Optimal control in a dissipative system : vibrational excitation of CO/Cu(100) by IR pulses
- The question as to whether state-selective population of molecular vibrational levels by shaped infrared laser pulses is possible in a condensed phase environment is of central importance for such diverse fields as time-resolved spectroscopy, quantum computing, or "vibrationally mediated chemistry." This question is addressed here for a model system, representing carbon monoxide adsorbed on a Cu(100) surface. Three of the six vibrational modes are considered explicitly, namely, the CO stretch vibration, the CO-surface vibration, and a frustrated translation. Optimized infrared pulses for state-selective excitation of "bright" and "dark" vibrational levels are designed by optimal control theory in the framework of a Markovian open-system density matrix approach, with energy flow to substrate electrons and phonons, phase relaxation, and finite temperature accounted for. The pulses are analyzed by their Husimi "quasiprobability" distribution in time-energy space.
Author details: | Stephanie BeyversGND, Y Ohtsuki, Peter SaalfrankORCiDGND |
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URL: | http://jcp.aip.org/ |
DOI: | https://doi.org/10.1063/1.2206593 |
ISSN: | 0021-9606 |
Publication type: | Article |
Language: | English |
Year of first publication: | 2006 |
Publication year: | 2006 |
Release date: | 2017/03/24 |
Source: | Journal of chemical physics. - ISSN 0021-9606. - 124 (2006), 23, Art 234706 |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
Peer review: | Referiert |
Institution name at the time of the publication: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik |