Tuning Magnetism of Metal Porphyrazine Molecules by a Ferroelectric In₂Se₃ Monolayer

Electric field tuning of magnetism is highly desirable for nanoelectronics, but volatility in electron spin manipulation presents a major challenge that needs urgent resolution. Here, we show by first-principles calculations that magnetism of metal porphyrazine (MPz) molecules can be effectively tuned by switching ferroelectric polarization of an adjacent In2Se3 monolayer. The magnetic moments of TiPz and VPz (MnPz, FePz, and CoPz) decrease (increase) at one polarization but remain unchanged at reversed polarization. This intriguing phenomenon stems from distinct metal d-orbital occupation caused by electron transfer and energy-level shift associated with the polarization switch of the In2Se3 monolayer. Moreover, the ferroelectric switch also tunes the underlying electronic properties, producing a metallic, half-metallic, or semiconducting state depending on polarization. These findings of robust ferroelectric tuning of magnetism and related electronic properties in MPz-adsorbed In2Se3 hold great promise for innovative design and implementation in advanced magnetic memory storage, sensor, and spintronic devices.