and therefore, decreasing the effective fluence.
Despite the high fluences applied in hole drilling, high quality processing can be
achieved. This is due to the fact that the drilling with ultrashort pulses is basically
a two-step process [4]. In the first phase of drilling high laser intensities are used
to rapidly drill a through-hole. Once this is accomplished the high intensity part
of the laser pulse directly propagates through the hole without any interaction with
the hole walls. Only the wings of the Gaussian intensity distribution which exhibit
a much lower fluence interact with the hole walls. This results in a very gentle
material removal with all the advantages of low-fluence ultrashort pulse ablation.
Thus, one can consider this low-fluence finishing as an “integrated” post-processing
step, which results in high hole quality without the need for any post-processing.
Apart from the advantages of using ultrashort pulses for drilling as discussed
above, simple percussion drilling could not sufficiently fulfil the requirements
for high precision, high quality, and high processing efficiency at the same time.
Thus, new processing techniques like helical drilling were developed. By applying
these drilling techniques the precision and quality of holes produced could be
considerably improved [81].
Moreover, such advanced processing techniques allow even for the fabrication
of special hole shapes. An example is presented in Fig. 12.6, which demonstrates
the fabrication of an inkjet nozzle in a stainless steel plate [82]. Here, picosecond
pulses are applied in a laser milling process in order to obtain a certain hole taper.
Therefore, a uniform thin layer of material is ablated by moving the laser spot on the
sample surface in a spiral way. The outer diameter of the spiral defines the diameter
of the layer removed. Subsequent layers are ablated while the outer diameter of the
spirals is reduced from layer to layer. This process is repeated until the desired depth
is reached. By controlling the depth of each layer removed and the outer diameter
reduction between successive spirals, the amount of taper of the milled hole can be
precisely adjusted. In order to obtain a high processing speed, up to 400 holes are
drilled simultaneously by this method after splitting the beam using a diffractive
optical beam splitter [82].
Fig. 12.6 Laser milling process to drill holes with precise taper control (Images courtesy of X.
Liu, Panasonic)
12.3.1.3 Surface Structuring
The microstructuring of surfaces is interesting for several applications. Currently,

the use of ultrashort laser pulses for the selective ablation of different layers in the
production of thin-film solar cells is investigated [83–85]. The goal is to section the
thin-film photovoltaic panels and to realize a monolithic serial interconnection in
order to obtain high-voltage, low-current devices.
Another application example is the structuring of cylinder walls in combustion
engines. Small cavities are serving as a reservoir for the oil, preventing a breakdown
of the oil-film. This results in significantly reduced particle emission [86]. Another
application is the direct structuring of press cylinders in printing industry. Here,
high quality shallow cavities are required without recast layers and burr but with
well-defined depths [87].
Such structures can be produced using ultrashort laser pulses. However, the
spatial geometry of the laser beam is in general not adapted to the cavity profile
desired. Apart from the possibility of beam shaping, the desired geometries can be
achieved by scanning the laser spot across the sample. The depth of the structures
can be influenced by the applied fluence, however, for recast-free structuring a
fluence slightly above the ablation threshold has to be chosen.
Alternatively, the ablation depth can be controlled by the scan speed of the laser
beam movement, i.e. by the overlap of the pulses on the sample, within a certain
range. If the scan speed is, however, too high, the pulse overlap is strongly decreased
and the single ablation spots barely overlap or are even separated, resulting in an
irregular groove. If the scan speed is, in contrast, too low, i.e., a high pulse overlap,
the ablation dynamics can change since deep structures are produced at one site,
which again results in irregular grooves. Thus, one has to find optimal conditions
concerning the applied fluence and scan speed with respect to the process quality.
Structures with the desired depth can then be generated by repeating the scanning
procedure several times.
12.3.2 Transparent Materials
12.3.2.1 Waveguide Based Devices
Femtosecond lasers have the ability to induce bulk refractive index changes inside
of transparent materials, as discussed in Sect. 12.2.3.2 (and also Chap. 13 by
Thomson and Cerullo). Where the intensity is high enough to induce damage, the
region will be modified, while the rest of the material remains unaffected. The
change in the refractive index must, in general, be positive in the irradiated region
for the fabrication of optical waveguides to be possible. Whether the refractive
index increases or decreases in the laser irradiated volume depends on the material
parameters as well as laser parameters. Note that even in glasses where irradiation
leads to a refractive index decrease in the irradiated volume, there is often a
refractive index increase just outside this volume, likely due to compression and
densification of the material that surrounds the, now less dense, irradiated volume
[69, 88, 89]. By translating the laser beam with respect to the sample, a cylinder
shaped region of index modification, and therefore a waveguide, can be formed.
The experimental parameters used in the micromachining process determine the re-
fractive index profile of the microstructures. Therefore, it is important to understand
their relationships when fabricating waveguide-based devices.
A major advantage of fabricating waveguides using femtosecond microma-
chining is the ability to create three-dimensional structures inside of transparent
materials. Standard waveguide fabrication methods are limited to planar or layer-
by-layer processing. By varying the focus of the laser beam, it can be precisely
controlled where the microstructuring occurs inside of a sample. This micromachin-
ing process has the flexibility to create structures that extend through the depth of the
sample (by varying the focal depth) or that fall in a single plane (by only translating
the sample transverse to the laser beam). Figure 12.7 shows two different geometries
that are used for fabricating straight waveguides inside of transparent materials:
transverse and longitudinal. In the transverse geometry, the sample is translated in
a perpendicular direction with respect to the laser beam. The longitudinal geometry
involves translating the sample in a direction parallel to the incident laser beam,
such that the depth of the laser focus in the material is constantly changing as the
sample is translated. As a result, a 10-mm long waveguide would require a focusing
element with at least a 10-mm focal length.
In choosing which geometry to use, one must consider the laser system,
the working distance of the microscope objective, and the shape of the focal
volume. With oscillator-only micromachining, cumulative heating leads to roughly
symmetric structures [27] (Fig. 12.8). Translating the sample either longitudinally
or transversely would result in the same waveguide shape. The limiting factor
for oscillator-only micromachining is the working distance of the microscope
objective. In order to reach high enough intensities to induce refractive index
changes, typically very high NA objectives are used, which consequently have very
short working distances. When using an amplified laser system, the asymmetry
Fig. 12.7 Geometries used for micromachining waveguides in the bulk of transparent samples.
The self-channelling and longitudinal geometries are sometimes used with amplified laser systems;
oscillator-only micromachining is done transversely
Fig. 12.8 (a) Optical microscope image of waveguides written inside bulk glass using a 25-MHz
train of 5-nJ energy, sub-100-fs duration laser pulses focused with a 1.4-NA microscope objective
while the sample was translated at 20 mm.s1 transverse to the beam propagation direction. The
inset shows an optical image of the end face of a waveguide. (b) Near-field mode of a waveguide
like that shown in (a) for 633-nm light (Reproduced and adapted with permission from Ref. [27])
of the focal volume (when using a low NA microscope objective) limits which
geometry can be used. If the sample is translated transversely to the objective, an
elliptical waveguide cross-section would result. This is sometimes undesirable and
so the longitudinal writing method is better suited for amplified systems. However,
adjustments can be made to use the transverse writing geometry with amplified
systems. For example, it has been demonstrated that circular cross-sections can
be obtained using an elliptical beam (by way of beam shaping or a simple slit)
[16, 77, 78] or by a multiscan approach, where the waveguide is composed of
several overlapping modification lines [90–93]. For a more in depth discussion of
waveguide shaping techniques, see Chap. 13 by Thomson and Cerullo.
Utilizing interesting material properties of a variety of materials is one path to

fabricating more advanced waveguide devices using micromachining. For instance,
nonlinear optical materials are attractive for making active waveguide devices
based on waveguide conversion processes, the electro-optic effect, or optically-
induced birefringence. The main requirement for materials is that femtosecond laser
pulses are able to induce the refractive index modification necessary for creating a
waveguide. Many photonic devices have been fabricated using femtosecond mi-
cromachining including waveguide couplers, beam shapers, waveguide amplifiers,
waveguide lasers, interferometers and resonators [9–11, 13, 94]. Various glasses
[8, 58, 75, 95, 96], doped glasses [9, 13, 97, 98], polymers [28, 99–101], and
crystalline materials [102–104] have all been successfully used.
12.3.2.2 Optical Data Storage
The ability to create micrometre-sized refractive index modifications inside trans-

parent materials provides an opportunity for high-density optical data storage.
The first writing of refractive index bits was demonstrated in 1996 [25]. In
this work, sub-micron-sized bits were written in various transparent materials by
focusing femtosecond laser pulses with a 0.65-N.A. microscope objective. Three-
dimensional memory was achieved by writing an array of 1- m diameter spots
in separate planes through the depth of the sample. Other work has focused on
optimizing density and refractive index contrast by varying laser writing conditions
and materials [73, 105]. Two-photon photopolymerisation using femtosecond lasers
and holography using femtosecond lasers have also been used for creating three-
dimensional optical data storage [106, 107].
12.3.2.3 Microfluidic Channels
Hollow micrometre-diameter channels with a three-dimensional arrangement can

be machined in the bulk of a transparent material with femtosecond laser pulses,
allowing the direct writing of microfluidic devices. Two different approaches for
manufacturing such channels have been demonstrated to date.
In the first method, a pattern of damage lines is written into the sample with
femtosecond laser pulses in the intermediate energy regime where nanogratings are
formed. When immersed in a dilute solution of Hydrofluoric acid (HF), these laser-
modified tracks etch much faster than unmodified glass [21, 108], leading to the
formation of hollow channels [15–18].
In the second method, many laser-produced voids are linked together to form
a hollow channel. Debris becomes a problem when fabricating a high aspect ratio
channel, an issue first addressed by Li et al. who introduced a wetting fluid that
wicks into the laser-drilled channels during their formation and carries away the
debris [19, 109]. With this method, channel diameters as small as 0.5 m and
aspect rations as high as 1,000:1 can be produced, with machining speeds as high as
0.2 mm.s1 [20, 22].
While channel fabrication is relatively slow with both methods, it is possible

to produce channel geometries that, because of their shape or location, cannot be
fabricated by traditional microfluidic manufacturing techniques such as moulding
and soft-lithography, providing an important compliment to these traditional man-
ufacturing methods. In addition, it is very attractive to have waveguides in these
devices for optical detection. Femtosecond structuring offers a perspective to realize
both, microfluidic channels and waveguides, within a single processing step [110].
12.3.2.4 Cutting of Biological Materials
Although one does not usually think of biological tissues as being transparent,
in the infrared wavelength range linear absorption becomes weak enough that
nonlinear absorption can dominate for tightly-focused femtosecond laser pulses.
Femtosecond lasers can thus provide a laser scalpel with sub-micrometre precision
that can disrupt specifically targeted structures several hundred micrometres beneath
a tissue surface without affecting surrounding tissue. This tool is gaining traction
in biomedical research, with important studies in cell biology [111, 112], in
invertebrate neuroscience [113, 114], in studies of drosophila development [115],
and in reproducing neurovascular diseases that affect humans in rodent animal
models for the evaluation of therapeutics [116].
12.3.3 New Frontiers
12.3.3.1 New Materials
Polymers are a popular class of materials that we find in many places in our daily
life. Poly(methyl methacrylate) or PMMA is a hard plastic polymeric material,
very similar to glass that is used in many applications where more durability
and lower cost is necessary. Polymers provide distinct advantages over glass due
to their flexible processing techniques and adjustable compositions. For example,
base polymers can be doped with molecules with a high nonlinear susceptibility
and used to make optical waveguide devices that allow efficient second and third
order nonlinear processes. Polymers have already been implemented in passive
optical waveguide devices mainly due to their low cost. The extension of waveguide
micromachining from glass into polymers shows promise, although the laser-
material interactions may prove to be very different.
Recently, research on micromachining optical waveguides in polymers has
achieved some success. Zoubir et al. showed that tubular waveguides could be
formed inside of poly(methyl methacrylate) (PMMA) using a 25 MHz repetition
rate femtosecond laser oscillator [28]. The structures have a circular cross-section
with diameter of 25 m but were shown to only guide 633 nm light in the outer
region of the waveguide. Symmetric single mode waveguides were fabricated in
PMMA using a 1-kHz repetition rate femtosecond laser system [101]. Here, a slit
was placed before the focusing lens for beam shaping in order to produce a circularly
symmetric focal spot.
Other recent work demonstrated microchannel fabrication using an 80 MHz
repetition rate laser oscillator with pulse energies of 0.9 nJ [117]. In this two-
step process, a cylindrical modified region is first formed by focusing the laser
into a PMMA sample using a water immersion lens. Next the structured sample
is annealed at a temperature above the glass transition temperature of PMMA to
cause expansion of the modified region and the creation of a microchannel inside
the bulk.
12.3.3.2 Photopolymerisation
A related research field utilizes femtosecond lasers to make three-dimensional

structures by photopolymerisation. Specifically, two-photon photopolymerisation
(TPP) is a process that achieves sub-micron resolution using femtosecond lasers
[118–121]. When we say a two-photon process, it means that the energy of two
photons add together to equal the energy required for an electronic transition
(compare to multiphoton absorption in Sect. 12.2.1.2). A two-photon process
becomes possible when the material is exposed to intense enough laser pulses.
Generally, femtosecond laser pulses can achieve these required intensities. The
possibility of two-photon absorption in materials is described by a quantity called
the two-photon absorption cross section. This quantity is quite small, typically on
the order of 1050 cm4 s/photon [118]. However, when there are enough photons
(i.e., enough intensity) this type of absorption becomes non-negligible. With a
Ti:sapphire laser, centred at 800 nm, two photon absorption occurs when a material
has a linear absorption near 400 nm.
The experiment starts with a viscous composition, consisting of one or more
monomers and a photoinitiator. Similar to micromachining in transparent materials,
the sample is translated with respect to the femtosecond laser to induce the desired
pattern. The pulses are focused into the sample using a microscope objective. The
two-photon absorption leads to polymerisation of monomers through a reaction
started by the interaction of the laser with the photoinitiator [118, 119]. Once the
material is polymerized the remaining monomer material can be removed, leaving a
three-dimensional microstructure. This fabrication method provides the opportunity
to create sub-micron polymer devices [120] and has applications in photonics,
electronics and biology (Fig. 12.9).
12.3.3.3 Photodeposition
Apart from the precise and practically damage free ablation discussed in Sect. 12.3.1
material deposition using ultrashort pulses is an upcoming application. In pulsed
laser deposition (PLD), where the ablated material is sputtered onto a target, the
Fig. 12.9 Scanning electron microscope images of (a) a “micro-bull” and (b) a woodpile structure
produced using two-photon photopolymerisation (Image in (a) courtesy of S. Kawata, Osaka Univ.
and reproduced and adapted with permission from Ref. [120])
use of ultrashort pulses is advantageous, since it allows optimal control of material

removal as well as minimized cluster and droplet formation [122, 123]. This allows
the production of continuous, smooth, and defect-free thin films [123]. Moreover,
the possibility to produce nanoparticles with narrow size distributions is favourable
for the synthesis of nanoparticle films [124, 125].
Recent work has shown that ultrashort PLD can be used for localized material
deposition from the gas phase, allowing, for example, the repair of photolitho-
graphic masks in cases where chrome is missing (compare Sect. 12.3.1.1) [126].
In this case a femtosecond laser beam with a wavelength of 400 nm is focused
through a saturated atmosphere of Cr(CO)6 . At the surface of the photomask an
organometallic layer is adsorbed, which decomposes if driven to an excited state.
Due to the multiphoton process triggered by the 400 nm pulses this decomposition
occurs only at the focus of the laser beam. This enables the deposition of opaque
chrome lines with widths as small as 200 nm and sharp edges onto the substrate.
Thus the repair of phololithographic masks becomes possible even in the case of
missing chrome [7].
12.4 Conclusions
Femtosecond lasers provide a unique method for microstructuring solid materials.

