Selecting two-photon sequential ionization pathways in H₂ through harmonic filtering

Recent experiments in gas-phase molecules have shown the versatility of using attosecond pulse trains combined with IR femtosecond pulses to track and control excitation and ionization yields on the attosecond timescale. The interplay between electron and nuclear motions drives the light-induced transitions favoring specific reaction paths, so that the time delay between the pulses can be used as the tracking parameter or as a control knob to manipulate the molecular dynamics. Here, we present ab initio simulations on the hydrogen molecule to demonstrate that by filtering the high harmonics in an attosecond pulse train one can quench or enhance specific quantum paths thus dictating the outcome of the reaction. It is then possible to discriminate the dominant sequential processes in two-photon ionization, as for example molecular excitation followed by ionization or the other way around. More interestingly, frequency filters can be employed to steer the one- and two-photon yields to favor electron emission in a specific direction.