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Deactivation Routes in Gold(I) Polypyridyl Complexes Internal Conversion Vs Fast Intersystem Crossing

2018-11-05Artigo científico Acesso aberto
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dc.contributor.authorAguiló, Elisabet
dc.contributor.authorMoro, Artur J.
dc.contributor.authorOutis, Mani
dc.contributor.authorPina, João
dc.contributor.authorSarmento, Daniela
dc.contributor.authorMelo, J. Sérgio Seixas de
dc.contributor.authorRodríguez, Laura
dc.contributor.authorLima, João Carlos
dc.contributor.institutionLAQV@REQUIMTE
dc.contributor.institutionDQ - Departamento de Química
dc.contributor.pblACS - American Chemical Society
dc.date.accessioned2019-05-30T22:19:34Z
dc.date.available2019-05-30T22:19:34Z
dc.date.issued2018-11-05
dc.descriptionThe research leading to these results has received funding from Laserlab-Europe (grant agreement 284464, EC's Seventh Framework Programme). The authors are grateful to the Ministry of Economy, Industry and Competitiveness of Spain (AEI/FEDER, UE Project CTQ2016-76120-P). This work was also supported by the Associated Laboratory for Sustainable Chemistry, Clean Processes and Technologies, LAQV, which is financed by national funds from FCT/MEC (UID/QUI/50006/2013) and cofinanced by the ERDF under the PT2020 Partnership Agreement (POCI-01-014S-FEDER-007265). We also acknowledge funding from FEDER (Fundo Europeu de Desenvolvimento Regional) through COMPETE (Programa Operacional Factores de Competitividade). The Coimbra Chemistry Centre is supported by the Fundacao para a Ciencia e a Tecnologia (FCT), Portuguese Agency for Scientific Research, through the programme UID/QUI/UI0313/2013. J.P. acknowledges the project SunStorage Harvesting and storage of solar energy", for financial support, reference POCI-01-0145-FEDER-016387, funded by European Regional Development Fund (ERDF), through COMPETE 2020 - Operational Programme for Competitiveness and Internationalization (OPCI), and by national funds, through FCT.
dc.description.abstractAn electronic spectral and photophysical characterization of three gold(I) complexes containing heterocyclic chromophores differing in the number and arrangement of pyridine rings (pyridine, bipyridine, and terpyridine, with the acronyms pD, bD, and tD respectively) was performed. Quantum yields of fluorescence, internal conversion and triplet state formation, together with the rate constants for singlet to triplet intersystem crossing, S1 ∼ ∼ ∼ S0 internal conversion and fluorescence were measured in order to equate the impact of fast triplet state formation on the amount of triplets formed. The results showed a correlation between the increase on the measured decay values of S1 (leading to the main formation of T1) and the increase in the charge transfer (CT) character of the lowest energy transition, as evaluated from the orthogonality of the frontier orbitals. The measured triplet state quantum yields range from ∼50-60% to 70%, whereas the intersystem crossing rate constants differ by almost 2 orders of magnitude, from 9.4 × 109 s-1 for tD to 8.1 × 1011 s-1 for bD. This constitutes an evidence for the existence of a correlation between the intersystem crossing and the internal conversion mechanisms.en
dc.description.versionauthorsversion
dc.description.versionpublished
dc.format.extent8
dc.format.extent958714
dc.identifier.doi10.1021/acs.inorgchem.8b01993
dc.identifier.issn0020-1669
dc.identifier.otherPURE: 13034698
dc.identifier.otherPURE UUID: b657a102-bfee-4ad4-a2c6-e01546212a1c
dc.identifier.otherScopus: 85055032385
dc.identifier.otherPubMed: 30351079
dc.identifier.otherWOS: 000449576900042
dc.identifier.otherORCID: /0000-0003-0528-1967/work/63726053
dc.identifier.urihttp://www.scopus.com/inward/record.url?scp=85055032385&partnerID=8YFLogxK
dc.identifier.urlhttps://www.scopus.com/pages/publications/85055032385
dc.language.isoeng
dc.peerreviewedyes
dc.relationinfo:eu-repo/grantAgreement/FCT/5876/147218/PT
dc.subjectPhysical and Theoretical Chemistry
dc.subjectInorganic Chemistry
dc.subjectSDG 7 - Affordable and Clean Energy
dc.titleDeactivation Routes in Gold(I) Polypyridyl Complexes Internal Conversion Vs Fast Intersystem Crossingen
dc.typejournal article
degois.publication.firstPage13423
degois.publication.issue21
degois.publication.lastPage13430
degois.publication.titleInorganic Chemistry
degois.publication.volume57
dspace.entity.typePublication
oaire.awardNumberUID/QUI/50006/2013
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/5876/UID%2FQUI%2F50006%2F2013/PT
oaire.fundingStream5876
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsopenAccess
relation.isProjectOfPublicationb46f8ec0-8992-489c-89d9-54c4a065dc4a
relation.isProjectOfPublication.latestForDiscoveryb46f8ec0-8992-489c-89d9-54c4a065dc4a

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