Selective excitation of coupled CO vibrations on a dissipative Cu(100) surface by shaped infrared laser pulses.

In a previous paper [Beyvers et al., J. Chem.

A hybrid local/global optimal control algorithm for dissipative systems with time-dependent targets: formulation and application to relaxing adsorbates.

Open-system quantum optimal control theory for optical control of the dynamics of a quantum system in contact with a dissipative bath is used here for explicitly time-dependent target operators, O(t). Global and local control strategies are combined in a novel algorithm by defining a set of time slices, into which the total control time is subdivided. The optimization then proceeds locally forward in time from subinterval to subinterval, while within each subinterval global control theory is used with iterative forward-backward propagation.

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.