Band-Order Anomaly at the γ-Al₂O₃/SrTiO₃ Interface Drives the Electron-Mobility Boost

The rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about 2 orders of magnitude has been demonstrated at the spinel-perovskite γ-Al₂O₃/SrTiO₃ interface compared to the paradigm perovskite-perovskite LaAlO₃/SrTiO₃ interface. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in γ-Al₂O₃/SrTiO₃ which depopulates electron states in the top SrTiO₃ layer. This rearrangement of the mobile electron system pushes the electron density away from the interface, which reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel γ-Al₂O₃ and perovskite SrTiO₃. Band-order engineering, exploiting the fundamental symmetry properties, emerges as another route to boost the performance of oxide devices.