Coherent Raman Scattering Spectral Shapes in a Strong Excitation Regime (Model Calculations)

The influence of the interference between coherent processes in third-order nonlinear Raman scattering on the spectral shapes of Raman-scattered light waves is numerically modeled and discussed in the cases of commonly used coherent Raman spectroscopy techniques. The effects on the lineshapes depending on the laser intensity are analyzed for the coherent Raman spectroscopy performed via the excitation of molecular systems with focused laser pulses at high intensities. In this case, the interplay between the coherent processes in nonlinear Raman scattering, as well as laser power-induced resonance effects, may be significant and should be taken into account in the spectral lineshape analysis in coherent Raman spectroscopy and its related applications, since the coherent Raman spectra may be considerably modified.