title: Observation of vibrational overtones by single-molecule resonant photodissociation.
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.
authors.affiliation: Schools of Chemistry and Biochemistry, Computational Science and Engineering, and Physics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USA.
authors.forename: Ncamiso B
authors.initials: NB
authors.lastname: Khanyile
authors.affiliation: Schools of Chemistry and Biochemistry, Computational Science and Engineering, and Physics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USA.
authors.forename: Gang
authors.initials: G
authors.lastname: Shu
authors.affiliation: Schools of Chemistry and Biochemistry, Computational Science and Engineering, and Physics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USA.
authors.forename: Kenneth R
authors.initials: KR
authors.lastname: Brown