Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films

Ultrathin epitaxial films of ferromagnetic insulators (FMIs) with Curie temperatures near room temperature are critically needed for use in dissipationless quantum computation and spintronic devices. However, such materials are extremely rare. Here, a room‐temperature FMI is achieved in ultrathin La0.9Ba0.1MnO3 films grown on SrTiO3 substrates via an interface proximity effect. Detailed scanning transmission electron microscopy images clearly demonstrate that MnO6 octahedral rotations in La0.9Ba0.1MnO3 close to the interface are strongly suppressed. As determined from in situ X‐ray photoemission spectroscopy, O K‐edge X‐ray absorption spectroscopy, and density functional theory, the realization of the FMI state arises from a reduction of Mn eg bandwidth caused by the quenched MnO6 octahedral rotations. The emerging FMI state in La0.9Ba0.1MnO3 together with necessary coherent interface achieved with the perovskite substrate gives very high potential for future high performance electronic devices. Ultrathin ferromagnetic insulators with Curie temperatures above room temperature are critically needed for developing dissipationless quantum electronic and spintronic devices. Unfortunately, such materials are extremely rare in nature. Room‐temperature ferromagnetic insulating states are successfully synthesized by an interfacial octahedral proximity effect in ultrathin La0.9Ba0.1MnO3 films, which could serve as promising candidates for future oxide‐based electronic devices.