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Multiphoton above-threshold ionisation of xenon at 0.53 and 1.06μm

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1982 J. Phys. B: At. Mol. Phys. 15 1353

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J. Phys. B: At. Mol. Phys. 15 (1982) 1353-1369. Printed in Great Britain

Multiphoton above-threshold ionisation of xenon at 0.53

and 1.06 p m
F Fabre, G Petite, P Agostini and M Clement
Service de Physique des Atomes et des Surfaces CEN-Saclay, 91191 Gif-Sur-Yvette
Cedex, France

Received 7 December 1981, in final form 1 February 1982

Abstract. Standard techniques of photoelectron spectrometry have been used to study

multiphoton ionisation of xenon. At 0.53 pm,up to ten-photon ionisation of the 5p shell
is detected above the six-photon ionisation threshold for both the Xe+ 2P1/2 and ‘P3/2
states. The intensity dependence is compared with the predictions of perturbation theory.
The branching ratio ’P3/2 : has been measured as a function of the ionisation order.
At 1 . 0 6 p m up to 21-photon ionisation has been detected above the eleven-photon
ionisation threshold.

1. Introduction

Since the first demonstration of above-threshold ionisation (ATI) (Agostini et a1 1979),

there has been a continuous interest in this topic. The study of the energy and angular
distributions of photoelectrons produced by multiphoton ionisation, in high-intensity
optical beams is of interest from the fundamental point of view as well as for some
applications.
As stated by Zernik and Klopfenstein (1965), the physical process involved is that
of N-order transitions occurring simultaneously with (N-1 )-order transitions. From
a theoretical point of view, this problem has some connection with the problem of
resonances in multiphoton ionisation, since, in both cases, the multiphoton transition
occurs through a real intermediate state, which brings about the question of the validity
of the lowest-order perturbation theory (LOPT). Even within this framework, the
calculation of the transition amplitude is a challenge for the theory: a list of theoretical
works tackling this difficult task will be found below. Experiments involving ATI also
provide a new approach to the study of the so called gradient force, which can
accelerate a free electron embedded in a light intensity gradient (Kibble 1966). This
force, also known as the ponderomotive force, has been studied mainly in high-density
plasmas and new aspects of it have been recently discussed (Kupersztych 1979).
In spite of this ‘theoretical’ interest there have been few experiments in this field.
In two preliminary experiments (Agostini et a1 1981, Fabre et a1 1981) we have
demonstrated the possibility of multiphoton ATI (i.e. absorption of several photons
above the ionisation threshold) and measured the angular distribution of ejected
electrons. Both experiments, as well as the one performed by Kruit et a1 (1981), used
xenon, a very simple gas to handle experimentally but, unfortunately, a very complex
atom. For Xe the calculation of the multiphoton ionisation transition amplitude still
cannot be computed. However, it seemed interesting to compare experiment with

0022-3700/82/091353 + 17$02.00 @ 1982 The Institute of Physics 1353

1354 F Fabre, G Petite, P Agostini and M Clement

the theoretical predictions made for simpler atoms since, for the time being, we are
interested in the simplest aspects of the theory. The aim of this experiment was
therefore to test the LOPT predictions concerning the amplitudes of the ATI transitions
observed in multiphoton ionisation (of Xe at 0.53 and 1.06 p m ) and their dependence
on the light intensity. It is the purpose of this paper to present and discuss its results.
In 8 2 we will briefly review the theory of ATI with some emphasis on its particular
aspects which can be tested on xenon. In 0 3 we describe the experimental apparatus
and the experimental procedure we have utilised. In Q 4 we present the experimental
results which are discussed in 8 5.

2. Theoretical considerations

2.1. General considerations

The physical process to be described here can be modelled as the multiphoton
ionisation of an atom to several continua. The earlier calculations of multiphoton
ionisation had generally taken into account only one final energy (figure l ( a ) ) . The
transitions towards higher-lying continua (figure l b ) ) were usually assumed to be
negligible, an assumption which was supported by a number of measurements. At
moderate laser intensities (Petite et a1 1979), as well as at rather high intensities
(Lompre et a1 1977), the dependence of the total ionisation rate on the laser intensity
was found to be in agreement with the predictions of the lowest-order perturbation
theory, except in the case of resonant processes. Therefore, the first question which
can be addressed to the theory is about the relative amplitude of the different
transitions. Then, if it is found that they are of some importance, the dependence of
these transitions on the laser intensity is very interesting, since the validity of the
lowest-order perturbation theory is questionable.

