Molecular trapping in the dissociation dynamics of N2 on W(110)

Corriol, C.; Darling, George R.

doi:10.1016/j.susc.2004.03.039

Cited by 8 publications

(7 citation statements)

References 31 publications

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“…We have carefully checked that no barrier in the entrance channel is found at large distances from the surface, in opposition to the calculations of Ref. [23]. We find a precursor well of roughly E c 705 meV at Z 2:6…”

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confidence: 67%

WhyN2Molecules with Thermal Energy Abundantly Dissociate on W(100) and Not on W(110)

et al. 2006

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Low-energy N2 molecules easily dissociate on W(100) but not on W(110). In this Letter, the six-dimensional potential energy surface for the dissociation of N2 molecules on W(110) has been determined by density functional calculations. Results are compared to those of N2 dissociation on W(100). The difference in reactivity between the two faces is shown to arise from the characteristics of the potential energy surface far from the surface (>3 A) and not from the properties of a precursor well or those of the final atomic adsorption sites.

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confidence: 67%

WhyN2Molecules with Thermal Energy Abundantly Dissociate on W(100) and Not on W(110)

et al. 2006

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“…The dissociation of nitrogen on metals is relevant as a model system for heterogeneous catalysis, as the N 2 dissociative adsorption on an iron catalyst is believed to be the rate limiting step of the industrial ammonia synthesis (Haber-Bosch) process 25 . However, in spite of the large number of experimental [26][27][28][29][30][31][32][33] and theoretical 24,[34][35][36][37][38][39][40][41][42][43][44][45][46][47][48] studies that investigated this reaction, an accurate description of the dissociative chemisorption of nitrogen on tungsten surfaces is still lacking 1 . Two dissociation channels have been found for this system 24,38,41,47 .…”

Section: Introductionmentioning

confidence: 99%

Modeling surface motion effects in N2 dissociation on W(110): Ab initio molecular dynamics calculations and generalized Langevin oscillator model

Nattino

Galparsoro

Costanzo

et al. 2016

The Journal of Chemical Physics

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Accurately modeling surface temperature and surface motion e↵ects is necessary to study molecule-surface reactions in which the energy dissipation to surface phonons can largely a↵ect the observables of interest. We present here a critical comparison of two methods that allow to model such e↵ects, namely the ab initio molecular dynamics (AIMD) method and the generalized Langevin oscillator (GLO) model, using the dissociation of N 2 on W(110) as a benchmark. AIMD is highly accurate as the surface atoms are explicitly part of the dynamics, but this advantage comes with a large computational cost. The GLO model is much more computationally convenient, but accounts for lattice motion e↵ects in a very approximate way. Results show that, despite its simplicity, the GLO model is able to capture the physics of the system to a large extent, returning dissociation probabilities which are in better agreement with AIMD than static-surface results. Furthermore, the GLO model and the AIMD method predict very similar energy transfer to the lattice degrees of freedom in the non-reactive events, and similar dissociation dynamics. a) These authors contributed equally to this work.

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“…The improvement of ab initio methods over the last few years has allowed to obtain detailed adiabatic PESs. Recent calculations based on density functional theory 11 ͑DFT͒ examine the dissociation in the N 2 /W͑110͒ system for initial kinetic energies in the range of 0.4-1.2 eV. According to the authors the dissociation would be indirect, i.e., dominated by molecular trapping.…”

Section: Introductionmentioning

confidence: 99%

Low sticking probability in the nonactivated dissociation of N2 molecules on W(110)

Alducin

Muiño

Busnengo

et al. 2006

The Journal of Chemical Physics

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The six-dimensional potential energy surface for the dissociation of N 2 molecules on the W͑110͒ surface has been determined by density functional calculations and interpolated using the corrugation reducing procedure. Examination of the resulting six-dimensional potential energy surface shows that nonactivated paths are available for dissociation. In spite of this, the dissociation probability goes to a very small value when the impact energy goes to zero and increases with increasing energy, a behavior usually associated with activated systems. Statistics on the dynamics indicate that this unconventional result is a consequence of the characteristics of the potential energy surface at long distances. Furthermore, two distinct channels are identified in the dissociation process, namely, a direct one and an indirect one. The former is responsible for dissociation at high energies. The latter, which includes long-lasting dynamic trapping in the vicinity of a potential well above the W top position, is the leading mechanism at low and intermediate energies.

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Molecular trapping in the dissociation dynamics of N2 on W(110)

Cited by 8 publications

References 31 publications

WhyN2Molecules with Thermal Energy Abundantly Dissociate on W(100) and Not on W(110)

WhyN2Molecules with Thermal Energy Abundantly Dissociate on W(100) and Not on W(110)

Modeling surface motion effects in N2 dissociation on W(110): Ab initio molecular dynamics calculations and generalized Langevin oscillator model

Low sticking probability in the nonactivated dissociation of N2 molecules on W(110)

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