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Strong charge-spin coupling is found in a layered transition-metaltrichalcogenide NiPS3, a van derWaals antiferromagnet, from our study of theelectronic 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 theoptical spectral weight at the magnetic ordering temperature, reflecting astrong coupling between the electronic and magnetic structures. X-rayabsorption, photoemission and optical spectra support a self-doped ground statein NiPS3. Our work demonstrates that layered transition-metal trichalcogenidemagnets are a useful candidate for the study of correlated-electron physics intwo-dimensional magnetic material.

Charge-spin correlation in van der Waals antiferromagenet NiPS3