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We report molecular detection using dual frequency-comb spectroscopy withhighly coherent broadband (6.6-11.4 {\m}m) long-wavelength infrared (LWIR)combs. The combs were produced via intra-pulse difference frequency generation(IDFG) in ZGP crystals using sub-three-cycle (20 fs) driving pulses frommode-locked Cr:ZnS lasers at the central wavelength of 2.4 {\m}m). Real-timeand up to video rate (0.1-12 s per spectrum) acquisition of molecular spectrawith some 240,000 comb-mode-resolved data points spaced by 80 MHz andreferenced to a Rb clock with a signal-to-noise ratio (SNR) >300 has beendemonstrated. The key to achieving such a high rate of massive spectral dataacquisition is a low phase and intensity noise of the LWIR combs and excellentmutual coherence. The high SNR was also facilitated by the high (7.5%) IDFGconversion efficiency resulting in an average LWIR comb power of 300 mW perchannel.

Video-rate broadband longwave IR dual-comb spectroscopy with 240,000 comb-mode resolved data points