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The two-dimensional polymer structure and lattice dynamics of the superionicconductor Li4 C60 are investigated by neutron diffraction and spectroscopy. Thepeculiar bonding architecture of this compound is definitely confirmed throughthe precise localisation of the carbon atoms involved in the intermolecularbonds. The spectral features of this phase are revealed through ab-initiolattice dynamics calculations and inelastic neutron scattering experiments. Theneutron observables are found to be in very good agreement with the simulationswhich predict a partial charge transfer from the Li atoms to the C60 cage. Theabsence of a well defined band associated to one category of the Li atoms inthe experimental spectrum suggests that this species is not ordered even at thelowest temperatures. The calculations predict an unstable Li sublattice at atemperature of 200 K, that we relate to the large ionic diffusivity of thissystem. This specificity is discussed in terms of coupling between the lowfrequency optic modes of the Li ions to the soft structure of the polymer.

Structure and dynamics of the fullerene polymer Li4 C60 studied with neutron scattering