The Excited‐State Creutz‐Taube Ion

Autores
Pieslinger, German Eduardo; Ramirez Wierzbicki, Ivana Elizabeth; Cadranel, Alejandro
Año de publicación
2022
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The excited-state version of the Creutz–Taube ion was prepared via visible light excitation of [(NH3)5RuII(μ-pz)RuII(NH3)5]4+. The resulting excited state is a mixed valence {RuIII–δ(μ-pz⋅−)RuII+δ} transient species, which was characterized using femtosecond transient absorption spectroscopy with vis-NIR detection. Very intense photoinduced intervalence charge transfers were observed at 7500 cm−1, revealing an excited-state electronic coupling element HDA=3750 cm−1. DFT calculations confirm a strongly delocalized excited state. A notable consequence of strong electron delocalization is the nanosecond excited state lifetime, which was exploited in a proof-of-concept intermolecular electron transfer. The excited-state Creutz–Taube ion is established as a reference, and demonstrates that electron delocalization in the excited state can be leveraged for artificial photosynthesis or other photocatalytic schemes based on electron transfer chemistry.
Fil: Pieslinger, German Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Físico-Química Biológicas "Prof. Alejandro C. Paladini". Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Físico-Química Biológicas; Argentina
Fil: Ramirez Wierzbicki, Ivana Elizabeth. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Cadranel, Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Materia
ELECTRON TRANSFER
ELECTRONIC COUPLING
EXCITED STATES
INTERVALENCE
MIXED VALENCE
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/213867
Acceder
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network_name_str CONICET Digital (CONICET)
spelling The Excited‐State Creutz‐Taube IonPieslinger, German EduardoRamirez Wierzbicki, Ivana ElizabethCadranel, AlejandroELECTRON TRANSFERELECTRONIC COUPLINGEXCITED STATESINTERVALENCEMIXED VALENCEhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The excited-state version of the Creutz–Taube ion was prepared via visible light excitation of [(NH3)5RuII(μ-pz)RuII(NH3)5]4+. The resulting excited state is a mixed valence {RuIII–δ(μ-pz⋅−)RuII+δ} transient species, which was characterized using femtosecond transient absorption spectroscopy with vis-NIR detection. Very intense photoinduced intervalence charge transfers were observed at 7500 cm−1, revealing an excited-state electronic coupling element HDA=3750 cm−1. DFT calculations confirm a strongly delocalized excited state. A notable consequence of strong electron delocalization is the nanosecond excited state lifetime, which was exploited in a proof-of-concept intermolecular electron transfer. The excited-state Creutz–Taube ion is established as a reference, and demonstrates that electron delocalization in the excited state can be leveraged for artificial photosynthesis or other photocatalytic schemes based on electron transfer chemistry.Fil: Pieslinger, German Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Físico-Química Biológicas "Prof. Alejandro C. Paladini". Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Físico-Química Biológicas; ArgentinaFil: Ramirez Wierzbicki, Ivana Elizabeth. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaFil: Cadranel, Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; ArgentinaWiley VCH Verlag2022-09info: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/11336/213867Pieslinger, German Eduardo; Ramirez Wierzbicki, Ivana Elizabeth; Cadranel, Alejandro; The Excited‐State Creutz‐Taube Ion; Wiley VCH Verlag; Angewandte Chemie; 61; 49; 9-2022; 1-71433-7851CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://onlinelibrary.wiley.com/doi/10.1002/anie.202211747info:eu-repo/semantics/altIdentifier/doi/10.1002/anie.202211747info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-10T13:19:20Zoai:ri.conicet.gov.ar:11336/213867instacron: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:34982025-09-10 13:19:21.067CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv The Excited‐State Creutz‐Taube Ion
title The Excited‐State Creutz‐Taube Ion
spellingShingle The Excited‐State Creutz‐Taube Ion
Pieslinger, German Eduardo
ELECTRON TRANSFER
