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Molecular ions can be held in a chain of laser-cooled atomic ions bysympathetic cooling. This system is ideal for performing high-precisionmolecular spectroscopy with applications in astrochemistry and fundamentalphysics. Here we show that this same system can be coupled with a broadbandlaser to discover new molecular transitions. We use three-ion chains ofCa$^{+}$ and CaH$^{+}$ to observe vibrational transitions via resonanceenhanced multiphoton dissociation detected by Ca$^{+}$ fluorescence. Based ontheoretical calculations, we assign the observed peaks to the transition fromthe ground vibrational state, $\nu=0$, to $\nu=9$ and $\nu=10$. Our methodallows us to track single molecular events, and it can be extended to work withany molecule by using normal mode frequency shifts to detect the dissociation.This survey spectroscopy serves as a bridge to the precision spectroscopyrequired for molecular ion control.

Observation of vibrational overtones by single molecule resonant photodissociation