review articleS

Published online: 18 September 2011 | doi: 10.1038/nphoton.2011.167

High-energy attosecond light sources

Giuseppe Sansone1, Luca Poletto2 and Mauro Nisoli1*

The development of attosecond technology is one of the most significant achievements in the field of ultrafast optics over the
past decade. Since the first experimental demonstration of attosecond pulses just ten years ago, novel techniques have been
introduced for the generation, characterization and application of subfemtosecond pulses. The development of attosecond
tools is continuously triggering the introduction of new spectroscopic and measurement methods, which will offer the oppor-
tunity to investigate unexplored research areas with unprecedented time resolution. The wealth of ultrafast processes, which
can be investigated by taking advantage of attosecond temporal resolution, can be greatly extended by the development of
high-intensity attosecond sources. This Review covers a selection of recent advances in the field of attosecond technology, with
particular attention being given to the generation and application of high-energy attosecond pulses.

O
ver the past few decades, the ability to investigate ultra-
fast phenomena at shorter and shorter temporal scales has
determined crucial progress in our understanding of the
fundamental processes in matter. The 1980s saw femtosecond tech-
nology revolutionize the field of time-resolved spectroscopy1, while
the past decade has brought remarkable developments in the field
of attosecond science2–5. Extreme-ultraviolet (XUV) coherent light
pulses with durations of a few tens of attoseconds are ideal tools
for investigating electronic dynamics on the atomic/molecular
scale. Such ultrashort pulses can be produced using high-order har-
monic generation (HHG)6,7, which involves focusing high-intensity
femtosecond pulses onto a gas medium3. Attosecond light bursts,
either in the form of isolated pulses or trains of pulses separated by
half an optical cycle of the driving radiation, have been generated
with conversion efficiencies in the range 10–4–10–8. Although many
important applications of attosecond pulses have already been dem-
onstrated, the widespread adoption of attosecond sources has so far
been limited. This is due not only to the complexity of the laser tools
required to reliably generate attosecond pulses, but also to the low
photon flux characteristics of attosecond sources, particularly for
producing isolated attosecond pulses. Although femtosecond meas-
urement techniques are now standard methods in ultrafast optics,
extending such principles to the attosecond temporal domain is
not straightforward. Novel experimental techniques to initiate and
probe electron dynamics on attosecond timescales are required.
Attosecond pump–probe spectroscopy has so far been demon-
strated only partially and in a very small number of laboratories,
owing to the high intensities required to produce observable two-
XUV-photon processes. The development of experimental methods
for generating high-energy attosecond pulses could pave the way for
crucial progress in the field of attosecond science.
This Review reports on recent advances in the field of attosecond
technology for the generation of high-energy attosecond pulses.
Although the generation of microjoule-energy trains of attosecond
pulses has been reported by various research groups, with impor-
tant applications to attosecond metrology based on nonlinear XUV
effects, the production, characterization and application of high-
energy isolated attosecond pulses is still under active investigation.
This Review analyses various techniques for the generation of high-
intensity attosecond pulses, both from gases and laser-produced
plasmas, with particular emphasis on isolated attosecond pulses.
Perspective is given on the status and prospects of the applications
of high-energy attosecond pulses in research fields such as nonlin-
ear attosecond metrology, electron correlation phenomena and the
measurement of ultrafast dynamics in atoms and molecules.
High-energy attosecond pulses from gas harmonics
Various schemes have been proposed and experimentally inves-
tigated for enhancing the conversion efficiency of the harmonic
generation process, based on the use of high-energy, femtosecond
driving pulses focused in hollow-core fibres8,9 or cells10–13. A very
powerful method for generating microjoule-energy XUV pulses
is to use the loose-focusing geometry, in which a driving beam
is focused in a long gas cell using long-focal-length optics14–16.
Favourable phase-matching conditions can be achieved in this
configuration by using the positive dispersion of the neutral gas
medium at low pressure to compensate for the Gouy geomet-
ric shift, which is equivalent to providing a negative dispersion.
Driving intensities below the saturation intensity of the medium
are generally required to reduce the negative dispersion induced
by the free-electron population. In a typical experimental set-up,
high-energy laser pulses are focused into a gas cell whose length,
L, is a few centimetres. Long focal lengths (1–5  m) are used to
increase the excitation spot size and, consequently, the Rayleigh
range. Driving pulse energy, beam spot size and gas pressure can be
adjusted to maximize the harmonic conversion yield. XUV radia-
tion reaching energies of 11.5 μJ at wavelengths of between 73.6 nm
and 42.6 nm (corresponding to harmonics between the 11th and
19th orders, respectively) has been generated in a 14-cm-long cell
filled with xenon at a pressure of 0.6 torr, by focusing 35 fs, 14 mJ
driving pulses onto the gas cell using a lens with a focal length
of 5 m (ref. 17). The loose-focusing geometry can also be used to
generate a low-divergence XUV beam, whose beam divergence is
proportional to L–1/2 (ref.  16). The temporal characteristics of an
attosecond pulse train generated using this technique have been
measured by second-order interferometric autocorrelation16,18,19.
Optimization of the harmonic conversion efficiency can be also
achieved by employing quasi-phase-matching techniques, which
prevent back-conversion of the harmonic generation process by
applying a periodical correction to the phase mismatch after every

