Chiral Phonons and Giant Magneto‐Optical Effect in CrBr₃ 2D Magnet

Phonons with chirality determine the optical helicity of inelastic light scattering processes due to their nonzero angular momentum. Here it is shown that 2D magnetic CrBr₃ hosts chiral phonons at the Brillouin-zone center. These chiral phonons are linear combinations of the doubly-degenerate Eg phonons, and the phonon eigenmodes exhibit clockwise and counterclockwise rotational vibrations corresponding to angular momenta of l = ± 1. Such Eg chiral phonons completely switch the polarization of incident circularly polarized light. On the other hand, the non-degenerate non-chiral Ag phonons display a giant magneto-optical effect under an external out-of-plane magnetic field, rotating the plane of polarization of the scattered linearly polarized light. The corresponding degree of polarization of the scattered light changes from 91% to -68% as the magnetic field strength increases from 0 to 5 T. In contrast, the chiral Eg modes display no field dependence. The results lay a foundation for the study of phonon chirality and magneto-optical phenomena in 2D magnetic materials, as well as their related applications, such as the phonon Hall effect, topological photonics, and Raman lasing.