Reactive scattering of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>from metal surfaces under fast-grazing-incidence conditions

Dı́az, Cristina; Martín, Fernando

doi:10.1103/physreva.82.012901

Cited by 11 publications

(7 citation statements)

References 56 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…44, this behavior has been observed for a variety of H 2 /metal surface systems, 243 from the activated to non-activated ones. Furthermore, these classical theoretical simulations have shown that the probability of dissociative scattering (the channel that is complementary to molecular reflectivity in fast grazing incidence (FGI) experiments) as a function of E n has a large resemblance to the dissociative adsorption probability obtained for thermal (and slightly above) energies at normal incidence.…”

Section: View Article Onlinementioning

confidence: 73%

“…Interesting predictions from the diffraction studies are that RID peaks should be larger than elastic diffraction peaks, 242 and that energy transfer to an intramolecular mode should be enhanced if the classical frequency corresponding to a specific rovibrational state is close to a nonlinear resonance condition. 243 This implies that experiments on dissociative scattering at FGI could be used to determine saturation values of dissociative chemisorption probabilities of highly activated systems like H 2 + Cu(111), Ag (111), and Au (111), which are not accessible in ordinary molecular beam experiments. 243 This implies that experiments on dissociative scattering at FGI could be used to determine saturation values of dissociative chemisorption probabilities of highly activated systems like H 2 + Cu(111), Ag (111), and Au (111), which are not accessible in ordinary molecular beam experiments.…”

Section: Discussionmentioning

confidence: 99%

“…The ''gold standard'' in methods for fitting or interpolating PESs for diatomic molecules scattering from metal surfaces, which has been used the most 11,48,53,54,56,109,114,116,128,129,131,133,145,148,151,156,161,170,174,176,181,[183][184][185][186]188,[192][193][194][195][196][197]199,200,208,216,217,[242][243][244][245][246][247][248][249] in studies of H 2 -metal surface scattering that appeared over the last decade, is the corrugation reducing procedure (or the CRP method) developed by Busnengo et al 27 and extended by Olsen et al 250 The CRP method performs so well because it takes ...…”

Section: Potential Surface Fittingmentioning

confidence: 99%

See 2 more Smart Citations

Quantum and classical dynamics of reactive scattering of H₂ from metal surfaces

2016

View full text Add to dashboard Cite

We review the state-of-the art in dynamics calculations on the reactive scattering of H2 from metal surfaces, which is an important model system of an elementary reaction that is relevant to heterogeneous catalysis. In many applications, quantum dynamics and classical trajectory calculations are performed within the Born-Oppenheimer static surface model. However, ab initio molecular dynamics (AIMD) is finding increased use in applications aimed at modeling the effect of surface phonons on the dynamics. Molecular dynamics with electronic friction has been used to model the effect of electron-hole pair excitation. Most applications are still based on potential energy surfaces (PESs) or forces computed with density functional theory (DFT), using a density functional within the generalized gradient approximation to the exchange-correlation energy. A new development is the use of a semi-empirical version of DFT (the specific reaction parameter (SRP) approach to DFT). We also discuss the accurate methods that have become available to represent electronic structure data for the molecule-surface interaction in global PESs. It has now become possible to describe highly activated H2 + metal surface reactions with chemical accuracy using the SRP-DFT approach, as has been shown for H2 + Cu(111) and Cu(100). However, chemical accuracy with SRP-DFT has yet to be demonstrated for weakly activated systems like H2 + Ru(0001) and non-activated systems like H2 + Pd(111), for which SRP DFs are not yet available. There is now considerable evidence that electron-hole pair (ehp) excitation does not need to be modeled to achieve the (chemically) accurate calculation of dissociative chemisorption and scattering probabilities. Dynamics calculations show that phonons can be safely neglected in the chemically accurate calculation of sticking probabilities on cold metal surfaces for activated systems, and in the calculation of a number of other observables. However, there is now sufficient evidence to suggest that the decision on whether or not to neglect phonons should be taken with care, with appropriate consideration of the observable to be computed and of the relevant surface temperature. AIMD calculations have provided valuable insights into the mechanisms that are operative in the dissociative adsorption and absorption of hydrogen on/in precovered metal surfaces. Classical and quantum dynamics calculations have shown that the reaction probability of H2 on Pt surfaces consisting of (100) steps and (111) terraces can to a very good approximation be computed as a weighted average of the reactivities on the steps and terraces. Progress obtained with dynamics calculations on the scattering of H2 from alloys and from simple low index metal surfaces is also reported. Insights that may be obtained on the reactivity of a metal surface from the prominent presence of out-of-plane diffraction or, conversely, the complete absence of diffraction, are discussed. A new field has been opened up by experiments on H2 scattering from surfaces at fast graz...

show abstract

Section: View Article Onlinementioning

confidence: 73%

Section: Discussionmentioning

confidence: 99%

Section: Potential Surface Fittingmentioning

confidence: 99%

See 1 more Smart Citation

Quantum and classical dynamics of reactive scattering of H₂ from metal surfaces

2016

View full text Add to dashboard Cite

show abstract

“…As already discussed in the literature [2,8,11,12], the physical mechanism behind this phenomenon is the strong decoupling between the fast motion parallel to the surface, and the slow motion normal to it. Due to the grazing incidence conditions, the potential felt by the projectile is periodic (or quasi-periodic).…”

Section: Introductionmentioning

confidence: 93%

Scattering of H(D) from LiF(100) under fast grazing incidence conditions: To what extent is classical dynamics a useful tool?

Muzas

Martín

Dı́az

2015

Nuclear Instruments and Methods in Physics Research Section B:

Self Cite

View full text Add to dashboard Cite

“…Beyond diffraction simulations, classical dynamics can also be used to study reactive scattering under fast grazing-incidence conditions. 197–199 These scattering simulations have shown that it is possible to determine sticking probabilities at thermal and quasi-thermal energies, from the threshold up to the saturation limit, by analysing molecular scattering under fast grazing incidence. Under these extreme conditions a molecule behaves much as it does under normal incidence and low incidence energy; that is, it can be reflected or dissociated.…”

Section: Grazing Incidence Fast Molecule Diffraction (Gifmd)mentioning

confidence: 99%