1
Department of Physics, Politecnico di Milano, National Research Council of Italy, Institute of Photonics and Nanotechnologies, Piazza L. da Vinci 32,
20133 Milano, Italy. 2National Research Council of Italy, Institute of Photonics and Nanotechnologies, Via Trasea 7, 35131 Padova, Italy.
*email: mauro.nisoli@fisi.polimi.it

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© 2011 Macmillan Publishers Limited. All rights reserved.
review articleS
a d
BS1
λ/4 BK7
Quartz plate BS2
b and the ground-state population depletion on the leading edge of
λ/2
BBO BS3
e
c Filament
Vacuum
XUV
Brewster
window Noble gas
Figure 1 | Isolated attosecond pulses from gases. Various approaches for
the generation of isolated attosecond pulses have been experimentally
demonstrated. a, Polarization gating. b, Double optical gating.
c, Generalized double optical gating. d, Interferometric polarization gating.
e, XUV generation from a laser filamentation in noble gases. BBO, β-barium
borate; BS, beamsplitter.
coherence length. A recent review by Popmintchev et al. compre-
hensively covers quasi-phase-matching methods in the harmonic
generation process20. A different quasi-phase-matching approach
— one that demonstrates the potential to enhance the photon flux
in the soft-X-ray spectral region — is based on the use of a multi-
gas-cell target21. This technique could be particularly useful for the
loose-focusing geometry because of the long confocal parameter of
the excitation beam, thus allowing the separation between consecu-
tive cells to be optimized.
High-energy isolated attosecond pulses can be produced from
gas harmonics in a variety of ways. This section discusses three
classes of generation techniques that are based on the use of suit-
able temporal gating schemes. The technique of spectrally filtering
the cut-off harmonics (known as amplitude gating) has been already
analysed in various reviews3,4; pulses as short as 80 as have been pro-
duced in neon (at a central photon energy of 80 eV) with a maxi-
mum on-target energy of 0.57 pJ (ref. 22). The main limiting factor
of this technique is the requirement of very short and energetic driv-
ing pulses, with durations below 5 fs, and a controlled electric field.
Polarization gating. Modulating the polarization state of the driv-
ing field is a powerful method for confining the XUV generation
process to a single event23. This technique is based on the strong
dependence of the harmonic-generation process on the ellipticity
of the driving pulses, and therefore exploits an excitation field that
is elliptically polarized on the pulse’s leading and trailing edges but
is almost linearly polarized in a short temporal window around
the pulse peak24. A good estimation for the duration of driving
pulse required to generate efficiently isolated attosecond pulses is
τ < 2.5 T0 (where T0 is the optical cycle of the driving field; ref. 25),
which is around 6.6 fs in the case of 800 nm excitation. The overall
conversion efficiency from the laser source to XUV light output
decreases as the laser pulse duration increases. In 2006, research-
ers generated isolated attosecond pulses using carrier–envelope
phase (CEP)-stabilized 5  fs, 0.2  mJ driving pulses (Fig.  1a)26,27.
Pulses as short as 130 as have been produced in argon, in the spec-
tral range of 25–50 eV, with energies of around 70 pJ. Table 1 lists
the relevant parameters of current attosecond sources. Adding a
second-harmonic field to the fundamental frequency can alleviate
the requirements on driving pulse duration. For particular values
of the relative phase between the two laser field components, and
when the amplitude of the second-harmonic field is high enough,
the symmetry of the driving electric field breaks and the genera-
tion of attosecond pulses takes place for every optical cycle of the
656 nature photonics | VOL 5 | NOVEMBER 2011 | www.nature.com/naturephotonics
© 2011 Macmillan Publishers Limited. All rights reserved.
Nature photonics doi: 10.1038/nphoton.2011.167
fundamental radiation28 (Fig. 2). Using such a two-colour scheme
(known as double optical gating; DOG)29, the width of the lin-
ear polarization gate can be close to one optical cycle of the fun-
damental radiation, as shown in Fig. 2. This has two advantages:
longer driving pulses with durations of up to ~12 fs can be used,
the driving pulses can be reduced30. Mashiko et al. reported that
using the DOG technique provides high XUV photon fluxes31
(Fig. 1b). The researchers measured continuous XUV spectra with
a maximum XUV pulse energy from argon of ~6.5  nJ (immedi-
ately after the generating medium) at a conversion efficiency of
6  × 10–6 (ref. 31). The on-target pulse energy was estimated to be
of the order of 1 nJ, after taking into account the transmission of
the aluminium filter used to block the fundamental radiation and
reflections from focusing optics.
The extension of temporal gating techniques to high-energy driv-
ing pulses with durations of a few tens of femtoseconds and peak
powers up to the petawatt level is currently a very active research
field. One of the main limiting factors is related to the depletion of
the neutral-atom population on the leading edge of the driving field.
The generalized DOG technique (Fig.  1c) is able to generate iso-
lated sub-150-as pulses from a sub-30-fs amplifier32. The idea of this
technique is to reduce the depletion of the neutral-atom population
by decreasing the ellipticity of the driving field, which is achieved
by adding a fused silica Brewster window to the DOG set-up33. In
2007, Tzallas et al. proposed and implemented a polarization gating
scheme known as interferometric polarization gating (Fig. 1d)34,35,
in which an ellipticity-modulated pulse is produced from four indi-
vidually controlled, linearly polarized pulses of variable field ampli-
tude, relative polarization and delay. This method has been used
to generate a coherent continuum of radiation by loosely focusing
55 fs driving pulses with a peak power of 2 TW into a pulsed gas
jet. Particularly interesting is the high photon flux of the radia-
tion, whose spectral bandwidth supports isolated pulses with dura-
tions down to ~260  as. In subsequent experiments, the energy of
the continuum was found to be around 20 nJ at photon energies of
30–70 eV, with an energy of ~10 nJ in the cut-off region36.
a
ω T0 /2
b
T0
ω + 2ω
Figure 2 | Temporal gating. a,b, A multicycle driving field (blue curves)
generates a train of attosecond pulses, separated by either half an optical
cycle, T0/2, in the case of single-colour excitation (a), or a full optical
cycle, T0, in the case of a two-colour excitation (b). Isolated attosecond
pulses can be generated using a temporal gate, which confines the XUV
generation process to a short window whose temporal extensions depends
on the separation between consecutive attosecond pulses.
Nature photonics doi: 10.1038/nphoton.2011.167 review articleS
a b
Ionization rate Ionization rate

