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Polymorphism control of superconductivity and magnetism in Cs3C60 close to the Mott transition


The crystal structure of a solid controls the interactions between the electronically active units and thus its electronic properties. In the high-temperature superconducting copper oxides, only one spatial arrangement of the electronically active Cu2+ units—a two-dimensional square lattice—is available to study the competition between the cooperative electronic states of magnetic order and superconductivity1. Crystals of the spherical molecular C603- anion support both superconductivity and magnetism but can consist of fundamentally distinct three-dimensional arrangements of the anions. Superconductivity in the A3C60 (A = alkali metal) fullerides has been exclusively associated with face-centred cubic (f.c.c.) packing of C603- (refs 2, 3), but recently the most expanded (and thus having the highest superconducting transition temperature, Tc; ref. 4) composition Cs3C60 has been isolated as a body-centred cubic (b.c.c.) packing, which supports both superconductivity and magnetic order5,6. Here we isolate the f.c.c. polymorph of Cs3C60 to show how the spatial arrangement of the electronically active units controls the competing superconducting and magnetic electronic ground states. Unlike all the other f.c.c. A3C60 fullerides, f.c.c. Cs3C60 is not a superconductor but a magnetic insulator at ambient pressure, and becomes superconducting under pressure. The magnetic ordering occurs at an order of magnitude lower temperature in the geometrically frustrated f.c.c. polymorph (Néel temperature TN = 2.2 K) than in the b.c.c.-based packing (TN = 46 K). The different lattice packings of C603- change Tc from 38 K in b.c.c. Cs3C60 to 35 K in f.c.c. Cs3C60 (the highest found in the f.c.c. A3C60 family). The existence of two superconducting packings of the same electronically active unit reveals that Tc scales universally in a structure-independent dome-like relationship with proximity to the Mott metal–insulator transition, which is governed by the role of electron correlations characteristic of high-temperature superconducting materials other than fullerides.

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Figure 1: Crystal structure and structural characterization of f.c.c. Cs3C60.
Figure 2: Ambient pressure magnetic properties of f.c.c. Cs3C60.
Figure 3: Superconductivity under pressure in f.c.c. Cs3C60.
Figure 4: Electronic phase diagrams shown as functions of volume occupied per fulleride anion and normalized conduction bandwidth in the two sphere packings of A 3 C 60 superconductors.


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We thank EPSRC for support (EP/G037132 and EP/G037949) and STFC for access to the synchrotron X-ray facilities at the ESRF (where we thank A. N. Fitch for assistance on beamline ID31) and Diamond (where we thank C. Tang for assistance on beamline I11) and to the muon facilities at ISIS. We also thank SPring-8 for access to the synchrotron X-ray facilities.

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Authors and Affiliations



M.J.R. and K.P. directed and coordinated the project. A.Y.G., M.T.M., M.D.T. and A.M. synthesized the samples. Y.T., A.Y.G. and K.P. performed the ambient pressure synchrotron XRD measurements and Y.T. analysed the data. Y.T., M.T.M. and M.D.T. carried out the ambient and high pressure magnetization measurements. Y.T., A.Y.G., Y.O., M.T. and K.P. performed the high pressure synchrotron XRD measurements and Y.T. analysed the data. Y.T., A.Y.G., P.J.B. and K.P. carried out the μSR measurements and K.P. and P.J.B. analysed the data. P.J., A.P. and D.A. performed and analysed the NMR measurements. G.R.D. carried out electronic structure calculations. M.J.R. and K.P. wrote the paper. All authors commented on the paper.

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Correspondence to Matthew J. Rosseinsky or Kosmas Prassides.

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The authors declare no competing financial interests.

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Ganin, A., Takabayashi, Y., Jeglič, P. et al. Polymorphism control of superconductivity and magnetism in Cs3C60 close to the Mott transition. Nature 466, 221–225 (2010).

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