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Interpolating DFT Data for 15D Modeling of Methane Dissociation on an fcc Metal

Frankcombe, Terry

Description

Detailed simulation of reactions occurring on and with the surfaces of crystalline materials usually require a continuous representation of the potential energy surface that describes the adsorbate–surface interaction. Only a few techniques are available to describe interactions with polyatomic adsorbates that respect all of the symmetries of the interactions. The modified Shepard interpolation has recently been reformulated to ensure symmetries are rigorously imposed. In this work, the...[Show more]

dc.contributor.authorFrankcombe, Terry
dc.date.accessioned2021-04-27T05:22:27Z
dc.identifier.issn0538-8066
dc.identifier.urihttp://hdl.handle.net/1885/231038
dc.description.abstractDetailed simulation of reactions occurring on and with the surfaces of crystalline materials usually require a continuous representation of the potential energy surface that describes the adsorbate–surface interaction. Only a few techniques are available to describe interactions with polyatomic adsorbates that respect all of the symmetries of the interactions. The modified Shepard interpolation has recently been reformulated to ensure symmetries are rigorously imposed. In this work, the modified Shepard interpolation is used to construct a 15D potential energy surface for the reaction of methane with the {100} surface of a face-centered cubic metal, in the Born--Oppenheimer static surface (BOSS) approximation. The energy of the system is calculated using density functional theory (DFT), and the geometries around which the potential is expanded are selected by quasi-classical trajectory calculations. The energy of the resulting continuous potential energy surface exactly matched the DFT energy at these points; there is no fitting error. It is demonstrated that the classical reaction probability converges with a reasonable number of interpolation points for this 15D system.
dc.description.sponsorshipThis work was supported by the NCI National Facility at the ANU. The author acknowledges the support of the Australian Research Council through a Future Fellowship (FT100100824) and Discovery Project grant (DP160100059).
dc.format.mimetypeapplication/pdf
dc.language.isoen_AU
dc.publisherJohn Wiley & Sons Inc
dc.rights© 2018 Wiley Periodicals, Inc.
dc.sourceInternational Journal of Chemical Kinetics
dc.titleInterpolating DFT Data for 15D Modeling of Methane Dissociation on an fcc Metal
dc.typeJournal article
local.description.notesImported from ARIES
local.identifier.citationvolume50
dcterms.dateAccepted2018-01-08
dc.date.issued2018-02-08
local.identifier.absfor030701 - Quantum Chemistry
local.identifier.absfor030603 - Colloid and Surface Chemistry
local.identifier.ariespublicationa383154xPUB9393
local.publisher.urlhttps://onlinelibrary.wiley.com/
local.type.statusAccepted Version
local.contributor.affiliationFrankcombe, Terry, College of Science, ANU
dc.relationhttp://purl.org/au-research/grants/arc/FT100100824
dc.relationhttp://purl.org/au-research/grants/arc/DP160100059
local.bibliographicCitation.issue4
local.bibliographicCitation.startpage285
local.bibliographicCitation.lastpage293
local.identifier.doi10.1002/kin.21157
dc.date.updated2020-11-23T11:45:13Z
local.identifier.scopusID2-s2.0-85041710910
dcterms.accessRightsOpen Access
dc.provenancehttps://v2.sherpa.ac.uk/id/publication/14765..."Author accepted manuscript can be made open access on non-commercial institutional repository after 12 month embargo" from SHERPA/RoMEO site (as at 29.4.2021).
CollectionsANU Research Publications

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