Path 1 Ψ=0 Path 1 Ψ = π/2

Time (cycles) Time (cycles)

Path 2 Path 2

c d

Total emission rate

1 Total emission rate
1
Emission rate (a.u.)

0.8

Emission rate (a.u.)

0.8
0.6
0.6
0.4
0.4
0.2
0.2
0
20 0
20
Pho 25
ton 30 Pho 25
ene Path 2 ton 30
rgy 35 ene Path 2
(eV 40 rgy 35
) Path 1 (eV 40
) Path 1

Figure 3 | Ionization gating: electron quantum path analysis. a,b, Ionization rate (green curves) calculated in xenon for the case of 5 fs driving pulses
(red curves), with a peak intensity of 2.5 × 1015 W cm–2, for two CEP values. The first two electron quantum paths are shown by dotted blue lines. c,d, XUV
emission rates associated with the first three electron quantum paths (black curves) and total XUV emission rate produced by coherent superposition of
all electron quantum paths (red curves) for two CEP values, calculated by using non-adiabatic saddle-point simulations.

Two-colour gating. Recent advances in the realization of high-
energy optical parametric amplifiers in the near-infrared spectral
region have allowed the investigation of HHG using long-wave-
length femtosecond pulses. The maximum photon energy obtain-
able through HHG in gases scales as Iλ2, where I and λ are the peak
intensity and central wavelength of the driving pulse, respectively.
The harmonic cut-off can therefore be significantly extended by
increasing λ, at the expense of a reduced single-atom harmonic
yield, which scales as λ–6 (refs 37–39). Parametric sources, which are
tunable in the near-infrared, have been developed to extend XUV
emission up to kilo-electronvolt energies40,41. In 2007, Merdji and
co-workers proposed a method for generating isolated attosecond
pulses by combining the fundamental field ω with its detuned sec-
ond harmonic at 2ω + δω (ref. 42).
In 2009, researchers reported an efficient XUV generation tech-
nique that combines an intense near-infrared pulse (λ = 1.45 μm,
I  =  2  ×  1014  W  cm–2) with an intense detuned second-harmonic
pulse (λ = 0.8 μm, I = 8.5 × 1014 W cm–2) comprising only a few opti-
cal cycles43. This method was used to generate coherent continuous
emission at energies of up to 160 eV in argon and 200 eV in neon.
Importantly, the researchers observed that the harmonic conversion
efficiency for two-colour excitation was much larger than of a sin-
gle-colour near-infrared field. This suggests that the intense 0.8 μm
component of the driving field was responsible for the increase in
conversion efficiency, thereby overcoming the major drawback of
using longer driving wavelengths. To relax the requirements on
driving pulse duration, Takahashi and co-workers recently dem-
onstrated the generation of continuous XUV radiation around the
cut-off spectral region by mixing 30  fs, 0.8  μm pulses with 40  fs,
1.3 μm pulses44,45. Continuous XUV spectra can be generated, even
without CEP control, when the two-colour field synthesis is prop-
erly optimized in terms of central wavelength of the near-infrared
component and intensity ratio between the two colours. Moreover,
the two-colour scheme offers the major advantage of being able to
significantly reduce the ionization of the gas medium, thus allow-
ing the use of efficient phase-matching techniques for the genera-
tion of intense attosecond pulses from a neutral gas12. By using the
loose-focusing geometry, it is reasonable to expect the generation
of microjoule-energy isolated attosecond pulses with conversion
efficiencies of the order of 10–5. Such a scheme could therefore lead
to new ways of generating isolated attosecond pulses for use in ter-
awatt-class laser systems.
Ionization gating. An alternative approach for the generation of
high-energy isolated attosecond pulses is based on the use of driving
pulses with above-saturation intensity. Complete depletion of the
neutral-atom population on the leading edge of the driving pulses
confines the harmonic-generation process. To generate isolated
attosecond pulses, the atoms of the generating gas must be exposed
to a large non-adiabatic increase in the electric field of the leading
edge; such a condition can be easily achieved using intense, few-
optical-cycle pulses with controlled electric field. This process has
been discussed in theoretical works by Cao et al.46 and Kim et al.47,
which both describe the generation of isolated attosecond pulses by
spectral selection of the high-frequency components in the XUV
spectrum. From an experimental point of view, the influence of ion-
ization dynamics on the generation of isolated attosecond pulses has
been investigated for 8 fs (ref. 48) and 15 fs (ref. 49) driving pulses.
In both cases, the enhancement of the confinement effect of the cut-
off harmonics of the XUV spectrum to a single pulse was explained

