Abstract

A stochastic theory of the nonliner susceptibility χ(3) is used to analyze coherent and spontaneous Raman spectra of polyatomic molecules in solution. The theory holds for any solvation time scale and interpolates between the homogeneous limit, in which the Bloch equations are valid, and the static limit of inhomogeneous line broadening, as the solvent time scale is increased. Application is made to β-carotene in alkanes and in CS2. The calculated spontaneous Raman profiles are found to be in good agreement with experiment, and the coherent Raman excitation profiles are predicted. The magnitude of the solvent–solute interaction and the solvation time scale for various solvents are obtained from our theoretical analysis. The relative contribution of inhomogeneous line broadening in isopentane is found to increase as the temperature is raised from 118 to 298 K.

© 1988 Optical Society of America

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