Abstract
NEARLY all of the molecular crystals containing C60, formed at ambient pressure1,2 have inter-fullerene separations of the order of 10 Å — the expected distance based on the molecular van der Waals radii. The sole exceptions are the room-temperature phases of AC60 (where A denotes K, Rb or Cs), which are formed by reversible solid-state transformation from high-temperature (>150 °C) phases3. These phases have lattice parameters about 9% shorter in one direction, and in addition RbC60 has magnetic properties suggestive of a one-dimensional metal4. We suggested in ref. 4 that this short distance may be due to covalent bonding between neighbouring C60 molecules. Here we provide direct evidence for such bonding from powder X-ray diffraction studies of RbC60 and KC60 . The linkage is through a [2+2] cycloaddition, which has been hypothesized to take place during photopolymerization of solid C60 (ref. 5), and which has also been proposed6 for RbC60. Such inter-fullerene linkages are calculated7,8 to be the preferred mode of dimerization of C60. The AC60 phases thus provide an example of a thermal phase transition driven by the reversible formation and breaking of covalent bonds.
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Stephens, P., Bortel, G., Faigel, G. et al. Polymeric fullerene chains in RbC60 and KC60. Nature 370, 636–639 (1994). https://doi.org/10.1038/370636a0
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DOI: https://doi.org/10.1038/370636a0
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