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Using quantum-mechanical, one-dimensional, non-Born–Oppenheimer simulations we study the control over the strong-field dynamics of the helium hydride molecular ion HeH+ due to interaction driven by short and strong two-color laser pulses. We calculate yields of two competing fragmentation channels: electron removal and dissociation. We find that by changing the relative phase of the two colors, we can select the dominating channel. Nuclear motion is decisive for explaining ionization in this target. Ionization yields are vastly underestimated when nuclear motion is excluded and they are substantially reduced in the heavier isotopologue HeD+. Coupling of the two lowest electronic states is crucial even for the ground-state dissociation process.

We study the effect of the nuclear-mass ratio in a diatomic molecular ion on the dissociation dynamics in strong infrared laser pulses. A molecular ion is a charged system, in which the dipole moment depends on the reference point and therefore on the position of the nuclear center of mass, so that the laser-induced dynamics is expected to depend on the mass asymmetry. Whereas usually both the reduced mass and the mass ratio are varied when different isotopologues are compared, we fix the reduced mass and artificially vary the mass ratio in a model system. This allows us to separate effects related to changes in the resonance frequency, which is determined by the reduced mass, from those that arise due to the mass asymmetry. Numerical solutions of the time-dependent Schrödinger equation are compared with classical trajectory simulations. We find that at a certain mass ratio, vibrational excitation is strongly suppressed, which decreases the dissociation probability by many orders of magnitude.