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Journal of Physics B Atomic and Molecular Physics

Raman-enhanced multiphoton ionisation

R. Parzyński

Published Oct 14, 1987• 6 citations
Publisher

Abstract

Two-laser multiphoton ionisation under the autoionising-like resonance condition is studied theoretically within an extended atomic model dictated by the experiment of Feldmann et al (1986). Ordinary coupling between a selected pair of bound states via the continuum only is supplemented in the author's model by Raman-type coupling involving the atomic spectrum below the ionisation threshold. In the case considered this additional Raman coupling enhances the ionisation rate to a much greater extent than the coupling via the continuum can do. The Raman coupling modifies the autoionising-like shape parameter and is decisive as far as the resonance peak profile is concerned. Exploiting this Raman coupling within the atomic model with four effective bound states, the author gives explanations for all the details of the ionisation spectrum detected by Feldmann et al, i.e. the number of resonance peaks, their strength, fine structure, shape, relative heights and sensitivity to the laser field.

DOI
10.1088/0022-3700/20/19/015

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Two-laser multiphoton ionisation under the autoionising-like resonance condition is studied theoretically within an extended atomic model dictated by the experiment of Feldmann et al (1986). Ordinary coupling between a selected pair of bound states via the continuum only is supplemented in the author's model by Raman-type coupling involving the atomic spectrum below the ionisation threshold. In the case considered this additional Raman coupling enhances the ionisation rate to a much greater extent than the coupling via the continuum can do. The Raman coupling modifies the autoionising-like shape parameter and is decisive as far as the resonance peak profile is concerned. Exploiting this Raman coupling within the atomic model with four effective bound states, the author gives explanations for all the details of the ionisation spectrum detected by Feldmann et al, i.e. the number of resonance peaks, their strength, fine structure, shape, relative heights and sensitivity to the laser field.
The author predicts that bound atomic or molecular states can be dressed by an applied field in a fashion analogous to the pseudo-autoionising structure induced in a photoionising continuum. Just as the continuum structure can enhance the photoionisation rate, the induced virtual structure between real states can be used to enhance multiphoton processes by tuning one of the intermediate fields near this virtual resonance. The author concentrates on stimulated Raman scattering, but the connection to multiphoton absorption is pointed out.
In a recent experiment involving multiphoton ionisation of Xe it was found that the photoelectron spectrum contained peaks which corresponded to absorption of more than the minimum number of photons required ionise. The effective orders of nonlinearity, furthermore, showed a striking uniformity. The authors investigated these effects with a model approximation consisting of a single bound state and m continua. Simple analytic expressions are obtained for the quantity measured in the experiment and the limit m to infinity is obtained. The results show good qualitative agreement with experiment.
Atoms in an autoionisation state can be excited to higher states in the continuum as well as performing spontaneous transitions to bound states by laser-induced autoionisation. Both effects are investigated by means of the reaction matrix. Results obtained by Armstrong et al (1978) using the same method are extended. The shape of the photoelectron spectrum is different from that of the photon spectrum emitted from the autoionisation state but is similar to that of the photon spectrum emitted from the same bound state which is excited to the ionisation states in the former case. It is predicted that the shape of the fluorescence yield with the pump laser detuning is Lorentzian. The multiphoton process contributes to the photoelectron spectrum in a complicated way.
The authors study doubly resonant multiphoton ionisation induced by two laser fields. The first field produces a near-resonant multiphoton transition between the ground state g and a discrete state 0. The second field is nearly resonant with a one-photon transition between 0 and an autoionising state 1. The spontaneous emission of both excited states is taken into account. The authors discuss and compare the spectral profiles expected for ionisation probability and fluorescence from state 1 when the first step laser is scanned.