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Electronic Structure and Band Alignment of LaMnO3/SrTiO3 Polar/Nonpolar Heterojunctions

  • Author(s): Kaspar, TC
  • Sushko, PV
  • Spurgeon, SR
  • Bowden, ME
  • Keavney, DJ
  • Comes, RB
  • Saremi, S
  • Martin, L
  • Chambers, SA
  • et al.

© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 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.

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