Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods

Progress in the design of functional perovskite oxides relies on advances in density functional theory (DFT) methods to efficiently and effectively model complex systems composed of several transition-metal ions. This work reports the application of DFT methods to investigate the electronic structur...

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Autores: Gómez-Toledo, Marianela, López Paz, Sara Almudena, García Martín, Susana, Arroyo De Dompablo, María Elena
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:Universidad Complutense de Madrid (UCM)
Repositorio:Docta Complutense
Idioma:inglés
OAI Identifier:oai:docta.ucm.es:20.500.14352/73017
Acceso en línea:https://hdl.handle.net/20.500.14352/73017
Access Level:acceso abierto
Palabra clave:546
Química
Informática (Química)
Materiales
Química inorgánica (Química)
23 Química
3312 Tecnología de Materiales
2303 Química Inorgánica
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spelling Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT MethodsGómez-Toledo, MarianelaLópez Paz, Sara AlmudenaGarcía Martín, SusanaArroyo De Dompablo, María Elena546QuímicaInformática (Química)MaterialesQuímica inorgánica (Química)23 Química3312 Tecnología de Materiales2303 Química InorgánicaProgress in the design of functional perovskite oxides relies on advances in density functional theory (DFT) methods to efficiently and effectively model complex systems composed of several transition-metal ions. This work reports the application of DFT methods to investigate the electronic structure of the YSr2Cu2FeO8−δ (0 < δ < 1) family in which the insulating, metal, or superconducting behaviors and even anion conductivity can be tuned by modifying the oxygen content. In particular, we assess the performance of the generalized gradient approximation (GGA), its Hubbard-U correction (GGA + U), and the strongly constrained and appropriately normed (SCAN) to model the metallic (idealized YSr2Cu2FeO8) and insulating (idealized YSr2Cu2FeO7) phases of the system. The analysis of the DFT results is supported by DC resistivity measurements that denote the metal character of the synthesized YSr2Cu2FeO7.86 and the semiconducting character of YSr2Cu2FeO7.08 prepared under reducing conditions. In addition, the band gap of YSr2Cu2FeO7.08, in the range of 0.73−1.2 eV, has been extracted from diffuse reflectance spectroscopy (DRS). While the three methodologies (GGA, GGA + U, SCAN) permit the reproduction of the crystal structures of the synthetized oxides (determined here in the case of YSr2Cu2FeO7.08 by neutron powder diffraction (NPD)), the SCAN emerges as the only one capable to predict the basic electronic and magnetic properties across the YSr2Cu2FeO8−δ (0 < δ < 1) series. The picture that emerges for the metal (δ = 0) to insulating (δ = 1) transition is the one in which oxygen vacancies contribute electrons to the filling of the Cu/Fe-3dx2−y2 states of the conduction band. These results validate the SCAN functional for future DFT investigations of complex functional oxides that combine severaltransition metals.American Chemical SocietyUniversidad Complutense de Madrid20232023-01-0120232023-01-01journal articlehttp://purl.org/coar/resource_type/c_6501info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/20.500.14352/73017reponame:Docta Complutenseinstname:Universidad Complutense de Madrid (UCM)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2Atribución-NoComercial 3.0 Españahttps://creativecommons.org/licenses/by-nc/3.0/es/info:eu-repo/semantics/openAccessoai:docta.ucm.es:20.500.14352/730172026-06-02T12:44:21Z
dc.title.none.fl_str_mv Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
title Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
spellingShingle Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
Gómez-Toledo, Marianela
546
Química
Informática (Química)
Materiales
Química inorgánica (Química)
23 Química
3312 Tecnología de Materiales
2303 Química Inorgánica
title_short Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
title_full Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
title_fullStr Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
title_full_unstemmed Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
title_sort Metal-to-Insulating Transition in the Perovskite System YSr2Cu2FeO8−δ (0 < δ < 1) Modeled by DFT Methods
dc.creator.none.fl_str_mv Gómez-Toledo, Marianela
López Paz, Sara Almudena
García Martín, Susana
Arroyo De Dompablo, María Elena
author Gómez-Toledo, Marianela
author_facet Gómez-Toledo, Marianela
López Paz, Sara Almudena
García Martín, Susana
Arroyo De Dompablo, María Elena
author_role author
author2 López Paz, Sara Almudena
García Martín, Susana
Arroyo De Dompablo, María Elena
author2_role author
author
author
dc.contributor.none.fl_str_mv Universidad Complutense de Madrid
dc.subject.none.fl_str_mv 546
Química
Informática (Química)
Materiales
Química inorgánica (Química)
23 Química
3312 Tecnología de Materiales
2303 Química Inorgánica
topic 546
Química
Informática (Química)
Materiales
Química inorgánica (Química)
23 Química
3312 Tecnología de Materiales
2303 Química Inorgánica
description Progress in the design of functional perovskite oxides relies on advances in density functional theory (DFT) methods to efficiently and effectively model complex systems composed of several transition-metal ions. This work reports the application of DFT methods to investigate the electronic structure of the YSr2Cu2FeO8−δ (0 < δ < 1) family in which the insulating, metal, or superconducting behaviors and even anion conductivity can be tuned by modifying the oxygen content. In particular, we assess the performance of the generalized gradient approximation (GGA), its Hubbard-U correction (GGA + U), and the strongly constrained and appropriately normed (SCAN) to model the metallic (idealized YSr2Cu2FeO8) and insulating (idealized YSr2Cu2FeO7) phases of the system. The analysis of the DFT results is supported by DC resistivity measurements that denote the metal character of the synthesized YSr2Cu2FeO7.86 and the semiconducting character of YSr2Cu2FeO7.08 prepared under reducing conditions. In addition, the band gap of YSr2Cu2FeO7.08, in the range of 0.73−1.2 eV, has been extracted from diffuse reflectance spectroscopy (DRS). While the three methodologies (GGA, GGA + U, SCAN) permit the reproduction of the crystal structures of the synthetized oxides (determined here in the case of YSr2Cu2FeO7.08 by neutron powder diffraction (NPD)), the SCAN emerges as the only one capable to predict the basic electronic and magnetic properties across the YSr2Cu2FeO8−δ (0 < δ < 1) series. The picture that emerges for the metal (δ = 0) to insulating (δ = 1) transition is the one in which oxygen vacancies contribute electrons to the filling of the Cu/Fe-3dx2−y2 states of the conduction band. These results validate the SCAN functional for future DFT investigations of complex functional oxides that combine severaltransition metals.
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-01-01
2023
2023-01-01
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/20.500.14352/73017
url https://hdl.handle.net/20.500.14352/73017
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Atribución-NoComercial 3.0 España
https://creativecommons.org/licenses/by-nc/3.0/es/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Atribución-NoComercial 3.0 España
https://creativecommons.org/licenses/by-nc/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv reponame:Docta Complutense
instname:Universidad Complutense de Madrid (UCM)
instname_str Universidad Complutense de Madrid (UCM)
reponame_str Docta Complutense
collection Docta Complutense
repository.name.fl_str_mv
repository.mail.fl_str_mv
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