Observation of vibrational overtones by single-molecule resonant photodissociation.

Journal Article (Journal Article)

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.

Full Text

Duke Authors

Cited Authors

  • Khanyile, NB; Shu, G; Brown, KR

Published Date

  • July 22, 2015

Published In

Volume / Issue

  • 6 /

Start / End Page

  • 7825 -

PubMed ID

  • 26197787

Pubmed Central ID

  • PMC4525170

Electronic International Standard Serial Number (EISSN)

  • 2041-1723

International Standard Serial Number (ISSN)

  • 2041-1723

Digital Object Identifier (DOI)

  • 10.1038/ncomms8825


  • eng