Chemically Engineering Magnetic Anisotropy of 2D Metalloporphyrin

Continuous miniaturization of magnetic units in spintronics devices inspires efforts to search for novel 2D magnetic materials with giant magnetic anisotropy energy (MAE). Through systematic first‐principles calculations, large MAE of 24 meV in W or Re embedded 2D polyporphyrin frameworks is found. Interestingly, the MAE can be enhanced up to 60 meV, through replacing the hydrogen atoms on the edges of the Re based 2D polyporphyrin framework by hydroxyl and amino radicals. Analysis of the electronic structures reveals that the enhancement of MAE is mainly attributed to charge redistributions and energy shifts of Re 5d orbitals induced by the functional radicals. The findings pave a new and feasible way for tailoring the magnetic properties of magnetic organic materials to fulfill the criteria for applications in spintronics devices at high temperature.