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1.
J Phys Chem Lett ; 13(18): 4015-4020, 2022 May 12.
Article in English | MEDLINE | ID: mdl-35485838

ABSTRACT

Low-frequency shear and breathing modes are important Raman signatures of two-dimensional (2D) materials, providing information on the number of layers and insights into interlayer interactions. We elucidate the nature of low-frequency modes in a 2D polar metal-2D Ga covalently bonded to a SiC substrate, using a first-principles Green's function-based approach. The low-frequency Raman modes are dominated by surface resonance modes, consisting primarily of out-of-phase shear modes in Ga, coupled to SiC phonons. Breathing modes are strongly coupled to the substrate and do not give rise to peaks in the phonon spectra. The highest-frequency shear mode blue-shifts significantly with increasing thickness, reflecting both an increase in the number of Ga layers and an increase in the effective interlayer force constant. The surface resonance modes evolve into localized 2D Ga modes as the phonon momentum increases. The predicted low-frequency modes are consistent with Raman measurements on 2D polar Ga.

2.
Adv Mater ; 33(36): e2101618, 2021 Sep.
Article in English | MEDLINE | ID: mdl-34302389

ABSTRACT

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.

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