Dual-comb spectroscopy is a rapidly developing spectroscopic technique that does not require any opto-mechanical moving parts and enables broadband and high-resolution measurements with microsecond time resolution. However, for high sensitivity measurements and extended averaging times, high mutual coherence of the comb-sources is essential. To date, most dual-comb systems employ coherent averaging schemes that require additional electro-optical components, which increase system complexity and cost. More recently, computational phase correction approaches that enables coherent averaging of spectra generated by free-running systems have gained increasing interest. Here, we propose such an all-computational solution that is compatible with real-time data acquisition architectures for free-running systems. The efficacy of our coherent averaging algorithm is demonstrated using dual-comb spectrometers based on quantum cascade lasers, interband cascade lasers, mode-locked lasers, and optically-pumped microresonators.

Hyperspectral imaging is a spectroscopic imaging technique that allows for the creation of images with pixels containing information from multiple spectral bands. At terahertz wavelengths, it has emerged as a prominent tool for a number of applications, ranging from nonionizing cancer diagnosis and pharmaceutical characterization to nondestructive artifact testing. Contemporary terahertz imaging systems typically rely on nonlinear optical downconversion of a fiber-based near-infrared femtosecond laser, requiring complex optical systems. Here, we demonstrate hyperspectral imaging with chip-scale frequency combs based on terahertz quantum cascade lasers. The dual combs are free-running and emit coherent terahertz radiation that covers a bandwidth of 220 GHz at 3.4 THz with $\sim 10\mathrm{\mu W}$ per line. The combination of the fast acquisition rate of dual-comb spectroscopy with the monolithic design, scalability, and chip-scale size of the combs is highly appealing for future imaging applications in biomedicine and the pharmaceutical industry.

Two semiconductor optical frequency combs, consuming less than 1 W of electrical power, are used to demonstrate high-sensitivity mid-infrared dual-comb spectroscopy in the important 3–4 μm spectral region. The devices are 4 mm long by 4 μm wide, and each emits 8 mW of average optical power. The spectroscopic sensing performance is demonstrated by measurements of methane and hydrogen chloride with optical multi-pass cell sensitivity enhancement. The system provides a spectral coverage of $33{\mathrm{cm}}^{-1}$ (1 THz), $0.32{\mathrm{cm}}^{-1}$ (9.7 GHz) frequency sampling interval, and peak signal-to-noise ratio of $\sim 100$ at 100 μs integration time. The monolithic design, low drive power, and direct generation of mid-infrared radiation are highly attractive for portable broadband spectroscopic instrumentation in future terrestrial and space applications.

Fabry-Pérot (FP) quantum cascade lasers (QCLs) provide purely electronically controlled monolithic sources for broadband mid-infrared (mid-IR) multiheterodyne spectroscopy (MHS), which benefits from the large gain bandwidth of the QCLs without sacrificing the narrowband properties commonly associated with the single mode distributed feedback variant. We demonstrate a FP-QCL based multiheterodyne spectrometer with a short-term noise-equivalent absorption of ∼3 $\times$ 10⁻⁴/$\sqrt{\mathrm{H}\mathrm{z}}$ , a mid-IR spectral coverage of 25 cm⁻¹, and very short acquisition time (10 μs) capability. The broadband potential is demonstrated by measuring the absorption spectra of ammonia and isobutane under atmospheric pressure conditions. The stability of the system is enhanced by a two-stage active frequency inter-locking procedure, where the two QCLs are pre-locked with a slow feedback loop based on an analog frequency discriminator, followed by a high bandwidth optical phase-locked loop. The locking system provides a relative frequency stability in the sub kHz range over seconds of integration time. The strength of the technique lies in the ability to acquire spectral information from all optical modes simultaneously and individually, which bodes for a versatile and cost effective spectrometer for mid-IR chemical gas sensing.

Detection of airborne chemical releases in densely populated urban environments requires precise sensors with high temporal and spatial resolution capable of covering large areas. For this purpose, we present a mobile mid-infrared quantum cascade laser dual-comb spectrometer for identification and quantification of chemical plumes. Field tests with the remote sensor were conducted during daytime in the downtown Boston area over a five day period during which chemical releases were simulated by intermittently emitting non-toxic substances. Open-air sensing was performed with retroreflectors positioned at up to 230 m distance and with sensitivities in the ppm m range for one second of averaging time. The field campaign demonstrates a step toward a semiconductor dual-comb spectroscopic sensor in the mid-infrared fingerprint region, suitable for long-term deployments. These types of sensors will be valuable complements to existing optical sensors for urban hazardous gas leak monitoring, air quality assessments, and localization of clandestine chemical production.