Band-filling-controlled magnetism from transition metal intercalation in \(N_{1/3}\)NbS\(_2\) revealed with first-principles calculations

We present a first-principles study of the effect of 3\(d\) transition metal intercalation on the magnetic properties of the 2H-NbS\(_2\) system, using spin-resolved density functional theory calculations to investigate the electronic structure of \(N_{1/3}\)NbS\(_2\) (\(N\) = Ti, V, Cr, Mn, Fe, Co, Ni). We are able to accurately determine the magnetic moments and crystal field splitting, and find that the magnetic properties of the materials are determined by a mechanism based on filling rigid bands with electrons from the intercalant. We predict the dominant magnetic interaction of these materials by considering Fermi surface nesting, finding agreement with experiment where data are available.