Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime

Autores
Berdakin, Matias; Féraud, Geraldine; Dedonder Lardeux, Claude; Jouvet, Christophe; Pino, Gustavo Ariel
Año de publicación
2014
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Recently, DNA molecules have received great attention because of their potential applications in material science. One interesting example is the production of highly fluorescent and tunable DNA–Agn clusters with cytosine (C)-rich DNA strands. Here, we report the UV photofragmentation spectra of gas-phase cytosine···Ag+···cytosine (C2Ag+) and cytosine···H+···cytosine (C2H+) complexes together with theoretical calculations. In both cases, the excitation energy does not differ significantly from that of isolated cytosine or protonated cytosine, indicating that the excitation takes place on the DNA base. However, the excited-state lifetime of the C2H+ (τ = 85 fs), estimated from the bandwidth of the spectrum, is at least 2 orders of magnitude shorter than that of the C2Ag+ (τ > 5000 fs). The increased excited-state lifetime upon silver complexation is quite unexpected, and it clearly opens the question about what factors are controlling the nonradiative decay in pyrimidine DNA bases. This is an important result for the expanding field of metal-mediated base pairing and may also be important to the photophysical properties of DNA-templated fluorescent silver clusters.
Fil: Berdakin, Matias. 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: Féraud, Geraldine. Aix Marseille Université. Marsella; Francia
Fil: Dedonder Lardeux, Claude. Aix Marseille Université. Marsella; Francia
Fil: Jouvet, Christophe. Aix Marseille Université. Marsella; Francia
Fil: Pino, Gustavo Ariel. 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
Materia
Dna Bases
Dna−Agn Cluster
Excited State
Metal-Mediated Base Pairs
Photofragmentation 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:11336/31368
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/31368
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated LifetimeBerdakin, MatiasFéraud, GeraldineDedonder Lardeux, ClaudeJouvet, ChristophePino, Gustavo ArielDna BasesDna−Agn ClusterExcited StateMetal-Mediated Base PairsPhotofragmentation Spectroscopyhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Recently, DNA molecules have received great attention because of their potential applications in material science. One interesting example is the production of highly fluorescent and tunable DNA–Agn clusters with cytosine (C)-rich DNA strands. Here, we report the UV photofragmentation spectra of gas-phase cytosine···Ag+···cytosine (C2Ag+) and cytosine···H+···cytosine (C2H+) complexes together with theoretical calculations. In both cases, the excitation energy does not differ significantly from that of isolated cytosine or protonated cytosine, indicating that the excitation takes place on the DNA base. However, the excited-state lifetime of the C2H+ (τ = 85 fs), estimated from the bandwidth of the spectrum, is at least 2 orders of magnitude shorter than that of the C2Ag+ (τ > 5000 fs). The increased excited-state lifetime upon silver complexation is quite unexpected, and it clearly opens the question about what factors are controlling the nonradiative decay in pyrimidine DNA bases. This is an important result for the expanding field of metal-mediated base pairing and may also be important to the photophysical properties of DNA-templated fluorescent silver clusters.Fil: Berdakin, Matias. 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: Féraud, Geraldine. Aix Marseille Université. Marsella; FranciaFil: Dedonder Lardeux, Claude. Aix Marseille Université. Marsella; FranciaFil: Jouvet, Christophe. Aix Marseille Université. Marsella; FranciaFil: Pino, Gustavo Ariel. 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; ArgentinaAmerican Chemical Society2014-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/31368Berdakin, Matias; Féraud, Geraldine; Dedonder Lardeux, Claude; Jouvet, Christophe; Pino, Gustavo Ariel; Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime; American Chemical Society; The Journal of Physical Chemistry Letters; 5; 13; 6-2014; 2295-23011948-7185CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/jz5009455info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/jz5009455info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:00:58Zoai:ri.conicet.gov.ar:11336/31368instacron: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:34982025-10-22 11:00:58.956CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
title Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
spellingShingle Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
Berdakin, Matias
Dna Bases
Dna−Agn Cluster
Excited State
Metal-Mediated Base Pairs
