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 CrBr 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.
Kim et al. (Thu,) studied this question.