Both surface and bulk modifications are possible, depending on the materials being
used. In transparent materials, laser pulses are absorbed nonlinearly by the sample.
The ultrashort pulse duration provides intensities necessary for this absorption.
In absorbing materials, the laser energy is absorbed linearly, though the energy
relaxation processes and heat transport are strongly dependent on the laser pulse
duration.
Pulse duration, repetition rate, wavelength and pulse energy are all laser pa-
rameters that impact the micromachining process. As described earlier, the laser
repetition rate has a significant effect on the modification due to heat accumulation
effects. Pulse duration affects the relaxation processes. Laser wavelength is impor-
tant in determining how the energy is absorbed. Pulse energy limits what type of
structures can be produced. The energy must be above some damage threshold value
to modify a material. In addition, when working above the threshold, the amount of
energy can affect the size and shape of the resulting structures.
Waveguide fabrication is probably the most widely studied application of mi-
cromachining in transparent materials. Over the past 10 years, work has been done
in a variety of glasses, crystals, and polymers, and many waveguide-based devices
have been made, including couplers, interferometers, gratings and sensors. Future
work will rely on using new materials to develop unique waveguide-based photonic
devices. A similar use of femtosecond lasers is the fabrication of microfluidic
channels in glass or transparent polymers. Femtosecond lasers also provide a way
of removing materials from the surface of metals, semiconductors, and transparent
materials. Laser drilling of sub-micron holes and removal of material to repair
photolithographic masks are two applications of micromachining in absorbing
materials.
The interaction of femtosecond laser pulses and solid materials has been widely
studied over the last four decades. In addition to the scientific understanding we
have gained, applications of femtosecond laser micromachining have had an impact
in photonics, electronics and biology. The field of micromachining continues to
provide us with interesting science and engineering challenges, as new materials
are developed and new applications are envisaged.
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Chapter 13
Ultrafast Laser Inscription of Photonic Devices
in Bulk Dielectrics
Robert R. Thomson and Giulio Cerullo
13.1 Introduction
Over the last decade a powerful new photonic device fabrication technology
has emerged. In this chapter, we shall refer to this technology as ultrafast laser
inscription (ULI), but it is also widely known by a variety of other names, including
femtosecond-laser direct-writing. ULI uses ultrashort laser pulse to directly write,
or inscribe, structures inside transparent materials, and it uniquely provides the
possibility of fabricating micro-optics [1], micro-fluidics [2], micro-mechanics [3]
and optical waveguides [4] all on a single substrate. This can be achieved in a single
ULI process, without removing the substrate from the inscription rig. As a result, all
the components on the substrate may, in principle, be aligned to within the positional
accuracy of the ULI rig, which can be in the region of a few nm. The aim of this
chapter is to introduce the reader to the technology of ULI, the techniques used for
ULI and some of the applications of ULI that are emerging.
13.2 The Ultrafast Laser Inscription Process
It is logical to start this chapter by briefly describing the basic ULI experimental
setup and process. As shown in Fig. 13.1, a typical ULI rig consists of an ultrafast
laser system. For ULI, pulses with temporal duration ranging between 50 fs and
1.0 ps have been successfully used and some laser systems are supplied with a
R.R. Thomson ()

Scottish Universities Physics Alliance (SUPA), Institute of Photonics and Quantum Sciences,
Heriot-Watt University, EH14 4AS Edinburgh, Scotland, UK
e-mail: R.R.Thomson@hw.ac.uk
G. Cerullo
Dipartimento di Fisica, Politecnico di Milano, Piazza L. da Vinci 32, 20133 Milan, Italy

324 R.R. Thomson and G. Cerullo
Fig. 13.1 Schematic diagram of a typical ULI rig. S shutter, HWP half wave plate, PBS
polarisation beam splitter, BD beam dump, BS beam splitter, D detector, AOM acousto-optic
modulator, QWP quarter wave plate, L lens, SUB substrate material, TS translation stages
compressor which allows the pulse duration to be varied. A shutter is used to control
the on/off state of the laser on the substrate, a half wave plate and polarising beam
splitter are used to control the laser power incident on the substrate, a beam splitter
and detector are used to monitor this power, an acousto-optic modulator can be used
to rapidly modulate the laser power during the inscription and a quarter wave plate
and half wave plate pair are used to control the polarisation state of the laser light
incident on the substrate. Once the power and polarisation properties of the laser
beam have been defined, the laser light is coupled into a lens and the pulses are
focused inside the substrate material which is mounted on a set of high precision
x–y–z translation stages. A computer is used to control the trajectory and speed of
the substrate translation, and synchronise the sample movement with other functions
described above.
To perform ULI, the substrate material and laser wavelength are chosen such that
the photon energy (Ep D h, where h D Planck’s constant and v D the oscillation
frequency of the light) is insufficient to excite an electron across the material band-
gap. Under these conditions, the laser radiation would normally travel through
the material without absorption. However, due to the high peak powers facilitated
by ultrashort pulse durations, the electric fields (E-fields) created in the focus
can be sufficient to induce nonlinear light-matter interaction phenomena which
initiate the generation of a free electron plasma [5]. If the irradiation conditions are
appropriately controlled, this plasma can be highly confined to the region directly
in and around the laser focal volume. After the pulse has left the focal volume,
the plasma transfers energy to the lattice, inducing a localised, and in many cases
permanent, modification to the structure of the irradiated material.
13 Ultrafast Laser Inscription of Photonic Devices in Bulk Dielectrics 325
The ULI induced modification can manifest itself in a variety of ways, examples
of which include changes to the refractive index [4, 6] or chemical etch-rate
[7, 8] of the modified material. Since the light-matter interaction is nonlinear,
only occurring in the focal region where the E-field intensity is sufficient, lines of
modified material can be inscribed inside the bulk of the material by translating it in
three-dimensions through the laser focus. The manifestations of the ULI induced
structural modification can thus be used to directly inscribe three-dimensional
components such as optical waveguides, microfluidics and lenses.
13.3 The Physics of Ultrafast Laser Inscription
13.3.1 Energy Transfer Processes
In any dielectric material at absolute zero, there is an energy bandgap (Eg ) between
the highest filled electron energy level (the valence band) and the next available level
(the conduction band). If a single photon of light is to excite an electron across the
band gap, its energy must be greater than or equal to this gap. As mentioned in the
previous section, ULI is performed by choosing the laser wavelength and substrate
material such that this condition is not met. However, due to the high peak powers of
ultrashort pulses, the E-field in the focal region can be sufficient to excite electrons
across the energy bandgap via nonlinear excitation processes such as tunnelling
and multi-photon ionisation [5, 9, 10]. During tunnelling ionisation (Fig. 13.2a),
the E-field of the laser suppresses the coulomb potential that binds the electron to
the nucleus. The electron is then able to tunnel through the lowered barrier into the
conduction band with a probability which increases with increasing E-field strength.
Electrons may also be excited through multi-photon ionisation (Fig. 13.2b), during
which n photons interact simultaneously to promote an electron across the band gap.
Fig. 13.2 Nonlinear photoionisation processes responsible for transferring energy from the
ultrashort laser pulse to the material. (a) Tunnelling ionisation (b) Multi-photon ionisation (c)
Avalanche ionisation (Reproduced and adapted with permission from Ref. [11])
Since all the photons must essentially be coincident on the electron, the probability
of multi-photon ionisation taking place is strongly dependent on the E-field strength.
Electrons may also be excited through a combination of multi-photon and tunnelling
ionisation.
Once an electron is excited to the bottom of the conduction band, it has a
continuum of states available above it, and it repeatedly absorbs single photons of
light through phonon mediated (to conserve momentum) absorption. The excited
electron absorbs photons until it has sufficient excess energy to impact ionise a
second electron residing at the top of the valence band. This ionisation process,
which is known as avalanche ionisation (Fig. 13.2c), repeats continually while the
laser field is present and results in an exponential increase in the density of the free
electron plasma while the laser field is present.
The free electron plasma created by the pulse exhibits a resonant plasma
frequency given by Eq. (13.1), which increases with increasing free electron density.
The plasma frequency therefore increases until it matches the laser frequency.
At this point the laser resonantly drives the plasma oscillation and a large fraction
of the rest of the pulse is absorbed.
s
N e2
!p D (13.1)
"0 m
Once the pulse has left the focal volume, the free electron plasma begins to
transfer energy to the cold lattice. This transfer begins on the picosecond timescale
through electron-ion collisions until the electronic and atomic systems reach thermal
equilibrium at about 105 K, and on the nanosecond timescale due to recombination
of the electrons with the ions [12]. Since these processes only begin on the
picosecond timescale, the heating of the lattice during the pulse is negligible for
sub-picosecond pulses. Ultrashort pulse irradiation therefore induces a highly non-
equilibrium situation where a hot dense free electron plasma is created within a
relatively cold lattice. This minimises thermal diffusion out of the focal volume
during the pulse and enables the material to be heated efficiently. This in turn
minimises the amount of energy required to modify the material, localising any
modification to the immediate focal region and minimising collateral damage.
13.3.2 Structural Modification Regimes
The transfer of energy from the plasma to the lattice rapidly heats the material. This
heating can induce either no modification to the lattice, locally melt the lattice or
drive it into a gas or plasma phase. These phase changes may also be accompanied
by shock waves and high thermal gradients. Heat then diffuses out of the focal region
on the microsecond timescale [13] and the material cools and re-solidifies. After re-
solidification the irradiated material may exhibit a variety of structural changes.
Thus far, it has been shown that there are three qualitatively different modifica-
tion regimes in glasses and crystals, examples of which are shown in Fig. 12.3.
When using pulse energies only slightly above the modification threshold a
smoothly varying change in the material structure may be observed (Fig. 12.3
(left)) [14]. This modification is characterised by a similarly smooth variation in the
refractive index across the modified region which can be either positive, negative or
a combination of both. The origin of the refractive index modification depends on
the substrate material and on the ULI parameters, but it may have contribution from
material densification, stress, chemical bond changes, colour centre formation and
photorefractivity. If slightly higher pulse energies are used, self-organised nano-
gratings can be formed in a number of materials (Fig. 12.3 (centre)) [15]. The
nano-gratings are always aligned perpendicular to the polarisation of the linearly
polarised incident light and may be either periodic variations in the stoichiometry
of the material or nano-cracks. The physical mechanisms responsible for the nano-
grating formation are still the subject of some debate and two possible explanations
have been suggested. Shimotsuma et al. [15] have suggested they form due to
interference between the incident light field and a density wave travelling through
the free electron plasma, whereas Taylor et al. [16] have suggested a mechanism
involving the growth of disc-shaped nano-plasmas and that the periodic nature is due
to waveguiding effects by these nano-plasmas. Finally, if even higher pulse energies
are used, the lattice itself can be transformed into a gas or plasma. The pressure
inside the irradiated volume can be sufficient to induce a micro-explosion, during
which hot material is driven into the surrounding cold material. The final result is
to leave a void or voxel of material that exhibits a significantly reduced density, as
shown in Fig. 12.3 (right) [6].
13.4 Fabrication Capabilities
From the preceding section it is clear that ultrashort laser pulses can induce a variety
of localised structural modifications inside a dielectric material. From a photonic
device fabrication point of view, however, it is the manifestations of these structural
changes that is of most interest. To date, it has been shown that ULI can be used to
modify the thermal conductivity [17], Young’s modulus [18] and optical absorption
[19] characteristics of the material. It is, however, ULI’s ability to locally modify the
refractive index [4, 6] and chemical etch rate [2, 7] of materials which has attracted
most attention for photonic device fabrication.
13.4.1 Refractive Index Modification
The ULI induced refractive index modification has been attributed to many different
mechanisms, including density changes [20], colour centre formation [21] and
photorefractivity [22]. The substrate material and ULI parameters determine the
Fig. 13.3 (a) Optical micrograph of the end facet of a ULI fabricated Type I optical waveguide in
a silicate glass. (b) Near field image of the 1,550 nm mode guided by the waveguide shown in (a).
(c) Optical micrograph of the end facet of a ULI fabricated double line Type II optical waveguide
in YAG ceramic. (d) Near field image of the 633 nm mode guided by the structure shown in (c).
The scale bar in (c) represents 20 m and is common to (d) (Figures (a) and (b) reproduced and
adapted with permission from Ref. [25], Figs. (c) and (d) reproduced and adapted with permission
from Ref. [28])
role, if any, that each mechanism plays. In certain polymer and crystalline materials
and many glass materials it is possible to directly modify a region of material that
then exhibits a net positive refractive index change. This is loosely known as a Type
I refractive index modification and it can be used to fabricate diffraction gratings
[23], Fresnel lenses [24] and most notably optical waveguides [4]. Figure 13.3a
presents an optical micrograph of the end facet of a Type I optical waveguide in
a silicate glass material. Figure 13.3b presents a near field image of the 1,550 nm
mode guided by the same waveguide [25].
In some materials, particularly those that are single- or polycrystalline, it may not
be possible to readily induce a Type I refractive index modification, perhaps since
the crystal structure usually minimises the free energy of the constituent atoms.
In this case, optical waveguides can be fabricated by inscribing lines of catastrophic

