Electrical Control of Magnetic Order Transition in 2D Antiferromagnetic Semiconductor FePS₃

Manipulating the magnetic order transition of 2D magnetic materials is an important way for the application of spintronic devices, and carrier concentration modulation is a commonly used effective regulation method. Here the magnetic ground state of FePS₃ is tuned from antiferromagnetic (AFM) to ferrimagnetic (FIM) and back to AFM by electron doping, which is achieved via the intercalation of various organic cations. The doped FePS₃ with FIM order exhibits a Curie temperature T_c of ≈110 K, a strong out-of-plane magnetic anisotropy, and particularly an unusual hysteresis loop, where with increasing temperature, the area of magnetic hysteresis loop increases below 50 K, then decreases above 50 K and eventually disappears. Theoretical calculations indicate that at a doping concentration of 0.3-0.9 electrons per cell, spin splitting of energy bands occurs, leading to the FIM order; whereas at a doping concentration of ≥ 1.0 electrons per cell, the AFM order recovers. Such AFM-FIM-AFM transition is ascribed to the competition between the Stoner exchange-dominated FM order and super-exchange-dominated AFM order. These results demonstrate an effective approach to engineering magnetism in 2D magnetic materials by purely electrical means for future device applications.