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Title: Parallel kinetic Monte Carlo simulation framework incorporating accurate models of adsorbate lateral interactions

Abstract

Ab initio kinetic Monte Carlo (KMC) simulations have been successfully applied for over two decades to elucidate the underlying physico-chemical phenomena on the surfaces of heterogeneous catalysts. These simulations necessitate detailed knowledge of the kinetics of elementary reactions constituting the reaction mechanism, and the energetics of the species participating in the chemistry. The information about the energetics is encoded in the formation energies of gas and surface-bound species, and the lateral interactions between adsorbates on the catalytic surface, which can be modeled at different levels of detail. The majority of previous works accounted for only pairwise-additive first nearest-neighbor interactions. More recently, cluster-expansion Hamiltonians incorporating long-range interactions and many-body terms have been used for detailed estimations of catalytic rate [C. Wu, D. J. Schmidt, C. Wolverton, and W. F. Schneider, J. Catal. 286, 88 (2012)]. In view of the increasing interest in accurate predictions of catalytic performance, there is a need for general-purpose KMC approaches incorporating detailed cluster expansion models for the adlayer energetics. We have addressed this need by building on the previously introduced graph-theoretical KMC framework, and we have developed Zacros, a FORTRAN2003 KMC package for simulating catalytic chemistries. To tackle the high computational cost in the presence ofmore » long-range interactions we introduce parallelization with OpenMP. We further benchmark our framework by simulating a KMC analogue of the NO oxidation system established by Schneider and co-workers [J. Catal. 286, 88 (2012)]. We show that taking into account only first nearest-neighbor interactions may lead to large errors in the prediction of the catalytic rate, whereas for accurate estimates thereof, one needs to include long-range terms in the cluster expansion.« less

Authors:
; ;  [1];  [2]
  1. Research Software Development Team, Research IT Services, University College London, Torrington Place, London WC1E 6BT (United Kingdom)
  2. Department of Chemical Engineering, University College London, Torrington Place, London WC1E 7JE (United Kingdom)
Publication Date:
OSTI Identifier:
22253805
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 139; Journal Issue: 22; Other Information: (c) 2013 Author(s); Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CATALYSTS; CLUSTER EXPANSION; COMPUTERIZED SIMULATION; FORMATION HEAT; HAMILTONIANS; INTERACTIONS; MONTE CARLO METHOD; REACTION KINETICS; SURFACES

Citation Formats

Nielsen, Jens, D’Avezac, Mayeul, Hetherington, James, and Stamatakis, Michail. Parallel kinetic Monte Carlo simulation framework incorporating accurate models of adsorbate lateral interactions. United States: N. p., 2013. Web. doi:10.1063/1.4840395.
Nielsen, Jens, D’Avezac, Mayeul, Hetherington, James, & Stamatakis, Michail. Parallel kinetic Monte Carlo simulation framework incorporating accurate models of adsorbate lateral interactions. United States. https://doi.org/10.1063/1.4840395
Nielsen, Jens, D’Avezac, Mayeul, Hetherington, James, and Stamatakis, Michail. 2013. "Parallel kinetic Monte Carlo simulation framework incorporating accurate models of adsorbate lateral interactions". United States. https://doi.org/10.1063/1.4840395.
@article{osti_22253805,
title = {Parallel kinetic Monte Carlo simulation framework incorporating accurate models of adsorbate lateral interactions},
author = {Nielsen, Jens and D’Avezac, Mayeul and Hetherington, James and Stamatakis, Michail},
abstractNote = {Ab initio kinetic Monte Carlo (KMC) simulations have been successfully applied for over two decades to elucidate the underlying physico-chemical phenomena on the surfaces of heterogeneous catalysts. These simulations necessitate detailed knowledge of the kinetics of elementary reactions constituting the reaction mechanism, and the energetics of the species participating in the chemistry. The information about the energetics is encoded in the formation energies of gas and surface-bound species, and the lateral interactions between adsorbates on the catalytic surface, which can be modeled at different levels of detail. The majority of previous works accounted for only pairwise-additive first nearest-neighbor interactions. More recently, cluster-expansion Hamiltonians incorporating long-range interactions and many-body terms have been used for detailed estimations of catalytic rate [C. Wu, D. J. Schmidt, C. Wolverton, and W. F. Schneider, J. Catal. 286, 88 (2012)]. In view of the increasing interest in accurate predictions of catalytic performance, there is a need for general-purpose KMC approaches incorporating detailed cluster expansion models for the adlayer energetics. We have addressed this need by building on the previously introduced graph-theoretical KMC framework, and we have developed Zacros, a FORTRAN2003 KMC package for simulating catalytic chemistries. To tackle the high computational cost in the presence of long-range interactions we introduce parallelization with OpenMP. We further benchmark our framework by simulating a KMC analogue of the NO oxidation system established by Schneider and co-workers [J. Catal. 286, 88 (2012)]. We show that taking into account only first nearest-neighbor interactions may lead to large errors in the prediction of the catalytic rate, whereas for accurate estimates thereof, one needs to include long-range terms in the cluster expansion.},
doi = {10.1063/1.4840395},
url = {https://www.osti.gov/biblio/22253805}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 22,
volume = 139,
place = {United States},
year = {Sat Dec 14 00:00:00 EST 2013},
month = {Sat Dec 14 00:00:00 EST 2013}
}