Hydrogen-Intercalated 2D Magnetic Bilayer: Controlled Magnetic Phase Transition and Half-Metallicity via Ferroelectric Switching

Electrically controlled magnetism in two-dimensional (2D) multiferroics is highly desirable for both fundamental research and the future development of low-power nanodevices. Herein, inspired by the recently experimentally realized 2D antiferromagnetic MnPSe₃ [Nat. Nanotechnol. 2021, 16 (7), 782] and guided by a heteromagnetic structural design, we engineer strong magnetoelectric coupling in a hydrogen-intercalated 2D MnPSe₃ bilayer. Hydrogen functionalization breaks the centrosymmetry of bilayer MnPSe₃, leading to out-of-plane ferroelectricity. Moreover, there is a phase transition from antiferromagnetic semiconductor to ferromagnetic half-metal in the H-bonded MnPSe₃ layer, while the other remains antiferromagnetic and semiconducting. When reversing the electrical polarization, the intercalated H atom can flip between the top and bottom layers with an ultralow switching barrier, which allows one to tune the magnetic order and conductivity of the individual layers via an external electric field. Our results pave a new avenue to realize strong magnetoelectric coupling in single-phase multiferroic material. The ferroelectricity-controlled magnetic phase transition and half-metallicity offer promising applications in nanoscale spintronics such as electrically written and magnetically read memories.