Observation of vibrational overtones by single-molecule resonant photodissociation

Ncamiso B. Khanyile, Gang Shu and Kenneth R. Brown ()
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Ncamiso B. Khanyile: Schools of Chemistry and Biochemistry, Computational Science and Engineering, and Physics, Georgia Institute of Technology
Gang Shu: Schools of Chemistry and Biochemistry, Computational Science and Engineering, and Physics, Georgia Institute of Technology
Kenneth R. Brown: Schools of Chemistry and Biochemistry, Computational Science and Engineering, and Physics, Georgia Institute of Technology

Nature Communications, 2015, vol. 6, issue 1, 1-4

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms8825

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