(bl
Iis)
- -- - -3 -- - --

Figure 1. Schematic diagram of ATI showing ( a ) the number N of photons just necessary
to ionise and ( b ) the number S of photons absorbed above the ionisation threshold. The
ground and final states are, respectively, ig), if) and Ifs).
 Multiphoton above-threshold ionisation of xenon 1355

Most of the theoretical works on ATI since the first paper by Zernik and Klopfen-
stein (1965) have been concerned with the numerical calculation of the transition
amplitudes of two-and three-photon ATI of hydrogen: Karule (1971, 1975, 1976,
1978), Klarsfeld (1970), Klarsfeld and Maquet (1979a, b,), Aymar and Crance (1980),
Gontier et a1 (1980). The first generalisations to higher-order ATI by Gontier and
Trahin (1980) and to alkali atoms by Aymar and Crance (1981) allow some general
rules to be inferred.
Using the notation of Gontier and Trahin (1980), the total ionisation rate WTfor
a giveii photon energy E , becomes

In this expression, I is the laser intensity, N is the minimum number of photons of

energy E, necessary to reach the continuum, S is the number of photons absorbed
above the ionisation threshold (see figure l(6)). proportional to the square
of a ( N + S)-order matrix element, depends on the atomic structure, the light polarisa-
tion and the photon energy. Finally, L Y ” * ~ ) ( E , ) is
I ~the
+ ~ionisation rate to the Sth
continuum. From (1)two important quantities can be defined.
( a ) Threshold intensity. The intensity at which two consecutive terms in (1)become
equal has been introduced by Gontier and Trahin (1980) and called the threshold
intensity. It is defined by

Gontier and Trahin (1980) have shown that, for S > 1, Ithvirtually does not depend
on S, except for a slight increase, which, fortunately, makes the series (1)convergent.
The consequence is that, for pulses of maximum intensity, IM-Ith, the ionisation
rates to the different continua are almost equal and the electron energy spectrum is
rapidly broadened. I t h depends on the atom: for six-photon ionisation of hydrogen
it is equal to W cm-’. I t h decreases with increasing ionisation order ( N ) ;for
example, it drops to lo1?W cm-* for N = 10.
(b) Saturation intensity. Saturation of the ionisation process occurs when all the
atoms in the interaction volume are ionised. This problem has been studied so far in
the case of ‘pure’ multiphoton ionisation, that is neglecting ATI. In this case, equation
(1)becomes
W*(E,) = (E,) I N (3)
and the saturation intensity for a given laser pulse can be defined as

where T~ is the Nth-order interaction time (Morellec et al 1976). If ATI is taken into
account, equation (3) no longer holds, but its physical content remains valid. For a
given pulse shape, there is a maximum value of the peak intensity beyond which any
increase of the laser intensity will not result in an increase of the ionisation probability,
ionisation taking place at the beginning of the pulse only, until neutral-atom depletion
is complete. Saturation intensities can be calculated for the case of ‘pure’ N-photon
ionisation. For six-photon ionisation of Xe at 0.53 p m , the saturation intensity is
found to be 10” W cm-’, while for eleven-photon ionisation of Xe at 1.06 wm it is
1356 F Fabre, G Petite, P Agostini and M Clement

3.5 X 10” W cm-’. These values are certainly modified if ATI is of importance, but
their order of magnitude should remain unchanged.
Clearly, the best conditions for the observation of ATI are
IM -Is - Ith.

