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Register a new userDual-comb cavity ring-down spectroscopy
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Authors
D. Lisak
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Cavity ring-down spectroscopy is a ubiquitous optical method used to study light-matter interactions with high resolution, sensitivity and accuracy. However, it has never been performed with the multiplexing advantages of direct frequency comb spectroscopy without sacrificing orders of magnitude of resolution. We present dual-comb cavity ring-down spectroscopy (DC-CRDS) based on the parallel heterodyne detection of ring-down signals with a local oscillator comb to yield absorption and dispersion spectra. These spectra are obtained from widths and positions of cavity modes. We present two approaches which leverage the dynamic cavity response to coherently or randomly driven changes in the amplitude or frequency of the probe field. Both techniques yield accurate spectra of methane - an important greenhouse gas and breath biomarker. The high sensitivity and accuracy of broadband DC-CRDS, shows promise for applications like studies of the structure and dynamics of large molecules, multispecies trace gas detection and isotopic composition.
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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.
Fast-responding detector arrays are commonly used for imaging rapidly-changing scenes. Besides array detectors, a single-pixel detector combined with a broadband optical spectrum can also be used for rapid imaging by mapping the spectrum into a spatial coordinate grid and then rapidly measuring the spectrum. Here, optical frequency combs generated from high-$Q$ silica microresonators are used to implement this method. The microcomb is dispersed in two spatial dimensions to measure a test target. The target-encoded spectrum is then measured by multi-heterodyne beating with another microcomb having a slightly different repetition rate, enabling an imaging frame rate up to 200 kHz and fillrates as high as 48 MegaPixels/s. The system is used to monitor the flow of microparticles in a fluid cell. Microcombs in combination with a monolithic waveguide grating array imager could greatly magnify these results by combining the spatial parallelism of detector arrays with spectral parallelism of optics.
Due to its fast and high resolution characteristics, dual-comb spectroscopy has attracted an increasing amount of interest since its first demonstration. In the terahertz frequency range where abundant absorption lines (finger prints) of molecules are located, multiheterodyne spectroscopy that employs the dual-comb technique shows an advantage in real-time spectral detection over the traditional Fourier transform infrared or time domain spectroscopies. Here, we demonstrate compact terahertz dual-comb spectroscopy based on quantum cascade lasers (QCLs). In our experiment, two free-running QCLs generate approximately 120 GHz wide combs centered at 4.2 THz, with slightly different repetition frequencies. We observe that $sim$490 nW terahertz power coupling of one laser into the other suffices for laser-self-detecting the dual-comb spectrum that is registered by a microwave spectrum analyzer. Furthermore, we demonstrate practical terahertz transmission dual-comb spectroscopy with our device, by implementing a short air path at room temperature. Spectra are shown of semiconductor samples and of moist air, the latter allowing rapid monitoring of the relative humidity. Our devices should be readily extendable to perform imaging, microscopy and near-field microscopy in the terahertz regime.
Broadband dual-comb spectroscopy (DCS) based on portable mode-locked fiber frequency combs is a powerful tool for in situ, calibration free, multi-species spectroscopy. While the acquisition of a single spectrum with mode-locked DCS typically takes microseconds to milliseconds, the applications of these spectrometers have generally been limited to systems and processes with time changes on the order of seconds or minutes due to the need to average many spectra to reach a high signal-to-noise ratio (SNR). Here, we demonstrate high-speed, continuous, fiber mode-locked laser DCS with down to 11 $mu$s time resolution. We achieve this by filtering the comb spectra using portable Fabry-Perot cavities to generate filtered combs with 1 GHz tooth spacing. The 1 GHz spacing increases the DCS acquisition speed and SNR for a given optical bandwidth while retaining a sufficient spacing to resolve absorption features over a wide range of conditions. We measure spectra of methane inside a rapid compression machine throughout the 16 ms compression cycle with 133 cm$^{-1}$ bandwidth (4000 comb teeth) and 1.4 ms time resolution by spectrally filtering one of the combs. By filtering both combs, we measured a single-shot, 25 cm$^{-1}$ (750 comb teeth) spectrum of CO around 6330 cm$^{-1}$ in 11 $mu$s. The technique enables simultaneously high-speed and high-resolution DCS measurements, and can be applied anywhere within the octave-spanning spectrum of robust and portable fiber mode-locked frequency combs.
Spectroscopy in the molecular fingerprint spectral region (6.5-20 $mu$m) yields critical information on material structure for physical, chemical and biological sciences. Despite decades of interest and effort, this portion of the electromagnetic spectrum remains challenging to cover with conventional laser technologies. In this report, we present a simple and robust method for generating super-octave, optical frequency combs in the fingerprint region through intra-pulse difference frequency generation in an orientation-patterned gallium phosphide crystal. We demonstrate the utility of this unique coherent light source for high-precision, dual-comb spectroscopy in methanol and ethanol vapor. These results highlight the potential of laser frequency combs for a wide range of molecular sensing applications, from basic molecular spectroscopy to nanoscopic imaging.
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