Ferroelectric control of magnetic properties in single metallocenes

Tunable quantum states and long spin-relaxation times are crucial requirements for the application of single-molecule magnets (SMMs) in spintronics and quantum information technologies. Here, we take metallocenes (MCp2) with various transition metal centers, together with ferroelectric In2Se3, as a model to explore the feasibility of ferroelectric control over the quantum states of SMMs through systematic first-principles calculations. The calculated results demonstrate that the quantum state of MCp2 can be effectively modulated by turning the polarization direction of the In2Se3 substrate. Particularly, for TaCp2, the magnetic anisotropy energy can be regulated from 2.82 to 16.67 meV. These findings provide fundamental insights into the ferroelectric manipulation of single spin.