Thermally Activated Delayed Fluorescence: Polarity, Rigidity, and Disorder in Condensed Phases.
| Autor: | Phan Huu DKA; Department of Chemistry, Life Sciences and Environmental Sustainability, University of Parma, 43124 Parma, Italy., Saseendran S; Department of Chemistry, Life Sciences and Environmental Sustainability, University of Parma, 43124 Parma, Italy., Dhali R; Department of Chemistry, Life Sciences and Environmental Sustainability, University of Parma, 43124 Parma, Italy., Franca LG; Department of Physics, Durham University, South Road, Durham DH1 3LE, U.K., Stavrou K; Department of Physics, Durham University, South Road, Durham DH1 3LE, U.K., Monkman A; Department of Physics, Durham University, South Road, Durham DH1 3LE, U.K., Painelli A; Department of Chemistry, Life Sciences and Environmental Sustainability, University of Parma, 43124 Parma, Italy. |
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| Jazyk: | angličtina |
| Zdroj: | Journal of the American Chemical Society [J Am Chem Soc] 2022 Aug 24; Vol. 144 (33), pp. 15211-15222. Date of Electronic Publication: 2022 Aug 09. |
| DOI: | 10.1021/jacs.2c05537 |
| Abstrakt: | We present a detailed and comprehensive picture of the photophysics of thermally activated delayed fluorescence (TADF). The approach relies on a few-state model, parametrized ab initio on a prototypical TADF dye, that explicitly accounts for the nonadiabatic coupling between electrons and vibrational and conformational motion, crucial to properly address (reverse) intersystem crossing rates. The Onsager model is exploited to account for the medium polarity and polarizability, with careful consideration of the different time scales of relevant degrees of freedom. TADF photophysics is then quantitatively addressed in a coherent and exhaustive approach that accurately reproduces the complex temporal evolution of emission spectra in liquid solvents as well as in solid organic matrices. The different rigidity of the two environments is responsible for the appearance in matrices of important inhomogeneous broadening phenomena that are ascribed to the intertwined contribution from (quasi)static conformational and dielectric disorder. |
| Databáze: | MEDLINE |
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