Guo Chen-Hao, Feng Liheng, Chen Chuan-Feng, Li Meng
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Molecular Recognition and Function, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan, 030006, China.
Angew Chem Int Ed Engl. 2025 Aug 17:e202516018. doi: 10.1002/anie.202516018.
The development of white circularly polarized organic light-emitting diodes (CP-OLEDs) faces a critical challenge in simultaneously achieving high external quantum efficiency (EQE) and large dissymmetry factors (g), due to the inherent trade-off between exciton utilization and chirality amplification. Herein, we propose an orthogonal architecture synergizing an achiral blue thermally activated delayed fluorescence (TADF) emitter with chiral orange assemblies to overcome this limitation. The chiral assemblies, featuring exceptional chiroptical activity (|g| = 0.95 and |g| = 0.85), are engineered as both photon-selective filters and emitters. When integrated with a blue TADF layer, this dual-layer design enables 100% internal quantum efficiency through TADF-enabled triplet harvesting and chiral amplification via selective absorption of blue photons with a specific polarization direction, generating amplified white circularly polarized electroluminescence (CPEL). The resulting white CP-OLED (CIE: 0.31, 0.34) achieves a record |g| of 0.34 alongside an EQE of 6.3%, demonstrating the unprecedented white CP-OLEDs when considering both EQE and g values. By optimizing the TADF doping ratio, a cool-white CP-OLED is realized with an EQE of 14.7% and |g| of 0.32. This work establishes a material orthogonal engineering to decouple exciton-chirality interdependencies, opening avenues for fabricating high-performance CPEL devices.
白色圆偏振有机发光二极管(CP - OLED)的发展面临着一个关键挑战,即由于激子利用和手性放大之间存在固有的权衡,要同时实现高外量子效率(EQE)和大不对称因子(g)。在此,我们提出一种正交结构,将非手性蓝色热激活延迟荧光(TADF)发射体与手性橙色组装体协同作用,以克服这一限制。这些手性组装体具有出色的旋光活性(|g| = 0.95和|g| = 0.85),被设计成既是光子选择性滤波器又是发射体。当与蓝色TADF层集成时,这种双层设计通过基于TADF的三重态捕获实现100%的内量子效率,并通过选择性吸收特定偏振方向的蓝色光子实现手性放大,从而产生放大的白色圆偏振电致发光(CPEL)。由此得到的白色CP - OLED(CIE:0.31,0.34)实现了创纪录的|g|值0.34以及6.3%的EQE,在同时考虑EQE和g值时展示了前所未有的白色CP - OLED。通过优化TADF掺杂比例,实现了一个冷白色CP - OLED,其EQE为14.7%,|g|为0.32。这项工作建立了一种材料正交工程,以解耦激子 - 手性的相互依赖性,为制造高性能CPEL器件开辟了道路。