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Register a new userTunable dual-comb spectrometer for mid-infrared trace gas analysis from 3 to 4.7 {mu}m
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Authors
Leonard Nitzsche
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Dual-frequency comb spectroscopy has emerged as a disruptive technique for measuring wide-spanning spectra with high resolution, yielding a particularly powerful technique for sensitive multi-component gas analysis. We present a spectrometer system based on dual electro-optical combs with subsequent conversion to the mid-infrared via tunable difference frequency generation, operating in the range from 3 to 4.7 $mu$m. The simultaneously recorded bandwidth is up to 454(1) GHz and a signal-to-noise ratio of 7.3(2) x 10$^2$ Hz$^{-1/2}$ can be reached. The conversion preserves the coherence of the dual-comb within 3 s measurement time. Concentration measurements of 5 ppm methane at 3.3 $mu$m, 100 ppm nitrous oxide at 3.9 $mu$m and a mixture of 15 ppm carbon monoxide and 5 % carbon dioxide at 4.5 $mu$m are presented with a relative precision of 1.4 % in average after 2 s measurement time. The noise-equivalent absorbance is determined to be less than 4.6(2) x 10$^{-3}$ Hz$^{-1/2}$.
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We demonstrate a high-accuracy dual-comb spectrometer centered at 3.4 mu m. The amplitude and phase spectra of the P, Q, and partial R-branch of the methane { u}3 band are measured at 25 MHz to 100 MHz point spacing with ~kHz resolution and a signal-to-noise ratio of up to 3500. A fit of the absorbance and phase spectra yield the center frequency of 132 rovibrational lines. The systematic uncertainty is estimated to be 300 kHz, which is 10-3 of the Doppler width and a tenfold improvement over Fourier transform spectroscopy. These data are the first high- accuracy molecular spectra obtained with a direct comb spectrometer.
Four-wave-mixing-based quantum cascade laser frequency combs (QCL-FC) are a powerful photonic tool, driving a recent revolution in major molecular fingerprint regions, i.e. mid- and far-infrared domains. Their compact and frequency-agile design, together with their high optical power and spectral purity, promise to deliver an all-in-one source for the most challenging spectroscopic applications. Here, we demonstrate a metrological-grade hybrid dual comb spectrometer, combining the advantages of a THz QCL-FC with the accuracy and absolute frequency referencing provided by a free-standing, optically-rectified THz frequency comb. A proof-of-principle application to methanol molecular transitions is presented. The multi-heterodyne molecular spectra retrieved provide state-of-the-art results in line-center determination, achieving the same precision as currently available molecular databases. The devised setup provides a solid platform for a new generation of THz spectrometers, paving the way to more refined and sophisticated systems exploiting full phase control of QCL-FCs, or Doppler-free spectroscopic schemes.
Coherent laser beams in the 3 to 20 {mu}m region of the spectrum are most applicable for chemical sensing by addressing the strongest vibrational absorption resonances of the media. Broadband frequency combs in this spectral range are of special interest since they can be used as a powerful tool for molecular spectroscopy offering dramatic gains in speed, sensitivity, precision, and massive parallelism of data collection. Here we show that a frequency comb realized through subharmonic generation in an optical parametric oscillator (OPO) based on orientation-patterned gallium phosphide (OP-GaP) pumped by a Kerr-lens mode-locked 2.35-{mu}m laser can reach a continuous wavelength span of 3-12 {mu}m, thus covering most of the molecular signature region. The key to achieving such a broad spectrum is to use a low-dispersion cavity entailing all gold-coated mirrors, minimally dispersive and optically thin intracavity elements, and a specially designed pump injector. The system features a smooth ultra-broadband spectral output that is phase coherent to the pump laser comb, 245-mW output power with high (>20%) optical conversion efficiency, and a possibility to reach close to unity conversion from a mode-locked drive, thanks to the non-dissipative downconversion processes and photon recycling.
Dual-comb spectroscopy has been proven a powerful tool in molecular characterization, which remains challenging to implement in the mid-infrared (MIR) region due to difficulties in the realization of two mutually locked comb sources and efficient photodetection. An effective way to overcome those limitations is optical upconversion; however, previously reported configurations are either demanding or inefficient. Here we introduce and experimentally demonstrate a variant of dual-comb spectroscopy called cross-comb spectroscopy, in which a MIR comb is upconverted via sum-frequency generation (SFG) with a near-infrared (NIR) comb with a shifted repetition rate and then interfered with a spectral extension of the NIR comb. We experimentally demonstrate a proof-of-concept measurement of atmospheric CO2 around 4.25 micrometer, with a 350-nm instantaneous bandwidth and 25000 resolved comb lines. Cross-comb spectroscopy can be realized using up- or down-conversion and offers an adaptable and efficient alternative to dual-comb spectroscopy outside the well-developed near-IR region, where having two mutually coherent sources and efficient photodetection is challenging. Moreover, the nonlinear gating in cross-comb spectroscopy promises a superior dynamic range compared to dual-comb spectroscopy.
We report the coherent phase-locking of a quantum cascade laser (QCL) at 10-$mu$m to the secondary frequency standard of this spectral region, a CO2 laser stabilized on a saturated absorption line of OsO4. The stability and accuracy of the standard are transferred to the QCL resulting in a line width of the order of 10 Hz, and leading to our knowledge to the narrowest QCL to date. The locked QCL is then used to perform absorption spectroscopy spanning 6 GHz of NH3 and methyltrioxorhenium, two species of interest for applications in precision measurements.
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