Breaking through the Size Control Dilemma of Silver Chalcogenide Quantum Dots via Trialkylphosphine-Induced Ripening: Leading to Ag 2 Te Emitting from 950 to 2100 nm

Ag Te is one of the most promising semiconductors with a narrow band gap and low toxicity; however, it remains a challenge to tune the emission of Ag Te quantum dots (QDs) precisely and continuously in a wide range. Herein, Ag Te QDs emitting from 950 to 2100 nm have been synthesized via trialkylpho...

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Published in:Journal of the American Chemical Society 2021-08, Vol.143 (32), p.12867-12877
Main Authors: Liu, Zhen-Ya, Liu, An-An, Fu, Haohao, Cheng, Qing-Yuan, Zhang, Ming-Yu, Pan, Man-Man, Liu, Li-Ping, Luo, Meng-Yao, Tang, Bo, Zhao, Wei, Kong, Juan, Shao, Xueguang, Pang, Dai-Wen
Format: Article
Language:English
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Summary:Ag Te is one of the most promising semiconductors with a narrow band gap and low toxicity; however, it remains a challenge to tune the emission of Ag Te quantum dots (QDs) precisely and continuously in a wide range. Herein, Ag Te QDs emitting from 950 to 2100 nm have been synthesized via trialkylphosphine-controlled growth. Trialkylphosphine has been found to induce the dissolution of small-sized Ag Te QDs due to its stronger ability to coordinate to the Ag ion than that of 1-octanethiol, predicated by the density functional theory. By controlling this dissolution effect, the monomer supply kinetics can be regulated, achieving precise size control of Ag Te QDs. This synthetic strategy results in state-of-the-art silver-based QDs with emission tunability. Only by taking advantage of such an ultrawide emission has the sizing curve of Ag Te been obtained. Moreover, the absolute photoluminescence quantum yield of Ag Te QDs can reach 12.0% due to their well-passivated Ag-enriched surface with a density of 5.0 ligands/nm , facilitating noninvasive fluorescence imaging. The high brightness in the long-wavelength near-infrared (NIR) region makes the cerebral vasculature and the tiny vessel with a width of only 60 μm clearly discriminable. This work reveals a nonclassical growth mechanism of Ag Te QDs, providing new insight into precisely controlling the size and corresponding photoluminescence properties of semiconductor nanocrystals. The ultrasmall, low-toxicity, emission-tunable, and bright NIR-II Ag Te QDs synthesized in this work offer a tremendous promise for multicolor and deep-tissue fluorescence imaging.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.1c06661