ELECTRONIC COUPLING
EXCITED STATES
INTERVALENCE
MIXED VALENCE
title_short The Excited‐State Creutz‐Taube Ion
title_full The Excited‐State Creutz‐Taube Ion
title_fullStr The Excited‐State Creutz‐Taube Ion
title_full_unstemmed The Excited‐State Creutz‐Taube Ion
title_sort The Excited‐State Creutz‐Taube Ion
dc.creator.none.fl_str_mv Pieslinger, German Eduardo
Ramirez Wierzbicki, Ivana Elizabeth
Cadranel, Alejandro
author Pieslinger, German Eduardo
author_facet Pieslinger, German Eduardo
Ramirez Wierzbicki, Ivana Elizabeth
Cadranel, Alejandro
author_role author
author2 Ramirez Wierzbicki, Ivana Elizabeth
Cadranel, Alejandro
author2_role author
author
dc.subject.none.fl_str_mv ELECTRON TRANSFER
ELECTRONIC COUPLING
EXCITED STATES
INTERVALENCE
MIXED VALENCE
topic ELECTRON TRANSFER
ELECTRONIC COUPLING
EXCITED STATES
INTERVALENCE
MIXED VALENCE
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 excited-state version of the Creutz–Taube ion was prepared via visible light excitation of [(NH3)5RuII(μ-pz)RuII(NH3)5]4+. The resulting excited state is a mixed valence {RuIII–δ(μ-pz⋅−)RuII+δ} transient species, which was characterized using femtosecond transient absorption spectroscopy with vis-NIR detection. Very intense photoinduced intervalence charge transfers were observed at 7500 cm−1, revealing an excited-state electronic coupling element HDA=3750 cm−1. DFT calculations confirm a strongly delocalized excited state. A notable consequence of strong electron delocalization is the nanosecond excited state lifetime, which was exploited in a proof-of-concept intermolecular electron transfer. The excited-state Creutz–Taube ion is established as a reference, and demonstrates that electron delocalization in the excited state can be leveraged for artificial photosynthesis or other photocatalytic schemes based on electron transfer chemistry.
Fil: Pieslinger, German Eduardo. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Houssay. Instituto de Química y Físico-Química Biológicas "Prof. Alejandro C. Paladini". Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Instituto de Química y Físico-Química Biológicas; Argentina
Fil: Ramirez Wierzbicki, Ivana Elizabeth. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Cadranel, Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
description The excited-state version of the Creutz–Taube ion was prepared via visible light excitation of [(NH3)5RuII(μ-pz)RuII(NH3)5]4+. The resulting excited state is a mixed valence {RuIII–δ(μ-pz⋅−)RuII+δ} transient species, which was characterized using femtosecond transient absorption spectroscopy with vis-NIR detection. Very intense photoinduced intervalence charge transfers were observed at 7500 cm−1, revealing an excited-state electronic coupling element HDA=3750 cm−1. DFT calculations confirm a strongly delocalized excited state. A notable consequence of strong electron delocalization is the nanosecond excited state lifetime, which was exploited in a proof-of-concept intermolecular electron transfer. The excited-state Creutz–Taube ion is established as a reference, and demonstrates that electron delocalization in the excited state can be leveraged for artificial photosynthesis or other photocatalytic schemes based on electron transfer chemistry.
publishDate 2022
dc.date.none.fl_str_mv 2022-09
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/11336/213867
Pieslinger, German Eduardo; Ramirez Wierzbicki, Ivana Elizabeth; Cadranel, Alejandro; The Excited‐State Creutz‐Taube Ion; Wiley VCH Verlag; Angewandte Chemie; 61; 49; 9-2022; 1-7
1433-7851
CONICET Digital
CONICET
url http://hdl.handle.net/11336/213867
identifier_str_mv Pieslinger, German Eduardo; Ramirez Wierzbicki, Ivana Elizabeth; Cadranel, Alejandro; The Excited‐State Creutz‐Taube Ion; Wiley VCH Verlag; Angewandte Chemie; 61; 49; 9-2022; 1-7
1433-7851
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://onlinelibrary.wiley.com/doi/10.1002/anie.202211747
info:eu-repo/semantics/altIdentifier/doi/10.1002/anie.202211747
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
application/pdf
dc.publisher.none.fl_str_mv Wiley VCH Verlag
publisher.none.fl_str_mv Wiley VCH Verlag
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 12.48226

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