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1. Broadband 1-GHz mid-infrared frequency comb

   https://doi.org/10.1038/s41377-022-00947-w  

   Hoghooghi, Nazanin ; Xing, Sida ; Chang, Peter ; Lesko, Daniel ; Lind, Alexander ; Rieker, Greg ; Diddams, Scott ( September 2022 , Light: Science & Applications)

   Mid-infrared (MIR) spectrometers are invaluable tools for molecular fingerprinting and hyper-spectral imaging. Among the available spectroscopic approaches, GHz MIR dual-comb absorption spectrometers have the potential to simultaneously combine the high-speed, high spectral resolution, and broad optical bandwidth needed to accurately study complex, transient events in chemistry, combustion, and microscopy. However, such a spectrometer has not yet been demonstrated due to the lack of GHz MIR frequency combs with broad and full spectral coverage. Here, we introduce the first broadband MIR frequency comb laser platform at 1 GHz repetition rate that achieves spectral coverage from 3 to 13 µm. This frequency comb is based on a commercially available 1.56 µm mode-locked laser, robust all-fiber Er amplifiers and intra-pulse difference frequency generation (IP-DFG) of few-cycle pulses inχ⁽²⁾nonlinear crystals. When used in a dual comb spectroscopy (DCS) configuration, this source will simultaneously enable measurements with μs time resolution, 1 GHz (0.03 cm⁻¹) spectral point spacing and a full bandwidth of >5 THz (>166 cm⁻¹) anywhere within the MIR atmospheric windows. This represents a unique spectroscopic resource for characterizing fast and non-repetitive events that are currently inaccessible with other sources.
2. A rapid, spatially dispersive frequency comb spectrograph aimed at gas phase chemical reaction kinetics

   https://doi.org/10.1080/00268976.2020.1733116  

   Roberts, Frances C. ; Lewandowski, H. J. ; Hobson, Billy F. ; Lehman, Julia H. ( February 2020 , Molecular Physics)

   This New Views article will highlight some recent advances in high sensitivity gas detection using direct infrared absorption frequency comb laser spectroscopy, with a focus on frequency comb use in chemical reaction kinetics and our own contribution to this field. Our recently implemented detection technique uses a combination of a 12.9 GHz free spectral range virtually imaged phased array and diffraction grating to spatially disperse the mid-infrared frequency comb onto a camera. Individual frequencies or ‘comb teeth’ of a 250 MHz repetition-rate frequency comb are able to be resolved. High molecular sensitivity is achieved by increasing the interaction path length using a Herriott multipass cell. High spectral resolution, broadband spectral coverage, and high molecular sensitivity are all achieved on an adjustable 1–50 µs timescale, making this frequency comb apparatus ideal for measuring chemical reaction kinetics where multiple absorbing species can be monitored simultaneously. This New Views article will also discuss some of the challenges and decisions that chemists might face in implementing this advanced physics technology in their own laboratory. Spatially dispersed 250 MHz mid-infrared frequency comb laser, with absorption of some frequencies by a dilute sample of methane. KEYWORDS: Frequency combs, chemical kinetics, trace gas detection
3. Thermal-light heterodyne spectroscopy with frequency comb calibration

   https://doi.org/10.1364/OPTICA.440389  

   Fredrick, Connor ; Olsen, Freja ; Terrien, Ryan ; Mahadevan, Suvrath ; Quinlan, Franklyn ; Diddams, Scott A. ( February 2022 , Optica)

   Precision laser spectroscopy is key to many developments in atomic and molecular physics and the advancement of related technologies such as atomic clocks and sensors. However, in important spectroscopic scenarios, such as astronomy and remote sensing, the light is of thermal origin, and interferometric or diffractive spectrometers typically replace laser spectroscopy. In this work, we employ laser-based heterodyne radiometry to measure incoherent light sources in the near-infrared and introduce techniques for absolute frequency calibration with a laser frequency comb. Measuring the solar continuum, we obtain a signal-to-noise ratio that matches the fundamental quantum-limited prediction given by the thermal photon distribution and our system’s efficiency, bandwidth, and averaging time. With resolving power$R\sim <\#comment/>{10}^6$, we determine the center frequency of an iron line in the solar spectrum to sub-MHz absolute frequency uncertainty in under 10 min, a fractional precision 1/4000 the linewidth. Additionally, we propose concepts that take advantage of refractive beam shaping to decrease the effects of pointing instabilities by$100\times <\#comment/>$, and of frequency comb multiplexing to increase data acquisition rates and spectral bandwidths by comparable factors. Taken together, our work brings the power of telecommunications photonics and the precision of frequency comb metrology to laser heterodyne radiometry, with implications formore »solar and astronomical spectroscopy, remote sensing, and precise Doppler velocimetry.

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4. Mid-infrared cross-comb spectroscopy

   https://doi.org/10.1038/s41467-023-36811-7  

   Liu, Mingchen ; Gray, Robert M. ; Costa, Luis ; Markus, Charles R. ; Roy, Arkadev ; Marandi, Alireza ( February 2023 , Nature Communications)

   Dual-comb spectroscopy has been proven beneficial in molecular characterization but remains challenging in the mid-infrared region due to difficulties in sources and efficient photodetection. Here we introduce cross-comb spectroscopy, in which a mid-infrared comb is upconverted via sum-frequency generation with a near-infrared comb of a shifted repetition rate and then interfered with a spectral extension of the near-infrared comb. We measure CO₂absorption around 4.25 µm with a 1-µm photodetector, exhibiting a 233-cm⁻¹instantaneous bandwidth, 28000 comb lines, a single-shot signal-to-noise ratio of 167 and a figure of merit of 2.4 × 10⁶Hz^1/2. We show that cross-comb spectroscopy can have superior signal-to-noise ratio, sensitivity, dynamic range, and detection efficiency compared to other dual-comb-based methods and mitigate the limits of the excitation background and detector saturation. This approach offers an adaptable and powerful spectroscopic method outside the well-developed near-IR region and opens new avenues to high-performance frequency-comb-based sensing with wavelength flexibility.
5. High-performance and scalable on-chip digital Fourier transform spectroscopy

   https://doi.org/10.1038/s41467-018-06773-2  

   Kita, Derek M. ; Miranda, Brando ; Favela, David ; Bono, David ; Michon, Jérôme ; Lin, Hongtao ; Gu, Tian ; Hu, Juejun ( October 2018 , Nature Communications)

   On-chip spectrometers have the potential to offer dramatic size, weight, and power advantages over conventional benchtop instruments for many applications such as spectroscopic sensing, optical network performance monitoring, hyperspectral imaging, and radio-frequency spectrum analysis. Existing on-chip spectrometer designs, however, are limited in spectral channel count and signal-to-noise ratio. Here we demonstrate a transformative on-chip digital Fourier transform spectrometer that acquires high-resolution spectra via time-domain modulation of a reconfigurable Mach-Zehnder interferometer. The device, fabricated and packaged using industry-standard silicon photonics technology, claims the multiplex advantage to dramatically boost the signal-to-noise ratio and unprecedented scalability capable of addressing exponentially increasing numbers of spectral channels. We further explore and implement machine learning regularization techniques to spectrum reconstruction. Using an ‘elastic-D₁’ regularized regression method that we develop, we achieved significant noise suppression for both broad (>600 GHz) and narrow (<25 GHz) spectral features, as well as spectral resolution enhancement beyond the classical Rayleigh criterion.