First-principles theory of ultrathin magnetic films

We report on a set of systematic first-principles electronic structure investigations of the magnetic spin moments, the magnetic spin configurations, and the magnetic coupling of ultrathin magnetic films on (001)- and (Ill)-oriented noble-metal substrates and on the Fe(001) substrate. Magnetism is found for 3d-, 4d-, and Sd-transition-metal monolayers on noble-metal substrates. For V, Cr, and Mn on (001) substrates a c(2 x 2) antiferromagnetic superstructure has the lowest energy, and Fe, Co, Ni are ferromagnetic. On(lll) substrates, for Cr the energy minimum is found for a 120 degrees non-collinear magnetic configuration in a (root 3 x root 3)R30 degrees unit cell, and for Mn a row-wise antiferromagnetic structure is found. On Fe(001), V and Cr monolayers prefer the layered antiferromagnetic coupling, and Fe, Co, and Ni monolayers favour the ferromagnetic coupling to Fe(001). The magnetic structure of Mn on Fe(001) is a difficult case: at least two competing magnetic states are found within an energy of 7 meV. The Cr/Fe(001) system is discussed in more detail as the surface-alloy formation is investigated, and this system is used as a test case to compare theoretical and experimental scanning tunnelling spectroscopy (STS) results. The possibility of resolving magnetic structures by STS is explored. The results are based on the local spin-density approximation and the generalized gradient approximation to the density functional theory. The calculations are carried out with the full-potential linearized augmented-plane-wave method in film geometry.