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Generation and Transfer of Triplet Electron Spin Polarization at the Solid–Liquid Interface

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2023, 14, 20, 4754-4759
    Physical Insights into Quantum Phenomena and Function

    Generation and Transfer of Triplet Electron Spin Polarization at the Solid–Liquid Interface
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    • Reiya Yabuki
      Reiya Yabuki
      Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan
      More by Reiya Yabuki
    • Koki Nishimura
      Koki Nishimura
      Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan
      More by Koki Nishimura
    • Tomoyuki Hamachi
      Tomoyuki Hamachi
      Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan
      More by Tomoyuki Hamachi
    • Naoto Matsumoto
      Naoto Matsumoto
      Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan
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    • Nobuhiro Yanai*
      Nobuhiro Yanai
      Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan
      FOREST, JST, Honcho 4-1-8, Kawaguchi, Saitama 332-0012, Japan
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0003-0297-6544
    Other Access OptionsSupporting Information (2)

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2023, 14, 20, 4754–4759
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    https://doi.org/10.1021/acs.jpclett.3c00627
    Published May 15, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    The photoexcited triplet state of dyes can generate highly polarized electron spins for sensing and dynamic nuclear polarization. However, while triplets exhibit long spin–lattice relaxation times (T1) on the microsecond scale in solids, the polarization quickly relaxes on the nanosecond scale in solution due to the rotational motion of chromophores. Here, we report that the immobilization of dye molecules on a solid surface allows molecular contact with a liquid while maintaining high polarization and long T1 as in a solid. By adsorbing anionic porphyrins on cationic mesoporous silica gel, porphyrin triplets exhibit high polarization and long T1 at the solid–liquid interface of silica and toluene. Furthermore, porphyrin triplets on the solid surface can exchange spin polarization with TEMPO radicals in solution. This simple and versatile method using the solid–liquid interface will open the door for utilizing the photoinduced triplet spin polarization in solution, which has been mainly limited to the solid-state.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.3c00627.

    • Experimental details, absorption and fluorescence spectra, confocal microscopy images, SEM images, BET plots, cw-ESR spectra, and transient absorption spectra and decays (PDF)

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    Cited By

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    This article is cited by 2 publications.

    1. Gang Fan, Nathan Corbin, Minju Chung, Thomas M. Gill, Evan B. Moore, Amruta A. Karbelkar, Ariel L. Furst. Highly Efficient Carbon Dioxide Electroreduction via DNA-Directed Catalyst Immobilization. JACS Au 2024, 4 (4) , 1413-1421. https://doi.org/10.1021/jacsau.3c00823
    2. K. Miyanishi, T. Sugiki, T. Matsui, R. Ozawa, Y. Hatanaka, H. Enozawa, Y. Nakamura, T. Murata, A. Kagawa, Y. Morita, T. Fujiwara, M. Kitagawa, M. Negoro. Protein–Ligand Interaction Analyses with Nuclear Magnetic Resonance Spectroscopy Enhanced by Dissolution Triplet Dynamic Nuclear Polarization. The Journal of Physical Chemistry Letters 2023, 14 (27) , 6241-6247. https://doi.org/10.1021/acs.jpclett.3c01002
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2023, 14, 20, 4754–4759
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.3c00627
    Published May 15, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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