Enhancing Circularly Polarized Luminescence in Quantum Dots through Chiral Coordination-Mediated Growth at the Liquid/Liquid Interface

手性(物理) 发光 量子点 化学 量子产额 荧光 配位复合体 光致发光 配体(生物化学) 光化学 结晶学 纳米技术 光电子学 材料科学 有机化学 光学 物理 受体 夸克 量子力学 生物化学 手征对称破缺 Nambu–Jona Lasinio模型 金属
作者
Jiarong Cai,An‐An Liu,Xue‐Hui Shi,Haohao Fu,Wei Zhao,Liguang Xu,Hua Kuang,Chuanlai Xu,Dai‐Wen Pang
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (44): 24375-24385 被引量:26
标识
DOI:10.1021/jacs.3c09448
摘要

Here, we develop a novel methodology for synthesizing chiral CdSe@ZnS quantum dots (QDs) with enhanced circularly polarized luminescence (CPL) by incorporating l-/d-histidine (l-/d-His) ligands during ZnS shell growth at the water/oil interface. The resulting chiral QDs exhibit exceptional absolute photoluminescence quantum yield of up to 67.2%, surpassing the reported limits of 40.0% for chiral inorganic QDs, along with absorption dissymmetry factor (|gabs|) and luminescence dissymmetry factor (|glum|) values of 10-2, exceeding the range of 10-5-10-3 and 10-4-10-2, respectively. Detailed investigations of the synthetic pathway reveal that the interface, as a binary synthetic environment, facilitates the coordinated ligand exchange and shell growth mediated by chiral His-Zn2+ coordination complexes, leading to a maximum fluorescent brightness and chiroptical activities. The growth process, regulated by the His-Zn2+ coordination complex, not only reduces trap states on the CdSe surface, thereby enhancing the fluorescence intensity, but also significantly promotes the orbital hybridization between QDs and chiral ligands, effectively overcoming the shielding effect of the wide bandgap shell and imparting pronounced chirality. The proposed growth pathway elucidates the origin of chirality and provides insights into the regulation of the CPL intensity in chiral QDs. Furthermore, the application of CPL QDs in multilevel anticounterfeiting systems overcomes the limitations of replication in achiral fluorescence materials and enhances the system's resistance to counterfeiting, thus opening new opportunities for chiral QDs in optical anticounterfeiting and intelligent information encryption.
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