Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domai...

Autores: Fasce, Diana Patricia; Williams, Roberto Juan Jose; Matejka, Libor; Plestil, Josef; Brus, Jiri; Serrano, Berna; Cabanelas, Juan C.; Baselga, Juan
Año de publicación: 2006
Idioma: inglés
Tipo de recurso: artículo
Estado: versión publicada
Descripción: The aim of this study was to investigate the changes produced in the nanostructures and the photoluminescence spectra of bridged silsesquioxanes containing urea or urethane groups, by varying the relative rates between the self-assembly of organic domains and the inorganic polycondensation. Precursors of the bridged silsesquioxanes were 4,4′-[1,3-phenylenebis(1- methylethylidene)]bis(aniline) and 4,4′-isopropylidenediphenol, end-capped with 3-isocyanatopropyltriethoxysilane. The inorganic polycondensation was produced using either high or low formic acid concentrations, leading to transparent films with different nanostructures as revealed by FTIR, SAXS, and 29Si NMR spectra. For the bridged silsesquioxanes containing urea groups the self-assembly of organic domains was much faster than the inorganic polycondensation for both formic acid concentrations. However, the arrangement was more regular and the short-range order higher when the rate of inorganic polycondensation was lower. The photoluminescence spectra of the most ordered structures revealed the presence of two main processes: radiative recombinations in inorganic clusters and photoinduced proton-transfer generating NH 2+ and N- defects and their subsequent radiative recombination. In the less-ordered urea-bridged silsesquioxanes a third process was present assigned to a photoinduced proton transfer in H-bonds exhibiting a broad range of strengths. For urethane-bridged silsesquioxanes the driving force for the self-assembly of organic bridges was lower than for urea-bridged silsesquioxanes. When the synthesis was performed with a high formic acid concentration, self-assembled structures were not produced. Instead, large inorganic domains composed of small inorganic clusters were generated. Self-assembly of organic domains took place only when employing low polycondensation rates. For both materials the photoluminescence was mainly due to radiative processes within inorganic clusters and varied significantly with their state of aggregation.
Fil: Fasce, Diana Patricia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Fil: Williams, Roberto Juan Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina
Fil: Matejka, Libor. Biology Centre of the Academy of Sciences of the Czech Republic; República Checa
Fil: Plestil, Josef. Biology Centre of the Academy of Sciences of the Czech Republic; República Checa
Fil: Brus, Jiri. Biology Centre of the Academy of Sciences of the Czech Republic; República Checa
Fil: Serrano, Berna. Universidad Carlos III de Madrid; España
Fil: Cabanelas, Juan C.. Universidad Carlos III de Madrid; España
Fil: Baselga, Juan. Universidad Carlos III de Madrid; España
Materia: Photoluminescence
Bridged Silsesquioxane
Urea
Urethane
Self-Assembly
Nivel de accesibilidad: acceso abierto
Condiciones de uso: https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
Institución: Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador: oai:ri.conicet.gov.ar:11336/86037

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repository_id_str	3498
network_name_str	CONICET Digital (CONICET)
spelling	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensationFasce, Diana PatriciaWilliams, Roberto Juan JoseMatejka, LiborPlestil, JosefBrus, JiriSerrano, BernaCabanelas, Juan C.Baselga, JuanPhotoluminescenceBridged SilsesquioxaneUreaUrethaneSelf-Assemblyhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1https://purl.org/becyt/ford/2.5https://purl.org/becyt/ford/2The aim of this study was to investigate the changes produced in the nanostructures and the photoluminescence spectra of bridged silsesquioxanes containing urea or urethane groups, by varying the relative rates between the self-assembly of organic domains and the inorganic polycondensation. Precursors of the bridged silsesquioxanes were 4,4′-[1,3-phenylenebis(1- methylethylidene)]bis(aniline) and 4,4′-isopropylidenediphenol, end-capped with 3-isocyanatopropyltriethoxysilane. The inorganic polycondensation was produced using either high or low formic acid concentrations, leading to transparent films with different nanostructures as revealed by FTIR, SAXS, and 29Si NMR spectra. For the bridged silsesquioxanes containing urea groups the self-assembly of organic domains was much faster than the inorganic polycondensation for both formic acid concentrations. However, the arrangement was more regular and the short-range order higher when the rate of inorganic polycondensation was lower. The photoluminescence spectra of the most ordered structures revealed the presence of two main processes: radiative recombinations in inorganic clusters and photoinduced proton-transfer generating