Electronic Structure and Band Alignment of LaMnO3/SrTiO3 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

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

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

DOI:https://doi.org/10.1002/admi.201801428· OSTI ID:1494141

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Auburn Univ., Auburn, AL (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC02-06CH11357; 10122; SC0012375; AC02‐06CH11357; AC02-05CH11231

OSTI ID:: 1494141

Alternate ID(s):: OSTI ID: 1482745; OSTI ID: 1530317

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

Publisher:: Wiley-VCHCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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36 MATERIALS SCIENCE
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oxygen vacancies
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Title: Electronic Structure and Band Alignment of LaMnO3/SrTiO3 Polar/Nonpolar Heterojunctions

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