Generation of multiple triplet states in an orthogonal bodipy dimer: a breakthrough spectroscopic and theoretical approach

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dc.contributor.authorGarcía Moreno, Inmaculada
dc.contributor.authorPostils, Verónica
dc.contributor.authorRebollar, Esther
dc.contributor.authorOrtiz García, María Josefa
dc.contributor.authorRodríguez Agarrabeitia, Antonia
dc.contributor.authorCasanova, David
dc.date.accessioned2023-06-22T10:53:43Z
dc.date.available2023-06-22T10:53:43Z
dc.date.issued2022-02-14
dc.descriptionSubmitted: 15 Dec 2021; Accepted: 14 Feb 2022; First published : 14 Feb 2022
dc.description.abstractGeneration of triplet states in assemblies of organic chromophores is extremely appealing for their potential use in optoelectronic applications. In this work, we investigate the intricacies of triplet state generation in an orthogonal BODIPY dimer by combining delayed photoemission techniques with electronic structure calculations. Our analysis provides a deep understanding of the electronic states involved, and describes different competing deactivation channels beyond prompt radiative decay. In particular, we identify charge-transfer (CT) mediated intersystem crossing (ISC) as the most likely mechanism for the triplet state generation in this system. The different emission bands at long times can be associated with delayed fluorescence, CT emission and phosphorescence from multiple low-energy triplets. Interestingly, the dependence of the yield of triplet state population and emission profiles with the solvent polarity evidences the decisive role of the CT configuration in the fate of the photoactivated dimer, controlling the relative ISC, reverse ISC, and internal conversion efficiencies. Overall, the present results provide a rather complete description of the delayed photophysics in the BODIPY dimer, but are not able to fully rationalize the unexpected photoluminescence recorded at long wavelengths (≥ 900 nm). We hypothesize that the origin of this emission, not present in BODIPY monomers, emerges from intermonomer interactions triggered by intramolecular distortions opening up a new vision in the controverted mechanism driving the photophysical behavior from orthogonally linked organic monomers.
dc.description.departmentSección Deptal. de Química Orgánica (Óptica y Optometría)
dc.description.facultyFac. de Óptica y Optometría
dc.description.refereedTRUE
dc.description.sponsorshipMinisterio de Ciencia e Innovación (MICINN)
dc.description.sponsorshipGobierno Vasco
dc.description.sponsorshipUniversidad del País Vasco
dc.description.statuspub
dc.eprint.idhttps://eprints.ucm.es/id/eprint/74026
dc.identifier.doi10.1039/D1CP05730H
dc.identifier.issn1463-9076
dc.identifier.officialurlhttps://doi.org/10.1039/D1CP05730H
dc.identifier.relatedurlhttps://pubs.rsc.org/en/content/articlelanding/2022/cp/d1cp05730h
dc.identifier.urihttps://hdl.handle.net/20.500.14352/71851
dc.issue.number10
dc.journal.titlePhysical chemistry chemical physics
dc.language.isoeng
dc.page.final5938
dc.page.initial5929
dc.publisherRoyal Society of Chemistry
dc.relation.projectID(PID2019-106125GB-I00/AEI/10.13039/ 501100011033, PID2020-114755GB-C31, PID2020-114755GB-C32 and PID2019-109555GB-I00)
dc.relation.projectIDPIBA19-0004
dc.relation.projectIDESPDOC18/85
dc.rights.accessRightsrestricted access
dc.subject.cdu547.1
dc.subject.cdu543.42
dc.subject.cdu621.383
dc.subject.keywordBODIPY
dc.subject.keywordtriplet states
dc.subject.keywordorganic chromophores
dc.subject.ucmPartículas
dc.subject.ucmQuímica orgánica (Química)
dc.subject.ucmOptoelectrónica
dc.subject.unesco2208 Nucleónica
dc.subject.unesco2306 Química Orgánica
dc.titleGeneration of multiple triplet states in an orthogonal bodipy dimer: a breakthrough spectroscopic and theoretical approach
dc.typejournal article
dc.volume.number24
dspace.entity.typePublication
relation.isAuthorOfPublication07f337af-8a30-4929-81db-4e92176e5c87
relation.isAuthorOfPublication0486160c-3df6-4270-bf91-3e96cd33d85d
relation.isAuthorOfPublication.latestForDiscovery0486160c-3df6-4270-bf91-3e96cd33d85d
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