Magnetic Structure and Metamagnetic Transitions in the van der Waals Antiferromagnet CrPS4

Abstract In 2D magnets, interlayer exchange coupling is generally weak due to the van der Waals layered structure but it still plays a vital role in stabilizing the long‐range magnetic ordering and determining the magnetic properties. Using complementary neutron diffraction, magnetic, and torque measurements, the complete magnetic phase diagram of CrPS 4 crystals is determined. CrPS 4 shows an antiferromagnetic ground state (A‐type) formed by out‐of‐plane ferromagnetic monolayers with interlayer antiferromagnetic coupling along the c axis below T N = 38 K. Due to small magnetic anisotropy energy and weak interlayer coupling, the low‐field metamagnetic transitions in CrPS 4, that is, a spin‐flop transition at ≈0.7 T and a spin‐flip transition from antiferromagnetic to ferromagnetic under a relatively low field of 8 T, can be realized for H ∥ c . Intriguingly, with an inherent in‐plane lattice anisotropy, spin‐flop‐induced moment realignment in CrPS 4 for H ∥ c is parallel to the quasi‐1D chains of CrS 6 octahedra. The peculiar metamagnetic transitions and in‐plane anisotropy make few‐layer CrPS 4 flakes a fascinating platform for studying 2D magnetism and for exploring prototype device applications in spintronics and optoelectronics.