Singlet fission as a polarized spin generator for dynamic nuclear polarization

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  • Kawashima, Yusuke
    Department of Applied Chemistry, Graduate School of Engineering
  • Hamachi, Tomoyuki
    Department of Applied Chemistry, Graduate School of Engineering
  • Yamauchi, Akio
    Department of Applied Chemistry, Graduate School of Engineering
  • Nishimura, Koki
    Department of Applied Chemistry, Graduate School of Engineering
  • Nakashima, Yuma
    Department of Applied Chemistry, Graduate School of Engineering
  • Fujiwara, Saiya
    Department of Applied Chemistry, Graduate School of Engineering
  • Kimizuka, Nobuo
    Department of Applied Chemistry, Graduate School of Engineering Center for Molecular Systems (CMS)
  • Ryu, Tomohiro
    Department of Chemistry, Graduate School of Science, Kyushu University
  • Tamura, Tetsu
    Department of Chemistry, Graduate School of Science, Kyushu University
  • Saigo, Masaki
    Department of Chemistry, Graduate School of Science, Kyushu University
  • Onda, Ken
    Department of Chemistry, Graduate School of Science, Kyushu University
  • Sato, Shunsuke
    Department of Physics, School of Science, Kitasato University
  • Kobori, Yasuhiro
    Molecular Photoscience Research Center Department of Chemistry, Graduate School of Science, Kobe University
  • Tateishi, Kenichiro
    Cluster for Pioneering Research, RIKEN RIKEN Nishina Center for Accelerator-Based Science
  • Uesaka, Tomohiro
    Cluster for Pioneering Research, RIKEN RIKEN Nishina Center for Accelerator-Based Science
  • Watanabe, Go
    Department of Physics, School of Science, Kitasato University Kanagawa Institute of Industrial Science and Technology (KISTEC)
  • Miyata, Kiyoshi
    Department of Chemistry, Graduate School of Science, Kyushu University
  • Yanai, Nobuhiro
    Department of Applied Chemistry, Graduate School of Engineering Center for Molecular Systems (CMS) PRESTO, JST FOREST, JST

Description

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.

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