宏手性液晶量子点增强自组织螺旋超结构中的不对称圆极化发光。

IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Nano Pub Date : 2024-11-04 DOI:10.1021/acsnano.4c10423
Huanan Yu, Kaige Zhang, Qiqi Yu, Jingji Zhang, Yongchun Ye, Carl Redshaw, Zhonghui Chen, Dongdong Xu, Georg H Mehl
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引用次数: 0

摘要

圆偏振发光(CPL)材料在三维成像、数据加密和不对称催化等各种先进光学应用领域引起了人们的极大兴趣。然而,高性能 CPL 的开发一直受阻于缺乏既能表现出高量子产率又能表现出不对称因子的手性发光体的简单合成方法。在本研究中,我们提出了一种创新的方法来合成大手性液晶量子点(Ch-QDs/LC),并通过掺杂 4-氰基-4'-戊基联苯(5CB)来提高其 CPL 性能,从而获得 CPL 发射发生器(CEG)。我们合成了 Ch-QDs/LC,并通过硫辛酸连接体锚定了手性介源配体(特别是胆固醇苯甲酸酯),使其表面功能化。在手性 2S-Zn2+ 配位复合物的调节下,手性 LC 封装过程促进了配位配体的置换,从而产生了 56.3% 的优异量子产率。与此同时,吸收不对称因子(gabs)和发光不对称因子(glum)的值也很高,从 10-3 到 10-2,比大多数报告的不对称因子至少高出一个数量级。模块化 Ch-QDs/LCs 展示了将手性有效转移到周围介质的能力,并在向列型 LC 矩阵中表现出宏手性特征。利用 Ch-QDs/LC 作为非手性 5CB 矩阵中有效的 CPL 发射器,使该系统达到了 0.35 的最大 Glum 值。由此产生的 CEG 设备可作为直接 CPL 源,启动对映体选择性光聚合。
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Enhanced Asymmetric Circularly Polarized Luminescence in Self-Organized Helical Superstructures Enabled by Macro-Chiral Liquid Crystal Quantum Dots.

Circularly polarized luminescent (CPL) materials have garnered considerable interest for a variety of advanced optical applications including 3D imaging, data encryption, and asymmetric catalysis. However, the development of high-performance CPL has been hindered by the absence of simple synthetic methods for chiral luminescent emitters that exhibit both high quantum yields and dissymmetry factors. In this study, we present an innovative approach for the synthesis of macro-chiral liquid crystal quantum dots (Ch-QDs/LC) and their CPL performance enhancement through doping with 4-cyano-4'-pentylbiphenyl (5CB), thus yielding a CPL-emitting generator (CEG). The Ch-QDs/LCs were synthesized, and their surfaces functionalized with a chiral mesogenic ligand, specifically cholesteryl benzoate, anchored via a lipoic acid linker. Under the regulation of chiral 2S-Zn2+ coordination complexes, the chiral LC encapsulation process promotes coordinated ligand substitution, resulting in an exceptional quantum yield of 56.3%. This is accompanied by high absorption dissymmetry factor (gabs) and luminescence dissymmetry factor (glum) values ranging from 10-3 to 10-2, surpassing most reported dissymmetry factors by at least an order of magnitude. The modular Ch-QDs/LCs demonstrate the ability to transfer chirality to the surrounding medium efficiently and manifest macro-chiral characteristics within a nematic LC matrix. Utilizing Ch-QDs/LC as an effective CPL emitter within achiral 5CB matrices enabled the system to achieve a maximum glum value of 0.35. The resultant CEG device acted as a direct CPL source, initiating enantioselective photopolymerization.

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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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