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dc.contributor.authorVeit, Max
dc.contributor.authorJain, Sandeep Kumar
dc.contributor.authorBonakala, Satyanarayana
dc.contributor.authorRudra, Indranil
dc.contributor.authorHohl, Detlef
dc.contributor.authorCsányi, Gábor
dc.date.accessioned2019-02-28T00:30:31Z
dc.date.available2019-02-28T00:30:31Z
dc.date.issued2019-04-09
dc.identifier.issn1549-9618
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/290053
dc.description.abstractThe predictive simulation of molecular liquids requires potential energy surface (PES) models that are not only accurate but also computationally efficient enough to handle the large systems and long time scales required for reliable prediction of macroscopic properties. We present a new approach to the systematic approximation of the first-principles PES of molecular liquids using the GAP (Gaussian Approximation Potential) framework. The approach allows us to create potentials at several different levels of accuracy in reproducing the true PES and thus to determine the level of quantum chemistry that is necessary to accurately predict macroscopic properties. We test the approach by building a series of many-body potentials for liquid methane (CH4), which is difficult to model from first principles because its behavior is dominated by weak dispersion interactions with a significant many-body component. The increasing accuracy of the potentials in predicting the bulk density correlates with their fidelity to the true PES, whereas the trend with the empirical potentials tested is surprisingly the opposite. We conclude that an accurate, consistent prediction of its bulk density across wide ranges of temperature and pressure requires not only many-body dispersion but also quantum nuclear effects to be modeled accurately.
dc.format.mediumPrint-Electronic
dc.languageeng
dc.publisherAmerican Chemical Society (ACS)
dc.titleEquation of State of Fluid Methane from First Principles with Machine Learning Potentials.
dc.typeArticle
prism.endingPage2586
prism.issueIdentifier4
prism.publicationDate2019
prism.publicationNameJ Chem Theory Comput
prism.startingPage2574
prism.volume15
dc.identifier.doi10.17863/CAM.37278
dcterms.dateAccepted2019-01-30
rioxxterms.versionofrecord10.1021/acs.jctc.8b01242
rioxxterms.versionAM
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.licenseref.startdate2019-04
dc.contributor.orcidVeit, Max [0000-0001-7813-4015]
dc.identifier.eissn1549-9626
dc.publisher.urlhttp://dx.doi.org/10.1021/acs.jctc.8b01242
rioxxterms.typeJournal Article/Review
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/P022596/1)
pubs.funder-project-idEPSRC (1602415)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/L015552/1)
cam.issuedOnline2019-02-22
cam.orpheus.successThu Jan 30 10:49:44 GMT 2020 - Embargo updated
datacite.issourceof.doi10.17863/CAM.26364
rioxxterms.freetoread.startdate2020-04-30


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