Resonance Raman scattering and anomalous anti-Stokes phenomena in CrSBr

CrSBr, a van der Waals material, stands out as an air-stable magnetic semiconductor with appealing intrinsic properties such as crystalline anisotropy, quasi-1D electronic characteristics, layer-dependent antiferromagnetism, and non-linear optical effects. We investigate the differences between the absorption and emission spectra, focusing on the origin of the emission peak near 1.7 eV observed in the photoluminescence spectrum of CrSBr. Our findings are corroborated by excitation energy-dependent Raman experiments. Additionally, we explore the anti-Stokes Raman spectra and observe an anomalously high anti-Stokes-to-Stokes intensity ratio of up to 0.8, which varies significantly with excitation laser power and crystallographic orientation relative to the polarization of the scattered light, highlighting the unique vibrational and electronic interactions in CrSBr. Lastly, we examine stimulated Raman scattering and calculate the Raman gain in CrSBr, which attains a value of 1 × 108 cm GW-1, nearly four orders of magnitude higher than that of previously studied three-dimensional systems.