The line shape of Coherent Antistokes Raman Scattering excited under resonance conditions

If Coherent Antistokes Raman Scattering (CARS) is excited by a biharmonic pump in resonance with one photon molecular transition, the Raman line shape is significantly changed compared to the case of nonresonant excitation. This is due to an essential alteration of the 3rd order susceptibility responsible for CARS. Aside from a considerable enhancement of the Raman signal (which makes it possible to detect dissolved molecules in concentration lower than 10^-4 mole/l) the most marked effects are a reversal of the spectral sequence of the Raman maximum and minimum in the CARS-spectrum and for a specially chosen concentration an enhanced contrast of the signal. The factors determining the CARS line shape are discussed theoretically and preliminary experimental results concerning resonance CARS spectra are reported.