Cerium Oxides without U: The Role of Many-Electron Correlation

Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common parameter-dependent one-electron approaches, such as density functional theor...

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Detalles Bibliográficos
Autores: Schärfe, Tobias, Daelman, Nathan, López, Núria
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2021
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2072/450551
Acceso en línea:http://hdl.handle.net/2072/450551
https://doi.org/10.1021/acs.jpclett.1c01589
Access Level:acceso abierto
Palabra clave:54
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spelling Cerium Oxides without U: The Role of Many-Electron CorrelationSchärfe, TobiasDaelman, NathanLópez, Núria54Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common parameter-dependent one-electron approaches, such as density functional theory (DFT) with a Hubbard correction, or hybrid functionals. As a response, we present the first benchmark of ab initio many-electron theory for electron transfer energies and lattice parameters under periodic boundary conditions. We show that the direct random phase approximation clearly outperforms all DFT variations. From this foundation, we, then, systematically improve even further. Periodic second-order Møller–Plesset perturbation theory meanwhile manages to recover standard hybrid functional values. Using these approaches to eliminate parameter bias allows for highly accurate benchmarks of strongly correlated materials, the reliable assessment of various density functionals, and functional fitting via machine-learning.2021info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersion6277 p.application/pdfhttp://hdl.handle.net/2072/450551https://doi.org/10.1021/acs.jpclett.1c01589RECERCAT (Dipòsit de la Recerca de Catalunya)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésBES-2016-076361L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:recercat.cat:2072/4505512026-05-29T05:05:01Z
dc.title.none.fl_str_mv Cerium Oxides without U: The Role of Many-Electron Correlation
title Cerium Oxides without U: The Role of Many-Electron Correlation
spellingShingle Cerium Oxides without U: The Role of Many-Electron Correlation
Schärfe, Tobias
54
title_short Cerium Oxides without U: The Role of Many-Electron Correlation
title_full Cerium Oxides without U: The Role of Many-Electron Correlation
title_fullStr Cerium Oxides without U: The Role of Many-Electron Correlation
title_full_unstemmed Cerium Oxides without U: The Role of Many-Electron Correlation
title_sort Cerium Oxides without U: The Role of Many-Electron Correlation
dc.creator.none.fl_str_mv Schärfe, Tobias
Daelman, Nathan
López, Núria
author Schärfe, Tobias
author_facet Schärfe, Tobias
Daelman, Nathan
López, Núria
author_role author
author2 Daelman, Nathan
López, Núria
author2_role author
author
dc.subject.none.fl_str_mv 54
topic 54
description Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common parameter-dependent one-electron approaches, such as density functional theory (DFT) with a Hubbard correction, or hybrid functionals. As a response, we present the first benchmark of ab initio many-electron theory for electron transfer energies and lattice parameters under periodic boundary conditions. We show that the direct random phase approximation clearly outperforms all DFT variations. From this foundation, we, then, systematically improve even further. Periodic second-order Møller–Plesset perturbation theory meanwhile manages to recover standard hybrid functional values. Using these approaches to eliminate parameter bias allows for highly accurate benchmarks of strongly correlated materials, the reliable assessment of various density functionals, and functional fitting via machine-learning.
publishDate 2021
dc.date.none.fl_str_mv 2021
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/2072/450551
https://doi.org/10.1021/acs.jpclett.1c01589
url http://hdl.handle.net/2072/450551
https://doi.org/10.1021/acs.jpclett.1c01589
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv BES-2016-076361
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 6277 p.
application/pdf
dc.source.none.fl_str_mv RECERCAT (Dipòsit de la Recerca de Catalunya)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
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