Six-Dimensional Quantum Dynamics of Adsorption and Desorption of H_2 at Pd(100): No Need for a Molecular Precursor Adsorption State

We report six-dimensional quantum dynamical calculations of dissociative adsorption and associative desorption of the system H_2/Pd(100) using an ab-initio potential energy surface. We focus on rotational effects in the steering mechanism, which is responsible for the initial decrease of the sticking probability with kinetic energy. In addition, steric effects are briefly discussed.Comment: RevTeX, 11 pages, 4 figure

Potential Energy Surface for H_2 Dissociation over Pd(100)

The potential energy surface (PES) of dissociative adsorption of H_2 on Pd(100) is investigated using density functional theory and the full-potential linear augmented plane wave (FP-LAPW) method. Several dissociation pathways are identified which have a vanishing energy barrier. A pronounced dependence of the potential energy on ``cartwheel'' rotations of the molecular axis is found. The calculated PES shows no indication of the presence of a precursor state in front of the surface. Both results indicate that steering effects determine the observed decrease of the sticking coefficient at low energies of the H_2 molecules. We show that the topology of the PES is related to the dependence of the covalent H(s)-Pd(d) interactions on the orientation of the H_2 molecule.Comment: RevTeX, 8 pages, 5 figures in uufiles forma

Dynamical Quantum Processes of Molecular Beams at Surfaces: Dissociative Adsorption of Hydrogen on Metal Surfaces

Due to the improvement of computer power and the development of efficient algorithms it is now possible to combine high-dimensional quantum dynamical calculations of the dissociative adsorption of molecular beams with reliable ab-initio potential energy surfaces (PES). In this brief review two recent examples of such studies of the systems H_2/Cu(111), where adsorption is hindered by a noticeable energy barrier, and H_2/Pd(100), where activated as well as non-activated paths to adsorption exist, are presented. The effect of lateral surface corrugations on the sticking probability in the tunneling and the classical regime and the role of additional parallel momentum are discussed in the context of the H_2/Cu(111) results. For the system H_2/Pd(100) it is shown that the initial decrease of the sticking probability with increasing kinetic energy, which is usually attributed to a precursor mechanism, can be explained by dynamical steering. In addition, the influence of rotation on the adsorption and desorption dynamics is examined.Comment: RevTeX, 22 pages, 6 figure

Ab initio Quantum and ab initio Molecular Dynamics of the Dissociative Adsorption of Hydrogen on Pd(100)

The dissociative adsorption of hydrogen on Pd(100) has been studied by ab initio quantum dynamics and ab initio molecular dynamics calculations. Treating all hydrogen degrees of freedom as dynamical coordinates implies a high dimensionality and requires statistical averages over thousands of trajectories. An efficient and accurate treatment of such extensive statistics is achieved in two steps: In a first step we evaluate the ab initio potential energy surface (PES) and determine an analytical representation. Then, in an independent second step dynamical calculations are performed on the analytical representation of the PES. Thus the dissociation dynamics is investigated without any crucial assumption except for the Born-Oppenheimer approximation which is anyhow employed when density-functional theory calculations are performed. The ab initio molecular dynamics is compared to detailed quantum dynamical calculations on exactly the same ab initio PES. The occurence of quantum oscillations in the sticking probability as a function of kinetic energy is addressed. They turn out to be very sensitive to the symmetry of the initial conditions. At low kinetic energies sticking is dominated by the steering effect which is illustrated using classical trajectories. The steering effects depends on the kinetic energy, but not on the mass of the molecules. Zero-point effects lead to strong differences between quantum and classical calculations of the sticking probability. The dependence of the sticking probability on the angle of incidence is analysed; it is found to be in good agreement with experimental data. The results show that the determination of the potential energy surface combined with high-dimensional dynamical calculations, in which all relevant degrees of freedon are taken into account, leads to a detailed understanding of the dissociation dynamics of hydrogen at a transition metal surface.Comment: 15 pages, 9 figures, subm. to Phys. Rev.

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Study of tantalum and iridium as adhesion layers for Pt/LGS high temperature SAW devices

International audienceIn this paper, we report on the use of tantalum and iridium as adhesion layers for platinum electrodes used in high temperature SAW devices based on langasite substrates (LGS). Unlike iridium, tantalum exhibits a great adhesive strength, and a very low mobility through the Pt film, ensuring a device lifetime of at least half an hour at 1000°C. The latter is limited by morphological modifications of platinum, starting by the apparition of crystallites on the surface, and followed by important terracing and breaking of the film continuity. SNMS and XRD measurements allowed us to show that these phenomena are likely intrinsic to platinum film, whatever be the nature of the adhesion layer. Finally, after having outlined a possible scenario leading to this deterioration, we consider some solutions that could replace platinum in order to increase the lifetime of LGS-based SAW devices in high temperatures conditions

Emmanuel Leclainche (1861-1953)

Alnot Laure, Lucas Jean, Dhennin Louis, Catsaras Marc. Emmanuel Leclainche (1861-1953). In: Bulletin de l'Académie Vétérinaire de France tome 151 n°2, 1998. pp. 197-203