Control of competing dissociation channels by femtosecond interferometry: Aspects of electron and nuclear dynamics

The interaction of a molecule with the laser field generated by two time-shifted interfering femtosecond laser pulses is shown to control electron and nuclear dynamics. We demonstrate that the product yields caused by the interferometric dissociation carry the signature of time dependent electronic polarization due to the correlated electronic and nuclear dynamics induced in the region of partial overlap of two laser pulses. Thus, the two pulse technique provides a powerful tool for bridging the gap between electron and nuclear dynamics.