Classical dynamics in a quantum spirit: Refining semi-classical corrections for the scattering of H2 on W(100)

The Journal of Chemical Physics, vol. 163

Abstract

The collision dynamics of hydrogen on tungsten is studied using a combination of classical and quantum molecular dynamics approaches, making use of a multidimensional potential energy surface interpolated from density functional theory energies based on the vdW-DF2 functional. Corrections inspired by a semi-classical model are then introduced to improve the predictions of the classical description. In particular, a refined version of the adiabaticity correction (AC) is developed. This study demonstrates that, for H2 on W(100) in its ground state and in various rotationally excited states, applying both Gaussian binning and this refined AC to classical trajectories yields unparalleled agreement with time-dependent quantum wave packet results.

Authors 5

1. L. T. Viaud

   Centre National de la Recherche Scientifique · Université de Bordeaux · Institut des Sciences Moléculaires

   Affiliation as printed

   CNRS, ISM, UMR5255 2 , F-33400 Talence,

   Université de Bordeaux, ISM, UMR5255 1 , F-33400 Talence,

2. Mark F. Somers Aachen

   Leiden University

   Affiliation as printed

   Leiden University, LIC, TC 3 , 2333 CC Leiden,

   Leiden University, LIC, TC, 2333 CC Leiden, The Netherlands

3. Cedric Crespos

   Centre National de la Recherche Scientifique · Université de Bordeaux · Institut des Sciences Moléculaires

   Affiliation as printed

   CNRS, ISM, UMR5255 2 , F-33400 Talence,

   Université de Bordeaux, ISM, UMR5255 1 , F-33400 Talence,

4. Laurent Bonnet

   Centre National de la Recherche Scientifique · Université de Bordeaux · Institut des Sciences Moléculaires

   Affiliation as printed

   CNRS, ISM, UMR5255 2 , F-33400 Talence,

   Université de Bordeaux, ISM, UMR5255 1 , F-33400 Talence,

5. P. Larrégaray

   Centre National de la Recherche Scientifique · Université de Bordeaux · Institut des Sciences Moléculaires

   Affiliation as printed

   CNRS, ISM, UMR5255 2 , F-33400 Talence,

   Université de Bordeaux, ISM, UMR5255 1 , F-33400 Talence,