Tuning magnetocrystalline anisotropy by controlling the orbital electronic configuration of two-dimensional magnetic materials

A suitable magnetic anisotropy energy (MAE) is a key factor for magnetic materials. However, an effective MAE control method has not yet been achieved. In this study, we propose a novel strategy to manipulate MAE by rearranging the d-orbitals of metal atoms with oxygen functionalized metallophthalocyanine (MPc) by first-principles calculations. By the dual regulation of electric field and atomic adsorption, we have achieved a substantial amplification of the single regulation method. The use of O atoms to modify the metallophthalocyanine (MPc) sheets effectively adjusts the orbital arrangement of the electronic configuration in the d-orbitals of the transition metal near the Fermi level, thereby modulating the MAE of the structure. More importantly, the electric field amplifies the effect of electric-field regulation by adjusting the distance between the O atom and metal atom. Our results demonstrate a new approach to modulating the MAE of two-dimensional magnetic films for practical application in information storage.