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

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 Rogalev, Jeffrey B. Neaton, Jeffrey R. Long, Corine Mathonière, Baptiste Vignolle (), Kasper S. Pedersen () and Rodolphe Clérac ()
Additional contact information
Panagiota Perlepe: Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP
Itziar Oyarzabal: Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP
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
Jeffrey R. Long: University of California Berkeley
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
Rodolphe Clérac: Univ. Bordeaux, CNRS, Centre de Recherche Paul Pascal, CRPP

Nature Communications, 2022, vol. 13, issue 1, 1-7

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-33342-5

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