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Title: Origin of band gaps in 3d perovskite oxides

Abstract

With their broad range of properties, ABO3 transition metal perovskite oxides have long served as a platform for device applications and as a testing bed for different condensed matter theories. Their insulating character and structural distortions are often ascribed to dynamical electronic correlations within a universal, symmetry-conserving paradigm. This view restricts predictive theory to complex computational schemes, going beyond density functional theory (DFT). Here, we show that, if one allows symmetry-breaking energy-lowering crystal symmetry reductions and electronic instabilities within DFT, one successfully and systematically recovers the trends in the observed band gaps, magnetic moments, type of magnetic and crystallographic ground state, bond disproportionation and ligand hole effects, Mott vs. charge transfer insulator behaviors, and the amplitude of structural deformation modes including Jahn-Teller in low temperature spin-ordered and high temperature disordered paramagnetic phases. We then provide a classification of the four mechanisms of gap formation and establish DFT as a reliable base platform to study the ground state properties in complex oxides.

Authors:
 [1]; ORCiD logo [1];  [2]
  1. Univ. Paris-Saclay, Palaiseau (France). Mixed Unit Of Physics CNRS/Thales
  2. Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
Univ. of Colorado, Boulder, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1594114
Grant/Contract Number:  
FG02-13ER46959; SC0010467
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

Citation Formats

Varignon, Julien, Bibes, Manuel, and Zunger, Alex. Origin of band gaps in 3d perovskite oxides. United States: N. p., 2019. Web. doi:10.1038/s41467-019-09698-6.
Varignon, Julien, Bibes, Manuel, & Zunger, Alex. Origin of band gaps in 3d perovskite oxides. United States. doi:10.1038/s41467-019-09698-6.
Varignon, Julien, Bibes, Manuel, and Zunger, Alex. Wed . "Origin of band gaps in 3d perovskite oxides". United States. doi:10.1038/s41467-019-09698-6. https://www.osti.gov/servlets/purl/1594114.
@article{osti_1594114,
title = {Origin of band gaps in 3d perovskite oxides},
author = {Varignon, Julien and Bibes, Manuel and Zunger, Alex},
abstractNote = {With their broad range of properties, ABO3 transition metal perovskite oxides have long served as a platform for device applications and as a testing bed for different condensed matter theories. Their insulating character and structural distortions are often ascribed to dynamical electronic correlations within a universal, symmetry-conserving paradigm. This view restricts predictive theory to complex computational schemes, going beyond density functional theory (DFT). Here, we show that, if one allows symmetry-breaking energy-lowering crystal symmetry reductions and electronic instabilities within DFT, one successfully and systematically recovers the trends in the observed band gaps, magnetic moments, type of magnetic and crystallographic ground state, bond disproportionation and ligand hole effects, Mott vs. charge transfer insulator behaviors, and the amplitude of structural deformation modes including Jahn-Teller in low temperature spin-ordered and high temperature disordered paramagnetic phases. We then provide a classification of the four mechanisms of gap formation and establish DFT as a reliable base platform to study the ground state properties in complex oxides.},
doi = {10.1038/s41467-019-09698-6},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {4}
}

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Cited by: 11 works
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