Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3

Autores
Abia, Carmen; Lopez, Carlos Alberto; Cañadillas Delgado, Laura; Fernández Diaz, María T.; Alonso, José A.
Año de publicación
2022
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Methylammonium (MA) lead trihalide perovskites, CH3NH3PbX3 (X = I, Br, Cl), have emerged as a new class of light-absorbing materials for photovoltaic applications, reaching efficiencies of 23% when implemented in solar cell heterojunctions. In particular, MAPbBr3 is a promising member with a large bandgap that gives rise to a high open circuit voltage. Here we present a structural study from neutron diffraction (ND) data of an undeuterated MAPbBr3 specimen, carried out to follow its crystallographic behaviour in the 2–298 K temperature range. Besides the known crystallographic phases, i.e. the high-temperature Pm3 ¯ m cubic structure, the intermediate I4/mcm tetragonal symmetry and the low-temperature Pnma orthorhombic phase, we additionally identified, from a detailed sequential ND analysis, a novel intermediate phase within the 148.5–154.0 K temperature range as an orthorhombic Imma structure, early associated with a coexistence of phases. Moreover, our ND data allowed us to unveil the configuration of the organic MA units and their complete localization within the mentioned temperature range, thus improving the crystallographic description of this compound. The evolution with temperature of the H-bonds between the organic molecule and the inorganic cage is also followed. A deep knowledge of the crystal structure and, in particular, the MA conformation inside the perovskite cage seems essential to establish structure–property correlations that may drive further improvements.
Fil: Abia, Carmen. Institut Laue Langevin; Francia. Instituto de Ciencia de Materiales de Madrid; España
Fil: Lopez, Carlos 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: Cañadillas Delgado, Laura. Institut Laue Langevin; Francia
Fil: Fernández Diaz, María T.. Institut Laue Langevin; Francia
Fil: Alonso, José A.. Instituto de Ciencia de Materiales de Madrid; España
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/210487
Acceder
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network_name_str CONICET Digital (CONICET)
spelling Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3Abia, CarmenLopez, Carlos AlbertoCañadillas Delgado, LauraFernández Diaz, María T.Alonso, José A.https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Methylammonium (MA) lead trihalide perovskites, CH3NH3PbX3 (X = I, Br, Cl), have emerged as a new class of light-absorbing materials for photovoltaic applications, reaching efficiencies of 23% when implemented in solar cell heterojunctions. In particular, MAPbBr3 is a promising member with a large bandgap that gives rise to a high open circuit voltage. Here we present a structural study from neutron diffraction (ND) data of an undeuterated MAPbBr3 specimen, carried out to follow its crystallographic behaviour in the 2–298 K temperature range. Besides the known crystallographic phases, i.e. the high-temperature Pm3 ¯ m cubic structure, the intermediate I4/mcm tetragonal symmetry and the low-temperature Pnma orthorhombic phase, we additionally identified, from a detailed sequential ND analysis, a novel intermediate phase within the 148.5–154.0 K temperature range as an orthorhombic Imma structure, early associated with a coexistence of phases. Moreover, our ND data allowed us to unveil the configuration of the organic MA units and their complete localization within the mentioned temperature range, thus improving the crystallographic description of this compound. The evolution with temperature of the H-bonds between the organic molecule and the inorganic cage is also followed. A deep knowledge of the crystal structure and, in particular, the MA conformation inside the perovskite cage seems essential to establish structure–property correlations that may drive further improvements.Fil: Abia, Carmen. Institut Laue Langevin; Francia. Instituto de Ciencia de Materiales de Madrid; EspañaFil: Lopez, Carlos 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: Cañadillas Delgado, Laura. Institut Laue Langevin; FranciaFil: Fernández Diaz, María T.. Institut Laue Langevin; FranciaFil: Alonso, José A.. Instituto de Ciencia de Materiales de Madrid; EspañaNature2022-12info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/210487Abia, Carmen; Lopez, Carlos Alberto; Cañadillas Delgado, Laura; Fernández Diaz, María T.; Alonso, José A.; Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3; Nature; Scientific Reports; 12; 1; 12-2022; 1-142045-2322CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1038/s41598-022-21544-2info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:54:34Zoai:ri.conicet.gov.ar:11336/210487instacron: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:34982025-09-29 09:54:35.203CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
title Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
spellingShingle Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
Abia, Carmen
title_short Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
title_full Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
title_fullStr Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
title_full_unstemmed Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
title_sort Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3
dc.creator.none.fl_str_mv Abia, Carmen
Lopez, Carlos Alberto
Cañadillas Delgado, Laura
Fernández Diaz, María T.
