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Single-electron charging and ultrafast dynamics of bimetallic Au144−xAgx(PET)60 nanoclusters

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Abstract

Alloying is an important strategy in tailoring the functionality of materials. In metal nanoclusters (NCs), the introduction of a heterometal leads to alloy nanoclusters that often outperform the homometal ones in terms of the physical and chemical properties. In this work, a series of four M144(PET)60 alloy NCs (where, M = Au/Ag, PET = −SCH2CH2Ph) are synthesized and characterized. The silver doping into the homogold template (Au144) leads to more prominent optical absorption features in the steady-state spectrum in the visible range. Femtosecond transient absorption spectroscopy reveals the effect of Ag doping on the electronic relaxation dynamics compared to Au144 and the pump fluence independent dynamics. Electrochemical results reflect a narrowing of HOMO—LUMO gap (Eg) induced by Ag doping. A temperature dependence of the single-electron charging is also observed for the series of alloy NCs, in which the Eg values of the alloy NCs enlarge as the temperature decreases, which is characteristic of semiconducting behavior.

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Acknowledgements

R. J. thanks the financial support from the National Science Foundation (No. DMR-1808675). G. W. acknowledges the funding support from National Science Foundation PAPID CHE(No. 2034498). H. W. thanks the financial support from, the Air Force Office of Scientific Research (AFOSR) Nos. (FA9550-17-1-0099 and sFA9550-21-1-0192).

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Author notes

  1. Xiangsha Du, Hedi Ma, and Xinwen Zhang contributed equally to this work.

Authors and Affiliations

  1. Department of Chemistry, Carnegie Mellon University, Pittsburgh, Pennsylvania, 15213, USA

    Xiangsha Du, Zhongyu Liu & Rongchao Jin

  2. Department of Chemistry, Georgia State University, Atlanta, Georgia, 30302, USA

    Hedi Ma & Gangli Wang

  3. Department of Physics, University of Miami, Coral Gables, Florida, 33146, USA

    Xinwen Zhang & He Wang

  4. Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China

    Meng Zhou

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  1. Xiangsha Du
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  4. Meng Zhou
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  5. Zhongyu Liu
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  6. He Wang
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Correspondence to He Wang, Gangli Wang or Rongchao Jin.

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Du, X., Ma, H., Zhang, X. et al. Single-electron charging and ultrafast dynamics of bimetallic Au144−xAgx(PET)60 nanoclusters. Nano Res. 15, 8573–8578 (2022). https://doi.org/10.1007/s12274-022-4445-9

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