C60 C60-based molecular crystals, with their unique self-assembly capabilities, have shown promise as viable solid-state electrolytes for Li/Na/Mg-ion batteries. However, there is still controversy regarding the ionic and electronic contributions to the total conductivity of these solids, as well as the specific diffusion mechanism of lithium through the crystal lattice. Further, the high-temperature rotations of C60 molecules in these solids play a significant role on the charge transport properties of the C60 molecular solid. Towards this end, using first-principles based density functional theory (DFT), we investigate the diffusion of lithium through a C60 molecular solid. Specifically, we rigorously examine the preferred diffusion pathways for lithium, and calculate a preliminary value for the effective activation barrier of diffusion. We also employ ab initio molecular dynamics (MD) calculations to begin investigation of the interplay between diffusion and high-temperature rotations of C60. These calculations represent an important step towards designing and developing C60 based solid-state electrolytes for Li-ion as well as Na/Mg ion batteries.
