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Journal of Physics B Atomic and Molecular Physics

Enhancement of off-resonant stimulated Raman scattering

David A. Cardimona

Published Jan 14, 1987• 29 citations
Publisher

Abstract

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.

DOI
10.1088/0022-3700/20/1/021

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•Jan 1, 1982•0 citations
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.
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 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.
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
Stimulated electronic Raman scattering, SERS, is a simple method of efficiently generating widely tunable infrared radiation. This work describes techniques by which the tuning capability of this process may be extended. To this end several schemes in Caesium and Barium vapours have been investigated. In Barium vapour two Raman transitions were studied using fixed frequency lasers. Poor performance of one of these transitions led to the application of biharmonic pumping or 'coherent Raman mixing' to enable generation of infrared light, and was the first observation of this process in an atomic vapour. This technique was subsequently used to generate infrared light from tunable dye laser light, which gave continuous tuning from 1.16µm to 1.5µm. The process was found to be limited by atomic saturation. The effect which saturation has on the generation efficiency is considered theoretically, and predicts quite accurately the observed tuning behaviour. Two methods aimed at reducing molecular absorption effects in SERS in alkali vapours were investigated. The techniques employed either laser excitation and dissociation of the molecules or a reduction in their ground state concentration by superheating of the vapour. Some degree of success was achieved in improving the available tuning from the 6s-7s transition in Caesium. However, the inclusion of the effect of collision broadening of atomic transitions into a calculation of the Raman threshold suggests that little further improvement can be obtained on this transition. A direct measurement of the Raman threshold power on the 6s-5d5/2 transition in Caesium gave excellent agreement with theoretical predictions based on collision broadening of this Raman transition. In addition, this work gave an insight into the role photoionization plays in increasing the threshold under certain circumstances. The analysis suggests that laser pulse duration and vapour column length are important in determining whether Raman threshold can be exceeded.