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Dimensionality Controlled Octahedral Symmetry-Mismatch and Functionalities in Epitaxial LaCoO3/SrTiO3 Heterostructures
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    Dimensionality Controlled Octahedral Symmetry-Mismatch and Functionalities in Epitaxial LaCoO3/SrTiO3 Heterostructures
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    School of Materials, The University of Manchester, Manchester, M13 9PL, United Kingdom
    Center for Nanophase Materials Sciences and §Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    ∥ □ School of Physical Electronics, and Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Stanford University, Menlo Park, California 94025, United States
    #Chemical Science and Engineering Division and Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
    School of Materials Science and Engineering, University of New South Wales, Sydney, 2052, NSW Australia
    Laboratoire CRISMAT, CNRS UMR 6508, ENSICAEN, Normandie Université, 6 Bd Maréchal Juin, F-14050 Caen Cedex 4, France
    Department of Physics, Lanzhou City University, Lanzhou 730070, China
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    Nano Letters

    Cite this: Nano Lett. 2015, 15, 7, 4677–4684
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    https://doi.org/10.1021/acs.nanolett.5b01471
    Published June 23, 2015
    Copyright © 2015 American Chemical Society

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    Epitaxial strain provides a powerful approach to manipulate physical properties of materials through rigid compression or extension of their chemical bonds via lattice-mismatch. Although symmetry-mismatch can lead to new physics by stabilizing novel interfacial structures, challenges in obtaining atomic-level structural information as well as lack of a suitable approach to separate it from the parasitical lattice-mismatch have limited the development of this field. Here, we present unambiguous experimental evidence that the symmetry-mismatch can be strongly controlled by dimensionality and significantly impact the collective electronic and magnetic functionalities in ultrathin perovskite LaCoO3/SrTiO3 heterojunctions. State-of-art diffraction and microscopy reveal that symmetry breaking dramatically modifies the interfacial structure of CoO6 octahedral building-blocks, resulting in expanded octahedron volume, reduced covalent screening, and stronger electron correlations. Such phenomena fundamentally alter the electronic and magnetic behaviors of LaCoO3 thin-films. We conclude that for epitaxial systems, correlation strength can be tuned by changing orbital hybridization, thus affecting the Coulomb repulsion, U, instead of by changing the band structure as the common paradigm in bulks. These results clarify the origin of magnetic ordering for epitaxial LaCoO3 and provide a route to manipulate electron correlation and magnetic functionality by orbital engineering at oxide heterojunctions.

    Copyright © 2015 American Chemical Society

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    Additional information regarding experimental/theoretical details as well as structural and property characterizations. The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.5b01471.

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    Nano Letters

    Cite this: Nano Lett. 2015, 15, 7, 4677–4684
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.5b01471
    Published June 23, 2015
    Copyright © 2015 American Chemical Society

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