-
Unfortunately, for any realistic pulse duration, the second condition (Is Ith)is
difficult to fulfil. The only freedom for the experiment is therefore to choose an
intensity I M - I s . If I M - I s , all the atoms are ionised during the first part of the
pulse (while I < I s ) as mentioned above.
It must be emphasised that the ( N + S)-photon ionisation rates, as predicted by
LOPT, are quite comparable with ‘normal’ ionisation rates which involve the same
total number of absorbed photons. As an example the three-photon ATI rate for
caesium at 0.53 p m is
W , = 6.3 x 1, s-’ ( I in G W cm-2)
(Aymar and Crance 1981) when the‘normal’three-photon ionisation rate for an alkali
at 0.53 p m is about (Morellec et a1 1982)
w,= i o 2 x 1,s-l.
All the above conclusions are valid for a uniform intensity distribution and a square
pulse. In order to describe real situations, the formula (1) should be averaged over
the space and time distribution of the intensity (Gontier and Trahin 1980). However,
the results are only slightly modified, at least for the usual smooth temporal and spatial
distributions.
Since all the calculations mentioned are made within the framework of the LOPT
they obviously predict that the rate for an ( N + S ) ionisation is proportional to IN+’
(see equation (1)). Crance and Aymar (1980) have developed a non-perturbative
treatment of this process, but they come to the conclusion that the predictions of the
LOPT are valid when Is is used instead. In a more detailed calculation (two-, three-
and four-photon ionisation of Cs and K, Aymar et a1 1981) they have taken into
account higher-order terms. However, for intensities of the order of Is, these terms
do not exceed a few per cent of the lowest-order one and do not significantly modify
the intensity dependence of the corresponding rate.
To summarise these theoretical considerations it can be said that, on the basis of
the LOPT, ( N + S ) above-threshold ionisation is very similar to an ( N + S ) ‘normal’
multiphotonionisation, as far as the rate magnitude and intensity dependence are
concerned.

2.2. Multiphoton ATI of xenon at 0.53 and 1.06 p m

Regarding the expected electron energy spectra in the special cases of multiphoton
ionisation of xenon at 0.53 and 1.06 p m , a few points have to be made. As is well
known, photonionisation of the p shell above the second ionisation threshold produces
ions either in the 2P3/2 state or in 2 Pl12 state (Wuilleumier et al 1977). As a
consequence, the ejected-electron energies ar expected to form two series of lines
(which are labelled in this paper t, S and 3, S where S is the number of photons
absorbed above the threshold). The energy gap between the two series, equal to the
core fine-structure splitting is 1.3 eV. The relative amplitudes of two lines with the
same S is expected to be equal to two, the statistical branching ratio. Figure 2 shows
 Multiphoton above-threshold ionisation of xenon 1357

Figure 2. Expected photoelectron spectra corresponding to ionisation of Xe at ( a )1.06 wm

and ( b ) 0.53 p,m. The two series of lines correspond to 'P312 and ion states and n
is in arbitrary units.

the photoelectron spectra corresponding to six- and eleven-photon ionisation of Xe

at respectively 0.53 and 1.06pm. It should be noted that in this last case the two
series are barely resolved.

3. The experiment: apparatus and procedures

3.1. Apparatus
The experiment was designed to meet the following requirements:
(i) achieve multiphoton ionisation of xenon gas at 1.06 and 0.53 p m .
(ii) measure the energy and angular distributions of the photoelectrons at moderate
resolution (since the peaks to be resolved are 1.17 and 2.34 eV apart).

3.1.1. The laser. The oscillator is a passively Q-switched Nd-YAG system (Quantel).
The output mirror is composed of two thick glass plates: one 12cm long and one
0.5 cm long, both made of high-index glass. They act as mode selectors, together
with the Q-switching BDN Kodak dye, to give a signal longitudinal mode output. A
2 m m aperture selects the T E M ~transverse
~ mode and a stack of Brewster-angled
glass plates forces a linear polarisation. The pulse duration is set to about 20 ns by
adjustment of the BDN concentration. The maximum repetition rate is 10 pps. The
pulse is then amplified by two Nd-YAG commercial amplifiers (4 = 7 mm, 4 = 9 mm,
1 = 10 cm) and the output energy per pulse is 700 mJ. The 1.06 p m (1.17 eV) funda-
mental-mode output can be frequency doubled by a crystal with a maximum efficiency
of 30%. The aveIage powers available are 7 W at 1.06 p m and 2 W at 0.53 p m .
While the oscillator output is, spatially, a smooth Gaussian ( T E M " ~ ) , after the two
1358 F Fabre, G Petite, P Agostini and M Clement

amplifiers the spatial distribution is strongly distorted, due to diffraction by the rod
walls and thermal effects.
When frequency doubling is used a reducing telescope, between the second
amplifier and the KDP crystal, allows us to compensate for the thermal-lens effect in
the rods and also increases the conversion efficiency. The laser beam is focused inside
the vacuum chamber by a sphero-parabolic lens with a 80 mm focal length corrected
from spherical aberration. From divergence measurements the maximum intensity at
the focal point is estimated to be a few lo1' W cm-2 at 1.06 p m , and between 5 x 10"
and 10l1W cm-' at 0.53 p m . A precise measurement of the intensity distribution in
the focal plane is possible in principle (Lompre et a1 1982), but was not carried out
in this experiment. Therefore, a rather large uncertainty remains for the intensity
(about a factor two), but this is not of too much consequence since quantitative
comparison with theory is not yet possible for xenon.

