Publications [#300012] of Gregory J. Herschlag

Papers Published

1. G.J. Herschlag, S. Mitran and G. Lin, A consistent hierarchy of generalized kinetic equation approximations to the chemical master equation applied to surface catalysis, J. Chem Phys, vol. 142 (2015), pp. 234703 [3696]
   (last updated on 2015/12/16)

   Abstract:
   We develop a hierarchy of approximations to the master equation for systems that exhibit translational invariance and finite-range spatial correlation. Each approximation within the hierarchy is a set of ordinary di↵erential equations that considers spatial correlations of varying lattice distance; the assumption is that the full system will have finite spatial correlations and thus the behavior of the models within the hierarchy will approach that of the full system. We provide evidence of this convergence in the context of one- and two-dimensional numerical examples. Lower levels within the hierarchy that consider shorter spatial correlations are shown to be up to three orders of magnitude faster than traditional kinetic Monte Carlo methods (KMC) for one-dimensional systems, while pre- dicting similar system dynamics and steady states as KMC methods. We then test the hierarchy on a two-dimensional model for the oxidation of CO on RuO2(110), showing that low-order truncations of the hierarchy e