Manipulation of coherent Raman scattering process in CS2 byusing chirpped circularly polarized femtosecond pulses

Abstract

The coherent anti-Stokes Raman scattering (CARS) and coherent Stokes Raman scattering (CSRS) signals of vibration mode at 397cm-1 of CS2 liquid are manipulated by using two chirped circularly polarized femtosecond pulses in non-collinear excitation geometry. Along the phase matching direction intensity distributions, polarizations and wavelengths of CARS and CSRS signals vary regularly as the polarizations of the laser beams are changed. The intensity distributions of CARS and CSRS reflect the scattering cross sections of the stimulated raman scattering of the sample under different circularly polarizations. The polarizations of CARS and CSRS follow the conservation law of the angular momentum of the excitations. The frequency shifts of CARS and CSRS demonstrate the transitions between the rotational energy levels of CS2. The above information is helpful for understanding the mechanism and the behaviors of the CARS and CSRS of CS2 as well as other molecules.