The emergence of magnetic ordering at complex oxide interfaces tuned by defects

Complex oxides show extreme sensitivity to structural distortions and defects, and the intricate balance of competing interactions which emerge at atomically defined interfaces may give rise to unexpected physics. In the interfaces of non-magnetic complex oxides, one of the most intriguing properties is the emergence of magnetism which is sensitive to chemical defects. Particularly, it is unclear which defects are responsible for the emergent magnetic interfaces. Here, we show direct and clear experimental evidence, supported by theoretical explanation, that the B-site cation stoichiometry is crucial for the creation and control of magnetism at the interface between non-magnetic ABO₃-perovskite oxides, LaAlO₃ and SrTiO₃. We find that consecutive defect formation, driven by atomic charge compensation, establishes the formation of robust perpendicular magnetic moments at the interface. Our observations propose a route to tune these emerging magnetoelectric structures, which are strongly coupled at the polar-nonpolar complex oxide interfaces.