Vibrational lifetimes of hydrogen on lead films : an ab initio molecular dynamics with electronic friction (AIMDEF) study
- Using density functional theory and Ab Initio Molecular Dynamics with Electronic Friction (AIMDEF), we study the adsorption and dissipative vibrational dynamics of hydrogen atoms chemisorbed on free-standing lead films of increasing thickness. Lead films are known for their oscillatory behaviour of certain properties with increasing thickness, e.g., energy and electron spill-out change in discontinuous manner, due to quantum size effects [G. Materzanini, P. Saalfrank, and P.J.D. Lindan, Phys. Rev. B 63, 235405 (2001)]. Here, we demonstrate that oscillatory features arise also for hydrogen when chemisorbed on lead films. Besides stationary properties of the adsorbate, we concentrate on finite vibrational lifetimes of H-surface vibrations. As shown by AIMDEF, the damping via vibration-electron hole pair coupling dominates clearly over the vibration-phonon channel, in particular for high-frequency modes. Vibrational relaxation times are a characteristic function of layer thickness due to the oscillating behaviour of the embedding surfaceUsing density functional theory and Ab Initio Molecular Dynamics with Electronic Friction (AIMDEF), we study the adsorption and dissipative vibrational dynamics of hydrogen atoms chemisorbed on free-standing lead films of increasing thickness. Lead films are known for their oscillatory behaviour of certain properties with increasing thickness, e.g., energy and electron spill-out change in discontinuous manner, due to quantum size effects [G. Materzanini, P. Saalfrank, and P.J.D. Lindan, Phys. Rev. B 63, 235405 (2001)]. Here, we demonstrate that oscillatory features arise also for hydrogen when chemisorbed on lead films. Besides stationary properties of the adsorbate, we concentrate on finite vibrational lifetimes of H-surface vibrations. As shown by AIMDEF, the damping via vibration-electron hole pair coupling dominates clearly over the vibration-phonon channel, in particular for high-frequency modes. Vibrational relaxation times are a characteristic function of layer thickness due to the oscillating behaviour of the embedding surface electronic density. Implications derived from AIMDEF for frictional many-atom dynamics, and physisorbed species will also be given. (C) 2014 AIP Publishing LLC.…
Author details: | Peter SaalfrankORCiDGND, J. I. Juaristi, Maite Alducin, Maria Blanco-Rey, R. Diez Muino |
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DOI: | https://doi.org/10.1063/1.4903309 |
ISSN: | 0021-9606 |
ISSN: | 1089-7690 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/25527952 |
Title of parent work (English): | The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr |
Publisher: | American Institute of Physics |
Place of publishing: | Melville |
Publication type: | Article |
Language: | English |
Year of first publication: | 2014 |
Publication year: | 2014 |
Release date: | 2017/03/26 |
Volume: | 141 |
Issue: | 23 |
Number of pages: | 11 |
Funding institution: | Deutsche Forschungsgemeinschaft (DFG) [Sa 547/8-2]; University of the Basque Country UPV/EHU [IT-756-13]; Spanish Ministerio de Economia y Competitividad [FIS2013-48286-C2-2-P] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
Peer review: | Referiert |