Ab initio investigation of the role of the choice transition metal on the structural, electronic, and magnetic properties of transition-metal intercalated 2D materials.

Intercalated transition-metal dichalcogenides (TMDs) host a range of novel magnetic and electronic phenomena including low-power switching, and new potential spin qubits. Manipulation of spins of these intercalating species could open the pathway towards developing new highly tunable magnetic interactions in low-dimensional structures. In this work, we study the effect of varying the intercalant species on the structural, electronic, and magnetic properties of transition-metal intercalated TMDs using first-principles calculations. We systematically study the inclusion of Fe, Ni, and Co intercalants between the TMD layers, in varying concentrations, and at different sites, and track the subsequent exchange interactions in these new magnetic superstructures. Our results indicate that intercalant site selection and concentration, in addition to the atomic species itself play a significant role in determining the ultimate properties of the intercalated TMD, and suggest routes for enabling their tunability. We further discuss the performance of  the exchange-correlation functional (DFT+U and hybrid DFT) on the calculated properties.