3.1.2. The electron analysis and detection. The interaction chamber is pumped to a
residual pressure of lo-' Torr by a standard diffusion pump. It contains the focusing
and output laser optics and the electron analyser and detector. All these parts are
enclosed in a CONETIC shield where the magnetic field is reduced to less than 1 mG.
The electron analyser is a conventional spherical (180") device (Ballu 1980). It is
made of molybdenum and the mean trajectory has a radius of 30 mm. It is operated
at a constant analysis energy i.e. the voltage between the internal and external
hemispheric electrodes is kept constant. The analysis energy is then proportional to
this voltage.
This operating mode keeps the resolution R constant (Ballu 1980) since it is equal
to
2E.4 AS
R=-=-= constant
AE Ro

Figure 3. Diagram of the experimental apparatus

 Multiphoton above-threshold ionisation of xenon 1359

where AE is the width (FWHM) of the apparatus function and EA is the analysis energy,
while AS is the input aperture diameter and Ro is the radius of the average trajectory.
The constant depends only on the analyser geometry. In the experiment Ea was
adjusted to about 20 V. This resolution was sufficient to resolve the photon energies
involved (1.17 and 2.34 V) and allowed a larger output current. The energy analysis
is carried out by scanning the average voltage of the analyser with respect to the
interaction region (electrical ground).
Since we were interested not only in the energy calibration of the spectrum but
also in the relative amplitudes of its different components, the input electron optics
was designed t+3 have a transmission as flat as possible. This consists of a lens with
four cylindrical electrodes (figure 4 ( a ) )terminating on a conical grounded electrode
which aims at the interaction volume. The voltages on the four electrodes are scanned,
together with the analysing voltage. The region separating the cone (whose voltage
is constant) from the first cylindrical electrode is limited by two plane, parallel, grids
in order to avoid any lens effect. The resulting transmission (figure 4 ( b ) )is almost
flat except for a drop below one volt which could be also due to contact potentials.
This transmission curve has been obtained by measuring the ratio between the output
and input current from an electron source which produces electrons in the 0-20 eV
range and is temporarily located in front of the optics. The overall transmission is of
the order of

0 5 10
E IV)

Figure 4. ( a ) Details of the electron optics: 0, a,

analyser input aperture; 0, @, 0,
cylindrical electrodes; @, 8, two grids which determine a field-free space. ( b )Transmission
( T )of the analyser and the electron optics system plotted against electron kinetic energy.

The electrons are detected by a standard electron multiplier (channeltron) which

can be operated at a pressure up to Torr. This produces 100 mV, 10 ns pulses
for one electron (gain about 10'). These pulses are then amplified and fed to a gated
discriminator which delivers normalised TTL pulses. Since the counting rate in the
experiment is about 1 counts-' there are no saturation problems for the channeltron.
A small computer both produces the scanning voltage and accumulates the counts:
1360 F Fabre, G Petite, P Agostini and M Clement

for each laser pulse a 500 ns gate is triggered and the pulses accumulated in memory.
This is repeated for ten laser pulses and then the analysing voltage is increased by
a programmed step. When the whole programmed energy range is scanned the whole
sequence is repeated until a satisfactory number of counts has been accumulated.
The electron optics adjustment and the energy calibration were carried out by
using an auxiliary electron gun and detecting the elastically scattered electrons. The
geometry of the laser beam, the detection axis and the electron gun are shown in
figure 3. Using this method the absolute calibration is obtained within the limit of
the contact potentials (a few tenths of a volt). The exact calibration is then obtained
by self identification of the spectrum (see below) (figure 5 ) .

i I t

0 50 100 150 200

Channel number

Figure 5. Calibration obtained by identification with the spectra at 0.53 pm ( + ) and

1.06 firm (A).

