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Main Authors: Sternemann, Lasse, Janas, David Maximilian, Banerjee, Eshan, Leven, Richard, Nitschke, Jonah Elias, Marino, Marco, Becker, Leon, Ademoğlu, Ahmet Can, Anders, Frithjof, Tappertzhofen, Stefan, Cinchetti, Mirko
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2511.17403
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author Sternemann, Lasse
Janas, David Maximilian
Banerjee, Eshan
Leven, Richard
Nitschke, Jonah Elias
Marino, Marco
Becker, Leon
Ademoğlu, Ahmet Can
Anders, Frithjof
Tappertzhofen, Stefan
Cinchetti, Mirko
author_facet Sternemann, Lasse
Janas, David Maximilian
Banerjee, Eshan
Leven, Richard
Nitschke, Jonah Elias
Marino, Marco
Becker, Leon
Ademoğlu, Ahmet Can
Anders, Frithjof
Tappertzhofen, Stefan
Cinchetti, Mirko
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2511_17403
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Momentum-Resolved Electronic Structure and Orbital Hybridization in the Layered Antiferromagnet CrPS$_4$
Sternemann, Lasse
Janas, David Maximilian
Banerjee, Eshan
Leven, Richard
Nitschke, Jonah Elias
Marino, Marco
Becker, Leon
Ademoğlu, Ahmet Can
Anders, Frithjof
Tappertzhofen, Stefan
Cinchetti, Mirko
Materials Science
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.
title Momentum-Resolved Electronic Structure and Orbital Hybridization in the Layered Antiferromagnet CrPS$_4$
topic Materials Science
url https://arxiv.org/abs/2511.17403