State resolved inelastic scattering of N2 from Ru(0001)

Mortensen, H.; Jensen, E. T.; Diekhöner, Lars; Baurichter, A.; Luntz, A. C.; Petrunin, V. V.

doi:10.1063/1.1575210

Cited by 37 publications

(52 citation statements)

References 51 publications

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“…As it was shown in Refs. 30 and 31, these theoretical results reproduce the surprisingly low dissociation probabilities [27,[50][51][52] found in the experiments. The results can be understood based on the very special characteristics of the N 2 /Ru(0001) PES: [28,30,31,51] The minimum barrier is very high, around 2.3 eV, and the PES displays high anisotropy and corrugation, i.e., small changes in the orientation and/or the position of the molecule gives rise to large changes in the potential energy (see Fig.…”

Section: A 6d Dynamics and The Vibrational Efficacysupporting

confidence: 79%

A note on the vibrational efficacy in molecule-surface reactions

Dı́az¹,

Olsen²

2009

The Journal of Chemical Physics

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The effectiveness of vibrational energy in promoting dissociation of molecules colliding with surfaces can be measured through the so-called vibrational efficacy. It is by many thought to be a pure "energetic" measure and therefore believed to be limited from below by zero (in the case that there is no increase in dissociation probability upon vibrational excitation) and from above by one (in the case that all of the vibrational excitation energy is used to promote reaction).However, the quantity vibrational efficacy is clearly linked to the detailed dynamics of the system, and straightforward considerations lead to the conclusion that it is not limited either from below or above. Here we discuss these considerations together with a quasi-classical dynamics study of a molecule-surface system, N 2 /Ru(0001), for which a vibrational efficacy bigger than one has been found both experimentally and theoretically. We show that an analysis of the vibrational efficacy only in terms of energy transfer from vibration to translation can be too simple to describe the behavior of systems for which the potential energy surfaces present (high) reaction barriers, potential corrugation and anisotropy, and curved reaction paths.

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Section: A 6d Dynamics and The Vibrational Efficacysupporting

confidence: 79%

A note on the vibrational efficacy in molecule-surface reactions

Dı́az¹,

Olsen²

2009

The Journal of Chemical Physics

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“…Previous studies of rare-gas and diatomic molecular scattering from clean Ru(0001) have revealed a large effective mass. An analysis of the energy-resolved spectra of Ar scattering from Ru(0001) [42,43] as well as scattering of N 2 molecules from similar Ru(0001) [44,45] gave for both projectile particles an effective mass of approximately 2.5 Ru atoms. Based on the analysis of those two systems it was proposed that the Ru(0001) surface would present a large effective mass for the scattering of all the rare gases and even for other projectiles [46].…”

Section: Surface Effective Masses From Ar Scatteringmentioning

confidence: 99%

Probing interlayer interactions between graphene and metal substrates by supersonic rare-gas atom scattering

et al. 2015

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We demonstrate that highly surface-sensitive supersonic rare-gas (He, Ar, and Xe) atom scattering, in both the quantum and classical regimes, can probe and quantify the interlayer interactions between graphene monolayers and metal substrates in terms of the Debye temperature corresponding to the surface normal vibration, and the surface effective mass. As models of the strongly and weakly interacting graphene, we investigated two systems, graphene on Ru(0001) and Pt (111), respectively. The experimental data for Ar and Xe are compared with the results from theoretical simulations based on the classical smooth surface model. For gr/Pt(111) we find that the scattering pattern of the rare-gas beam, including the Debye-Waller attenuation of the He beam, are quite similar to that from highly oriented pyrolytic graphite (HOPG); this suggests that the graphene-Pt (111) interaction is much like a van der Waals interaction. On the contrary, for the gr/Ru(0001) system, we find a smaller Debye-Waller attenuation and a larger surface effective mass, indicating that graphene on Ru(0001) is tightly bonded to the substrate. Furthermore, asymmetrical spectral shapes in the Ar and Xe scattering spectra from gr/Ru(0001) are interpreted as a result of the lateral distribution of the interlayer interaction corresponding to the moiré pattern. It is found that the "valley" region of the moiré pattern has high effective mass reflecting stronger bonding to the substrate, contributing to the high reflectivity of the He beam reported for this system. On the other hand, the effective mass of the "hill" region is found to be similar to that of HOPG, indicating that this region is well decoupled from the substrate. These results demonstrate a unique capability of atom scattering to probe and evaluate the molecule-substrate interaction and its spatial distributions.

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“…6 No isotope effect has been observed in the classical regime ͑E i ജ V * ͒, but for lower energies the reaction probability for 15 N 2 is smaller than for 14 N 2 , which has been interpreted in terms of tunneling through a large barrier for dissociation. 6 Another unexpected feature is the lack of vibrational excitation in molecularbeam experiments for N 2 scattering from Ru͑0001͒, 13 and the small amount of vibrational excitation observed in laser assisted associative desorption ͑LAAD͒, 11 associative desorption being the reverse process to dissociative chemisorption. Late barrier systems ͑reaction barrier found for an extended vibrational coordinate͒ are expected to exhibit significant vibrational excitation of the molecule upon scat-tering and associative desorption.…”

Section: Introductionmentioning

confidence: 99%

“…As a consequence of this interest a large number of experimental [1][2][3][4][5][6][7][8][9][10][11][12][13] and theoretical 5,11,14 studies have been published, showing unusual and sometimes controversial results. Although recent theoretical and experimental work [15][16][17] has proved that dissociation at Ru steps is much more efficient than at the Ru͑0001͒ terraces, N 2 /Ru͑0001͒ is of much fundamental interest.…”

Section: Introductionmentioning

confidence: 99%

Reactive and nonreactive scattering of N2 from Ru(0001): A six-dimensional adiabatic study

Dı́az

Vincent

Krishnamohan

et al. 2006

The Journal of Chemical Physics

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). Reactive and nonreactive scattering of N-2 from Ru(0001): A six-dimensional adiabatic study. Journal of Chemical Physics, 125(11), 114706. DOI: 10.1063/1.2229197 Reactive and nonreactive scattering of N 2 from Ru"0001…: A six-dimensional adiabatic study We have studied the dissociative chemisorption and scattering of N 2 on and from Ru͑0001͒, using a six-dimensional quasiclassical trajectory method. The potential energy surface, which depends on all the molecular degrees of freedom, has been built applying a modified Shepard interpolation method to a data set of results from density functional theory, employing the RPBE generalized gradient approximation. The frozen surface and Born-Oppenheimer ͓Ann. Phys. ͑Leipzig͒ 84, 457 ͑1927͔͒ approximations were used, neglecting phonons and electron-hole pair excitations. Dissociative chemisorption probabilities are found to be very small even for translational energies much higher than the minimum reaction barrier, in good agreement with experiment. A comparison to previous low dimensional calculations shows the importance of taking into account the multidimensional effects of N 2 rotation and translation parallel to the surface.

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State resolved inelastic scattering of N2 from Ru(0001)

Cited by 37 publications

References 51 publications

A note on the vibrational efficacy in molecule-surface reactions

A note on the vibrational efficacy in molecule-surface reactions

Probing interlayer interactions between graphene and metal substrates by supersonic rare-gas atom scattering

Reactive and nonreactive scattering of N2 from Ru(0001): A six-dimensional adiabatic study

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