Probe Beam Dichroism and Birefringence in Stimulated Raman Scattering in Polyatomic Molecules

Abstract

Dichroism and birefringence in Stimulated Raman Scattering (SRS) in polyatomic molecules were studied theoretically. General expressions describing the change of the polarization matrix of the probe laser beam transmitted through initially isotropic molecular sample excited by the pump laser beam have been derived. Arbitrary polarization states and propagation directions of the incoming pump and probe beams were considered. The expressions were written in terms of spherical tensor operators that allowed for separation of the field polarization tensor and the molecular part containing three scalar values of nonlinear optical susceptibility χ(3)Kpu with Kpu = 0,1,2. The geometry of almost collinear propagation of the pump and probe beams through the molecular sample was considered in greater details. It was shown that the dichroism and birefringence refer to the nonlinear optical susceptibility element χ(3)2 and that their contributions to the SRS signal can be separated experimentally by using an appropriate probe beam polarization analyzer installed in front of the photodetector. Particular cases of the off‐resonant SRS and resonant SRS have been considered. The results obtained were expressed in terms of the Stokes polarization parameters of the pump and probe beams.