Massively parallel dual-comb molecular detection with subharmonic optical parametric oscillators

Abstract: Mid-infrared (mid-IR) spectroscopy offers unparalleled sensitivity for the detection of trace gases, solids and liquids, which is based on the existence of strong telltale vibrational bands in this part of the spectrum. It was shown more than a decade ago that a dual-comb Fourier spectroscopy could provide superior spectral coverage combined with high resolution and extremely fast data acquisition. Capabilities of this method were limited because of difficulty of producing twins of mutually coherent frequency combs in the mid- IR. Here we report a phase-coherent and broadband dual-comb system that is based on a pair of subharmonic (frequency-divide-by-two) optical parametric oscillators, pumped in turn by two phase-locked thulium fiber lasers at 2-micron wavelength. We demonstrate simultaneous detection of multiple molecular species in the whole band of 3.2-5.3 microns (frequency span 1200 cm^{-1}) augmented by the pump laser band of 1.85-2 microns (span 400 cm^{-1}), with spectral resolution 0.01-0.07 cm^{-1} and acquisition speed of up to 160,000 resolution elements in few seconds.