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Heterospin frustration in a metal-fullerene-bonded semiconductive antiferromagnet

Author

Listed:
  • Yongbing Shen

    (Tohoku University)

  • Mengxing Cui

    (Tohoku University)

  • Shinya Takaishi

    (Tohoku University)

  • Hideyuki Kawasoko

    (Tohoku University)

  • Kunihisa Sugimoto

    (Diffraction & Scattering Division Synchrotron Radiation Research Institute)

  • Takao Tsumuraya

    (Kumamoto University)

  • Akihiro Otsuka

    (Kyoto University
    Kyoto University)

  • Eunsang Kwon

    (Tohoku University)

  • Takefumi Yoshida

    (Tohoku University)

  • Norihisa Hoshino

    (Tohoku University)

  • Kazuhiko Kawachi

    (Idea International Co., Ltd.)

  • Yasuhiko Kasama

    (Idea International Co., Ltd.)

  • Tomoyuki Akutagawa

    (Tohoku University)

  • Tomoteru Fukumura

    (Tohoku University
    Tohoku University)

  • Masahiro Yamashita

    (Tohoku University
    Nankai University)

Abstract

Lithium-ion-encapsulated fullerenes (Li+@C60) are 3D superatoms with rich oxidative states. Here we show a conductive and magnetically frustrated metal–fullerene-bonded framework {[Cu4(Li@C60)(L)(py)4](NTf2)(hexane)}n (1) (L = 1,2,4,5-tetrakis(methanesulfonamido)benzene, py = pyridine, NTf2− = bis(trifluoromethane)sulfonamide anion) prepared from redox-active dinuclear metal complex Cu2(L)(py)4 and lithium-ion-encapsulated fullerene salt (Li+@C60)(NTf2−). Electron donor Cu2(L)(py)2 bonds to acceptor Li+@C60 via eight Cu‒C bonds. Cu–C bond formation stems from spontaneous charge transfer (CT) between Cu2(L)(py)4 and (Li+@C60)(NTf2−) by removing the two-terminal py molecules, yielding triplet ground state [Cu2(L)(py)2]+(Li+@C60•−), evidenced by absorption and electron paramagnetic resonance (EPR) spectra, magnetic properties and quantum chemical calculations. Moreover, Li+@C60•− radicals (S = ½) and Cu2+ ions (S = ½) interact antiferromagnetically in triangular spin lattices in the absence of long-range magnetic ordering to 1.8 K. The low-temperature heat capacity indicated that compound 1 is a potential candidate for an S = ½ quantum spin liquid (QSL).

Suggested Citation

  • Yongbing Shen & Mengxing Cui & Shinya Takaishi & Hideyuki Kawasoko & Kunihisa Sugimoto & Takao Tsumuraya & Akihiro Otsuka & Eunsang Kwon & Takefumi Yoshida & Norihisa Hoshino & Kazuhiko Kawachi & Yasu, 2022. "Heterospin frustration in a metal-fullerene-bonded semiconductive antiferromagnet," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28134-w
    DOI: 10.1038/s41467-022-28134-w
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