Liu Yuchao, Hua Lei, Zhao Zhennan, Ying Shian, Ren Zhongjie, Yan Shouke
State Key Laboratory of Chemical Resource Engineering, College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.
Key Laboratory of Rubber-Plastics, Ministry of Education, Qingdao University of Science & Technology, Qingdao, 266042, P.R. China.
Adv Sci (Weinh). 2021 Sep;8(18):e2101326. doi: 10.1002/advs.202101326. Epub 2021 Jul 26.
The state-of-the-art luminescent materials are gained widely by utilizing thermally activated delayed fluorescence (TADF) mechanism. However, the feasible molecular designing strategy of fully exploiting triplet excitons to enhance TADF properties is still in demand. Herein, TADF emitters with multiple conversion channels of triplet excitons are designed by concisely halogenating the electron acceptors containing carbonyl moiety. Compared with the chlorinated and brominated analogues, the fluorinated emitter exhibits distinguishing molecular stacking structures, participating in the formation of trimers through integrating CH···F and C═O···H hydrogen bonds together. It is also demonstrated that the multiple channels can be involved synergistically to accelerate the spin-flip of triplet excitons, and to take charge of the relatively superior reverse intersystem crossing constant rate of 6.20 × 10 s , and thus excellent photoluminescence quantum yields over 90% can easily be achieved. Then the solution-processable organic light emitting diode based on fluorinated emitter can achieve a record-high external quantum efficiency value of 27.13% and relatively low efficiency roll-off with remaining 24.74% at 1000 cd m . This result manifests the significance of enhancing photophysical properties through constructing multiple conversion channels of triplets excitons for high-efficiency TADF emitters and provides a guideline for the future study.
通过利用热激活延迟荧光(TADF)机制,先进的发光材料得到了广泛应用。然而,充分利用三线态激子来增强TADF性能的可行分子设计策略仍有待探索。在此,通过对含羰基部分的电子受体进行简洁的卤化,设计了具有三线态激子多重转换通道的TADF发光体。与氯化和溴化类似物相比,氟化发光体呈现出独特的分子堆积结构,通过整合CH···F和C═O···H氢键参与三聚体的形成。研究还表明,多重通道可协同作用,加速三线态激子的自旋翻转,并负责相对较高的反向系间窜越常数率6.20×10 s,从而轻松实现超过90%的优异光致发光量子产率。基于氟化发光体的溶液可加工有机发光二极管可实现创纪录的27.13%的高外量子效率值,且在1000 cd m时效率滚降相对较低,仍为24.74%。这一结果表明了通过构建三线态激子的多重转换通道来增强光物理性能对于高效TADF发光体的重要性,并为未来的研究提供了指导。