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Excited State Engineering in Ag29 Nanocluster through Peripheral Modification with Silver(I) Complexes for Bright Near-Infrared Photoluminescence

  • Wataru Ishii
    Wataru Ishii
    Department of Chemistry, Graduate School of Science, Osaka Metropolitan University, Osaka 558-8585, Japan
    More by Wataru Ishii
  • Yoshinori Okayasu
    Yoshinori Okayasu
    Department of Applied Chemistry, College of Life Sciences, Ritsumeikan University, Kusatsu 525-8577, Japan
  • Yoichi Kobayashi
    Yoichi Kobayashi
    Department of Applied Chemistry, College of Life Sciences, Ritsumeikan University, Kusatsu 525-8577, Japan
  • Rika Tanaka
    Rika Tanaka
    X-ray Crystal Analysis Laboratory, Graduate School of Engineering, Osaka Metropolitan University, Osaka 558-8585, Japan
    More by Rika Tanaka
  • Shohei Katao
    Shohei Katao
    Division of Materials Science, Graduate School of Science and Technology, Nara Institute of Science and Technology, Nara 630-0192, Japan
    More by Shohei Katao
  • Yoshiko Nishikawa
    Yoshiko Nishikawa
    Division of Materials Science, Graduate School of Science and Technology, Nara Institute of Science and Technology, Nara 630-0192, Japan
  • Tsuyoshi Kawai
    Tsuyoshi Kawai
    Division of Materials Science, Graduate School of Science and Technology, Nara Institute of Science and Technology, Nara 630-0192, Japan
  • , and 
  • Takuya Nakashima*
    Takuya Nakashima
    Department of Chemistry, Graduate School of Science, Osaka Metropolitan University, Osaka 558-8585, Japan
    Division of Materials Science, Graduate School of Science and Technology, Nara Institute of Science and Technology, Nara 630-0192, Japan
    *Email: [email protected]
Cite this: J. Am. Chem. Soc. 2023, 145, 20, 11236–11244
Publication Date (Web):April 26, 2023
https://doi.org/10.1021/jacs.3c01259
Copyright © 2023 American Chemical Society

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    Abstract

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    The optical property of an ionic metal nanocluster (NC) is affected by the ionic interaction with counter ions. Here, we report that the modification of trianionic [Ag29(BDT)12(TPP)4]3– NC (BDT: 1.3-benzenedithiol; TPP: triphenylphosphine) with silver(I) complexes led to the intense photoluminescence (PL) in the near-infrared (NIR) region. The binding of silver(I) complexes to the peripheral region of Ag29 NC is confirmed by the single-crystal X-ray diffraction (SCXRD) measurement, which is further supported by electrospray ionization mass spectrometry (ESI-MS) and nuclear magnetic resonance (NMR) spectroscopy. The change of excited-state dynamics by the binding of silver(I) complexes is discussed based on the results of a transient absorption study as well as temperature-dependent PL spectra and PL lifetime measurements. The modification of Ag29 NCs with cationic silver(I) complexes is considered to give rise to a triplet excited state responsible for the intense NIR PL. These findings also afford important insights into the origin of the PL mechanism as well as the possible light-driven motion in Ag29-based NCs.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c01259.

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    CCDC 22368262236827 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Cited By

    This article is cited by 1 publications.

    1. Chengkai Zhang, Wei-Dan Si, Zhi Wang, Acharya Dinesh, Zhi-Yong Gao, Chen-Ho Tung, Di Sun. Solvent-Mediated Hetero/Homo-Phase Crystallization of Copper Nanoclusters and Superatomic Kernel-Related NIR Phosphorescence. Journal of the American Chemical Society 2024, 146 (15) , 10767-10775. https://doi.org/10.1021/jacs.4c00881

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