A rapid method to derive horizontal distributions of trace gases and aerosols near the surface using multi-axis differential optical absorption spectroscopy

摘要

We apply a novel experimental procedure for the rapid measurement of the average volume mixing ratios (VMRs) and horizontal distributions of trace gases such as NO_2, SO_2, and HCHO in the boundary layer, which was recently suggested by Sinreich et al. (2013). The method is based on two-dimensional scanning multi-axis differential optical absorption spectroscopy (MAX-DOAS). It makes use of two facts (Sinreich et al., 2013): first, the light path for observations at 1° elevation angle traverses mainly air masses located close to the ground (typically < 200 m); second, the light path length can be calculated using the simultaneous measured absorption of the oxygen dimer O_4. Thus, the average value of the trace gas VMR in the atmospheric layer between the surface and the particular altitude, for which this observation was sensitive, can be calculated. Compared to the originally proposed method, we introduce several important modifications and improvements: We apply the method only to measurements at 1° elevation angle (besides zenith view), for which the uncertainties of the retrieved values of the VMRs and surface extinctions are especially small. Using only 1° elevation angle for off-axis observation also allows an increased temporal resolution. We determine (and apply) correction factors (and their uncertainties) directly as function of the measured O_4 absorption. Finally, the method is extended to trace gases analysed at other wavelengths and also to the retrieval of aerosol extinction. Depending on atmospheric visibility, the typical uncertainty of the results ranges from about 20% to 30%. We apply the rapid method to observations of a newly-developed ground-based multifunctional passive differential optical absorption spectroscopy (GM-DOAS) instrument in the north-west outskirts near Hefei in China. We report NO_2, SO_2, and HCHO VMRs and aerosol extinction for four azimuth angles and compare these results with those from simultaneous long-path DOAS observations. Good agreement is found (squares of the correlation coefficients for NO_2, SO_2, and HCHO were 0.92, 0.85, and 0.60, respectively), verifying the reliability of this novel method. Similar agreement is found for the comparison of the aerosol extinction with results from visibility meters. Future studies may conduct measurements using a larger number of azimuth angles to increase the spatial resolution.