Ferroelectric control of magnetism of 3d transition metal-adsorbed graphene monolayers

Electric control of magnetism has significant application prospect in magnetic storage. In this work, first-principles calculations are carried out to study the ferroelectric control of magnetism of the 3d transition metal (TM = V, Cr, Mn, Fe, Co, or Ni)-adsorbed graphene monolayers by using an organic ferroelectric poly(vinylidene-fluoride) (PVDF). Although we observe the ferroelectric control of the magnetocrystalline anisotropy energy (MAE) of all the studied 3d transition metal atoms, the flip of the easy magnetization axis is only achieved in the case of Ni adsorption. When the Ni atom is adsorbed at the bridge site on the graphene monolayer, the easy axis of magnetization would undergo a transition from out-of-plane (MAE = 0.07 meV/atom) to in-plane (MAE = −0.23 meV/atom) when the polarization turns down to up. As a result, the study of Ni is particularly highlighted, and the underlying mechanism is discussed by second-order perturbation theories. We provide a means to realize electric control of the magnetism of graphene, which will facilitate relevant experimental and theoretical research.