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Competition between exchange interactions and magnetocrystalline anisotropymay bring new magnetic states that are of great current interest. An appliedhydrostatic pressure can further be used to tune their balance. In this work weinvestigate the magnetization process of a biaxial antiferromagnet in anexternal magnetic field applied along the easy axis. We find that the singlemetamagnetic transition of the Ising type observed in this material underambient pressure transforms under hydrostatic pressure into two transitions, afirst-order spin flop transition followed by a second order transition towardsa polarized ferromagnetic state near saturation. This reversible tuning into anew magnetic phase is obtained in layered bulk CrSBr at low temperature byvarying the interlayer distance using high hydrostatic pressure, whichefficiently acts on the interlayer magnetic exchange, and is probed bymagneto-optical spectroscopy.

Magneto-optical sensing of the pressure driven magnetic ground states in bulk CrSBr