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Fe3GeTe2 has emerged as one of the most fascinating van der Waals crystalsdue to its two-dimensional (2D) itinerant ferromagnetism, topological nodallines and Kondo lattice behavior. However, lattice dynamics, chirality ofphonons and spin-phonon coupling in this material, which set the foundation forthese exotic phenomena, have remained unexplored. Here we report the firstexperimental investigation of the phonons and mutual interactions between spinand lattice degrees of freedom in few-layer Fe3GeTe2. Our results elucidatethree prominent Raman modes at room temperature: two A1g({\Gamma}) and oneE2g({\Gamma}) phonons. The doubly degenerate E2g({\Gamma}) mode reverses thehelicity of incident photon, indicating the pseudo-angular momentum andchirality. Through analysis of temperature-dependent phonon energies andlifetimes, which strongly diverge from the anharmonic model below Curietemperature, we determine the spin-phonon coupling in Fe3GeTe2. Suchinteraction between lattice oscillations and spin significantly enhances theRaman susceptibility, allowing us to observe two additional Raman modes at thecryogenic temperature range. In addition, we reveal laser radiation induceddegradation of Fe3GeTe2 in ambient conditions and the corresponding Ramanfingerprint. Our results provide the first experimental analysis of phonons inthis novel 2D itinerant ferromagnet and their applicability for furtherfundamental studies and application development.

Lattice dynamics, phonon chirality and spin-phonon coupling in 2D itinerant ferromagnet Fe3GeTe2