Electronic Structure and Band Alignment of LaMnO 3 /SrTiO 3 Polar/Nonpolar Heterojunctions

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.

doi:10.1002/admi.201801428

Electronic Structure and Band Alignment of LaMnO ₃ /SrTiO ₃ Polar/Nonpolar Heterojunctions

Journal Article · Mon Nov 19 04:00:00 EST 2018 · Advanced Materials Interfaces

DOI:https://doi.org/10.1002/admi.201801428· OSTI ID:1506987

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Physical and Computational Sciences DirectoratePacific Northwest National Laboratory Richland WA 99354 USA
Energy and Environment DirectoratePacific Northwest National Laboratory Richland WA 99354 USA
Environmental Molecular Sciences LaboratoryPacific Northwest National Laboratory Richland WA 99354 USA
Advanced Photon SourceArgonne National Laboratory Argonne IL 60439 USA
Department of PhysicsAuburn University Auburn AL 36849 USA
Department of Materials Science and EngineeringUniversity of California Berkeley CA 94720 USA
Department of Materials Science and EngineeringUniversity of California Berkeley CA 94720 USA; Materials Sciences DivisionLawrence Berkeley National Laboratory Berkeley CA 94720 USA

The behavior of polar LaMnO3 (LMO) thin films deposited epitaxially on non-polar 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 spectros-copy (XPS), we directly measure the valence band offset (VBO) of LMO/STO heterojunctions as a function of thickness, and find that the VBO is 2.5 eV for thicker (= 3 u.c.) films. We find no evidence of a built-in potential in LMO films of any thickness. Measurements of the Mn valence by Mn L-edge x-ray absorption spectroscopy (XAS) and by spatially-resolved electron energy loss spectra in scanning transmission electron microscopy images (STEM-EELS) reveal that Mn2+ is present at the LMO surface, but not at the LMO/STO interface. These results are corroborated by DFT simula-tions that confirm a VBO of approximately 2.5 eV for both ideal and intermixed interfaces. We propose a model for the behavior of polar / non-polar LMO/STO heterojunctions in which the built-in potential is alleviated by the formation of oxygen vacancies at the LMO surface.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1506987

Report Number(s):: PNNL-SA-137669

Journal Information:: Advanced Materials Interfaces, Journal Name: Advanced Materials Interfaces Journal Issue: 1 Vol. 6; ISSN 2196-7350

Publisher:: Wiley-VCH

Country of Publication:: United States

Language:: English

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