Abstract

A longstanding goal in chemical physics has been the control of atoms and molecules using coherent light fields. This paper provides a brief overview of the field and discusses experiments that use a programmable pulse shaper to control the quantum state of electronic wavepackets in Rydberg atoms and electronic and nuclear dynamics in molecular liquids. The shape of Rydberg wavepackets was controlled by using tailored ultrafast pulses to excite a beam of caesium atoms. The quantum state of these atoms was measured using holographic techniques borrowed from optics. The experiments with molecular liquids involved the construction of an automated learning machine. A genetic algorithm directed the choice of shaped pulses which interacted with the molecular system inside a learning control loop. Analysis of successful pulse shapes that were found by using the genetic algorithm yield insight into the systems being controlled.

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