3.2. Procedures
3.2.1. Energy scan. The electron energy is scanned with the laser intensity and
polarisation and the gas pressure being kept constant. The average laser power,
measured by a Scientech power meter after the interaction chamber, is monitored on
a chart recorder. A slow variation of this average power (&.5%) is tolerated during
the accumulation. The results are not corrected for these variations. Also, about
10% of the laser shots are multimode (about three modes) and, therefore produce
an ionisation rate higher than the average because of intensity modulations. Since
the counting rate is about 0.1 electron per laser shot, this correction has been neglected
as well.
The pressure is kept constant, by adjusting the input gas flow, within the precision
of the pressure guage reading.

3.2.2. Intensity variation. Since we were not monitoring the spot size of the focused
beam, it was important to use a method which kept this size, as well as the focus,
constant (Lompre et a1 1982). Therefore, we could not adjust the pumping of the
amplifiers or insert optical densities in the beam (those cannot be used anyway since
they are destroyed in a very short time), to vary the laser intensity.
 Multiphoton above-threshold ionisation of xenon 1361

Intensity adjustment was obtained with the following system (not shown in
figure 3): a polariser (consisting of a stack of Brewster-angled thin plates) is crossed
compared with the laser output polarisation. A half-wave plate is inserted before the
polariser and the output power is adjusted by rotating this plate. In this way the
polarisation, the divergence and the spatial distribution of the beam are kept constant.
The power variation is then proportional to cos2 24 where 4 is the angle between
the ;A optical axis and the initial polarisation.

3.2.3. Pressure scan. The pressure is set to a specified value by adjusting the input
gas flow. The maximum pressure in the chamber is 10-4Torr since there is no
differential pumping.

3.3.4. Polarisation variation and angular distribution. This procedure has been
described in a previous paper (Fabre et a1 1981). We just recall here that the
polarisation direction is varied by rotating the $ A plate without the polariser.
In the next section we present the experimental results corresponding to the
pressure and intensity variations. The results of angular distributions measurement
have been previously published (Fabre et al 1981).

4. Experimental results

4.1. Six-photon ionisation at 0.53

The absorption of up to four photons more than the minimum (six) required to
photoionise xefion atoms at 0.53 p m has been reported already (Agostini et a1 1981).
Using the electron optics adjustment corresponding to figure 4 it is not, in general,
possible to observe the (i,0) line associated with the second ionisation limit. This is
due to several reasons: the transmission drop for energies below 2 eV, contact poten-
tials of the order of the electron kinetic energy and space charge effects. It is, however,
possible to enhance the transmission at low energy by using different voltages on the
optics, with the drawback that the transmission curve is no longer 'flat'. Figure 6
shows a spectrum obtained under these conditions and where the ($, 0) line is observed.
On this spectrum the lines appear to have a width of about 0.5 eV which is due to
an instrumental width (0.3 eV) on the one hand and to a space charge broadening on
the other hand.
For the maximum power available, the intensities of the (9, S ) series lines relative
to the (+, 0) line are given in table 1, and compared with the ratio a ( 6 , S ) / a ( 6 , 0 )
calculated from Gontier and Trahin (1980), for an intensity of 10" W cm-2 in the
case of hydrogen.
The error bars have been calculated assuming an uncertainty of & for a count
of n. The large discrepancy between the two rows shows that a simple hydrogenic
model is not suitable for describing the ATI of xenon.
Regarding the branching ratio, R,the statistical value expected is 2.0 (3P3/2/2P1/2).
Most of the measurements reported in the literature (obtained in photoionisation
experiments) deviate from this value (Wuilleumier et a1 1977).
For the resonant multiphoton ionisation of Xe the only published value is that of
Compton et a1 (1980). They found R = 1 and explained this discrepancy by a rapid
fall-off of the photoionisation cross section when the photoelectron energy increases,
1362 F Fabre, G Petite, P Agostini and M Clement

E (VI

Figure 6. Spectrum of electrons showing the ti, 0) line A = 0.53 Fm.

