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Journal of Physics B Atomic Molecular and Optical Physics

Contrasted behaviour of Stark-induced resonances in multiphoton ionization of krypton

E. Mével, P. Breger, Rusty P. Trainham, G. Petite, Pierre Agostini, J. P. Chambaret, A. Migus, A. Antonetti

Published Sep 14, 1992• 19 citations
Publisher

Abstract

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.

DOI
10.1088/0953-4075/25/17/001

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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.
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 levels of atoms and molecules exposed to intense, short, high-frequency laser pulses undergo time-dependent distortion known as dynamic Stark shift (DSS). These level shifts are induced by the coupling with nonresonant (nonessential) states and follow the temporal intensity profile of the laser pulse. Owing to the different DSSs of the individual atomic levels, transient resonance suppressions and enhancements significantly modify the multiphoton ionization pathway, leaving clear fingerprints (asymmetry, splitting, and shifting) in the energy spectrum of emitted photoelectrons. Here we investigate this phenomenon by solving the time-dependent Schr\"odinger equation of the valence electron of Na and Li in increasing levels of complexity: (i) developing minimal models for two-photon transition and (2+12+12+1)-photon ionization, (ii) applying a spectral method without continuum-continuum couplings, and (iii) propagating the electron wave packet on a large spatial grid accounting for all possible couplings. We show that appropriately detuned transform limited pulses provide a high level of control in strong-field excitation, when the atomic levels are dynamically shifted. Furthermore, we demonstrate the role of DSSs in the multipeak structure of the Autler-Townes doublet, found when several Rabi oscillations are induced during the strong-field resonant ionization.
Multiphoton ionization of krypton has been experimentally investigated for the first time with a single-mode tunable Nd3+{\mathrm{Nd}}^{3+}Nd3+: glass laser producing an electric field of $E=8\ifmmode\times\else\texttimes\fi{}{10}^{7}$ V/cm. In the range 10 585 \AA{} to 10 605 \AA{}, two resonances have been found, shifted towards the high-energy side from the nearest states 5d[12]15d{[\frac{1}{2}]}_{1}5d[21​]1​ and $4{d}^{\ensuremath{'}}{[\frac{5}{2}]}_{3}$ by 39.5 ${\mathrm{cm}}^{\ensuremath{-}1}$ and 42 ${\mathrm{cm}}^{\ensuremath{-}1}$, respectively. Far from resonances, the dependence of the ionization rate on the laser intensity agrees with the lowest-order perturbation-theory prediction.
We present experimental and theoretical data on the electron energy spectra from resonance-enhanced multiphoton ionization of atoms. In experiments performed with 594-nm wavelength, linearly polarized laser pulses of 300-fs and 600-fs durations, it is found that excitation of the intermediate resonances during the rising edge of the laser pulse can dominate the electron spectrum. Good agreement is found between the experimental results and a model based on the Landau-Zener energy level crossing theory. Theoretical results obtained with direct integration of the Schrödinger equation show that intermediate resonances can be excited appreciably off resonance if the coupling between the ground state and the excited state is highly nonlinear. The excitation of the intermediate state is not localized at the intensity which makes it six-photon resonant with the ground state. A multilevel model used to simulate the experimental spectra, based on direct integration of the Schrödinger equation, shows excellent agreement with the data.