CC BY 4.0 UnportedKoitzsch, A.Klaproth, T.Selter, S.Shemerliuk, Y.Aswartham, S.Janson, O.Büchner, B.Knupfer, M.2023-10-122023-10-122023https://oa.tib.eu/renate/handle/123456789/12454https://doi.org/10.34657/11484Many unusual and promising properties have been reported recently for the transition metal trichalcogenides of the type MPS3 (M = V, Mn, Fe, Ni..), such as maintaining magnetic order to the atomically thin limit, ultra-sharp many-body excitons, metal-insulator transitions and, especially for Fe2P2S6, giant linear dichroism among others. Here we conduct a detailed investigation of the electronic structure of Fe2P2S6 using angle-resolved photoemission spectroscopy, q-dependent electron energy loss spectroscopy, optical spectroscopies and density functional theory. Fe2P2S6 is a Mott insulator with a gap of E gap ≈ 1.4 eV and zigzag antiferromagnetism below T N = 119 K. The low energy excitations are dominated by Fe 3d states. Large and sign-changing linear dichroism is observed. We provide a microscopic mechanism explaining key properties of the linear dichroism based on the correlated character of the electronic structure, thereby elucidating the nature of the spin-charge coupling in Fe2P2S6 and related materials.enghttps://creativecommons.org/licenses/by/4.0/530Electronic properties and materialsSurfaces, interfaces and thin filmsArticle