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Interplay of multiple clusters and initial interface positioning for forward flux sampling simulations of crystal nucleation
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Blow, Katarina E., Tribello, Gareth A., Sosso, Gabriele C. and Quigley, David (2023) Interplay of multiple clusters and initial interface positioning for forward flux sampling simulations of crystal nucleation. The Journal of Chemical Physics, 158 (22). 224102 . doi:10.1063/5.0152343 ISSN 1089-7690.
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Official URL: https://doi.org/10.1063/5.0152343
Abstract
Forward flux sampling (FFS) is a path sampling technique widely used in computer simulations of crystal nucleation from the melt. In such studies, the order parameter underpinning the progress of the FFS algorithm is often the size of the largest crystalline nucleus. In this work, we investigate the effects of two computational aspects of FFS simulations, using the prototypical Lennard-Jones liquid as our computational test bed. First, we quantify the impact of the positioning of the liquid basin and first interface in the space of the order parameter. In particular, we demonstrate that these choices are key to ensuring the consistency of the FFS results. Second, we focus on the frequently encountered scenario where the population of crystalline nuclei is such that there are multiple clusters of size comparable to the largest one. We demonstrate the contribution of clusters other than the largest cluster to the initial flux; however, we also show that they can be safely ignored for the purposes of converging a full FFS calculation. We also investigate the impact of different clusters merging, a process that appears to be facilitated by substantial spatial correlations—at least at the supercooling considered here. Importantly, all of our results have been obtained as a function of system size, thus contributing to the ongoing discussion on the impact of finite size effects on simulations of crystal nucleation. Overall, this work either provides or justifies several practical guidelines for performing FFS simulations that can also be applied to more complex and/or computationally expensive models.
Item Type: | Journal Article | |||||||||
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Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Science > Physics Faculty of Science, Engineering and Medicine > Science > Centre for Scientific Computing |
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SWORD Depositor: | Library Publications Router | |||||||||
Library of Congress Subject Headings (LCSH): | Crystal growth, Nucleation, Computational physics, Molecular crystals, Crystallography | |||||||||
Journal or Publication Title: | The Journal of Chemical Physics | |||||||||
Publisher: | AIP Publishing | |||||||||
ISSN: | 1089-7690 | |||||||||
Official Date: | 8 June 2023 | |||||||||
Dates: |
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Volume: | 158 | |||||||||
Number: | 22 | |||||||||
Article Number: | 224102 | |||||||||
DOI: | 10.1063/5.0152343 | |||||||||
Status: | Peer Reviewed | |||||||||
Publication Status: | Published | |||||||||
Access rights to Published version: | Open Access (Creative Commons) | |||||||||
Date of first compliant deposit: | 11 July 2023 | |||||||||
Date of first compliant Open Access: | 11 July 2023 | |||||||||
RIOXX Funder/Project Grant: |
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