Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation

Autores
Arsenault, Eric A.; Guerra, Walter Damián; Shee, James; Reyes Cruz, Edgar A.; Yoneda, Yusuke; Wadsworth, Brian L.; Odella, Emmanuel; Urrutia, María Noel; Kodis, Gerdenis; Moore, Gary F.; Head-Gordon, Martin; Moore, Ana L.; Moore, Thomas A.; Fleming, Graham R.
Año de publicación
2022
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Photoinduced proton-coupled electron transfer and long-range two-proton transport via a Grotthuss-type mechanism are investigated in a biomimetic construct. The ultrafast, nonequilibrium dynamics are assessed via two-dimensional electronic vibrational spectroscopy, in concert with electrochemical and computational techniques. A low-frequency mode is identified experimentally and found to promote double proton and electron transfer, supported by recent theoretical simulations of a similar but abbreviated (non-photoactive) system. Excitation frequency peak evolution and center line slope dynamics show direct evidence of strongly coupled nuclear and electronic degrees of freedom, from which we can conclude that the double proton and electron transfer processes are concerted (up to an uncertainty of 24 fs). The nonequilibrium pathway from the photoexcited Franck-Condon region to the E2PT state is characterized by an ∼110 fs time scale. This study and the tools presented herein constitute a new window into hot charge transfer processes involving an electron and multiple protons.
Fil: Arsenault, Eric A.. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos. Berkeley College Of Chemistry; Estados Unidos
Fil: Guerra, Walter Damián. Arizona State University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Shee, James. Berkeley College Of Chemistry; Estados Unidos. Lawrence Berkeley National Laboratory; Estados Unidos
Fil: Reyes Cruz, Edgar A.. Arizona State University; Estados Unidos
Fil: Yoneda, Yusuke. Berkeley College Of Chemistry; Estados Unidos. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos
Fil: Wadsworth, Brian L.. Arizona State University; Estados Unidos
Fil: Odella, Emmanuel. Arizona State University; Estados Unidos
Fil: Urrutia, María Noel. Arizona State University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Kodis, Gerdenis. Arizona State University; Estados Unidos
Fil: Moore, Gary F.. Arizona State University; Estados Unidos
Fil: Head-Gordon, Martin. Lawrence Berkeley National Laboratory; Estados Unidos. Berkeley College Of Chemistry; Estados Unidos
Fil: Moore, Ana L.. Arizona State University; Estados Unidos
Fil: Moore, Thomas A.. Arizona State University; Estados Unidos
Fil: Fleming, Graham R.. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos. Berkeley College Of Chemistry; Estados Unidos
Materia
PROTON-MOTIVE FORCE
GROTTHUSS-TYPE PROCESSES
PHOTODRIVEN PROTON-COUPLED ELECTRON TRANSFER
TWO-DIMENSIONAL ELECTRONIC VIBRATIONAL SPECTROSCOPY
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:11336/205064
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/205064
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocationArsenault, Eric A.Guerra, Walter DamiánShee, JamesReyes Cruz, Edgar A.Yoneda, YusukeWadsworth, Brian L.Odella, EmmanuelUrrutia, María NoelKodis, GerdenisMoore, Gary F.Head-Gordon, MartinMoore, Ana L.Moore, Thomas A.Fleming, Graham R.PROTON-MOTIVE FORCEGROTTHUSS-TYPE PROCESSESPHOTODRIVEN PROTON-COUPLED ELECTRON TRANSFERTWO-DIMENSIONAL ELECTRONIC VIBRATIONAL SPECTROSCOPYhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Photoinduced proton-coupled electron transfer and long-range two-proton transport via a Grotthuss-type mechanism are investigated in a biomimetic construct. The ultrafast, nonequilibrium dynamics are assessed via two-dimensional electronic vibrational spectroscopy, in concert with electrochemical and computational techniques. A low-frequency mode is identified experimentally and found to promote double proton and electron transfer, supported by recent theoretical simulations of a similar but abbreviated (non-photoactive) system. Excitation frequency peak evolution and center line slope dynamics show direct evidence of strongly coupled nuclear and electronic degrees of freedom, from which we can conclude that the double proton and electron transfer processes are concerted (up to an uncertainty of 24 fs). The nonequilibrium pathway from the photoexcited Franck-Condon region to the E2PT state is characterized by an ∼110 fs time scale. This study and the tools presented herein constitute a new window into hot charge transfer processes involving an electron and multiple protons.Fil: Arsenault, Eric A.. