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Journal of the Optical Society of America B

Ac Stark shifts induced by a YAG laser in the nP and nF Rydberg series in xenon

Didier Normand, Louis A. Lompre, Anne L’Huillier, J. Morellec, Michel Ferray, J. Lavancier, G. Mainfray, C. Manus

Published Aug 1, 1989• 39 citations
Publisher

Abstract

Nonresonant ac Stark shifts of Rydberg states in Xe have been investigated by probing an atomic transition with a weak UV light in the presence of an intense YAG-laser pulse. Rydberg atoms produced through two-photon excitation, 5p → np (n = 15–48) and 5p → nf (n = 12–49), are subsequently ionized. IR-laser-induced shifts of the resonant ionization profiles are then measured. The measured shift, 3.9 ± 0.3 cm−1 at 1010 W cm−2, is more than a factor of 2 smaller than that expected from the basis of ponderomotive term, 8.5 cm−1 at 1010 W cm−2. In addition, the shift varies linearly as a function of the IR-laser intensity and does not depend on the principal quantum number of the np and nf series investigated here.

DOI
10.1364/josab.6.001513

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Nonresonant ac Stark shifts of Rydberg states in Xe have been investigated by probing an atomic transition with a weak UV light in the presence of an intense YAG-laser pulse. Rydberg atoms produced through two-photon excitation, 5p → np (n = 15–48) and 5p → nf (n = 12–49), are subsequently ionized. IR-laser-induced shifts of the resonant ionization profiles are then measured. The measured shift, 3.9 ± 0.3 cm−1 at 1010 W cm−2, is more than a factor of 2 smaller than that expected from the basis of ponderomotive term, 8.5 cm−1 at 1010 W cm−2. In addition, the shift varies linearly as a function of the IR-laser intensity and does not depend on the principal quantum number of the np and nf series investigated here.
We present a theoretical analysis of a recent experiment [ J. Opt. Soc. Am. B6, 1513 ( 1989)] on two-color three-photon ionization of Xe through resonant even-parity Rydberg states. We calculate second-order ac-Stark shifts, two-photon Rabi frequencies, and ionization widths by using wave functions obtained from a multichannel quantum-defect-theory analysis of the Rydberg series in Xe. We perform a detailed description of the experiment, using the density-matrix formalism, accounting for the temporal and spatial distributions of the laser fields. The agreement with the experiment is good except for the ac-Stark shift of the Rydberg states, which, in our calculation is close to the ponderomotive energy, whereas in the experiment it is measured to be half of this value.
The Stark spectra of autoionizing Rydberg states of Xe converging to the second ionization limit 5p5{p}^{5}p5 2P1/2^{2}P_{1/2}2P1/2​ have been investigated as a function of applied electric field over the range 26--2362 V/cm. Single-photon excitation from the Xe ground state was achieved using coherent radiation near 92.5 nm, generated by frequency tripling the pulsed output of a frequency-doubled dye laser in a free jet of rare-gas atoms. For the lowest electric field only the ns' and nd' series were observed. As the electric field was increased the np' series appeared because of the mixing of wave functions with different l values. Further increase of the electric field caused the appearance of hydrogenlike Stark manifolds. The Stark spectrum was simulated in a two-step procedure with no adjustable parameters. Using a jl-coupling basis set the Hamiltonian matrix was diagonalized to determine the energy levels and corresponding eigenfunctions for a given electric field strength. The intensities and line shapes were then calculated using the formalism developed by Fano for a many-discrete-level--single-continuum configuration interaction. This treatment was sufficient to reproduce the positions, widths, and shapes of most observed features. At field strengths between 1000 and 2000 V/cm, however, an additional modulation structure with a spacing of about 2.7 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ appeared on top of the \ensuremath{\Vert}M\ensuremath{\Vert}=1 autoionizing resonances, which could not be explained by our simple theoretical model.
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.
Neutral Rydberg state excitation in strong UV laser fields of Xe atoms has been studied and compared with direct ionization. The yields of both strong-field excitation and ionization have been measured as a function of UV laser intensity and ellipticity. The underlying physical mechanism has been discussed based on the experimental results, indicating that the Rydberg states are populated via multi-photon resonance excitation in strong 400 nm laser fields. Finally, a comparative study of Xe and O2O_2O2​ with similar ionization potentials have been performed, showing the suppressed excitation of molecules in strong UV laser fields.
In order to perform multi-photon ionization experiments at a particular light intensity, the AC Stark-shift of the xenon 6s level is used as a probe to select that intensity from the range of intensities present in the laser focus. Our analysis provides an accurate, wide-range distribution function of the intensities in our multi-mode laser pulses. Using this method we determined there al order of non-linearity of the resonant ionization process and the probability for additional photon absorption.
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.