First principles studies of magnetic ion-intercalated transition metal dichalcogenide bilayers*

Monolayer transition metal dichalcogenides (TMDs) offer a promising framework for valleytronic applications given their degenerate, yet non-equivalent K,K’ points from broken inversion symmetry which exhibit significant spin-orbit interaction induced spin-valley coupling. Recent experimental work1,2 in transferring monolayer TMDs onto ferromagnetic substrates has shown splitting of the K-K’ band degeneracy associated with the breaking of time-reversal symmetry. Here we perform ab initio density functional theory calculations of the structural, electronic, and magnetic properties of magnetic ion intercalated MoS2 bilayers. Through investigation of intercalant element, intercalant density, and bilayer spacing and registry, we assess the promise of intercalated bilayer architectures for valley splitting and valleytronic applications.

1. Nature Nanotechnology volume 12, pages 757–762 (2017)
2. Science Advances volume 3, pages e1603113 (2017)