Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy

Autores
Keefer, Daniel; Freixas Lemus, Victor Manuel; Song, Huajing; Tretiak, Sergei; Fernández Alberti, Sebastián; Mukamel, Shaul
Año de publicación
2021
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The role of quantum-mechanical coherences in the elementary photophysics of functional optoelectronic molecular materials is currently under active study. Designing and controlling stable coherences arising from concerted vibronic dynamics in organic chromophores is the key for numerous applications. Here, we present fundamental insight into the energy transfer properties of a rigid synthetic heterodimer that has been experimentally engineered to study coherences. Quantum non-adiabatic excited state simulations are used to compute X-ray Raman signals, which are able to sensitively monitor the coherence evolution. Our results verify their vibronic nature, that survives multiple conical intersection passages for several hundred femtoseconds at room temperature. Despite the contributions of highly heterogeneous evolution pathways, the coherences are unambiguously visualized by the experimentally accessible X-ray signals. They offer direct information on the dynamics of electronic and structural degrees of freedom, paving the way for detailed coherence measurements in functional organic materials.
Fil: Keefer, Daniel. University of California at Irvine; Estados Unidos
Fil: Freixas Lemus, Victor Manuel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina
Fil: Song, Huajing. Los Alamos National Laboratory; Estados Unidos
Fil: Tretiak, Sergei. Los Alamos National Laboratory; Estados Unidos
Fil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina
Fil: Mukamel, Shaul. University of California at Irvine; Estados Unidos
Materia
Dinámica molecular
Señales espectroscópicas
TRUECARS
NEXMD
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:11336/165137
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/165137
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopyKeefer, DanielFreixas Lemus, Victor ManuelSong, HuajingTretiak, SergeiFernández Alberti, SebastiánMukamel, ShaulDinámica molecularSeñales espectroscópicasTRUECARSNEXMDhttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The role of quantum-mechanical coherences in the elementary photophysics of functional optoelectronic molecular materials is currently under active study. Designing and controlling stable coherences arising from concerted vibronic dynamics in organic chromophores is the key for numerous applications. Here, we present fundamental insight into the energy transfer properties of a rigid synthetic heterodimer that has been experimentally engineered to study coherences. Quantum non-adiabatic excited state simulations are used to compute X-ray Raman signals, which are able to sensitively monitor the coherence evolution. Our results verify their vibronic nature, that survives multiple conical intersection passages for several hundred femtoseconds at room temperature. Despite the contributions of highly heterogeneous evolution pathways, the coherences are unambiguously visualized by the experimentally accessible X-ray signals. They offer direct information on the dynamics of electronic and structural degrees of freedom, paving the way for detailed coherence measurements in functional organic materials.Fil: Keefer, Daniel. University of California at Irvine; Estados UnidosFil: Freixas Lemus, Victor Manuel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; ArgentinaFil: Song, Huajing. Los Alamos National Laboratory; Estados UnidosFil: Tretiak, Sergei. Los Alamos National Laboratory; Estados UnidosFil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; ArgentinaFil: Mukamel, Shaul. University of California at Irvine; Estados UnidosRoyal Society of Chemistry2021-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/165137Keefer, Daniel; Freixas Lemus, Victor Manuel; Song, Huajing; Tretiak, Sergei; Fernández Alberti, Sebastián; et al.; Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy; Royal Society of Chemistry; Chemical Science; 12; 14; 4-2021; 5286-52942041-65202041-6539CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2021/SC/D0SC06328Binfo:eu-repo/semantics/altIdentifier/doi/10.1039/D0SC06328Binfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-11-12T09:45:44Zoai:ri.conicet.gov.ar:11336/165137instacron: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:34982025-11-12 09:45:44.68CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
title Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
spellingShingle Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
Keefer, Daniel
Dinámica molecular
Señales espectroscópicas
TRUECARS
NEXMD
