A spectroscopic method of molecular detection based on dispersion measurements using a frequency-chirped laser source is presented. An infrared quantum cascade laser emitting around 1912 cm⁻¹ is used as a tunable spectroscopic source to measure dispersion that occurs in the vicinity of molecular ro-vibrational transitions. The sample under study is a mixture of nitric oxide in dry nitrogen. Two experimental configurations based on a coherent detection scheme are investigated and discussed. The theoretical models, which describe the observed spectral signals, are developed and verified experimentally. The method is particularly relevant to optical sensing based on mid-infrared quantum cascade lasers as the high chirp rates available with those sources can significantly enhance the magnitude of the measured dispersion signals. The method relies on heterodyne beatnote frequency measurements and shows high immunity to variations in the optical power received by the photodetector.

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.

A transportable prototype Faraday rotation spectroscopic system based on a tunable external cavity quantum cascade laser has been developed for ultrasensitive detection of nitric oxide (NO). A broadly tunable laser source allows targeting the optimum Q _3/2 (3/2) molecular transition at 1875.81 cm ⁻¹ of the NO fundamental band. For an active optical path of 44 cm and 1-s lock-in time constant minimum NO detection limits (1σ) of 4.3 parts per billion by volume (ppbv) and 0.38 ppbv are obtained by using a thermoelectrically cooled mercury–cadmium–telluride photodetector and liquid nitrogen-cooled indium–antimonide photodetector, respectively. Laboratory performance evaluation and results of continuous, unattended monitoring of atmospheric NO concentration levels are reported.

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.

In this paper we present a prototype instrument for remote open-path detection of nitrous oxide. The sensor is based on a 4.53 μm quantum cascade laser and uses the chirped laser dispersion spectroscopy (CLaDS) technique for molecular concentration measurements. To the best of our knowledge this is the first demonstration of open-path laser-based trace-gas detection using a molecular dispersion measurement. The prototype sensor achieves a detection limit down to the single-ppbv level and exhibits excellent stability and robustness. The instrument characterization, field deployment performance, and the advantages of applying dispersion sensing to sensitive trace-gas detection in a remote open-path configuration are presented.