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Observation of vibrational overtones by single-molecule resonant photodissociation

Author

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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)

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.

Suggested Citation

  • Ncamiso B. Khanyile & Gang Shu & Kenneth R. Brown, 2015. "Observation of vibrational overtones by single-molecule resonant photodissociation," Nature Communications, Nature, vol. 6(1), pages 1-4, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms8825
    DOI: 10.1038/ncomms8825
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