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Atomic-scale identification of invisible cation vacancies at an oxide homointerface

Materials Today Physics

Cation vacancies play an important role in creating new functionalities in complex oxides on par with oxygen vacancies. Directly identifying the cation vacancies at the atomic scale is thus key to addressing quantum phenomena related to acceptor states. Here, atomic-scale identification of invisible cation vacancies at an oxide interface via energy-dispersive X-ray spectroscopy (EDX) spectrum imaging is demonstrated. At the homointerface of SrTiO3 (STO) film and a Nb-doped SrTiO3 substrate, the veiled behavior of cation vacancies of Sr and Ti is revealed by the approach for the first time; they are found to reside on their sublattices within the first three or four unit cells of the film in the absence of oxygen vacancies. Theoretical calculations show that two-dimensional electron gas with three unit-cells at the Nb:STO/STO interface is formed by the charge transfer, which leads to the spontaneous formation of cation vacancies for charge compensation, and induces the lattice distortion as well. The results suggest that our EDX approach is useful for obtaining atomic-site-specific information on point defect chemistry with unparalleled precision, which facilitates a path towards atomically precise defect engineering.

Materials Today Physics, 16, 100302 (2021)