Optical frequency comb spectroscopy in the mid-infrared fingerprint region combines broad spectral bandwidth with high detection sensitivity and allows simultaneous detection of trace amounts of many molecular species. We have recently demonstrated a continuous-filtering Vernier spectrometer based on a mid-infrared optical frequency comb and an enhancement cavity for fast and sensitive detection of CH4 . Here we present an improved, fully automatized and frequency calibrated continuous-filtering Vernier spectrometer, schematically shown in Fig. 1(a). The comb source is a doubly resonant optical parametric oscillator (DROPO) based on an orientation-patterned GaAs crystal synchronously pumped by a Tm:fiber femtosecond laser (125 MHz repetition rate, frep). The signal comb (3.1–3.4 µm, 30 mW) is mode matched to a 60-cm long Vernier enhancement cavity with a finesse of ~350 at 3.25 μm, placed in an enclosure that can be filled with the gas sample. The output mirror is attached to a PZT and mounted on a translation stage. When the cavity free spectral range is perfectly matched to twice the frep (250 MHz) every other signal comb mode is transmitted through the cavity. By detuning the cavity length from this perfect match position the cavity resonances act as a filter and transmit groups of comb modes called Vernier orders . A diffraction grating mounted on a galvo-scanner separates these orders after the cavity and the chosen order is sent to the detection system. The Vernier order is tuned across the signal comb spectrum by scanning the cavity length (at 20 Hz) and the grating is rotated synchronously to fix the order in space and allow acquisition of the entire spectrum in 25 ms. Any residual mismatch between the cavity length scan and the grating rotation is compensated by a feedback loop acting on the frep of the pump laser and the PZT of the Vernier cavity . A Fabry-Perot etalon is used for frequency calibration of the spectrometer. Figure 1(b) shows in black the normalized transmission spectrum of a sample containing 5.0 ppm CH4 and 160 ppm water. The red and blue curves show the corresponding fit of the Vernier spectrum  of CH4 and water, respectively, calculated using Voigt profiles, line parameters from the HITRAN database, and the experimentally determined cavity finesse. The figure of merit of the spectrometer is 1×10−9 cm−1 Hz−1∕2 per spectral element and multiline fitting yields minimum detectable concentration of CH4 of 2 ppb in 25 ms, translating into 400 ppt Hz−1∕2 Since the spectrum of the signal comb covers the fundamental C-H stretch transitions we expect low detection limits for other hydrocarbons as well. In conclusion, mid-infrared comb-based continuous-filtering Vernier spectroscopy allows fast and highly sensitive measurement of broadband absorption spectra using a robust and compact detection system.
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