damage. These induce a strain field in the surrounding material which then exhibits
a refractive index change via the stress-optic effect. This form of refractive index
modification is loosely known as a Type II modification, and has been used to
inscribe waveguides in materials such as LiNbO3 [26] and yttrium aluminium garnet
(YAG) ceramic [27]. Figure 13.3c presents a transmission mode optical micrograph
of the end facet of a ULI fabricated double line Type II optical waveguide in YAG
ceramic. Figure 13.3d presents a near field image of the 633 nm mode guided by the
same waveguide [28].
Generally speaking, Type I waveguides exhibit lower propagation losses than
Type II waveguides since the latter inherently require the inscription of a highly
scattering damage region in close proximity to the guided mode. Type I waveguides
have been reported which exhibit propagation losses as low as 0.1 dB.cm1 [29],
whereas Type II waveguides generally exhibit propagation losses of 0.5 dB.cm1
or higher. Eaton et al. have performed an in-depth investigation [30] into the origin
of the propagation losses of Type I waveguides and reported that both Rayleigh and
Mei scattering processes contributed significantly to the propagation losses of their
waveguides.
13.4.2 Selective Etching
One of the most unique and interesting capabilities of ULI is its ability to locally
increase the chemical etch rate of certain materials. This effect has only been
demonstrated in a few substrate materials, examples of which include fused silica
[2, 7] and Foturan glass [1], and the mechanisms by which the chemical etch rate is
increased is highly dependent on the substrate material.
In fused silica, Bellouard et al. have tentatively suggested that the etch rate
increase is due to the generation of planes of material that exhibit a reduction in the
Si–O–Si bond angle, and that these bonds are more readily broken by hydrofluoric
(HF) acid [17]. Hnatovsky et al. [8] have proposed a second mechanism involving
the generation of nano-cracks which enable HF acid to penetrate more easily into
the modified material than into the virgin material. Regardless of the true physical
mechanisms by which the etch rate is increased, ULI can be used to locally increase
the HF acid etch rate of fused silica by a factor of around 100. This incredible
capability has been used to fabricate structures such as micro-mechanics [3] and
micro-fluidics [31], as shown in Fig. 13.4.
ULI can also be used to locally increased the chemical etch rate of Foturan, a
photosensitive silicate glass supplied by Schott which contains cerium and silver
in the form of Ce3C and AgC ions. Although an investigation into the exact
mechanisms by which ULI increases in the chemical etch rate of Foturan is still
to be conducted, the mechanisms by which UV light induces an etch rate increase
in Foturan have been studied extensively and the mechanisms are expected to be
similar for ULI. In the case of UV light exposure, the high energy photons convert
Fig. 13.4 Scanning electron microscope images of (a) a selectively etched fused silica flexure
hinge and (b) a selectively etched subsurface micro-fluidic channel in fused silica (Figures (a) and
(b) are reproduced and adapted with permission from Refs. [3] and [31] respectively)
Fig. 13.5 SEM images of a micro-optical cylindrical lens fabricated from Foturan glass using (a)
ULI induced selective etching only and (b) selective etching and a post-etch annealing process
(Both images are reproduced and adapted with permission from Ref. [1])
some of the Ce3C ions to Ce4C ions. This generates trapped electrons which, through
a controlled heat treatment up to 500 ı C, combine with the AgC ions to create
Ag atoms. These atoms then agglomerate to form silver nano-clusters which act as
nucleation sites for the growth of a lithium metasilicate crystalline phase (Li2 SiO3 )
when the substrate temperature is raised further to 600 ı C. This crystalline phase
exhibits an HF acid etch rate approximately 50 times higher than the original
Foturan material.
Unlike fused silica, which has a melting point above 1,500 ı C, Foturan has
a relatively low melting point of around 600 ı C. As a result, a relatively low-
temperature post-etch annealing process can be readily performed on selectively
etched Foturan structures to smooth out high spatial frequency surface roughness.
Figure 13.5 shows two SEM images of a micro-optical cylindrical lens that has been
selectively etched from Foturan [1]. The image on the left shows the lens before the
post-etch annealing step, the image on the right shows the lens after the annealing.
From these images, it is clear that the annealing has significantly smoothed the
surface of the lens, removing the periodic lines that are characteristic of the ULI line-
by-line rastering process. This post-etch annealing step has been shown to enable the
fabrication of surfaces with a remarkable sub-nm surface roughness [32]. It should
also be mentioned that it has also recently been shown that high temperature flame
brushing can also be used to smoothen the surfaces of selectively etched fused silica
structures [33].
13.5 Controlling the Ultrafast Laser Inscription Process
The ULI process is controlled via the ULI parameters. These include those
associated with the ultrafast laser itself, such as laser wavelength, polarisation, pulse
repetition frequency (PRF), pulse duration, pulse energy, pulse front tilt, as well as
others, such as substrate translation velocity, translation direction, focusing optics
and substrate material. All have been shown to play a role with varying degrees of
importance.
Generally speaking, the “optimum” ULI parameters for a given job are found
using a quasi trial-and-error approach, where structures are repeatedly fabricated
and tested, and with each cycle the parameters are improved. The starting parameters
for this process are of course made based on previous knowledge of how each
parameter may affect the ULI process. Although an extensive review of the effect of
each parameter on the ULI process would be outside the scope of this chapter, it is
necessary to at least briefly review the roles that the most important parameters play.
Due to its importance, a short section is included at the end of this part of the chapter
which focuses on how the cross-section of ULI fabricated optical waveguides may
be controlled.
13.5.1 Writing Geometry
During ULI, the substrate can either be translated primarily along, or transverse, to
the direction of propagation of the inscription laser beam – as shown in Fig. 12.7.
These writing geometries are known as the longitudinal and transverse writing
geometries (LWG & TWG) respectively. Optical waveguide inscription using the
LWG has the advantage that the cross section of the inscribed waveguide is
inherently circular due to the rotational symmetry of the inscription laser beam, but
has the disadvantage that the maximum waveguide length is limited by the working
distance of the lens. Furthermore, due to the depth dependent degree of spherical
aberration imparted on the laser beam by the substrate-air interface, the properties
of the ULI induced modification vary as a function of depth unless steps are taken
to correct for this [34]. For these reasons, the LWG has attracted progressively less
attention. In contrast, the TWG is extremely flexible and enables the inscription of
structures with effectively arbitrary path and length inside the substrate. Unlike the
LWG however, the cross section of the modified region may be highly asymmetric
as discussed in the following section. This is particularly problematic for optical
waveguide inscription since an asymmetric waveguide core results in waveguide
birefringence and asymmetric waveguide modes.
13.5.2 Focusing Optics
The focusing optics control the E-field distribution in and around the ULI focal
region, and hence the spatial distribution of the photo-induced free electron plasma
[35]. If thermal accumulation and thermal diffusion play a minimal role (see next
section for a discussion of these effects), and if beam distortion effects due to
nonlinear refraction are ignored, the dimensions of the plasma created by each pulse
are directly related to the confocal parameter (Eq. 13.2) and beam waist diameter
(Eq. 13.3) of the focused beam inside the sample. In Eqs. (13.2) and (13.3), b is the
confocal parameter, n is the refractive index of the substrate at the laser wavelength,
D and ! 0 are the focused beam waist diameter and radius respectively, is the free
space wavelength and NA is the numerical aperture of the focusing.
2 n !02
bD (13.2)

2
D D 2 !0 D (13.3)
NA
For structures written using the LWG, the diameter of the inscribed structure is
directly related to the focused beam waist diameter. However, due to its flexibility,
it is the TWG that is of most interest. In this case, the dimensions of the structure
cross section are directly related to both the confocal parameter and the beam
waist diameter inside the material. An inspection of Eqs. (13.2) and (13.3) indicate
that when using the TWG the cross section of the modified region will be highly
asymmetric unless the NA of the focusing is close to n. Such tight focusing is, in
general, impractical for ULI applications and numerical apertures in the region of
0.6 are generally used. At the end of this section we review how the cross section of
ULI fabricated optical waveguides can be controlled.
13.5.3 Laser Wavelength
Since ULI relies on the nonlinear absorption of light, the laser wavelength deter-
mines the number of photons required to overcome the substrate material bandgap.
The inscription laser wavelength that can be used is therefore set by the substrate
material. For example, in order to perform ULI in silicon, the laser wavelength must
be significantly longer than the band edge of silicon (1.1 m). If the wavelength
of the laser system is not immediately suited to the application, its wavelength
can be shifted using nonlinear techniques such as second harmonic generation or
parametric amplification. For example, by pumping an optical parametric amplifier
using a Ti:sapphire laser operating at 810 nm, Nejadmalayeri et al. [36] generated
ultrashort pulses of 2.4 m light to inscribe waveguides in crystalline silicon.
Frequency conversion can also be used to enhance the absorption of the laser
radiation. For example, Shah et al. [37] generated ultrashort pulses of 522 nm light
by frequency doubling the 1,045 nm light from a Yb-doped fibre laser. Waveguides
inscribed in fused silica using the 522 nm light were found to guide infra-red light
significantly better than those inscribed using the 1,045 nm light – presumably due
to the enhanced absorption of the shorter wavelength light.
13.5.4 Laser Pulse Repetition Frequency
The pulse repetition frequency (PRF) is one of the most important ULI parameters
due to the role of thermal accumulation. Since heat requires 1.0 s to diffuse
out of the focal region [13], the use of laser systems operating at PRFs greater
than 1.0 MHz prevents the material in the focal volume from cooling completely
between pulses. The temperature of the irradiated material may therefore be driven
significantly higher when using high PRFs – even though the total energy fluence
on the sample may be the same.
To demonstrate the importance of heat accumulation and thermal diffusion in
ULI, Eaton et al. [38] used a finite difference model to model the effect of PRF on
the temperature in the focal region when performing ULI in borosilicate glass. The
results of this simulation are presented in Fig. 13.6 where it can be seen that at a PRF
of 100 kHz the temperature of the material is continually cycled around the material
working point of 1,225 ı C. When the PRF is raised to 500 kHz and then 1.0 MHz,
thermal accumulation is found to play an increasing role and the temperature of the
material increases significantly.
Since heat diffuses out of the focal region equally in all directions, structures
inscribed in the thermal accumulation regime may exhibit a considerably more
symmetric cross section than would be expected from the theoretical E-field
distribution in the focal region. A further effect of thermal accumulation and thermal
diffusion is to increase the size of the modified region cross section. As an example,
Fig. 13.7 presents optical micrographs of structures inscribed in borosilicate glass
using static exposures. The key point to note here is that the size of the modified
region is only weakly dependent on the exposure fluence, which is varied by
four orders of magnitude, whereas a tenfold increase in the size of the modified
region is observed when the PRF is increased from 100 kHz to 1.0 MHz. This
clearly demonstrates the role that thermal accumulation plays in determining the
temperature induced in the focal region during ULI. Finally, it should also be noted
that even when lasers operating at relatively low PRFs (200 kHz) are used, high
Fig. 13.6 Modelled temperature versus exposure at a radial position of 2.0 m from the centre of
the focus. Material: AF45 borosilicate glass, absorbed pulse energy: 260 nJ, focused spot diameter:
2.0 m (Reproduced and adapted with permission from Ref. [38])
pulse energies can be used to drive strong thermal diffusion effects. This can in turn
create a structure cross section that is significantly different than would be expected
from the theoretical E-field distribution [39].
13.5.5 Pulse Energy
As would be expected, the pulse energy is a critical ULI parameter, as it directly