Table 1. Relative line intensities.

s 0 1 2 3 4

1 0.54k0.08 0.35 *0.06 0.12k 0.03 0.016*0.008

tf, 0)
a ( 6 , SI
1 2.04 2.0 2.01 1.91 io-22
a (6,O)

There we report measurements of R as a function of S. The results are given in table

2.
The measurements in table 2 have been taken for a polarisation which is parallel
to the detection. For a polarisation perpendicular to the detection, this ratio increases
dramatically and the series corresponding to 2P1,2is barely detectable (Agostini et a1
1981). The uncertainty mentioned is the standard deviation over several measure-
ments. The results have been corrected for the electron optics transmission. No
attempt has been made to eliminate the systematic error due to the scattering of
photoelectrons on the xenon gas (Dehmer and Berkowitz 1974) since this error is
small compared with the overall uncertainty of the measurements.
It appears that the measured values of R are quite different from the statistical
ratio. This is not too much of a surprise since, even for single-photon ionisation the

Table 2. Values of R as a function of S.

s 0 1 2

2P3/2
0.74 k 0.2 2.3k0.1 3.3 1.0.3
2P1/2
 Multiphoton above-threshold ionisation of xenon 1363

value of 2.0 is almost never observed. In fact, as mentioned by Compton et a1 (1980),

several factors influence the branching ratio: configuration interaction, intermediate
resonances and final electron energy, and it is quite difficult to make a reasonable
prediction. It can be noted that the observed ratios seem to increase with S. Among
the above mentioned factors only the last one could be reasonable for this effect since
the others do not depend on S.

4.1,I. Pressure dependence. The pressure dependence of the electron spectrum has
been investigated between 5 x lo-’ and 5 x lo-’ Torr. Between 5 x lo-’ and 5 x
10-6Torr the total number of counts in each peak increases linearly (see figure 7).
This is to be expected since for such low atomic densities, collisions cannot play any
significant role. This linear dependence confirms that the observed process is a direct
one-step transition from the ground state to the continua.

P (Torr1

Figure 7. Total number of counts C (arbitrary units) as a function of the pressure for
two average powers. I = 1 Wand f = 0 . 6 W.

While the total count increases linearly, each peak is shifted towards low energies
and is asymetrically broadened in the same direction (figure 8). This is presumably
due to the space charge effect of the ions: the laser pulse creates a large ion and
electron density (almost total ionisation of the interaction volume); the electrons
whose kinetic energy is much larger than thermal energies leave this volume and
are slowed down by the ionic attraction. Using a very rough model of this effect (one
electron with a initial kinetic energy of a few electron volts submitted to the Coulomb
force of a charge equal to the sum of all the ion charges) one can estimate the
broadening to a few tenths of an electron volt, comparable with the observed effect.
Above lO-’Torr this space charge effect is so large that the line structure of the
spectrum is washed out, and the total counts summed over the whole spectrum begin
1364 FFabre, G Petite, P Agostini and M Clement

Pz 4 7Y Torr

counts /
350 l a s e r
pulses

E (eV1

Figure 8. Pressure effect in the (4,O) peak: the shift towards low energies and broadening.

to saturate. All the measurements have been carried out around 10-6Torr, in the
linear region of the pressure dependence.

4.1.2. Intensity dependence. The intensity dependence of the different lines has been
investigated between 0.5 and 1 W average laser power, measured after the interaction
chamber. This range was limited at one end by the maximum laser power available
and by the accumulation time the other end. It was not possible, in this experiment,
to measure the absolute value of the intensity. Due to the poor spatial distribution
of the beam intensity it would have been necessary to use sophisticated techniques
(Lompre et a1 1982) which were not yet available. However, by comparing these
results with older findings on multiphoton ionisation of xenon and krypton (Agostini
et a1 1970),especially for the saturation intensity, it was possible to situate the intensity
between 5 x 10" and 10l1W cm--2. These values are also in agreement with a direct
estimate of the focus spot size. As a consequence, an average power of 1 W i n figures
9 ( a ) ,9(b),9(c)and 9 ( d )corresponds to an intensity of 10" W cmP2 to within a factor
of two.
Figures 9 ( a ) , 9 ( b ) ,9 ( c ) ,9 ( d ) show, on a log-log scale, the intensity dependence
of selected lines of the electron spectrum. These results were obtained by adjusting
the electron energy at one peak, setting the $A plate to obtain the desired average
power and scanning the analyser over a small number of channels (3 to 6) around the
mean value. The counts were then accumulated until a few hundred were obtained.
The time necessary for such an accumulation was from a few minutes to about half
an hour, depending on the line and laser power. In all cases, the noise shots were
counted for the same time (with the laser running, but blocked before the chamber)
 Multiphoton above-threshold ionisation of xenon 1365

i iw)
I
.

