within a hydrocarbon molecule holds promise for far-reaching applications.
Here,
we demonstrate the steering of hydrogen migration in simple hydrocarbons, namely acetylene and allene,
using waveform-controlled,
few-cycle laser pulses.
The rearrangement dynamics are monitored
using coincident 3D momentum imaging spectroscopy,
and described with a quantum-dynamical model.
Our observations reveal that the underlying control mechanism is due to the manipulation of the phases in a vibrational wavepacket by the intense
off-resonant laser field.