Three pyridine-carbonitrile-carbazole-based thermally activated delayed fluorescence (TADF) materials with highly sterically congested structures have been synthesized. The donor-acceptor-type TADF emitters (26-, 246-, and 35tCzPPC) consist of a 2,6-diphenylpyridine-3,5-dicarbonitrile core (PPC) as the acceptor and a di( t-butyl)carbazole-substituted phenyl group attached to C4 of the PC core as the donor. The molecules show a unique structure containing two consecutive large twisted angles along the donor and acceptor groups. The structure leads to a nearly complete space separation of the highest occupied molecular orbital and lowest unoccupied molecular orbital, a small Δ E value, and excellent TADF property. Moreover, the 26- and 246tCzPPC dopants favor a horizontal alignment enhancing the light outcoupling of the device. In contrast, 35tCzPPC favors a perpendicular alignment reducing the light outcoupling efficiency of the device. The 246tCzPPC-based devices show external quantum efficiency as high as 29.6% because of excellent TADF property, very high photoluminescence quantum yield, and high Θ value in the thin films. The device performance is the best among the pyridine-carbonitrile-based TADF emitters.
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