Charge oscillation controlled molecular excitation.

The direct manipulation of charge oscillations has emerged as a new perspective in chemical reaction control. Here, we demonstrate, in a joint experimental and theoretical study, that the electron dynamics of a molecule is efficiently steered by controlling the interplay of a driving femtosecond laser pulse with the photoinduced charge oscillation. These oscillations have a typical Bohr period of around 1 fs for valence electrons; therefore, control has to be exerted on a shorter time scale. Specifically, we show how precision pulse shaping is used to manipulate the coupled electron and nuclear dynamics in order to address different bound electronic target states in a molecule. We present a strong-field coherent control mechanism which is understood in terms of a simple classical picture and at the same time verified by solving the time-dependent Schrödinger equation. This mechanism is universally applicable and opens a wide spectrum of applications in the reaction control of complex systems.