Momentum-Resolved Electronic Structure and Orbital Hybridization in the Layered Antiferromagnet CrPS${}_4$

Abstract

Chromium thiophosphate (CrPS${}_4$) is a layered two-dimensional antiferromagnetic semiconductor exhibiting intriguing spintronic and magneto-optical properties, yet its electronic band structure has remained experimentally uncharacterized. Here, we employ momentum-resolved photoemission spectroscopy above and below the Néel temperature, complemented by density functional theory with Hubbard U corrections (DFT+U), to reveal a valence band dominated by Cr $3d$ and S $3p$ states with a ligand-to-metal charge-transfer band gap. We identify weakly hybridized t${}_{2g}$ orbitals responsible for magnetic ordering and strongly hybridized e${}_g$ orbitals that relax dipole selection rules, enabling optically active orbital transitions. These findings establish a foundational understanding of CrPS${}_4$'s electronic structure, providing a benchmark for theoretical models and informing future investigations into its orbital physics and potential device applications.

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