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© 2011 Macmillan Publishers Limited. All rights reserved.
review articleS
a b c pulses is explained by considering the spatiotemporal dynamics of
3TL
Time
λ/5 λ/5 λ/5
Normal space coordinates
Figure 4 | Isolated attosecond pulses by harmonic generation from a
solid surface. a–c, Motion of the plasma surface induced by excitation
pulses with linear (a), circular (b) and time-dependent polarization (the
corresponding electric field, characterized by a short temporal window
of linear polarization, is also shown) (c). Attosecond pulses, generated in
the case of linear and time-dependent polarization, are shown in yellow.
By properly filtering the reflected radiation, a single attosecond pulse can
be isolated. λ and TL are driving laser wavelength and period, respectively.
Figure reproduced with permission from ref. 67, © 2008 IOP.
by the very rapid loss of phase-matching occurring on the leading
edge of the excitation pulses.
More recently, researchers generated sub-160-as isolated pulses by
exposing the sub-cycle ionization dynamics of a gas medium to high-
intensity, 5 fs pulses with controlled electric field50. The experiment
achieved an on-target energy of 2.1 nJ for xenon and 1.4 nJ for argon,
with an overall conversion efficiency of around 5 × 10–6 (ref. 50). The
physical processes of the ionization gating scheme can be under-
stood through a single-atom approach based on the non-adiabatic
saddle-point model51,52. In such a model, the Fourier transform of
the atomic dipole moment responsible for harmonic generation can
be written as a coherent superposition of the contributions from the
different electron quantum paths. Figure 3c,d shows emission rates
associated with the electron trajectories displayed in Fig. 3a,b for two
CEP values. Depending on the temporal evolution of the ionization
rate (shown in Fig.  3a,b), either one or two quantum trajectories
effectively contribute to the total emission rate, giving rise to either
one or two attosecond pulses, respectively. By using a non-adiabatic
three-dimensional numerical propagation model53, we investigated
the possibility of using the loose-focusing geometry to increase the
photon flux of attosecond pulses. In particular, we calculated how
attosecond pulses in a xenon gas cell evolve when the energy of the
5 fs driving pulses is increased while maintaining a constant excita-
tion intensity of 2.5  × 1015 W cm–2. Simulations show that the XUV
pulse energy could be increased up to the microjoule level while still
preserving the excellent spatial characteristics of the XUV beam.
Another promising technique for generating high-photon-flux
isolated attosecond pulses is based on the production of XUV radia-
tion from laser filamentation in noble gases (Fig. 1e). This process
has been investigated extensively by Gaarde and co-workers54,55.
From an experimental point of view, continuous XUV spectra sup-
porting isolated attosecond pulses have been recently obtained from
35  fs infrared pulses undergoing filamentation in a semi-infinite
argon gas cell56,57. In this case, the production of isolated attosecond
658 nature photonics | VOL 5 | NOVEMBER 2011 | www.nature.com/naturephotonics
© 2011 Macmillan Publishers Limited. All rights reserved.
Nature photonics doi: 10.1038/nphoton.2011.167
the driving field during the filamentation process. In particular, as
pointed out in ref. 55, filamentation gives rise to the formation of
high-intensity driving spikes with single-optical-cycle duration,
which are responsible for the generation of isolated attosecond
pulses.
High-energy attosecond pulses from laser-produced plasmas
The loose-focusing approach becomes experimentally unfeasible for
gaseous media if the energy of the excitation pulses is increased to a
few hundred millijoules. Harmonic generation from solid targets has
been suggested as an alternative technique for delivering high-energy
attosecond pulses up to the X-ray energy range. In this scheme, the
electric field of a high-intensity infrared pulse (I > 1016 W cm–2) ion-
izes the surface of a solid target to create an overdense plasma at the
boundary between the vacuum and the solid. The generation of XUV
radiation from such a laser-produced plasma has been analysed in
a recent review by Thaury and Quéré58. The interaction of the laser
with the plasma is governed by the normalized vector potential
a0 = eE/ωLmc, where E and ωL are the electric field and frequency of
the driving pulse, respectively, c is the velocity of light in vacuum,
and e and m are the electron charge and mass, respectively. Efficient
harmonic generation can be achieved for values of a0 close to or larger
than unity. Two generating mechanisms that can lead to HHG from
solid targets have so far been investigated: coherent wake emission59,
which dominates when a0 ≤ 1, and the relativistic oscillating mirror
mechanism60, which dominates when a0 >> 1. Both cases cause the
generation of odd and even harmonics of the fundamental radiation.
In contrast, HHG in gases using one-colour, multiple-optical-cycle
excitation leads to only odd-order harmonics. The coherent wake
emission process has analogies with harmonic generation in gases.
At each maximum of the electric field, electrons in the plasma cre-
ated by the excitation pulse are ejected into the vacuum and then
driven back towards the plasma surface. This gives rise to ultrafast
electron bunches that recollide with the plasma, where they trigger
high-frequency collective electron oscillations in their wake and thus
cause the emission of attosecond pulses. The maximum frequency
of the generated XUV spectrum is given by the maximum plasma
frequency of the laser-induced plasma, which typically corresponds
to harmonics between the 15th and 30th order of an 800 nm driv-
ing field. In 2009, Nomura  et  al. experimentally demonstrated that
the XUV radiation produced by coherent wake emission consists of a
train of attosecond pulses by measuring the corresponding autocor-
relation trace61. They estimated the XUV intensity in the interaction
region to be approximately (0.5–1) × 1011 W cm–2.
When a0 >> 1, the influence of the magnetic field on the electron
motion cannot be neglected. Owing to the magnetic component of
the Lorentz force ev × B (where v is the electron velocity and B is the
magnetic field of the excitation pulse) and also to the restoring force
provided by the ions, the electrons move in an oscillatory motion
around their equilibrium position with a velocity perpendicular to
the surface given by v⊥  ∝ a02(t)[1  +  sin(2ωLt)]. The incident laser
radiation is reflected by the oscillating electron layer, which acts as
a plasma mirror; because of the relativistic Doppler effect, the spec-
trum of the reflected radiation can extend up to the X-ray region,
depending on the value of a0 (ref. 62). Baeva et al. have shown that a
more correct description of the harmonic-generation process from
solid surfaces considers the velocity of the electrons to be almost
always close to c (refs  63,64). In this ultrarelativistic regime, the
gamma factor of the plasma surface can be approximated as:
p⊥2
γs = 1 +
p||2
where p|| and p⊥ are the components of the electron momentum (p)
parallel and perpendicular to the surface, respectively. The factor γS
Nature photonics doi: 10.1038/nphoton.2011.167 review articleS
a b
35 3 c
10
i
8 2pσu 2.5
30 νf

