Variation between Antiferromagnetism and Ferrimagnetism in NiPS3 by Electron Doping

To electrically control magnetic properties of material is promising toward spintronic applications, where the investigation of carrier doping effects on antiferromagnetic (AFM) materials remains challenging due to their zero net magnetization. In this work, the authors find electron doping dependent variation of magnetic orders of a 2D AFM insulator NiPS3, where doping concentration is tuned by intercalating various organic cations into the van der Waals gaps of NiPS3 without introduction of defects and impurity phases. The doped NiPS3 shows an AFM‐ferrimagnetic (FIM) transition at a doping level of 0.2–0.5 electrons/cell and a FIM‐AFM transition at a doping level of ≥0.6 electrons/cell. The authors propose that the found phenomenon is due to competition between Stoner exchange dominated inter‐chain ferromagnetic order and super‐exchange dominated AFM order at different doping level. The studies provide a viable way to exploit correlation between electronic structures and magnetic properties of 2D magnetic materials for realization of magnetoelectric effect. Van der Waals (vdW) antiferromagnet NiPS3 undergoes a magnetic order transition from antiferromagnetic (AFM) to ferrimagnetic and then AFM with the increasing of electron concentration, where the concentration levels are tuned by intercalating various organic cations into vdW gaps of NiPS3. The carrier doping dependent magnetic transition offers a viable tool for electrically controlling magnetic properties of vdW magnets.