Imaging Domain Reversal in an Ultrathin Van der Waals Ferromagnet

Abstract The recent isolation of 2D van der Waals magnetic materials has uncovered rich physics that often differs from the magnetic behavior of their bulk counterparts. However, the microscopic details of fundamental processes such as the initial magnetization or domain reversal, which govern the magnetic hysteresis, remain largely unknown in the ultrathin limit. Here a widefield nitrogen‐vacancy (NV) microscope is employed to directly image these processes in few‐layer flakes of the magnetic semiconductor vanadium triiodide (VI₃). Complete and abrupt switching of most flakes is observed at fields H_c ≈ 0.5–1 T (at 5 K) independent of thickness. The coercive field decreases as the temperature approaches the Curie temperature (T_c ≈ 50 K); however, the switching remains abrupt. The initial magnetization process is then imaged, which reveals thickness‐dependent domain wall depinning fields well below H_c. These results point to ultrathin VI₃ being a nucleation‐type hard ferromagnet, where the coercive field is set by the anisotropy‐limited domain wall nucleation field. This work illustrates the power of widefield NV microscopy to investigate magnetization processes in van der Waals ferromagnets, which can be used to elucidate the origin of the hard ferromagnetic properties of other materials and explore field‐ and current‐driven domain wall dynamics.