Abstract
The authors use the time-dependent theory of Raman scattering to investigate, both semiclassically and quantum mechanically, the effects of nonconstant transition dipoles on Raman excitation profiles and total Raman emission spectra. The system with a single excited electronic state dominating the scattering process is studied. Semiclassical analytic formulas are derived that can be used to obtain information of the transition dipole and the excited-state surface. Depending on the parameters, significant deviations from the previous works on the Raman scattering, where the constant transition dipole (Condon approximation) was invoked, are observed.
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