Manipulating Reaction Intermediates to Aqueous-Phase ZnSe Magic-Size Clusters and Quantum Dots at Room Temperature
Manipulating Reaction Intermediates to Aqueous-Phase ZnSe Magic-Size Clusters and Quantum Dots at Room Temperature
复制标题
室温下将反应中间体控制为水相 ZnSe 神奇尺寸团簇和量子点
DOI：
10.1002/ange.202209615
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发表时间：
2022
影响因子：
--
通讯作者：
Li Y
中科院分区：
文献类型：
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作者：
Li Y
目前还没有解决哪种模型更好地描述半导体量子点（QD）的水相成核和生长，经典的一步还是非经典的多步。在这里，我们设计了一个室温反应，以捕获ZnSe量子点的预成核阶段的反应中间体（作为模型系统）。我们发现，被捕获的中间体可以通过分子内重组转化为神奇大小的簇（MSC），并且可以片段化以使量子点生长。MSC在299 nm处表现出尖锐的光吸收峰，标记为MSC-299。 中间体，MSC-299的前体化合物（PC-299），在299 nm和更长的波长下是光学透明的。 该中间体在各种Zn和Se反应体系中形成。本研究提供了明确的证据，即非经典和经典途径都是解释水相量子点成核和生长所必需的，前者更受高反应浓度的青睐。
It is not resolved which model describes better the aqueous‐phase nucleation and growth of semiconductor quantum dots (QDs), the classical one‐step one or the nonclassical multi‐step one. Here, we design a room‐temperature reaction to trap reaction intermediates in the prenucleation stage of ZnSe QDs (as a model system). We show that the trapped intermediate can transform to magic‐size clusters (MSCs) via intra‐molecular reorganization and can fragment to enable the growth of QDs. The MSCs exhibit a sharp optical absorption peaking at 299 nm, labelled MSC‐299. The intermediate, the precursor compound (PC‐299) of MSC‐299, is optically transparent at 299 nm and to longer wavelengths. This intermediate forms in various Zn and Se reaction systems. The present study provides unambiguous evidence that the nonclassical and classical pathways are both necessary to explain the nucleation and growth of aqueous‐phase QDs, with the former pathway favored more by high reaction concentrations.