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Bilayer Metal–Organic Framework Altermagnets with Electrically Tunable Spin-Split Valleys

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    Bilayer Metal–Organic Framework Altermagnets with Electrically Tunable Spin-Split Valleys
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    • Yixuan Che
      Yixuan Che
      Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Yixuan Che
      Orcidhttps://orcid.org/0000-0002-3990-6868
    • Haifeng Lv*
      Haifeng Lv
      State Key Laboratory of Precision and Intelligent Chemistry, CAS Key Laboratory of Materials for Energy Conversion, School of Chemistry and Materials Science, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, Hefei, Anhui 230026, China
      *Email: [email protected]
      More by Haifeng Lv
      Orcidhttps://orcid.org/0000-0001-9491-6367
    • Xiaojun Wu*
      Xiaojun Wu
      State Key Laboratory of Precision and Intelligent Chemistry, CAS Key Laboratory of Materials for Energy Conversion, School of Chemistry and Materials Science, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, Hefei, Anhui 230026, China
      Hefei National Laboratory, University of Science and Technology of China, Hefei, Anhui 230088, China
      *Email: [email protected]
      More by Xiaojun Wu
      Orcidhttps://orcid.org/0000-0003-3606-1211
    • Jinlong Yang
      Jinlong Yang
      Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China
      State Key Laboratory of Precision and Intelligent Chemistry, CAS Key Laboratory of Materials for Energy Conversion, School of Chemistry and Materials Science, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, Hefei, Anhui 230026, China
      Hefei National Laboratory, University of Science and Technology of China, Hefei, Anhui 230088, China
      More by Jinlong Yang
      Orcidhttps://orcid.org/0000-0002-5651-5340
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2025, 147, 17, 14806–14814
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.5c04106
    Published April 18, 2025
    Copyright © 2025 American Chemical Society
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    Abstract

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    Bilayer altermagnets featuring layer-mediated spin-valley locking hold significant promise in spintronics and valleytronics. In this study, we perform a comprehensive symmetry analysis of bilayer altermagnets and identify seven spin point group candidates with spin-valley-layer coupling, including 22, 222212, 24̅, 142222, 24̅221m, 1322, and 162222. Focusing on the platform of bilayer metal–organic frameworks, we theoretically design materials with S4 symmetry through chemical modification, achieving spin-splitting in the valence band. Furthermore, the spin valleys from different layers exhibit tunable responses to external static gate electric fields, enabling precise control of spin-splitting. Our findings presented a framework that integrates spin, valley, and layer degrees of freedom in bilayer altermagnets, paving the way for nanoscale spintronics and valleytronics applications.

    Copyright © 2025 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/jacs.5c04106.

    • Magnetic states and spin densities; band structures with SOC and HSE06 functional; noncollinear magnetic configurations; phonon band structures; AIMD simulations; interlayer distance and shifting; band structures with applied electric fields; mechanical properties; Brillouin zone and k-paths; list of 37 altermagnetic spin point group; crystallographic details; magnetic moments and anisotropies (PDF)

    • Stereographic projections of all 37 altermagnetic point groups (PDF)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2025, 147, 17, 14806–14814
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.5c04106
    Published April 18, 2025
    Copyright © 2025 American Chemical Society
    Request reuse permissions

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