A photoelectron velocity map imaging spectrometer for experiments

combining synchrotron and laser radiations

P. O’Keeffe, P. Bolognesi, M. Coreno, A. Moise, R. Richter et al.

Citation: Rev. Sci. Instrum. 82, 033109 (2011); doi: 10.1063/1.3563723

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 REVIEW OF SCIENTIFIC INSTRUMENTS 82, 033109 (2011)

A photoelectron velocity map imaging spectrometer for experiments

combining synchrotron and laser radiations
P. O’Keeffe,1 P. Bolognesi,1 M. Coreno,1 A. Moise,2 R. Richter,2 G. Cautero,2 L. Stebel,2
R. Sergo,2 L. Pravica,3 Y. Ovcharenko,4 and L. Avaldi1
1
CNR-IMIP, Area della Ricerca di Roma 1, Monterotondo Scalo, Italy
2
Sincrotrone Trieste SCpA, Area Science Park, I-34149 Basovizza (Trieste), Italy
3
The University of Western Australia, 35 Stirling Hwy, Crawley, Western Australia, Australia
4
Institute of Electron Physics, 88017 Uzhgorod, Ukraine
(Received 5 January 2011; accepted 16 February 2011; published online 24 March 2011)
A velocity map imaging/ion time-of-flight spectrometer designed specifically for pump–probe exper-
iments combining synchrotron and laser radiations is described. The in-house built delay line detector
can be used in two modes: the high spatial resolution mode and the coincidence mode. In the high
spatial resolution mode a kinetic energy resolution of 6% has been achieved. The coincidence mode
can be used to improve signal-to-noise ratio for the pump–probe experiments either by using a gate
to count electrons only when the laser is present or by recording coincidences with the ion formed in
the ionization process. © 2011 American Institute of Physics. [doi:10.1063/1.3563723]

I. INTRODUCTION nation with the centroiding and event counting methods14, 15 )

Since its initial introduction in 1997 (Ref. 1) the veloc-
ity map imaging (VMI) technique has become one of the
most extensively used methods for the investigation of pho-
toionization and photodissociation dynamics of atoms and
molecules.2 Indeed, the number of publications based on the
use of this technique has been constantly increasing since that
date. VMI is based on the projection of 3D distributions of
charged particles onto a position sensitive detector (PSD) by
inhomogeneous electrostatic fields which have the property
of mapping particles of the same initial velocity to the same
point on the detector, independent of the point within the in-
teraction zone at which the particle was born. The original 3D
distribution can then be recovered from this 2D projection by
a mathematical inversion procedure, provided the system has
cylindrical symmetry around the axis parallel to the face of
the detector.2
This technique has been applied to the measurement of
the kinetic energies and angular distributions of photofrag-
ments produced by the photodissociation of molecules as
well as photoelectrons emitted, following photoionization of
atoms, molecules, and clusters. Furthermore, the method has
been coupled to numerous sources such as intense femtosec-
ond lasers,3 high harmonic generation sources,4 synchrotron
light sources,5–9 free electron lasers,10, 11 and nanosecond
lasers in combination with resonant multiphoton ionization
and even electron impact sources.12 The most common type
of PSD used in these experiments is the microchannel plate
(MCP)/phosphor screen/CCD camera setup which was used
in the original VMI paper.1 These PSDs work by amplify-
ing the signal using the MCPs and then accelerating the elec-
tron bunch thus formed onto a phosphor screen. The position
of arrival of the charged particle on the detector is recorded
by imaging the light produced on the phosphor screen onto a
CCD camera. The advantages of this method are that it is pos-
sible to achieve very high spatial resolution13 which in certain
cases is only limited by the pore size of the MCPs (in combi-
and furthermore, it is an intrinsically multihit technique in
which numerous particles can be detected simultaneously.
However, this type of detector has the disadvantage that the
timing information related to the arrival of the charged par-
ticle cannot be correlated with the position on the detector
with a greater timing resolution than the phosphorescence
lifetime of the phosphor screen which is usually on the or-
der of tens of nanoseconds (although some fast phosphors
can reach lifetimes of less than 10 ns at the expense of effi-
ciency). To overcome this problem numerous detectors mak-
ing use either of split anodes (e.g., see Ref. 16) or of delay
line anodes have been developed (e.g., see Refs. 17 and 18).
These types of detectors have the advantage that they can be
effectively used in coincidence type of experiments, where
it is necessary to correlate the position of the particle to the
position or arrival time of another particle arriving either on
the same or indeed on an entirely different detector. On the
other hand this type of detector does have limits on the num-
ber of particles which can be detected simultaneously. New
detectors such as the in-vacuum pixel detector recently de-
veloped aim at combining the advantages of these two types
of detectors providing a multihit, time- and position-sensitive
detector.19
In this paper we will describe the development of a new
VMI instrument designed specifically for use in experiments
combining laser and synchrotron radiation sources. As
mentioned above, the VMI technique is widely used in
laser laboratories throughout the world; however, it is still
relatively rarely used at synchrotron light sources. There are
of course some notable exceptions such as the experimental
setups developed at ALS,7, 9 Soleil,5 SLS,6 and Hefei8 in
recent years. The main limitation for the use of the VMI
technique at synchrotron light sources is due to the range of
kinetic energy of the particles which can be analyzed using
this technique. For example, the highest energy electrons
which have been analyzed to date using this method are of
40 eV although simulations suggest that with certain setups it

