The search result changed since you submitted your search request. Documents might be displayed in a different sort order.
  • search hit 31 of 1303
Back to Result List

Excitation, relaxation, and quantum diffusion of CO on copper

  • We investigate the effect of intermode coupling and anharmonicity on the excitation and relaxation dynamics of CO on Cu(100). The nonadiabatic coupling of the adsorbate to the surface is treated perturbatively using a position-dependent state-resolved transition rate model. Using the potential energy surface of Marquardt et al. [J. Chem. Phys. 132, 074108 (2010)], which provides an accurate description of intermode interactions, we propose a four-dimensional model that represents simultaneously the diffusion and the desorption of the adsorbate. The system is driven by both rational and optimized infrared laser pulses to favor either selective mode and state excitations or lateral displacement along the diffusion coordinate. The dissipative dynamics is simulated using the reduced density matrix in its Lindblad form. We show that coupling between the degrees of freedom, mediated by the creation and annihilation of electron-hole pairs in the metal substrate, significantly affects the system excitation and relaxation dynamics. InWe investigate the effect of intermode coupling and anharmonicity on the excitation and relaxation dynamics of CO on Cu(100). The nonadiabatic coupling of the adsorbate to the surface is treated perturbatively using a position-dependent state-resolved transition rate model. Using the potential energy surface of Marquardt et al. [J. Chem. Phys. 132, 074108 (2010)], which provides an accurate description of intermode interactions, we propose a four-dimensional model that represents simultaneously the diffusion and the desorption of the adsorbate. The system is driven by both rational and optimized infrared laser pulses to favor either selective mode and state excitations or lateral displacement along the diffusion coordinate. The dissipative dynamics is simulated using the reduced density matrix in its Lindblad form. We show that coupling between the degrees of freedom, mediated by the creation and annihilation of electron-hole pairs in the metal substrate, significantly affects the system excitation and relaxation dynamics. In particular, the angular degrees of freedom appear to play an important role in the energy redistribution among the molecule-surface vibrations. We also show that coherent excitation using simple IR pulses can achieve population transfer to a specific target to some extent but does not allow enforcement of the directionality to the diffusion motion.show moreshow less

Export metadata

Additional Services

Share in Twitter Search Google Scholar Statistics
Metadaten
Author:Jean Christophe TremblayORCiDGND, Gernot Füchsel, Peter SaalfrankORCiDGND
DOI:https://doi.org/10.1103/PhysRevB.86.045438
ISSN:1098-0121 (print)
ISSN:1550-235X (online)
Parent Title (English):Physical review : B, Condensed matter and materials physics
Publisher:American Physical Society
Place of publication:College Park
Document Type:Article
Language:English
Year of first Publication:2012
Year of Completion:2012
Release Date:2017/03/26
Volume:86
Issue:4
Pagenumber:13
Funder:Deutsche Forschungsgemeinschaft [Sa 547/8-1]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Peer Review:Referiert