Vibrational mode-specific polarization effect in circularly polarized stimulated Raman scattering

As one of the popular coherent Raman scattering techniques, stimulated Raman scattering (SRS) has made significant progress in recent years, especially in label-free biological imaging. Polarization provides an additional degree of freedom to manipulate the SRS process. In previous studies, only linearly polarized SRS was fully investigated, in which both pump and Stokes laser fields are linearly polarized. Here, we theoretically analyzed the SRS process excited by two circularly polarized laser fields and then experimentally demonstrated it by taking a spherical symmetric CH₄ molecule as a model system. The experimental results are in good agreement with the theoretical ones. It is shown that circularly polarized SRS (CP-SRS) has unique characteristics different from linear polarization. When the handedness of circular polarization states of two laser fields is the same, CP-SRS further suppresses the depolarized vibrational band while keeping the polarized band almost unaffected. On the other hand, when the handedness is opposite, CP-SRS enhances the depolarized band while suppressing the polarized band. Therefore, the CP-SRS not only allows us to resolve the symmetry of vibrational modes but also can enhance vibrational contrast based on symmetry selectivity by suppressing or enhancing the signal from a specific vibrational mode. These results will have potential applications in improving chemical selectivity and imaging contrast as well as spectral resolution SRS microscopy. In addition, the CP-SRS has the ability to determine the depolarization ratio ρ and identify the overlapping Raman bands.