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 033109-2 O’Keeffe et al.
should be possible to analyze electrons with kinetic energies
of up to 100 eV.10, 11 Nonetheless, these kinetic energies are
quite limited with respect to the traditional hemispherical
analyzers used at synchrotron sources. However, in the case
of experiments combining synchrotron and laser radiations
and, in particular, when the laser is used as the ionizing
radiation, the kinetic energy of the particles (in this case
electrons) is limited by the energy of the laser (less than 6 eV
for most commonly used lasers) and, therefore, is amenable
to the analysis using the VMI technique. This VMI type of
analyzer has the significant advantage over the hemispherical
type of analyzer that it collects all electrons produced in
the interaction zone (i.e., 4π collection efficiency). This last
characteristic is especially important for synchrotron + laser
experiments in which the necessity to ionize a dilute sample
of synchrotron excited intermediate states results in a low
number of ionization events per second. Furthermore, this
characteristic is also very important for coincidence exper-
iments in which the overall efficiency of the coincidence
experiment is a function of the product of the detection effi-
ciency of each particle involved in the coincidence. In most
experiments performed to date using synchrotron radiation as
the pump and laser radiation as a probe ions were detected.
One exception to this is the work of Mitsuke et al.20 who
used a hemispherical analyzer to collect electrons from the
laser ionization of synchrotron excited Rydberg argon atoms.
In that work the quoted acceptance angle was ±8.5◦ which
when taken in proportion to the full solid angle yields a ratio
of 1:100. This means that with all other experimental param-
eters being equal a VMI analyzer would have 100 times more
counts than such a hemispherical analyzer. However, a higher
efficiency is accompanied by a larger background signal and
much of this work concentrates on methods to deal with that
background.
In this paper we will describe the first experiments com-
bining a VMI analyzer with synchrotron + laser. In Sec. II we
will make a description of the experimental apparatus, while
in Sec. III we will describe some demonstrative results taking
care to illustrate the advantages of this technique over tradi-
tional methods used in experiments combining synchrotron
and laser radiations.
II. EXPERIMENTAL SETUP
A. Apparatus
The experimental chamber houses a VMI setup opti-
mized for photoelectron detection mounted opposite to an
ion time-of-flight (TOF) tube [see schematic in Fig. 1(a)].
The synchrotron and laser beams are focused and overlapped
(both spatially and temporally) at the center of the chamber
in a counter-propagating geometry. At this point they inter-
act with the atoms or molecules under investigation which
are introduced into the chamber via a continuous super-
sonic beam formed by expanding a 1–2 bar of gas through a
50 μm nozzle. This nozzle is mounted on an XYZ-manipulator
in order to allow the nozzle to be centered on a 0.5 mm skim-
mer, the tip of which is placed at a distance of 12 cm from
the interaction zone. The expansion chamber is evacuated us-
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Rev. Sci. Instrum. 82, 033109 (2011)
ing a 1800 l/s magnetically levitated turbo molecular pump
(Adixen ATP 2300 M) and the working pressure in this ex-
pansion region was on the order of 5 × 10−5 mbar. Optimiza-
tion of the overlap of the two light beams with the supersonic
beam was possible by fine adjustment of the position of the
entire experimental chamber along all three axes. The dimen-
sions of the electrostatic optics used in these experiments are
shown in Fig. 1(b).
The entire setup is surrounded by a 2 mm thick μ-metal
shield in order to mask the effects of the earth’s magnetic
field. The residual magnetic field in the interaction zone was
not measured; however, it was sufficiently suppressed in or-
der to allow the measurement of the angular distribution of
electrons with kinetic energies as low as 13 meV.21
The geometry of the electrostatic lens used near the ion-
ization region is similar to that used in the original VMI
setup,1 although it should be noted that the TOF for elec-
trons is significantly shorter. Gold meshes with 70 lines/in.
were placed over the apertures on the ion side of the spec-
trometer. It should be noted that two meshes separated by
1 mm and operating at the same voltage were used in order to
prevent penetration of the voltages of the ion electrostatic op-
tics into the interaction zone which would have perturbed the
electron images. This region is pumped by a 1000 l/s pump,
while a 70 l/s pump is mounted almost orthogonal to the prop-
agation direction of the supersonic jet and acts as a beam
catcher in order to reduce backscattered gas. The operating
pressures in the main chamber with and without the super-
