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Orbital Ordering of the Mobile and Localized Electrons at Oxygen-Deficient LaAlO3/SrTiO3 Interfaces

  • Alla Chikina*
    Alla Chikina
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
    *E-mail: [email protected]
    More by Alla Chikina
  • Frank Lechermann
    Frank Lechermann
    Institut für Theoretische Physik, Universität Hamburg, Jungiusstrasse 9, Hamburg DE-20355, Germany
  • Marius-Adrian Husanu
    Marius-Adrian Husanu
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
    National Institute of Materials Physics, Atomistilor 405A, Magurele RO-077125, Romania
  • Marco Caputo
    Marco Caputo
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
    More by Marco Caputo
  • Claudia Cancellieri
    Claudia Cancellieri
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
    Empa, Swiss Federal Laboratories for Materials Science & Technology, Ueberlandstrasse 129, Duebendorf CH-8600, Switzerland
  • Xiaoqiang Wang
    Xiaoqiang Wang
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
  • Thorsten Schmitt
    Thorsten Schmitt
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
  • Milan Radovic
    Milan Radovic
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
  • , and 
  • Vladimir N. Strocov*
    Vladimir N. Strocov
    Swiss Light Source, Paul Scherrer Institute, Villigen CH-5232, Switzerland
    *E-mail: [email protected]
Cite this: ACS Nano 2018, 12, 8, 7927–7935
Publication Date (Web):July 11, 2018
Copyright © 2018 American Chemical Society

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    Abstract Image

    Interfacing different transition-metal oxides opens a route to functionalizing their rich interplay of electron, spin, orbital, and lattice degrees of freedom for electronic and spintronic devices. Electronic and magnetic properties of SrTiO3-based interfaces hosting a mobile two-dimensional electron system (2DES) are strongly influenced by oxygen vacancies, which form an electronic dichotomy, where strongly correlated localized electrons in the in-gap states (IGSs) coexist with noncorrelated delocalized 2DES. Here, we use resonant soft-X-ray photoelectron spectroscopy to prove the eg character of the IGSs, as opposed to the t2g character of the 2DES in the paradigmatic LaAlO3/SrTiO3 interface. We furthermore separate the dxy and dxz/dxz orbital contributions based on deeper consideration of the resonant photoexcitation process in terms of orbital and momentum selectivity. Supported by a self-consistent combination of density functional theory and dynamical mean field theory calculations, this experiment identifies local orbital reconstruction that goes beyond the conventional eg-vs-t2g band ordering. A hallmark of oxygen-deficient LaAlO3/SrTiO3 is a significant hybridization of the eg and t2g orbitals. Our findings provide routes for tuning the electronic and magnetic properties of oxide interfaces through “defect engineering” with oxygen vacancies.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.8b02335.

    • DFT+DMFT calculations for the stoichiometric LAO–STO interface; ResPE map measured for LAO–STO and bare STO samples; DFT+DMFT calculations for the LAO–STO interface with VO in the SrO layer just below the interface TiO2 layer (PDF)

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