Electron-phonon interactions in transition metal oxides in the framework of DFT+U

ORAL

Abstract

First-principles approaches for computing electron-phonon (e-ph) interactions enable quantitative studies in a wide range of solids. However, e-ph interactions in many transition-metal oxides (TMOs) remain challenging to treat due to the dominant on-site Coulomb repulsion from open-shell d electrons. Here we develop calculations of e-ph interactions within the framework of Hubbard-corrected density functional perturbation theory (so-called DFPT+U), which can describe the linear response of TMOs and provide an improved treatment of electron self-interactions. Employing a Hubbard U parameter computed ab initio, we demonstrate fully first-principles calculations of the e-ph coupling and the resulting electron spectral functions in various TMOs. While standard DFT e-ph calculations lead to unphysically divergent e-ph coupling, DFT+U restores the correct physics, giving well-behaved e-ph matrix elements that properly include the Frohlich interaction. Our results highlight the key role of the Hubbard U term on e-ph interactions. They further provide a broadly applicable method for predicting e-ph interactions and transport properties in TMOs with localized open-shell d electrons.

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Presenters

  • Jinsoo Park

    • Department of Applied Physics and Materials Science, California Institute of Technology
    • Caltech

Authors

  • Jinsoo Park

    • Department of Applied Physics and Materials Science, California Institute of Technology
    • Caltech

  • Jin-Jian Zhou

    • California Institute of Technology
    • Department of Applied Physics and Materials Science, California Institute of Technology
    • Caltech
    • Applied Physics & Materials Science, Caltech

  • Iurii Timrov

    • Ecole Polytechnique Federale de Lausanne
    • Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (E
    • Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL, CH-1015 Lausanne, Switzerland

  • Andrea Floris

    • School of Chemistry, University of Lincoln

  • Matteo Cococcioni

    • University of Pavia
    • Department of Physics, University of Pavia

  • Nicola Marzari

    • Ecole Polytechnique Federale de Lausanne
    • Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique Federale de Lausanne
    • École Polytechnique Fédérale de Lausanne
    • Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique Federale de Lausanne,
    • Theory and Simulation of Materials (THEOS), Faculté des Sciences et Techniques de l’Ingénieur, École Polytechnique Fédérale de Lausanne
    • THEOS, EPFL
    • École Polytechnique Fédérale de Lausanne (EPFL)
    • Theory and Simulation of Materials (THEOS) and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (E
    • Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL, CH-1015 Lausanne, Switzerland
    • Theory and simulation of materials (THEOS), National Centre for Computational Design and Discovery of Novel Materials (MARVEL), EPFL
    • Materials Engineering, EPFL
    • Theory and Simulations of Materials (THEOS), and National Center for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique Federale de Lausanne

  • Marco Bernardi

    • Caltech
    • California Institute of Technology
    • Department of Applied Physics and Materials Science, California Institute of Technology
    • Applied Physics & Materials Science, Caltech