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Journal of Physics B Atomic and Molecular Physics

Interpretation of short-pulse resonant ionisation in Cs I

Michele Crance

Published Nov 28, 1979• 3 citations
Publisher

Abstract

By using the effective-operators method, an interpretation of the four-photon 6f-resonant ionisation of Cs I is presented for picosecond pulsed excitation. Theoretical calculations are compared with recently published experimental results. The predictions of several authors when applied to this particular case are discussed.
DOI
10.1088/0022-3700/12/22/013

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Journal of Physics B Atomic and Molecular Physics•Aug 14, 1978•7 citations
Presents the first application to a physical case of the effective-operators method introduced by Armstrong, Beers and Feneuille (1975) to interpret resonant multiphoton ionisation. In particular, the four-photon ionisation of Cs I near the 6f resonance is considered. Atomic quantities needed for the evaluation of effective operators are obtained by using a non-relativistic central-potential model. Theoretical results are compared with experimental data recently obtained by Morellec, Normand and Petite (1976). Taking into account the uncertainty of the measurements, the main experimental features and, in particular, the shapes of the resonance curves are reproduced well by the calculation described here.
A previously presented narrow-bandwidth theory is used to interpret recent data on the four-photon ionization of Cs near the 6F6F6F resonance. The theory is based on treating the amplitude of the radiation field as a constant relative to its rapid phase oscillations. The ionization rate adiabatically follows a pulsed amplitude leading to maximum ionization for times at which the pulse develops sufficient intensity to shift the $6S\ensuremath{\rightarrow}6F$ transition into resonance.
For pt.I see ibid., vol. 17, p.4643 (1984). The authors apply the theoretical results obtained in a previous paper in order to study the two-photon resonant ionisation of atomic caesium in the neighbourhood of the fine-structure doublet 7P 1/2 -7P 3/2 when the incident light is right-hand circularly polarised. This formalism allows one to consider these two resonant states on an equal footing and it includes the effects of the infinite summations involved in higher-order perturbation theory. The numerical results show that the two-photon resonant ionisation of caesium takes place through an anticrossing of levels, at least in the intensity range studied. The temporal behaviour of the probability exhibits two distinct temporal regimes: linear for long interaction times and cubic for the shorter ones. The intermediate regime is characterised by quantum beats. At high intensity values, it is found that the induced light shift of the resonances is time dependent. It is also shown that the contribution of the higher-order effects may explain the slight departures between the theoretical and experimental results in the off-resonant two-photon ionisation of atomic caesium.
Four-photon ionisation of caesium requires strong electromagnetic fields and the usual interpretation in terms of generalised cross sections has to be questioned. A theoretical calculation in the experimental conditions of a recent measurement provides a new interpretation of the results of Morellec and Normand (1979): the effect of light shifts masks the effect of saturation and leads one to overestimate the multiphoton ionisation cross section. The expected overestimation is only 25 per cent for the quoted experiment, but could be larger in some other physical cases.