determines the energy limit of the free electron plasma induced by each pulse. As
discussed in Sect. 13.3.2, this determines the modification regime and the degree of
modification. The pulse energy also affects the size of the laser modified region –
since higher pulse energies are able to induce larger plasmas and modify larger
voxels of material through thermal diffusion.
When inscribing optical waveguides, the optimum pulse energy is the energy
which induces the required refractive index modification while minimising the
generation of scattering and absorption centres which increase waveguide propaga-
tion losses. Clearly, the optimum pulse energy for a given job will vary as a function
of the other fabrication parameters. The pulse energy has also been shown to be a
critical parameter for controlling both the magnitude of the ULI induced etch-rate
increase in fused silica, as well as the quality of selectively etched surfaces [8].
Fig. 13.7 Optical micrographs of structures inscribed in AF45 borosilicate glass using static
exposures. The 1,045 nm light was focused inside the substrate using a 1.4 NA objective lens.
Each column of structures was inscribed using the same exposure fluence, whereas each row was
inscribe using the same pulse repetition frequency (Reproduced and adapted with permission from
Ref. [38])
13.5.6 Substrate Translation Velocity
The substrate translation velocity is used to vary the laser fluence on the substrate –
while keeping the pulse energy and therefore the modification regime the same.
Generally speaking, a reduced translation velocity increases the magnitude of the
induced modification. If thermal accumulation and diffusion is significant in the
ULI process, the translation velocity can also be used to vary the energy fluence
on the substrate, which can in turn be used to control the size of the laser affected
zone as shown in Fig. 13.7. This effect has been shown to be particularly useful
for controlling the cross section of optical waveguides and can enable the precise
control of the guided optical mode [40].
13.5.7 Other Parameters
Generally speaking, the ULI parameters that should first be chosen and optimised
are the writing geometry, focusing optics, laser wavelength, laser PRF, pulse energy,
and translation velocity, but it has also be shown that other parameters such as the
laser polarisation and pulse duration can all play important roles.
A number of studies have reported that the laser polarisation significantly affects
the magnitude of the refractive index modification that may be induced in both
amorphous and crystalline materials using ULI. In one study, Little et al. [41]
studied the effect of polarisation on the refractive index change induced in fused
Fig. 13.8 (a) and (b) SEM images of ULI fabricated nano-gratings in fused silica after a weak
etch. In both (a) and (b), S represents the sample translation direction, E represents the orientation
of the E-field and k represents the direction of propagation of the incident light. (c) Optical
micrographs of sub-surface channels etched in fused silica. The top channel corresponds to (a), the
bottom channel corresponds to (b) and the channel in the middle corresponds to linear polarisation
with E at 45ı to S (All images reproduced and adapted with permission from Ref. [8])
silica using sub 120 fs pulses of 800 nm light at a PRF of 1.0 kHz. They observed
that at low irradiances linearly polarised light induces a larger refractive index
modification than circularly polarised light, and that the situation reverses at larger
irradiances. The authors suggested that at lower irradiances multi-photon ionisation
dominates over tunnelling ionisation and that linearly polarised light therefore
induces higher photoionisation frequencies than circularly polarised light. At higher
irradiances the situation may be reversed as tunnelling ionisation plays a more
significant role.
The laser polarisation has also been shown to play an important role in the
refractive index modification of crystalline materials. Nejadmalayeri et al. [42]
demonstrated that the use of circularly polarised light significantly enhanced the
magnitude of the refractive index modification that could be induced in LiNbO3 .
They suggested that the use of circular polarisation may increase the efficiency and
localisation of energy deposition into the material by reducing nonlinear absorption
and refraction effects as the pulse propagates towards the focus.
The laser polarisation can also strongly influence the magnitude of the chemical
etch-rate increase that can be induced in fused silica using ULI. As shown in
Fig. 13.8, Hnatovsky et al. [8] demonstrated that the ULI induced nano-grating
structures shown in Fig. 12.3b enable HF acid to efficiently penetrate efficiently into
the irradiated material. They also demonstrated that when ULI was used to fabricate
a subsurface micro-channel, a dramatically higher etch rate was achieved when the
nano-gratings were aligned parallel, rather than perpendicular, to the direction of
the micro-channel.
The pulse duration has been shown to play an important role in the ULI process.
Zhang et al. [43] investigated the effect of pulse duration on the propagation loss
and birefringence of waveguides inscribed in fused silica using 800 nm pulses
at a pulse repetition frequency of 1.0 kHz. The authors varied the pulse duration
between 100 fs and 2 ps and found two windows at 100 fs and 1 ps which enabled
the inscription of waveguides with relatively low propagation losses (0.5 dB/cm).
Interestingly, they also found that waveguides inscribed using the 1 ps pulse duration
exhibited significantly reduced birefringence compared to those inscribed using
lower pulse durations. The mechanisms by which the pulse duration impacted the
properties of the waveguides are not yet understood.
The pulse duration has also been shown to play a crucial role when inscribing
waveguides in highly nonlinear materials such as LiNbO3 [42] and ZnSe [44].
Macdonald et al. [44] investigated the effect of pulse duration when inscribing
waveguides in ZnSe using the 1,047 nm pulses at a PRF of 2.0 MHz. They varied the
pulse duration between 500 fs and 2.0 ps and found that waveguides could only be
inscribed using pulse durations >1.0 ps. The authors suggested that the use of longer
pulses reduced the peak power for a given pulse energy, thus reducing nonlinear
effects (such as self focusing, pulse break up and filamentation) which reduce the
efficiency with which energy can be deposited in the focal region.
The effect of pulse duration on the chemical etch rate increase that can be induced
in fused silica using ULI has been comprehensively studied by Hnatovsky et al.
[8]. They used 800 nm pulses at a PRF of 100 kHz and observed that the pulse
duration strongly affected the magnitude of the ULI induced chemical etch rate
increase. For example, when the authors inscribed sub-surface structures using a
TWG, linearly polarised light with the E-field perpendicular to the scan direction,
and 1.0 J pulses, they observed that structures inscribed with a pulse duration of
50 fs exhibited a chemical etch rate of 2.0 m/min, whereas structures inscribed
using a pulse duration of 185 fs exhibited a chemical etch rate of 5.5 m/min.
The authors were able to demonstrate that the chemical etch rate differences were
related to the properties of the nano-grating structures formed using the two different
pulse durations. The interested reader is directed to Refs. [15] and [16] for theories
about the nano-gratings formation, and Refs. [8] and [16] which explore the effect
of nano-gratings on the chemical etch rate in fused silica.
Finally, it is also worth noting that when using the TWG, the properties of the
inscribed structure may also depend on whether the substrate is translated along
the Cve or ve direction. In crystalline LiNbO3 for example, it has been observed
that the morphology of the inscribed structure may depend on whether the sample
is translated along the Cve or ve crystallographic y-axis, and that this directional
dependence is reversed when the direction of propagation of the inscription beam
along the crystallographic z-axis is reversed [45]. It has been suggested that this
phenomena is due to a light-induced thermal current – the direction of which is
dependent on the crystal orientation with respect to the sample translation direction
and the beam propagation direction. Non-reciprocal phenomena have also been
observed in amorphous silica glass [46]. In this case, the authors demonstrated
that pulse front tilt across the beam results in an intensity gradient in the E-field
across the focal region. This gradient acts, via the ponderomotive force, to trap and
displace the free-electron plasma. The non-reciprocity in the ULI process comes
from the fact the direction of the ponderomotive force is determined by the direction
of the pulse front tilt. It is reasonable therefore to expect that the properties of
the inscribed structure would depend on the relative angle between the sample
translation direction and the direction of the ponderomotive force.
13.5.8 Controlling the Cross-Section of ULI-Waveguides
The potential asymmetry of structures inscribed using the TWG can be a particular
problem for optical waveguide inscription. A number of techniques have therefore
been demonstrated which address this issue. These include the astigmatic beam
shaping [35], slit-beam shaping [47], deformable mirror [48] and multiscan [29, 49]
techniques. The first three of these techniques use beam shaping in some manner
to shape the E-field distribution in and around the focus and hence the waveguide
cross section. The multiscan technique on the other hand simply accepts that the ULI
modification created by a single scan of the material through the focus may exhibit
a high degree of asymmetry, and relies on correcting this by scanning the sample
through the focus multiple times to “build” the desired waveguide cross section
from the modified regions created by each scan. It should be noted that waveguides
inscribed using a TWG are not always asymmetric, and thermal accumulation and
diffusion effects can act to create waveguides that exhibit cross sections that are
significantly more symmetric than would be expected from the E-field distribution in
and around the focus. The techniques described in this section are therefore mostly
applicable to waveguides inscribed using low PRF laser systems.
The first technique developed to control the cross section of ULI fabricated
optical waveguides was the astigmatic beam shaping technique – first demonstrated
by Cerullo et al. [35, 50] in 2002. The idea behind the astigmatic beam shaping
technique, the experimental setup for which is shown in Fig. 13.9, is that the width of
a waveguide inscribed along the x-axis is not normally dependant on the beam waist
diameter along the x-axis. This fact can be exploited by focusing tightly in the x–z
plane to reduce the Rayleigh range of the focus in this plane. The rapid divergence of
the beam in the x–z plane reduces the depth of focus of the beam, reducing the width
of the waveguide along the z-axis. The size of the focus along the y-axis can then be
used to control the width of the waveguide along the y-axis. Although this technique
would work well in theory, in practice a beam waist ratio (! 0y /! 0x ) of 10 would
be required to achieve a symmetric waveguide cross section. This would require a
high demagnification cylindrical telescope, which would be difficult to align, would
introduce significant aberrations and would be difficult to optimise. To solve these
issues, Cerullo et al. demonstrated that by adjusting the astigmatic difference (z0 ),
the offset in the focal planes for ! 0y and ! 0x , a symmetric waveguide could be
inscribed using beam waist ratios of only 2–3. The basis of this suggestion is that
for a focused astigmatic beam, the region of highest intensity is normally positioned
Fig. 13.9 Experimental

setup for the astigmatic beam
shaping technique
(Reproduced and adapted
with permission from
Ref. [35])
in the plane corresponding to the smallest spot – ! 0x in this case. As shown in

Fig. 13.10, the width of the modified region, and hence the waveguide core, can
therefore be adjusted by simply varying the astigmatic difference without increasing
the beam waist ratio.
The astigmatic beam shaping technique is just one of the waveguide shaping
techniques that have been developed. As mentioned above, the slit-beam shaping,
deformable mirror and multiscan techniques have also been developed. Both the
slit-beam shaping and deformable mirror techniques essentially operate using the
same principles as the astigmatic beam shaping technique – and as a result will
not be discussed further here. In the multiscan technique, the final cross section of
the modified region is constructed by repeatedly scanning the sample through the
laser focus. In this case, the asymmetric modified regions created by each scan
are used as a building block for the final cross section. In comparison to other
waveguide shaping techniques, the multiscan technique provides the highest degree
of control over the spatial distribution of the modification. Furthermore, because
the modified region is built up over many scans, the multiscan technique allows
the peak irradiance on the sample to be minimised, which may be important for
inscribing structures in materials where excessively high irradiances can induce
unwanted material modifications e.g. amorphisation of a crystal [22].
Finally, to conclude this section on waveguide shaping, it should also be men-
tioned that there is also another technique based on spatio-temporal focusing (STF)
which also has the potential to enable the inscription of symmetric waveguides. In
the STF technique, first applied to ULI by He et al. [51], a spectral chirp is induced
Fig. 13.10 (Left) Modelled beam profiles in the y/z plane (solid curves) and the x/z plane (dashed
curves) for focused astigmatic Gaussian beams with ! 0x D 1.0 m, ! 0y D 3.0 m and (a) Z0 D 0
(b) Z0 D 100 m. The shaded area corresponds to the waveguide shape that would be expected
according to the modelled distribution of the free electron plasma induced by the pulse. (Right) Left
column: Optical microscope images of the waveguide cross section written using an astigmatic
beam with ! 0x D 1.2 m and ! 0y D3.6 m. Right column: Corresponding simulated electron
density profiles (All images reproduced and adapted with permission from Ref. [35])
across the beam prior to entering the lens. The effect of this chirp is to reduce the
spectral bandwidth of the pulse at each point across the beam. According to Fourier
theory, this reduction stretches the pulse temporally, and its duration can only be
fully restored in the focal region where the spectral components of the pulse are
spatially reunited. In effect, the pulse is focused both spatially and temporally by
the objective lens. Since the pulse duration directly determines the peak power of
the pulse, the gradient of the temporal focusing can be used to control the Rayleigh
range of the peak E-field distribution of the focus. The STF technique therefore
uniquely enables the creation of a peak E-field distribution that is close to spherical
in structure. Under these circumstances, the cross section of the inscribed structure
would be symmetric, regardless of the sample translation direction. This technique
is yet to be applied to the inscription of optical waveguides and has only been used
to fabricate microfluidics using selective etching. It is reasonable to expect that it
will soon be applied to waveguide inscription.
13.6 Applications of Ultrafast Laser Inscription
Due to its unique fabrication capabilities, ULI is finding applications in a wide

variety of areas – far too many to comprehensively review in this chapter. This
section is therefore intended to provide the reader with a flavour of a few of these.
13.6.1 Passive Waveguide Devices
Compared to the multi-million dollar setup and high running costs of a conventional
planar waveguide fabrication plant, the few hundred thousand dollar setup costs and
low running costs of a ULI system are insignificant. Furthermore, despite the inher-
ently serial fabrication nature of ULI, the possibility of translation velocities in the
10’s of mm.s1 makes ULI potentially well suited to the mass production of simple
passive waveguide devices for applications in areas such as telecommunications and
optical sensor networks.
To date, a range of passive waveguide devices, including wavelength division
multiplexers [30], power splitters [40], Bragg-waveguides [52] and multicore fibre
couplers [53] have been fabricated using ULI. For example, Eaton et al. [40] used
ULI to fabricate evanescent field power splitters which performed a broadband
splitting operation throughout the 1,250–1,650 nm spectral region. The authors
of this study were able to achieve a range of power splitting ratios by inscribing
asymmetric splitters which were realised using different translation velocities for
each arm of the splitter.
Another ULI fabrication capability that is attractive for passive waveguide
devices is the inscription of waveguides with Bragg-gratings – Bragg-waveguides.
Bragg-waveguides can be inscribed using a number of different approaches. The
first ULI fabricated Bragg-waveguide was demonstrated by Marshall et al. in 2006
[54]. In this work, 800 nm pulses at a PRF of 1.0 kHz were used to first inscribe a
waveguide in fused silica. A second order grating operating at 1,550 nm was then
inscribed on top of the waveguide by translating the substrate through the focus a
second time, exposing the waveguide to a single pulse at each grating period. These
Bragg-waveguides exhibited a low grating strength and were slow to inscribe due to
the low pulse repetition rate of the laser system. To overcome these issues, Zhang
et al. [52] later demonstrated that high strength (>30 dB transmission attenuation)
first order gratings could be inscribed in fused silica using an externally modulated
ultrafast fibre laser operating at a PRF of 500 kHz, thus opening the way to the rapid
ULI fabrication of high quality, commercially interesting Bragg-waveguide devices
in fused silica.
13.6.2 Active Waveguide Devices
ULI can be used to fabricate waveguides in almost any transparent material, making
it exceptionally well suited to the fabrication of novel active waveguide devices
such as waveguide amplifiers and lasers. Much of the initial work in this area
was pioneered by the group at the Politecnico di Milano. For example, the first
demonstration of fibre-to-fibre net gain by a ULI fabricated waveguide amplifier
was in 2004 by Osellame et al. [55], who inscribed a waveguide in an ErYb-doped
phosphate glass. The 12 mm long amplifier exhibited a peak net gain of 1.2 dB at
1,533 nm under pumping at 980 nm. Later the same year, Taccheo et al. [56] used a
20 mm long ULI fabricated ErYb-doped waveguide amplifier as the gain element in
the first ULI fabricated waveguide laser. This device emitted 1.7 mW of continuous
wave 1533.5 nm radiation under 420 mW of pumping at around 980 nm. In 2006,
the same group demonstrated the first ULI fabricated mode-locked waveguide laser
by constructing an optical fibre-ring cavity which incorporated a carbon nanotube
saturable absorber and a 39 mm long ULI fabricated ErYb-doped amplifier [57].
Under 430 mW of pumping at 980 nm, the device emitted a 16.74 MHz train of
1.76 ps pulses with a central wavelength of 1,535 nm and an average output power
of 0.1 mW.
The active waveguide applications of ULI have now progressed considerably,
and waveguide lasers operating at around 1.9 m [58, 59], 1.5 m [60], 1.04 m
[61] and 1.06 m [62] have been realised by inscribing waveguides in Tm-, Er-,
Yb- and Nd-doped glasses respectively. In 2010, Thomson et al. [63] demonstrated
the ULI fabrication of a high gain Er-doped bismuthate glass waveguide amplifier
which exhibited a peak fibre-to-fibre net gain of 16.0 dB at 1,533 nm under 1.0 W of
980 nm pumping. Beecher et al. [64] later used this waveguide amplifier as the laser
gain element in a mode-locked laser cavity. Under 350 mW of 980 nm pumping, the
laser emitted a 40 MHz train of 320 fs pulses with a central wavelength of 1.56 m
and an average output power of 1.25 mW.
The level of integration that can be achieved in ULI waveguide lasers has
also been the subject of significant research attention. The group at Macquarie
University successfully demonstrated the first ULI fabricated distributed feedback
waveguide laser by inscribing a Bragg-waveguide in an ErYb-doped phosphate glass
substrate [65]. Under 710 mW of pumping at 980 nm, the 20.0 mm long device
emitted a maximum output power of 0.37 mW at a lasing wavelength of 1,537 nm.
The same group later reported the ULI fabrication of a high power and efficient
distributed feedback waveguide laser by inscribing a Bragg-waveguide in a Yb-
doped phosphate glass substrate [61]. When pumped using 726 mW of 976 nm
light, the 9.5 mm long waveguide laser emitted 102 mW of 1,033 nm light with a
slope efficiency of 17.3 %.
A number of groups have worked to increase the slope efficiencies and output
powers that can be achieved from ULI fabricated waveguide lasers. In 2008 Torchia
et al. [27] reported the ULI fabrication of a 5.0 mm long Nd-doped YAG ceramic
waveguide laser that emitted >80 mW of 1,064 nm radiation under 200 mW of
Fig. 13.11 3D rendering

of the monolithic optical
stretcher fabricated by Bellini
et al. using ULI. The cells
flowing in the microchannel
are trapped and stretched in
the dual beam optical trap
created by the optical
waveguides (Reproduced and
adapted with permission from
Ref. [68])
pumping at 748 nm, resulting in a slope efficiency of 60 %. In 2011 Calmano et al.

