Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6

Autores
Larregola, Sebastian Alberto; Alonso, José A.; de la Peña O'Shea, Victor A.; Sheptyakov, Denis; Pomjakushin, Vladimir; Fernandez Díaz, María T.; Pedregosa, Jose Carmelo
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The synthesis and crystal structure evolution of the double perovskite Pb2YSbO6 is reported for the first time. The structure has been analyzed in the temperature range between 100 and 500 K by using a combination of synchrotron and neutron powder diffraction. This compound shows two consecutive first order phase transformations as previously observed for a subgroup of Pb2RSbO6 perovkites (R = rare earths). The thermodynamic parameters associated with the phase transitions were calculated using differential scanning calorimetry (DSC), and the role of the diverse cations of the structure was studied from DFT calculations for the room temperature polymorph. The crystal structure evolves from a C2/c monoclinic structure (a–b–b– tilting system in Glazer’s notation) to another monoclinic P21/n (a–a–b+) phase with an incommensurate modulation and finally to a cubic Fm3̅m perovskite (a0a0a0). The highly distorted nature of the room temperature crystal structure seems to be driven by the polarization of the Pb lone pair which shows a marked local effect in the atomic spatial arrangements. Moreover, the lone pairs have been localized from DFT calculations and show an antiferroelectric ordering along the b monoclinic axis.
Fil: Larregola, Sebastian Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; Argentina
Fil: Alonso, José A.. Instituto de Ciencia de Materiales de Madrid; España
Fil: de la Peña O'Shea, Victor A.. IMDEA Energy Institute; España
Fil: Sheptyakov, Denis. Laboratory for Neutron Scattering; Suiza
Fil: Pomjakushin, Vladimir. Paul Scherrer Institute; Suiza
Fil: Fernandez Díaz, María T.. Institut Max Von Laue Paul Langevin; Francia
Fil: Pedregosa, Jose Carmelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; Argentina
Materia
Perovskite
Electronic Structure
Lone Pair
Non Bonded Electron Pair
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/32219
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/32219
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6Larregola, Sebastian AlbertoAlonso, José A.de la Peña O'Shea, Victor A.Sheptyakov, DenisPomjakushin, VladimirFernandez Díaz, María T.Pedregosa, Jose CarmeloPerovskiteElectronic StructureLone PairNon Bonded Electron Pairhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The synthesis and crystal structure evolution of the double perovskite Pb2YSbO6 is reported for the first time. The structure has been analyzed in the temperature range between 100 and 500 K by using a combination of synchrotron and neutron powder diffraction. This compound shows two consecutive first order phase transformations as previously observed for a subgroup of Pb2RSbO6 perovkites (R = rare earths). The thermodynamic parameters associated with the phase transitions were calculated using differential scanning calorimetry (DSC), and the role of the diverse cations of the structure was studied from DFT calculations for the room temperature polymorph. The crystal structure evolves from a C2/c monoclinic structure (a–b–b– tilting system in Glazer’s notation) to another monoclinic P21/n (a–a–b+) phase with an incommensurate modulation and finally to a cubic Fm3̅m perovskite (a0a0a0). The highly distorted nature of the room temperature crystal structure seems to be driven by the polarization of the Pb lone pair which shows a marked local effect in the atomic spatial arrangements. Moreover, the lone pairs have been localized from DFT calculations and show an antiferroelectric ordering along the b monoclinic axis.Fil: Larregola, Sebastian Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; ArgentinaFil: Alonso, José A.. Instituto de Ciencia de Materiales de Madrid; EspañaFil: de la Peña O'Shea, Victor A.. IMDEA Energy Institute; EspañaFil: Sheptyakov, Denis. Laboratory for Neutron Scattering; SuizaFil: Pomjakushin, Vladimir. Paul Scherrer Institute; SuizaFil: Fernandez Díaz, María T.. Institut Max Von Laue Paul Langevin; FranciaFil: Pedregosa, Jose Carmelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; ArgentinaAmerican Chemical Society2014-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/32219de la Peña O'Shea, Victor A.; Alonso, José A.; Larregola, Sebastian Alberto; Sheptyakov, Denis; Fernandez Díaz, María T.; Pomjakushin, Vladimir; et al.; Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6; American Chemical Society; Inorganic Chemistry; 53; 11; 5-2014; 5609-56180020-1669CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/ic500278yinfo:eu-repo/semantics/altIdentifier/doi/10.1021/ic500278yinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:01:52Zoai:ri.conicet.gov.ar:11336/32219instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-03 10:01:52.298CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
title Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
spellingShingle Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
Larregola, Sebastian Alberto
Perovskite
Electronic Structure
Lone Pair
Non Bonded Electron Pair
title_short Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
title_full Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
title_fullStr Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
title_full_unstemmed Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
title_sort Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6
dc.creator.none.fl_str_mv Larregola, Sebastian Alberto
Alonso, José A.
de la Peña O'Shea, Victor A.
