Interfacial engineering of orbital orientation for perpendicular magnetic anisotropy in Co-implanted CrI3 monolayer

Two-dimensional (2D) van der Waals (vdW) magnets are believed to be promising candidates for next-generation information storage, which requires both high Curie points (TC) and large perpendicular magnetic anisotropy (PMA). As one of the most well-known 2D magnets, CrI3 has large PMA but a relatively low TC. Recent theoretical works proposed that implanting metal atoms into the hollow sites of CrI3 could greatly boost TC. However, this process may have the unintended consequence of reducing the PMA and introducing in-plane magnetic anisotropy (IMA) instead. It is, therefore, highly required to implement an additional technique to enhance the PMA. In this work, we use the first-principles method to study the underlying mechanisms of the suppressed PMA (and induced IMA) in the Co-implanted CrI3 monolayer denoted as Co-(CrI3)2 as an example. It is found that the Co-implantation-induced itinerant electrons cause the transition from PMA to IMA by tuning the orbital orientation of the states around the Fermi level, noting that an in-plane (or out-of-plane) electronic orbital leads to the out-of-plane (or in-plane) momentum that favors PMA (or IMA) due to the spin–orbit coupling. In order to restore the PMA, we predict that using the vdW substrate PtTe2 to construct a heterostructure with the Co-(CrI3)2 monolayer not only reduces the contributions of the interfacial out-of-plane orbitals but also generates additional intralayer in-plane orbitals, both supporting the PMA. Thus, this work provides alternative perspectives on enhancing PMA by interfacial engineering of orbital orientation, paving the way for the development of 2D strong magnets.