[66] demonstrated the generation of 2.35 W of 1,030 nm radiation by a 9.25 mm
long Yb-doped YAG waveguide under 5.52 W of pumping at 969 nm. Finally, in
2011, the Macquarie group [59] demonstrated the ULI fabrication of a Tm-doped
fluorine glass waveguide laser which emitted 47 mW of 1.88 m light with a slope
efficiency of 50 %.
13.6.3 Microfluidics and Bio-photonics
The selective etching capability of ULI has been used to fabricate both surface [2]
and sub-surface microfluidic structures [67]. However, the ability of ULI to readily
integrate microfluidics with optical waveguides is potentially an extremely powerful
capability. In one example, Bellini et al. [68] used ULI to fabricate a monolithic
cell stretcher – a sketch of which is shown in Fig. 13.11. This device consisted
of a ULI fabricated sub-surface microfluidic and two optical waveguides which
intercepted the microfluidic. The authors demonstrated that red blood cells could
be inserted into the microfluidic and optically trapped by counter-propagating laser
beams coupled into the optical waveguides. The authors also demonstrated that the
cells could be stretched by the optical forces when the trapping laser power was
increased.
Interestingly, the optical stretching properties of cells have been shown to be a
marker for the malignant state of a cell [69], without a requirement for chemical
labelling. This simple and elegant demonstration clearly demonstrates the power of
ULI for fabricating novel and monolithic microfluidic and optofluidic devices for a
plethora of applications in biophotonics and beyond.
Fig. 13.12 Computer assisted drawing of the ULI fabricated displacement sensor (Reproduced
and adapted with permission from Ref. [3])
13.6.4 Micro-Systems
The capability of ULI to fabricate micro-optics, micro-mechanics and integrated

optics is highly attractive for the development of novel micro-systems. In one
particularly impressive demonstration, Bellouard et al. [3] used ULI to fabricate
a monolithic displacement sensor. The device, which is shown conceptually in
Fig. 13.12, was fabricated from a single piece of fused silica. It consisted of a mobile
platform suspended on micro-flexure hinges (like the one shown in Fig. 13.4a)
which connected it to the stationary frame. One end of the mobile platform acted as
a sensor tip which could be placed into contact with a surface whose displacement
was to be sensed. At the opposite end of the mobile platform, an array of optical
waveguides acted as an integrated linear encoder (ILE). The displacement of the
sensor tip could be optically read out to a resolution of 50 nm as the ILE
moved passed a readout waveguide inscribed in the stationary frame. As mentioned
above, the entire device was fabricated from a single piece of silica using ULI.
The hinges and mobile platform were formed using ULI induced selective etching
and the optical waveguides were fabricated using the ULI induced refractive index
modification. Since all the components were inscribed using a single ULI procedure,
all complements were passively aligned to within the accuracy of the translation
stages. Although it still remains to be seen if this specific micro-system will find
real world applications, it is certainly an excellent example of how ULI is extremely
well suited to certain high value manufacturing applications.
13.6.5 Astrophotonics
Astrophotonics is the field where photonic principles are applied to instrumentation

for astronomy, with the aim of reducing the cost, size, weight and complexity
Fig. 13.13 Sketch of a

multimode-to-single mode
integrated photonic lantern
transition which can be
fabricated using ULI. The
device is viewed from the
multimode waveguide end
of instruments while increasing their performance. Astrophotonic technologies

currently under development include compact high-resolution spectrographs based
on arrayed waveguide gratings (AWGs) [70], highly complex filters based on
Fibre-Bragg-Gratings (FBGs) [71] for removing the light generated by the Earth’s
atmosphere from the celestial light of interest, and integrated optical circuits for
coherent beam combination in stellar interferometry [72]. The unique fabrication
capabilities of ULI have now been identified as being a key to a number of
astrophotonic applications.
The so-called “photonic lantern” is one of the most remarkable astrophotonic
devices that has been developed so far – a guided-wave structure which facilitates
the low-loss coupling of light between a multimode fibre and an array of single
mode fibres [73, 74]. The photonic lantern facilitates the efficient use of single mode
photonic devices, such as AWGs and FBGs, with the often inherently multimode
light captured by a telescope. Until recently, photonic lanterns had only been
fabricated using optical fibre transitions created using either a stack-and-draw
techniques or using tapered multicore fibres. In 2011, Thomson et al. [75] used
the three-dimensional waveguide fabrication capability of ULI to demonstrate the
first integrated photonic lantern (shown conceptually in Fig. 13.13) which has the
capability to perform multimode-to-single modes conversion on-chip. As shown
in Fig. 13.13 the device was fabricated by inscribing a two-dimensional array of
single mode waveguides at one end of the device, and bringing these waveguides
together using three-dimensional transitions to form a single large multimode
waveguide. Using ULI, it may in the future, be possible to fabricate mass-producible
astrophotonic devices which provide diffraction limited processing functions such
as filtering, dispersion and detection but are fed directly with multimode fibres from
the telescope.
The photonic lantern is just one astrophotonic application of ULI that is attracting
attention and it should be noted that a number of groups around the world are using
ULI to develop astrophotonic technologies such as 3D photonic beam combiners
[76, 77], mid-IR integrated optics [77, 78] and 3D pupil re-mapping devices for
exoplanet imaging [79]. Although a ULI fabricated device is yet to produce a
significant astrophysical result, it is surely only a matter of time given the range
of applications that are being investigated.
13.7 Chapter Summary
In this chapter the basic physics of the ULI process was reviewed. We have seen
that ULI relies on the nonlinear absorption of sub-bandgap ultrashort pulses inside
a transparent dielectric, and that the deposited energy induces a local modification
to the material structure. We have seen how this structural modification may
manifest itself in a variety of ways, and that the nature of these manifestations
can be controlled via the various ULI parameters. We have discussed how the ULI
induced refractive index change and chemical etch rate modification can be used
and controlled to inscribed structures such as optical waveguides, micro-mechanics,
microfluidics and micro-optics. Finally, we have outlined a few of the many ULI
applications that are being investigated. To conclude, it is clear that ULI presents
itself as an extremely flexible and unique fabrication tool. In the future we envisage
that ULI, like many other fabrication techniques, will move towards becoming more
of an established fabrication route for both industrial and research scale applications.
Until then, there remains much to be explored in this exciting field.
Acknowledgments RRT acknowledges support through and STFC Advanced Fellowship – Grant
No. ST/H005595/1.
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55. R. Osellame, N. Chiodo, G. Valle, S. Taccheo, R. Ramponi, G. Cerullo, A. Killi, U. Morgner,
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56. S. Taccheo, G. Della Valle, R. Osellame, G. Cerullo, N. Chiodo, P. Laporta, O. Svelto, A. Killi,
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68. N. Bellini, K.C. Vishnubhatla, F. Bragheri, L. Ferrara, P. Minzioni, R. Ramponi, I. Cristiani,
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69. J. Guck, S. Schinkinger, B. Lincoln, F. Wottawah, S. Ebert, M. Romeyke, D. Lenz,

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71. J. Bland-Hawthorn, M. Englund, G. Edvell, New approach to atmospheric OH suppression
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72. P. Kern, E. Le Coärer, P. Benech, On-chip spectro-detection for fully integrated coherent beam
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75. R.R. Thomson, T.A. Birks, S.G. Leon-Saval, A.K. Kar, J. Bland-Hawthorn, Ultrafast laser
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79. N. Jovanovic, P. Tuthill, S. Lacour, M. Ams, S. Gross, B. Norris, P. Stewart, J. Lawrence,
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Poster Sessions
R. Aviles-Espinosa, G. J. Tserevelakis, S. I. C. O. Santos, G. Filippidis,

A. J. Krmpot, M. Vlachos, N. Tavernarakis, A. Brodschelm, W. Kaenders,
D. Artigas, and P. Loza-Alvarez: Cell division stage in C. elegans imaged using
third harmonic generation microscopy.
C. R. E. Baer, O. H. Heckl, C. J. Saraceno, C. Kraenkel, T. Sudmeyer and
U. Keller: Yb-doped sesquioxides: Novel materials for highest average power and
shortest pulse duration from mode-locked thin disk laser oscillators.
S. J. Beecher, R. R. Thomson, N. D. Psaila, A. K. Kar, Z. Sun, T. Hasan,
A. G. Rozhin and A. Ferrari: 320 fs pulses from an ultrafast laser inscribed erbium
doped bismuthate waveguide laser.
P. P. Beličev, I. Ilić, Lj. Hadžievski, M. Stepić, Y. Tan and F. Chen: Formation of
nonlinear localized modes in periodic waveguide array with defect.
M. Beresna and P. G. Kazansky: Polarization diffractive optical elements written
by ultrafast direct writing.
M. Blazek and W. Elsaesser: The intensity noise behaviour of multiplexed
superluminescent light emitting diodes.
D. Brida and G. Cerullo: Few-optical-cycle pulse generation from UV to mid-IR
by optical parametric amplifiers.
Y. Bromberg, Y. Lahini, E. Small and Y. Silberberg: Hanbury Brown and Twiss
interferometry with interacting photons.
M. Butkus, J. Rautiainen, O. G. Okhotnikov, S. S. Mikhrin, I. L. Krestnikov,
D. A. Livshits and E. U. Rafailov: Quantum dot based semiconductor disk lasers
at 1–1.3 m region.
Y. Chen, Z. Chen, W. J. Wadsworth and T. A. Birks: Generation of higher-order
modes for experiments in nonlinear fibre optics.

Graduate Series, DOI 10.1007/978-3-319-00017-6,
352 Poster Sessions
R. Cherif and M. Zghal: Supercontinuum generation and Brillouin scattering in

highly nonlinear crystal fibres.
J. M. Dahlstrom, E. Mansten, M. Swoboda, K. Klunder, T. Fordell, P. Johnsson,
X. He, R. Rakowski, M. Gisselbrecht, T. Ruchon, A. L’Huillier and
J. Mauritsson: Characterization and control of high-order harmonic generation
using two-color laser fields.
J. Darginavicius and A. Dubietis: Generation of 30 fs ultraviolet pulses by four-
wave optical parametric chirped pulse amplification.
T. Denis, P. J. M. van der Slot and K.-J. Boller: The compact photonic FEL – A
proof of principle.
S. Doring, S. Richter, S. Nolte and A. Tunnermann: In-situ imaging of the deep
drilling of silicon with ultrashort laser pulses.
G. Dridi, S. Guerin, V. Hakobyan and H. R. Jauslin: Ultrafast stimulated Raman
parallel adiabatic passage by shaped pulses.
M. Duffy, O. Kelly, C. R. Calvert, R. B. King, I. D. Williams and J. B.
Greenwood: The analysis of molecules in intense femtosecond laser pulses.
H. Fattahi, C. Y. Teisset, V. Pervak , F. Krausz and A. Apolonski: Sub 10 fs,
700 nJ broadband MHz optical parametric amplifier.
K. A. Fedorova, M. A. Cataluna, I. Krestnikov, D. Livshits and E. U. Rafailov:
Tuning range enhancement in external-cavity InAs/GaAs quantum-dot lasers.
V. K. S. Feige: Non-destructive coating thickness measurements with terahertz
time-domain spectroscopy.
T. I. Ferreiro, J. H. Sun and D. T. Reid: Locking the carrier-envelope-offset
frequency of an optical parametric oscillator without f-2f self-referencing.
X. Ge, D. Gauthier, M. Guizar-Sicairos and H. Merdji: Single shot soft X-ray
holography using extended reference.
G. Golovin, D. Uryupina, R. Volkov, and A. Savel’ev: Registration of 14.4 keV
57Fe nuclear state excitation induced with the help of plasma created by the
powerful femtosecond laser pulse.
M. A. Gonzalez-Galicia, M. Rosethe-Aguilar and J. Garduno-Mejia: Design
and construction of a laser of 10 femtoseconds for the study of aberrations and
dispersive effects.
I. Gris-Sanchez, B. J. Mangan and J. C. Knight: Reducing spectral attenuation
in solid-core photonic crystal fibers.
D. J. Hadden and V. G. Stavros: Photodissociation from aromatic heteroatoms:
Competition between hydrogen and methyl radical elimination.
V. Hakobyan and S. Guerin: Optimization of multi-photon population transfer in
atoms by ultrafast shaped laser pulses.
Poster Sessions 353
T. Hasan, Z. P. Sun, D. Popa, F. Torrisi, F. Wang and A. C. Ferrari: Sub-ps pulse

generation from carbon nanotube and graphene saturable absorbers.
C. Hazera, J. Nillon, S. Montant, E. Cormier and S. Petit: 10 fs, 1 J, 100 kHz
by direct seeding of a NOPA and its fiber pump by a CEP-stabilized oscillator.
O. H. Heckl, C. R. E. Baer, C. J. Saraceno, C. Kraenkel, T. Sudmeyer and
U. Keller: Towards high harmonic generation using a thin disk laser.
M. Heinrich, F. Dreisow, R. Keil, A. Szameit, S. Nolte and A. Tunnermann:
Nonlinear discrete optics in femtosecond laser-written waveguide arrays.
G. G. Henderson, O. Johansson and E. E. B. Campbell: Interaction of ultrashort
laser pulses with carbon nanomaterials.
C. Hernandez-Garcia, E. Conejero, J. Ramos, J. A. Perez-Hernandez, L. Roso
and L. Plaja: Computing high order harmonic propagation within the discrete
dipole approximation.
G. D. Hobbs, C. E. de Nobriga, W. Ding, W. J. Wadsworth, A. V. Gorbach,
D. V. Skryabin, J. C. Knight, A. Samarelli, M. Sorel and R. M. De La Rue:
Linear dispersion measurements of supermodes in strongly coupled SOI photonic
wires.
L. E. Hooper, P. J. Mosley, A. C. Muir, W. J. Wadsworth and J. C. Knight: All-
normal dispersion photonic crystal fiber for low-noise supercontinuum generation.
D. A. Horke, G. M. Roberts, J. Lecointre, and J. R. R. Verlet: Ultrafast
photoelectron imaging of complex molecular and cluster anions.
I. Ilić, P. P. Beličev, A. Kanshu, M. Stepić, D. Kip and C. Ruter: Analysis of
localized modes in nonlinear assymetric waveguide arrays.
A. James, J. van Thor, J. Tisch and J. Marangos: Laser spectroscopy of
photoactive proteins.
C. Jappy, C. Leburn, N. K. Metzer, C. T. A. Brown and W. Sibbett: Repetition
rate tuning in mid infra red ultrafast solid state lasers.
E. Jelmakas, R. Tomasiunas, E. Rafailov and I. Krestnikov: Absorption recovery
on femtosecond time scale of 9-V nanostructures.
O. Johansson, G. Henderson and E. E. B. Campbell: Ionisation dynamics of
complex molecules.
C. Kern, M. Zurch, S. Eyring and C. Spielmann: Limitations of ultrafast
nonlinear nano-optics.
F. Kienle, K. K. Chen, S.-U. Alam, C. B. E. Gawith, J. I. Mackenzie, D. C.
Hanna, D. J. Richardson and D. P. Shepherd: A high power optical parametric
oscillator synchronously pumped by a fibre-amplified gain switched laser diode.
M. C. Kohler, K. Z. Hatsagortsyan and C. H. Keitel: Phase-matched coherent
hard X-rays from relativistic high-order harmonic generation.
354 Poster Sessions
N. Krebs, R. A. Probst and E. Reidle: Generation of sub-20 fs shaped UV pulses

