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The laser-induced fragmentation dynamics of this most fundamental polar molecule HeH^{+} are measured using an ion beam of helium hydride and an isotopologue at various wavelengths and intensities. In contrast to the prevailing interpretation of strong-field fragmentation, in which stretching of the molecule results primarily from laser-induced electronic excitation, experiment and theory for nonionizing dissociation, single ionization, and double ionization both show that the direct vibrational excitation plays the decisive role here. We are able to reconstruct fragmentation pathways and determine the times at which each ionization step occurs as well as the bond length evolution before the electron removal. The dynamics of this extremely asymmetric molecule contrast the well-known symmetric systems leading to a more general picture of strong-field molecular dynamics and facilitating interpolation to systems between the two extreme cases.

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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.

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