Li Yang, Rowell Nelson, Luan Chaoran, Zhang Meng, Chen Xiaoqin, Yu Kui
Engineering Research Center in Biomaterials, Sichuan University, Chengdu, Sichuan, 610065, P. R. China.
Metrology Research Centre, National Research Council Canada, Ottawa, Ontario, K1A 0R6, Canada.
Adv Mater. 2022 Nov;34(46):e2107940. doi: 10.1002/adma.202107940. Epub 2022 Feb 4.
A fundamental understanding of formation pathways is critical to the controlled synthesis of colloidal semiconductor nanocrystals. As ultrasmall-size quantum dots (QDs) sometimes emerge in reactions along with magic-size clusters (MSCs), distinguishing their individual pathway of evolution is important, but has proven difficult. To decouple the evolution of QDs and MSCs, an unconventional, selective approach has been developed, along with a two-pathway model that provides a fundamental understanding of production selectivity. For on-demand production of either ultrasmall QDs or MSCs, the key enabler is in how to allow a reaction to proceed in the time prior to nucleation and growth of QDs. In this prenucleation stage, an intermediate compound forms, which is the precursor compound (PC) to the MSC. Here, the two-pathway model and the manipulation of such PCs to synthesize either ultrasmall QDs or binary and ternary MSCs are highlighted. The two-pathway model will assist the development of nucleation theory as well as provide a basis for a mechanism-enabled design and predictive synthesis of functional nanomaterials.
对形成途径的基本理解对于胶体半导体纳米晶体的可控合成至关重要。由于超小尺寸量子点(QD)有时会在反应中与魔法尺寸团簇(MSC)一同出现,区分它们各自的演化途径很重要,但事实证明这很困难。为了解耦量子点和魔法尺寸团簇的演化,已经开发出一种非常规的选择性方法,以及一个双途径模型,该模型提供了对生产选择性的基本理解。对于按需生产超小量子点或魔法尺寸团簇,关键因素在于如何使反应在量子点成核和生长之前的时间段内进行。在这个成核前阶段,会形成一种中间化合物,它是魔法尺寸团簇的前体化合物(PC)。在此,重点介绍双途径模型以及对这种前体化合物的操控,以合成超小量子点或二元和三元魔法尺寸团簇。双途径模型将有助于成核理论的发展,并为基于机制的功能性纳米材料设计和预测性合成提供基础。