and their application in spectroscopy.
T. P. Lamour, J. Sun and D. T. Reid: Wavelength stabilisation of a synchronously-
pumped optical parametric oscillator.
S. Landon, E. Audouard and R. Stoian: Micro- and nano- femto machining
workstation with spatial control of the phase.
R. Livingstone, O. Schalk, A. Boguslavskiy, R. J. Donaldson, M. Iljina, G. Wu,
A. Stolow and D. Townsend: Ultrafast molecular dynamics of model biological
systems.
L. Lotscher, T. Ganz, A. Apolonskiy and F. Krausz: High energy pulse compres-
sion using ROD-photonic crystal fiber.
G. Machinet, F. Lacroix and E. Cormier: Development of a high average power
femtosecond fiber laser and applications.
B. Mahieu, G. De Ninno and D. Garzella: FERMI@Electtra: A seeded single-pass
free-electron laser in the VUV-XUV spectral range.
M. Mang, A. Schiavi, D. Austin, A. Wyatt, and I. Walmsley: Space-time
characterization of attosecond pulses and quasi-phase matched harmonics.
E. Mansson, M. Gisselbrecht, T. Fordell, K. Klunder, P. Johnsson, M. Miranda,
M. Dalhstrom, J. Mauritsson, A. L’Huillier and S. L. Sorensen: Imaging
attosecond ionization dynamics.
K. Mazur, I. A. Heisler and S. R. Meech: Solvation of peptides: A dynamic
perspective.
D. McCabe, D. Austin, S. Gigan and B. Chatel: Spatiotemporal characterization
of the speckle patterns produced by scattered ultrafast pulses.
R. McCracken, J. Sun and D. T. Reid: Multicolour outputs from a Ti:sapphire
laser and a synchronously pump OPO for single cycle optical pulse synthesis.
G. Nava, J. Parravicini, P. Minzioni, I. Cristiani and V. Degiorgio: Photorefrac-
tive properties of zirconium doped lithium niobate crystals.
J. Nillon, G. Machinet, S. Montant and E. Cormier: High repetition rate fiber
pumped optical parametric amplifier.
D. I. Nikitichev, M. A. Cataluna, D. Livshits, I. Krestnikov and E. Rafailov:
Ultrashort pulse generation from quantum-dot laser diodes.
R. M. Oldenbeuving, E. J. Klein, H. L. Offerhaus, C. J. Lee, K.-J. Boller and
M. Verhaegen: Waveguide-based external cavity semiconductor laser arrays.
J. R. Orchard, D. T. D. Childs, L.-C., Lin, J. S. Roberts, B. J. Stevens and R. A.
Hogg: Development of electrically pumped VECSELs.
Poster Sessions 355
C. Ott, P. Raith and T. Pfeifer: Attosecond-timescale electronic wavefunction

beating.
S. Pekarek, M. C. Stumpf, A. E. H. Oehler, T. Sudmeyer and U. Keller:
CEO frequency measurement of a SESAM-modelocked 1.5 m solid-state laser
oscillator.
P. Piksarv, M. Lohmus, H. Valtna-Lukner, P. Bowlan, R. Trebino, and P. Saari:
New insights into the diffraction of ultrashort light pulses.
D. Popa, Z. Sun, F. Torrisi, T. Hasan, F. Wang, F. Bonaccorso, D. M. Basko and
A. C. Ferrari: Graphene mode-locked ultrafast laser.
P. Raith, C. Ott and T. Pfeifer: Control of attosecond pulse generation using
kinetic heterodyne mixing.
R. Rakowski, X. He, J. Dalhstrom, C. Heyl, C. Erny, E. Mansten and
A. L’Huillier: Intensity modulation in harmonic spectra.
E. Ramsay, R. R. Thomson, N. D. Psaila, A. K. Kar and D.T. Reid: Ultrafast
laser inscribed monolithic ring laser.
S. Ricaud, M. Delaigue, A. Courjaud, F. Druon, P. Georges, P. Camy,
R. Moncorge and E. Mottay: Broadband Yb:CaF2 regenerative amplifier.
S. Richter, S. Doring, S. Nolte and A. Tunnermann: Bonding of glass with
femtosecond laser pulses at high repetition rates.
C. Romero, R. Borrego-Varillas, J. R. Vazquez de Aldana, G. Minguez-Vega,
O. Mendoza-Yero and L. Roso: Ultrafast second harmonic generation with a
kinoform diffractive lens.
M. Rossetti, P. Bardella and I. Montrosset: Modeling passive mode-locking in
quantum dot lasers: A comparison between a finite difference travelling-wave model
and a delayed differential equation approach.
P. W. Roth, A. J. Maclean, D. Burns and A. J. Kemp: Directly diode-laser-
pumped Ti:sapphire laser.
E. Rubino, S. Cacciatori, F. Belgiorno, G. Ortenzi, V. Gorini, V. G. Sala,
M. Clerici and D. Faccio: Direct observation of analogue Hawking radiation.
C. J. Saraceno, O. H. Heckl, C. R. E Baer, T. Sudmeyer and U. Keller: Pulse
compression in passive and active fibers using high power modelocked thin disk
oscillators as seeds.
M. Schenk, M. Kruger and P. Hommelhoff: Energy-resolved measurements of
laser-triggered electron pulses from sharp metal tips.
A. Schiavi, M. Mang, D. Austin, A. Wyatt and I. Walmsley: Space-time
characterization of complex pulses in the UV, NIR and MIR.
A. Tajalli, S. Weber, D. Austin, D. McCabe and B. Chatel: Full spatio-temporal
characterization of shaped ultrashort UV pulses.
356 Poster Sessions
G. J. Tserevelakis, A. J. Krmpot, M. Vlachos, C. Fotakis, N. Tavernarakis and

G. Filippidis: Imaging different C. elegans embryonic stages by employing third
harmonic generation microscopy.
A. Vernaleken, B. Bernhardt, A. Ozawa, T. W. Hansch and T. Udem: On the
road to HeC : A status report in the XUV.
F. Wang, Z. Sun, T. Hasan, D. Popa and A. C. Ferrari: Duration-switchable,
wideband tunable ultrafast laser mode-locked by carbon nanotubes.
Z. Zhang and D. T. Reid: FTIR using asynchronously pumped OPOs.
Participants
Abdullah Alharbi
(University of Ottawa)
Vid Agrež
(University of Ljubljana)
Alexandria Anderson
(Femtolasers GmbH)
Rodrigo Aviles-Espinosa
(Institut de Ciencies Fotoniques)
Cyrill Baer
(ETH Zurich)
Tom Baer
(Stanford University)
Stephen Beecher
(Heriot-Watt University)
Petra Beličev
(Vinca Institute of Nuclear Sciences)
Martynas Beresna
(University of Southampton)
Martin Blazek
(Technische Universitat Darmstadt)
Henry Bookey
Elisabeth Bothschafter
(Technische Universitat Munchen)

358 Participants
Daniele Brida
(Politecnico di Milano)
Phil Bucksbaum
(Stanford University)
Mantas Butkus
(University of Dundee)
Giulio Cerullo
(Politecnico de Milano)
Yong Chen
(University of Bath)
Rim Cherif
(Ecole Superiuere des Communications des Tunis)
Debaditya Choudhury
Marcus Dahlstrom
(Lund University)
Louis Daniault
(Institut d’Optique)
Julius Darginavicius
(Vilnius University)
Thomas Denis
(University of Twente)
Sven Doring
(Universitat Jena)
Chris Dorman
(Coherent Scotland)
Ghassen Dridi
(Universite de Bourgogne)
John Dudley
(Universite de Franche-Comte)
Martin Duffy
(Queen’s University Belfast)
Hanieh Fattahi
(Max-Planck-Institut fur Quantenoptik)
Ksenia Fedorova
Participants 359
Volker Feige
(Automation Dr.)
Allister Ferguson
(University of Strathclyde)
Teresa Ferreiro
Georg Gademann
(FOM-AMOLF)
Xunyou Ge
(CEA Saclay)
Gregory Golovin
(Moscow State University)
Miguel Gonzalez-Galicia
(Universidad Nacional Autonoma de Mexico)
Itandehui Gris Sanchez
David Hadden
(University of Warwick)
Vahe Hakobyan
(Universite de Bourgogne)
Tawfique Hasan
(University of Cambridge)
Christophe Hazera
(Universite de Bordeaux)
Oliver Heckl
(ETH Zurich)
Matthias Heinrich
(Universitat Jena)
Gordon Henderson
(University of Edinburgh)
Carlos Hernandez-Garcia
(Universidad de Salamanca)
Christoph Heyl
(Lund University)
Gareth Hobbs
360 Participants
Lucy Hooper
Daniel Horke
(University of Durham)
Christopher Hutchison
(Imperial College London)
Igor Ilic Vinca
(Institute of Nuclear Sciences)
Ann James
Christine Jappy
(University of St Andrews)
Edgaras Jelmakas
(Vilnius University)
Olof Johansson
(University of Edinburgh)
Ajoy Kar
Ursula Keller
(ETH Zurich)
Christian Kern
(Universitat Jena)
Juho Kerttula
(Tampere University of Technology)
Vikaran Khanna
(University of Hamburg)
Florian Kienle
(University of Southampton)
Markus Kohler
(Max-Planck-Institut fur Kernphysik)
Nils Krebs
(LMU Munich)
Tobias Lamour
Sebastien Landon
(Universite de Saint-Etienne)
Participants 361
Ken Ledingham
Ruth Livingstone
Madis Lohmus
(University of Tartu)
Lauryna Lotscher
(LMU Munich)
John Macdonald
Guillaume Machinet
Benoit Mahieu
(University of Nova Gorica & CEA Saclay)
Matthias Mang
(University of Oxford)
Erik Mansson
(Lund University)
Cristian Manzoni
Jon Marangos
Rose Mary
Kamila Mazur
(University of East Anglia)
David McCabe
(Universite de Toulouse)
John McCarthy
Richard McCracken
Joanna McLenaghan
Niels Meiser
(KTH Stockholm)
362 Participants
Margaret Murnane
(University of Colorado)
Giovanni Nava
(University of Pavia)
Catalin Neacsu
(Femtolasers GmbH)
Danill Nikitichev
Julien Nillon
Stefan Nolte
(Universitat Jena)
Ruud Oldenbeuving
(University of Twente)
Malte Oppermann
Jonathan Orchard
(University of Sheffield)
Christian Ott
Tim Paasch-Colberg
Monika Pawłowska
(Freie Universitat Berlin)
Selina Pekarek
(ETH Zurich)
Peeter Piksarv
(University of Tartu)
Dario Polli
Daniel Popa
Philipp Raith
Rafal Rakowski
(Lund University)
Participants 363
Cristtel Ramirez
Euan Ramsay
Jussi Rautiainen
(Tampere University of Technology)
Derryck Reid
Sandrine Ricaud
(Laboratoire Charles Fabry de l’Institut d’Optique)
Soren Richter
(Universitat Jena)
Carolina Romero
(Universidad de Salamanca)
Mattia Rossetti
(Politecnico di Torino)
Peter Roth
Eleonora Rubino
(Universita degli Studi dell’Insubria)
Clara Saraceno
(ETH Zurich)
Markus Schenk
Andrea Schiavi
Kai Seger
(KTH Stockholm)
Wilson Sibbett
Teresa Sibillano
(University of Bari)
Eran Small
(Weizmann Institute)
Richard Squibb
364 Participants
Jeff Squier
(Colorado School of Mines)
Robert Stefanuik
(University College Dublin)
Jinghua Sun
Ayhan Tajalli
(Universite de Toulouse)
Robert Thomson
Dave Townsend
George Tserevelakis
(IESL – Foundation for Research and Technology – Hellas)
Thomas Udem
Mor Verbin
(Weizmann Institute)
Andreas Vernaleken
William Wadsworth
Ian Walmsley
Frank Wang
Zhaowei Zhang
The SUSSP66 Participants
16th Aug. 2010 – The Sunken Garden – Heriot-Watt University – Edinburgh

Index
A Auger
Aberration decay, 68
chromatic, 303 electrons, 162, 164
spherical, 303 photoelectron peaks, 164, 165
Acoustic wave propagation, 166
Acousto-optic tunable filter (AOTF), 282
Adiabatic B
gas preparation for Raman conversion, 64 Backfolding, 156
pulse compression, 211 Back-projection algorithm, 14
Akhmediev breathers, 186, 187 Backscattered photons, 243, 245
Ammosov, Delone and Krainov (ADK) Ballistic correction, 166
theory, 51 Beam waist, 332, 338, 339
Analytic signal, 3–5 Beer’s law, 293, 297
frequency representation, 4 Binding energy, 155
Ancilla, 17–18 Blazed grating, 281
chirp rate, 17 Born-Oppenheimer, 106–107
Angle-resolved photoemission spectroscopy approximation, 107, 108, 113
(ARPES), 154, 156–158 surfaces, 106–107
nano ARPES, 170 Bragg
Ankylography, 168 gratings, 341
AOTF. See Acousto-optic tunable filter (AOTF) mirror, 81, 82, 88, 91
Apollon laser, 246 peak, 236
Arbitrary waveform generator, 120 Bremsstrahlung, 242
ARPES. See Angle-resolved photoemission Brillouin
spectroscopy (ARPES) scattering, 198
Arrayed waveguide gratings (AWGs), 345 zone, 156
Astrophotonics, 344–345 Brumer-Shapiro, 106, 111–113
Atomic clock, 129, 135, 136, 138, 143
Attosecond
dynamics, 61 C
generation, 45–69 Cancer therapy using protons and ions,
measurement technology, 45 235–237
pulse bursts, 152 Carrier envelope, 120, 142–143
pulse production, 56–58 offset frequency, 4, 134
pulse train (APT), 57 phase shift, 130
single pulse, 67 phase (CEP) stabilisation, 47, 58

