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Title: Quantum dynamics of hydrogen atoms on graphene. II. Sticking

Following our recent system-bath modeling of the interaction between a hydrogen atom and a graphene surface [Bonfanti et al., J. Chem. Phys. 143, 124703 (2015)], we present the results of converged quantum scattering calculations on the activated sticking dynamics. The focus of this study is the collinear scattering on a surface at zero temperature, which is treated with high-dimensional wavepacket propagations with the multi-configuration time-dependent Hartree method. At low collision energies, barrier-crossing dominates the sticking and any projectile that overcomes the barrier gets trapped in the chemisorption well. However, at high collision energies, energy transfer to the surface is a limiting factor, and fast H atoms hardly dissipate their excess energy and stick on the surface. As a consequence, the sticking coefficient is maximum (∼0.65) at an energy which is about one and half larger than the barrier height. Comparison of the results with classical and quasi-classical calculations shows that quantum fluctuations of the lattice play a primary role in the dynamics. A simple impulsive model describing the collision of a classical projectile with a quantum surface is developed which reproduces the quantum results remarkably well for all but the lowest energies, thereby capturing the essential physics of the activatedmore » sticking dynamics investigated.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [5]
  1. Dipartimento di Chimica, Università degli Studi di Milano, v. Golgi 19, 20133 Milano (Italy)
  2. Department of Chemistry, University of Massachusetts, Amherst, Massachusetts 01003 (United States)
  3. School of Chemistry, Bangor University, Bangor, Gwynedd LL57 2UW (United Kingdom)
  4. Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt, Max-von-Laue-Str. 7, 60438 Frankfurt/Main (Germany)
  5. (Italy)
Publication Date:
OSTI Identifier:
22489653
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 12; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; ATOMS; CHEMISORPTION; COLLISIONS; COMPARATIVE EVALUATIONS; ENERGY TRANSFER; GRAPHENE; HYDROGEN; INTERACTIONS; SCATTERING; SURFACES; TIME DEPENDENCE