-0 Id)
v)
+
C

010-

005-

t
05 10 05 10
i iwi i IW)
Figure 9. Total number of counts per laser shot for some lines of the electron spectra as
a function of the average laser power on a log-log scale. ( a ) , line ($, 0); ( b ) ,line (3,
I);
(4,
(c), line ($,2)and ( d ) , line 1). The straight lines have the ( N + S ) theoretical slope.

and was, at least, ten times smaller than the smallest signal counts. The experimental
results were then fitted, by linear regression, to the expected theoretical dependence
log c, = ( N + S ) log I. (4)
1366 F Fabre, G Petite, P Agostini and M Clement

In this expression, C, is the total number of counts summed over all the channels
corresponding to one line divided by the number of laser shots, I is the intensity and
( N + S) is the total number of absorbed photons. Table 3 summarises the results and
the comparison.

Table 3.

Line

N + S (Theor) 6 7 8 6 7 8
N + S (Exp) not 7.3*0.1 7.8k0.3 5.5zk0.7 6.5zk1.6 5.7k1.8
measured

The experimental values are the averages over several independent measurements
and the uncertainties are the standard deviations divided by the square root of the
number of measurements. There are several serious limitations to the precision of
such measurements. First, there is the onset of saturation (visible in figure 9 ( a ) )which
induces a deviation from the linear dependence (4). Second, the ion space charge
effect (similar to the one mentioned above) broadens the peaks and, therefore limits
the counts summed over to a fixed number of channels. Third, the statistical scattering
of the counts, especially at low-count values. All these reasons tend to systematically
lower the observed ‘slope’ ( N + 3 ) . However, except for the ($,2) line, the expected
values are within the errcr bars. It should be pointed out, neverthe-
less, that, especially for the $ configuration, the observed slopes are lower than the
expected ones and that higher-order effects (Aymar and Crance 1981) are not com-
pletely excluded by these results, although they are very unlikely.

4.2. Eleven-photon ionisation at 1 . 0 6 ~ m

The ATI of Xe at the fundamental frequency of our Nd-YAG laser was also studied.
An electron energy spectrum obtained in this case is shown in figure 10. It displays
a series of eleven peaks, resulting from up to ten-photon ATI of Xe. This spectrum
was obtained for a Xe pressure of 4.7 x Torr. The determination of the laser
intensity used in this experiment is subject to the same limitations as in the case of
(6 + S)-photon ionisation at 0.53 p m , since no precise photometric measurements of
the focal spot were made. The results of figure 10 were obtained for pulse energies
only three times higher than in the case of 0.53 p m , but the beam quality in this
experiment was much better, because some optics and the KDP were removed from
the beam. An argument based on the intensity dependence of the spectrum can also
be used here. The slope of curves identical to those of figure 9 for the peaks
corresponding to S = 1, 2 and 3 is found to be the same for the three peaks, and equal
to 3.4 This definitely places our intensity in the saturation region of the eleven-photon
ionisation of Xe. However, highly saturated multiphoton processes are known to lead
to slopes much lower than three (Agostini et a1 1970, Cervenan et a1 1975, Delone
et a1 1971, Arslanbekov et a1 1975, Normand and Morellec 1980, LomprC et a1 1980).
The intensity leading to complete saturation of xenon of the process was found to
 Multiphoton above-threshold ionisation of xenon 1367

100 -
m
- m
3
a
b
- 0

0
0.
p.

