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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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.
The authors declare no competing interests.
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Muraviev, A.V., Smolski, V.O., Loparo, Z.E. et al. Massively parallel sensing of trace molecules and their isotopologues with broadband subharmonic mid-infrared frequency combs. Nature Photon 12, 209–214 (2018). https://doi.org/10.1038/s41566-018-0135-2
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