Abstract
Two-dimensional ferromagnetic materials hold great promise to develop energy-efficient magnetoelectric memory devices and next-generation spintronics. However, one of the crucial challenges for these materials is the realization of tunable magnetocrystalline anisotropy (MCA) to balance thermal stability and energy efficiency. Here, we systematically study the adsorption effects of 3d transition metals (3d-TMs) on the electronic structure and magnetic property of the Fe3GeTe2 (FGT) monolayer. The adsorption systems exhibit different ground state configurations depending on the adatoms, while the controlled perpendicular magnetic anisotropy has also been achieved. Notably, the Mn/FGT system can maintain the out-of-plane magnetic orientation with a changing amplitude of MCA energy up to 3.057 erg/cm2 as the external strain varies from −4% to 1%. In contrast, the Fe/FGT structure undergoes spin reorientation from in-plane to out-of-plan magnetization with a distinct modification behavior of MCA. We elucidate that the underlying atomistic mechanism mainly arises from the alteration of Fe-derived 3d-orbital states in response to the strain effect, leading to competitive changes in the different coupling states. These findings can not only provide useful guidance to optimize two-dimensional magnets for fundamental research but also reveal the promising potential of TMs/FGT materials for the development of ultra-low energy spintronic devices.
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