Spectroscopy is a well-established nonintrusive tool that has played an important role in identifying and quantifying substances, from quantum descriptions to chemical and biomedical diagnostics. Challenges exist in accurate spectrum analysis in free space, which hinders us from understanding the composition of multiple gases and the chemical processes in the atmosphere. A photon-counting distributed free-space spectroscopy is proposed and demonstrated using lidar technique, incorporating a comb-referenced frequency-scanning laser and a superconducting nanowire single-photon detector. It is suitable for remote spectrum analysis with a range resolution over a wide band. As an example, a continuous field experiment is carried out over 72 h to obtain the spectra of carbon dioxide (CO2) and semi-heavy water (HDO, isotopic water vapor) in 6 km, with a range resolution of 60 m and a time resolution of 10 min. Compared to the methods that obtain only column-integrated spectra over kilometer-scale, the range resolution is improved by 2–3 orders of magnitude in this work. The CO2 and HDO concentrations are retrieved from the spectra acquired with uncertainties as low as ±1.2% and ±14.3%, respectively. This method holds much promise for increasing knowledge of atmospheric environment and chemistry researches, especially in terms of the evolution of complex molecular spectra in open areas.

A multi-frequency differential absorption lidar incorporating a tunable laser and an optical frequency comb is demonstrated for precise spectrum analysis of atmospheric gas. The single frequency tunable laser is stabilized by locking to the optical frequency comb, with a standard deviation of 0.5 MHz. To achieve a high signal-to-noise ratio, a multi-mode superconducting nanowire single-photon detector with an active-area diameter of 50 µm, a quantum efficiency of 31.5%, and dark noise of 100 counts per second is implemented, which enables to avoid the need for high energy lasers. In the experiment, the range-resolved spectrum of atmospheric mixture gases (CO2 and HDO) in a region of 1572.2 - 1572.45 nm is obtained. Results show different partially overlapped absorption of two gases in different seasons, with a stronger influence of HDO on CO2 in summer than in winter. The interactions are taken into account by separating the mixture absorption spectrum (one CO2 line and two HDO lines) with triple-peak Voigt fitting. The retrieved concentrations over 6 km with a range resolution of 120 m and a time resolution of 10 min are compared with in-situ sensors. The uncertainties of the retrieved concentrations are as low as 6.5 µmol/mol (ppm) and 1×10−3 g/kg for CO2 and HDO, respectively.

Dual-comb spectroscopy is a promising method for precise optical spectrum analysis with fast data acquisition speed. Here, avoiding using a dual-comb source, femtosecond imbalanced time-stretch spectroscopy with a simple optical layout is proposed and demonstrated. Time-stretch interferometry from one femtosecond laser builds mapping from the optical frequency domain to the radio frequency regime. In experiment, the absorption line of a hydrogen cyanide cell is encoded in the probing arm of a Mach–Zehnder interferometer (MZI). The down-converted radio frequency comb is transformed from a periodically chirped waveform, which is the interferogram of the MZI with different dispersion values on two arms. In a single measurement, the optical frequency comb with a span of 112.5 GHz is down-converted to a range of about 20.8 GHz in the radio frequency domain with a comb spacing equal to the laser repetition frequency of 100 MHz. By turning the optical filter, a spectrum range around 2 THz is analyzed. The acquired optical spectrum resolution is 540 MHz.

The monitoring and tracking of urban air pollution is a challenging environmental issue. The approach of synchronous 3-D detection of wind and pollution using a solo coherent Doppler wind lidar (CDWL) is developed and demonstrated. The 3-D distribution of pollutant is depicted by the backscatter coefficient based on signal intensity of CDWL. Then, a high-resolution wind field is derived to track the local air pollution source with its diffusion and to analyze transboundary air pollution episodes. The approach is experimentally implemented in a chemical industry park. Smoke plumes caused by point source pollutions are captured well using plan position indicator (PPI) scanning with low elevation. A typical source of pollution is located, combining the trajectory of the smoke plume and the horizontal wind vector. In addition, transboundary air pollution caused by the transport of dust storms is detected in a vertical profile scanning pattern, which is consistent with the results of national monitoring stations and backward trajectory models. Our present work provides a significant 3-D detection approach to air pollution monitoring with its sources, paths, and heights by using a solo-CDWL system.