2 L 6 8 10 12 E (VI
Y I, ,I II ,I I, I, U ,I
*
0 2 4 6 8 10 5
Figure 10. Energy spectrum of ejected electrons at 1.06 pm. S is the number of photons
absorbed above the ionisation threshold. The two series of lines corresponding to the two
states of the ion are not resolved.

be 3.5 x 10” W cm-’, This indicates that our intensity must have been of the order
of a few lo1*w cm-’.
Unfortunately, spectra like those of figure 10 are of limited interest since, as shown
in 92, each peak is the result of the superposition of two different orders of ATI leaving
ions in different states. However, the comparison of this result with other similar data
calls for some comments.
Observation of a similar spectrum is reported in Kruit et a1 (1981) for laser
intensities around 10l2W cm-’. These two results differ noticeably from those repor-
ted in Agostini et a1 (1979), which showed only a broad peak centred around 4.5 eV.
In addition to a lower resolution of the apparatus used in our 1979 experiment, at
least two reasons can explain these differences. The 1979 experiment was performed
with a laser intensity of about 1013W cm-’ and at a Xe pressure of Torr. As
we have shown above, the use of higher intensities and pressures both lead to a
broadening of the peaks of figure 10, which may have led to a complete smearing in
the case of the spectrum obtained in the 1979 experiment. This, in particular, suggests
that the conclusions derived from this first experiment on the possible role played by
gradient (or ponderomotive) forces at such laser intensities seem far from certain.

4. Discussion

The electron energy spectra we have reported in this paper prove that ATI is by no
means a negligible phenomenon in the multiphoton ionisation of Xe. Threshold
intensities of about 1011W cm-’ ( N = 6), and 10” W cm-2 ( N = 11) are noticeably
lower than those calculated by Gontier and Trahin (1980) who found it to be of the
1368 F Fabre, G Petite, P Agostini and M Clement

order of W cm-2 in the case of hydrogen ( N = 6). The question then arises as
to whether this is due to a specific behaviour of Xe towards ATI or if LOPT, which has
been used in the hydrogen calculation, is questionable. It may be worth noting here
that multiphoton ionisation probabilities of Xe are generally much higher than those
of hydrogen, but it is far from certain that this should have an effect on the threshold
intensity.
Another comparison can be made between multiphoton processes of the same
order, but which include or do not include ATI. Here we have observed nineteen-
and 21-photon ionisation of Xe for intensities of the order of 10” W cm-’ when
10’’ W cm-’ was required to observe ‘pure’ multiphoton ionisation of Ne ( N = 19)
and He ( N = 21) (LomprC et a1 1976). This supports the conclusion already drawn
in Agostini et a1 (1981) that multiphoton processes which include multiphoton con-
tinuum-continuum transitions are much more probable than those which do not
include such transitions. This particular feature of ATI brings to mind the comparison
with resonant multiphoton processes whose probability is also higher than that of the
non-resonant ones.
The situation is different concerning the slope measurements which gave results
compatible with LOPT predictions. However, this does not prove that LOPT is adequate
in the case of ATI processes because this type of measurement, subject to a number
of systematic errors, is not accurate enough to detect higher-order effects which could
be less dramatic than in the case of resonant processes.
These results bring about an important question concerning earlier measurements
of slopes using ion detection. If, in these experiments, a significant part of the measured
ions were created through ATI processes, slopes higher than the one expected from
a ‘pure’ ionisation process should have been measured. However, it should be noted
that comparison between our results and earlier results of Agostini et a1 (1970) is
difficult because the latter experiment was performed with a broad band laser. More
puzzling is the case of the Lompr6 et a1 (1977) experiment where a slope of 111k0.2
was measured for the ion signal as a function of the laser intensity which was of the
order of W cm-’. Clearly, further studies of this problem are necessary to
understand these differences.

5. Conclusion

In this paper we have reported multiphoton ATI of xenon atoms. Ten-photon ionisation
at 0.53 p m and 21-photon ionisation at 1.06 p m were detected. As shown by the
linear pressure dependence of the signal, ATI is a direct, one-step process which does
not involve any collision. The intensity dependence is in agreement with the LOPT
predictions, within the experimental precision. However, the probabilities of ( N + S )
ATI for Xe are much higher than those that could be ‘extrapolated’ from a calculation
for H or Cs. An experiment currently in progress, on Cs atoms, will hopefully bring
a more quantitative comparison between theory and experiment since, for Cs, calcula-
tion seems to be reasonably possible (Aymar and Crance 1981).
When stripped from space charge and instrumental broadenings, the energy spec-
trum linewidths do not demonstrate any gradient force broadening. However, since
this broadening would have been, at most, about 0.1 eV (for I = 10” W cm-’), the
existence of the gradient force is not disproved either.
 Multiphoton above-threshold ionisation of xenon 1369

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