Resonant coherent hyper-Raman scattering (CHRS). II. A theory on the general relationship between CHRS and coherent Raman scattering (CRS) processes

A theoretical description of the resonant coherent hyper-Raman scattering for an arbitrary system-bath interaction is presented. Particularly the relationship between the coherent hyper-Raman scattering (CHRS) and coherent Raman scattering (CRS) signals is established without alluding to any specific model of optical broadening. The permanent dipole moment difference between the excited and ground states of a given chromophore is shown to be proportional to the ratio of the CHRS to CRS signals, and it is proved that this result is valid regardless of the model for the chromophore-bath interaction.