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An Oligomer Approach for Blue Thermally Activated Delayed Fluorescent Emitters Based on Twisted Donor-Acceptor Units.


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 report an approach to enhance the efficiency of TADF-related processes without changing the blue photoluminescence color.

SUBMITTER: Duda E 

PROVIDER: S-EPMC10018739 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature

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An Oligomer Approach for Blue Thermally Activated Delayed Fluorescent Emitters Based on Twisted Donor-Acceptor Units.

Duda Eimantas E   Madayanad Suresh Subeesh S   Hall David D   Bagnich Sergey S   Saxena Rishabh R   Cordes David B DB   Slawin Alexandra M Z AMZ   Beljonne David D   Olivier Yoann Y   Köhler Anna A   Zysman-Colman Eli E  

Chemistry of materials : a publication of the American Chemical Society 20230228 5


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 (T<sub>1</sub>) and singlet (S<sub>1</sub>) excited states. Here, we introduce an oligomer approach using repetitive donor-acceptor units to gradually increase the n  ...[more]

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