Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond

Hyperthermal polyatomic fluorocarbon (FC) deposition upon the diamond (111) surface is simulated and analyzed at several levels of computational theory. Classical molecular dynamics simulations using the reactive empirical bond order (REBO) potential are used to categorize the surface reactions that...

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Main Authors: Devine, B., Jang, I., Kemper, T., Lee, D., Gale, Julian, Iordanova, N., Simmott, S.
Format: Journal Article
Published: American Chemical Society 2010
Online Access:http://hdl.handle.net/20.500.11937/5318
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author Devine, B.
Jang, I.
Kemper, T.
Lee, D.
Gale, Julian
Iordanova, N.
Simmott, S.
author_facet Devine, B.
Jang, I.
Kemper, T.
Lee, D.
Gale, Julian
Iordanova, N.
Simmott, S.
author_sort Devine, B.
building Curtin Institutional Repository
collection Online Access
description Hyperthermal polyatomic fluorocarbon (FC) deposition upon the diamond (111) surface is simulated and analyzed at several levels of computational theory. Classical molecular dynamics simulations using the reactive empirical bond order (REBO) potential are used to categorize the surface reactions that occur during radical deposition. Molecular dynamics (MD) simulations, using density functional theory (DFT-MD) via the SIESTA method and program, are used to corroborate the findings from the classical simulations and to categorize reactions that occur during cation deposition. Finally, reaction enthalpies are calculated with higher level quantum mechanical methods using a cluster model to verify and refine the predictions from the MD simulations. The multilevel analysis predicts that FC radicals add directly to the diamond (111) surface with the simultaneous formation of HF. In contrast, FC cations preferentially dissociate H from the surface leaving behind a cationic carbon site. Cations and radical species are found to prefer different reaction pathways, which limits the applicability of REBO. Furthermore, the comparison reveals a difference in the predicted reaction probabilities between REBO and DFT which is attributable to the short cut off distance for interaction in the current REBO formulation.
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institution Curtin University Malaysia
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spelling curtin-20.500.11937-53182017-09-13T16:06:25Z Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond Devine, B. Jang, I. Kemper, T. Lee, D. Gale, Julian Iordanova, N. Simmott, S. Hyperthermal polyatomic fluorocarbon (FC) deposition upon the diamond (111) surface is simulated and analyzed at several levels of computational theory. Classical molecular dynamics simulations using the reactive empirical bond order (REBO) potential are used to categorize the surface reactions that occur during radical deposition. Molecular dynamics (MD) simulations, using density functional theory (DFT-MD) via the SIESTA method and program, are used to corroborate the findings from the classical simulations and to categorize reactions that occur during cation deposition. Finally, reaction enthalpies are calculated with higher level quantum mechanical methods using a cluster model to verify and refine the predictions from the MD simulations. The multilevel analysis predicts that FC radicals add directly to the diamond (111) surface with the simultaneous formation of HF. In contrast, FC cations preferentially dissociate H from the surface leaving behind a cationic carbon site. Cations and radical species are found to prefer different reaction pathways, which limits the applicability of REBO. Furthermore, the comparison reveals a difference in the predicted reaction probabilities between REBO and DFT which is attributable to the short cut off distance for interaction in the current REBO formulation. 2010 Journal Article http://hdl.handle.net/20.500.11937/5318 10.1021/jp100667n American Chemical Society restricted
spellingShingle Devine, B.
Jang, I.
Kemper, T.
Lee, D.
Gale, Julian
Iordanova, N.
Simmott, S.
Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond
title Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond
title_full Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond
title_fullStr Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond
title_full_unstemmed Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond
title_short Multilevel Computational Analysis of Fluorocarbon Polyatomic Deposition on Diamond
title_sort multilevel computational analysis of fluorocarbon polyatomic deposition on diamond
url http://hdl.handle.net/20.500.11937/5318