Campus Units
Chemistry, Ames Laboratory
Document Type
Article
Publication Version
Published Version
Publication Date
2009
Journal or Book Title
Journal of Physical Chemistry A
Volume
113
Issue
3
First Page
607
Last Page
616
DOI
10.1021/jp805688j
Abstract
The use of ab initio potentials in Monte Carlo simulations aimed at investigating the nucleation kinetics of water clusters is complicated by the computational expense of the potential energy determinations. Furthermore, the common desire to investigate the temperature dependence of kinetic properties leads to an urgent need to reduce the expense of performing simulations at many different temperatures. A method is detailed that allows a Markov chain (obtained via Monte Carlo) at one temperature to be scaled to other temperatures of interest without the need to perform additional large simulations. This Markov chain temperature-scaling (TeS) can be generally applied to simulations geared for numerous applications. This paper shows the quality of results which can be obtained by TeS and the possible quantities which may be extracted from scaled Markov chains. Results are obtained for a 1-D analytical potential for which the exact solutions are known. Also, this method is applied to water clusters consisting of between 2 and 5 monomers, using Dynamical Nucleation Theory to determine the evaporation rate constant for monomer loss. Although ab initio potentials are not utilized in this paper, the benefit of this method is made apparent by using the Dang−Chang polarizable classical potential for water to obtain statistical properties at various temperatures.
Copyright Owner
American Chemical Society
Copyright Date
2009
Language
en
File Format
application/pdf
Recommended Citation
Crosby, Lonnie D. and Windus, Theresa Lynn, "Temperature Scaling Method for Markov Chains" (2009). Chemistry Publications. 922.
https://lib.dr.iastate.edu/chem_pubs/922
Comments
Reprinted (adapted) with permission from Journal of Physical Chemistry A 113 (2009): 607, doi:10.1021/jp805688j. Copyright 2009 American Chemical Society.