Kwon Yongju, Oh Juwon, Lee Eunjae, Lee Sang Hyeon, Agnes Anastasia, Bang Gyuhyun, Kim Jeongmin, Kim Dongho, Kim Sungjee
Department of Chemistry, Pohang University of Science and Technology, Pohang, 37673, South Korea.
Department of Chemistry and Spectroscopy Laboratory for Functional π-Electronic Systems, Yonsei University, Seoul, 03722, South Korea.
Nat Commun. 2020 Jun 19;11(1):3127. doi: 10.1038/s41467-020-16855-9.
Magic-sized clusters (MSCs) can be isolated as intermediates in quantum dot (QD) synthesis, and they provide pivotal clues in understanding QD growth mechanisms. We report syntheses for two families of heterogeneous-atom-incorporated InP MSCs that have chlorine or zinc atoms. All the MSCs could be directly synthesized from conventional molecular precursors. Alternatively, each series of MSCs could be prepared by sequential conversions. 386-InP MSCs could be converted to F360-InP:Cl MSCs, then to F399-InP:Cl MSCs. Similarly, F360-InP:Zn MSCs could be converted to F408-InP:Zn MSCs, then to F393-InP:Zn MSCs. As the conversion proceeded, evolution from uni-molecule-like to QD-like characters was observed. Early stage MSCs showed active inter-state conversions in the excited states, which is characteristics of small molecules. Later stage MSCs exhibited narrow photoinduced absorptions at lower-energy region like QDs. The crystal structure also gradually evolved from polytwistane to more zinc-blende.
魔尺寸团簇（MSCs）可作为量子点（QD）合成过程中的中间体被分离出来，并且它们为理解量子点生长机制提供了关键线索。我们报告了两类含有氯或锌原子的异质原子掺杂InP MSCs的合成方法。所有的MSCs都可以直接由传统分子前驱体合成。或者，每一系列的MSCs都可以通过顺序转化来制备。386-InP MSCs可以转化为F360-InP:Cl MSCs，然后再转化为F399-InP:Cl MSCs。类似地，F360-InP:Zn MSCs可以转化为F408-InP:Zn MSCs，然后再转化为F393-InP:Zn MSCs。随着转化过程的进行，观察到了从类单分子到类量子点特征的演变。早期的MSCs在激发态表现出活跃的态间转换，这是小分子的特征。后期的MSCs在较低能量区域表现出类似量子点的窄光致吸收。晶体结构也逐渐从聚扭烷演变为更多的闪锌矿结构。
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