Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality
Autor(a) principal: | |
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Data de Publicação: | 2008 |
Outros Autores: | , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10316/10659 https://doi.org/10.1021/jp0747104 |
Resumo: | We have investigated the energy transfer dynamics in mixed lanthanide open-framework silicates, known as Ln-AV-20 materials, with the stoichiometric formula Na1.08K0.5Ln1.14Si3O8.5·1.78H2O (Ln = Gd3+, Tb3+, Eu3+), using steady-state and time-resolved luminescence spectroscopy. Energy transfer between donor and acceptor Ln3+ ions is extremely efficient, even at low molar ratios of the acceptor Ln3+ (<5%). The presence of two different Ln3+ environments makes the Ln-AV-20 intralayer structure intermediate between purely one-dimensional (1D) and two-dimensional (2D). The unusual dimensionality of the Ln-AV-20 layers prevents modeling of energy transfer kinetics by conventional kinetic models. We have developed a computer modeling program for the analysis of energy transfer kinetics in systems of unusual dimensions and show how it may be applied successfully to the AV-20 system. Using the program, nearest neighbor energy transfer rate constants are calculated as (5.30 ± 0.07) × 106 and (6.00 ± 0.13) × 106 s-1, respectively, for Gd/Tb- and Tb/Eu-AV-20 at 300 K. With increasing acceptor concentration, the energy transfer dynamics tend toward purely one-dimensional behavior, and thus, with careful selection of the ratio of individual Ln3+ ions, it is possible to tune the energy transfer dimensionality of the AV-20 layers from pure 1D to something intermediate between 1D and 2D. |
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Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual DimensionalityWe have investigated the energy transfer dynamics in mixed lanthanide open-framework silicates, known as Ln-AV-20 materials, with the stoichiometric formula Na1.08K0.5Ln1.14Si3O8.5·1.78H2O (Ln = Gd3+, Tb3+, Eu3+), using steady-state and time-resolved luminescence spectroscopy. Energy transfer between donor and acceptor Ln3+ ions is extremely efficient, even at low molar ratios of the acceptor Ln3+ (<5%). The presence of two different Ln3+ environments makes the Ln-AV-20 intralayer structure intermediate between purely one-dimensional (1D) and two-dimensional (2D). The unusual dimensionality of the Ln-AV-20 layers prevents modeling of energy transfer kinetics by conventional kinetic models. We have developed a computer modeling program for the analysis of energy transfer kinetics in systems of unusual dimensions and show how it may be applied successfully to the AV-20 system. Using the program, nearest neighbor energy transfer rate constants are calculated as (5.30 ± 0.07) × 106 and (6.00 ± 0.13) × 106 s-1, respectively, for Gd/Tb- and Tb/Eu-AV-20 at 300 K. With increasing acceptor concentration, the energy transfer dynamics tend toward purely one-dimensional behavior, and thus, with careful selection of the ratio of individual Ln3+ ions, it is possible to tune the energy transfer dimensionality of the AV-20 layers from pure 1D to something intermediate between 1D and 2D.American Chemical Society2008-01-10info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articlehttp://hdl.handle.net/10316/10659http://hdl.handle.net/10316/10659https://doi.org/10.1021/jp0747104engThe Journal of Physical Chemistry C. 112:1 (2008) 260-2681932-7447Evans, Rachel C.Ananias, DuarteDouglas, AlastairDouglas, PeterCarlos, Luís D.Rocha, Joãoinfo:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2021-08-16T07:51:02Zoai:estudogeral.uc.pt:10316/10659Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-19T20:55:38.496177Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
title |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
spellingShingle |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality Evans, Rachel C. |
title_short |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
title_full |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
title_fullStr |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
title_full_unstemmed |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
title_sort |
Energy Transfer and Emission Decay Kinetics in Mixed Microporous Lanthanide Silicates with Unusual Dimensionality |
author |
Evans, Rachel C. |
author_facet |
Evans, Rachel C. Ananias, Duarte Douglas, Alastair Douglas, Peter Carlos, Luís D. Rocha, João |
author_role |
author |
author2 |
Ananias, Duarte Douglas, Alastair Douglas, Peter Carlos, Luís D. Rocha, João |
author2_role |
author author author author author |
dc.contributor.author.fl_str_mv |
Evans, Rachel C. Ananias, Duarte Douglas, Alastair Douglas, Peter Carlos, Luís D. Rocha, João |
description |
We have investigated the energy transfer dynamics in mixed lanthanide open-framework silicates, known as Ln-AV-20 materials, with the stoichiometric formula Na1.08K0.5Ln1.14Si3O8.5·1.78H2O (Ln = Gd3+, Tb3+, Eu3+), using steady-state and time-resolved luminescence spectroscopy. Energy transfer between donor and acceptor Ln3+ ions is extremely efficient, even at low molar ratios of the acceptor Ln3+ (<5%). The presence of two different Ln3+ environments makes the Ln-AV-20 intralayer structure intermediate between purely one-dimensional (1D) and two-dimensional (2D). The unusual dimensionality of the Ln-AV-20 layers prevents modeling of energy transfer kinetics by conventional kinetic models. We have developed a computer modeling program for the analysis of energy transfer kinetics in systems of unusual dimensions and show how it may be applied successfully to the AV-20 system. Using the program, nearest neighbor energy transfer rate constants are calculated as (5.30 ± 0.07) × 106 and (6.00 ± 0.13) × 106 s-1, respectively, for Gd/Tb- and Tb/Eu-AV-20 at 300 K. With increasing acceptor concentration, the energy transfer dynamics tend toward purely one-dimensional behavior, and thus, with careful selection of the ratio of individual Ln3+ ions, it is possible to tune the energy transfer dimensionality of the AV-20 layers from pure 1D to something intermediate between 1D and 2D. |
publishDate |
2008 |
dc.date.none.fl_str_mv |
2008-01-10 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10316/10659 http://hdl.handle.net/10316/10659 https://doi.org/10.1021/jp0747104 |
url |
http://hdl.handle.net/10316/10659 https://doi.org/10.1021/jp0747104 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
The Journal of Physical Chemistry C. 112:1 (2008) 260-268 1932-7447 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.publisher.none.fl_str_mv |
American Chemical Society |
publisher.none.fl_str_mv |
American Chemical Society |
dc.source.none.fl_str_mv |
reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
instname_str |
Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
instacron_str |
RCAAP |
institution |
RCAAP |
reponame_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
collection |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
repository.name.fl_str_mv |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
repository.mail.fl_str_mv |
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1799133843195691008 |