Reactive and nonreactive scattering of N-2 from Ru(0001): A six-dimensional adiabatic study

C. Diaz, J.K. Vincent, G.P. Krishnamohan, R.A. Olsen, G.J. Kroes, Johanna Karoliina Honkala, Jens Kehlet Nørskov

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Abstract

We have studied the dissociative chemisorption and scattering of N-2 on and from Ru(0001), 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. (Leipzig) 84, 457 (1927)] 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. The new calculations strongly suggest a much smaller role of nonadiabatic effects than previously assumed on the basis of a comparison between low dimensional results and experiments [J. Chem. Phys. 115, 9028 (2001)]. Also in agreement with experiment, our theoretical results show a strong dependence of reaction on the initial vibrational state. Computed angular scattering distributions and parallel translation energy distributions are in good agreement with experiments on scattering, but the theory overestimates vibrational and rotational excitations in scattering. (c) 2006 American Institute of Physics.
Original languageEnglish
JournalJournal of Chemical Physics
Volume125
Issue number11
Pages (from-to)114706
ISSN0021-9606
DOIs
Publication statusPublished - 2006

Bibliographical note

Copyright (2006) American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.

Keywords

  • METAL-SURFACES
  • DIATOMIC-MOLECULES
  • VIBRATIONAL-EXCITATION
  • POTENTIAL-ENERGY SURFACES
  • SOLID-SURFACE
  • ANGULAR-DISTRIBUTION
  • QUANTUM DYNAMICS
  • CU(111) SURFACE
  • ASSOCIATIVE DESORPTION
  • DISSOCIATIVE CHEMISORPTION

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