Abstract Semiconducting CrSBr is a layered A-type antiferromagnet, with individual layers antiferromagnetically coupled along the stacking direction. Due to its unique orthorhombic crystal structure, CrSBr exhibits highly anisotropic mechanical and optoelectronic properties acting itself as a quasi-1D material. CrSBr demonstrates complex coupling phenomena involving phonons, excitons, magnons, and polaritons. Here we show through polarization-resolved resonant Raman scattering the intricate interaction between the vibrational and electronic properties of CrSBr. For samples spanning from few-layer to bulk thickness, we observe that the polarization of the $${{\rm{A}}}_{g}^{2}$$ A g 2 Raman mode can be rotated by 90 degrees, shifting from alignment with the crystallographic a (intermediate magnetic) axis to the b (easy magnetic) axis, depending on the excitation energy. In contrast, the $${{\rm{A}}}_{g}^{1}$$ A g 1 and $${{\rm{A}}}_{g}^{3}$$ A g 3 modes consistently remain polarized along the b axis, regardless of the laser energy used. We access real and imaginary parts of the Raman tensor in our analysis, uncovering resonant electron-phonon coupling.

Kevin Hagmann

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