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Physica Scripta

Stark-shift induced resonances in multiphoton ionization

R. M. Potvliege, Svetlana Vuči

Published Sep 7, 2006• 9 citations
Publisher

Abstract

The resonance enhancements marking the ATI spectrum of argon are discussed in the light of a recently compiled map of the quasienergies of this atom. Many of the dressed excited states of interest shift nonponderomotively in complicated ways, but keep an ionization width narrow enough to produce sharp substructures of both low and high ATI peaks through Stark-shift induced resonances. The most prominent enhancement observed in the high-order ATI peaks originates from ionization from the dressed ground state perturbed by the influence of neighbouring resonant dressed states.

DOI
10.1088/0031-8949/74/4/n01

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The resonance enhancements marking the ATI spectrum of argon are discussed in the light of a recently compiled map of the quasienergies of this atom. Many of the dressed excited states of interest shift nonponderomotively in complicated ways, but keep an ionization width narrow enough to produce sharp substructures of both low and high ATI peaks through Stark-shift induced resonances. The most prominent enhancement observed in the high-order ATI peaks originates from ionization from the dressed ground state perturbed by the influence of neighbouring resonant dressed states.
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.
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.
Two investigations are reported on the application of resonantly enhanced multiphoton ionization (RMPI) to gaseous mixtures of an atomic vapor and a few Torr of argon. Photon fluxes large enough to ionize atoms by RMPI were produced by focussing down the light from a tunable pulsed dye laser. The irradiances generated were of the order of 500MWcm⁻². Ionization was detected by a voltage biased wire electrode that simply collected the photoelectrons either directly or after some gas multiplication. One investigation was the measurement of the dependence of RMPI processes in mercury on the polarization of the incident light for comparisons with theoretical calculations. The processes were four-photon resonant absorptions to either a ¹S₀ or ¹’³D₂ level followed by single photon ionization. Complete photoionization of all atoms excited to the resonant levels is established and the measured polarization dependences are found to agree with the calculated polarization dependence for the resonant excitation step of the RMPI process. Unexplained observations of the distortions in the polarization dependence of the ion yield and the absorption linewidth of the 6d ¹D₂ resonance are discussed. The second investigation was a study of the density dependent electric dipole forbidden two-photon resonant transition ²S → ²P in three-photon RMPI spectra of the Rydberg states of potassium. Stark interactions are shown to be unlikely and too weak. From the characteristics of the spectra, the excitation process is identified as a laser-assisted collision interaction.
We present results from a time-dependent two-level-plus-continuum model of multiphoton ionization in order to better understand the short-pulse photoelectron spectrum resulting from multiphoton ionization and the role of intermediate states. Both resonant and nonresonant population transfer to the upper state are found to play an important role in the multiphonon ionization process. The dynamic modeling reveals the potential for broadening and shifting peaks in the photoelectron spectrum. However, we conclude that despite the complex dynamics of the excitation, short-pulse photoelectron spectra can be used to measure ac Stark shifts of both ponderomotively and nonponderomotively shifted states in strong laser fields.