368 Index
Carrier frequency, 26, 40, 46, 47, 60, 63, 86, first-order dispersion (group delay), 80
129, 131, 142 flattened fibre, 213
chirp, 86, 131 geometrical, 80, 82
Catalysis, 162 grating pairs, 80
Cell stretcher, 343 group-delay dispersion (GDD), 15, 82, 268
Charge group velocity dispersion (GVD), 26, 98,
density wave, 156, 158 179, 202–203, 210, 215, 272
migration, 46, 47 high-order, 184
transfer, 149, 162, 163 intra-cavity, 80, 130
Chirped pulse amplification (CPA), 2, 40, 228 material, 56, 80, 203–206, 213, 303
Chronocyclic mirror, 81, 82
phase space, 6, 7 normal, 86, 184, 189, 190, 204, 205, 208,
tomography, 14 213, 215, 219
wigner function, 6 optical fibre, 202–205
Coherent second-order, 80, 268
diffractive imaging, 167–169 shifted fibre, 132
oversampling phase retrieval third-order (TOD), 80, 81, 209, 211,
technique, 169 268, 270
phase retrieval algorithm, 168 waveguide, 82, 153, 179, 204, 206–208,
wakefield emission, 65 213, 215, 220
x-ray generation, 150 zero dispersion wavelength, 132, 182, 184,
Colour centres, 301, 327 185, 187, 190, 203, 214, 215, 219
Complex field envelope, 25 Dispersive waves, 184, 186, 189
Compton scattering, 243, 246 Dream beams, 232
Confocal parameter, 332 Dressed states, 51
Conical intersections, 108–109 laser dressed state continuum state, 51
Correlated-electron materials, 154–158, 161 Dynamic gain saturation, 86, 87
Correlation function, 5, 6, 9, 10
Cosmic rays, 230
Coulomb interaction, 46, 105 E
CPA. See Chirped pulse amplification (CPA) Elbe electron beam, 244
Cross phase modulation (XPM), 197, 198, 202 Electrochemical processes, 162
Cutoff photon energy, 150, 152 Electron
beams via laser plasma interaction,
230–232
D cooling time, 295, 296
Debye sheath, 235 dynamics, 46, 47, 162
Dephasing, 106 heat capacity, 295, 296
DESY, Hamburg, 67 hot, 156, 163, 292, 297
Difference-frequency generation (DFG), 38, 39 laser
Diffraction before destruction, 149 acceleration, 228, 243
Diode-pumping, 73 production, 228–230
Dispersion lattice coupling, 294
anomalous, 86, 87, 184–186, 203, 205, 208, quasi monoenergetic, 232, 235
209, 212, 213, 217–219 quiver
characteristic dispersion, 75, 94, 180, 188 energy, 228, 229
chromatic, 178, 202 motion, 231
compensation, 81, 93, 254, 271 velocity, 231
control in optical fibres, 202–208 relaxation time, 297
control in PCF, 213 spectra, 60, 232
convex, 188–189 temperature, 295–297
double-passed prism, 80 thermal conductivity, 297
engineering, 179 wave-packet, 52
Index 369
Electronic Femtosecond laser micromachining

heat transport, 296 applications, 315. See also Ultrafast
phase locked loops, 129 laser inscription
ELI. See Extreme light infrastructure (ELI) cutting biological materials, 312
Endogenous non-bleaching, 251 hole drilling, 307
Energy relaxation after laser irradiation, 292 laser scalpel, 312
short pulse interaction, 294–297 mask-repair, 304–306
Energy relaxation after laser irradiation long microfluidic channels, 311–312
pulse interaction, 292–294 optical data storage, 311
ENLSE. See Extended nonlinear Schrödinger photodeposition, 313–314
equation (ENLSE) waveguide writing, 302, 310
Evanescent field, 341 Femtosecond laser waveguide writing, 315.
Exawatt laser, 227, 228 See also Ultrafast laser inscription
Extended nonlinear Schrödinger equation longitudinal writing geometry,
(ENLSE), 82 310, 311
Extreme light infrastructure (ELI), 227, transverse writing geometry, 310
243–247 waveguide shaping techniques, 310, 339
Femtosecond x-rays, 150
F Fermat’s principle, 272
FBGs. See Fibre-Bragg-gratings (FBGs) Fermi
Femtochemistry, 45 edge, 162, 163
Femtomagnetism, 158 energy, 158, 296, 297
Femtosecond laser-induced demagnetization, Fermi-Dirac distribution, 292
161 Fermi’s golden rule, 111
Femtosecond laser micromachining, 287–315. level, 155
See also Ultrafast laser incription surface topology, 154
ablation, 273, 287, 289, 298–300 temperature, 296
birefringent refractive index change, Fibre-Bragg-gratings (FBGs), 345
300, 301 Field programmable gate array (FPGA), 253,
bulk damage in transparent materials, 275
300–301 Flourophore photostability, 267
color centre creation, 301, 327 Fluorescence
craniotomy, 272, 273 quantum efficiency, 268
cumulative regime, 302 recovery after photobleaching (FRAP), 266
experimental setup, 168, 302 yield, 266–271
focusing and aberrations (role of), 302–303 Foturan glass, 329, 330
microexplosion, 288, 301 Four-wave mixing (FWM), 38, 212–217
microstructuring, 288, 289, 303, 308, phasematching, 212–215, 219
309, 314 single/pair photon generation, 215–217
nanocrack formation, 301 FPGA. See Field programmable gate array
nanograting formation, 311 (FPGA)
nanoplasma creation, 301 Fraunhofer lines, 140
pulse dispersion (role of), 303–304 Free
pulse duration (role of), 303–304 carrier absorption, 290, 292
pulse interaction with solids, 294 space wavevector, 199, 202
refractive index modification, 288, 311 Free electron laser, 48, 149, 168, 170
repetitive regime, 302 attosecond pulse production, 65–68
spatio-temporal focusing, 271 seeding, 67
sub-diffraction limited machining, 306 Frequency
surface structuring, 308 counters, 129
transparent materials, 309–312 metrology, 132, 178, 182, 190, 219
two-photon photopolymerization, 311, resolved optical gating (FROG), 9
313, 314 FWM. See Four-wave mixing (FWM)
void formation, 300 FZD facility-Dresden, 243
370 Index
G short trajectories during HHG, 54, 61

Gain simple man’s model, 49
factor, 30, 268 spectroscopy, 60–63
saturation, 83, 86, 87 three step model, 49, 50, 151
Gaussian beam optics, 198 waveguide gas pressure, 153
Gires-Tournois interferometer (GTI), 82 waveguide gas species, 153
Gouy phase shift, 153 waveguide size, 153
Group X-ray generation, 150
delay, 79 Husimi distribution, 118
velocity, 36, 79, 80, 130, 131, 133, 179,
201, 202, 220
velocity matching, 219 I
GTI. See Gires-Tournois interferometer (GTI) Impulsive
laser heating, 166
Raman method, 64
H Infinite square potential well, 200
Hadrontherapy, 236, 237 Inhomogeneously-broadened laser, 74
Harmonic Instantaneous
frequency chains, 129 optical frequency, 79
generation, 2 optical power, 77
optical klystron (HOK), 67 Intensity autocorrelation, 10–11
HARPS spectrometer, 140 Interband transitions, 290, 299
Heat Interferogram, 12–13, 17, 19, 282
diffusion, 293–299, 301 Interferometry, 7, 12, 15, 20, 345
diffusion length, 294, 296–298 Inverse scattering transform, 184
of evaporation, 298 Inversion
transport, 164, 166, 293–297 algorithms, 4, 6, 8, 9
Heralded single photon source, 215 procedure, 4
High protocols, 4
field physics, 23, 45–69 Ion
order perturbation theory, 49 beams (laser production), 232–235
value manufacturing, 344 cancer therapy, 235–238
High-harmonic generation (HHG), 57, laser production, 228–232
149–171 Ionisation
classical trajectory picture, 150 avalanche, 291, 292, 299, 325, 326
efficiency, 57, 152 fraction, 153
elastic collision during HHG, 53 impact, 292
electron recollision during HHG, 150 multiphoton, 49, 50, 291, 325, 326, 336
gas-filled waveguide, 153 photoionisation, 291, 292, 325, 336
generating soft x-ray beams, 150–154 potential, 49, 51, 151
hollow waveguide, 153, 169 tunnelling, 50, 51, 150, 291, 325, 336
inelastic excitation during HHG, 53 Isomerization, 115, 116, 121
long trajectories during HHG, 54, 56 ozone, 116
material science experiments, 154–169
optical parametric processes, 53
phase-matching, 23, 150, 152 J
the physics of HHG, 48–53 Jablonski diagram, 267
for probing ultrafast material science, JETI-Jena, 242, 250
149–171
quantum representation, 151
quantum simulations, 150 K
recollision processes, 52–53 Keldysh parameter, 50
return energy during HHG, 54 Kerr
return time during HHG, 54, 56 angle, 159
Index 371
nonlinearity, 76, 179 Microscope objective, 253

optical Kerr effect, 86, 132 achromat, 260
Kramers–Kronig relations, 208 air immersion, 262
infinity-corrected, 253
meniscus, 260
L multi-element, 254
Lamb shift, 139 numerical aperture, 254
Laser oil immersion, 260
acceleration, 228, 243 water immersion, 253
driven transmutation, 248 Modelocking, 74
laser-assisted Auger decay (LAAD), amplitude modulation, 75
165 Kerr-lens modelocking (KLM), 84, 86,
laser-assisted photoelectric effect 93, 130
(LAPE), 162 mechanisms, 74
milling, 307, 308 modelocked condition, 74
production net gain window, 86
electrons, protons, ions and photons, passive, 74–76, 84–91
228–230 Q-switched modelocking (QML), 88
high energy photons, 243–245 resonant passive, 90
positron emission tomography isotope, solitonic, 85, 87
238–240 time-domain/frequency domain
proton and ion beams, 232–235 representations, 75
Lattice temperature, 295–297 Modes. See Optical, fibre modes
Learning feedback algorithms, 121–127 Modulation instability (MI), 186, 190, 197,
Lens. See Microscope objective 218
Linac coherent light source (LCLS), Molecular
Stanford, 67 beam epitaxy (MBE), 89
Liquid crystal tunable filter (LCTF), 282 electronics, 162
Longitudinal hole dynamics, 63
cavity modes, 129–130 Most correlated feature analysis (MCFA), 126
geometry for electron excitation, 159 Multi-dimensional data for control, 126–127
Lorentz force, 231 Multipath interference, 112
Multiphoton microscopy, 278
biomedical imaging, 251
M deep tissue imaging, 271
Magnetic detector choice, 251
asymmetry, 159 dispersion compensation, 254
undulator, 65 fluorophores, 271
Many-body effects, 154 laser scanning, 275
Material working point, 333 lens selection, 259
Maximum emission principle, 84 multifocal systems, 255
Maxwell’s propagation equation, 25 power limited imaging, 271
MCFA. See Most correlated feature analysis pragmatic collection optics, 257–266
(MCFA) pulse chirp/pre-chirping, 254
M-edge, 159, 161 scanning, 251
Merit function, 258 scan optics and scan system, 255–257
Metal-organic chemical vapour deposition spectrally resolved, 278–283
(MOCVD), 89 spectroscopy, 278–280
Micro system architecture, 252–253
explosion, 301, 327
fluidics, 311–312, 341
lens (ultrafast laser driven), 235 N
mechanics, 323, 329, 344, 346 Nano-gratings, 327, 336
optics, 323, 344, 346 Nanoplasmonics, 46
372 Index
Nanoscale thermal transport, 164, 167 effective index, 201

Nonlinear modal effective area (Aeff ), 210
absorption, 290–291 propagation constant (“), 199
coefficient (œ), 83, 179 ray picture, 198
fibre optics, 177–191 scalar wave equation, 199
field ionisation, 299 V-parameter, 207
lengths (LD ) and (LNL ), 180 weak guiding approximation, 199
optical Kerr effect, 88 frequency combs, 129–143
optics, 195 astronomical frequency combs,
polarisation, 27, 28 140–141
pulse propagation, 195 attosecond generation, 129–143
pulse propagation in a laser resonator, basic research, 136–138
82–84 carrier envelope phase stabilisation, 148
refractive index (n2 ), 179, 197 cavity enhanced spectroscopy, 142–143
spectral broadening, 177 comb filtering, 140
spectrogram, 12 cosmic expansion detection, 141
wavelength conversion, 195–221 direct frequency comb spectroscopy,
Nonlinear Schrödinger equation (NLSE), 179 141–142
focussing regime, 181 extra-solar planet detection, 140
generalised, 182 fine structure constant measurement,
simulating soliton solutions, 181 137
Non-perturbative QED, 247 frequency conversions, 135
Nuclear frequency offset, 131
dynamics, 62 f-to-2f self-referencing, 133, 134
resonance fluorescence (NRF), 246 general relativity test/refine, 138
waste transmutation, 240 high harmonic generation (HHG) and
Nucleosynthesis, 246 HeC, 138–139
multi-heterodyne frequency comb
spectroscopy, 142
O noise considertions, 131
OER. See Oxygen enhancement ratio (OER) octave spanning, 132
OPAs. See Optical parametric amplifiers optical clocks, 136
(OPAs) optical standards, 136
Operators in genetic algorithms, 122 RF referencing, 133–135
adaptive operators, 123 Rydberg const. determination, 137
average crossover, 122 self-referencing, 133–135
mutation, 123 stabilization, 143
normal crossover, 122 strong interaction constant
polynomial phase mutation, 124 measurement, 137
Optical frequency metrology, 178, 190, 219
breakdown, 288 penetration depth, 294, 296, 299
carrier wave, 131 rogue waves, 188
fibre trapping/tweezing, 95, 343
couplers, 204 Optical parametric amplifiers (OPAs), 23–41
endlessly single mode optical fibre, 218 amplification with ultrashort pulses,
highly nonlinear fibres, 202 31–33
holey fibre, 204 beam breakup, 30
microstructured fibre, 204 broadband OPA, 35–37
multicore fibre & couplers, 341 broadband phase matching, 36
parametric amplifiers, 23–41 carrier-envelope phase (CEP) stabilization
silica micro/nano wire, 205–206 in an OPA, 37–39
taper, 205 collinear interaction geometry, 35
fibre modes, 198–201 compressor schemes, 37
cladding modes, 201 crystal length, 30
Index 373
degeneracy condition, 24 Paraxial

degenerate configuration, 35 design, 260–261
gain bandwidth, 32 ray tracing, 260
gain influencing factors, 30 Parseval’s theorem, 270
group velocity matched OPA, 33, 35 Permalloy, 159–161
group velocity mismatch (GVM), 28, 31 Perturbation theory, 49, 108, 111
idler generation, 24 PET. See Positron emission tomography (PET)
interaction length, 31 Petawatt laser, 227, 238, 241
large gain limit, 30 Phase
non-collinear OPA, 35, 36 locking, 64, 67, 68
nonlinear coupling coefficients, 28 -space tomography, 7, 8
OPCPA vs. CPA, 40, 41 -transition, 149, 154, 156
optical parametric chirped pulse velocity, 80, 130, 131, 133, 152,
amplification (OPCPA), 39–41 153, 201
parametric conversion, 51 Phonon
parametric gain, 30 mean free path, 164, 166
phase matching bandwidth, 31 transport, 163
phase-matching condition, 28, 30, 32, Photobleaching, 275, 280
35, 40 pathways, 267
pulse splitting length, 31 photokinetic pathways, 267
pump-seed synchronization in OPCPA, 40 rates, 267, 271
seed beam, 33, 36 Photochemistry, 149
signal generation, 24 Photoelectron, 159, 168
signal/idler nonlinear coupled equations, 29 spectrum, 60, 162, 164
theory, 27–30 streaking, 59, 60, 162
ultra-broadband OPAs, 23–41 Photoemission, 159, 161, 169, 170
ultrafast OPA architecture, 33–34 spin-resolved, 154, 158
ultrashort pulsed OPAs, 24 time-resolved, 154, 158
wave-vector mismatch, 27, 28 Photon counting, 260, 284, 287
Optical waveguide architecture basics, 277–278
amplifiers, 342 averaged detection, 274
Bragg-waveguides, 341 histogram, 275, 276
evanescent field power splitters, 341 time-correlated single photon counting
lasers, 342 (TCSPC), 275, 276
modes (see Optical, fibre modes) Photonic
multicore fibre couplers, 341 bandgap, 208
power splitters, 341 beam combiners, 345
Optimal control theory, 113–115 lantern, 345
objective functional, 113 Photonic crystal fibre (PCF), 187, 188, 213
optimal control algorithm, 115 dispersion, 182, 205, 206
principal equation, 114 hollow core, 208
Oxygen enhancement ratio (OER), 236 low air filling fraction, 206–207
Photo nuclear pillar-Romania, 227, 243–247
Photorefraction, 327
P Photosynthesis, 149
PACER technique, 61, 62 Plasma
Parabolic heat equation, 293, 295 free electron, 324, 326, 327, 332, 334,
Parametric 338, 340
down conversion (PDC), 217 frequency, 292, 326
gain bandwidth, 32 mirrors, 65
gain in optical fibres, 214 oscillation, 158, 231, 326
superfluorescence, 33, 37 oscillation period, 158
superfluorescence OPA seed, 33 shielding, 300
374 Index
Polar geometry for electron excitation, 159 orbit model, 53

