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Title: Multiply accelerated ReaxFF molecular dynamics: coupling parallel replica dynamics with collective variable hyper dynamics

Abstract

To address the time scales required to study complex chemical reactions, methods performing accelerated molecular dynamics are necessary even with the recent advancement in high-performance computing. A number of different acceleration techniques are available. Here we explore potential synergies between two popular acceleration methods – Parallel Replica Dynamics (PRD) and Collective Variable Hyperdynamics (CVHD), by analysing the speedup obtained for the pyrolysis of n-dodecane. We determine that PRD + CVHD provides additional speedup to CVHD by reaching the required time scales for the reaction at an earlier wall-clock time. Although some speedup is obtained with the additional replicas, we found that the effectiveness of the inclusion of PRD is depreciated for systems where there is a dramatic increase in reaction rates induced by CVHD. Similar observations were made in the simulation of ethylene-carbonate/Li system, which is inherently more reactive than pyrolysis, suggest that the speedup obtained via the combination of the two acceleration methods can be generalised to most practical chemical systems.

Authors:
 [1];  [1];  [1]
  1. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Univ. of Utah, Salt Lake City, UT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); US Army Research Laboratory (ARO); National Science Foundation (NSF)
OSTI Identifier:
1596124
Grant/Contract Number:  
[SC0019285; W911NF-12-2-0023]
Resource Type:
Accepted Manuscript
Journal Name:
Molecular Simulation
Additional Journal Information:
[ Journal Volume: 45; Journal Issue: 14-15]; Journal ID: ISSN 0892-7022
Publisher:
Taylor & Francis
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; Parallel replica dynamics; collective variable hyperdynamics; pyrolysis; battery electrolytes; ReaxFF

Citation Formats

Ganeshan, Karthik, Hossain, Md. Jamil, and van Duin, Adri C. T. Multiply accelerated ReaxFF molecular dynamics: coupling parallel replica dynamics with collective variable hyper dynamics. United States: N. p., 2019. Web. doi:10.1080/08927022.2019.1646911.
Ganeshan, Karthik, Hossain, Md. Jamil, & van Duin, Adri C. T. Multiply accelerated ReaxFF molecular dynamics: coupling parallel replica dynamics with collective variable hyper dynamics. United States. doi:10.1080/08927022.2019.1646911.
Ganeshan, Karthik, Hossain, Md. Jamil, and van Duin, Adri C. T. Thu . "Multiply accelerated ReaxFF molecular dynamics: coupling parallel replica dynamics with collective variable hyper dynamics". United States. doi:10.1080/08927022.2019.1646911.
@article{osti_1596124,
title = {Multiply accelerated ReaxFF molecular dynamics: coupling parallel replica dynamics with collective variable hyper dynamics},
author = {Ganeshan, Karthik and Hossain, Md. Jamil and van Duin, Adri C. T.},
abstractNote = {To address the time scales required to study complex chemical reactions, methods performing accelerated molecular dynamics are necessary even with the recent advancement in high-performance computing. A number of different acceleration techniques are available. Here we explore potential synergies between two popular acceleration methods – Parallel Replica Dynamics (PRD) and Collective Variable Hyperdynamics (CVHD), by analysing the speedup obtained for the pyrolysis of n-dodecane. We determine that PRD + CVHD provides additional speedup to CVHD by reaching the required time scales for the reaction at an earlier wall-clock time. Although some speedup is obtained with the additional replicas, we found that the effectiveness of the inclusion of PRD is depreciated for systems where there is a dramatic increase in reaction rates induced by CVHD. Similar observations were made in the simulation of ethylene-carbonate/Li system, which is inherently more reactive than pyrolysis, suggest that the speedup obtained via the combination of the two acceleration methods can be generalised to most practical chemical systems.},
doi = {10.1080/08927022.2019.1646911},
journal = {Molecular Simulation},
number = [14-15],
volume = [45],
place = {United States},
year = {2019},
month = {8}
}

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