title: Optimal control in a dissipative system: vibrational excitation of CO/Cu(100) by IR pulses.
abstract: 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.
authors.affiliation: Institut für Chemie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, D-14476 Potsdam-Golm, Germany.
authors.forename: Stephanie
authors.initials: S
authors.lastname: Beyvers
authors.forename: Yukiyoshi
authors.initials: Y
authors.lastname: Ohtsuki
authors.forename: Peter
authors.initials: P
authors.lastname: Saalfrank