title_short Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
title_full Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
title_fullStr Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
title_full_unstemmed Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
title_sort Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy
dc.creator.none.fl_str_mv Keefer, Daniel
Freixas Lemus, Victor Manuel
Song, Huajing
Tretiak, Sergei
Fernández Alberti, Sebastián
Mukamel, Shaul
author Keefer, Daniel
author_facet Keefer, Daniel
Freixas Lemus, Victor Manuel
Song, Huajing
Tretiak, Sergei
Fernández Alberti, Sebastián
Mukamel, Shaul
author_role author
author2 Freixas Lemus, Victor Manuel
Song, Huajing
Tretiak, Sergei
Fernández Alberti, Sebastián
Mukamel, Shaul
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Dinámica molecular
Señales espectroscópicas
TRUECARS
NEXMD
topic Dinámica molecular
Señales espectroscópicas
TRUECARS
NEXMD
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The role of quantum-mechanical coherences in the elementary photophysics of functional optoelectronic molecular materials is currently under active study. Designing and controlling stable coherences arising from concerted vibronic dynamics in organic chromophores is the key for numerous applications. Here, we present fundamental insight into the energy transfer properties of a rigid synthetic heterodimer that has been experimentally engineered to study coherences. Quantum non-adiabatic excited state simulations are used to compute X-ray Raman signals, which are able to sensitively monitor the coherence evolution. Our results verify their vibronic nature, that survives multiple conical intersection passages for several hundred femtoseconds at room temperature. Despite the contributions of highly heterogeneous evolution pathways, the coherences are unambiguously visualized by the experimentally accessible X-ray signals. They offer direct information on the dynamics of electronic and structural degrees of freedom, paving the way for detailed coherence measurements in functional organic materials.
Fil: Keefer, Daniel. University of California at Irvine; Estados Unidos
Fil: Freixas Lemus, Victor Manuel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina
Fil: Song, Huajing. Los Alamos National Laboratory; Estados Unidos
Fil: Tretiak, Sergei. Los Alamos National Laboratory; Estados Unidos
Fil: Fernández Alberti, Sebastián. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina
Fil: Mukamel, Shaul. University of California at Irvine; Estados Unidos
description The role of quantum-mechanical coherences in the elementary photophysics of functional optoelectronic molecular materials is currently under active study. Designing and controlling stable coherences arising from concerted vibronic dynamics in organic chromophores is the key for numerous applications. Here, we present fundamental insight into the energy transfer properties of a rigid synthetic heterodimer that has been experimentally engineered to study coherences. Quantum non-adiabatic excited state simulations are used to compute X-ray Raman signals, which are able to sensitively monitor the coherence evolution. Our results verify their vibronic nature, that survives multiple conical intersection passages for several hundred femtoseconds at room temperature. Despite the contributions of highly heterogeneous evolution pathways, the coherences are unambiguously visualized by the experimentally accessible X-ray signals. They offer direct information on the dynamics of electronic and structural degrees of freedom, paving the way for detailed coherence measurements in functional organic materials.
publishDate 2021
dc.date.none.fl_str_mv 2021-04
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/11336/165137
Keefer, Daniel; Freixas Lemus, Victor Manuel; Song, Huajing; Tretiak, Sergei; Fernández Alberti, Sebastián; et al.; Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy; Royal Society of Chemistry; Chemical Science; 12; 14; 4-2021; 5286-5294
2041-6520
2041-6539
CONICET Digital
CONICET
url http://hdl.handle.net/11336/165137
identifier_str_mv Keefer, Daniel; Freixas Lemus, Victor Manuel; Song, Huajing; Tretiak, Sergei; Fernández Alberti, Sebastián; et al.; Monitoring molecular vibronic coherences in a bichromophoric molecule by ultrafast X-ray spectroscopy; Royal Society of Chemistry; Chemical Science; 12; 14; 4-2021; 5286-5294
2041-6520
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://pubs.rsc.org/en/content/articlelanding/2021/SC/D0SC06328B
info:eu-repo/semantics/altIdentifier/doi/10.1039/D0SC06328B
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
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score 13.24909

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