Alonso, José A.
author Abia, Carmen
author_facet Abia, Carmen
Lopez, Carlos Alberto
Cañadillas Delgado, Laura
Fernández Diaz, María T.
Alonso, José A.
author_role author
author2 Lopez, Carlos Alberto
Cañadillas Delgado, Laura
Fernández Diaz, María T.
Alonso, José A.
author2_role author
author
author
author
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Methylammonium (MA) lead trihalide perovskites, CH3NH3PbX3 (X = I, Br, Cl), have emerged as a new class of light-absorbing materials for photovoltaic applications, reaching efficiencies of 23% when implemented in solar cell heterojunctions. In particular, MAPbBr3 is a promising member with a large bandgap that gives rise to a high open circuit voltage. Here we present a structural study from neutron diffraction (ND) data of an undeuterated MAPbBr3 specimen, carried out to follow its crystallographic behaviour in the 2–298 K temperature range. Besides the known crystallographic phases, i.e. the high-temperature Pm3 ¯ m cubic structure, the intermediate I4/mcm tetragonal symmetry and the low-temperature Pnma orthorhombic phase, we additionally identified, from a detailed sequential ND analysis, a novel intermediate phase within the 148.5–154.0 K temperature range as an orthorhombic Imma structure, early associated with a coexistence of phases. Moreover, our ND data allowed us to unveil the configuration of the organic MA units and their complete localization within the mentioned temperature range, thus improving the crystallographic description of this compound. The evolution with temperature of the H-bonds between the organic molecule and the inorganic cage is also followed. A deep knowledge of the crystal structure and, in particular, the MA conformation inside the perovskite cage seems essential to establish structure–property correlations that may drive further improvements.
Fil: Abia, Carmen. Institut Laue Langevin; Francia. Instituto de Ciencia de Materiales de Madrid; España
Fil: Lopez, Carlos 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: Cañadillas Delgado, Laura. Institut Laue Langevin; Francia
Fil: Fernández Diaz, María T.. Institut Laue Langevin; Francia
Fil: Alonso, José A.. Instituto de Ciencia de Materiales de Madrid; España
description Methylammonium (MA) lead trihalide perovskites, CH3NH3PbX3 (X = I, Br, Cl), have emerged as a new class of light-absorbing materials for photovoltaic applications, reaching efficiencies of 23% when implemented in solar cell heterojunctions. In particular, MAPbBr3 is a promising member with a large bandgap that gives rise to a high open circuit voltage. Here we present a structural study from neutron diffraction (ND) data of an undeuterated MAPbBr3 specimen, carried out to follow its crystallographic behaviour in the 2–298 K temperature range. Besides the known crystallographic phases, i.e. the high-temperature Pm3 ¯ m cubic structure, the intermediate I4/mcm tetragonal symmetry and the low-temperature Pnma orthorhombic phase, we additionally identified, from a detailed sequential ND analysis, a novel intermediate phase within the 148.5–154.0 K temperature range as an orthorhombic Imma structure, early associated with a coexistence of phases. Moreover, our ND data allowed us to unveil the configuration of the organic MA units and their complete localization within the mentioned temperature range, thus improving the crystallographic description of this compound. The evolution with temperature of the H-bonds between the organic molecule and the inorganic cage is also followed. A deep knowledge of the crystal structure and, in particular, the MA conformation inside the perovskite cage seems essential to establish structure–property correlations that may drive further improvements.
publishDate 2022
dc.date.none.fl_str_mv 2022-12
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/11336/210487
Abia, Carmen; Lopez, Carlos Alberto; Cañadillas Delgado, Laura; Fernández Diaz, María T.; Alonso, José A.; Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3; Nature; Scientific Reports; 12; 1; 12-2022; 1-14
2045-2322
CONICET Digital
CONICET
url http://hdl.handle.net/11336/210487
identifier_str_mv Abia, Carmen; Lopez, Carlos Alberto; Cañadillas Delgado, Laura; Fernández Diaz, María T.; Alonso, José A.; Crystal structure thermal evolution and novel orthorhombic phase of methylammonium lead bromide, CH3NH3PbBr3; Nature; Scientific Reports; 12; 1; 12-2022; 1-14
2045-2322
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1038/s41598-022-21544-2
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Nature
publisher.none.fl_str_mv Nature
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
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score 13.070432

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