Quantum dynamics of hydrogen atoms on graphene. II. Sticking
Abstract
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 »
- Authors:
-
- Dipartimento di Chimica, Università degli Studi di Milano, v. Golgi 19, 20133 Milano (Italy)
- Department of Chemistry, University of Massachusetts, Amherst, Massachusetts 01003 (United States)
- School of Chemistry, Bangor University, Bangor, Gwynedd LL57 2UW (United Kingdom)
- Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt, Max-von-Laue-Str. 7, 60438 Frankfurt/Main (Germany)
- Publication Date:
- OSTI Identifier:
- 22489653
- Resource Type:
- Journal Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 143; Journal Issue: 12; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
- 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
Citation Formats
Bonfanti, Matteo, Jackson, Bret, Hughes, Keith H., Burghardt, Irene, Martinazzo, Rocco, and Istituto di Scienze e Tecnologie Molecolari, Consiglio Nazionale delle Richerche, v. Golgi 19, 20133 Milano. Quantum dynamics of hydrogen atoms on graphene. II. Sticking. United States: N. p., 2015.
Web. doi:10.1063/1.4931117.
Bonfanti, Matteo, Jackson, Bret, Hughes, Keith H., Burghardt, Irene, Martinazzo, Rocco, & Istituto di Scienze e Tecnologie Molecolari, Consiglio Nazionale delle Richerche, v. Golgi 19, 20133 Milano. Quantum dynamics of hydrogen atoms on graphene. II. Sticking. United States. https://doi.org/10.1063/1.4931117
Bonfanti, Matteo, Jackson, Bret, Hughes, Keith H., Burghardt, Irene, Martinazzo, Rocco, and Istituto di Scienze e Tecnologie Molecolari, Consiglio Nazionale delle Richerche, v. Golgi 19, 20133 Milano. 2015.
"Quantum dynamics of hydrogen atoms on graphene. II. Sticking". United States. https://doi.org/10.1063/1.4931117.
@article{osti_22489653,
title = {Quantum dynamics of hydrogen atoms on graphene. II. Sticking},
author = {Bonfanti, Matteo and Jackson, Bret and Hughes, Keith H. and Burghardt, Irene and Martinazzo, Rocco and Istituto di Scienze e Tecnologie Molecolari, Consiglio Nazionale delle Richerche, v. Golgi 19, 20133 Milano},
abstractNote = {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 activated sticking dynamics investigated.},
doi = {10.1063/1.4931117},
url = {https://www.osti.gov/biblio/22489653},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 12,
volume = 143,
place = {United States},
year = {Mon Sep 28 00:00:00 EDT 2015},
month = {Mon Sep 28 00:00:00 EDT 2015}
}