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Journal of Physics B Atomic and Molecular Physics

The AC Stark shift as an intensity probe in resonant multiphoton ionisation of xenon

P Kruit, J. Kimman, Harm Geert Muller, Marnix J. van der Wiel

Published Mar 28, 1983• 43 citations
Publisher

Abstract

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.

DOI
10.1088/0022-3700/16/6/011

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Journal of Physics B Atomic and Molecular Physics•Oct 28, 1984•15 citations
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.
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.
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 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.
For pt.I see ibid., vol.17, p.4135 (1984). Using a previously described new method to evaluate light-induced level shifts, it is experimentally demonstrated that the two possible intermediate 6D 2 states in four-photon resonant five-photon ionisation of mercury are mixed at high laser intensities. Due to this mixing, the AC Stark shifts of these levels are no longer quadratic in field amplitude. This is in good agreement with a simple theoretical model. This makes a direct determination of the oscillator strengths for two mercury lines possible.
A new analytical treatment is developed for resonant multiphonon ionisation which takes into account the physical properties of the exciting laser such as the spatial intensity distribution of a focused Gaussian beam and light statistics effects in the narrow bandwidth limit. The ion number as a function of laser intensity and wavelength follows a 'displacement law', which means that it may be expressed as a single variable function and provides a more reliable way to determine light-induced level shifts than previous methods. Three-photon resonant five-photon ionisation of mercury in a chaotic field serves as an experimental test and agrees excellently with the displacement law. However, the derived dynamical Stark shift differs by about a factor of three from that calculated from currently known oscillator strengths.