Spin-orbital excitations encoding the magnetic phase transition in the van der Waals antiferromagnet FePS3

Van der Waals (vdW) materials are featuring intertwined electronic order and collective phenomena. Elucidating the dynamics of the elementary excitations within the fundamental electronic degrees of freedom is of paramount importance. Here we performed resonant inelastic X-ray scattering (RIXS) to elaborate the spin-orbital excitations of the vdW antiferromagnet FePS₃ and their role for magnetism. We observed the spectral enhancement of spin-orbital multiplet excitations at about ~100 and ~220 meV, as well as the quasielastic response, when entering the antiferromagnetic phase with an order-parameter-like evolution in temperature. By comparing with model calculations, we discovered the trigonal lattice distortion, spin-orbit interaction and metal-ligand charge-transfer to be essential for these emergent excitations. We further reveal their spectral robustness down to the few atomic-layer limit by mechanical exfoliation, in accordance with the persistent antiferromagnetism reported previously. Our study highlights the crucial role of lattice and orbital anisotropy for stabilizing the quasi-two-dimensional magnetism and tailoring vdW magnets.