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Cooperative effects of strain and electron correlation in epitaxial VO2 and NbO2

Wei-Cheng Lee, Matthew J. Wahila, , Christopher N. Singh, Tyler Eustance, Anna Regoutz, H. Paik, Jos E. Boschker, Fanny Rodolakis, Tien-Lin LeeShow More
Published in American Institute of Physics Inc.
2019
Volume: 125
   
Issue: 8
Abstract
We investigate the electronic structure of epitaxial VO 2 films in the rutile phase using density functional theory combined with the slave-spin method (DFT + SS). In DFT + SS, multi-orbital Hubbard interactions are added to a DFT-fit tight-binding model, and slave spins are used to treat electron correlations. We find that while stretching the system along the rutile c-axis results in a band structure favoring anisotropic orbital fillings, electron correlations favor equal filling of the t2g orbitals. These two distinct effects cooperatively induce an orbital-dependent redistribution of the electron occupations and spectral weights, driving strained VO 2 toward an orbital selective Mott transition (OSMT). The simulated single-particle spectral functions are directly compared to V L-edge resonant X-ray photoemission spectroscopy of epitaxial 10 nm VO 2/TiO 2 (001) and (100) strain orientations. Excellent agreement is observed between the simulations and experimental data regarding the strain-induced evolution of the lower Hubbard band. Simulations of rutile NbO 2 under similar strain conditions are performed, and we predict that an OSMT will not occur in rutile NbO 2. Our prediction is supported by the high-temperature hard x-ray photoelectron spectroscopy measurement on relaxed NbO 2 (110) thin films with no trace of the lower Hubbard band. Our results indicate that electron correlations in VO 2 are important and can be modulated even in the rutile phase before the Peierls instability sets in. © 2019 Author(s).
About the journal
JournalData powered by TypesetJournal of Applied Physics
PublisherData powered by TypesetAmerican Institute of Physics Inc.
Open AccessNo
Concepts (18)
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    Electron correlations
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    Electronic structure
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    Electrons
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    Niobium oxide
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    Oxide minerals
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    Photoelectron spectroscopy
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    Titanium dioxide
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    X ray photoelectron spectroscopy
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    X rays
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    CO-OPERATIVE EFFECTS
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    ELECTRON OCCUPATION
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    HARD X-RAY PHOTOELECTRON SPECTROSCOPY
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    HUBBARD INTERACTION
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    SINGLE-PARTICLE SPECTRAL FUNCTION
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    STRAIN ORIENTATIONS
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    Tight binding model
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    X ray photoemission spectroscopy
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    Density functional theory