Realization of room-temperature magnetism and multistep magnetization switching in 2D metallic ferrimagnets

Achieving multistep magnetization switching in two-dimensional (2D) ferrimagnets demonstrates substantial promise for advancing high-density non-Boolean logic and memory devices. However, existing 2D ferrimagnets are still hampered by low Curie temperatures and a lack of tunable multiple magnetic states. Here, we report the successful synthesis of a family of 2D Fe 0.875 S (1− x ) Se x alloy with robust room-temperature ferrimagnetism. The key magnetic and electrical properties can be effectively regulated by tailoring the chalcogen ratio in Fe 0.875 S (1− x ) Se x alloy. Notably, multiple magnetic states and resistance plateaus are observed because of the spin canting behavior, enabling the realization of several distinct spin states by adjusting magnetic fields and temperatures, thereby demonstrating great potential for multistate applications. Density functional theory calculations further reveal that the evolution of magnetic anisotropy originates from variations in the orbital occupation of electronic states near the Fermi level. Our work can expand the library of 2D metallic ferrimagnets and pave the way for designing high-density spintronic devices.