Polarisation gating, 65 path integrals, 52
Ponderomotive trajectories, 61
energy, 49, 54 Quasi-ballistic heat transport, 166
force, 231, 232, 338 Quiver energy, 60, 228
potential, 150, 231, 232
Positron emission tomography (PET), 238–240
Principal component general projections R
algorithm, 12 RABBITT technique, 56, 57
Programmable logic device, 275 Radiation toxicity, 236
Propagation equation, 25, 178–182 Radio frequency standards, 136, 137
Proton Radon transform, 9
laser production, 227–235 Raman
mono-energetic, 232, 235 amplification, 188
quasi-monoenergetic, 232, 235 based sub-fs sources, 63–64
therapy, 236, 237 effect, 183, 184, 209, 212, 220
transfer, 46 gain, 183, 189, 211
Pulse response function, 183
chirped, 15, 18, 79, 117, 211, 272 scattering, 198, 202, 215, 217
complex temporal amplitude, 77 soliton self-frequency shift, 184
compression in optical fibres, 211–212 stimulated Raman scattering, 63, 184
compressor, 33 Rayleigh range, 56, 198, 338
delivery in optical fibres, 208–212 Relativistic
envelope function, 130 Doppler upshift, 64
power spectrum, 14, 77, 111 equation, 232
shaper, 119 factor, 231
Dazzler, 119, 120 high harmonic generation (RHHG), 64
linear filter, 119 oscillating mirror, 65
nonlinear filter, 119 plasmas, 228
refresh rate, 120 Remote focusing system, 257
shaping mechanisms, 85–87 Response function, 5, 9
unchirped, 79 time-nonstationary filter, 8, 9
Pump-dump control, 109, 110 time-stationary filter, 8
Pump-probe technique, 23, 46, 47, 161, 164 Roundtrip
amplitude gain coefficient (g), 83
amplitude loss coefficient (l), 83
Q Rutherford laboratory, 241
Quantum
bits (Qbits), 217
control schemes, 106–113 S
diffusion, 51, 106 Saddle point method, 53
dot, 7 Salle Jaune laser at LOA, 238
quantum well, 90 Saturable absorber, 77, 86–88
saturation energy, 73, 89 bleaching, 86, 90
semiconductor saturable absorber carbon nanotubes, 76, 98
mirror (see SESAM) fast saturable absorber, 76, 84–86
slow saturable absorber, 76, 84, 85, 88 Kerr-effect nonlinear polarisation rotation,
systems, 90 75
electrodynamics (QED), 137 Kerr-effect self focusing, 75
evolution, 105, 111, 114 Kerr-effect self-phase modulation (SPM),
information, 127, 217 75
interference, 217 organic dye, 75
mechanical tunnelling, 50 Saturable Bragg reflectors (SBRs). See
noise, 136, 189, 197 SESAM
Index 375
Saturation Single shot pulse measurements, 6

energy of the gain, 89 Slowly varying envelope approximation
fluence, 83, 86, 88–90, 93, 98 (SVEA), 26
power, 84, 89 Solar corona, 230
Scalar wave equation, 199 Soliton
Scanning microscopy. See Multiphoton compression, 211
microscopy evolution, 181, 184, 186
Scattering fission, 184–186, 190
media (imaging), 276 high order, 184, 219
Mei, 329 length, 211
Rayleigh, 329 optical, 202, 208, 217
Schrödinger equation, 49, 82, 105, 195, 199, parameters, 210
200, 202, 208, 209 self-frequency shift, 184, 186
Schwartz decomposition, 126 telecommunications transmission, 188
Second trapping process, 184
harmonic generation (SHG), 36, 38, Sonography, 7
251, 333 Space-charge effects, 68, 163, 232
order nonlinear response, 23, 28, 30 Spatial shearing interferometry, 12
-order temporal coherence (g), 268, 269 Spatio-temporal focusing (STF), 251, 252,
Seed electrons, 292, 299 271, 283, 339
Seidel coefficients, 257 Spectral
Self imaging, 278, 282
-amplified spontaneous emission process phase, 2, 4, 7, 9, 13–17, 19, 57–59, 78, 80,
(SASE), 67, 68 111, 112, 123, 124, 180, 268
-amplitude modulation (SAM), 75, 84, 98 shear, 13, 15–17, 19
-focusing, 30, 37, 303, 339 shearing interferometer, 13
-phase modulation (SPM), 2, 30, 38, 58, 82, Spectrograms, 11–12, 116, 117
83, 86, 119, 132, 185, 197, 209, 219 Spectrography, 7, 10, 11, 20
-referencing, 12, 133–135, 142 spectrographic techniques, 9
Sellmeier equation, 179 Spectrometer
SESAM, 87, 89, 92, 95, 97 Fourier transform infrared (FTIR)
anti-resonant, 93, 94 spectrometer, 282
electrical and optical control, 95–97 grating-based spectrometer, 280, 283
fabrication routes, 91 imaging spectrometer, 280
for high power modelocked lasers, 92 scanning spectrometer, 280–282
for high pulse repetition rate modelocked spectral range, 280
lasers, 92–94 SPIDER, 15–19
impulse recovery time (£A ), 87 effect of crystal thickness, 18–19
ion bombarded, 98 effect of test pulse separation, 18
for long wavelength lasers, 189 measurement of complex pulses, 11
material systems, 89–91 optimal design, 16
modulation depth ( R), 87, 88, 90, 93, 94 Spin-orbit splitting, 159
non-saturable loss (RNS ), 87, 88 Split-step Fourier technique, 180, 191
properties, 87–89 SPring 8 Japan, 67
quantum dot, 85, 90, 95 Stellar interferometry, 345
quantum well, 90, 91, 93, 96 STF. See Spatio-temporal focusing (STF)
saturation fluence (Fsat ), 89, 93, 98 Stokes shift, 279
spectral bandwidth ( œ), 87 Streaking measurements, 58–60
structure, 90, 91, 95, 98 Strong
two-photon absorption (TPA) in SESAMs, field approximation (SFA) theory, 52
89 field interactions, 68, 105
typical reflectivity, 87, 88 field limit, 48–50
SFG. See Sum-frequency generation (SFG) Substage condenser, 258, 259
Shape factor, 268, 269 Abbe two-lens condenser, 259
376 Index
Sum-frequency generation (SFG), 38 Tomography, 7, 8, 10, 13, 14, 20, 238

Superconductivity, 154 tomographic techniques, 9
Supercontinuum Total track, 258, 259, 261, 266
anomalous dispersion regime pumping, Transform-limited pulse duration, 10, 11,
184–186 18, 33
evolution, 183–189 Transmutation, 240–242
evolution (femtosecond pump pulses), Trapped atom/ion standards, 136
183–186 Two
evolution (picosecond pump pulses and -frequency correlation function, 13
longer), 186–188 -photon absorption (TPA), 89, 112,
extended wavelength coverage, 219–221 266, 313
generation, 177–192, 195, 202, 217–221 -photon excitation fluorescence (TPEF)
generation via self phase modulation, 219 imaging, 252
noise seeds, 187 -photon excited fluorescence, 267–270
normal dispersion regime pumping, 184, -photon laser scanning microscopy
190 (TPLSM), 266
pump pulse duration regimes, 186 -photon photopolymerization, 311,
shot-to-shot stability, 189, 190 313, 314
simple sources, 218–219 -step photolysis, 271
spectral slicing, 178, 188 -temperature model, 294
stability, 189–190 -time correlation function, 5
telecommunications applications, 183, 188
Superheated liquids, 298
Surface oscillations, 65 U
SVEA. See Slowly varying envelope Ultrafast
approximation (SVEA) coherent magnetization dynamics, 16
demagnetization, 159
laser oscillators, 73–98
T magnetism, 158–161
Tannor-Rice, 106, 109–112, 114, 115 surface dynamics, 162–163
Target normal sheath acceleration (TNSA), x-ray sources, 150, 170
232 x-ray spectroscopy, 46
Telecentric plane, 255–257 Ultrafast laser inscription, 323–346.
Teller, 108 See also Femtosecond laser
Terawatt laser, 234, 238 micromachining
Test-plus-reference, 12 active waveguide devices, 342–343
Thermal diffusivity, 294, 297 applications, 341–345
THG. See Third harmonic generation (THG) astigmatic beam shaping technique, 338
Thin-disk lasers, 92 astrophotonic devices, 345
Third harmonic generation (THG), 197, 251 controlling the ULI process, 331–341
Thomson scattering, 243 energy transfer processes, 325–326
Time experimental setup, 338
-bandwidth product, 77, 78 fabrication capabilities, 327–331
-dependent envelope, 4 focusing optics (role of), 332
-dependent saturable loss coefficient (q(t)), laser wavelength (role of), 332–333
83 longitudinal writing geometry (TWG), 331,
-of-flight detector, 164 332, 337, 338
-resolved electron spectroscopy for microfluidic and bio-photonic devices,
chemical analysis (ESCA ), 170 343–344
-resolved optical spectroscopy, 23 micro-systems, 344
T-MOKE, 159–161 modification regimes, 326–327
TNSA. See Target normal sheath acceleration multiscan technique, 338, 339
(TNSA) non-reciprocal phenomena, 337
Index 377
passive waveguide devices, 341 V

polarisation (role of), 331, 336 Vector wave equation, 199
post-etch annealing, 330, 331 Vibronic laser crystals, 74
pulse duration (role of), 324, 331, Volkov state, 51
337 von Neumann, 108, 117
pulse energy (role of), 334–335 distribution, 117
pulse repetition frequency (role of), 331, VULCAN, 238–241, 243
333, 335, 337
refractive index modification, 327–329,
335, 336 W
selective etching, 329–331, 341, 343, 344 Wakefield acceleration, 232, 245
spatio-temporal focusing, 339 Water window, 69, 150, 154, 170
substrate translation velocity (role of), Wave filtering, 119
331, 335 Waveguide mode. See Optical, fibre modes
thermal accumulation (role of), 333 Wavelength-division multiplexing, 178,
thermal diffusion (role of), 332–334 188, 341
transverse writing geometry (TWG), 331, Wavepacket state, 51
332, 337, 338 Wave-vector mismatch, 27, 28, 32, 35, 56
type I and II index modifications, 329 Wigner, 112
waveguide shaping, 310, 339 chronocyclic representation, 6, 7
writing geometry, 331–332, 335 distribution, 117, 118
Ultrashort pulse function, 6–9, 11, 13, 14
generation dynamics, 77–84 representation, 6, 8
generation fundamentals, 74–84 Windowed Fourier transform, 7, 116
propagation in a laser resonator, 82–84 Work function, 155
Ultrashort pulse characterisation, 1, 10
Frequency resolved optical gating
(FROG)-CRAB algorithm, 9, 60 X
intensity autocorrelation, 10–11 XPM. See Cross phase modulation (XPM)
interferograms, 112–13 X-ray absorption spectroscopy, 168, 170
spectrograms, 11–12 XUV pulse sources, 66
tomograms, 13–14
Ultrashort pulsed laser deposition (PLD),
313, 314 Z
Undulator parameter, 67 Zetawatt laser, 227, 228

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Scottish Graduate Series

For further volumes:

Ultrafast Nonlinear Optics

Prof. Derryck Reid

ISBN 978-3-319-00016-9 ISBN 978-3-319-00017-6 (eBook)

© Springer International Publishing Switzerland 2013

Printed on acid-free paper

Springer is part of Springer Science+Business Media (www.springer.com)

1 1960 Dispersion Relations

29 1985 Laser-Plasma Interactions: 3

Philip H. Bucksbaum Stanford University

International Advisory Committee

The Scottish Universities Summer Schools in Physics (SUSSP) was established in

Including lecturers, guest lec-

Edinburgh, January 2012 Robert R. Thomson

1 Measuring Ultrashort Optical Pulses. . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 1

11 Utilising Ultrafast Lasers for Multiphoton Biomedical Imaging .. . . . . 251

Poster Sessions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . 351

Adam S. Wyatt and Ian A. Walmsley

A.S. Wyatt () • I.A. Walmsley

R. Thomson et al. (eds.), Ultrafast Nonlinear Optics, Scottish 1

function of time or frequency, or at least providing some temporal information such

self-action of intense optical pulses in nonlinear media gives rise to a complicated

1.2 General Considerations

E.t/ D ".t/ C " .t/ (1.1)

E.t/ D jE.t/j exp Œi t .t/ exp.i 0 / exp.i !o t/; (1.3)

Where jE.t/j is referred to as the time-dependent envelope, !0 is the carrier

where TR is the integration time of the detector apparatus.

A particular feature of the Wigner representation is that the marginals of the

Where WS .!; tI ; T / is the Wigner chronocyclic representation of the apparatus

Dispersive line W SQ P .!/ D e i'

Spectrometer W SQ A .!/ D e .!/ = ;

Spectrographic techniques make use of two sequential filters, one time-stationary

1.3 A Catalogue of Methods

1.3.1 Intensity Autocorrelation

The simplest technique for gathering at least moderate quantitative information

The autocorrelation yields directly a measure of the root-mean-square (rms)

Fig. 1.2 Implementation of a

autocorrelation combined with the bandwidth obtained from a measurement of the

Spectrography is based on the sequential action of a time-stationary and time-

Interferometry is a well-known approach to the characterization of optical fields

Fig. 1.3 A spectral shearing

The spectrum of a light source is easy to measure experimentally. Mathematically

Fig. 1.4 Simplified

The derivative of this function with respect to the angle of rotation ’ at ’ D 0

A rotation of the phase space of the pulse requires a combination of a quadratic

1.4 Case Study: SPIDER

Spectral phase interferometry for direct electric-field reconstruction (SPIDER) is a

Fig. 1.5 Conventional SPIDER concept

1.4.1 Optimal Design

1.4.1.1 Spectral Shear

1.4.1.2 Ancilla Chirp Rate

1.4.1.3 Test Pulse Separation (£)

1.4.1.4 Crystal Thickness

k .!0 ; !/ Š .2!0 ˙ !/ n .2!0 ˙ !/ =c .!0 ˙ !/

1.4.1.5 Pulse Complexity

The establishment of general principles of pulse characterization, and the instanti-

6. C. Dorrer, B. de Beauvoir, C. Le Blanc, S. Ranc, J.-P. Rousseau, P. Rousseau, J.-P. Chambaret,

Giulio Cerullo and Daniele Brida

E.t/ D jE.t/j exp Œi t .t/ exp.i 0 / exp.i !o t/; (1.3)

Spectrometer W SQ A .!/ D e .!/ = ;

PL .z; t / D pL .z; t / expŒi .!0 t k0 z/ (2.5)

k 2 .!/ k02 Š 2k0 Œk .!/ k0 (2.13)

where k D kp k0 is the so-called “wave-vector mismatch” between the nonlinear

1 A1 .z; t / exp Œi .!1 t k1 z/ C A2 .z; t / exp Œi .!2 t k2 z/ C

k D k .!N 3 / Œk .!N 1 / C k1 Œk .!N 2 / C k2 D k1 k2 (2.32)