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From an antiferromagnetic insulator to a strongly correlated metal in square-lattice MCl2(pyrazine)2 coordination solids

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  • Panagiota Perlepe

    (Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP
    Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB)

  • Itziar Oyarzabal

    (Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP
    University of the Basque Country, UPV/EHU
    BCMaterials, Basque Center for Materials, Applications and Nanostructures, UPV/EHU Science Park
    IKERBASQUE, Basque Foundation for Science)

  • Laura Voigt

    (Technical University of Denmark)

  • Mariusz Kubus

    (Technical University of Denmark)

  • Daniel N. Woodruff

    (The University of Oxford)

  • Sebastian E. Reyes-Lillo

    (Universidad Andres Bello)

  • Michael L. Aubrey

    (University of California Berkeley)

  • Philippe Négrier

    (Univ. Bordeaux, CNRS, Laboratoire Ondes et Matière d’Aquitaine)

  • Mathieu Rouzières

    (Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP)

  • Fabrice Wilhelm

    (ESRF—The European Synchrotron)

  • Andrei Rogalev

    (ESRF—The European Synchrotron)

  • Jeffrey B. Neaton

    (Lawrence Berkeley National Laboratory, Berkeley
    The University of California, Berkeley
    Kavli Energy Nanosciences Institute at Berkeley)

  • Jeffrey R. Long

    (University of California Berkeley
    University of California Berkeley
    Lawrence Berkeley National Laboratory)

  • Corine Mathonière

    (Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP)

  • Baptiste Vignolle

    (Univ. Bordeaux, CNRS, Bordeaux INP, ICMCB)

  • Kasper S. Pedersen

    (Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP
    Technical University of Denmark)

  • Rodolphe Clérac

    (Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP)

Abstract

Electronic synergy between metal ions and organic linkers is a key to engineering molecule-based materials with a high electrical conductivity and, ultimately, metallicity. To enhance conductivity in metal-organic solids, chemists aim to bring the electrochemical potentials of the constituent metal ions and bridging organic ligands closer in a quest to obtain metal-d and ligand-π admixed frontier bands. Herein, we demonstrate the critical role of the metal ion in tuning the electronic ground state of such materials. While VCl2(pyrazine)2 is an electrical insulator, TiCl2(pyrazine)2 displays the highest room-temperature electronic conductivity (5.3 S cm–1) for any metal-organic solid involving octahedrally coordinated metal ions. Notably, TiCl2(pyrazine)2 exhibits Pauli paramagnetism consistent with the specific heat, supporting the existence of a Fermi liquid state (i.e., a correlated metal). This result widens perspectives for designing molecule-based systems with strong metal-ligand covalency and electronic correlations.

Suggested Citation

  • Panagiota Perlepe & Itziar Oyarzabal & Laura Voigt & Mariusz Kubus & Daniel N. Woodruff & Sebastian E. Reyes-Lillo & Michael L. Aubrey & Philippe Négrier & Mathieu Rouzières & Fabrice Wilhelm & Andrei, 2022. "From an antiferromagnetic insulator to a strongly correlated metal in square-lattice MCl2(pyrazine)2 coordination solids," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33342-5
    DOI: 10.1038/s41467-022-33342-5
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    1. Renhao Dong & Zhitao Zhang & Diana C. Tranca & Shengqiang Zhou & Mingchao Wang & Peter Adler & Zhongquan Liao & Feng Liu & Yan Sun & Wujun Shi & Zhe Zhang & Ehrenfried Zschech & Stefan C. B. Mannsfeld, 2018. "A coronene-based semiconducting two-dimensional metal-organic framework with ferromagnetic behavior," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    2. B. Vignolle & A. Carrington & R. A. Cooper & M. M. J. French & A. P. Mackenzie & C. Jaudet & D. Vignolles & Cyril Proust & N. E. Hussey, 2008. "Quantum oscillations in an overdoped high-Tc superconductor," Nature, Nature, vol. 455(7215), pages 952-955, October.
    3. Chongqing Yang & Renhao Dong & Mao Wang & Petko St. Petkov & Zhitao Zhang & Mingchao Wang & Peng Han & Marco Ballabio & Sascha A. Bräuninger & Zhongquan Liao & Jichao Zhang & Friedrich Schwotzer & Ehr, 2019. "A semiconducting layered metal-organic framework magnet," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
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