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Rich functionalities of transition-metal oxides and their interfaces bear anenormous technological potential. Its realization in practical devicesrequires, however, a significant improvement of yet relatively low electronmobility in oxide materials. Recently, a mobility boost of about two orders ofmagnitude has been demonstrated at the spinel/perovskite {\gamma}-Al2O3/SrTiO3interface compared to the paradigm perovskite/perovskite LaAlO3/SrTiO3. Weexplore the fundamental physics behind this phenomenon from direct measurementsof the momentum-resolved electronic structure of this interface using resonantsoft-X-ray angle-resolved photoemission. We find an anomaly in orbital orderingof the mobile electrons in {\gamma}-Al2O3/SrTiO3 which depopulates electronstates in the top STO layer. This rearrangement of the mobile electron systempushes the electron density away from the interface that reduces its overlapwith the interfacial defects and weakens the electron-phonon interaction, botheffects contributing to the mobility boost. A crystal-field analysis shows thatthe band order alters owing to the symmetry breaking between the spinel{\gamma}-Al2O3 and perovskite SrTiO3. The band-order engineering exploiting thefundamental symmetry properties emerges as another route to boost theperformance of oxide devices.

Band-Order Anomaly at the {\gamma}-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost