Recent progress has shown promising advancements in enhancing the Reverse intersystem crossing (RISC) process between high‐energy triplet states (Tn, n ≥ 1) and radiative singlet states (Sm) through the utilization of the classic D‐A‐D' strategy. In this study, 12 molecules employing phenyl carbazole and a peripheral phenanthroimidazole as the donors and fused cores as acceptors are theoretically designed. Additionally, electron‐withdrawing groups such as fluorine and cyano, as well as electron‐donating group like methoxy, are incorporated into anthracene, napthaoxadiazole, and napthothiadiazole derivatives, acting as fused core components. Theoretical analyses reveal that among the molecules examined, eight adhere to the three golden principle rules, demonstrating a large energy gap between S1‐T1, the minimal ΔES1‐T2, and large T2‐T1. Additionally, these molecules exhibit significant Spin‐orbit coupling (SOC) and maintain a strong Hybridized local and charge transfer (HLCT) character, facilitating the fast hRISC from T2 to S1. The auxiliary inclusion of heteroatoms, such as oxygen and sulfur, on the anthracene core, aligns with the prerequisite strategy, ultimately reinforcing the SOC. Furthermore, replacing the methoxy group on the Nz bridge significantly enhances the SOC, resulting in a substantial increase in the hRISC rate (10 +08 s−1). Overall, the findings substantially elevate the photophysical attributes of the designed molecules through the utilization of the hRISC channel.

中文翻译：

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通过稠环修饰增强热激子热激活延迟荧光发射器中的快速 RISC：理论见解


最近的进展表明，通过利用经典的 D-A-D' 策略，在增强高能三重态 (Tn, n ≥ 1) 和辐射单重态 (Sm) 之间的反向系间窜越 (RISC) 过程方面取得了有希望的进展。在这项研究中，理论上设计了12个采用苯基咔唑和外围菲并咪唑作为供体和融合核作为受体的分子。此外，氟、氰基等吸电子基团以及甲氧基等供电子基团被引入到蒽、萘并恶二唑和萘并噻二唑衍生物中，作为稠合的核心成分。理论分析表明，在所检查的分子中，有八个遵循三个黄金原理规则，证明 S1-T1、最小 ΔES1-T2 和大 T2-T1 之间存在较大的能隙。此外，这些分子表现出显着的自旋轨道耦合（SOC）并保持强大的混合局部和电荷转移（HLCT）特征，促进hRISC从T2快速到S1。蒽核心上辅助包含氧和硫等杂原子，与先决条件策略相一致，最终增强了 SOC。此外，取代 Nz 桥上的甲氧基可显着增强 SOC，从而大幅提高 hRISC 速率 (10 +08 s−1)。总体而言，这些发现通过利用 hRISC 通道大大提高了设计分子的光物理属性。