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Soviet Journal of Quantum Electronics

Increase in nonlinear resonant susceptibility induced by polarization transfer in molecular collisions

L. T. Bolotskikh, Yu. I. Geller, A. K. Popov

Published May 31, 1980• 0 citations
Publisher

Abstract

A study is made of the influence of collisional spectral exchange on the nonlinear susceptibility of a molecular medium. It is shown that the nonlinear resonant susceptibility may increase by several orders of magnitude in the infrared and investigations of intra- and intermolecular coherence transfer in collisions are reported.
DOI
10.1070/qe1980v010n05abeh010173

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The role of collision-induced transfer of electronic state coherence on the spectral response of an atomic vapor is investigated. It is shown that such collisional effects can lead to the appearance of narrow resonances in the nonlinear spectroscopy of three-level systems. Collisional transfer between different multipoles of electronic state coherence is shown to lead to a breakdown of several percent in Becquerel's relation between the Faraday rotation and dispersion of a vapor. All calculations are carried out in the impact limit of pressure broadening theory. Particular emphasis is given to the order in which the various averages over the velocity distributions of both the active atoms and perturbers must be performed. In particular, for the effects described herein, the various collisional transfer rates vanish when averaged over the active atom velocity distribution. It is essential, therefore, to obtain the final line-shape formulas, including velocity-dependent collisional transfer rates, before carrying out the average over the active atom velocity distribution. The experimental observation of these spectral features would provide direct evidence for the existence of these collisional transfer processes.
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The effect of level degeneracy on saturated absorption in a resonant medium is considered using a simple but realistic three-level system to model $J=1\ensuremath{\rightarrow}J=0$ atomic transition. Assuming homogeneous broadening and exact resonance, an analytic nonperturbative expression for the medium susceptibility is obtained and used to study propagation of an arbitrarily polarized optical field. Optical saturation affects considerably Zeeman-coherence-induced circular dichroism. The analysis may find application in high-resolution spectroscopy and other branches of nonlinear optics.
It is shown that in order to obtain a correct interpretation of experiments on four-photon nonlinear spectroscopy within the absorption line, it is necessary to allow not only for a coherent four-photon process due to a resonant electronic nonlinearity but also for a similar process involving generation of optically induced diffraction gratings followed by the diffraction of one of the probe beams from these gratings. It is also necessary to allow for the contribution of highly excited molecular states to the resonant electronic nonlinearity. General expressions are derived and investigated for the cubic susceptibility in an isotropic medium. It is found that all nonzero components of this tensor may be expressed in terms of a single scalar function of the interacting wave frequencies. The explicit form of this function is determined in the lowest order of perturbation theory.