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.

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The refractive index structure constant (Cn2) is a key parameter used in describing the influence of turbulence on laser transmissions in the atmosphere. Three different methods for estimating Cn2 were analyzed in detail. A new method that uses a combination of these methods for continuous Cn2 profiling with both high temporal and spatial resolution is proposed and demonstrated. Under the assumption of the Kolmogorov “2/3 law”, the Cn2 profile can be calculated by using the wind field and turbulent kinetic energy dissipation rate (TKEDR) measured by coherent Doppler wind lidar (CDWL) and other meteorological parameters derived from a microwave radiometer (MWR). In a horizontal experiment, a comparison between the results from our new method and measurements made by a large aperture scintillometer (LAS) is conducted. The correlation coefficient, mean error, and standard deviation between them in a six-day observation are 0.8073, 8.18 × 10−16 m−2/3, and 1.27 × 10−15 m−2/3, respectively. In the vertical direction, the continuous profiling results of Cn2 and other turbulence parameters with high resolution in the atmospheric boundary layer (ABL) are retrieved. In addition, the limitation and uncertainty of this method under different circumstances were analyzed, which shows that the relative error of Cn2 estimation normally does not exceed 30% under the convective boundary layer (CBL).

Abstract. The refractive index structure constant (Cn2) is a key parameter in describing the influence of turbulence on laser transmission in the atmosphere. A new method for continuous Cn2 profiling with both high temporal and spatial resolution is proposed and demonstrated. Under the assumption of the Kolmogorov “2/3 law”, the Cn2 profile can be calculated by using the wind field and turbulent kinetic energy dissipation rate (TKEDR) measured by coherent Doppler wind lidar (CDWL) and other meteorological parameters derived from microwave radiometer (MWR). In the horizontal experiment, a comparison between the results from our new method and measurements made by a large aperture scintillometer (LAS) is conducted. Except for the period of stratification stabilizing, the correlation coefficient between them in the six-day observation is 0.8389, the mean error and standard deviation is 1.09 × 10−15 m−2/3 and 2.14 × 10−15 m−2/3, respectively. In the vertical direction, the continuous observation results of Cn2 and other turbulence parameter profiles in the atmospheric boundary layer (ABL) are retrieved. More details of the atmospheric turbulence can be found in the ABL owe to the high temporal and spatial resolution of MWR and CDWL (spatial resolution of 26 m, temporal resolution of 147 s).