Insulator‐Metal Transition and Magnetic Collapse of CrSBr Under High Pressure

We investigate the structural, electronic, and magnetic properties of the van der Waals antiferromagnet CrSBr under high pressure using ab initio calculations. At ambient pressure, CrSBr is a Mott insulator with A ‐type antiferromagnetic order and a local moment of ∼3 μ B per Cr atom, originating from three electrons in the t 2 g manifold. Upon increasing pressure, the moment collapses to ∼1 μ B , accompanied by a volume reduction and an inversion of the distorted CrS 4 Br 2 octahedron with elongated CrBr bonds. This transition is accompanied by an insulator‐metal crossover, driven by crystal electric field reconstruction that redistributes the Cr 3 d electrons among four low‐lying states. Our results reveal a pressure‐induced transition in CrSBr, from a Mott‐localized high‐spin state to an itinerant metallic state with a substantially reduced magnetic moment.