Toward Realistic Transfer Rates within the Coupled Molecular Dynamics/Lattice Monte Carlo Approach Gabriel Kabbe Christian Dreßler Daniel Sebastiani 10.1021/acs.jpcc.6b05821.s001 https://acs.figshare.com/articles/journal_contribution/Toward_Realistic_Transfer_Rates_within_the_Coupled_Molecular_Dynamics_Lattice_Monte_Carlo_Approach/3799398 We refine our recently developed coupled molecular dynamics/lattice Monte Carlo (cMD/LMC) scheme for the simulation of protonation dynamics in complex hydrogen-bonded solids in view of improving the resulting transport processes. The distance dependency of the proton jump rate between lattice sites and its dependence on additional geometric criteria (bond angles) are derived in a systematic and consistent way. The distance dependency follows an accurate potential energy surface (PES) scan from quantum chemical calculations. The novel geometric criterion takes into account that proton hopping occurs almost exclusively along linear hydrogen bonds. We illustrate the capabilities and the versatility of our scheme on the example of two chemically quite different condensed phase systems: a crystalline solid acid compound and a liquid crystal. Surprisingly, we find that our cMD/LMC scheme yields converged mobility parameters even when based on underlying <i>ab initio</i> molecular dynamics (AIMD) trajectories which themselves are not fully converged. Our method yields more accurate values for the mean square displacement, the OH bond autocorrelation function and the proton jump frequencies in agreement with both reference AIMD simulations and experimental values. 2016-08-22 00:00:00 resulting transport processes quantum chemical calculations proton jump rate proton jump frequencies mean square displacement additional geometric criteria ab initio </ lattice monte carlo reference aimd simulations distance dependency follows coupled molecular dynamics distance dependency molecular dynamics lattice sites protonation dynamics method yields liquid crystal fully converged experimental values consistent way complex hydrogen bonded solids bond angles accurate values