The fragmentation dynamics of the hydrogen molecular ion H2+ and of its isotopic derivate HD+subjected to an intense pulsed laser radiation are studied using quantum wave packet propagations. It is shown that bichromatic optical excitations are subject to a high degree of control through the variation of the relative phase between the two fields. A phase‐locked (ω,2ω) laser pulse is used to induce asymmetry in the angular distribution of the emitted fragments. In addition, an appreciable isotope separation in the fragmentation of HD+ is predicted. The critical role of quantum molecular interferences in such phase‐controllable processes is demonstrated.

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