Competition between exchange interactions and magnetocrystalline anisotropy may bring new magnetic states that are of great current interest. An applied hydrostatic pressure can further be used to tune their balance. In this work, we investigate the magnetization process of a biaxial antiferromagnet in an external magnetic field applied along the easy axis. We find that the single metamagnetic transition of the Ising type observed in this material under ambient pressure transforms under hydrostatic pressure into two transitions, a first-order spin-flop transition followed by a second-order transition toward a polarized ferromagnetic state near saturation. This reversible tuning into a new magnetic phase is obtained in layered bulk CrSBr at low temperature by varying the interlayer distance using high hydrostatic pressure, which efficiently acts on the interlayer magnetic exchange and is probed by magneto-optical spectroscopy.

CENTERA Laboratories Institute of High Pressure Physics PAS 01 142 Warsaw Poland

Department of Inorganic Chemistry University of Chemistry and Technology Prague Technicka 5 166 28 Prague 6 Czech Republic

Institut Laue Langevin F 38042 Grenoble Cedex 9 France

Institut Neel Université Grenoble Alpes 38000 Grenoble France

LNCMI UPR 3228 CNRS EMFL Université Grenoble Alpes 38000 Grenoble France

Université Grenoble Alpes CEA Grenoble INP IRIG Pheliqs 38000 Grenoble France

Walter Schottky Institut Physics Department and MCQST Technische Universitat Munchen 85748 Garching Germany

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Ferromagnetic Interlayer Coupling in CrSBr Crystals Irradiated by Ions