Theory of resonant Raman scattering. II. Overtones and hot bands

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Abstract
Resonant Raman scattering is discussed in the framework of the Green’s function method in both the strong and weak vibronic coupling limits. We further elaborate on the meaning of each matrix element of the Green’s function, evaluated in the convenient basis set which is commonly referred to as the Longuet–Higgins representation. Cross sections for absorption, Rayleigh, Raman fundamentals, Raman overtones, hot bands, etc., can all be related to the matrix elements of the Green’s function. It is further emphasized that only in the vibronic view elaborated here does a simple and direct correlation exist between the light scattering processes and the Green’s functions. Some typical excitation profiles for overtones and hot bands are calculated and the consequences of strong vibronic couplings are discussed in contrast to the weak vibronic coupling case.

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