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CrSBr, a van der Waals material, stands out as an air-stable magneticsemiconductor with appealing intrinsic properties such as crystallineanisotropy, quasi-1D electronic characteristics, layer-dependentantiferromagnetism, and non-linear optical effects. In this study, weinvestigate the differences between the absorption and emission spectra,focusing on the origin of the emission peak near 1.7 eV observed in thephotoluminescence spectrum of CrSBr. Our findings are corroborated byexcitation-dependent Raman experiments. Additionally, we explore theanti-Stokes Raman spectra and observe an anomalously high anti-Stokes to Stokesintensity ratio of up to 0.8, which varies significantly with excitation laserpower and crystallographic orientation relative to the polarization of thescattered light. This ratio is notably higher than that observed in graphene($\approx$ 0.1) and MoS$_2$ ($\approx$ 0.4), highlighting the uniquevibrational and electronic interactions in CrSBr. Lastly, we examine stimulatedRaman scattering and calculate the Raman gain in CrSBr, which attains a valueof 1 $\times$ 10$^{8}$ cm/GW, nearly four orders of magnitude higher than thatof previously studied three-dimensional systems.

Resonance Raman Scattering and Anomalous Anti-Stokes Phenomena in CrSBr