Unusually High Occupation of Co 3d State in Magnetic Weyl Semimetal Co₃Sn₂S₂

The physical properties of magnetic topological materials are strongly influenced by their nontrivial band topology coupled with the magnetic structure. Co₃Sn₂S₂ is a ferromagnetic kagome Weyl semimetal displaying giant intrinsic anomalous Hall effect which can be further tuned via elemental doping, such as Ni substitution for Co. Despite significant interest, the exact valency of Co and the magnetic order of the Ni dopants remained unclear. Here, we report a study of Ni-doped Co₃Sn₂S₂ single crystals using synchrotron-based X-ray magnetic circular dichroism (XMCD), X-ray photoelectron emission microscopy (XPEEM), and hard/soft X-ray photoemission spectroscopy (XPS) techniques. We confirm the presence of spin-dominated magnetism from Co in the host material, and also the establishment of ferromagnetic order from the Ni dopant. The oxygen-free photoemission spectrum of the Co 2p core levels in the crystal well resembles that of a metallic Co film, indicating a Co⁰⁺ valency. Surprisingly, we find the electron filling in the Co 3d state can reach 8.7-9.0 electrons in these single crystals. Our results highlight the importance of element-specific X-ray spectroscopy in understanding the electronic and magnetic properties that are fundamental to a heavily studied Weyl semimetal, which could aid in developing future spintronic applications based on magnetic topological materials.