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos. Berkeley College Of Chemistry; Estados UnidosFil: Guerra, Walter Damián. Arizona State University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; ArgentinaFil: Shee, James. Berkeley College Of Chemistry; Estados Unidos. Lawrence Berkeley National Laboratory; Estados UnidosFil: Reyes Cruz, Edgar A.. Arizona State University; Estados UnidosFil: Yoneda, Yusuke. Berkeley College Of Chemistry; Estados Unidos. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados UnidosFil: Wadsworth, Brian L.. Arizona State University; Estados UnidosFil: Odella, Emmanuel. Arizona State University; Estados UnidosFil: Urrutia, María Noel. Arizona State University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; ArgentinaFil: Kodis, Gerdenis. Arizona State University; Estados UnidosFil: Moore, Gary F.. Arizona State University; Estados UnidosFil: Head-Gordon, Martin. Lawrence Berkeley National Laboratory; Estados Unidos. Berkeley College Of Chemistry; Estados UnidosFil: Moore, Ana L.. Arizona State University; Estados UnidosFil: Moore, Thomas A.. Arizona State University; Estados UnidosFil: Fleming, Graham R.. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos. Berkeley College Of Chemistry; Estados UnidosAmerican Chemical Society2022-05info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/205064Arsenault, Eric A.; Guerra, Walter Damián; Shee, James; Reyes Cruz, Edgar A.; Yoneda, Yusuke; et al.; Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation; American Chemical Society; The Journal of Physical Chemistry Letters; 13; 20; 5-2022; 4479-44851948-7185CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/acs.jpclett.2c00585info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpclett.2c00585info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:54:21Zoai:ri.conicet.gov.ar:11336/205064instacron: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 09:54:22.186CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
title Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
spellingShingle Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
Arsenault, Eric A.
PROTON-MOTIVE FORCE
GROTTHUSS-TYPE PROCESSES
PHOTODRIVEN PROTON-COUPLED ELECTRON TRANSFER
TWO-DIMENSIONAL ELECTRONIC VIBRATIONAL SPECTROSCOPY
title_short Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
title_full Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
title_fullStr Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
title_full_unstemmed Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
title_sort Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation
dc.creator.none.fl_str_mv Arsenault, Eric A.
Guerra, Walter Damián
Shee, James
Reyes Cruz, Edgar A.
Yoneda, Yusuke
Wadsworth, Brian L.
Odella, Emmanuel
Urrutia, María Noel
Kodis, Gerdenis
Moore, Gary F.
Head-Gordon, Martin
Moore, Ana L.
Moore, Thomas A.
Fleming, Graham R.
author Arsenault, Eric A.
author_facet Arsenault, Eric A.
Guerra, Walter Damián
Shee, James
Reyes Cruz, Edgar A.
Yoneda, Yusuke
Wadsworth, Brian L.
Odella, Emmanuel
Urrutia, María Noel
Kodis, Gerdenis
Moore, Gary F.
Head-Gordon, Martin
Moore, Ana L.
Moore, Thomas A.
Fleming, Graham R.
author_role author
author2 Guerra, Walter Damián
Shee, James
Reyes Cruz, Edgar A.
Yoneda, Yusuke
Wadsworth, Brian L.
Odella, Emmanuel
Urrutia, María Noel
Kodis, Gerdenis
Moore, Gary F.
Head-Gordon, Martin
Moore, Ana L.
Moore, Thomas A.
Fleming, Graham R.
