The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures

The optical absorption spectrum and lowest photoluminescence PL signal for silanone terminated silica nanostructures are studied using time-dependent density functional theory calculations on a range of realistic low energy silica nanocluster models. We show that the broad experimental absorption sp...

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Autores: Zwijnenburg, M. A., Sokol, A. A., Sousa Romero, Carmen, Bromley, Stefan Thomas
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2009
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/150698
Acceso en línea:https://hdl.handle.net/2445/150698
Access Level:acceso abierto
Palabra clave:Isomeria
Teoria del funcional de densitat
Luminescència
Silicats
Isomerism
Density functionals
Luminescence
Silicates
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spelling The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructuresZwijnenburg, M. A.Sokol, A. A.Sousa Romero, CarmenBromley, Stefan ThomasIsomeriaTeoria del funcional de densitatLuminescènciaSilicatsIsomerismDensity functionalsLuminescenceSilicatesThe optical absorption spectrum and lowest photoluminescence PL signal for silanone terminated silica nanostructures are studied using time-dependent density functional theory calculations on a range of realistic low energy silica nanocluster models. We show that the broad experimental absorption spectrum for silanone centers V. A. Radtsig and I. M. Senchenya Russ. Chem. Bull. 45, 1849 1996 is most likely the result of a synergetic combination of inhomogeneous broadening, thermal broadening and the small energy differences between different excitations. We further demonstrate that upon relaxation of the excited state the excited electron and hole localize on only one silanone center, and that there is a clear and distinct link between the local environment of a silanone center and its absorption and PL spectra. Finally, we provide strong evidence that the silanone center does not have a double bond between the constituent silicon and oxygen atoms but rather can be probably more aptly described as the =Si+-O− charge-transfer species.American Institute of Physics2020202020092020info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion1 p.application/pdfhttps://hdl.handle.net/2445/150698Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésReproducció del document publicat a: https://doi.org/10.1063/1.3155083Journal of Chemical Physics, 2009, vol. 131, num. 3, p. 034705-1-034705-7https://doi.org/10.1063/1.3155083(c) American Institute of Physics , 2009info:eu-repo/semantics/openAccessoai:recercat.cat:2445/1506982026-05-29T05:05:01Z
dc.title.none.fl_str_mv The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
title The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
spellingShingle The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
Zwijnenburg, M. A.
Isomeria
Teoria del funcional de densitat
Luminescència
Silicats
Isomerism
Density functionals
Luminescence
Silicates
title_short The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
title_full The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
title_fullStr The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
title_full_unstemmed The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
title_sort The effect of local environment on photoluminescence: a TD-DFT study of silanone groups on the surface of silica nanostructures
dc.creator.none.fl_str_mv Zwijnenburg, M. A.
Sokol, A. A.
Sousa Romero, Carmen
Bromley, Stefan Thomas
author Zwijnenburg, M. A.
author_facet Zwijnenburg, M. A.
Sokol, A. A.
Sousa Romero, Carmen
Bromley, Stefan Thomas
author_role author
author2 Sokol, A. A.
Sousa Romero, Carmen
Bromley, Stefan Thomas
author2_role author
author
author
dc.subject.none.fl_str_mv Isomeria
Teoria del funcional de densitat
Luminescència
Silicats
Isomerism
Density functionals
Luminescence
Silicates
topic Isomeria
Teoria del funcional de densitat
Luminescència
Silicats
Isomerism
Density functionals
Luminescence
Silicates
description The optical absorption spectrum and lowest photoluminescence PL signal for silanone terminated silica nanostructures are studied using time-dependent density functional theory calculations on a range of realistic low energy silica nanocluster models. We show that the broad experimental absorption spectrum for silanone centers V. A. Radtsig and I. M. Senchenya Russ. Chem. Bull. 45, 1849 1996 is most likely the result of a synergetic combination of inhomogeneous broadening, thermal broadening and the small energy differences between different excitations. We further demonstrate that upon relaxation of the excited state the excited electron and hole localize on only one silanone center, and that there is a clear and distinct link between the local environment of a silanone center and its absorption and PL spectra. Finally, we provide strong evidence that the silanone center does not have a double bond between the constituent silicon and oxygen atoms but rather can be probably more aptly described as the =Si+-O− charge-transfer species.
publishDate 2009
dc.date.none.fl_str_mv 2009
2020
2020
2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/150698
url https://hdl.handle.net/2445/150698
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1063/1.3155083
Journal of Chemical Physics, 2009, vol. 131, num. 3, p. 034705-1-034705-7
https://doi.org/10.1063/1.3155083
dc.rights.none.fl_str_mv (c) American Institute of Physics , 2009
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) American Institute of Physics , 2009
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 1 p.
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 Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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