Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes

Autores
Alfonso Hernandez, Laura; Athanasopoulos, Stavros; Tretiak, Sergei; Miguel, Beatriz; Bastida, Adolfo; Fernández Alberti, Sebastián
Año de publicación
2020
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Photoinduced electronic energy transfer in conjugated donor-acceptor systems is naturally accompanied by intramolecular vibrational energy redistributions accepting an excess of electronic energy. Herein, we simulate these processes in a covalently linked donor-acceptor molecular dyad system by using nonadiabatic excited state molecular dynamics simulations. We analyze different complementary criteria to systematically identify the subset of vibrational normal modes that actively participate on the donor → acceptor (S2→ S1) electronic relaxation. We analyze energy transfer coordinates in terms of state-specific normal modes defined according to the different potential energy surfaces (PESs) involved. On one hand, we identify those vibrations that contribute the most to the direction of the main driving force on the nuclei during electronic transitions, represented by the non-adiabatic derivative coupling vector between donor and acceptor electronic states. On the other hand, we monitor normal mode transient accumulations of excess energy and their intramolecular energy redistribution fluxes. We observe that the subset of active modes varies according to the PES on which they belong and these modes experience the most significant rearrangements and mixing. Whereas the nuclear motions that promote donor → acceptor energy funneling can be localized mainly on one or two normal modes of the S2 state, they become spread out across multiple normal modes of the S1 state following the energy transfer event.
Fil: Alfonso Hernandez, Laura. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina
Fil: Athanasopoulos, Stavros. Universidad Carlos III de Madrid. Departamento de Física; España
Fil: Tretiak, Sergei. Los Alamos National High Magnetic Field Laboratory; Estados Unidos
Fil: Miguel, Beatriz. Universidad Politécnica de Cartagena; España
Fil: Bastida, Adolfo. Universidad de Murcia; España
Fil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina
Materia
Molecular dynamics
Normal modes
Energy transfer
Nonadiabatic dynamics
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:11336/115132
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/115132
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modesAlfonso Hernandez, LauraAthanasopoulos, StavrosTretiak, SergeiMiguel, BeatrizBastida, AdolfoFernández Alberti, SebastiánMolecular dynamicsNormal modesEnergy transferNonadiabatic dynamicshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Photoinduced electronic energy transfer in conjugated donor-acceptor systems is naturally accompanied by intramolecular vibrational energy redistributions accepting an excess of electronic energy. Herein, we simulate these processes in a covalently linked donor-acceptor molecular dyad system by using nonadiabatic excited state molecular dynamics simulations. We analyze different complementary criteria to systematically identify the subset of vibrational normal modes that actively participate on the donor → acceptor (S2→ S1) electronic relaxation. We analyze energy transfer coordinates in terms of state-specific normal modes defined according to the different potential energy surfaces (PESs) involved. On one hand, we identify those vibrations that contribute the most to the direction of the main driving force on the nuclei during electronic transitions, represented by the non-adiabatic derivative coupling vector between donor and acceptor electronic states. On the other hand, we monitor normal mode transient accumulations of excess energy and their intramolecular energy redistribution fluxes. We observe that the subset of active modes varies according to the PES on which they belong and these modes experience the most significant rearrangements and mixing. Whereas the nuclear motions that promote donor → acceptor energy funneling can be localized mainly on one or two normal modes of the S2 state, they become spread out across multiple normal modes of the S1 state following the energy transfer event.Fil: Alfonso Hernandez, Laura. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; ArgentinaFil: Athanasopoulos, Stavros. Universidad Carlos III de Madrid. Departamento de Física; EspañaFil: Tretiak, Sergei. Los Alamos National High Magnetic Field Laboratory; Estados UnidosFil: Miguel, Beatriz. Universidad Politécnica de Cartagena; EspañaFil: Bastida, Adolfo. Universidad de Murcia; EspañaFil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; ArgentinaRoyal Society of Chemistry2020-09info: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/11336/115132Alfonso Hernandez, Laura; Athanasopoulos, Stavros; Tretiak, Sergei; Miguel, Beatriz; Bastida, Adolfo; et al.; Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 22; 33; 9-2020; 18454-184661463-90761463-9084CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=D0CP03102Jinfo:eu-repo/semantics/altIdentifier/doi/10.1039/D0CP03102Jinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:16:02Zoai:ri.conicet.gov.ar:11336/115132instacron: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:34982025-10-22 11:16:02.379CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
title Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
spellingShingle Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
Alfonso Hernandez, Laura
Molecular dynamics
Normal modes
Energy transfer
Nonadiabatic dynamics
title_short Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
