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Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs

Nature Photonicsvolume 12pages209214 (2018) | Download Citation

Abstract

Mid-infrared spectroscopy offers supreme sensitivity for the detection of trace gases, solids and liquids based on tell-tale vibrational bands specific to this spectral region. Here, we present a new platform for mid-infrared dual-comb Fourier-transform spectroscopy based on a pair of ultra-broadband subharmonic optical parametric oscillators pumped by two phase-locked thulium-fibre combs. Our system provides fast (7 ms for a single interferogram), moving-parts-free, simultaneous acquisition of 350,000 spectral data points, spaced by a 115 MHz intermodal interval over the 3.1–5.5 µm spectral range. Parallel detection of 22 trace molecular species in a gas mixture, including isotopologues containing isotopes such as 13C, 18O, 17O, 15N, 34S, 33S and deuterium, with part-per-billion sensitivity and sub-Doppler resolution is demonstrated. The technique also features absolute optical frequency referencing to an atomic clock, a high degree of mutual coherence between the two mid-infrared combs with a relative comb-tooth linewidth of 25 mHz, coherent averaging and feasibility for kilohertz-scale spectral resolution.

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Change history

  • 01 June 2018

    In the version of this Article originally published, in equation (9), the ‘Δ’ in the first ‘Δfrep’ shouldn’t have been included and, in equation (10), within the brackets, frep and f were the wrong way round. These equations have now been corrected in the online versions.

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Acknowledgements

K.L.V. acknowledges support from the Office of Naval Research (ONR), grant number N00014-15-1-2659 and from the Defense Advanced Research Projects Agency (DARPA), grant number W31P4Q-15-1-0008. Z.E.L. acknowledges support from the National Science Foundation under Graduate Research Fellowship Program, grant number 1144246. We thank J. Jiang and K. Lee for sharing their expertise on the Tm-fibre frequency combs, and N. Newbury and S. Diddams for stimulating discussions.

Author information

Affiliations

  1. CREOL, College of Optics and Photonics, University of Central Florida, Orlando, FL, USA

    • A. V. Muraviev
    • , V. O. Smolski
    •  & K. L. Vodopyanov
  2. IPG Photonics-Mid-Infrared Lasers, Birmingham, AL, USA

    • V. O. Smolski
  3. Mechanical and Aerospace Engineering, University of Central Florida, Orlando, FL, USA

    • Z. E. Loparo

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Contributions

A.V.M. and V.O.S. constructed the experimental setup. A.V.M. carried out the measurements and analysed the data. Z.E.L. developed the algorithm for data acquisition and processing. K.L.V. initiated and supervised the project; he also analysed the data and wrote the paper.

Competing interests

The authors declare no competing interests.

Corresponding author

Correspondence to K. L. Vodopyanov.

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DOI

https://doi.org/10.1038/s41566-018-0135-2