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Research Article

Atomically precise metal-chalcogenide semiconductor molecular nanoclusters with high dispersibility: Designed synthesis and intracluster photocarrier dynamics

Jiaxu Zhang1,§, Chaochao Qin2,§, Yeshuang Zhong3,§, Xiang Wang1, Wei Wang1,3, Dandan Hu1, Xiaoshuang Liu1, Chaozhuang Xue1, Rui Zhou1, Lei Shen4, Yinglin Song4, Dingguo Xu3, Zhien Lin3, Jun Guo5, Haifeng Su6, Dong-Sheng Li7, Tao Wu1()
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China
Henan Key Laboratory of Infrared Materials & Spectrum Measures and Applications, School of Physics, Henan Normal University, Xinxiang 453007, China
College of Chemistry, Sichuan University, Chengdu 610064, China
School of Physical Science and Technology, Soochow University, Suzhou 215123, China
Testing & Analysis Centre, Soochow University, Suzhou 215123, China
College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
College of Materials and Chemical Engineering, Hubei Provincial Collaborative Innovation Centre for New Energy Microgrid, Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials, China Three Gorges University, Yichang 443002, China

§ Jiaxu Zhang, Chaochao Qin, and Yeshuang Zhong contributed equally to this work.

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Abstract

A comprehensive understanding of excited-state dynamics of semiconductor quantum dots or nanomaterials at the atomic or molecular level is of scientific importance. Pure inorganic (or non-covalently protected) seimiconductor molecular nanoclusters with atomically precise structure are contributive to establish accurate correlation of excited-state dynamics with their composition/ structure, however, the related studies are almost blank because of unresolved solvent dispersion issue. Herein, we designedly created the largest discrete chalcogenide seimiconductor molecular nanoclusters (denoted P2-CuMSnS, M = In or/and Ga) with great dispersibility, and revealed an interesting intracluster "core-shell" charge transfer relaxation dynamics. A systematic red shift in absorption spectra with the gradual substitution of In by Ga was experimentally and computationally investigated, and femtosecond transient absorption measurements further manifested there were three ultrafast processes in excited-state dynamics of P2 nanoclusters with the corresponding amplitudes directed by composition variation. Current results hold the great promise of the solution-processible applications of semiconductor-NC-based quantum dots and facilitate the development of atomically precise nano-chemistry.

Keywords

semiconductornanoclustersphotocarrier dynamicscharge transferatomically precise

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Nano Research
Volume 13 Issue 10,
October 2020
Pages 2828-2836
DOI: 10.1007/s12274-020-2936-0
Cite this article:
Zhang J, Qin C, Zhong Y, et al. Atomically precise metal-chalcogenide semiconductor molecular nanoclusters with high dispersibility: Designed synthesis and intracluster photocarrier dynamics. Nano Research, 2020, 13(10): 2828-2836. https://doi.org/10.1007/s12274-020-2936-0
Topics:
ChalcogenidesCharge transferNanoclustersNanocrystalsSemiconductor quantum dots
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