Weak-Field Coherent Control of Molecular Photofragment State Distributions.

It is known that the long-time energy-resolved photofragment state distribution produced upon photodissociation of a molecule cannot be modified in the weak-field limit for a fixed pump pulse spectral profile. This work, however, demonstrates both computationally and mathematically that the above limitation can be circumvented in practice when the molecule presents overlapping resonances. It is shown that when two or more energies where the resonances overlap are excited by different laser pulses delayed in time, interference is induced between the product fragment states associated with the different energies populated. The occurrence of interference is found to be independent of the delay time between the pulses exciting the different energies. Thus, as demonstrated, this finding makes it possible to modify the fragment distribution at a given energy, as far in time and as many times as desired.