Abstract
Molecular ions can be held in a chain of laser-cooled atomic ions by sympathetic cooling. This system is ideal for performing high-precision molecular spectroscopy with applications in astrochemistry and fundamental physics. Here we show that this same system can be coupled with a broadband laser to discover new molecular transitions. We use three-ion chains of Ca+ and CaH+ to observe vibrational transitions via resonance-enhanced multiphoton dissociation detected by Ca+ fluorescence. On the basis of theoretical calculations, we assign the observed peaks to the transition from the ground vibrational state, ν=0 to ν=9 and 10. Our method allows us to track single-molecular events, and it can be extended to work with any molecule by using normal mode frequency shifts to detect the dissociation. This survey spectroscopy serves as a bridge to the precision spectroscopy required for molecular ion control.
Highlights
Molecular ions can be held in a chain of laser-cooled atomic ions by sympathetic cooling
Coulomb crystals composed of laser-cooled atomic ions and molecular ions provide a pristine environment for studying the properties of molecules[3]
The experimental apparatus has previously been employed for sympathetic heating spectroscopy[21] and the sideband cooling of molecular ions[22]
Summary
Molecular ions can be held in a chain of laser-cooled atomic ions by sympathetic cooling. Precision spectroscopy of molecules and molecular ions can yield insight into the fundamental physical constants and astrochemical processes[1,2]. Coulomb crystals composed of laser-cooled atomic ions and molecular ions provide a pristine environment for studying the properties of molecules[3].
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