Potential energy (eV)

6
Kinetic energy (eV)

Intensity (a.u.)
4 25 d
iii
ii 1.5 ii
iii 3νf
2 20 i ×100
ii 5th 3rd 1st D + D+ 1
1 1sσg e 5νf
15 iii
i 5 11th D+D 0.5
6νf
0 ×5
0 0
−2 −1 0 1 2 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 0 2 4 6 8 10
Optical cycle Internuclear distance (Å) Harmonic order

Figure 5 | Attosecond nonlinear Fourier transform spectroscopy. a, Kinetic energy distribution of D+ ions as a function of the delay between a pair
of harmonic fields. The horizontal axis was scaled by the optical cycle of the fundamental radiation. b, Potential energy curves of D2. The one-photon
absorption of the 11th harmonic generates D2+ in the 1sσg state; the fifth, third and first harmonics excite D2+ ions to the 2pσu state, resulting in the
dissociation of D2+ into D+ and D. c, Fourier transform intensities of the kinetic energy temporal evolution of D+ ions as a function of the harmonic order for
the energy intervals (i), (ii) and (iii). Figure reproduced with permission from ref. 76, © 2010 APS.

is always of the order of unity, except for cases when the momentum
of the plasma mirror is perpendicular to the surface (p||(t–) = 0),
which leads to sharp features in the time evolution of γS. These
spikes are responsible for the rich harmonic content in the reflected
radiation. Using the ‘γS spikes’ model, it is possible to demonstrate
that the harmonic scaling law is given by I(ω) ∝ ω–8/3 up to the max-
imum frequency ωmax = (√8)γmax3ωL, which was experimentally con-
firmed by Dromey et al.65. The spectral brightness of the harmonic
radiation was in the range of 1022–1024 photons  s–1  mm–2  mrad–2
(0.1% bandwidth) for 4 nm and 17 nm, respectively, with estimated
energies of 0.07–0.7 mJ and 0.2–20 mJ, respectively. Harmonic gen-
eration of up to 3.8  keV from a CH target was reported in 2007,
with harmonic energies of ~17 μJ at 1.4 keV and ~5 μJ at 3.1 keV in
1% bandwidth66.
In analogy with harmonic generation in gases, surface plasma
harmonics driven by multicycle linearly polarized pulses are emit-
ted in trains of attosecond pulses. Isolated pulses can be attained
by employing the polarization gating technique. In this case, the
conversion efficiency diminishes when the ellipticity of the driv-
ing pulse is increased, which can be understood by considering
the motion of the oscillating mirror67. For linear polarization, this
motion corresponds to a periodic oscillation every half-cycle of
the fundamental radiation, thus providing a train of attosecond
pulses (Fig.  4a). For a circularly polarized incident pulse, the
plasma mirror does not present strong oscillations but instead
varies on the timescale of the laser envelope, according to the rela-
tion v⊥ ∝ a02(t). The envelope of the pulse determines a ‘smooth’
force on the electron plasma (Fig. 4b) and thus no harmonics are
generated. The generation of isolated pulses (Fig.  4c) is possible
using few-cycle pulses with a time-dependent polarization simi-
lar to the one described above. One-dimensional particle-in-cell
simulations have shown that the dependence of the harmonic
generation efficiency on the ellipticity is in turn dependent on
the parameter a0; the higher the normalized vector potential, the
more sensitive the harmonics are to small deviations in ellipticity
from the linear case.
It is worth mentioning that the efficient generation of attosec-
ond pulses has been predicted when high-energy, few-optical-cycle
laser pulses are focused onto a solid target at a spot size compara-
ble to the laser wavelength (λ). This achieves intensities of more
than 1018 W cm–2 and contains the laser energy within a focal vol-
ume of ~λ3 (the λ3 regime). Particle-in-cell simulations show that,
in the λ3 regime, the radiation reflected by the overdense plasma is
composed of a train of attosecond pulses, with each pulse deflected
to a specific angle68. As pointed out by Naumova et al., this efficient
XUV generation process is produced by the deformation of the
plasma profile, which results in large changes in the local incidence
angle (the angle between the original wavefront and the deformed
reflecting surface) on a sub-cycle temporal scale. Moreover, in the
relativistic λ3 regime, the intense and coherent relativistic electron
motion in the direction parallel to the wave vector of the reflected
wave can give rise to dramatic compression of the reflected pulses,
which allows reflection, deflection and compression to act together
to generate isolated attosecond pulses. Particle-in-cell simulations
suggest that this technique could be used to produce isolated
pulses with durations as low as 200 as and conversion efficiencies
of up to 10%.
Recent progress in laser technology — in particular the devel-
opment of laser systems based on optical parametric chirped-pulse
amplification69 — has opened the way to the generation of multi-
terawatt few-cycle light pulses70, which have potentially crucial
applications in the field of attosecond science. On the basis of recent
results, the development of laser systems with powers reaching sev-
eral tens of terawatts and repetition rates in the kilohertz regime
are within our reach. Such laser systems will be ideal drivers for the
efficient generation of attosecond pulses in the kilo-electronvolt
spectral range from laser-produced plasmas.
Applications of high-energy attosecond pulses
The generation of high-energy attosecond pulses poses a number
of constraints in the optical design of XUV facilities. One problem
is that the high-energy driving beam must be removed after XUV
generation to avoid damage to the optics and the sample under
investigation. The second important issue is using a design of XUV
focusing optics that achieves a high on-target beam intensity. In this
section we will concentrate on a few applications of high-intensity
attosecond pulses, including both theoretical proposals and partial
experimental implementations.
Attosecond XUV nonlinear processes. The production of high-
intensity isolated attosecond pulses is crucial for the investigation
of nonlinear processes in the XUV spectral region, particularly for
the development of attosecond metrology by XUV nonlinear opti-
cal methods. Watanabe and co-workers used two-photon above-
threshold ionization to demonstrate the first autocorrelation and
frequency-resolved optical gating measurement of isolated ~0.9 fs
pulses by using a scandium/silicon multilayer mirror to select
the ninth harmonic (28  eV) of the incident light71,72. In 1998, the
researchers used two-photon nonlinear absorption in helium to
measure the first autocorrelation trace of the ninth harmonic of a