Sheptyakov, Denis
Pomjakushin, Vladimir
Fernandez Díaz, María T.
Pedregosa, Jose Carmelo
author Larregola, Sebastian Alberto
author_facet Larregola, Sebastian Alberto
Alonso, José A.
de la Peña O'Shea, Victor A.
Sheptyakov, Denis
Pomjakushin, Vladimir
Fernandez Díaz, María T.
Pedregosa, Jose Carmelo
author_role author
author2 Alonso, José A.
de la Peña O'Shea, Victor A.
Sheptyakov, Denis
Pomjakushin, Vladimir
Fernandez Díaz, María T.
Pedregosa, Jose Carmelo
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv Perovskite
Electronic Structure
Lone Pair
Non Bonded Electron Pair
topic Perovskite
Electronic Structure
Lone Pair
Non Bonded Electron Pair
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The synthesis and crystal structure evolution of the double perovskite Pb2YSbO6 is reported for the first time. The structure has been analyzed in the temperature range between 100 and 500 K by using a combination of synchrotron and neutron powder diffraction. This compound shows two consecutive first order phase transformations as previously observed for a subgroup of Pb2RSbO6 perovkites (R = rare earths). The thermodynamic parameters associated with the phase transitions were calculated using differential scanning calorimetry (DSC), and the role of the diverse cations of the structure was studied from DFT calculations for the room temperature polymorph. The crystal structure evolves from a C2/c monoclinic structure (a–b–b– tilting system in Glazer’s notation) to another monoclinic P21/n (a–a–b+) phase with an incommensurate modulation and finally to a cubic Fm3̅m perovskite (a0a0a0). The highly distorted nature of the room temperature crystal structure seems to be driven by the polarization of the Pb lone pair which shows a marked local effect in the atomic spatial arrangements. Moreover, the lone pairs have been localized from DFT calculations and show an antiferroelectric ordering along the b monoclinic axis.
Fil: Larregola, Sebastian Alberto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; Argentina
Fil: Alonso, José A.. Instituto de Ciencia de Materiales de Madrid; España
Fil: de la Peña O'Shea, Victor A.. IMDEA Energy Institute; España
Fil: Sheptyakov, Denis. Laboratory for Neutron Scattering; Suiza
Fil: Pomjakushin, Vladimir. Paul Scherrer Institute; Suiza
Fil: Fernandez Díaz, María T.. Institut Max Von Laue Paul Langevin; Francia
Fil: Pedregosa, Jose Carmelo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - San Luis. Instituto de Investigaciones en Tecnología Química. Universidad Nacional de San Luis. Facultad de Química, Bioquímica y Farmacia. Instituto de Investigaciones en Tecnología Química; Argentina
description The synthesis and crystal structure evolution of the double perovskite Pb2YSbO6 is reported for the first time. The structure has been analyzed in the temperature range between 100 and 500 K by using a combination of synchrotron and neutron powder diffraction. This compound shows two consecutive first order phase transformations as previously observed for a subgroup of Pb2RSbO6 perovkites (R = rare earths). The thermodynamic parameters associated with the phase transitions were calculated using differential scanning calorimetry (DSC), and the role of the diverse cations of the structure was studied from DFT calculations for the room temperature polymorph. The crystal structure evolves from a C2/c monoclinic structure (a–b–b– tilting system in Glazer’s notation) to another monoclinic P21/n (a–a–b+) phase with an incommensurate modulation and finally to a cubic Fm3̅m perovskite (a0a0a0). The highly distorted nature of the room temperature crystal structure seems to be driven by the polarization of the Pb lone pair which shows a marked local effect in the atomic spatial arrangements. Moreover, the lone pairs have been localized from DFT calculations and show an antiferroelectric ordering along the b monoclinic axis.
publishDate 2014
dc.date.none.fl_str_mv 2014-05
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/32219
de la Peña O'Shea, Victor A.; Alonso, José A.; Larregola, Sebastian Alberto; Sheptyakov, Denis; Fernandez Díaz, María T.; Pomjakushin, Vladimir; et al.; Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6; American Chemical Society; Inorganic Chemistry; 53; 11; 5-2014; 5609-5618
0020-1669
CONICET Digital
CONICET
url http://hdl.handle.net/11336/32219
identifier_str_mv de la Peña O'Shea, Victor A.; Alonso, José A.; Larregola, Sebastian Alberto; Sheptyakov, Denis; Fernandez Díaz, María T.; Pomjakushin, Vladimir; et al.; Localization and Impact of Pb-Non-Bonded Electronic Pair on the Crystal and Electronic Structure of Pb2YSbO6; American Chemical Society; Inorganic Chemistry; 53; 11; 5-2014; 5609-5618
0020-1669
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/ic500278y
info:eu-repo/semantics/altIdentifier/doi/10.1021/ic500278y
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
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:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
_version_ 1842269722541817856
score 12.885934

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