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

Interpolating DFT Data for 15D Modeling of Methane Dissociation on an fcc Metal 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 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. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png International Journal of Chemical Kinetics Wiley

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

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Publisher
Wiley
Copyright
Copyright © 2018 Wiley Periodicals, Inc., A Wiley Company
ISSN
0538-8066
eISSN
1097-4601
D.O.I.
10.1002/kin.21157
Publisher site
See Article on Publisher Site

Abstract

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 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.

Journal

International Journal of Chemical KineticsWiley

Published: Jan 1, 2018

References

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