Lattice Dynamics, Phonon Chirality, and Spin–Phonon Coupling in 2D Itinerant Ferromagnet Fe 3 GeTe 2

Fe 3 GeTe 2 has emerged as one of the most fascinating van der Waals crystals due to its 2D itinerant ferromagnetism, topological nodal lines, and Kondo lattice behavior. However, lattice dynamics, chirality of phonons, and spin–phonon coupling in this material, which set the foundation for these exotic phenomena, have remained unexplored. Here, the first experimental investigation of the phonons and mutual interactions between spin and lattice degrees of freedom in few‐layer Fe 3 GeTe 2 is reported. The results elucidate three prominent Raman modes at room temperature: two A 1g (Γ) and one E 2g (Γ) phonons. The doubly degenerate E 2g (Γ) mode reverses the helicity of incident photons, indicating the pseudoangular momentum and chirality. Through analysis of temperature‐dependent phonon energies and lifetimes, which strongly diverge from the anharmonic model below Curie temperature, the spin–phonon coupling in Fe 3 GeTe 2 is determined. Such interaction between lattice oscillations and spin significantly enhances the Raman susceptibility, allowing to observe two additional Raman modes at the cryogenic temperature range. In addition, laser radiation‐induced degradation of Fe 3 GeTe 2 in ambient conditions and the corresponding Raman fingerprint is revealed. The results provide the first experimental analysis of phonons in this novel 2D itinerant ferromagnet and their applicability for further fundamental studies and application development.