Understanding the role of defects in oxide heterostructures is crucial for future materials control and functionalization. We hence study the impact of oxygen vacancies (OVs) at variable concentrations on orbital and spin exchange in the ${\mathrm{LaAlO}}_3/\mathrm{Sr}{\mathrm{TiO}}_3$ interface by first-principles many-body theory and real-space model-Hamiltonian techniques. Intricate interplay between the Hubbard $U$ and Hund's coupling $J_H$ for OV-induced correlated states is demonstrated. Orbital polarization towards an effective $e_g$ state with predominant local antiferromagnetic alignment on Ti sites near OVs is contrasted with $t_{2g}\left(xy\right)$ states with ferromagnetic tendencies in the defect-free regions. Different magnetic phases are identified, giving rise to distinct net-moment behavior at low and high OV concentrations. This provides a theoretical basis for prospective tailored magnetism by defect manipulation in oxide interfaces.

• Received 23 June 2015

DOI:https://doi.org/10.1103/PhysRevB.92.125148