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Title: Subtlety of TiO2 phase stability: Reliability of the density functional theory predictions and persistence of the self-interaction error

Abstract

TiO2 is an important material with broad applications that can exist in different phases with dramatically different properties. Theoretical prediction of their polymorph energetics is therefore critical for the material design and for identifying thermodynamically accessible structures. Determining TiO2 relative phase stabilities remains challenging for first-principles methods, and density functional theory is the only approach available for studying phase stabilities at finite temperatures with acceptable computational efficiency. Here, we show that density functional theory using the recently developed efficient strongly constrained and appropriately normed (SCAN) [Sun et al., Phys. Rev. Lett. 115, 036402 (2015)] exchange-correlation functional for the first time predicts the phase stability in qualitative agreement with the experimental results at realistic conditions. Further analysis shows that the self-interaction error intrinsic in the density functional persists in the stability prediction. By correcting the self-interaction error through an empirical approach, SCAN predicts the relative stability as well as defect properties in excellent agreement with the experimental results.

Authors:
 [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
  1. Tulane Univ., New Orleans, LA (United States); Dept. of Physics and Engineering Physics
  2. Xi’an Jiaotong Univ., Xi’an (China). State Key Laboratory of Electric Insulation and Power Equipment
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1543892
Grant/Contract Number:  
SC023502
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 150; Journal Issue: 1; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics

Citation Formats

Zhang, Yubo, Furness, James W., Xiao, Bing, and Sun, Jianwei. Subtlety of TiO2 phase stability: Reliability of the density functional theory predictions and persistence of the self-interaction error. United States: N. p., 2019. Web. doi:10.1063/1.5055623.
Zhang, Yubo, Furness, James W., Xiao, Bing, & Sun, Jianwei. Subtlety of TiO2 phase stability: Reliability of the density functional theory predictions and persistence of the self-interaction error. United States. doi:10.1063/1.5055623.
Zhang, Yubo, Furness, James W., Xiao, Bing, and Sun, Jianwei. Mon . "Subtlety of TiO2 phase stability: Reliability of the density functional theory predictions and persistence of the self-interaction error". United States. doi:10.1063/1.5055623. https://www.osti.gov/servlets/purl/1543892.
@article{osti_1543892,
title = {Subtlety of TiO2 phase stability: Reliability of the density functional theory predictions and persistence of the self-interaction error},
author = {Zhang, Yubo and Furness, James W. and Xiao, Bing and Sun, Jianwei},
abstractNote = {TiO2 is an important material with broad applications that can exist in different phases with dramatically different properties. Theoretical prediction of their polymorph energetics is therefore critical for the material design and for identifying thermodynamically accessible structures. Determining TiO2 relative phase stabilities remains challenging for first-principles methods, and density functional theory is the only approach available for studying phase stabilities at finite temperatures with acceptable computational efficiency. Here, we show that density functional theory using the recently developed efficient strongly constrained and appropriately normed (SCAN) [Sun et al., Phys. Rev. Lett. 115, 036402 (2015)] exchange-correlation functional for the first time predicts the phase stability in qualitative agreement with the experimental results at realistic conditions. Further analysis shows that the self-interaction error intrinsic in the density functional persists in the stability prediction. By correcting the self-interaction error through an empirical approach, SCAN predicts the relative stability as well as defect properties in excellent agreement with the experimental results.},
doi = {10.1063/1.5055623},
journal = {Journal of Chemical Physics},
number = 1,
volume = 150,
place = {United States},
year = {2019},
month = {1}
}

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    Works referencing / citing this record:

    Rationalizing accurate structure prediction in the meta-GGA SCAN functional
    journal, July 2019