Structural control of highly efficient thermally activated delayed fluorescence in carbene zinc(II) dithiolates

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dc.contributor.authorMitra, Mousree
dc.contributor.authorMrózek, Ondřej
dc.contributor.authorPutscher, Markus
dc.contributor.authorGuhl, Jasper
dc.contributor.authorHupp, Benjamin
dc.contributor.authorBelyaev, Andrey
dc.contributor.authorMarian, Christel M.
dc.contributor.authorSteffen, Andreas
dc.date.accessioned2025-04-03T07:50:17Z
dc.date.available2025-04-03T07:50:17Z
dc.date.issued2023-12-08
dc.description.abstractLuminescent metal complexes based on earth abundant elements are a valuable target to substitute 4d/5d transition metal complexes as triplet emitters in advanced photonic applications. Whereas CuI complexes have been thoroughly investigated in the last two decades for this purpose, no structure-property-relationships for efficient luminescence involving triplet excited states from ZnII complexes are established. Herein, we report on the design of monomeric carbene zinc(II) dithiolates (CZT) featuring a donor-acceptor-motif that leads to highly efficient thermally activated delayed fluorescence (TADF) with for ZnII compounds unprecedented radiative rate constants kTADF=1.2×106 s−1 at 297 K. Our high-level DFT/MRCI calculations revealed that the relative orientation of the ligands involved in the ligand-to-ligand charge transfer (1/3LLCT) states is paramount to control the TADF process. Specifically, a dihedral angle of 36–40° leads to very efficient reverse intersystem-crossing (rISC) on the order of 109 s−1 due to spin-orbit coupling (SOC) mediated by the sulfur atoms in combination with a small ΔES1-T1 of ca. 56 meV.en
dc.identifier.urihttp://hdl.handle.net/2003/43589
dc.identifier.urihttp://dx.doi.org/10.17877/DE290R-25422
dc.language.isoen
dc.relation.ispartofseriesAngewandte Chemie. International edition; 63(7)
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.subjectCarbenesen
dc.subjectCircularly Polarized Luminescenceen
dc.subjectDFT/MRCIen
dc.subjectTADFen
dc.subjectZincen
dc.subject.ddc540
dc.titleStructural control of highly efficient thermally activated delayed fluorescence in carbene zinc(II) dithiolatesen
dc.typeText
dc.type.publicationtypeResearchArticle
dcterms.accessRightsopen access
eldorado.secondarypublicationtrue
eldorado.secondarypublication.primarycitationM. Mitra, O. Mrózek, M. Putscher, J. Guhl, B. Hupp, A. Belyaev, C. M. Marian, A. Steffen, Angew. Chem. Int. Ed. 2024, 63, e202316300. https://doi.org/10.1002/anie.202316300
eldorado.secondarypublication.primaryidentifierhttps://doi.org/10.1002/anie.202316300

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