Molecular Fragmentation in the CH2XY Family of Halomethanes

There is substantial interest in controlling wavepacket dynamics in molecular states with ultrafast pulses. We demonstrate control over the dissociation of CH2Br2, CH2BrI, and CH2I2 molecules. Time dynamics of the dissociations show signatures of parent ion vibrations. Ab initio structure calculations confirm these signatures with strong quantitative agreement. We explore wavepacket dynamics on the parent ion potential energy surface, and use them to control population transfer from the bound parent ion to the dissociative states.