N atoms recombination on a silica surface: A global theoretical approach

Rutigliano, M.; Pieretti, Andrea; Cacciatore, M.; Sanna, Nico; Barone, Vincenzo

doi:10.1016/j.susc.2005.12.080

Cited by 41 publications

(50 citation statements)

References 20 publications

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“…In turn, a fully classical description of the collisional pathways without any quantummechanics refinement of the N, O, N 2 , and O 2 interactions with silica polymorphs should be considered, at least in principle, as affected by such a limitation during the attachment to the surface of the adsorbant. 6 In this contribution, inspired by the above computational evidence, 6,7 we have addressed the O and O 2 interaction potentials with an on top silicon atom and its nearest oxygen both localized over predefined β-quartz surface models cleaved from the unit cell as reported in ref 12 (Figure 1). To this end, and for a direct comparison with previous data obtained for β-cristobalite, we used the hybrid PBE0 functional 13 based on Perdew−Burke−Erzenrhof exchange−correlation functionals 14 in which a portion of Hartree−Fock exchange is added selfconsistently to the DFT (PBE) contribution.…”

Section: Interaction Potentials Of O and O 2 Overmentioning

confidence: 99%

Oxygen Adsorption on β-Quartz Model Surfaces: Some Insights from Density Functional Theory Calculations and Semiclassical Time-Dependent Dynamics

et al. 2012

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The O/β-quartz interaction is described by combining our time-dependent semiclassical approach to atom-molecule/surface scattering with first-principles electronic structure calculations at the DFT (PBE0) level of accuracy. In particular, the O, O(2) interaction potentials with an on-top Si atom and its nearest O atom both localized over three different silica clusters have been calculated as a function of the oxygen-silica approaching distance. The calculated DFT potential energy surface has been used in semiclassical trajectory calculations to investigate the sticking and inelastic reflection of oxygen atoms from a model β-quartz surface. The collisional mechanism, including the role played by the phonon dynamics, is brought to light and accurate sticking probabilities are calculated at five impact energies in the range [0.05-0.8] eV and T(S) = 1000 K. The different catalytic response of β-quartz and β-cristobobalite to the atomic oxygen flux is also discussed and highlighted.

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Section: Interaction Potentials Of O and O 2 Overmentioning

confidence: 99%

Oxygen Adsorption on β-Quartz Model Surfaces: Some Insights from Density Functional Theory Calculations and Semiclassical Time-Dependent Dynamics

et al. 2012

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“…The calculations were performed within the size-scaled cluster approach [11,12]. Spin polarized wave functions were used as basis sets.…”

Section: (Some) Cases Studiedmentioning

confidence: 99%

Molecular Dynamics Studies on Fundamental Molecular Surface Processes

Cacciatore

Rutigliano

2011

AIP Conference Proceedings

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Abstract. In this contribution, we give examples of results recently obtained in fundamental molecular dynamics studies and DFT electronic structure calculations performed on prototype surface processes due to the interaction of atomic and molecular oxygen, nitrogen, hydrogen, C on substrates of different nature. The discussed systems are known to be among the most important heterogeneous systems relevant to laboratory and natural gas-surface systems. The surface processes followed in the MD simulations include atom recombination reactions, dissociative chemisorption, adsorption and adsorption/desorption of atoms and molecules. Correlations between the dynamics of the surface processes and the molecular properties of the gas-phase particles and the structural behaviours of the surfaces will be highlighted. GENERAL CONSIDERATIONSThe chemi and physisorption of atoms and molecules on solid surfaces can lead to a large number of chemicophysical processes of great interest in many important research fields both from a fundamental and technological point of view: material science and plasma-chemical processes, aerothermodynamics, interstellar chemistry and others. Among the many possible molecular processes active at surfaces, we mention the direct and indirect inelastic scattering (desorption and adsorption/desorption processes), sticking, chemical reactions, charge transfer and charge neutralization, formation of volatile surface radicals. Each of these processes is active in a specific range of collisional energies according to the behaviours of the surfaces involved in the interaction. The data needed in kinetic modeling of the chemistry at the gas-surface interlayer, as for example in kinetic Monte Carlo simulation, are: state-selected and global recombination coefficients, state-to-state dissociation probabilities, distributions in angles and energies of the scattered particles, energy accommodation coefficient, diffusion coefficients etc. Of key importance is the dependence of the collisional coefficients on the surface parameters ( surface site and surface structure, corrugation, surface contamination), and on the molecular parameters of the gas-phase particles hitting the surface (translational and internal energy content, incident angles). Unfortunately, contrary to gas-phase processes where large database of state-to-state rate constants and cross-sections are available[see for example [1,2], the collisional data for heterogeneous processes needed by the plasma-chemistry and plasma-physics community are rather sparse.In this contribution we focus on two classes of heterogeneous processes: inelastic direct desorption and indirect adsorption-desorption, and molecule formation after atom recombination at surfaces. Special attention is given to the latter reactive process. This reaction can be both an important channel for surface atom abstraction and an effective source of energetically activated molecules. Recombination reactions can follow three basic mechanisms.According to the Langmuir-Hinshelwood (L-H) m...

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“…Time‐dependent semiclassical collision method, modeling the heterogeneous recombination process via E–R mechanism, has been applied to the study of the N 2 formation on a silica surface, using an accurate DFT PES for the β ‐cristobalite crystalline structure, which is the stable phase at T = 1 000 K 80…”

Section: N2mentioning

confidence: 99%

“… Vibrational population distribution of N 2 molecules formed by atomic recombination on a silica surface at temperature T S = 1 000 K and kinetic energy E kin = 0.055 eV 80…”

Section: N2mentioning

confidence: 99%

Molecular Dynamics for State‐to‐State Kinetics of Non‐Equilibrium Molecular Plasmas: State of Art and Perspectives

Capitelli

Celiberto

Esposito

et al. 2009

Plasma Processes & Polymers

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The theoretical prediction of molecular plasma features in non‐equilibrium conditions relys on the knowledge of the microscopic collisional dynamics. The state‐to‐state kinetic approach in fact requires complete sets of cross‐sections for the main reaction channels, including their dependence on the internal degrees of freedom. In this paper, the main three classes (electron–molecule, atom–molecule, and gas–surface interaction) of elementary processes have been considered, reviewing old and recent results for hydrogen, oxygen, and nitrogen molecular plasmas. Within each class selected processes have been discussed, summarizing the evidences of theoretical investigation and validating different methods by comparison with available experiments. Future achievements are outlined moving to polyatomic systems, of great interest in many technological plasma‐chemical systems.

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N atoms recombination on a silica surface: A global theoretical approach

Cited by 41 publications

References 20 publications

Oxygen Adsorption on β-Quartz Model Surfaces: Some Insights from Density Functional Theory Calculations and Semiclassical Time-Dependent Dynamics

Oxygen Adsorption on β-Quartz Model Surfaces: Some Insights from Density Functional Theory Calculations and Semiclassical Time-Dependent Dynamics

Molecular Dynamics Studies on Fundamental Molecular Surface Processes

Molecular Dynamics for State‐to‐State Kinetics of Non‐Equilibrium Molecular Plasmas: State of Art and Perspectives

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