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Journal Articles Nature Communications Year : 2022

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

Laura Voigt
Michael L Aubrey
Philippe Négrier
Mathieu Rouzières
Corine Mathonière

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 VCl 2 (pyrazine) 2 is an electrical insulator, TiCl 2 (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, TiCl 2 (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.
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Origin Publication funded by an institution

Dates and versions

hal-03794863 , version 1 (03-10-2022)

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Cite

Panagiota Perlepe, Itziar Oyarzabal, Laura Voigt, Mariusz Kubus, Daniel N Woodruff, et al.. From an antiferromagnetic insulator to a strongly correlated metal in square-lattice MCl2(pyrazine)2 coordination solids. Nature Communications, 2022, 13, pp.5766. ⟨10.1038/s41467-022-33342-5⟩. ⟨hal-03794863⟩
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