Sub-femtosecond Control of Hydrogen-Bond Rearrangement*

We present experimental and theoretical data supporting a new and very general coherent control scheme, where the directional hydrogen migration in hydrocarbon molecules is initiated via light-driven attosecond electron motion. The strong coupling between electron and nuclear motions allows for efficient control of both electrons and heavier nuclei within the wave cycle of near-single-cycle laser pulses. We show that the waveform of the near-single-cycle laser pulses can be tailored to preferentially steer protons to different sites of the hydrocarbons prior to the molecular disintegration by the strong laser fields.