sonic beam were of the order of 5 × 10−7 and 7 × 10−8 mbar,
respectively.
B. Synchrotron light source
The apparatus outlined above has been installed at the
branch line of gas phase beamline at Elettra, the Italian syn-
chrotron light source. As this beamline has been described in a
previous publication,22 only the salient characteristics will be
outlined here. The light source is an undulator with a period of
12.5 cm and 4.5 m long. The linearly polarized radiation from
the undulator is deflected to a variable-angle-spherical grating
monochromator by a prefocusing mirror. The monochromator
consists of two optical elements: a plane mirror and a spher-
ical grating. Five interchangeable gratings allow the energy
range between 13 and 1000 eV to be covered. Two refocusing
mirrors after the exit slit provide an approximately circular
focus of diameter 300 μm at the interaction region in the ex-
perimental chamber.
C. Laser light source and synchronization
The laser light is generated by a mode-locked Ti:Saphhire
laser which is tunable in the range 670–1000 nm (1.25–
1.85 eV). This light source has also been described quite ex-
tensively in a previous work23 and again only the most rele-
vant characteristics of this source will be outlined here. The
Tsunami (Spectra Physics) laser can be operated either in the
continuous wave mode or as a mode-locked laser at a fre-
quency of 83.3 MHz. The temporal width of the laser can
 033109-3 O’Keeffe et al.
FIG. 1. (Color online) (a) Schematic overview of the experimental setup showing the VMI spectrometer for electrons mounted opposite to an ion time of flight.
(b) Dimensions of the electrostatic optics used in the spectrometer: a = 15 mm, b = 20 mm, d = 70 mm, c = 29 mm (active diameter of PSD), L ion = 127 mm),
and L elect = 210 mm.
be chosen to be either in the picosecond (12 ps FWHM) or
in the femtosecond range (50 fs FWHM). In the experiments
outlined in this paper the laser has been operated in the pi-
cosecond mode in order to provide the best temporal overlap
with the synchrotron light bunches (70 ps FWHM).23
The laser pulses are synchronized to one in every six syn-
chrotron light pulses (83.3 MHz is exactly one sixth of the
synchrotron repetition frequency of 500 MHz) using a com-
mercial lok-to-clock module (Model 3930, Spectra Physics),
while the ring frequency has been divided using a commercial
(clock distribution board AD9510, Analog Devices) timing
board. All measurements have been performed in the stan-
dard multibunch operation of Elettra. In this mode the time
separation between consecutive bunches is 2 ns, with ∼95%
of the ring filled.
The two light sources are focused to the center of the ex-
perimental chamber in a counter-propagating geometry [see
Fig. 1(a)]. The focused spot of the synchrotron light is a circle
of diameter 300 μm, while the laser is focused with a 50 cm
planoconvex (thus giving a spot size of ∼250 μm) and over-
lapped with the synchrotron light at the center of the chamber.
A small angle was introduced between the directions of prop-
agation of the two light sources in order to reduce the quantity
of IR laser light propagating inside the beamline. This was
necessary to avoid problems related to heating of the beam-
line optics by the laser light.
The axis describing the linear polarization of the light is
rotated around the direction of propagation of the laser light
using an achromatic half-wave plate. Furthermore, the wave-
length of the light was monitored throughout the experiments
by collecting some stray light from one of the alignment mir-
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Rev. Sci. Instrum. 82, 033109 (2011)
rors and transporting it to a wavelength spectrometer via a
fiber optic. Finally, the temporal width of the laser pulses was
monitored using an autocorrelator.
D. Position sensitive detector
The position sensitive detector employed in this veloc-
ity map imaging apparatus was designed and constructed at
the Instrumentation and Detectors Laboratory of Sincrotrone
Trieste.18 The detector consists of two resistance matched
MCPs behind which is placed a cross delay line anode with
two meander lines. This detector can be operated in two dis-
tinct modes.
1. High spatial resolution mode
This mode is illustrated in Fig. 2(a). When an electron ar-
rives on the front of the MCP an electron cascade takes place,
which eventually causes a localized shower of electrons to
arrive at specific X, Y positions on the delay lines. The four
signals, taken from each end of the delay lines, are amplified
immediately at the air-side of the detector in order to mini-
mize the noise pickup. Furthermore, to minimize the inaccu-
racies of the measured arrival times of the signals due to the
variation of their amplitudes, they are fed to constant frac-
tion discriminators (CFDs). Subsequently, the signals are dig-
itized by two time-to-digital converter (TDC) boards (ACAM
