Physical Review Letters · 2016 · 90 citations · 29 references
Natural SciencesChemistryPhysicsQuantum ChemistryQuantum MechanicsSpectroscopyLaser PhysicsLaser SpectroscopyMolecular DynamicsMolecular Quantum MechanicsMolecular VibrationVibrational StructureAliphatic HydrocarbonsFew-cycle PulsesHydrocarbon CombustionLaser-induced ExcitationMolecular Vibrational DynamicsNuclear Wavepacket DynamicsQuantum Mechanical ModelQuantum Wavepacket Dynamics
Proton migration is a ubiquitous process in chemical reactions related to biology, combustion, and catalysis. Thus, the ability to manipulate the movement of nuclei with tailored light 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 is monitored using coincident 3D momentum imaging spectroscopy and described with a widely applicable quantum-dynamical model. Our observations reveal that the underlying control mechanism is due to the manipulation of the phases in a vibrational wave packet by the intense off-resonant laser field.
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