Airborne DOAS measurements in Arctic: vertical distributions of aerosol extinction coefficient and NO2 concentration

作者：Merlaud A^*; Van Roozendael M; Theys N; Fayt C; Hermans C; Quennehen B; Schwarzenboeck A; Ancellet G; Pommier M; Pelon J; Burkhart J; Stohl A; De Maziere M

来源：Atmospheric Chemistry and Physics, 2011, 11(17): 9219-9236.

DOI：10.5194/acp-11-9219-2011

We report on airborne Differential Optical Absorption Spectroscopy (DOAS) measurements of aerosol extinction and NO2 tropospheric profiles performed off the North coast of Norway in April 2008. The DOAS instrument was installed on the Safire ATR-42 aircraft during the POLARCAT-France spring campaign and recorded scattered light spectra in near-limb geometry using a scanning telescope. We use O-4 slant column measurements to derive the aerosol extinction at 360 nm. Regularization is based on the maximum a posteriori solution, for which we compare a linear and a logarithmic approach. The latter inherently constrains the solution to positive values and yields aerosol extinction profiles more consistent with independently measured size distributions. We present results from two soundings performed on 8 April 2008 above 71 degrees N, 22 degrees E and on 9 April 2008 above 70 degrees N, 17.8 degrees E. The first profile shows aerosol extinction and NO2 in the marine boundary layer with respective values of 0.04 +/- 0.005 km(-1) and 1.9 +/- 0.3 x 10(9) molec cm(-3). A second extinction layer of 0.01 +/- 0.003 km(-1) is found at 4 km altitude where the NO2 concentration is 0.32 +/- 0.2 x 10(9) molec cm(-3). During the second sounding, clouds prevent retrieval of profile parts under 3 km altitude but a layer with enhanced extinction (0.025 +/- 0.005 km(-1)) and NO2 (1.95 +/- 0.2 x 10(9) molec cm(-3)) is clearly detected at 4 km altitude.
From CO and ozone in-situ measurements complemented by back-trajectories, we interpret the measurements in the free troposphere as, for the first sounding, a mix between stratospheric and polluted air from Northern Europe and for the second sounding, polluted air from Central Europe containing NO2. Considering the boundary layer measurements of the first flight, modeled source regions indicate closer sources, especially the Kola Peninsula smelters, which can explain the NO2 enhancement not correlated with a CO increase at the same altitude.

• 出版日期2011