Direct Imaging of Antiferromagnet‐Ferromagnet Phase Transition in van der Waals Antiferromagnet CrSBr

Abstract The advent of van der Waals (vdW) ferromagnetic (FM) and antiferromagnetic (AFM) materials offers unprecedented opportunities for spintronics and magneto‐optic devices. Combining magnetic Kerr microscopy and density functional theory calculations, the AFM‐FM transition is investigated and a surprising abnormal magneto‐optic anisotropy in vdW CrSBr associated with different magnetic phases (FM, AFM, or paramagnetic state) is discovered. This unique magneto‐optic property leads to different anisotropic optical reflectivity from different magnetic states, permitting direct imaging of the AFM Néel vector orientation and the dynamic process of the AFM‐FM transition within a magnetic field. Using Kerr microscopy, not only the domain nucleation and propagation process is imaged but also the intermediate spin‐flop state in the AFM‐FM transition is identified. The unique magneto‐optic property and clear identification of the dynamics process of the AFM‐FM phase transition in CrSBr demonstrate the promise of vdW magnetic materials for future spintronic technology.