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Two-Dimensional Cobalt(II) Benzoquinone Frameworks for Putative Kitaev Quantum Spin Liquid Candidates

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    Two-Dimensional Cobalt(II) Benzoquinone Frameworks for Putative Kitaev Quantum Spin Liquid Candidates
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    • Songwei Zhang
      Songwei Zhang
      Department of Chemistry & Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States
      More by Songwei Zhang
      Orcidhttps://orcid.org/0000-0001-5930-826X
    • Xu Yang
      Xu Yang
      Department of Physics, The Ohio State University, Columbus, Ohio 43210, United States
      More by Xu Yang
    • Brandi L. Wooten
      Brandi L. Wooten
      Department of Materials Science and Engineering, The Ohio State University, Columbus, Ohio 43210, United States
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    • Rabindranath Bag
      Rabindranath Bag
      Department of Physics, Duke University, Durham, North Carolina 27708, United States
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    • Lalit Yadav
      Lalit Yadav
      Department of Physics, Duke University, Durham, North Carolina 27708, United States
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    • Curtis E Moore
      Curtis E Moore
      Department of Chemistry & Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States
      More by Curtis E Moore
      Orcidhttps://orcid.org/0000-0002-3311-7155
    • Smrutimedha Parida
      Smrutimedha Parida
      Department of Chemistry & Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States
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    • Nandini Trivedi*
      Nandini Trivedi
      Department of Chemistry & Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States
      *E-mail: [email protected]
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    • Yuanming Lu*
      Yuanming Lu
      Department of Physics, The Ohio State University, Columbus, Ohio 43210, United States
      *E-mail: [email protected]
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    • Joseph P. Heremans*
      Joseph P. Heremans
      Department of Mechanical & Aerospace Engineering, The Ohio State University, Columbus, Ohio 43210, United States
      *E-mail: [email protected]
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    • Sara Haravifard*
      Sara Haravifard
      Department of Physics, Duke University, Durham, North Carolina 27708, United States
      *E-mail: [email protected]
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    • Yiying Wu*
      Yiying Wu
      Department of Chemistry & Biochemistry, The Ohio State University, Columbus, Ohio 43210, United States
      *E-mail: [email protected]
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      Orcidhttps://orcid.org/0000-0001-9359-1863
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 22, 15061–15069
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c14537
    Published May 24, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    The realization and discovery of quantum spin liquid (QSL) candidate materials are crucial for exploring exotic quantum phenomena and applications associated with QSLs. Most existing metal–organic two-dimensional (2D) quantum spin liquid candidates have structures with spins arranged on the triangular or kagome lattices, whereas honeycomb-structured metal–organic compounds with QSL characteristics are rare. Here, we report the use of 2,5-dihydroxy-1,4-benzoquinone (X2dhbq, X = Cl, Br, H) as the linkers to construct cobalt(II) honeycomb lattices (NEt4)2[Co2(X2dhbq)3] as promising Kitaev-type QSL candidate materials. The high-spin d7 Co2+ has pseudospin-1/2 ground-state doublets, and benzoquinone-based linkers not only provide two separate superexchange pathways that create bond-dependent frustrated interactions but also allow for chemical tunability to mediate magnetic coupling. Our magnetization data show antiferromagnetic interactions between neighboring metal centers with Weiss constants from −5.1 to −8.5 K depending on the X functional group in X2dhbq linkers (X = Cl, Br, H). No magnetic transition or spin freezing could be observed down to 2 K. Low-temperature susceptibility (down to 0.3 K) and specific heat (down to 0.055 K) of (NEt4)2[Co2(H2dhbq)3] were further analyzed. Heat capacity measurements confirmed no long-range order down to 0.055 K, evidenced by the broad peak instead of the λ-like anomaly. Our results indicate that these 2D cobalt benzoquinone frameworks are promising Kitaev QSL candidates with chemical tunability through ligands that can vary the magnetic coupling and frustration.

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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/jacs.3c14537.

    • Experimental summary of single crystal X-ray diffraction studies; Tables S1–S15; thermodynamic measurements of compounds 1 and 2; Figures S1 and S2 (PDF)

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    CCDC 2320927–2320929 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 1223336033.

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    Cited By

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    This article is cited by 1 publications.

    1. Joseph A. M. Paddison, Matthew J. Cliffe. Discovering Classical Spin Liquids by Topological Search of High Symmetry Nets. ACS Central Science 2024, 10 (10) , 1821-1828. https://doi.org/10.1021/acscentsci.4c01020
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 22, 15061–15069
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.3c14537
    Published May 24, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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