UCL Discovery
UCL home » Library Services » Electronic resources » UCL Discovery

A Caching Scheme to Accelerate Kinetic Monte Carlo Simulations of Catalytic Reactions

Ravipati, S; d'Avezac, M; Nielsen, J; Hetherington, J; Stamatakis, M; (2020) A Caching Scheme to Accelerate Kinetic Monte Carlo Simulations of Catalytic Reactions. The Journal of Physical Chemistry A 10.1021/acs.jpca.0c03571. (In press).

[img] Text
ProductCaching_Revised.pdf - Accepted version
Access restricted to UCL open access staff until 30 July 2021.

Download (991kB)

Abstract

Kinetic Monte Carlo (KMC) simulations have been instrumental in advancing our fundamental understanding of heterogeneously catalyzed reactions, with particular emphasis on structure sensitivity, ensemble effects, and the interplay between adlayer structure and adsorbate-adsorbate lateral interactions in shaping the observed kinetics. Yet, the computational cost of KMC remains high, thereby motivating the development of acceleration schemes that would improve the simulation effciency. We present an exact such scheme, which implements a caching algorithm along with shared-memory parallelization to improve the computational performance of simulations incorporating long-range adsorbate-adsorbate lateral interactions. This scheme is based on caching information about the energetic interaction patterns associated with the products of each possible lattice process (adsorption, desorption, reaction etc). Thus, every time a reaction occurs ("ongoing reaction") it enables fast updates of the rate constants of "affected reactions", i.e. possible reactions in the region of influence of the "ongoing reaction". Benchmarks on KMC simulations of NOx oxidation/reduction, yield acceleration factors of up to 20× when comparing single-thread runs without caching to runs on 16 threads with caching, for simulations with a cluster expansion Hamiltonian that incorporates up to 8th nearest-neighbor interactions.

Type: Article
Title: A Caching Scheme to Accelerate Kinetic Monte Carlo Simulations of Catalytic Reactions
DOI: 10.1021/acs.jpca.0c03571
Publisher version: https://doi.org/10.1021/acs.jpca.0c03571
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Computer Science
URI: https://discovery.ucl.ac.uk/id/eprint/10106559
Downloads since deposit
1Download
Download activity - last month
Download activity - last 12 months
Downloads by country - last 12 months

Archive Staff Only

View Item View Item