Coverage level dependence of magnetization reorientation of Fe adatoms on MoSe2 monolayer

Herein we report the results of first-principles density functional theory calculations on the adsorption coverage and intrinsic magnetic properties of the Fe adatoms on the MoSe2 monolayer. It is predicted that the Fe atoms prefer to chemically adsorb at the Mo-top site in close proximity rather than having uniform or cluster coverage. Moreover, our calculations show that while the spin magnetic moment of the Fe atoms is rather robust, the magnetization direction is reversible upon the change in coverage level. This magnetization reversal is mainly driven by the coverage dependence of the spin-orbit coupled Fe 3d energy levels associated with the strong hybridization between the Fe 3d and Mo 4d orbital states. These findings open interesting prospects for manipulating the coverage level of the chemically adsorbed magnetic adatoms to control their magnetization direction on transition metal dichalcogenide structures.