Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer

Autores
Athanasopoulos, Stavros; Alfonso Hernandez, Laura; Beljonne, David; Fernández Alberti, Sebastián; Tretiak, Sergei
Año de publicación
2017
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S2 → S1 internal conversion process, revealing an efficient unidirectional donor → acceptor energy-transfer process. Detailed analysis of the excited-state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S2-S1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition.
Fil: Athanasopoulos, Stavros. Universidad Carlos III; España. University of Bayreuth; Alemania
Fil: Alfonso Hernandez, Laura. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes; Argentina
Fil: Beljonne, David. University of Mons; Bélgica
Fil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes; Argentina
Fil: Tretiak, Sergei. Los Alamos National High Magnetic Field Laboratory; Estados Unidos
Materia
Non-Adiabatic Molecular Dynamics
Excited States
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:11336/40677
Acceder
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network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy TransferAthanasopoulos, StavrosAlfonso Hernandez, LauraBeljonne, DavidFernández Alberti, SebastiánTretiak, SergeiNon-Adiabatic Molecular DynamicsExcited Stateshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S2 → S1 internal conversion process, revealing an efficient unidirectional donor → acceptor energy-transfer process. Detailed analysis of the excited-state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S2-S1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition.Fil: Athanasopoulos, Stavros. Universidad Carlos III; España. University of Bayreuth; AlemaniaFil: Alfonso Hernandez, Laura. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes; ArgentinaFil: Beljonne, David. University of Mons; BélgicaFil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes; ArgentinaFil: Tretiak, Sergei. Los Alamos National High Magnetic Field Laboratory; Estados UnidosAmerican Chemical Society2017-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/40677Athanasopoulos, Stavros; Alfonso Hernandez, Laura; Beljonne, David; Fernández Alberti, Sebastián; Tretiak, Sergei; Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer; American Chemical Society; Journal of Physical Chemistry Letters; 8; 7; 4-2017; 1688-16941948-7185CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.7b00259info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpclett.7b00259info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:53:08Zoai:ri.conicet.gov.ar:11336/40677instacron: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:34982025-09-03 09:53:08.446CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
title Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
spellingShingle Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
Athanasopoulos, Stavros
Non-Adiabatic Molecular Dynamics
Excited States
title_short Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
title_full Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
title_fullStr Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
title_full_unstemmed Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
title_sort Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
dc.creator.none.fl_str_mv Athanasopoulos, Stavros
Alfonso Hernandez, Laura
Beljonne, David
Fernández Alberti, Sebastián
Tretiak, Sergei
author Athanasopoulos, Stavros
author_facet Athanasopoulos, Stavros
Alfonso Hernandez, Laura
Beljonne, David
Fernández Alberti, Sebastián
Tretiak, Sergei
author_role author
author2 Alfonso Hernandez, Laura
Beljonne, David
Fernández Alberti, Sebastián
Tretiak, Sergei
author2_role author
author
author
author
dc.subject.none.fl_str_mv Non-Adiabatic Molecular Dynamics
Excited States
topic Non-Adiabatic Molecular Dynamics
Excited States
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S2 → S1 internal conversion process, revealing an efficient unidirectional donor → acceptor energy-transfer process. Detailed analysis of the excited-state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S2-S1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition.
Fil: Athanasopoulos, Stavros. Universidad Carlos III; España. University of Bayreuth; Alemania
Fil: Alfonso Hernandez, Laura. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes; Argentina
Fil: Beljonne, David. University of Mons; Bélgica
Fil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes; Argentina
Fil: Tretiak, Sergei. Los Alamos National High Magnetic Field Laboratory; Estados Unidos
description Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S2 → S1 internal conversion process, revealing an efficient unidirectional donor → acceptor energy-transfer process. Detailed analysis of the excited-state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S2-S1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition.
publishDate 2017
dc.date.none.fl_str_mv 2017-04
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/11336/40677
Athanasopoulos, Stavros; Alfonso Hernandez, Laura; Beljonne, David; Fernández Alberti, Sebastián; Tretiak, Sergei; Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer; American Chemical Society; Journal of Physical Chemistry Letters; 8; 7; 4-2017; 1688-1694
1948-7185
CONICET Digital
CONICET
url http://hdl.handle.net/11336/40677
identifier_str_mv Athanasopoulos, Stavros; Alfonso Hernandez, Laura; Beljonne, David; Fernández Alberti, Sebastián; Tretiak, Sergei; Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer; American Chemical Society; Journal of Physical Chemistry Letters; 8; 7; 4-2017; 1688-1694
1948-7185
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.7b00259
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpclett.7b00259
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
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)
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 13.13397

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