Abstract

With the invention of the laser, the dream was realized to actively exert control over quantum systems. Active control over the dynamics of quantum mechanical systems is a fascinating perspective in modern physics. Cleavage and creation of predetermined chemical bonds, selective population transfer in atoms and molecules, and steering the dynamics of bound and free electrons have been important milestones along this way. A promising tool for this purpose is available with femtosecond laser technologies. In this chapter we review some of our work on adaptive femtosecond quantum control where a learning algorithm and direct experimental feedback signals are employed to optimize user-defined objectives. Femtosecond laser pulses are modified in frequency-domain pulse shapers, which apart from phase- and intensity-modulation can also modify the polarization state as a function of time. We will highlight the major advances in the field of optimal control by presenting our own illustrative experimental examples such as gas-phase and liquid-phase femtochemistry, control in weak and strong laser fields, and control of electron dynamics.

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