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

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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.

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Acknowledgements

The authors acknowledge financial support from the National Natural Science Foundation of China (Nos. 21671142, 11804084 and 21875150), the Jiangsu Province Natural Science Fund for Distinguished Young Scholars (No. BK20160006), the 111 Project (No. D20015), the Project of Scientific and Technologic Infrastructure of Suzhou (No. SZS201905) and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). The authors also thank Dr. D. C. Ma at Analytical and Testing Center, Sichuan University for technical help with the Material Studio calculations.

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

Authors and Affiliations

  1. College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, 215123, China

    Jiaxu Zhang, Xiang Wang, Wei Wang, Dandan Hu, Xiaoshuang Liu, Chaozhuang Xue, Rui Zhou & Tao Wu

  2. Henan Key Laboratory of Infrared Materials & Spectrum Measures and Applications, School of Physics, Henan Normal University, Xinxiang, 453007, China

    Chaochao Qin

  3. College of Chemistry, Sichuan University, Chengdu, 610064, China

    Yeshuang Zhong, Wei Wang, Dingguo Xu & Zhien Lin

  4. School of Physical Science and Technology, Soochow University, Suzhou, 215123, China

    Lei Shen & Yinglin Song

  5. Testing & Analysis Centre, Soochow University, Suzhou, 215123, China

    Jun Guo

  6. College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Haifeng Su

  7. 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

    Dong-Sheng Li

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  1. Jiaxu Zhang
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  2. Chaochao Qin
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Correspondence to Tao Wu.

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

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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 Res. 13, 2828–2836 (2020). https://doi.org/10.1007/s12274-020-2936-0

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