Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations

Autores
Perez Castillo, Royle; Freixas, Victor M.; Mukamel, Shaul; Martinez Mesa, Aliezer; Uranga Piña, Llinersy; Tretiak, Sergei; Gelin, Maxim F.; Fernández Alberti, Sebastián
Año de publicación
2024
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The efficiency of light-harvesting and energy transfer in multi-chromophore ensembles underpins natural photosynthesis. Dendrimers are highly branched synthetic multi-chromophoric conjugated supramolecules that mimic these natural processes. After photoexcitation, their repeated units participate in a number of intramolecular electronic energy relaxation and redistribution pathways that ultimately funnel to a sink. Here, a model four-branched dendrimer with a pyrene core is theoretically studied using nonadiabatic molecular dynamics simulations. We evaluate excited-state photoinduced dynamics of the dendrimer, and demonstrate on-the-fly simulations of its transient absorption pump–probe (TAPP) spectra. We show how the evolutions of the simulated TA-PP spectra monitor in real time photoinduced energy relaxation and redistribution, and provide a detailed microscopic picture of the relevant energy-transfer pathways. To the best of our knowledge, this is the first of this kind of on-thef ly atomistic simulation of TA-PP signals reported for a large molecular system.
Fil: Perez Castillo, Royle. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Freixas, Victor M.. University of California at Irvine; Estados Unidos
Fil: Mukamel, Shaul. University of California at Irvine; Estados Unidos
Fil: Martinez Mesa, Aliezer. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina
Fil: Uranga Piña, Llinersy. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina
Fil: Tretiak, Sergei. Los Alamos National Laboratory; Estados Unidos
Fil: Gelin, Maxim F.. Hangzhou Dianzi University; China
Fil: Fernández Alberti, Sebastián. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Materia
transient absorption
dendrimers
excited-states
nonadiabatic dynamics
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/245802
Acceder
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network_name_str CONICET Digital (CONICET)
spelling Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulationsPerez Castillo, RoyleFreixas, Victor M.Mukamel, ShaulMartinez Mesa, AliezerUranga Piña, LlinersyTretiak, SergeiGelin, Maxim F.Fernández Alberti, Sebastiántransient absorptiondendrimersexcited-statesnonadiabatic dynamicshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The efficiency of light-harvesting and energy transfer in multi-chromophore ensembles underpins natural photosynthesis. Dendrimers are highly branched synthetic multi-chromophoric conjugated supramolecules that mimic these natural processes. After photoexcitation, their repeated units participate in a number of intramolecular electronic energy relaxation and redistribution pathways that ultimately funnel to a sink. Here, a model four-branched dendrimer with a pyrene core is theoretically studied using nonadiabatic molecular dynamics simulations. We evaluate excited-state photoinduced dynamics of the dendrimer, and demonstrate on-the-fly simulations of its transient absorption pump–probe (TAPP) spectra. We show how the evolutions of the simulated TA-PP spectra monitor in real time photoinduced energy relaxation and redistribution, and provide a detailed microscopic picture of the relevant energy-transfer pathways. To the best of our knowledge, this is the first of this kind of on-thef ly atomistic simulation of TA-PP signals reported for a large molecular system.Fil: Perez Castillo, Royle. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Freixas, Victor M.. University of California at Irvine; Estados UnidosFil: Mukamel, Shaul. University of California at Irvine; Estados UnidosFil: Martinez Mesa, Aliezer. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; ArgentinaFil: Uranga Piña, Llinersy. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; ArgentinaFil: Tretiak, Sergei. Los Alamos National Laboratory; Estados UnidosFil: Gelin, Maxim F.. Hangzhou Dianzi University; ChinaFil: Fernández Alberti, Sebastián. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaRoyal Society of Chemistry2024-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/245802Perez Castillo, Royle; Freixas, Victor M.; Mukamel, Shaul; Martinez Mesa, Aliezer; Uranga Piña, Llinersy; et al.; Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations; Royal Society of Chemistry; Chemical Science; 15; 33; 7-2024; 13250-132612041-6539CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://xlink.rsc.org/?DOI=D4SC01019Ainfo:eu-repo/semantics/altIdentifier/doi/10.1039/D4SC01019Ainfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:46:04Zoai:ri.conicet.gov.ar:11336/245802instacron: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 09:46:04.469CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
title Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
spellingShingle Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
Perez Castillo, Royle
transient absorption
dendrimers
excited-states
nonadiabatic dynamics
title_short Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
title_full Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
title_fullStr Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
title_full_unstemmed Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
title_sort Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations
dc.creator.none.fl_str_mv Perez Castillo, Royle
Freixas, Victor M.
