黄忠衍老师、谢鸿辉、曹啸松老师的研究成果发表在JACS上!
Multiple resonance thermally activated delayed fluorescence (MR-TADF) emitters are promising candidates for narrowband organic light-emitting diodes, but their electroluminescent performance is typically hindered by the slow reverse intersystem crossing rate (k(RISC)). Herein, we present an effective strategy to introduce a multichannel reverse intersystem crossing (RISC) pathway with large spin-orbit coupling by orthogonally linking an electron-donating unit to the MR framework. Through delicate manipulation of the excited-state energy levels, an additional intersegmental charge transfer triplet state could be "silently" induced without perturbing the MR character of the lowest excited singlet state. The proof-of-concept emitter CzBN3 not only affords 23-fold increase of k(RISC) compared with its prototypical MR skeleton but also realizes close-to-unity photoluminescence quantum yield, large radiative rate constant, and very narrow emission spectrum. These merits enable high maximum external quantum efficiency (EQE(max)) of up to 37.1% and alleviated efficiency roll-off in the sensitizer-free device (EQE(1000) = 30.4%), and a further boost of efficiency (EQE(max/1000) = 42.3/34.1%) is realized in the hyperfluorescent device. The state-of-the-art electroluminescent performance validates the superiority of our molecular design strategy.
Journal of the American Chemical Society ( IF 16.383 )
Pub Date : 2023-06-05
DOI: 10.1021/jacs.3c01267