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Toward a Consistent Prediction of Defect Chemistry in CeO2

Zhang, Xingfan; Zhu, Lei; Hou, Qing; Guan, Jingcheng; Lu, You; Keal, Thomas W; Buckeridge, John; ... Sokol, Alexey A; + view all (2022) Toward a Consistent Prediction of Defect Chemistry in CeO2. Chemistry of Materials 10.1021/acs.chemmater.2c03019. Green open access

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Abstract

Polarizable shell-model potentials are widely used for atomic-scale modeling of charged defects in solids using the Mott−Littleton approach and hybrid Quantum Mechanical/ Molecular Mechanical (QM/MM) embedded-cluster techniques. However, at the pure MM level of theory, the calculated defect energetics may not satisfy the requirement of quantitative predictions and are limited to only certain charged states. Here, we proposed a novel interatomic potential development scheme that unifies the predictions of all relevant charged defects in CeO2 based on the Mott−Littleton approach and QM/MM electronicstructure calculations. The predicted formation energies of oxygen vacancies accompanied by different excess electron localization patterns at the MM level of theory reach the accuracy of density functional theory (DFT) calculations using hybrid functionals. The new potential also accurately reproduces a wide range of physical properties of CeO2, showing excellent agreement with experimental and other computational studies. These findings provide opportunities for accurate large-scale modeling of the partial reduction and nonstoichiometry in CeO2, as well as a prototype for developing robust interatomic potentials for other defective crystals.

Type: Article
Title: Toward a Consistent Prediction of Defect Chemistry in CeO2
Open access status: An open access version is available from UCL Discovery
DOI: 10.1021/acs.chemmater.2c03019
Publisher version: https://doi.org/10.1021/acs.chemmater.2c03019
Language: English
Additional information: © 2022 The Authors. Published by American Chemical Society. This is an open access article under the CC BY 4.0 license Attribution 4.0 International (https://creativecommons.org/licenses/by/4.0/)
Keywords: Chemical calculations, Defects, Defects in solids, Energy, QM/MM
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10162438
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