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