Photofragmentation Spectroscopy
title_short Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
title_full Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
title_fullStr Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
title_full_unstemmed Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
title_sort Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime
dc.creator.none.fl_str_mv Berdakin, Matias
Féraud, Geraldine
Dedonder Lardeux, Claude
Jouvet, Christophe
Pino, Gustavo Ariel
author Berdakin, Matias
author_facet Berdakin, Matias
Féraud, Geraldine
Dedonder Lardeux, Claude
Jouvet, Christophe
Pino, Gustavo Ariel
author_role author
author2 Féraud, Geraldine
Dedonder Lardeux, Claude
Jouvet, Christophe
Pino, Gustavo Ariel
author2_role author
author
author
author
dc.subject.none.fl_str_mv Dna Bases
Dna−Agn Cluster
Excited State
Metal-Mediated Base Pairs
Photofragmentation Spectroscopy
topic Dna Bases
Dna−Agn Cluster
Excited State
Metal-Mediated Base Pairs
Photofragmentation 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 Recently, DNA molecules have received great attention because of their potential applications in material science. One interesting example is the production of highly fluorescent and tunable DNA–Agn clusters with cytosine (C)-rich DNA strands. Here, we report the UV photofragmentation spectra of gas-phase cytosine···Ag+···cytosine (C2Ag+) and cytosine···H+···cytosine (C2H+) complexes together with theoretical calculations. In both cases, the excitation energy does not differ significantly from that of isolated cytosine or protonated cytosine, indicating that the excitation takes place on the DNA base. However, the excited-state lifetime of the C2H+ (τ = 85 fs), estimated from the bandwidth of the spectrum, is at least 2 orders of magnitude shorter than that of the C2Ag+ (τ > 5000 fs). The increased excited-state lifetime upon silver complexation is quite unexpected, and it clearly opens the question about what factors are controlling the nonradiative decay in pyrimidine DNA bases. This is an important result for the expanding field of metal-mediated base pairing and may also be important to the photophysical properties of DNA-templated fluorescent silver clusters.
Fil: Berdakin, Matias. 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: Féraud, Geraldine. Aix Marseille Université. Marsella; Francia
Fil: Dedonder Lardeux, Claude. Aix Marseille Université. Marsella; Francia
Fil: Jouvet, Christophe. Aix Marseille Université. Marsella; Francia
Fil: Pino, Gustavo Ariel. 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
description Recently, DNA molecules have received great attention because of their potential applications in material science. One interesting example is the production of highly fluorescent and tunable DNA–Agn clusters with cytosine (C)-rich DNA strands. Here, we report the UV photofragmentation spectra of gas-phase cytosine···Ag+···cytosine (C2Ag+) and cytosine···H+···cytosine (C2H+) complexes together with theoretical calculations. In both cases, the excitation energy does not differ significantly from that of isolated cytosine or protonated cytosine, indicating that the excitation takes place on the DNA base. However, the excited-state lifetime of the C2H+ (τ = 85 fs), estimated from the bandwidth of the spectrum, is at least 2 orders of magnitude shorter than that of the C2Ag+ (τ > 5000 fs). The increased excited-state lifetime upon silver complexation is quite unexpected, and it clearly opens the question about what factors are controlling the nonradiative decay in pyrimidine DNA bases. This is an important result for the expanding field of metal-mediated base pairing and may also be important to the photophysical properties of DNA-templated fluorescent silver clusters.
publishDate 2014
dc.date.none.fl_str_mv 2014-06
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/11336/31368
Berdakin, Matias; Féraud, Geraldine; Dedonder Lardeux, Claude; Jouvet, Christophe; Pino, Gustavo Ariel; Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime; American Chemical Society; The Journal of Physical Chemistry Letters; 5; 13; 6-2014; 2295-2301
1948-7185
CONICET Digital
CONICET
url http://hdl.handle.net/11336/31368
identifier_str_mv Berdakin, Matias; Féraud, Geraldine; Dedonder Lardeux, Claude; Jouvet, Christophe; Pino, Gustavo Ariel; Effect of Ag+ on the Excited-State Properties of a Gas-Phase (Cytosine)2Ag+ Complex: Electronic Transition and Estimated Lifetime; American Chemical Society; The Journal of Physical Chemistry Letters; 5; 13; 6-2014; 2295-2301
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/jz5009455
info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/10.1021/jz5009455
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 12.982451

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