Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4

Autores
Lasave, Jorge Augusto; Koval, Sergio Fabian; Migoni, Ricardo Luis; Dalal, N. S.
Año de publicación
2011
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A study of differently polarized structures relevant to the H-bonded antiferroelectric (AFE) compound NH4H2PO4 (ADP) is performed by first-principles calculations in the framework of the density functional theory. The calculated structures for the AFE and paraelectric (PE) phases are found in general good agreement with the available experimental data. We study the energetics and relative stability of different polarized clusters embedded in a PE matrix of ADP. We find that local ferroelectric and AFE clusters are stable and may coexist in the PE phase, which explains the coexistence of both type of microregions determined by electron spin probe measurements above the AFE-PE transition temperature. The dependency with the O–H......O bridge length of the energy barrier heights for proton transfer is studied for coordinated proton displacements along the bridges within clusters of different sizes. This dependency may have implications for the geometric isotopic effects on Tc. We analyze Mulliken orbital and bond populations which confirm the existence of a charge flow within the NH 4+ ion, an essential fact for the stabilization of the AFE phase over other possible polarized structures. This charge transfer is correlated with the optimization of the N–H......O bridges and with distortions of the NH 4+ group.
Fil: Lasave, Jorge Augusto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Koval, Sergio Fabian. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Migoni, Ricardo Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Dalal, N. S.. Florida State University; Estados Unidos
Materia
ADP
FERROELECTRICS
H-BONDED
ANTIFERROELECTRIC
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:11336/278621
Acceder
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network_acronym_str CONICETDig
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network_name_str CONICET Digital (CONICET)
spelling Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4Lasave, Jorge AugustoKoval, Sergio FabianMigoni, Ricardo LuisDalal, N. S.ADPFERROELECTRICSH-BONDEDANTIFERROELECTRIChttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1A study of differently polarized structures relevant to the H-bonded antiferroelectric (AFE) compound NH4H2PO4 (ADP) is performed by first-principles calculations in the framework of the density functional theory. The calculated structures for the AFE and paraelectric (PE) phases are found in general good agreement with the available experimental data. We study the energetics and relative stability of different polarized clusters embedded in a PE matrix of ADP. We find that local ferroelectric and AFE clusters are stable and may coexist in the PE phase, which explains the coexistence of both type of microregions determined by electron spin probe measurements above the AFE-PE transition temperature. The dependency with the O–H......O bridge length of the energy barrier heights for proton transfer is studied for coordinated proton displacements along the bridges within clusters of different sizes. This dependency may have implications for the geometric isotopic effects on Tc. We analyze Mulliken orbital and bond populations which confirm the existence of a charge flow within the NH 4+ ion, an essential fact for the stabilization of the AFE phase over other possible polarized structures. This charge transfer is correlated with the optimization of the N–H......O bridges and with distortions of the NH 4+ group.Fil: Lasave, Jorge Augusto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; ArgentinaFil: Koval, Sergio Fabian. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; ArgentinaFil: Migoni, Ricardo Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; ArgentinaFil: Dalal, N. S.. Florida State University; Estados UnidosAmerican Institute of Physics2011-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/278621Lasave, Jorge Augusto; Koval, Sergio Fabian; Migoni, Ricardo Luis; Dalal, N. S.; Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4; American Institute of Physics; Journal of Chemical Physics; 135; 8; 8-2011; 1-80021-9606CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1063/1.3624616info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2026-04-08T11:33:30Zoai:ri.conicet.gov.ar:11336/278621instacron: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:34982026-04-08 11:33:30.86CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
title Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
spellingShingle Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
Lasave, Jorge Augusto
ADP
FERROELECTRICS
H-BONDED
ANTIFERROELECTRIC
title_short Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
title_full Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
title_fullStr Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
title_full_unstemmed Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
title_sort Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4
dc.creator.none.fl_str_mv Lasave, Jorge Augusto
Koval, Sergio Fabian
Migoni, Ricardo Luis
Dalal, N. S.
author Lasave, Jorge Augusto
author_facet Lasave, Jorge Augusto
Koval, Sergio Fabian
Migoni, Ricardo Luis
Dalal, N. S.
author_role author
author2 Koval, Sergio Fabian
Migoni, Ricardo Luis
Dalal, N. S.
author2_role author
author
author
dc.subject.none.fl_str_mv ADP
FERROELECTRICS
H-BONDED
ANTIFERROELECTRIC
topic ADP
FERROELECTRICS
H-BONDED
ANTIFERROELECTRIC
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv A study of differently polarized structures relevant to the H-bonded antiferroelectric (AFE) compound NH4H2PO4 (ADP) is performed by first-principles calculations in the framework of the density functional theory. The calculated structures for the AFE and paraelectric (PE) phases are found in general good agreement with the available experimental data. We study the energetics and relative stability of different polarized clusters embedded in a PE matrix of ADP. We find that local ferroelectric and AFE clusters are stable and may coexist in the PE phase, which explains the coexistence of both type of microregions determined by electron spin probe measurements above the AFE-PE transition temperature. The dependency with the O–H......O bridge length of the energy barrier heights for proton transfer is studied for coordinated proton displacements along the bridges within clusters of different sizes. This dependency may have implications for the geometric isotopic effects on Tc. We analyze Mulliken orbital and bond populations which confirm the existence of a charge flow within the NH 4+ ion, an essential fact for the stabilization of the AFE phase over other possible polarized structures. This charge transfer is correlated with the optimization of the N–H......O bridges and with distortions of the NH 4+ group.
Fil: Lasave, Jorge Augusto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Koval, Sergio Fabian. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Migoni, Ricardo Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Dalal, N. S.. Florida State University; Estados Unidos
description A study of differently polarized structures relevant to the H-bonded antiferroelectric (AFE) compound NH4H2PO4 (ADP) is performed by first-principles calculations in the framework of the density functional theory. The calculated structures for the AFE and paraelectric (PE) phases are found in general good agreement with the available experimental data. We study the energetics and relative stability of different polarized clusters embedded in a PE matrix of ADP. We find that local ferroelectric and AFE clusters are stable and may coexist in the PE phase, which explains the coexistence of both type of microregions determined by electron spin probe measurements above the AFE-PE transition temperature. The dependency with the O–H......O bridge length of the energy barrier heights for proton transfer is studied for coordinated proton displacements along the bridges within clusters of different sizes. This dependency may have implications for the geometric isotopic effects on Tc. We analyze Mulliken orbital and bond populations which confirm the existence of a charge flow within the NH 4+ ion, an essential fact for the stabilization of the AFE phase over other possible polarized structures. This charge transfer is correlated with the optimization of the N–H......O bridges and with distortions of the NH 4+ group.
publishDate 2011
dc.date.none.fl_str_mv 2011-08
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/11336/278621
Lasave, Jorge Augusto; Koval, Sergio Fabian; Migoni, Ricardo Luis; Dalal, N. S.; Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4; American Institute of Physics; Journal of Chemical Physics; 135; 8; 8-2011; 1-8
0021-9606
CONICET Digital
CONICET
url http://hdl.handle.net/11336/278621
identifier_str_mv Lasave, Jorge Augusto; Koval, Sergio Fabian; Migoni, Ricardo Luis; Dalal, N. S.; Ab initio studies of the para- and antiferroelectric structures and local polarized configurations in NH4H2PO4; American Institute of Physics; Journal of Chemical Physics; 135; 8; 8-2011; 1-8
0021-9606
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1063/1.3624616
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
application/pdf
dc.publisher.none.fl_str_mv American Institute of Physics
publisher.none.fl_str_mv American Institute of Physics
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 13.018236

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