TDC-GPX operated in R-mode) with a time resolution of
27 ps. The results are collected on a field programmable gate
array (FPGA) motherboard (Altera Cyclone II FPGA) which
manages the flux of events, their logical consistency, and the
 033109-4 O’Keeffe et al.
FIG. 2. Schematic illustration of the two operative modes of the delay line
detector used in this work: (a) high spatial resolution mode and (b) coinci-
dence mode. See text for details.
transfer of the digitized data via a SCSI II cable to a home-
made PCI interface board on a standard personal computer.
The main difference between the operation modes lies in
how the four stops (two stops for each ACAM TDC) are used:
in the case of the high-resolution mode all stops are employed
for the position decoding, while in the coincidence mode two
of the four stops are used for correlating other external events
with each electron collected. In both cases the “TDC starts”
can be triggered internally or externally (with the MCP pulse
or pulse generator provided) so that TDCs work in “multi-
hit mode.” In the high-resolution mode the two stops of each
of the TDCs are the two ends of the delay lines. The X and
Y positions are then calculated from the differences between
these two “stop” times. When the internal trigger is used all
the “hits” are accumulated on the ACAM and transferred to
FPGA every 1 to 10 μs, depending on the trigger frequency
chosen (by means of a LABVIEW software controlling the
electronics).
The position of each hit is then binned into an image
which can be accumulated and stored by means of a dedi-
cated LABVIEW software. The main advantage of this method
is that measuring the time interval between the arrival time of
the signal at the two ends of the delay lines rather than the
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Rev. Sci. Instrum. 82, 033109 (2011)
time difference between one end and external trigger we ef-
fectively double the spatial resolution. This can be understood
by considering the arrival of a particle slightly off the center
of the delay line with respect to a particle arriving at the ex-
act center of the delay line; the time for propagation of the
signal to one end will be increased by t, while to the other
end it will be decreased by t. It is therefore clear that the
difference signal changes by 2t, and since this value must
be compared to the resolution of the TDC we have gained a
factor of 2 in the spatial resolution.
2. Coincidence mode
The second mode is different in approach as the electron-
ics and both TDC starts are now triggered by a pickoff pulse
from the microchannel plates of the PSD. To do this the sig-
nal must be decoupled from the high voltage. This is achieved
by a pickoff circuit on the high voltage line to the MCP con-
sisting of a high voltage capacitor, pulse amplifier, and CFD.
For a schematic illustration of this mode of operation, see
Fig. 2(b).
It is sufficient to take the signal from only one extrem-
ity of each of the delay lines in order to be able to determine
the position of arrival on the detector. This approach although
degrading the spatial resolution frees up two channels of the
TDCs so that the electron position can be recorded in coinci-
dence with the arrival time of the ions at the ion TOF detector
and with respect to the ring clock (1.15 MHz). This latter sig-
nal can be used to identify the arrival time of the electron with
respect to the laser pulse (see Sec. III B) and thus to determine
whether the electron was generated in the presence of the laser
field or not. We have chosen the ring clock (the frequency of
arrival of a given bunch—1.15 MHz) over the bunch clock
(the frequency of arrival of all the bunches—500 MHz) in or-
der to reduce the number of events recorded and thus the size
of the resulting data files.
As will be shown below this technique allows a signifi-
cant reduction of the background signal during the detection
of photoelectrons from two-color experiments using the VMI
apparatus. It does, however, result in a factor of 2 loss in reso-
lution, for the reasons explained in Sec. II D 1, i.e., due to the
fact that we are only taking signal from one side of the delay
line. In this mode of operation each start event is written out
to a file with all associated stop events. Postprocessing is then
performed on the data to extract the images and the coinci-
dence data.
Results from both of the above modes of operation of the
detector will be illustrated in Sec. III.
E. Image inversion software
The photoelectron images consist of a projection of the
original 3D distribution of electrons emitted from the target
onto a 2D surface. The photoelectron angular distribution of
electrons emitted in an n-photon process involving linearly
polarized light, when the polarization of all photons is paral-
lel, is completely described within the dipole approximation
by the following formula:24
 033109-5 O’Keeffe et al. Rev. Sci. Instrum. 82, 033109 (2011)

