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Enhancing thermally activated delayed fluorescence by fine-tuning the dendron donor strength

Research output: Contribution to journalArticlepeer-review

Author(s)

Eimantas Duda, David Hall, Sergey Bagnich, Cameron Lewis Carpenter-Warren, Rishabh Saxena, Michael Y. Wong, David Bradford Cordes, Alexandra Martha Zoya Slawin, David Beljonne, Yoann Olivier, Eli Zysman-Colman

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Abstract

Thermally activated delayed fluorescence (TADF) relies on a small energy gap between the emissive singlet and the non-emissive triplet state, obtained by reducing the wavefunction overlap between donor and acceptor moieties. Efficient emission, however, requires maintaining a good oscillator strength, which is itself based on sufficient overlap of the wavefunctions between donor and acceptor moieties. We demonstrate an approach to subtly fine-tune the required wavefunction overlap by employing donor-dendrons of changing functionality. We use a carbazolyl-phthalonitrile based donor-acceptor core, 2CzPN, as a reference emitter, and progressively localize the hole density through substitution at the 3,6-positions of the carbazole donors (Cz) with further carbazole, (4-tert-butylphenyl)amine (tBuDPA) and phenoxazine (PXZ). Using detailed photoluminescence studies, complemented with Density Functional Theory (DFT) calculations, we show that this approach permits
a gradual decrease of the singlet-triplet gap, ΔEST, from 300 meV to around 10 meV in toluene, yet we also demonstrate why a small ΔEST alone is not enough. While sufficient oscillator strength is maintained with the Cz- and tBuDPA-based donor dendrons, this is not the case for the PXZ-based donor dendron, where the wavefunction overlap is reduced too strongly. Overall, we find the donor-dendron extension approach allows successful fine-tuning of the emitter photoluminescence properties.
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Original languageEnglish
JournalJournal of Physical Chemistry
DOIs
Publication statusAccepted/In press - 1 Oct 2021

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