Ferroelectric control of single-molecule magnetism in 2D limit

The electric control of magnetic properties based on magnetoelectric effect is crucial for the development of future data storage devices. Here, based on first-principles calculations, a strong magnetoelectric effect is proposed to effectively switch on/off the magnetic states as well as alter the in-plane/perpendicular easy axes of metal-phthalocyanine molecules (MPc) by reversing the electric polarization of the underlying two-dimensional (2D) ferroelectric α-In₂Se₃ substrate with the application of an external electric field. The mechanism originates from the different hybridization between the molecule and the ferroelectric substrate in which the different electronic states of surface Se layer play a dominant role. Moreover, the magnetic moments and magnetic anisotropy energies (MAE) of OsPc/In₂Se₃ can be further largely enhanced by a functionalized atom atop the OsPc molecule. The I-OsPc/In₂Se₃ system possesses large MAE up to 30 meV at both polarization directions, which is sufficient for room-temperature applications. These findings provide a feasible scheme to realize ferroelectric control of magnetic states in 2D limit, which have great potential for applications in nanoscale electronics and spintronics.