Electric field tuning of magnetic states in single magnetic molecules

Abstract

Single magnetic molecules may be the smallest functional magnets. An electric-field controllable spin state of magnetic molecules is of fundamental importance for applications while its realization remains challenging. To date the observed spin-electric interaction based on spin-orbit coupling or spin dipole coupling is useful to tune fine spin structures but too weak to flip the spin state. In this work, we propose a new mechanism to realize enhanced spin-electric coupling and flip the spin states by tuning the spin superexchange between local spins. Using first-principles calculations and Heisenberg Hamiltonian, we demonstrate this effect in a family of magnetic molecules, transition metallic Porphyrins. We show that their d-π and π-π spin superexchange couplings are determined by the relative energies of d and π electronic states, which are sensitive to the applied electric field. Therefore, applying electric field can tune a wide range of magnetic ground states, including ferromagnetic, ferrimagnetic, and antiferromagnetic configurations. This spin-electric coupling may provide a new approach for designing and controlling molecular spintronics.