Woon, Kai Lin and Nikishau, Pavel A. and Sini, Gjergji (2022) Fast and accurate determination of the singlet-triplet gap in donor-acceptor and multiresonance TADF molecules by using hole-hole Tamm-Dancoff approximated density functional theory. Advanced Theory and Simulations, 5 (8). ISSN 2513-0390, DOI https://doi.org/10.1002/adts.202200056.
Full text not available from this repository.Abstract
One of the requirements to design efficient emitters based on the multiresonance (MR)- or donor-acceptor (D-A) thermally activated delayed fluorescence (TADF) materials is a relatively small energy gap between the lowest singlet and triplet excited states (Delta E-ST). High-level ab initio calculations of their Delta E-ST provide benchmark results, but they are very time consuming and little practical for large-size systems. Here, the performances of hole-hole Tamm-Dancoff approximated density functional theory (hh-TDA-DFT) and the functional dependent accuracy of hh-TDA are examined on SE of a large number of MR- and D-A TADF molecules. The results indicate that hh-TDA combined with the hybrid functional B3LYP can predict Delta E-ST values for a wide number of MR-TADF molecules with mean absolute error (MAE) within 0.04 eV with correlation as high as 0.75. For D-A TADF molecules, Delta E-ST is less sensitive to the nature of the functionals, with MAE as low as 0.07 eV. The larger discrepancy between Delta E-ST obtained obtained from hh-TDA-DFT and experimental data in several oxygen-containing MR-TADF molecules is assumed to stem from the aggregation tendency of these compounds in solution. These findings provide important insights on the role of aggregation in reducing the Delta E-ST of of MR-TADF compounds.
| Item Type: | Article |
|---|---|
| Funders: | Marie Curie Actions (Grant No: 823720), University Malaya Research University (Grant No: GPF086B-2020) |
| Uncontrolled Keywords: | Aggregation; Hole-hole Tamm-Dancoff approximated density functional theory; Multiresonance thermally activated delayed fluorescence; Singlet-triplet splitting |
| Subjects: | Q Science > QC Physics |
| Divisions: | Faculty of Science > Department of Physics |
| Depositing User: | Ms. Juhaida Abd Rahim |
| Date Deposited: | 26 Oct 2023 06:12 |
| Last Modified: | 26 Oct 2023 06:12 |
| URI: | http://eprints.um.edu.my/id/eprint/41714 |
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