Abstract

AbstractThe theory of the hyper‐Raman effect in molecular gases is reviewed. In order to calculate relative intensities of vibration‐rotation lines in hyper‐Raman spectra, line strengths are introduced and these are calculated using the method of irreducible spherical tensors. It transpires that the hyper‐Raman effect caused by scattering of a quasi‐monochromatic light beam can be fully described by five independent line strength expressions. Rotational and vibrational selection rules as well as depolarization ratios for linearly, circularly and naturally polarized incident light are derived and discussed. The angular dependence of the scattered intensity is also given in the form of polar diagrams. To some extent the paper presented here parallels that published by Placzek and Teller54 in 1933 on the rotational structure of vibrational bands in conventional Raman spectra caused by a spontaneous two‐photon scattering process.

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