Direct Observation of Room-Temperature Stable Magnetism in LaAlO3/SrTiO3 Heterostructures

Along with an unexpected conducting interface between nonmagnetic insulating perovskites LaAlO₃ and SrTiO₃ (LaAlO₃/SrTiO₃), striking interfacial magnetisms have been observed in LaAlO₃/SrTiO₃ heterostructures. Interestingly, the strength of the interfacial magnetic moment is found to be dependent on oxygen partial pressures during the growth process. This raises an important, fundamental question on the origin of these remarkable interfacial magnetic orderings. Here, we report a direct evidence of room-temperature stable magnetism in a LaAlO₃/SrTiO₃ heterostructure prepared at high oxygen partial pressure by using element-specific soft X-ray magnetic circular dichroism at both Ti L_3,2 and O K edges. By combining X-ray absorption spectroscopy at both Ti L_3,2 and O K edges and first-principles calculations, we qualitatively ascribe that this strong magnetic ordering with dominant interfacial Ti³⁺ character is due to the coexistence of LaAlO₃ surface oxygen vacancies and interfacial (Ti_Al-Al_Ti) antisite defects. On the basis of this new understanding, we revisit the origin of the weak magnetism in LaAlO₃/SrTiO₃ heterostructures prepared at low oxygen partial pressures. Our calculations show that LaAlO₃ surface oxygen vacancies are responsible for the weak magnetism at the interface. Our result provides direct evidence on the presence of room-temperature stable magnetism and a novel perspective to understand magnetic and electronic reconstructions at such strategic oxide interfaces.