Individual fulvene and acetonitrile molecules were geometry optimized in isolation with TeraChem using CAM-B3LYP/6-31G(d). The PACKMOL program was then used to generate a 20 Å3 solvated box of 200 acetonitrile molecules with the fulvene at the center, from which the closest 20 solvent molecules to the fulvene solute were selected to generate configurations for timings. Solvent molecules were then sorted by their distance from the fulvene center to generate configurations with fewer solvent molecules. A final ground state geometry optimization and normal-mode analysis was performed on each of the fulvene-solvent clusters, for which the geometries and normal mode properties of each cluster were used to generate initial conditions for the NAMD simulations according to Eq. 8. The smallest system, consisting of a single acetonitrile solvent molecule and fulvene, as well as the largest 20 solvent molecule-fulvene subsystem, are depicted as insets in Figure .