title_full Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
title_fullStr Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
title_full_unstemmed Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
title_sort Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes
dc.creator.none.fl_str_mv Alfonso Hernandez, Laura
Athanasopoulos, Stavros
Tretiak, Sergei
Miguel, Beatriz
Bastida, Adolfo
Fernández Alberti, Sebastián
author Alfonso Hernandez, Laura
author_facet Alfonso Hernandez, Laura
Athanasopoulos, Stavros
Tretiak, Sergei
Miguel, Beatriz
Bastida, Adolfo
Fernández Alberti, Sebastián
author_role author
author2 Athanasopoulos, Stavros
Tretiak, Sergei
Miguel, Beatriz
Bastida, Adolfo
Fernández Alberti, Sebastián
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Molecular dynamics
Normal modes
Energy transfer
Nonadiabatic dynamics
topic Molecular dynamics
Normal modes
Energy transfer
Nonadiabatic dynamics
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Photoinduced electronic energy transfer in conjugated donor-acceptor systems is naturally accompanied by intramolecular vibrational energy redistributions accepting an excess of electronic energy. Herein, we simulate these processes in a covalently linked donor-acceptor molecular dyad system by using nonadiabatic excited state molecular dynamics simulations. We analyze different complementary criteria to systematically identify the subset of vibrational normal modes that actively participate on the donor → acceptor (S2→ S1) electronic relaxation. We analyze energy transfer coordinates in terms of state-specific normal modes defined according to the different potential energy surfaces (PESs) involved. On one hand, we identify those vibrations that contribute the most to the direction of the main driving force on the nuclei during electronic transitions, represented by the non-adiabatic derivative coupling vector between donor and acceptor electronic states. On the other hand, we monitor normal mode transient accumulations of excess energy and their intramolecular energy redistribution fluxes. We observe that the subset of active modes varies according to the PES on which they belong and these modes experience the most significant rearrangements and mixing. Whereas the nuclear motions that promote donor → acceptor energy funneling can be localized mainly on one or two normal modes of the S2 state, they become spread out across multiple normal modes of the S1 state following the energy transfer event.
Fil: Alfonso Hernandez, Laura. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina
Fil: Athanasopoulos, Stavros. Universidad Carlos III de Madrid. Departamento de Física; España
Fil: Tretiak, Sergei. Los Alamos National High Magnetic Field Laboratory; Estados Unidos
Fil: Miguel, Beatriz. Universidad Politécnica de Cartagena; España
Fil: Bastida, Adolfo. Universidad de Murcia; España
Fil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina
description Photoinduced electronic energy transfer in conjugated donor-acceptor systems is naturally accompanied by intramolecular vibrational energy redistributions accepting an excess of electronic energy. Herein, we simulate these processes in a covalently linked donor-acceptor molecular dyad system by using nonadiabatic excited state molecular dynamics simulations. We analyze different complementary criteria to systematically identify the subset of vibrational normal modes that actively participate on the donor → acceptor (S2→ S1) electronic relaxation. We analyze energy transfer coordinates in terms of state-specific normal modes defined according to the different potential energy surfaces (PESs) involved. On one hand, we identify those vibrations that contribute the most to the direction of the main driving force on the nuclei during electronic transitions, represented by the non-adiabatic derivative coupling vector between donor and acceptor electronic states. On the other hand, we monitor normal mode transient accumulations of excess energy and their intramolecular energy redistribution fluxes. We observe that the subset of active modes varies according to the PES on which they belong and these modes experience the most significant rearrangements and mixing. Whereas the nuclear motions that promote donor → acceptor energy funneling can be localized mainly on one or two normal modes of the S2 state, they become spread out across multiple normal modes of the S1 state following the energy transfer event.
publishDate 2020
dc.date.none.fl_str_mv 2020-09
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/11336/115132
Alfonso Hernandez, Laura; Athanasopoulos, Stavros; Tretiak, Sergei; Miguel, Beatriz; Bastida, Adolfo; et al.; Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 22; 33; 9-2020; 18454-18466
1463-9076
1463-9084
CONICET Digital
CONICET
url http://hdl.handle.net/11336/115132
identifier_str_mv Alfonso Hernandez, Laura; Athanasopoulos, Stavros; Tretiak, Sergei; Miguel, Beatriz; Bastida, Adolfo; et al.; Vibrational energy redistribution during donor-acceptor electronic energy transfer: criteria to identify subsets of active normal modes; Royal Society of Chemistry; Physical Chemistry Chemical Physics; 22; 33; 9-2020; 18454-18466
1463-9076
1463-9084
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=D0CP03102J
info:eu-repo/semantics/altIdentifier/doi/10.1039/D0CP03102J
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 Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
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
_version_ 1846781603252011008
score 12.982451

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