Abstract
Compared to other vdW-layered magnetic semiconductors, research on the intrinsic phonon properties of antiferromagnetic CrPS(4) is in its infancy, and elucidating these properties is crucial for unlocking its emerging applications. In this work, we combined Raman spectroscopy and first-principles calculations to thoroughly investigate the lattice vibrations of CrPS(4), uncovering its anisotropic phonon symmetry and phonon-phonon interactions. Angle-resolved polarized Raman spectroscopy was used to determine the orientation of the anisotropic CrPS(4) crystal. Temperature-dependent Raman studies revealed red shifts and line width broadening of phonon peaks with increasing temperature, indicating lattice anharmonicity. Notably, quartic-phonon scattering processes were found to dominate the broadening of high-energy phonons. Our findings provide valuable insights into the lattice vibrations of CrPS(4) and encourage further theoretical and experimental investigations of its potential thermoelectric applications.