Multiple resonance induced thermally activated delayed fluorescence: Effect of chemical modification
Multiple resonance induced thermally activated delayed fluorescence: Effect of chemical modification
复制标题
多重共振诱导的热激活延迟荧光：化学修饰的影响
DOI：
10.1088/2516-1075/acc70e
复制
发表时间：
2023
影响因子：
2.6
通讯作者：
Marom, Noa
中科院分区：
文献类型：
--
作者：
Wang, Xiaopeng;Gao, Siyu;Wang, Aizhu;Wang, Bo;Marom, Noa
热激活延迟荧光（TADF）是通过反向系统间交叉（RISC）将三重态激子内部转换为单线态激子。它提高了有机发光二极管（OLED）的效率，使非辐射三重态激子的收获成为可能。多共振（MR）诱导的TADF发色团由于其刚性构象而具有高颜色纯度的额外优势。然而，由于严格的设计规则，已知的MR-TADF发色团数量有限。对于全彩高分辨率OLED显示器的应用，需要扩展可用发色团的种类及其颜色范围。我们通过计算探讨了化学修饰对MR-TADF发色团喹啉[3,2,1 -de]吖啶- 5,9 -二酮（QAD）性质的影响。QAD衍生物的评价基于以下几个指标：生成能与合成难易程度相关；前沿轨道的空间分布表明化合物是保持MR-TADF发色团还是转变为供体-受体TADF发色团；与母体化合物相比，单线态激发能的变化对应于颜色的变化；最低单重态和三重态之间的能量差对应于RISC的势垒；重组能与颜色纯度有关。基于这些指标，QAD-6CN被预测为具有青色调的有前途的MR-TADF发色团。这表明计算机模拟可以通过化学修饰帮助设计新的MR-TADF发色团。
Thermally activated delayed fluorescence (TADF) is the internal conversion of triplet excitons into singlet excitons via reverse intersystem crossing (RISC). It improves the efficiency of organic light-emitting diodes (OLED) by enabling the harvesting of nonradiative triplet excitons. Multiple resonance (MR) induced TADF chromophores exhibit an additional advantage of high color purity due to their rigid conformation. However, owing to the strict design rules there is a limited number of known MR-TADF chromophores. For applications in full-color high-resolution OLED displays, it is desirable to extend the variety of available chromophores and their color range. We computationally explore the effect of chemical modification on the properties of the MR-TADF chromophore quinolino [3, 2, 1-de] acridine-5, 9-dione (QAD). QAD derivatives are evaluated based on several metrics: The formation energy is associated with the ease of synthesis; The spatial distribution of the frontier orbitals indicates whether a compound remains an MR-TADF chromophore or turns into a donor–acceptor TADF chromophore; The change of the singlet excitation energy compared to the parent compound corresponds to the change in color; The energy difference between the lowest singlet and triplet states corresponds to the barrier to RISC; The reorganization energy is associated with the color purity. Based on these metrics, QAD-6CN is predicted to be a promising MR-TADF chromophore with a cyan hue. This demonstrates that computer simulations may aid the design of new MR-TADF chromophores by chemical modification.