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

Loading next page...
 
/lp/wiley/interpolating-dft-data-for-15d-modeling-of-methane-dissociation-on-an-tPHp6X3U8X
Publisher
Wiley Subscription Services, Inc., A Wiley Company
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

You’re reading a free preview. Subscribe to read the entire article.


DeepDyve is your
personal research library

It’s your single place to instantly
discover and read the research
that matters to you.

Enjoy affordable access to
over 12 million articles from more than
10,000 peer-reviewed journals.

All for just $49/month

Explore the DeepDyve Library

Unlimited reading

Read as many articles as you need. Full articles with original layout, charts and figures. Read online, from anywhere.

Stay up to date

Keep up with your field with Personalized Recommendations and Follow Journals to get automatic updates.

Organize your research

It’s easy to organize your research with our built-in tools.

Your journals are on DeepDyve

Read from thousands of the leading scholarly journals from SpringerNature, Elsevier, Wiley-Blackwell, Oxford University Press and more.

All the latest content is available, no embargo periods.

See the journals in your area

DeepDyve Freelancer

DeepDyve Pro

Price
FREE
$49/month

$360/year
Save searches from Google Scholar, PubMed
Create lists to organize your research
Export lists, citations
Access to DeepDyve database
Abstract access only
Unlimited access to over
18 million full-text articles
Print
20 pages/month
PDF Discount
20% off