Revisiting the Nonreactive Scattering of N<sub>2</sub> off W(100): On the Influence of the Scattering Azimuth on In-Plane Angular Distributions

Pétuya, Rémi; Plötz, Per-Arno; Larrégaray, P.

doi:10.1021/jp5016774

Cited by 10 publications

(20 citation statements)

References 32 publications

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“…for the hollow-parallel configuration, see Tables 4 and 5), are also reported in Table 8. [21], who looked at the non-reactive scattering of N 2 from a different tungsten surface (W(100)) and included dissipation to phonons using the GLO method.…”

Section: Energy Transfer To the Latticementioning

confidence: 99%

“…Tungsten surfaces, among others, have received much attention [2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21], with particular focus on the large crystallographic anisotropy that this metal exhibits with respect to nitrogen adsorption. For instance, the thermal reactivity of W(100) is about two orders of magnitude larger than the W(110) reactivity [2].…”

Section: Introductionmentioning

confidence: 99%

“…They found that the inclusion of phonon dissipative forces is more relevant than electronic ones, and suggested that the static surface electronically adiabatic calculations already include relevant aspects of the scattering dynamics. More recently, Petuya et al looked at the non-reactive scattering of N 2 from W(100) [21]. They modeled energy dissipation to phonons using the GLO method, and compared these results to static-surface data and to experiments, finding reasonable agreement between experimental data and both models.…”

Section: Introductionmentioning

confidence: 99%

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N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

Nattino

Costanzo

Kroes

2015

The Journal of Chemical Physics

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Accurately modeling the chemisorption dynamics of N 2 on metal surfaces is of both practical and fundamental interest. The factors that may have hampered this achievement so far are the lack of an accurate density functional and the use of approximate methods to deal with surface phonons and non-adiabatic effects. In the current work, the dissociation of molecular nitrogen on W(110) has been studied using ab initio molecular dynamics (AIMD) calculations, simulating both surface temperature effects, such as lattice distortion, and surface motion effects, like recoil. The forces were calculated using density functional theory, and two density functionals were tested, namely the PBE and the RPBE functionals. The computed dissociation probability considerably differs from earlier static surface results, with AIMD predicting a much larger contribution of the indirect reaction channel, in which molecules dissociate after being temporally trapped in the proximity of the surface. Calculations suggest that the surface motion effects play a role here, since the energy transfer to the lattice does not allow molecules that have been trapped into potential wells close to the surface to find their way back to the gas ⇤ Email: f.nattino@chem.leidenuniv.nl 1 phase. In comparison to experimental data, AIMD results overestimate the dissociation probability at the lowest energies investigated, where trapping dominates, suggesting a failure of both tested exchange-correlation functionals in describing the potential energy surface in the area sampled by trapped molecules.

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Section: Energy Transfer To the Latticementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

Nattino

Costanzo

Kroes

2015

The Journal of Chemical Physics

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“…At relatively low surface temperature and thermal energies of the beam, the sticking coefficient is roughly S ≈ 1 on W(100). [8][9][10] However, the dissociation probability is decreased by two orders of magnitude on W(110) for the same range of surface temperature and kinetic energies. 11,12 The variation 2 in the reactivity between the two tungsten faces is due to the contribution of dynamical effects at distances relatively far from the surface and not to specific features of the surface active sites in which the atoms are eventually adsorbed after dissociation.…”

Section: Introductionmentioning

confidence: 95%

Adsorption dynamics of molecular nitrogen at an Fe(111) surface

Nosir

Martin-Gondre

Bocan

et al. 2017

Phys. Chem. Chem. Phys.

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We present an extensive theoretical study of N adsorption mechanisms on an Fe(111) surface. We combine the static analysis of a six-dimensional potential energy surface (6D-PES), based on ab initio density functional theory (DFT) calculations for the system, with quasi-classical trajectory (QCT) calculations to simulate the adsorption dynamics. There are four molecular adsorption states, usually called γ, δ, α, and ε, arising from our DFT calculations. We find that N adsorption in the γ-state is non-activated, while the threshold energy is associated with the entrance channel for the other three adsorption states. Our QCT calculations confirm that there are activated and nonactivated paths for the adsorption of N on the Fe(111) surface, which is in agreement with previous experimental investigations. Molecular dynamics at a surface temperature T = 300 K and impact energies E in the 0-5 eV range show the relative occupancy of the γ, δ, α, and ε states. The δ-state, however, is only marginally populated despite its adsorption energy being very similar to that of the γ-state. Our QCT calculations trace the dependence of molecular trapping on the surface temperature T and initial impact energy E and quantify the rates of the different competitive channels that eventually lead to molecular adsorption.

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“…They showed that hydrogen prefers the TF position, in good agreement with other works based on DFT 20,21 . The penetration of hydrogen into the bulk via the W(100) 19,20,21 and W(110) 20,21,23,24 surfaces was also investigated by DFT, while the dissociation of molecular hydrogen was calculated via Molecular Dynamics (MD) calculations either based on DFT 25 or on model potentials 26,27 . However, in all cases, these works were conducted on a clean W surface, hence modeling a very low coverage; this is in contrast with real experimental conditions.…”

Section: Introductionmentioning

confidence: 99%

Saturation of tungsten surfaces with hydrogen: A density functional theory study complemented by low energy ion scattering and direct recoil spectroscopy data

Piazza¹,

Ajmalghan²,

Ferro³

et al. 2018

Acta Materialia

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Herein, we investigate the saturation limits of hydrogen on the (110) and (100) surfaces of tungsten via Density Functional Theory (DFT) and complement our findings with experimental measurements. We present a detailed study of the various stable configurations that hydrogen can adopt upon the surfaces at coverage ratios starting below 1.0, up to the point of their experimental coverage ratios, and beyond. Our findings allow us to estimate that the saturation limit on each surface exists with one monolayer of hydrogen atoms adsorbed. In the case of (110) this corresponds to a coverage ratio of one hydrogen atom per tungsten atom, while in the case of (100) a full monolayer is present at a coverage ratio of 2.0. Preliminary Low Energy Ion Scattering (LEIS) and Direct Recoil Spectroscopy (DRS)measurements complement these results and tend to confirm the findings obtained by DFT. In particular, the preferred adsorption sites on both surfaces at any coverage, the reconstruction of the (100) surface and the saturation limits agree well. We show that depending on the coverage, hydrogen surface binding energies can be of the same magnitude as binding energies to defects like vacancies. As a consequence, surface effects should be included in models aiming to simulate retention and desorption of hydrogen from the bulk.

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Revisiting the Nonreactive Scattering of N₂ off W(100): On the Influence of the Scattering Azimuth on In-Plane Angular Distributions

Cited by 10 publications

References 32 publications

N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

Adsorption dynamics of molecular nitrogen at an Fe(111) surface

Saturation of tungsten surfaces with hydrogen: A density functional theory study complemented by low energy ion scattering and direct recoil spectroscopy data

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Revisiting the Nonreactive Scattering of N2 off W(100): On the Influence of the Scattering Azimuth on In-Plane Angular Distributions

Cited by 10 publications

References 32 publications

N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

N2 dissociation on W(110): An ab initio molecular dynamics study on the effect of phonons

Adsorption dynamics of molecular nitrogen at an Fe(111) surface

Saturation of tungsten surfaces with hydrogen: A density functional theory study complemented by low energy ion scattering and direct recoil spectroscopy data

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Product

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Revisiting the Nonreactive Scattering of N₂ off W(100): On the Influence of the Scattering Azimuth on In-Plane Angular Distributions