⎡ ⎤
σ ⎣
n
dσ
= (β2 j P2 j (cos θ ))⎦ , (1)
d 4π j=0

where dσ/d is the differential photoionization cross section,

n is the number of photons involved in the process, σ is the
total (angle-integrated) cross section, P2 j (x) are the Legendre
polynomials of order 2 j, θ is the angle between the polariza-
tion of the incident photons and the direction of the ejected
electron, and β2 j are the asymmetry parameters.
The goal of the measurement of the angular distribu-
tion of charged particles emitted from a photoinitiated event
is to extract these asymmetry parameters from the images
recorded. The method adopted here is the pBasex routine in-
troduced by Garcia et al.25 The pBasex method works by re-
constructing the original 3D distributions of the emitted elec-
trons by fitting a set of basis functions with known inverse
Abel integral to the 2D projected image. The β2 j parameters
can then be extracted from the coefficients of the analytical
functions.
We have ported the original code of Garcia et al.25 into a
Windows compatible program and have added extensive im-
age processing capabilities such as the possibility to rotate
the image, stretch it along one of the axes, and subtract back- FIG. 3. (Color online) Photoelectron image produced by ionizing argon
atoms with synchrotron photons of 16.262 eV. The left-hand side shows the
ground images.26
raw image, while the right-hand side shows the inverted image. The photo-
electron spectrum extracted is shown in the lower part of the figure.

