Realizing ferromagnetism in organic-ions intercalated antiferromagnet MnPSe3

The magnetic properties of two-dimensional magnetic van der Waals materials can be efficiently tailored through pure electrical control, particularly via electron doping. This approach modulates orbital occupation of transition metal atoms, thereby altering the exchange interaction and enabling an effective control on magnetic ground state. However, the related investigation on the electrical control of intralayer antiferromagnetic (AFM) order remains limited. Here, we report that the magnetic ground state of MnPSe3 can be effectively modulated from an AFM to a ferromagnetic (FM) order via electron doping, achieved through the intercalation of different alkylammonium ions. All the intercalated MnPSe3 show FM order with Tc ranging from 40 to 50 K and in-plane magnetic anisotropy. Density functional theory calculations indicate that when the electron doping concentration reaches or exceeds 0.6 electrons per cell, the FM state becomes energetically favorable and stabilizes as the magnetic ground state of doped MnPSe3. This work not only elucidates the mechanisms underlying the modulation of magnetic properties in MnPSe3 but also highlights the potential for tailoring magnetic order in layered materials through electrochemical intercalation, offering valuable insights for the development of spintronic devices.