An oligomer approach for blue thermally activated delayed fluorescent emitters based on twisted donor-acceptor units

Eimantas Duda, Subeesh Madayanad Suresh, David Hall, Sergey Bagnich, Rishabh Saxena, David B. Cordes, Alexandra M. Z. Slawin, David Beljonne, Yoann Olivier*, Anna Köhler*, Eli Zysman-Colman*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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Abstract

The development of efficient blue donor–acceptor thermally activated delayed fluorescence (TADF) emitters remains a challenge. To enhance the efficiency of TADF-related processes of the emitter, we targeted a molecular design that would introduce a large number of intermediate triplet states between the lowest energy excited triplet (T1) and singlet (S1) excited states. Here, we introduce an oligomer approach using repetitive donor–acceptor units to gradually increase the number of quasi-degenerate states. In our design, benzonitrile (BN) moieties were selected as acceptors that are connected together via the amine donors, acting as bridges to adjacent BN acceptors. To preserve the photoluminescence emission wavelength across the series, we employed a design based on an ortho substitution pattern of the donors about the BN acceptor that induces a highly twisted conformation of the emitters, limiting the conjugation. Via a systematic photophysical study, we show that increasing the oligomer size allows for enhancement of the intersystem crossing and reverse intersystem crossing rates. We attribute the increasing intersystem crossing rate to the increasing number of intermediate triplet states along the series, confirmed by the time-dependent density functional theory. Overall, we reportan approach to enhance the efficiency of TADF-related processes without changing the blue photoluminescence color.
Original languageEnglish
Pages (from-to)2027-2037
Number of pages11
JournalChemistry of Materials
Volume35
Issue number5
Early online date28 Feb 2023
DOIs
Publication statusPublished - 14 Mar 2023

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