Giant orbital magnetization in two-dimensional materials

Abstract Orbital magnetization typically plays a minor role in compounds where the magnetic properties are governed by transition metal elements. However, in some cases, the orbital magnetization may be fully unquenched, which can have dramatic consequences for magnetic anisotropy and various magnetic response properties. In the present work, we start by summarizing how unquenched orbital moments arise from particular combinations of crystal field splitting and orbital filling. We exemplify this for the cases of two-dimensional (2D) VI 3 and FePS 3 , and show that Hubbard corrections as well as self-consistent spin–orbit coupling (SOC) are crucial ingredients for predicting correct orbital moments from first principles calculations. We then search the computational 2D materials database for monolayers having tetrahedral or octahedral crystal field splitting of transition metal d -states and orbital occupancy that is expected to lead to large orbital moments. We identify 112 monolayers with octahedral crystal field splitting and 62 monolayers with tetrahedral crystal field splitting and for materials with partially-filled t 2 g bands, we verify that inclusion of Hubbard corrections as well as self-consistent SOC typically increases the magnitude of predicted orbital moments by an order of magnitude.