NH 2+ and N- defects and their subsequent radiative recombination. In the less-ordered urea-bridged silsesquioxanes a third process was present assigned to a photoinduced proton transfer in H-bonds exhibiting a broad range of strengths. For urethane-bridged silsesquioxanes the driving force for the self-assembly of organic bridges was lower than for urea-bridged silsesquioxanes. When the synthesis was performed with a high formic acid concentration, self-assembled structures were not produced. Instead, large inorganic domains composed of small inorganic clusters were generated. Self-assembly of organic domains took place only when employing low polycondensation rates. For both materials the photoluminescence was mainly due to radiative processes within inorganic clusters and varied significantly with their state of aggregation.Fil: Fasce, Diana Patricia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; ArgentinaFil: Williams, Roberto Juan Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; ArgentinaFil: Matejka, Libor. Biology Centre of the Academy of Sciences of the Czech Republic; República ChecaFil: Plestil, Josef. Biology Centre of the Academy of Sciences of the Czech Republic; República ChecaFil: Brus, Jiri. Biology Centre of the Academy of Sciences of the Czech Republic; República ChecaFil: Serrano, Berna. Universidad Carlos III de Madrid; EspañaFil: Cabanelas, Juan C.. Universidad Carlos III de Madrid; EspañaFil: Baselga, Juan. Universidad Carlos III de Madrid; EspañaAmerican Chemical Society2006-05info: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/11336/86037Fasce, Diana Patricia; Williams, Roberto Juan Jose; Matejka, Libor; Plestil, Josef; Brus, Jiri; et al.; Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation; American Chemical Society; Macromolecules; 39; 11; 5-2006; 3794-38010024-9297CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/abs/10.1021/ma052105yinfo:eu-repo/semantics/altIdentifier/doi/10.1021/ma052105yinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:22:55Zoai:ri.conicet.gov.ar:11336/86037instacron: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:34982025-10-15 15:22:56.062CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
title	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
spellingShingle	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation Fasce, Diana Patricia Photoluminescence Bridged Silsesquioxane Urea Urethane Self-Assembly
title_short	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
title_full	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
title_fullStr	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
title_full_unstemmed	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
title_sort	Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation
dc.creator.none.fl_str_mv	Fasce, Diana Patricia Williams, Roberto Juan Jose Matejka, Libor Plestil, Josef Brus, Jiri Serrano, Berna Cabanelas, Juan C. Baselga, Juan
author	Fasce, Diana Patricia
author_facet	Fasce, Diana Patricia Williams, Roberto Juan Jose Matejka, Libor Plestil, Josef Brus, Jiri Serrano, Berna Cabanelas, Juan C. Baselga, Juan
author_role	author
author2	Williams, Roberto Juan Jose Matejka, Libor Plestil, Josef Brus, Jiri Serrano, Berna Cabanelas, Juan C. Baselga, Juan
author2_role	author author author author author author author
dc.subject.none.fl_str_mv	Photoluminescence Bridged Silsesquioxane Urea Urethane Self-Assembly
topic	Photoluminescence Bridged Silsesquioxane Urea Urethane Self-Assembly
purl_subject.fl_str_mv	https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 https://purl.org/becyt/ford/2.5 https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv	The aim of this study was to investigate the changes produced in the nanostructures and the photoluminescence spectra of bridged silsesquioxanes containing urea or urethane groups, by varying the relative rates between the self-assembly of organic domains and the inorganic polycondensation. Precursors of the bridged silsesquioxanes were 4,4′-[1,3-phenylenebis(1- methylethylidene)]bis(aniline) and 4,4′-isopropylidenediphenol, end-capped with 3-isocyanatopropyltriethoxysilane. The inorganic polycondensation was produced using either high or low formic acid concentrations, leading to transparent films with different nanostructures as revealed by FTIR, SAXS, and 29Si NMR spectra. For the bridged silsesquioxanes containing urea groups the self-assembly of organic domains was much faster than the inorganic polycondensation for both formic acid concentrations. However, the arrangement was more regular and the short-range order higher when the rate of inorganic polycondensation was lower. The photoluminescence spectra of the most ordered structures revealed the presence of two main processes: radiative recombinations in inorganic clusters and photoinduced proton-transfer generating NH 2+ and N- defects and their subsequent radiative recombination. In the less-ordered urea-bridged silsesquioxanes a third