Mukamel, Shaul
Martinez Mesa, Aliezer
Uranga Piña, Llinersy
Tretiak, Sergei
Gelin, Maxim F.
Fernández Alberti, Sebastián
author Perez Castillo, Royle
author_facet Perez Castillo, Royle
Freixas, Victor M.
Mukamel, Shaul
Martinez Mesa, Aliezer
Uranga Piña, Llinersy
Tretiak, Sergei
Gelin, Maxim F.
Fernández Alberti, Sebastián
author_role author
author2 Freixas, Victor M.
Mukamel, Shaul
Martinez Mesa, Aliezer
Uranga Piña, Llinersy
Tretiak, Sergei
Gelin, Maxim F.
Fernández Alberti, Sebastián
author2_role author
author
author
author
author
author
author
dc.subject.none.fl_str_mv transient absorption
dendrimers
excited-states
nonadiabatic dynamics
topic transient absorption
dendrimers
excited-states
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 The efficiency of light-harvesting and energy transfer in multi-chromophore ensembles underpins natural photosynthesis. Dendrimers are highly branched synthetic multi-chromophoric conjugated supramolecules that mimic these natural processes. After photoexcitation, their repeated units participate in a number of intramolecular electronic energy relaxation and redistribution pathways that ultimately funnel to a sink. Here, a model four-branched dendrimer with a pyrene core is theoretically studied using nonadiabatic molecular dynamics simulations. We evaluate excited-state photoinduced dynamics of the dendrimer, and demonstrate on-the-fly simulations of its transient absorption pump–probe (TAPP) spectra. We show how the evolutions of the simulated TA-PP spectra monitor in real time photoinduced energy relaxation and redistribution, and provide a detailed microscopic picture of the relevant energy-transfer pathways. To the best of our knowledge, this is the first of this kind of on-thef ly atomistic simulation of TA-PP signals reported for a large molecular system.
Fil: Perez Castillo, Royle. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Freixas, Victor M.. University of California at Irvine; Estados Unidos
Fil: Mukamel, Shaul. University of California at Irvine; Estados Unidos
Fil: Martinez Mesa, Aliezer. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina
Fil: Uranga Piña, Llinersy. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina
Fil: Tretiak, Sergei. Los Alamos National Laboratory; Estados Unidos
Fil: Gelin, Maxim F.. Hangzhou Dianzi University; China
Fil: Fernández Alberti, Sebastián. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología. Area Química; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
description The efficiency of light-harvesting and energy transfer in multi-chromophore ensembles underpins natural photosynthesis. Dendrimers are highly branched synthetic multi-chromophoric conjugated supramolecules that mimic these natural processes. After photoexcitation, their repeated units participate in a number of intramolecular electronic energy relaxation and redistribution pathways that ultimately funnel to a sink. Here, a model four-branched dendrimer with a pyrene core is theoretically studied using nonadiabatic molecular dynamics simulations. We evaluate excited-state photoinduced dynamics of the dendrimer, and demonstrate on-the-fly simulations of its transient absorption pump–probe (TAPP) spectra. We show how the evolutions of the simulated TA-PP spectra monitor in real time photoinduced energy relaxation and redistribution, and provide a detailed microscopic picture of the relevant energy-transfer pathways. To the best of our knowledge, this is the first of this kind of on-thef ly atomistic simulation of TA-PP signals reported for a large molecular system.
publishDate 2024
dc.date.none.fl_str_mv 2024-07
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/11336/245802
Perez Castillo, Royle; Freixas, Victor M.; Mukamel, Shaul; Martinez Mesa, Aliezer; Uranga Piña, Llinersy; et al.; Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations; Royal Society of Chemistry; Chemical Science; 15; 33; 7-2024; 13250-13261
2041-6539
CONICET Digital
CONICET
url http://hdl.handle.net/11336/245802
identifier_str_mv Perez Castillo, Royle; Freixas, Victor M.; Mukamel, Shaul; Martinez Mesa, Aliezer; Uranga Piña, Llinersy; et al.; Transient-absorption spectroscopy of dendrimers via nonadiabatic excited-state dynamics simulations; Royal Society of Chemistry; Chemical Science; 15; 33; 7-2024; 13250-13261
2041-6539
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://xlink.rsc.org/?DOI=D4SC01019A
info:eu-repo/semantics/altIdentifier/doi/10.1039/D4SC01019A
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc/2.5/ar/
dc.format.none.fl_str_mv 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_ 1842268771711975424
score 13.13397

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