On the spectra of resonant coherent Raman scattering

The spectra of resonant coherent anti-Stokes and Stokes Raman scattering of excited molecules are calculated and discussed. The interaction of light and molecules is treated semi-classically. The energy level diagram of four energy levels describing the process is used in four modifications possible for excited molecules. It is shown that non-vibrational resonances give extra maxima in some of the spectra. Comparison of the spectral structure in the Stokes and anti-Stokes components gives information on which of the four schemes the interaction is realized by. The influence of the pumping detuning on the Stokes component shape is pointed out.