Two-pulse control over double ionization pathways in CO2.

We visualize and control molecular dynamics taking place on intermediately populated states during different sequential double ionization pathways of CO2 using a sequence of two delayed laser pulses which exhibit different peak intensities. Measured yields of CO2 (2+) and of fragment pairs CO(+)/O(+) as a function of delay between the two pulses are weakly modulated by various vibronic dynamics taking place in CO2 (+). By Fourier analysis of the modulations we identify the dynamics and show that they can be assigned to merely two double ionization pathways. We demonstrate that by reversing the sequence of the two pulses it becomes possible to control the pathway which is taken across CO2 (+) towards the final state in CO2 (2+). A comparison between the yields of CO2 (2+) and CO(+)/O(+) reveals that the modulating vibronic dynamics oscillate out-of-phase with each other, thus opening up opportunities for strong-field fragmentation control on extended time scales.