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Journal of Physics B Atomic Molecular and Optical Physics

Resonant multiphoton ionisation of xenon with high-intensity femtosecond pulses

Pierre Agostini, A. Antonetti, P. Breger, Michele Crance, A. Migus, Harm Geert Muller, G. Petite

Published Jun 28, 1989• 53 citations
Publisher

Abstract

The authors report on the intensity and polarisation dependences of electron energy spectra from multiphoton ionisation of xenon with 120 fs pulses at 615 nm. The spectra show a large number of narrow structures assigned to resonances induced by the AC Stark shift. The structures are suppressed with circular polarisation. The maximum shift is observed for the 6s state which is up-shifted by 1.6 eV. The assignments are based on a lowest-order perturbative calculation of the AC Stark shifts.

DOI
10.1088/0953-4075/22/12/012

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The authors report on the intensity and polarisation dependences of electron energy spectra from multiphoton ionisation of xenon with 120 fs pulses at 615 nm. The spectra show a large number of narrow structures assigned to resonances induced by the AC Stark shift. The structures are suppressed with circular polarisation. The maximum shift is observed for the 6s state which is up-shifted by 1.6 eV. The assignments are based on a lowest-order perturbative calculation of the AC Stark shifts.
The authors report a high-resolution electron spectroscopic study of three-photon resonant, five-photon ionisation of xenon. The results are analysed in terms of a dynamic resonance of three photons with an AC Stark-shifted intermediate level (6s), followed by a saturated two-photon transition to the continuum. They demonstrate a linear relationship between detuning from the zero-field resonance position and the local momentary light intensity causing the five-photon ionisation. Thus, the AC Stark shift acts as a probe which selects a particular intensity from the wide range present in the laser focus. They determined the AC Stark shift of the 6s level the distribution function of the light intensities and the intensity dependence of the ionisation probability. High-resolution electron spectra are used in arguments to support the validity of their analysis.
As it is well known now1, electron energy spectra from multiphoton ionization (MPI) and Above-Threshold Ionization (ATI) of atoms by subpicosecond pulses reveal Stark-induced resonances and provide an elegant and unique method to investigate AC-Stark shifts of strongly perturbed excited states. In this work we have systematically studied such spectra and their interpretation in the case of MPI of Rare gases with 100 fs, 617 nm pulses. The intensity ranges from 1013 (for xenon) to 1015 W.cm−2 (for helium). The corresponding shifts range from .3 eV to 30 eV and may be, in principle, larger than the atomic ionization potential. Besides the measurement of AC-Stark shifts, the photoelectron spectra provide valuable information about the ionization process itself in a highly non-perturbative regime.
The energy spectrum of electrons produced by multiphoton ionisation of xenon atoms has been measured, using a new type of electron energy analyser with an acceptance angle of 2 pi sr. Absorption of additional photons above the minimum number required for ionisation has been observed in the non-resonant as well as in the resonant multiphoton ionisation process. In the resonant proces the AC Stark shift is used to link wavelength detuning to the light intensity, in order to find the probability of extra photon absorption as a function of light intensity.
Electron energy spectra from multiphoton ionization of krypton with 617 nm, 70 fs pulses have been recorded over a large intensity range. Near the appearance intensity, the spectra display Stark-induced resonances with s and d states. Up to about 8*10 13 W cm -2 , the spectra broaden and the structures are progressively washed out. Above this intensity, a strong resonance emerges, corresponding to the 4f state for which the static detuning is 2.94 eV, a value larger than the photon energy. The influence of a large static detuning and populations of excited states with shifts different from the threshold shift are discussed.
An electron spectroscopic study is reported of multiphoton ionisation of Xe and Cs using two laser beams. One of the two beams is tuned to multiphoton resonance with an intermediate state and causes a considerable AC Stark shift. The second beam acts as a probe of the population and shift of the intermediate state. In Xe the authors deal with a three-photon resonance with the 6s level ( lambda approximately=440 nm); in Cs with two-photon resonances with Rydberg levels of the nd series. As probes, beams of either lambda =1064 or 532 nm have been used.
We present photoelectron spectra measured by `short' pulse ( ps) MPI of xenon at 526.5 nm excitation wavelength in the intensity range to . Ionization into and channels is observed and resonance structures are found in both ionization channels. They are induced by the AC Stark shift of bound Xe states within the light pulse which brings them into transient n-photon resonance with the Xe ground state. The resonant states are tentatively identified as d- and s-angular momentum states having AC Stark shifts which differ from the shift of the xenon ionization threshold. In the high-intensity limit, ionization into the channel is completely suppressed.