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Singlet fission as a polarized spin generator for dynamic nuclear polarization

Author

Listed:
  • Yusuke Kawashima

    (Graduate School of Engineering)

  • Tomoyuki Hamachi

    (Graduate School of Engineering)

  • Akio Yamauchi

    (Graduate School of Engineering)

  • Koki Nishimura

    (Graduate School of Engineering)

  • Yuma Nakashima

    (Graduate School of Engineering)

  • Saiya Fujiwara

    (Graduate School of Engineering)

  • Nobuo Kimizuka

    (Graduate School of Engineering
    Center for Molecular Systems (CMS))

  • Tomohiro Ryu

    (Kyushu University)

  • Tetsu Tamura

    (Kyushu University)

  • Masaki Saigo

    (Kyushu University)

  • Ken Onda

    (Kyushu University)

  • Shunsuke Sato

    (Kitasato University)

  • Yasuhiro Kobori

    (Molecular Photoscience Research Center
    Kobe University)

  • Kenichiro Tateishi

    (RIKEN
    RIKEN Nishina Center for Accelerator-Based Science)

  • Tomohiro Uesaka

    (RIKEN
    RIKEN Nishina Center for Accelerator-Based Science)

  • Go Watanabe

    (Kitasato University
    Kanagawa Institute of Industrial Science and Technology (KISTEC))

  • Kiyoshi Miyata

    (Kyushu University)

  • Nobuhiro Yanai

    (Graduate School of Engineering
    Center for Molecular Systems (CMS)
    PRESTO, JST
    JST)

Abstract

Singlet fission (SF), converting a singlet excited state into a spin-correlated triplet-pair state, is an effective way to generate a spin quintet state in organic materials. Although its application to photovoltaics as an exciton multiplier has been extensively studied, the use of its unique spin degree of freedom has been largely unexplored. Here, we demonstrate that the spin polarization of the quintet multiexcitons generated by SF improves the sensitivity of magnetic resonance of water molecules through dynamic nuclear polarization (DNP). We form supramolecular assemblies of a few pentacene chromophores and use SF-born quintet spins to achieve DNP of water-glycerol, the most basic biological matrix, as evidenced by the dependence of nuclear polarization enhancement on magnetic field and microwave power. Our demonstration opens a use of SF as a polarized spin generator in bio-quantum technology.

Suggested Citation

  • Yusuke Kawashima & Tomoyuki Hamachi & Akio Yamauchi & Koki Nishimura & Yuma Nakashima & Saiya Fujiwara & Nobuo Kimizuka & Tomohiro Ryu & Tetsu Tamura & Masaki Saigo & Ken Onda & Shunsuke Sato & Yasuhi, 2023. "Singlet fission as a polarized spin generator for dynamic nuclear polarization," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36698-4
    DOI: 10.1038/s41467-023-36698-4
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    References listed on IDEAS

    as
    1. Hiroshi Nonaka & Ryunosuke Hata & Tomohiro Doura & Tatsuya Nishihara & Keiko Kumagai & Mai Akakabe & Masashi Tsuda & Kazuhiro Ichikawa & Shinsuke Sando, 2013. "A platform for designing hyperpolarized magnetic resonance chemical probes," Nature Communications, Nature, vol. 4(1), pages 1-7, December.
    2. M. A. Baldo & D. F. O'Brien & Y. You & A. Shoustikov & S. Sibley & M. E. Thompson & S. R. Forrest, 1998. "Highly efficient phosphorescent emission from organic electroluminescent devices," Nature, Nature, vol. 395(6698), pages 151-154, September.
    3. Daphné Lubert-Perquel & Enrico Salvadori & Matthew Dyson & Paul N. Stavrinou & Riccardo Montis & Hiroki Nagashima & Yasuhiro Kobori & Sandrine Heutz & Christopher W. M. Kay, 2018. "Identifying triplet pathways in dilute pentacene films," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
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