Spin‐Lattice Coupled Metamagnetism in Frustrated van der Waals Magnet CrOCl

Abstract The long‐range magnetic ordering in frustrated magnetic systems is stabilized by coupling magnetic moments to various degrees of freedom, for example, by enhancing magnetic anisotropy via lattice distortion. Here, the unconventional spin‐lattice coupled metamagnetic properties of atomically‐thin CrOCl, a van der Waals antiferromagnet with inherent magnetic frustration rooted in the staggered square lattice, are reported. Using temperature‐ and angle‐dependent tunneling magnetoconductance (TMC), in complementary with magnetic torque and first‐principles calculations, the antiferromagnetic (AFM)‐to‐ferrimagnetic (FiM) metamagnetic transitions (MTs) of few‐layer CrOCl are revealed to be triggered by collective magnetic moment flipping rather than the established spin‐flop mechanism, when external magnetic field (H) enforces a lattice reconstruction interlocked with the five‐fold periodicity of the FiM phase. The spin‐lattice coupled MTs are manifested by drastic jumps in TMC, which show anomalous upshifts at the transition thresholds and persist much higher above the AFM Néel temperature. While the MTs exhibit distinctive triaxial anisotropy, reflecting divergent magnetocrystalline anisotropy of thec‐axis AFM ground state, the resulting FiM phase has ana‐ceasy plane in which the magnetization axis is freely rotated byH. At the 2D limit, such a field‐tunable FiM phase may provide unique opportunities to explore exotic emergent phenomena and novel spintronics devices.