Niu Jixiu, Gao Feifei, Wang Ye, Lu Wu, Zhang Jing, He Jiexu, Lou Xinjin, Ma Yuanxin, Duan Chunbo, Han Chunmiao, Xu Hui
Key Laboratory of Functional Inorganic Material Chemistry, School of Chemistry and Material Science, Heilongjiang University, 74 Xuefu Road, Harbin, 150080, China.
Angew Chem Int Ed Engl. 2025 Jul 7;64(28):e202508667. doi: 10.1002/anie.202508667. Epub 2025 May 24.
Luminescent materials have important applications in biology, medicine, catalysis, energy, information technology, and so on. However, to suppress quenching and improve efficiencies, how to balance singlet and triplet radiations for efficient dual emission composed of equalized thermally activated delayed fluorescence (TADF) and phosphorescence remains a formidable challenge. Here, we report that based on a rigid skeleton of triphosphine CuI complex, modification with carbazole donors results in high-lying ligand-centered charge transfer states, which provide additional channels for accurately optimizing the singlet-triplet ratios. We achieve equalized dual emissions containing 53% TADF and 47% phosphorescence, ∼100% photo- and electro-luminescence quantum efficiencies and record-high external quantum efficiencies of ∼30% for pure-yellow organic light-emitting diodes. Photophysical and exciton kinetics analyses indicate the incorporation of high-lying ligand-centered triplet states into dual-emissive electroluminescence is based on energy-level matching with the first triplet states of host matrixes.
发光材料在生物学、医学、催化、能源、信息技术等领域有着重要应用。然而，为了抑制猝灭并提高效率，如何平衡单重态和三重态辐射以实现由均衡的热活化延迟荧光（TADF）和磷光组成的高效双发射仍是一个巨大挑战。在此，我们报道基于三膦碘化亚铜配合物的刚性骨架，用咔唑供体进行修饰会导致以配体为中心的电荷转移态处于较高能级，这为精确优化单重态 - 三重态比例提供了额外通道。我们实现了包含53% TADF和47%磷光的均衡双发射、约100%的光致发光和电致发光量子效率，以及纯黄色有机发光二极管创纪录的约30%的外量子效率。光物理和激子动力学分析表明，将以配体为中心的高能级三重态纳入双发射电致发光是基于与主体基质的第一三重态的能级匹配。
