The Effects of electron-hole pair coupling on the infrared laser-controlled vibrational excitation of NO on Au(111)
- In this work, we present theoretical simulations of laser-driven vibrational control of NO adsorbed on a gold surface. Our goal is to tailor laser pulses to selectively excite specific modes and vibrational eigenstates, as well as to favor photodesorption of the adsorbed molecule. To this end, various control schemes and algorithms are applied. For adsorbates at metallic surfaces, the creation of electron hole pairs in the substrate is known to play a dominant role in the transfer of energy from the system to the surroundings. These nonadiabatic couplings are included perturbatively in our reduced density matrix simulations using a generalization of the state-resolved position-dependent anharmonic rate model we recently introduced. An extension of the reduced density matrix is also proposed to provide a sound model for photodesorption in dissipative systems.
Author details: | Jean Christophe TremblayORCiDGND, Serge Monturet, Peter SaalfrankORCiDGND |
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DOI: | https://doi.org/10.1021/jp205902k |
ISSN: | 1089-5639 |
Title of parent work (English): | The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment & general theory |
Publisher: | American Chemical Society |
Place of publishing: | Washington |
Publication type: | Article |
Language: | English |
Year of first publication: | 2011 |
Publication year: | 2011 |
Release date: | 2017/03/26 |
Volume: | 115 |
Issue: | 39 |
Number of pages: | 10 |
First page: | 10698 |
Last Page: | 10707 |
Funding institution: | Deutsche Forschungsgemeinschaft (DFG) [Sa 547/8]; Centre National de la Recherche Scientifique (CNRS); European Commission [ICT-270028] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
Peer review: | Referiert |