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The dichroism and birefringence effects in stumulated Raman scattering (SRS)in polyatomic molecules were studied theoretically. General expressions havebeen derived describing the change of the intensity and polarization of theprobe pulse after transmission through a solution of arbitrary polyatomicmolecules for any initial polarization of each of the laser pulses. Theexpressions were written in terms of spherical tensor operators that allowedfor separation of the both beams polarization matrices and the material partcontaining three scalar values of nonlinear optical susceptibility where thatrank K is limited to the values K=0,1,2. The expressions are valid forarbitrary directions of propagation of both pump and Stokes light beams andarbitrary polarizations of both beams. The expressions contain contributionsfrom linear dichroism and birefringence in the molecular excited states. It wasshown that, under certain conditions, both effects can be observedsimultaneously. The geometry of almost collinear propagation of the pump andStokes pulse beams through the molecular sample was considered, and it wasshown that the contributions from linear dichroism and birefringence to thesignal can be completely separated in the experiment by means of an appropriatechoice of a probe beam polarization analyzer placed in front of thephotodetector. The expressions obtained were used to describe the signalsobtained using the polarization-modulation technique developed recently by theauthors (Gorbunova et al, Phys. Chem. Chem. Phys. 2020, Vol. 22, 18155-18168).It was shown that the modulated dichroism and birefringence signals could beobserved in quadrature to the second harmonic of the modulated referencesignal.

Probe Beam Dichroism and Birefringence in Stumulated Raman Scattering of Biologically Relevant Polyatomic Molecules