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Upconverting and downshifting circularly polarized luminescence in a superstructural helix
Science China Chemistry ( IF 10.4 ) Pub Date : 2024-06-20 , DOI: 10.1007/s11426-024-2100-x
Honghan Ji , Bin Wu , Enquan Tian , Chao Ren , Xue Jin , Liangliang Zhu , Pengfei Duan

The modulation of circularly polarized luminescence (CPL) has become an increasingly prominent area of research. In this study, we propose a unique “one-excitation-to-three-emissions” CPL system through the co-assembly of an upconversion system, incorporating one sensitizer (Pt(II) mesotetraphenyl tetrabenzoporphyrine, PtTPBP) and two annihilators (R/S-DPA and R/S-BDP) within liquid crystals. The chiral nature of the annihilators induces a transformation of the nematic liquid crystal into chiral nematic liquid crystals (N*LC), establishing an excellent chiral matrix. Upon the incorporation of the sensitizer PtTPBP and subsequent excitation at 635 nm, the system demonstrates two independent triplet-triplet annihilation photon upconversion (TTA-UC) with the emission in blue and yellow, aided by thermally activated triplet-triplet energy transfer (TTET). This is accompanied by the simultaneous generation of upconverting circularly polarized luminescence (UC-CPL) and downshifting near-infrared circularly polarized luminescence (DS-CPL) originating from the residual luminescence of PtTPBP. Remarkably, fine-tuning the ratio between the two annihilators allows the TTA-UC system to exhibit multicolor CPL emission with an amplified luminescence dissymmetry factor (glum, reaching up to 0.6). Our study unveils a previously unreported “one-excitation-to-three-emissions” system and provides a versatile strategy for modulating CPL emissions, surpassing conventional methodologies.



中文翻译:


上层结构螺旋中的上转换和下转换圆偏振发光



圆偏振发光(CPL)的调制已成为一个日益重要的研究领域。在这项研究中,我们通过上转换系统的共同组装提出了一种独特的“一次激发三发射”CPL系统,该系统包含一种敏化剂(Pt(II)间四苯基四苯并卟啉,PtTPBP)和两种消灭剂(R/ S-DPA 和 R/S-BDP)在液晶内。湮没子的手性性质导致向列液晶转变为手性向列液晶(N*LC),建立了良好的手性矩阵。在加入敏化剂 PtTPBP 并随后在 635 nm 处激发后,系统展示了两个独立的三重态-三重态湮灭光子上转换 (TTA-UC),并在热激活三重态-三重态能量转移 (TTET) 的辅助下发出蓝色和黄色光。这伴随着源自 PtTPBP 残余发光的上转换圆偏振发光 (UC-CPL) 和下移近红外圆偏振发光 (DS-CPL) 的同时产生。值得注意的是,微调两个歼灭子之间的比率使得TTA-UC系统能够表现出具有放大的发光不对称因子(g lum ,达到0.6)的多色CPL发射。我们的研究揭示了一种先前未报道的“一次激发到三次发射”系统,并提供了一种超越传统方法的调节 CPL 发射的通用策略。

更新日期:2024-06-24
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