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© 2011 Macmillan Publishers Limited. All rights reserved.
review articleS
r1
t = 0 fs
ω = 23.7 eV
r2
r1
t = 1.5 fs
r2
r1
t = 5.6 fs
ω = 90 eV r2
Figure 6 | Attosecond pump–probe experiment for investigating electron
motion inside an atom. The first pump XUV pulse (central energy of
23.7 eV) excites the ground state to the superposition 1s + 1snp. The radial
distributions in the (r1, r2) plane are shown before (t = 0 fs) and after
(t = 1.5 fs) the pump pulse. The wave packet evolves in time on a timescale
of a few femtoseconds, thus determining a ‘breathing mode’ of the radial
density of the two electrons. This motion can be imaged by doubly ionizing
the system using an intense attosecond pulse centred at 90 eV. After the
probe pulse, the radial density distribution shows that the electrons are at
large radial distances of r1 and r2, which corresponds to double ionization.
Figure reproduced with permission from ref. 79, © 2006 APS.
Ti:sapphire laser (ref.  73). The same nonlinear process was used
in 2003 to achieve the first autocorrelation trace of a train of atto-
second pulses produced by phase-locked harmonics from the sev-
enth to the 15th order74. In this case, the estimated XUV intensity
was 1011 W cm–2. The ion yield measured as a function of the delay
between two XUV pulse replicas showed a clear attosecond struc-
ture characteristic of a train of attosecond pulses with an average
duration of 780 as.
The Coulomb explosion of diatomic molecules has been used to
measure the interferometric autocorrelation trace of a train of atto-
second pulses16,18,19. In particular, two-photon absorption in N2 was
achieved by using an XUV field composed of harmonics ranging
from the ninth to the 19th order. Diatomic molecules were chosen
instead of single atoms of similar ionization potential because dia-
tomic molecules exhibit a larger cross-section for XUV two-photon
absorption. The loose-focusing geometry was used to generate the
attosecond pulse train, and the estimated intensity of the 11th-order
harmonic field at the focal point was 3  ×  1014  W  cm–2. The pulse
train was divided into two XUV pulse replica at a beamsplitter and
the N+ ion yield was subsequently integrated as a function of the
delay between the two. The resulting yield exhibited bunches with
an average duration of 320  as and a periodicity twice that of the
driving field, corresponding to the interferometric autocorrelation
trace of the train of attosecond pulses.
660 nature photonics | VOL 5 | NOVEMBER 2011 | www.nature.com/naturephotonics
© 2011 Macmillan Publishers Limited. All rights reserved.
Nature photonics doi: 10.1038/nphoton.2011.167
Such an interferometric technique forms the basis of the recently
developed attosecond nonlinear Fourier transform spectroscopy
technique — a very powerful method for characterizing coupled
electronic–nuclear dynamics in molecules. The first experiments to
use this technique were performed in CO2 (ref. 75) and D2 (ref. 76).
In general, the interferometric trace of the attosecond pulse train
as a function of the delay between two pulse replicas, I(τ), can be
written as:
I(τ) = ∑I
p, q
(τ)
p, q
where the single terms Ip,q can be expressed as:
∫ 2
Ip,q(τ) = σp,q [E2p+1(t − τ) + E2p+1(t)][E2q+1(t − τ) + E2q+1(t)] dt
∫
= σp,q [Fb + FIC(τ) + Fp(τ) + Fq(τ) + Fp−q(τ) + Fp+q(τ)] dt (1)
The term σp,q represents the cross-section for the absorption of
one photon of the 2q + 1 harmonic and one photon of the 2p + 1
harmonic. The term Fb represents a constant background given by
the two-photon signal associated with the two pulses separately, and
does not depend on the relative delay τ. The term FIC(τ) gives the
