Lattice Vibration, Raman Modes and Room-Temperature Spin-Phonon Coupling in Intrinsic 2D van der Waals Ferromagnetic Fe3GaTe2

Abstract: Two-dimensional (2D) van der Waals (vdW) magnets with spin-phonon coupling are crucial for next-generation spintronics. Among them, Fe3GaTe2 has attracted widespread attention due to above-room-temperature intrinsic ferromagnetism and large perpendicular magnetic anisotropy. However, the lattice vibrations and the interplay between ferromagnetism and lattice vibrations in Fe3GaTe2 are still unexplored. Here, we report the lattice vibration, Raman modes, and room-temperature spin-phonon coupling in 2D Fe3GaTe2 with above-room-temperature Curie temperature (TC). Two typical Raman modes with out-of-plane lattice vibrations are identified: "A" _"1g" ^"1" and "A" _"1g" ^"2" , whose frequencies increase as the thickness decreases from bulk to 2D Fe3GaTe2 due to the weakening of interlayer vdW interactions and spin exchange coupling. Moreover, the difference between phonon band dispersions under ferromagnetic and nonmagnetic interlayer spin ordering indicates the existence of spin-phonon coupling. The phonon frequency diverges from the anharmonic model below TC and thus the strength of spin-phonon coupling is ~0.28 cm-1 at 300 K, which is the first experimental identification of room-temperature spin-phonon coupling in 2D vdW magnets. This work deepens the understanding of novel 2D vdW magnets and provides a basis for spintronic applications at and above room temperature.