Signatures of noncollinear ferrimagnetism in the van der Waals semiconductor CrSCl

Noncollinear ferrimagnets combining the advantages of both controllable net magnetization and ultrafast spin dynamics are promising for spintronic and spin-torque devices. However, they are rare in the van der Waals (vdW) materials. Here, we systematically studied the magnetic behavior of a vdW semiconductor CrSCl exhibiting potential noncollinear ferrimagnetism. The nature of two-sublattice ferrimagnetic order was confirmed by fitting the temperature-dependent reciprocal of molar magnetic susceptibility above TC. Remarkably, an unusual decrease that can be suppressed by the external field was observed on the temperature-dependent magnetization curves, which is beyond the expectation for the collinear ferrimagnet. Combined with further analyses on the field-dependent magnetization curves and critical behavior and first-principles calculations, we propose that the potential spin canting is responsible for these observations. These findings render CrSCl a prospective vdW noncollinear ferrimagnetic semiconductor that could benefit spintronic applications.