intensity autocorrelation of the electric field; the terms Fp(τ), Fq(τ),
Fp−q(τ) and Fp+q(τ) are functions oscillating at 2p + 1, 2q + 1, 2(p − q)
and 2(p + q + 1) times the fundamental frequency νf, respectively.
Fourier analysis of the measured signal allows the different Fourier
components to be isolated and provides physical insight into the
nonlinear photoabsorption process (that is, the order of the har-
monic fields involved in the photoabsorption process).
Nonlinear Fourier transform spectroscopy has been used to
retrieve information about the photodissociation of D2 molecules
by irradiating D2 molecules with an attosecond pulse train con-
taining harmonics from the first to the 19th order76. The D+ signal,
shown in Fig. 5a as a function of τ, exhibits periodic modulations
with different periods in three kinetic energy regions, (i), (ii) and
(iii), shown in Fig. 5a,b. Analysis of the oscillation frequencies indi-
cates that the generation of D+ ions proceeds through the absorp-
tion of one photon (mainly from the 11th-order harmonic field),
which ionizes the neutral molecules and projects the nuclear wave
packet onto the ground ionic state 1sσg, followed by the absorption
of a second photon from the fifth, third and fundamental harmonic
fields, which excite the ion to the dissociative state 2pσu (Fig. 5b).
For higher harmonic orders, the excitation takes place at shorter
internuclear distances and the ion acquires a larger kinetic energy
on the dissociating curve, as shown in Fig. 5b. The contributions of
the different harmonic orders to the energy ranges (i), (ii) and (iii)
can be easily recognized in the Fourier transform of the temporal
evolution of the ion kinetic energy (Fig. 5c–e). Indeed, the ion sig-
nals associated with the first (i), third (ii) and fifth (iii) harmonics
present a clear oscillation at frequencies of νf, 3νf and 5νf, respec-
tively, corresponding to the term Fp (or Fq) of equation (1). The dif-
ference term Fp−q, which corresponds to components at 10νf, 8νf
and 6νf, is also weakly visible in the Fourier transform of the signals
in Fig. 5c–e. The sum term Fp+q cannot be observed owing to the
experiment’s insufficient delay resolution. Nonlinear Fourier trans-
form spectroscopy is a particularly powerful technique because
only the nonlinear interactions, which are generally rather weak,
are characterized by interference fringes that can be evidenced by
Fourier analysis of the experimental traces.
XUV-pump/XUV-probe measurements. Recently, Skantzakis
and co-workers demonstrated the first XUV-pump/XUV-probe
Nature photonics doi: 10.1038/nphoton.2011.167 review articleS
Table 1 | Relevant parameters of current attosecond sources based on HHG in gases.
Method Gas ħω (eV) τ (as) E Type Efficiency Reference
AG Neon 80 80 0.5 nJ IAP 1.7 × 10–6 22
PG Argon 35 130 70 pJ IAP 3.5 × 10–7 26,27
PG Neon 60 — 1 pJ IAP 5 × 10–9 26
DOG Argon 38 — 6.5 nJ IAP 6 × 10–6 31
DOG Neon 45 107 170 pJ IAP 1.5 × 10–7 31,85
IG Xenon 27 155 9 nJ IAP 2.6 × 10–5 50
IPG Xenon 50 <1,000 20 nJ IAP 2 × 10–5 36
LF Xenon 20 320 10 μJ APT 7 × 10–4 16
ħω is the central energy of the XUV spectrum, τ is the measured pulse duration and E is the pulse energy at the source (in the case of isolated pulses, E corresponds to the XUV energy in the spectral region
characterized by a continuous profile). The efficiency is defined as the ratio between the XUV pulse energy and the driving laser pulse energy. AG, amplitude gating; PG, polarization gating; DOG, double-optical
gating; IG, ionization gating; IPG, interferometric polarization gating; LF, loose-focusing; IAP, isolated attosecond pulses; and APT, attosecond pulse trains.

