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Cao, Shi ; Sinha, Kishan ; Zhang, Xin ; Zhang, Xiaozhe ; Wang, Xiao ; Yin, Yuewei ; N'Diaye, Alpha T. ; Wang, Jian ; Keavney, David J. ; Paudel, Tula R. ; et al ( , Physical Review B)
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Kaspar, Tiffany C. ; Sushko, Peter V. ; Spurgeon, Steven R. ; Bowden, Mark E. ; Keavney, David J. ; Comes, Ryan B. ; Saremi, Sahar ; Martin, Lane ; Chambers, Scott A. ( , Advanced Materials Interfaces)
Abstract The behavior of polar LaMnO3(LMO) thin films deposited epitaxially on nonpolar SrTiO3(001) (STO) is dictated by both the LMO/STO band alignment and the chemistry of the Mn cation. Using in situ X‐ray photoelectron spectroscopy, the valence band offset (VBO) of LMO/STO heterojunctions is directly measured as a function of thickness, and found that the VBO is 2.5 eV for thicker (≥3 u.c.) films. No evidence of a built‐in electric field in LMO films of any thickness is found. Measurements of the Mn valence by Mn
L ‐edge X‐ray absorption spectroscopy and by spatially resolved electron energy loss spectra in scanning transmission electron microscopy images reveal that Mn2+is present at the LMO surface, but not at the LMO/STO interface. These results are corroborated by density functional theory simulations that confirm a VBO of ≈2.5 eV for both ideal and intermixed interfaces. A model is proposed for the behavior of polar/nonpolar LMO/STO heterojunctions in which the polar catastrophe is alleviated by the formation of oxygen vacancies at the LMO surface.