Thickness dependent rare earth segregation in magnetron deposited NdCo$_{4.6}$ thin films studied by Xray reflectivity and Hard Xray photoemission

Abstract

Magnetic anisotropy in disordered rare-earth-transition metals (RE-TM) compounds arises from RE atoms occupying asymmetric environments within the TM lattice. However, the underlying mechanism that promotes such environments remains not fully understood. In this study, we investigate amorphous NdCo$_{4.6}$ thin films deposited by magnetron sputtering, where the magnetic anisotropy evolves with thickness from in-plane to out-of-plane orientation above 40 nm. X-ray reflectivity measurements revealed the progressive formation of an additional layer between the 3 nm Si capping layer and the NdCo film with increasing film thickness. To probe the composition and distribution of Co and Nd near the surface, Hard X-ray Photoemission Spectroscopy (HAXPES) was performed on films ranging from 5 nm to 65 nm in thickness using incident photon energies of 7, 10, and 13 keV. These correspond to inelastic electron mean free paths of 7.2-12.3 nm in cobalt. The cobalt atomic concentration, deduced from HAXPES at the Nd 3d and Co 2p excitations, was consistently below the nominal value and varied with both thickness and photon energy. This indicates segregation of RE atoms at the film surface, which becomes more pronounced with increasing thickness. Background analysis of the Co 2p and Nd 3d peaks supports this conclusion. The thickness of the Nd segregated layer is estimated in 2-3 nm. These findings demonstrate that incorporating neodymium into the cobalt lattice incurs an energy cost which is associated with strain due to the volume mismatch between the two elements. Reducing this strain energy promotes anisotropic atomic environments for Nd, thereby explaining the emergence of perpendicular anisotropy and its dependence on film thickness in these RE-TM compounds.