Four-mode multi-selection in the dual phase control of a molecular ionization induced by Fourier-synthesized laser fields

Coherent laser fields have been used to maximize the rate of a photochemical reaction or provide control over a single targeted property or function of matter by tuning of single-laser or multi-laser parameters. However, there is a need for multi-functionality control, albeit with as few parameters as possible. Here, we report simultaneous control of molecular geometry (selection of molecular orientation) and electron dynamics (electron removal) with dual-phase control of Fourier-synthesized laser fields. Directionally asymmetric tunneling ionization induced by intense, nanosecond, three-color Fourier-synthesized laser fields led to four-mode selection with a combination of positive/negative orientation-selected and yield-enhanced/suppressed molecular ionization of carbonyl sulfide.