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Title: Electronic-Structure Origin of Cation Disorder in Transition-Metal Oxides

Cation disorder is an important design criterion for technologically relevant transition-metal (TM) oxides, such as radiation-tolerant ceramics and Li-ion battery electrodes. In this Letter, we use a combination of first-principles calculations, normal mode analysis, and band-structure arguments to pinpoint a specific electronic-structure effect that influences the stability of disordered phases. We find that the electronic configuration of a TM ion determines to what extent the structural energy is affected by site distortions. In conclusion, this mechanism explains the stability of disordered phases with large ionic radius differences and provides a concrete guideline for the discovery of novel disordered compositions.
Authors:
 [1] ;  [2] ;  [2] ;  [1] ;  [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231; 7056411
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 119; Journal Issue: 17; Related Information: © 2017 us. Published by the American Physical Society.; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1476555
Alternate Identifier(s):
OSTI ID: 1404754

Urban, Alexander, Abdellahi, Aziz, Dacek, Stephen, Artrith, Nongnuch, and Ceder, Gerbrand. Electronic-Structure Origin of Cation Disorder in Transition-Metal Oxides. United States: N. p., Web. doi:10.1103/PhysRevLett.119.176402.
Urban, Alexander, Abdellahi, Aziz, Dacek, Stephen, Artrith, Nongnuch, & Ceder, Gerbrand. Electronic-Structure Origin of Cation Disorder in Transition-Metal Oxides. United States. doi:10.1103/PhysRevLett.119.176402.
Urban, Alexander, Abdellahi, Aziz, Dacek, Stephen, Artrith, Nongnuch, and Ceder, Gerbrand. 2017. "Electronic-Structure Origin of Cation Disorder in Transition-Metal Oxides". United States. doi:10.1103/PhysRevLett.119.176402. https://www.osti.gov/servlets/purl/1476555.
@article{osti_1476555,
title = {Electronic-Structure Origin of Cation Disorder in Transition-Metal Oxides},
author = {Urban, Alexander and Abdellahi, Aziz and Dacek, Stephen and Artrith, Nongnuch and Ceder, Gerbrand},
abstractNote = {Cation disorder is an important design criterion for technologically relevant transition-metal (TM) oxides, such as radiation-tolerant ceramics and Li-ion battery electrodes. In this Letter, we use a combination of first-principles calculations, normal mode analysis, and band-structure arguments to pinpoint a specific electronic-structure effect that influences the stability of disordered phases. We find that the electronic configuration of a TM ion determines to what extent the structural energy is affected by site distortions. In conclusion, this mechanism explains the stability of disordered phases with large ionic radius differences and provides a concrete guideline for the discovery of novel disordered compositions.},
doi = {10.1103/PhysRevLett.119.176402},
journal = {Physical Review Letters},
number = 17,
volume = 119,
place = {United States},
year = {2017},
month = {10}
}

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