Abstract
C60-based solids1 are archetypal molecular superconductors with transition temperatures (Tc) as high as 33 K (refs 2–4). Tc of face-centred-cubic (f.c.c.) A3C60 (A=alkali metal) increases monotonically with inter C60 separation, which is controlled by the A+ cation size. As Cs+ is the largest such ion, Cs3C60 is a key material in this family. Previous studies revealing trace superconductivity in CsxC60 materials have not identified the structure or composition of the superconducting phase owing to extremely small shielding fractions and low crystallinity. Here, we show that superconducting Cs3C60 can be reproducibly isolated by solvent-controlled synthesis and has the highest Tc of any molecular material at 38 K. In contrast to other A3C60 materials, two distinct cubic Cs3C60 structures are accessible. Although f.c.c. Cs3C60 can be synthesized, the superconducting phase has the A15 structure based uniquely among fullerides on body-centred-cubic packing. Application of hydrostatic pressure controllably tunes A15 Cs3C60 from insulating at ambient pressure to superconducting without crystal structure change and reveals a broad maximum in Tc at ∼7 kbar. We attribute the observed Tc maximum as a function of inter C60separation—unprecedented in fullerides but reminiscent of the atom-based cuprate superconductors—to the role of strong electronic correlations near the metal–insulator transition onset.
This is a preview of subscription content, access via your institution
Relevant articles
Open Access articles citing this article.
-
Searching for ductile superconducting Heusler X2YZ compounds
npj Computational Materials Open Access 09 August 2023
-
Flattened 1D fragments of fullerene C60 that exhibit robustness toward multi-electron reduction
Nature Communications Open Access 15 May 2023
-
Heterospin frustration in a metal-fullerene-bonded semiconductive antiferromagnet
Nature Communications Open Access 25 January 2022
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Rent or buy this article
Prices vary by article type
from$1.95
to$39.95
Prices may be subject to local taxes which are calculated during checkout




References
Hebard, A. F. et al. Superconductivity at 18 K in potassium-doped fullerene (C60). Nature 350, 600–601 (1991).
Iwasa, Y. & Takenobu, T. Superconductivity, Mott–Hubbard states, and molecular orbital order in intercalated fullerides. J. Phys. Condens. Matter 15, R495–R519 (2003).
Gunnarsson, O. Superconductivity in fullerides. Rev. Mod. Phys. 69, 575–606 (1997).
Tanigaki, K. et al. Superconductivity at 33 K in cesium rubidium fulleride (CsxRbyC60). Nature 352, 222–223 (1991).
Zhou, O. & Cox, D. E. Structures of fullerene (C60) intercalation compounds. J. Phys. Chem. Solids 53, 1373–1390 (1992).
Kelty, S. P., Chen, C. C. & Lieber, C. M. Superconductivity at 30 K in cesium-doped fullerene. Nature 352, 223–225 (1991).
Kinoshita, N., Tanaka, Y., Tokumoto, M. & Matsumiya, S. Superconductivity and electron spin resonance in Cs-doped C60 . Solid State Commun. 83, 883–886 (1992).
Palstra, T. T. M. et al. Superconductivity at 40 K in cesium doped C60 . Solid State Commun. 93, 327–330 (1995).
Messaoudi, A., Conard, J., Setton, R. & Beguin, F. New intercalation compounds of C60 with cesium. Chem. Phys. Lett. 202, 506–508 (1993).
Fujiki, S. et al. Structure and Raman scattering of Cs3C60 under high pressure. Phys. Rev. B. 62, 5366–5369 (2000).
Cooke, S., Glenis, S., Chen, X., Lin, C. L. & Labes, M. New preparation of superconducting alkali-metal fullerides utilizing monomethylamine as solvent. J. Mater. Chem. 6, 1–3 (1996).
Ganin, A. Y. et al. Methylaminated potassium fulleride, (CH3NH2)K3C60: Towards hyperexpanded fulleride lattices. J. Am. Chem. Soc. 128, 14784–14785 (2006).
Takabayashi, Y., Ganin, A. Y., Rosseinsky, M. J. & Prassides, K. Direct observation of magnetic ordering in the (CH3NH2)K3C60 fulleride. Chem. Commun. 870–872 (2007).
Dahlke, P., Denning, M. S., Henry, P. F. & Rosseinsky, M. J. Superconductivity in expanded fcc C603− fullerides. J. Am. Chem. Soc. 122, 12352–12361 (2000).
Stephens, P. W. et al. Structure of single-phase superconducting potassium buckminsterfullerene (K3C60). Nature 351, 632–634 (1991).
Lof, R. W., van Veenendaal, M. A., Koopmans, B., Jonkman, H. T. & Sawatzky, G. A. Band gap, excitons, and Coulomb interaction in solid fullerene C60 . Phys. Rev. Lett. 68, 3924–2927 (1992).
Gunnarsson, O., Koch, E. & Martin, R. M. Mott–Hubbard insulators for systems with orbital degeneracy. Phys. Rev. B 56, 1146–1152 (1997).
Han, J. E., Koch, E. & Gunnarsson, O. Metal–insulator transitions. Influence of lattice structure, Jahn–Teller effect, and Hund’s rule coupling. Phys. Rev. Lett. 84, 1276–1279 (2000).
Han, J. E., Gunnarsson, O. & Crespi, V. H. Strong superconductivity with local Jahn–Teller phonons in C60 solids. Phys. Rev. Lett. 90, 167006 (2003).
Capone, M., Fabrizio, M., Castellani, C. & Tosatti, E. Strongly correlated superconductivity. Science 296, 2364–2366 (2002).
Diederichs, J., Schilling, J. S., Herwig, K. W. & Yelon, W. B. Dependence of the superconducting transition temperature and lattice parameter on hydrostatic pressure for Rb3C60 . J. Phys. Chem. Solids 58, 123–132 (1997).
Zhou, O. et al. Compressibility of M3C60 fullerene superconductors: Relation between Tc and lattice parameter. Science 255, 833–835 (1992).
Margadonna, S. et al. Pressure and temperature evolution of the structure of the superconducting Na2CsC60 fulleride. J. Solid State Chem. 145, 471–478 (1999).
Acknowledgements
We thank EPSRC for financial support under EP/C511794 and GR/S77820 and for access to the synchrotron X-ray facilities at the SRS (where we thank A. Lennie and M. A. Roberts for assistance on stations 9.5 and 9.1) and the European Synchrotron Radiation Facility (where we thank A. N. Fitch, W. van Beek and D. Papanikolaou for assistance on beamlines ID31 and BM1).
Author information
Authors and Affiliations
Corresponding authors
Supplementary information
Supplementary Information
Supplementary Scheme S1,S2, Supplementary Table S1–S2 and Supplementary Figures S1–S6 (PDF 2387 kb)
Rights and permissions
About this article
Cite this article
Ganin, A., Takabayashi, Y., Khimyak, Y. et al. Bulk superconductivity at 38 K in a molecular system. Nature Mater 7, 367–371 (2008). https://doi.org/10.1038/nmat2179
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nmat2179
This article is cited by
-
Flattened 1D fragments of fullerene C60 that exhibit robustness toward multi-electron reduction
Nature Communications (2023)
-
Searching for ductile superconducting Heusler X2YZ compounds
npj Computational Materials (2023)
-
Heterospin frustration in a metal-fullerene-bonded semiconductive antiferromagnet
Nature Communications (2022)
-
Tuning the electronic states and superconductivity in alkali fulleride films
AAPPS Bulletin (2022)
-
Realizing nearly-free-electron like conduction band in a molecular film through mediating intermolecular van der Waals interactions
Nature Communications (2019)