Multilevel computational analysis of fluorocarbon polyatomic deposition on diamond

Bryce Devine, Inkook Jang, Travis Kemper, Donghwa Lee, Julian D. Gale, Nedialka Iordanova, Susan B. Sinnott

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

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 cutoff distance for interaction in the current REBO formulation.

Original languageEnglish (US)
Pages (from-to)12535-12544
Number of pages10
JournalJournal of Physical Chemistry C
Volume114
Issue number29
DOIs
StatePublished - Jul 29 2010

Fingerprint

Fluorocarbons
Diamond
fluorocarbons
Molecular dynamics
Diamonds
diamonds
molecular dynamics
Cations
Positive ions
cations
Discrete Fourier transforms
Computer simulation
simulation
Surface reactions
surface reactions
Density functional theory
Enthalpy
cut-off
Carbon
enthalpy

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Devine, Bryce ; Jang, Inkook ; Kemper, Travis ; Lee, Donghwa ; Gale, Julian D. ; Iordanova, Nedialka ; Sinnott, Susan B. / Multilevel computational analysis of fluorocarbon polyatomic deposition on diamond. In: Journal of Physical Chemistry C. 2010 ; Vol. 114, No. 29. pp. 12535-12544.
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Devine, B, Jang, I, Kemper, T, Lee, D, Gale, JD, Iordanova, N & Sinnott, SB 2010, 'Multilevel computational analysis of fluorocarbon polyatomic deposition on diamond', Journal of Physical Chemistry C, vol. 114, no. 29, pp. 12535-12544. https://doi.org/10.1021/jp100667n

Multilevel computational analysis of fluorocarbon polyatomic deposition on diamond. / Devine, Bryce; Jang, Inkook; Kemper, Travis; Lee, Donghwa; Gale, Julian D.; Iordanova, Nedialka; Sinnott, Susan B.

In: Journal of Physical Chemistry C, Vol. 114, No. 29, 29.07.2010, p. 12535-12544.

Research output: Contribution to journalArticle

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AU - Sinnott, Susan B.

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Devine B, Jang I, Kemper T, Lee D, Gale JD, Iordanova N et al. Multilevel computational analysis of fluorocarbon polyatomic deposition on diamond. Journal of Physical Chemistry C. 2010 Jul 29;114(29):12535-12544. https://doi.org/10.1021/jp100667n