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Journal of Physics B Atomic and Molecular Physics

Absorption of additional photons in the multiphoton ionisation continuum of xenon at 1064, 532 and 440 nm

P Kruit, J. Kimman, Marnix J. van der Wiel

Published Oct 14, 1981• 158 citations
Publisher

Abstract

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.

DOI
10.1088/0022-3700/14/19/003

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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.
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.
By focusing an excimer pumped dye laser on an atomic beam, the authors have observed multiphoton multiple ionisation of the neutral strontium atom in the tuned wavelength range 532-41 nm. Sr + and Sr ++ yields were measured with a time of flight spectrometer. At least three photons are required to produce Sr + and eight photons to produce Sr ++ . As a function of the wavelength, the Sr + yield exhibits resonances which correspond to two-photon excitation of bound states (5s 2 -5p 2 1 D 2 and 5s 2 -5p 2 1 S 0 ) and three-photon excitation of autoionising states 4d5f J=1 and J=3 of the neutral atom. The Sr ++ yield exhibits four broad smooth resonances that they interpret, from known spectroscopic data, as two-photon (5p 1/2 -4f), three-photon (5s-6p 1/2, 3/2 ) and four-photon (5s-7d) resonances in the singly charged ion. The latter transitions start from a singly charged ion in the 5s or 5p 1/2 state reached after three- or four-photon ionisation of the neutral ground state. The variation of the Sr ++ pattern as a function of the dye laser beam intensity shows that resonances are shifted and broadened when the intensity is increased. These features have been interpreted by a perturbative treatment of Sr + ionisation based on the use of an effective Hamiltonian which takes into account higher-order terms involved in the calculation of resonance effects. Calculated multiphoton ionisation probabilities are in good agreement with experimental data.