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New Polymeric Phase in Low‐Doped Lithium Intercalated Fullerides

Abstract The low‐doped Li x C60 compounds (x≤6) were investigated using laboratory X‐ray and synchrotron radiation diffraction, 13C NMR and Raman spectroscopy. Li4C60 shows an unusual 2D polymerisation in which the C60 units are connected both by [2+2] cycloaddition and by single carbon–carbon bonds, a unique feature among the known polymerised fullerene compounds. This picture is fully supported also by static NMR and Raman measurements. The charge transfer to C60 in the polymeric phase was evaluated from the shift of the Ag(2) mode. The depolymerisation process was investigated as well; despite the presence of two different bonds, the polymer‐to‐monomer transition induced by thermal treatments is a single‐step phenomenon.