Competition between electron and phonon excitations in the scattering of nitrogen atoms and molecules off tungsten and silver surfaces

We investigate the role played by electron-hole pair and phonon excitations in the interaction of reactive gas molecules and atoms with metal surfaces. We present a theoretical framework that allows us to evaluate within a full-dimensional dynamics the combined contribution of both excitation mechanisms while the gas particle-surface interaction is described by an ab-initio potential energy surface. The model is applied to study energy dissipation in the scattering of N$_2$ on W(110) and N on Ag(111). Our results show that phonon excitation is the dominant energy loss channel whereas electron-hole pair excitations represent a minor contribution. We substantiate that, even when the energy dissipated is quantitatively significant, important aspects of the scattering dynamics are well captured by the adiabatic approximation.Comment: 4pages and 3 figure

Non-equilibrium Anisotropic Phases, Nucleation and Critical Behavior in a Driven Lennard-Jones Fluid

We describe short-time kinetic and steady-state properties of the non--equilibrium phases, namely, solid, liquid and gas anisotropic phases in a driven Lennard-Jones fluid. This is a computationally-convenient two-dimensional model which exhibits a net current and striped structures at low temperature, thus resembling many situations in nature. We here focus on both critical behavior and details of the nucleation process. In spite of the anisotropy of the late--time spinodal decomposition process, earlier nucleation seems to proceed by Smoluchowski coagulation and Ostwald ripening, which are known to account for nucleation in equilibrium, isotropic lattice systems and actual fluids. On the other hand, a detailed analysis of the system critical behavior rises some intriguing questions on the role of symmetries; this concerns the computer and field-theoretical modeling of non-equilibrium fluids.Comment: 7 pages, 9 ps figures, to appear in PR

Development of Suitable CuO-Based Materials Supported on Al2O3, MgAl2O4, and ZrO2 for Ca/Cu H2 Production Process

Functional materials for the sorption enhanced reforming process for H2 production coupled to a Cu/CuO chemical loop have been synthesized. The performance of CuO-based materials supported on Al2O3, MgAl2O4, and ZrO2 and synthesized by different routes has been analyzed. Highly stable materials supported on Al2O3 or MgAl2O4 synthesized by coprecipitation and mechanical mixing with sufficient Cu loads (around 65% wt) have been successfully developed. However, it has been found that coprecipitation under these conditions is not a suitable route for ZrO2. Spray-drying and deposition precipitation did not provide the best chemical features to the materials. As the Ca/Cu process is operated in fixed bed reactors, the best candidates were pelletized and their stability was again assessed. Pellets with high chemical and mechanical stability, high oxygen transport capacity, and good mechanical properties have been finally obtained by coprecipitation. The good homogeneity that provides this route would allow an easy scaling up

Density functional theory calculations of nitrogen adsorption features on Fe(111) surfaces

Trabajo presentado al Workshop on Controlled Atomic Dynamics on Solid Surfaces: Atom an Molecular Manipulation, celebrado en Donostia-San sebastián (España) del 13 al 16 de Mayo de 2013.The interaction of nitrogen with metal surfaces has been one of the most popular topics of research in surface science for the last decades. This is due in part to the industrial importance of ammonia synthesis, typically obtained from nitrogen and hydrogen catalyzed over iron-based compounds. The rate limiting step in ammonia synthesis is the adsorption and dissociation of nitrogen on the catalyst surface. In Fe surfaces, the reactivity of the process depends on the face, the Fe(111) and Fe(211) surfaces being the most reactive ones. Although Fe(111) is the most reactive iron face for N2 dissociation, the dynamics of such process has not been analyzed in detail. In this work we present exhaustive calculations of the interaction of nitrogen atoms and molecules with the Fe(111) surface. These calculations set the basis for subsequent analysis of the N2 dissociation dynamics. We perform Density functional Theory spin-polarized calculations using VASP code. We first study the relaxation of the Fe(111) surface, which was a matter of controversy in the past. From here, we calculate the interaction energy of nitrogen atoms and molecules when approaching the Fe(111) surface. Our results show the preferred adsorption paths and sites for nitrogen adsorption, as well as the adsorption energies. We finally discuss the dynamics of the dissociation process and make the link with the high reactivity properties of the surface.Peer reviewe

SUPG-based stabilization using a separated representations approach

We have developed a new method for the construction of Streamline Upwind Petrov Galerkin (SUPG) stabilization techniques for the resolution of convection-diffusion equations based on the use of separated representations inside the Proper Generalized Decompositions (PGD) framework. The use of SUPG schemes produces a consistent stabilization adding a parameter to all the terms of the equation (not only the convective one). SUPG obtains an exact solution for problems in 1D, nevertheless, a generalization does not exist for elements of high order or for any system of convection-diffusion equations. We introduce in this paper a method that achieves stabilization in the context of Proper Generalzied Decomposition (PGD). This class of approximations use a representation of the solution by means of the sum of a finite number of terms of separable functions. Thus it is possible to use the technique of separation of variables in the context of problems of convection-diffusion that will lead to a sequence of problems in 1D where the parameter of stabilization is well known.Postprint (published version