Single-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation

Handle URI:
http://hdl.handle.net/10754/612967
Title:
Single-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation
Authors:
Kadoura, Ahmad Salim ( 0000-0001-9317-682X ) ; Siripatana, Adil; Sun, Shuyu ( 0000-0002-3078-864X ) ; Knio, Omar; Hoteit, Ibrahim ( 0000-0002-3751-4393 )
Abstract:
In this work, two Polynomial Chaos (PC) surrogates were generated to reproduce Monte Carlo (MC) molecular simulation results of the canonical (single-phase) and the NVT-Gibbs (two-phase) ensembles for a system of normalized structureless Lennard-Jones (LJ) particles. The main advantage of such surrogates, once generated, is the capability of accurately computing the needed thermodynamic quantities in a few seconds, thus efficiently replacing the computationally expensive MC molecular simulations. Benefiting from the tremendous computational time reduction, the PC surrogates were used to conduct large-scale optimization in order to propose single-site LJ models for several simple molecules. Experimental data, a set of supercritical isotherms, and part of the two-phase envelope, of several pure components were used for tuning the LJ parameters (ε, σ). Based on the conducted optimization, excellent fit was obtained for different noble gases (Ar, Kr, and Xe) and other small molecules (CH4, N2, and CO). On the other hand, due to the simplicity of the LJ model used, dramatic deviations between simulation and experimental data were observed, especially in the two-phase region, for more complex molecules such as CO2 and C2 H6.
KAUST Department:
Computational Transport Phenomena Lab; Earth Sciences and Engineering; Physical Sciences and Engineering (PSE) Division; Earth Fluid Modeling and Prediction Group; Uncertainty Quantification Center; Applied Mathematics and Computational Science Program; Computer, Electrical and Mathematical Science and Engineering (CEMSE) Division
Citation:
Single-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation 2016, 144 (21):214301 The Journal of Chemical Physics
Publisher:
AIP Publishing
Journal:
The Journal of Chemical Physics
Issue Date:
1-Jun-2016
DOI:
10.1063/1.4952976
Type:
Article
ISSN:
0021-9606; 1089-7690
Sponsors:
This research is funded by King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia.
Additional Links:
http://scitation.aip.org/content/aip/journal/jcp/144/21/10.1063/1.4952976
Appears in Collections:
Articles

Full metadata record

DC FieldValue Language
dc.contributor.authorKadoura, Ahmad Salimen
dc.contributor.authorSiripatana, Adilen
dc.contributor.authorSun, Shuyuen
dc.contributor.authorKnio, Omaren
dc.contributor.authorHoteit, Ibrahimen
dc.date.accessioned2016-06-14T08:09:36Z-
dc.date.available2016-06-14T08:09:36Z-
dc.date.issued2016-06-01-
dc.identifier.citationSingle-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation 2016, 144 (21):214301 The Journal of Chemical Physicsen
dc.identifier.issn0021-9606-
dc.identifier.issn1089-7690-
dc.identifier.doi10.1063/1.4952976-
dc.identifier.urihttp://hdl.handle.net/10754/612967-
dc.description.abstractIn this work, two Polynomial Chaos (PC) surrogates were generated to reproduce Monte Carlo (MC) molecular simulation results of the canonical (single-phase) and the NVT-Gibbs (two-phase) ensembles for a system of normalized structureless Lennard-Jones (LJ) particles. The main advantage of such surrogates, once generated, is the capability of accurately computing the needed thermodynamic quantities in a few seconds, thus efficiently replacing the computationally expensive MC molecular simulations. Benefiting from the tremendous computational time reduction, the PC surrogates were used to conduct large-scale optimization in order to propose single-site LJ models for several simple molecules. Experimental data, a set of supercritical isotherms, and part of the two-phase envelope, of several pure components were used for tuning the LJ parameters (ε, σ). Based on the conducted optimization, excellent fit was obtained for different noble gases (Ar, Kr, and Xe) and other small molecules (CH4, N2, and CO). On the other hand, due to the simplicity of the LJ model used, dramatic deviations between simulation and experimental data were observed, especially in the two-phase region, for more complex molecules such as CO2 and C2 H6.en
dc.description.sponsorshipThis research is funded by King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia.en
dc.language.isoenen
dc.publisherAIP Publishingen
dc.relation.urlhttp://scitation.aip.org/content/aip/journal/jcp/144/21/10.1063/1.4952976en
dc.rightsArchived with thanks to The Journal of Chemical Physicsen
dc.titleSingle-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulationen
dc.typeArticleen
dc.contributor.departmentComputational Transport Phenomena Laben
dc.contributor.departmentEarth Sciences and Engineeringen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentEarth Fluid Modeling and Prediction Groupen
dc.contributor.departmentUncertainty Quantification Centeren
dc.contributor.departmentApplied Mathematics and Computational Science Programen
dc.contributor.departmentComputer, Electrical and Mathematical Science and Engineering (CEMSE) Divisionen
dc.identifier.journalThe Journal of Chemical Physicsen
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorKadoura, Ahmad Salimen
kaust.authorSiripatana, Adilen
kaust.authorSun, Shuyuen
kaust.authorKnio, Omaren
kaust.authorHoteit, Ibrahimen
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