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The Mott–Hubbard insulating state and orbital degeneracy in the superconducting C603− fulleride family

Nature Materials volume 2, pages 605–610 (2003)Cite this article

Abstract

Electron correlation controls the properties of important materials such as superconducting and magnetoresistive transition metal oxides and heavy fermion systems. The role of correlation in driving metal-to-insulator transitions assumes further importance because many superconducting materials are located close to such transitions. The nature of the insulating ground state often reveals the dominant interactions in the superconductor, as shown by the importance of the properties of La2CuO4 in understanding the high-temperature-superconducting cuprates. The A3C60 alkali metal fullerides are superconducting systems in which the role of correlation in both the normal state and the superconducting pairing mechanism is controversial, because no magnetic insulator comparable to the superconducting materials has been identified. We describe the first example of a cubic C603− system with degenerate orbitals that adopts the Mott–Hubbard insulating localized electron ground state. Electron repulsion is identified as the interaction that is suppressed on the transition to metallic and superconducting behaviour in the fullerides. This observation is combined with ab initio calculations to demonstrate that it is the orbital degeneracy that allows the superconducting cubic A3C60 fullerides to remain metallic while provoking electron localization in systems with lower symmetry.

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Figure 1: The body-centred-cubic (b.c.c.) unit cell of Li3(NH3)6C60 1 (space group Im3̄, lattice parameter a = 11.9230(7) Å).
Figure 2: Magnetic susceptibility versus temperature for 1 measured in a 7 T field.
Figure 3: The low-temperature magnetic transition in 1.
Figure 4: The density of states of the t1u band derived from the fulleride anion overlaps by the density functional theory (DFT) band structure calculations in 1 and K3C60.
Figure 5: The electronic properties of C603− fullerides with structures derived from face-centred-cubic (f.c.c.; square and diamond symbols) and b.c.c. sphere packings (b.c.c.-derived phases are denoted with circles).

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Acknowledgements

We thank the referees for useful suggestions. The SQUID magnetometer was funded by the EPSRC (Engineering and Physical Sciences Research Council) UK, under GR/M91242.

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Authors and Affiliations

  1. Department of Chemistry, University of Liverpool, Liverpool, L69 7ZD, UK

    P. Durand, G. R. Darling & M. J. Rosseinsky

  2. Pirelli Labs S.p.A., Viale Sarca 222, Milan, I-20126, Italy

    Y. Dubitsky & A. Zaopo

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  1. P. Durand
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Correspondence to M. J. Rosseinsky.

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Durand, P., Darling, G., Dubitsky, Y. et al. The Mott–Hubbard insulating state and orbital degeneracy in the superconducting C603− fulleride family. Nature Mater 2, 605–610 (2003). https://doi.org/10.1038/nmat953

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