III. RESULTS AND DISCUSSION

In this section the first results obtained by combining
all of the above components will be described. First, images
produced via direct photoionization of atoms with the syn-
chrotron light will be discussed, while in Sec. III B the results
obtained by combining the synchrotron light and laser radia-
tion to image electrons emitted from polarized atoms will be
described.
A. One-color experiments
Figure 3 shows the photoelectron image collected fol-
lowing photoionization of a beam of argon atoms with syn-
chrotron light of photon energy 16.262 eV. The photoelec-
trons produced on absorption of a photon of this energy can
have a kinetic energy of either 503 or 338 meV depending
whether the residual ion is left in the 2 P3/2 or 2 P1/2 state. The
figure shows the raw data on the left-hand side of the image,
while the inverted image is on the right-hand side. Finally, the
photoelectron spectrum extracted from the image is shown in
the bottom part of the figure. The measured relative inten-
sity of the two peaks in the photoelectron spectrum is given
by a ratio of 2.08:1, which principally reflects the degener-
acy of the 2 P3/2 :2 P1/2 states. Fitting a Gaussian to the 2 P3/2
peak with the FWHM as a free parameter yields a value of
30 meV which corresponds to a E/E of 6%. This image was
recorded while operating the detector in the high-resolution
mode outlined above.
Furthermore, as can be seen from the image the β
parameter describing the one-photon angular distribution of
electrons emitted is negative, i.e., electrons are preferentially
emitted perpendicular to the polarization axis of the electric
field vector of the ionizing light. Indeed, upon inversion of
the image we have extracted values of β = −0.05 ± 0.06 and
β = −0.05 ± 0.07 for the parameters describing the angular
distribution of electrons emitted, following the ionization
of Ar leaving behind the 2 P3/2 and 2 P1/2 states of the
ion, respectively. This value is consistent with the work of
Southworth et al.27 on the angular distribution of the electrons
produced by photoionization of Ar with radiation of energy
16.31 eV, in which they presented a value of β = −0.17
± 0.11 for photoionization to the 2 P3/2 state of the ion.
B. Timing and two-color experiments
To illustrate the performance of this experimental setup
for pump–probe experiments, results on the ionization of
aligned states of helium atoms prepared by absorption of a
photon of linearly polarized synchrotron radiation and then
ionized by a laser photon are presented. The examples chosen
are electron images recorded by photoionization of aligned
He 1s3 p 1 P1 atoms.
First, however, it is necessary to demonstrate the general
operation of the coincidence mode of the detector outlined in
Sec. II D and in particular the use of the ring clock of the
storage ring as a marker for the presence of the laser. To do
this we present a histogram [shown in Fig. 4(a)] of the ring
clock stops with respect to the starts given by electrons ar-
riving on the MCP (pickoff pulse) in the case of single pho-
ton ionization of helium [see schematic illustration shown in
Fig. 4(c)]. The important point to note is that this histogram
clearly maps out the bunch structure of the electrons in the
synchrotron storage ring in the multibunch mode. In the mode

