Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule

Intramolecular charge transfer (CT) processes play a crucial role in fields such as energy conversion, molecular electronics, and biochemistry. Defined by the movement of electronic charge between donor and acceptor groups within a molecule, CT is inherently coupled with nuclear motions, making it e...

Descripción completa

Detalles Bibliográficos
Autores: Mocci, Daniele, Reino González, Juan, Wu, Yingxuan, González Vázquez, Jesús, Vismarra, Federico, Fernández-Villoria, Francisco, Urieta-Mora, Javier, Palacios Cañas, Alicia, Recio, Pedro, Cachon, Javier, Bañares, Luis, Lucchini, Matteo, Reduzzi, Maurizio, Borrego-Varillas, Rocío, Martín, Nazario, Martín García, Fernando, Nisoli, Mauro
Tipo de recurso: artículo
Fecha de publicación:2025
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/735100
Acceso en línea:https://hdl.handle.net/10486/735100
https://dx.doi.org/10.34133/ultrafastscience.0108
Access Level:acceso abierto
Palabra clave:Química
id ES_e646b9f7ef0d2fbfef0a55dc4e60a0ab
oai_identifier_str oai:repositorio.uam.es:10486/735100
network_acronym_str ES
network_name_str España
repository_id_str
spelling Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl MoleculeMocci, DanieleReino González, JuanWu, YingxuanGonzález Vázquez, JesúsVismarra, FedericoFernández-Villoria, FranciscoUrieta-Mora, JavierPalacios Cañas, AliciaRecio, PedroCachon, JavierBañares, LuisLucchini, MatteoReduzzi, MaurizioBorrego-Varillas, RocíoMartín, NazarioMartín García, FernandoNisoli, MauroQuímicaIntramolecular charge transfer (CT) processes play a crucial role in fields such as energy conversion, molecular electronics, and biochemistry. Defined by the movement of electronic charge between donor and acceptor groups within a molecule, CT is inherently coupled with nuclear motions, making it essential for the understanding of energy flow and reaction mechanisms in molecular systems. Here, we employ attosecond pump-probe spectroscopy to explore the ultrafast dynamics of 4-amino-4′-nitrobiphenyl (ANB), a donor–π–acceptor molecule. Our experimental results in combination with time-dependent density functional theory and trajectory surface hopping simulations uncover a complex temporal evolution of CT spanning from a few to tens of femtoseconds. The process unfolds in distinct stages. An initial phase is marked by an ultrafast charge migration driven by a molecular planarization process, and it is followed by oscillations in the charge distribution that have a 2-fold origin: the electronic coherence induced by the broadband attosecond pulse and the coupling with nuclear motion. In ANB, these dynamics are exemplified by oscillations in charge density and structural parameters, such as dihedral angles and bond lengths, underscoring the interconnection between electronic and nuclear degrees of freedomThis project has received funding from the EuropeanResearch Council (ERC) under the European Union’s Horizon2020 research and innovation programme (grant agreementno. 951224, TOMATTO). P.R., J.C., and L.B. acknowledge financial support from the Spanish Ministry of Science and Innovation under grants PID2021-122839NB-I00 and PID2023-146373OB-I00, and from Laserlab Europe EU-H2020 grantagreement number 654148, project CUSBO002616American Association for the Advancement of ScienceDepartamento de QuímicaFacultad de CienciasEuropean Research CouncilGobierno de España20252025-08-05research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttps://hdl.handle.net/10486/735100https://dx.doi.org/10.34133/ultrafastscience.0108reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengEuropean Commission http://dx.doi.org/10.13039/501100000780 Horizon 2020 Framework Programme 951224open accesshttp://purl.org/coar/access_right/c_abf2Attribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7351002026-06-23T12:46:27Z
dc.title.none.fl_str_mv Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
title Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
spellingShingle Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
Mocci, Daniele
Química
title_short Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
title_full Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
title_fullStr Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
title_full_unstemmed Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
title_sort Ultrafast Structural Reorganization and Charge Dynamics in a Photoionized Donor–Acceptor Biphenyl Molecule
dc.creator.none.fl_str_mv Mocci, Daniele
Reino González, Juan
Wu, Yingxuan
González Vázquez, Jesús
Vismarra, Federico
Fernández-Villoria, Francisco
Urieta-Mora, Javier
Palacios Cañas, Alicia
Recio, Pedro
Cachon, Javier
Bañares, Luis
Lucchini, Matteo
Reduzzi, Maurizio
Borrego-Varillas, Rocío
Martín, Nazario
Martín García, Fernando
Nisoli, Mauro
author Mocci, Daniele
author_facet Mocci, Daniele
Reino González, Juan
Wu, Yingxuan
González Vázquez, Jesús
Vismarra, Federico
Fernández-Villoria, Francisco
Urieta-Mora, Javier
Palacios Cañas, Alicia
Recio, Pedro
Cachon, Javier
Bañares, Luis
Lucchini, Matteo
Reduzzi, Maurizio
Borrego-Varillas, Rocío
Martín, Nazario
Martín García, Fernando
Nisoli, Mauro
author_role author
author2 Reino González, Juan
Wu, Yingxuan
González Vázquez, Jesús
Vismarra, Federico
Fernández-Villoria, Francisco
Urieta-Mora, Javier
Palacios Cañas, Alicia
Recio, Pedro
Cachon, Javier
Bañares, Luis
Lucchini, Matteo
Reduzzi, Maurizio
Borrego-Varillas, Rocío
Martín, Nazario
Martín García, Fernando
Nisoli, Mauro
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Departamento de Química
Facultad de Ciencias
European Research Council
Gobierno de España
dc.subject.none.fl_str_mv Química
topic Química
description Intramolecular charge transfer (CT) processes play a crucial role in fields such as energy conversion, molecular electronics, and biochemistry. Defined by the movement of electronic charge between donor and acceptor groups within a molecule, CT is inherently coupled with nuclear motions, making it essential for the understanding of energy flow and reaction mechanisms in molecular systems. Here, we employ attosecond pump-probe spectroscopy to explore the ultrafast dynamics of 4-amino-4′-nitrobiphenyl (ANB), a donor–π–acceptor molecule. Our experimental results in combination with time-dependent density functional theory and trajectory surface hopping simulations uncover a complex temporal evolution of CT spanning from a few to tens of femtoseconds. The process unfolds in distinct stages. An initial phase is marked by an ultrafast charge migration driven by a molecular planarization process, and it is followed by oscillations in the charge distribution that have a 2-fold origin: the electronic coherence induced by the broadband attosecond pulse and the coupling with nuclear motion. In ANB, these dynamics are exemplified by oscillations in charge density and structural parameters, such as dihedral angles and bond lengths, underscoring the interconnection between electronic and nuclear degrees of freedom
publishDate 2025
dc.date.none.fl_str_mv 2025
2025-08-05
dc.type.none.fl_str_mv research article
http://purl.org/coar/resource_type/c_2df8fbb1
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/10486/735100
https://dx.doi.org/10.34133/ultrafastscience.0108
url https://hdl.handle.net/10486/735100
https://dx.doi.org/10.34133/ultrafastscience.0108
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv European Commission http://dx.doi.org/10.13039/501100000780 Horizon 2020 Framework Programme 951224
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International
http://creativecommons.org/licenses/by/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution 4.0 International
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Association for the Advancement of Science
publisher.none.fl_str_mv American Association for the Advancement of Science
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869422752099729408
score 15,811543

Similares en LA Referencia