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It is shown that the Raman line-shape function and/or vibrational dephasing times can reflect random frequency modulation of high-frequency vibrational modes via exchange with low-frequency modes. When exchange is incorporated into the vibrational correlation function, lifetimes and scattering rates between modes can be quantitatively determined from the temperature dependence of the spontaneous Raman spectrum. Finally, some experimental results on vibrational redistribution are presented which demonstrate the salient features of the theory.
Harris et al. (Mon,) studied this question.