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 033109-6 O’Keeffe et al.
FIG. 4. (Color online) Histogram of ring clock stops with respect to electrons arriving on the detector (MCP pickoff pulse) for (a) one-photon ionization of
helium atoms [see schematic in (c)] and (b) two-photon resonant ionization of helium atoms via the He 1s3p 1 P1 intermediate state [see schematic in (d)].
of operation of the synchrotron at Elettra used during these
experiments the electron bunches have a FWHM of ∼70 ps
and are separated by 2 ns. Therefore, it is clear that using the
ring clock as a stop with respect to the arrival time of the elec-
tron on the MCPs of the VMI apparatus maintains the electron
bunch structure in the storage ring. Indeed, fitting these peaks
with a Gaussian leaving the FWHM as a free parameter leads
to a value of 250 ± 30 ps. The photoelectrons are formed by a
synchrotron light pulse of FWHM of 70 ps in the interaction
zone; this further implies that once we have deconvoluted the
temporal width of the light pulses we are left with a apparatus
response of FWHM of 240 ps (assuming Gaussian functions
for both the light pulse and the apparatus response). The ap-
paratus response function is due to the spread of the electrons
during their flight from the interaction region to the detec-
tor, the temporal resolution of the MCPs themselves, and the
temporal response of the electronics. However, the principal
contributions are the first two of these. It is somewhat surpris-
ing that the spread of the electrons during their flight time is
so small as they have to fly 210 mm to the detector which
takes about 100 ns (depending on the extraction voltages) but
can be understood if one considers the pancaking effect of the
VMI electrostatic optics on the electron trajectories.
The timing structure of the signal is not of great use
for one-color experiments involving direct ionization, but be-
comes an extremely effective filter in the case of pump–
probe studies. This can be illustrated by examining the his-
togram ring clock stops with respect to electron starts shown
in Fig. 4(b) for the case of the two-photon excitation scheme
shown in Fig. 4(d). In contrast to the case of direct ioniza-
tion with one photon where electrons are only produced in the
presence of the synchrotron radiation, in this case the interme-
diate state, which is produced by absorption of a synchrotron
photon, has a half life of 1.7 ns. In this case the histogram
consists of a contribution from the two-photon signal (the
signal we are interested in), thus forming peaks every 12 ns
and another contribution from a background signal which
varies much less markedly on time. The background signal
in Fig. 4(b) consists mainly of electrons created by fluores-
cence photons hitting surfaces in the vicinity of the interac-
tion zone thus creating electrons which are accelerated to the
detector by the VMI electrostatic fields. This signal gives the
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Rev. Sci. Instrum. 82, 033109 (2011)
“sawtooth” shape to the signal as the half life of the inter-
mediate states is just less than the time spacing between the
synchrotron bunches. Other contributions arise from scattered
synchrotron light and back reflected synchrotron light from
the laser input window which lies on the opposite side of the
interaction zone with respect to the beamline. Again, in both
of these cases, the electrons are created at surfaces near the
interaction zone as verified by the disappearance of the back-
ground signal when the extraction voltages are switched off.
By recording the image signal in correspondence to the
two-color experiment it is possible to eliminate almost 96% of
the background (for a “laser-on” gate of 500 ps and a “laser-
off” gate of 11 500 ps). The 500 ps gate was chosen in order
to include all of the two-color signal. To demonstrate this we
have performed this operation on two photoelectron images
produced, following photoionization of He 1s3 p 1 P1 atoms
with laser light of wavelength 750 and 698.5 nm, thus pro-
ducing ensembles of electrons with kinetic energies of 175
and 275 meV, respectively.
The process is illustrated in Figs. 5(a) and 5(b) for the the
case of ionization of the He 1s3 p 1 P1 atoms with laser light
of wavelength 750 nm, where the image in (a) is the image
integrated over all times while that shown in (b) is the gated
image. As is well known the cross section for ionization of
the p state into the continuum decreases with photon energy
above the ionization threshold.29 As the fluorescence that pro-
duces the electron background remains constant this means
that the signal/background ratio gets smaller when increasing
the photon energy of the laser. This effect can be clearly seen
from the lower signal-to-noise ratio of the image in Fig. 6(a).
The gating process is, nonetheless, able to extract the image.
It is possible to compare the above method of cleaning up
the image to the more direct method of simply recording two
images; one with the laser and the other without, for approxi-
mately the same time and then subtracting one image from the
other. In this case there is no need for coincidences with the
ring clock and therefore can be performed in the high spatial
resolution mode of the detector. In Fig. 7 the images recorded
in this way in the same conditions (same hνSR and hνlaser ), as
those recorded in the coincidence, are presented.
The main difference which is immediately visible
is the higher resolution of the images recorded in the
