Signatures and control of strong-field dynamics in a complex system

Source abstract

Significance Using intense lasers to control complex molecules is a long-held dream in science. In this article, we develop a physics concept for measuring and controlling the quantum states of complex molecules by strong laser fields. We show that, in particular, the quantum-mechanical phase of excited molecular states can be manipulated by the intense laser, a key quantity for full (amplitude and phase) control of molecular quantum states. With the help of time- and intensity-resolved absorption spectroscopy experiments, we apply this idea to the dynamics of a large dye molecule in solution. The demonstrated phase-control concept thus represents a major leap toward the ultimate goal of laser chemistry.