Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 39, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202209615
Keywords
Aqueous Phase; Magic-Size Clusters; Nucleation and Growth; Quantum Dots; Zinc Selenide
Categories
Funding
- National Natural Science Foundation of China (NSFC) [21773162]
- State Key Laboratory of Polymer Materials Engineering of Sichuan University [sklpme2020-2-09]
- Open Project of Key State Laboratory for Supramolecular Structures and Materials of Jilin University [SKLSSM 2022029]
- NSFC [22002099]
- China Postdoctoral Science Foundation [2020T130441]
- Science and Technology Facilities Council [ST/V000039/1]
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This study designs a room-temperature reaction to trap reaction intermediates in the prenucleation stage of ZnSe QDs and provides evidence that both nonclassical and classical pathways are necessary for explaining the nucleation and growth of aqueous-phase QDs.
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.
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