Thickness Dependent Properties in Oxide Heterostructures Driven by Structurally Induced Metal–Oxygen Hybridization Variations |
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| Authors: | Zhaoliang Liao Nicolas Gauquelin Robert J. Green Sebastian Macke Julie Gonnissen Sean Thomas Zhicheng Zhong Lin Li Liang Si Sandra Van Aert Philipp Hansmann Karsten Held Jing Xia Johan Verbeeck Gustaaf Van Tendeloo George A. Sawatzky Gertjan Koster Mark Huijben Guus Rijnders |
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| Affiliation: | 1. MESA+ Institute for Nanotechnology, University of Twente, AE, Enschede, The Netherlands;2. Electron Microscopy for Materials Science (EMAT), University of Antwerp, Antwerp, Belgium;3. Quantum Matter Institute and Department of Physics and Astronomy, University of British Columbia, Vancouver, Canada;4. Max Planck Institute for Chemical Physics of Solids, Dresden, Germany;5. Max Planck Institute for Solid State Research, Stuttgart, Germany;6. Department of Physics and Astronomy, University of California, Irvine, Irvine, CA, USA;7. Institute of Solid State Physics, TU WIEN, Vienna, Austria |
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| Abstract: | Thickness‐driven electronic phase transitions are broadly observed in different types of functional perovskite heterostructures. However, uncertainty remains whether these effects are solely due to spatial confinement, broken symmetry, or rather to a change of structure with varying film thickness. Here, this study presents direct evidence for the relaxation of oxygen‐2p and Mn‐3d orbital (p–d) hybridization coupled to the layer‐dependent octahedral tilts within a La2/3Sr1/3MnO3 film driven by interfacial octahedral coupling. An enhanced Curie temperature is achieved by reducing the octahedral tilting via interface structure engineering. Atomically resolved lattice, electronic, and magnetic structures together with X‐ray absorption spectroscopy demonstrate the central role of thickness‐dependent p–d hybridization in the widely observed dimensionality effects present in correlated oxide heterostructures. |
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| Keywords: | interfaces manganites metal– oxygen hybridization oxide heterostructures oxygen octahedral couplings |
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