期刊
ACS CENTRAL SCIENCE
卷 9, 期 3, 页码 519-530出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.2c01394
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This study explores the isomerization reactions of colloidal semiconductor magic-size clusters (MSCs), specifically CdTeSe, and reveals two pathways regulated by acidity and ligand amount. Pathway 1 involves direct changes in intracluster configuration and a large energy barrier, while pathway 2 is indirect and involves MSC precursor compounds (PCs). Pathway 1 is activated when the conversion from PC-422 to MSC-422 is suppressed. The findings provide insights into the transformative behavior of MSCs through ligand-induced isomerization upon external chemical stimuli.
The field of isomerization reactions for colloidal semiconductor magic-size clusters (MSCs) remains largely unexplored. Here, we show that MSCs isomerize via two fundamental pathways that are regulated by the acidity and amount of an incoming ligand, with CdTeSe as the model system. When MSC-399 isomerizes to MSC-422 at room temperature, the peak red-shift from 399 to 422 nm is continuous (pathway 1) and/or stepwise (pathway 2) as monitored in situ and in real time by optical absorption spectroscopy. We propose that pathway 1 is direct, with intracluster configuration changes and a relatively large energy barrier. Pathway 2 is indirect, assisted by the MSC precursor compounds (PCs), from MSC-399 to PC-399 to PC-422 to MSC-422. Pathway 1 is activated when PC-422 to MSC-422 is suppressed. Our findings unambiguously suggest that when a change occurs directly on a nanospecies, its absorption peak continuously shifts. The present study provides an in-depth understanding of the transformative behavior of MSCs via ligand-induced isomerization upon external chemical stimuli.
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