process was present assigned to a photoinduced proton transfer in H-bonds exhibiting a broad range of strengths. For urethane-bridged silsesquioxanes the driving force for the self-assembly of organic bridges was lower than for urea-bridged silsesquioxanes. When the synthesis was performed with a high formic acid concentration, self-assembled structures were not produced. Instead, large inorganic domains composed of small inorganic clusters were generated. Self-assembly of organic domains took place only when employing low polycondensation rates. For both materials the photoluminescence was mainly due to radiative processes within inorganic clusters and varied significantly with their state of aggregation. Fil: Fasce, Diana Patricia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina Fil: Williams, Roberto Juan Jose. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mar del Plata. Instituto de Investigaciones en Ciencia y Tecnología de Materiales. Universidad Nacional de Mar del Plata. Facultad de Ingeniería. Instituto de Investigaciones en Ciencia y Tecnología de Materiales; Argentina Fil: Matejka, Libor. Biology Centre of the Academy of Sciences of the Czech Republic; República Checa Fil: Plestil, Josef. Biology Centre of the Academy of Sciences of the Czech Republic; República Checa Fil: Brus, Jiri. Biology Centre of the Academy of Sciences of the Czech Republic; República Checa Fil: Serrano, Berna. Universidad Carlos III de Madrid; España Fil: Cabanelas, Juan C.. Universidad Carlos III de Madrid; España Fil: Baselga, Juan. Universidad Carlos III de Madrid; España
description	The aim of this study was to investigate the changes produced in the nanostructures and the photoluminescence spectra of bridged silsesquioxanes containing urea or urethane groups, by varying the relative rates between the self-assembly of organic domains and the inorganic polycondensation. Precursors of the bridged silsesquioxanes were 4,4′-[1,3-phenylenebis(1- methylethylidene)]bis(aniline) and 4,4′-isopropylidenediphenol, end-capped with 3-isocyanatopropyltriethoxysilane. The inorganic polycondensation was produced using either high or low formic acid concentrations, leading to transparent films with different nanostructures as revealed by FTIR, SAXS, and 29Si NMR spectra. For the bridged silsesquioxanes containing urea groups the self-assembly of organic domains was much faster than the inorganic polycondensation for both formic acid concentrations. However, the arrangement was more regular and the short-range order higher when the rate of inorganic polycondensation was lower. The photoluminescence spectra of the most ordered structures revealed the presence of two main processes: radiative recombinations in inorganic clusters and photoinduced proton-transfer generating NH 2+ and N- defects and their subsequent radiative recombination. In the less-ordered urea-bridged silsesquioxanes a third process was present assigned to a photoinduced proton transfer in H-bonds exhibiting a broad range of strengths. For urethane-bridged silsesquioxanes the driving force for the self-assembly of organic bridges was lower than for urea-bridged silsesquioxanes. When the synthesis was performed with a high formic acid concentration, self-assembled structures were not produced. Instead, large inorganic domains composed of small inorganic clusters were generated. Self-assembly of organic domains took place only when employing low polycondensation rates. For both materials the photoluminescence was mainly due to radiative processes within inorganic clusters and varied significantly with their state of aggregation.
publishDate	2006
dc.date.none.fl_str_mv	2006-05
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/11336/86037 Fasce, Diana Patricia; Williams, Roberto Juan Jose; Matejka, Libor; Plestil, Josef; Brus, Jiri; et al.; Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation; American Chemical Society; Macromolecules; 39; 11; 5-2006; 3794-3801 0024-9297 CONICET Digital CONICET
url	http://hdl.handle.net/11336/86037
identifier_str_mv	Fasce, Diana Patricia; Williams, Roberto Juan Jose; Matejka, Libor; Plestil, Josef; Brus, Jiri; et al.; Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domains and the inorganic polycondensation; American Chemical Society; Macromolecules; 39; 11; 5-2006; 3794-3801 0024-9297 CONICET Digital CONICET
dc.language.none.fl_str_mv	eng
language	eng
dc.relation.none.fl_str_mv	info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/abs/10.1021/ma052105y info:eu-repo/semantics/altIdentifier/doi/10.1021/ma052105y
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)
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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	13.22299

Photoluminescence of bridged silsesquioxanes containing urea or urethane groups with nanostructures generated by the competition between the rates of self-assembly of organic domai...

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