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Ligand-mediated magnetic coupling across metamagnetic transitions in CrPS4

Giuseppe Buccoliero1,2,*, Rachel Nickel1, Roberto Sant3, Marli dos Reis Cantarino1, Andrei Rogalev1, Nathan J. Yutronkie1, Tristan Riccardi2, Daniel A. Chaney1, Kurt Kummer1 et al.

Johann Coraux2 and Nicholas B. Brookes1

  • *Contact author: giuseppe.buccoliero@esrf.fr
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Phys. Rev. Research 8, 023323 – Published 22 June, 2026

DOI: https://doi.org/10.1103/g38t-lcj3

Abstract

Chromium thiophosphate (CrPS4) is a long-known material: A layered semiconducting antiferromagnet. Its recently discovered gate-tunable metamagnetic phase transitions, the remarkable positive and oscillating magnetoresistance as a tunnel barrier, and its Fano-resonance luminescence, elusive among the multitude of Cr3+ compounds, call for revisiting the understanding of its electronic structure, especially regarding how it relates to magnetic order. Here, we employ X-ray magnetic circular dichroism, implemented in both absorption and resonant inelastic X-ray spectroscopies, together with quantum many-body calculations, to unveil the role of metal-ligand covalency in mediating the metamagnetic transitions in CrPS4, using crystal-field and charge-transfer excitations as fingerprints of the evolving magnetic order. We reveal the role of extended superexchange paths involving P and S atoms, coupling interactions between the Cr spins across the different magnetic phases—antiferromagnetic, canted, and ferromagnetic. Our results elucidate the electronic states involved in these phases and provide prescriptions for engineering the metamagnetic phase diagram of CrPS4.

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Phys. Rev. Research 8, 023323– Published 22 June, 2026
  • Received 19 February 2026
  • Accepted 4 June 2026
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