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv PROTON-MOTIVE FORCE
GROTTHUSS-TYPE PROCESSES
PHOTODRIVEN PROTON-COUPLED ELECTRON TRANSFER
TWO-DIMENSIONAL ELECTRONIC VIBRATIONAL SPECTROSCOPY
topic PROTON-MOTIVE FORCE
GROTTHUSS-TYPE PROCESSES
PHOTODRIVEN PROTON-COUPLED ELECTRON TRANSFER
TWO-DIMENSIONAL ELECTRONIC VIBRATIONAL SPECTROSCOPY
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 proton-coupled electron transfer and long-range two-proton transport via a Grotthuss-type mechanism are investigated in a biomimetic construct. The ultrafast, nonequilibrium dynamics are assessed via two-dimensional electronic vibrational spectroscopy, in concert with electrochemical and computational techniques. A low-frequency mode is identified experimentally and found to promote double proton and electron transfer, supported by recent theoretical simulations of a similar but abbreviated (non-photoactive) system. Excitation frequency peak evolution and center line slope dynamics show direct evidence of strongly coupled nuclear and electronic degrees of freedom, from which we can conclude that the double proton and electron transfer processes are concerted (up to an uncertainty of 24 fs). The nonequilibrium pathway from the photoexcited Franck-Condon region to the E2PT state is characterized by an ∼110 fs time scale. This study and the tools presented herein constitute a new window into hot charge transfer processes involving an electron and multiple protons.
Fil: Arsenault, Eric A.. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos. Berkeley College Of Chemistry; Estados Unidos
Fil: Guerra, Walter Damián. Arizona State University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
Fil: Shee, James. Berkeley College Of Chemistry; Estados Unidos. Lawrence Berkeley National Laboratory; Estados Unidos
Fil: Reyes Cruz, Edgar A.. Arizona State University; Estados Unidos
Fil: Yoneda, Yusuke. Berkeley College Of Chemistry; Estados Unidos. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos
Fil: Wadsworth, Brian L.. Arizona State University; Estados Unidos
Fil: Odella, Emmanuel. Arizona State University; Estados Unidos
Fil: Urrutia, María Noel. Arizona State University; Estados Unidos. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina
Fil: Kodis, Gerdenis. Arizona State University; Estados Unidos
Fil: Moore, Gary F.. Arizona State University; Estados Unidos
Fil: Head-Gordon, Martin. Lawrence Berkeley National Laboratory; Estados Unidos. Berkeley College Of Chemistry; Estados Unidos
Fil: Moore, Ana L.. Arizona State University; Estados Unidos
Fil: Moore, Thomas A.. Arizona State University; Estados Unidos
Fil: Fleming, Graham R.. Lawrence Berkeley National Laboratory; Estados Unidos. Kavli Energy Nanosciences Institute At Berkeley; Estados Unidos. Berkeley College Of Chemistry; Estados Unidos
description Photoinduced proton-coupled electron transfer and long-range two-proton transport via a Grotthuss-type mechanism are investigated in a biomimetic construct. The ultrafast, nonequilibrium dynamics are assessed via two-dimensional electronic vibrational spectroscopy, in concert with electrochemical and computational techniques. A low-frequency mode is identified experimentally and found to promote double proton and electron transfer, supported by recent theoretical simulations of a similar but abbreviated (non-photoactive) system. Excitation frequency peak evolution and center line slope dynamics show direct evidence of strongly coupled nuclear and electronic degrees of freedom, from which we can conclude that the double proton and electron transfer processes are concerted (up to an uncertainty of 24 fs). The nonequilibrium pathway from the photoexcited Franck-Condon region to the E2PT state is characterized by an ∼110 fs time scale. This study and the tools presented herein constitute a new window into hot charge transfer processes involving an electron and multiple protons.
publishDate 2022
dc.date.none.fl_str_mv 2022-05
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/11336/205064
Arsenault, Eric A.; Guerra, Walter Damián; Shee, James; Reyes Cruz, Edgar A.; Yoneda, Yusuke; et al.; Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation; American Chemical Society; The Journal of Physical Chemistry Letters; 13; 20; 5-2022; 4479-4485
1948-7185
CONICET Digital
CONICET
url http://hdl.handle.net/11336/205064
identifier_str_mv Arsenault, Eric A.; Guerra, Walter Damián; Shee, James; Reyes Cruz, Edgar A.; Yoneda, Yusuke; et al.; Concerted electron-nuclear motion in proton-coupled electron transfer-driven grotthuss-type proton translocation; American Chemical Society; The Journal of Physical Chemistry Letters; 13; 20; 5-2022; 4479-4485
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.2c00585
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/acs.jpclett.2c00585
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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