  Strong charge-spin coupling is found in a layered transition-metal
trichalcogenide NiPS3, a van derWaals antiferromagnet, from our study of the
electronic structure using several experimental and theoretical tools:
spectroscopic ellipsometry, x-ray absorption and photoemission spectroscopy,
and density-functional calculations. NiPS3 displays an anomalous shift in the
optical spectral weight at the magnetic ordering temperature, reflecting a
strong coupling between the electronic and magnetic structures. X-ray
absorption, photoemission and optical spectra support a self-doped ground state
in NiPS3. Our work demonstrates that layered transition-metal trichalcogenide
magnets are a useful candidate for the study of correlated-electron physics in
two-dimensional magnetic material.
