Achieving selective cleavage of specific chemical bonds using ultrafast laser pulses remains a central challenge in ultrafast strong-field molecular physics. Here, we theoretically investigate the coherent control of strong-field dissociation of the heteronuclear molecular ion HD+ initially prepared in vibrationally excited states driven by an ultrashort pulse with a quadratic spectral phase. Our results reveal a pronounced sensitivity of both the total dissociation probability and the branching ratio (H+ + D vs. H + D+) to the chirp rate of the laser pulse. To uncover the underlying physical mechanism, we analyze the population dynamics in the coupled 1sσ and 2pσ electronic states and identify pronounced Rabi oscillations arising from the coherent interplay between multiphoton excitation and field-induced stimulated emission. By tuning the laser chirp rate, these oscillations can be suppressed via quantum interference, thereby reshaping the dissociation dynamics and significantly enhancing the dissociation probability of the H + D+ channel. These findings demonstrate that spectral-phase engineering provides a robust and versatile strategy for selective control of branching ratios in strong-field molecular dissociation.
Cheng et al. (Thu,) studied this question.
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