measurements of atomic coherence dynamics with a temporal
resolution of 1 fs (ref. 77). The XUV radiation, produced using the
interferometric polarization gating technique and characterized
by a broadband continuum in the range of 15–25 eV, was focused
by a split spherical mirror into a xenon pulsed gas jet, which gener-
ated two pulse replicas. The XUV pump pulse used single-photon
absorption to excite an electronic wave packet that was generated
by the coherent manifold of doubly excited states and inner-shell
excited auto-ionizing states of xenon. The atomic dipole induced
by the time-delayed XUV probe presented a phase-shift that was
determined by the temporal delay τ between the pump and probe
pulses. One would therefore expect to observe Ramsey fringes
resulting from quantum interference in the auto-ionization signal,
which gives information about the energy separation and lifetimes
of nearby states78. Indeed, the Fourier transform of the measured
auto-ionizing signal as a function of τ reproduced the spectrum
of the series of excited states. It is worth pointing out that in this
experiment, the ionization was not a two-XUV-photon process77.
The use of attosecond-pump attosecond-probe schemes for
investigating the dynamics of electron wave packets has been sug-
gested in several theoretical studies. Hu and Collins79 analysed
the possibility of exciting a coherent wave packet consisting of
a superposition of 1snp states (where n = 2, 3, 4...) in helium by
using an XUV pulse with a peak intensity of 6  × 1014 W cm–2, a
duration of 1.5 fs and a central photon energy of 23.7 eV. After the
excitation pulse, the radial distribution of the electron wave packet
temporally oscillates in a ‘breathing’ motion. The periodic oscilla-
tion of the radial distribution can be imaged by doubly ionizing
the atom using an intense 90 eV attosecond pulse. The evolution
of the electron wave packet during application of the pump–probe
can be described by the radial distribution P(r1, r2) of the two elec-
trons in the (r1, r2) plane, given by:
∫∫Φ(r , r ) dΩ dΩ
2
P(r1, r2) =
1 2 1 2
where Φ(r1,  r2) is the two-electron wavefunction and the inte-
gration is performed over the solid angles Ω1 and Ω2. Before the
arrival of the pump pulse at t = 0 fs, the two electrons are in the
ground state 1s2 (Fig. 6a). Just after the pump pulse at t = 1.5 fs, one
electron is close to the nucleus while the other has a spread in the
radial distribution (Fig.  6b), which is indicative of a single-elec-
tron excitation process. At a later time (t = 5.1 fs), a probe pulse
with a duration of 250 as, a peak intensity of 3  × 1015 W cm–2 and
a central photon energy of 90 eV is used to image the wave packet
motion by doubly ionizing the system. The electron distribution at
t = 5.6 fs indicates a substantial probability of finding both elec-
trons at a large distance apart, which corresponds to a double-
ionization process (Fig. 6c). The high intensity of the attosecond
probe pulse is required to achieve a substantial double-ionization
probability. The single-photon double-ionization process is based
on the correlation between the two electrons and is therefore sen-
sitive to the relative distance between them. When they are in
close proximity, the electron correlation is relevant and facilitates
their ejection, thus maximizing the probability of double ioniza-
tion. When the electron distance is large, a minimum in double
ionization occurs as a consequence of the reduced correlation. In
such a case, the probe photon is mostly absorbed by the core elec-
tron, which is promptly ejected by the atom. The second electron
is subsequently ejected by a shake-off process80. The total yield of
doubly ionized helium therefore oscillates according to the oscil-
lations of the inter-electron distance and to the correlated angu-
lar distribution of the two electrons as a function of the relative
delay between the pump and probe pulses. In this respect, isolated
attosecond pulses are very efficient for imaging the evolution of
the electron wave packet because they allow the correlation (and
therefore the distance) between the two electrons to be ‘frozen’ at
the point of ionization.
Chu and Lin proposed the use of an XUV-pump/XUV-probe
approach for investigating the time evolution of electronic wave
packets of auto-ionizing states in atoms81. Auto-ionization of Fano
resonances82 — a fundamental process that involves electron cor-
relation — can be studied in a benchmark system such as helium,
using XUV radiation at 60 eV as the pump and an ultrashort syn-
chronized infrared field as the probe83,84. However, as pointed out by
Chu and Lin, the photoelectron spectra resulting from the interac-
tion of the auto-ionizing levels with the infrared field are often too
complex to deliver an intuitive picture of the outgoing wave packet.
More direct characterization of the wave packet can be achieved by
using an ultrashort XUV pulse as the probe.
Conclusions
Continuous progress in the development of laser sources for the
generation of femtosecond pulses and the exploitation of novel
techniques for the efficient generation of XUV pulses promises
to offer very important tools for the generation of attosecond
pulses with energies ranging from a few tens of nanojoules to a
few millijoules. In particular, in the case of joule-level driving
sources, the relativistic interaction of intense laser pulses with
overdense plasma could offer a route for the generation of attosec-
ond pulses with unprecedented intensities, which might be use-
ful for the investigation of yet unexplored research topics such as
non-perturbative and relativistic inner-shell processes or exotic
high-field physics in the XUV spectral region. Access to XUV
nonlinear optics using high-intensity attosecond pulses paves the
way to the observation of novel classes of ultrafast phenomena,
which will trigger further progress in the field of ultrafast optics
and spectroscopy.

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review articleS
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Acknowledgements
The research leading to the results presented in this Review received funding from the
European Research Council under the European Community’s Seventh Framework
Programme (FP7/2007-2013)/ERC grant agreement n.227355-ELYCHE. The authors
acknowledge financial support from the Italian Ministry of Research (FIRB-IDEAS
RBID08CRXK), support from the European Union under contract n.228334 JRA-
ALADIN (Laserlab Europe II) and from MC-RTN ATTOFEL (FP7-238362). G.S.
acknowledges financial support from the Alexander von Humboldt Foundation
(project Tirinto).