Slow Magnetic Relaxation of Dy Adatoms with In-Plane Magnetic Anisotropy on a Two-Dimensional Electron Gas

We report on the magnetic properties of Dy atoms adsorbed on the (001) surface of SrTiO₃. X-ray magnetic circular dichroism reveals slow relaxation of the Dy magnetization on a time scale of about 800 s at 2.5 K, unusually associated with an easy-plane magnetic anisotropy. We attribute these properties to Dy atoms occupying hollow adsorption sites on the TiO₂-terminated surface. Conversely, Ho atoms adsorbed on the same surface show paramagnetic behavior down to 2.5 K. With the help of atomic multiplet simulations and first-principles calculations, we establish that Dy populates also the top-O and bridge sites on the coexisting SrO-terminated surface. A simple magnetization relaxation model predicts these two sites to have an even longer magnetization lifetime than the hollow site. Moreover, the adsorption of Dy on the insulating SrTiO₃ crystal leads, regardless of the surface termination, to the formation of a spin-polarized two-dimensional electron gas of Ti 3d character, together with an antiferromagnetic Dy-Ti coupling. Our findings support the feasibility of tuning the magnetic properties of the rare-earth atoms by acting on the substrate electronic gas with electric fields.