 033109-7 O’Keeffe et al.
FIG. 5. (Color online) Raw photoelectron images corresponding to the pho-
toionization of aligned He 1s3p 1 P1 atoms with laser light of wavelength
750 nm thus produced electrons of kinetic energy 175 meV. Image (a) is
the time integrated image, while image (b) is the time-filtered image with
a laser-on bin of 500 ps. Images (c) and (d) are 3D representations of the
images generated by the software developed in Ref. 28. This representation
illustrates more clearly the signal-to-noise ratio of the unfiltered and filtered
images.
noncoincidence mode. The FWHM of the peak in the coin-
cidence spectrum is 33.4 ± 0.1 meV, while that taken in the
high-resolution mode is 20.3 ± 0.5 meV which correspond
to E/E of 12% and 7%, respectively, thus experimentally
demonstrating the 50% loss in kinetic energy resolution on
passing from the high resolution to the coincidence mode of
the detector (as discussed in detail in Sec. II D). However, if
we compare the photoelectron spectra extracted from the im-
ages in Figs. 6(b) and 7(c) (see Fig. 8) one can see that the
signal to background ratio of the coincidence-filtered image
is much better. Obviously in the case of the coincidence im-
FIG. 6. (Color online) Raw photoelectron images corresponding to the pho-
toionization of aligned He 1s3p 1 P1 atoms with laser light of wavelength
698.5 nm thus produced electrons of kinetic energy 275 meV. Image (a) is
the time integrated image, while image (b) is the time-filtered image with
a laser-on bin of 500 ps. Images (c) and (d) are 3D representations of the
images generated by the software developed in Ref. 28. This representation
illustrates more clearly the signal-to-noise ratio of the unfiltered and filtered
images.
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Rev. Sci. Instrum. 82, 033109 (2011)
FIG. 7. (Color online) Photoelectron images recorded in the high spatial res-
olution mode of the detector. Image (a) corresponds to ionization of He 1s3p
1 P atoms with laser photons of wavelength 698.5 nm (i.e., same conditions
1
as the image reported in Fig. 6). Image (b) is taken without the laser beam
present and images (c) and (d) are two different ways of portraying the sub-
tracted image (a)–(b).
age it is possible to extract a background image taken under
exactly the same conditions and to subtract this from the fil-
tered image, thus further improving the signal to background
of the final image.
Another way to filter the image in order to improve
signal-to-noise ratio is by recording coincidences with the
He+ ions formed during the ionization process, i.e., by us-
ing photoelectron-photoion coincidence (PEPICO). This pro-
cedure has also been performed in the same conditions as in
the case of the images presented in Fig. 6. A similar image to
that shown in Figs. 6(b) and 6(d) is obtained, however, with
∼50% less intensity in comparison to the time-filtered im-
age. The reason for this is that the transmission of the ion
FIG. 8. (Color online) The photoelectron spectra extracted from the velocity
mapped images shown in Figs. 6(b) and 7(c). The dotted line corresponds to
the image recorded in the high spatial resolution mode (Fig. 6), while the full
line corresponds to the image recorded in coincidence mode (Fig. 7).
 033109-8 O’Keeffe et al.
TOF is reduced from 100% due to the presence of the gold
meshes on all of the apertures on the ion collection side of the
spectrometer. Furthermore, the time filtering method could be
used in cases where the intermediate state is above the ion-
ization threshold. In this case the use of PEPICO would not
distinguish between one- and two-photon signals.
IV. CONCLUSIONS
The VMI apparatus described in this paper has been de-
signed specifically for experiments combining synchrotron
and laser radiation sources in pump–probe experiments. It
has been demonstrated that by using the timing informa-
tion from the synchronization between the laser and the syn-
chrotron light pulses it is possible to obtain a gain in the
signal/background ratio of the two-color images of a fac-
tor of ∼25. This time filtering method has certain advan-
tages over the more commonly used PEPICO methods such
as (a) an ion TOF is not required, (b) signal is not lost due
to less than 100% efficiency in detection of the ions, and
(c) this method could be used when the intermediate state of
a two-photon process is above the ionization threshold when
PEPICO would not reduce the one-photon background. In
contrast, in cases when the background is extremely large the
use of PEPICO may be more efficient as the time filtering
removes only 96% of the background. In general, the gain
in signal-to-noise ratio resulting from these two methods will
allow the detection of very weak signals and allow the 4π col-
lection efficiency of the VMI apparatus to be fully exploited.
ACKNOWLEDGMENTS
The authors thank the Elettra support program for Italian
users and the staff of Elettra for providing high quality light.
This research was partly supported by a Marie Curie Rein-
tegration Grant within the 7th European Community Frame-
work Programme. Y. O. thanks the ICTP-Elettra Users’ Pro-
gram. They would also like to thank Laser Optronic S.p.A.
for a loan of the autocorrelator. Finally, they would also like
to thank the authors of Ref. 25 for providing us with the orig-
inal code of pBasex and P. Bertoch, R. Di Nino, C. Leghissa,
M. Petrucci and F. Salvador for technical support.
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