Abstract. We attempt for the first time to retrieve lowertropospheric vertical profile information for 8 quantities from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations. The components retrieved are the aerosol extinction coefficients at two wavelengths, 357 and 476 nm, and NO 2 , HCHO, CHOCHO, H 2 O, SO 2 , and O 3 volume mixing ratios. A Japanese MAX-DOAS profile retrieval algorithm, version 1 (JM1), is applied to observations performed at Cabauw, the Netherlands (51.97 • N, 4.93 • E), in June-July 2009 during the Cabauw Intercomparison campaign of Nitrogen Dioxide measuring Instruments (CINDI). Of the retrieved profiles, we focus here on the lowest-layer data (mean values at altitudes 0-1 km), where the sensitivity is usually highest owing to the longest light path. In support of the capability of the multi-component retrievals, we find reasonable overall agreement with independent data sets, including a regional chemical transport model (CHIMERE) and in situ observations performed near the surface (2-3 m) and at the 200-m height level of the tall tower in Cabauw. Plumes of enhanced HCHO and SO 2 were likely affected by biogenic and ship emissions, respectively, and an improvement in their emission strengths is suggested for better agreement between CHIMERE simulations and MAX-DOAS observations. Analysis of air mass factors indicates Correspondence to: H. Irie (irie@jamstec.go.jp) that the horizontal spatial representativeness of MAX-DOAS observations is about 3-15 km (depending mainly on aerosol extinction), comparable to or better than the spatial resolution of current UV-visible satellite observations and model calculations. These demonstrate that MAX-DOAS provides multi-component data useful for the evaluation of satellite observations and model calculations and can play an important role in bridging different data sets having different spatial resolutions.
[1] Bromoform (CHBr 3 ), dibromochloromethane (CHBr 2 Cl), and dibromomethane (CH 2 Br 2 ) in the atmosphere were measured at various sites, including tropical islands, the Arctic, and the open Pacific Ocean. Up to 40 ppt of bromoform was observed along the coasts of tropical islands under a sea breeze. Polybromomethane concentrations were highly correlated among the coastal samples, and the ratios CH 2 Br 2 /CHBr 3 and CHBr 2 Cl/ CHBr 3 showed a clear tendency to decrease with increasing CHBr 3 concentration. These findings are consistent with the observations that polybromomethanes are emitted mostly from macroalgae whose growth is highly localized to coastal areas and that CHBr 3 has the shortest lifetime among these three compounds. The relationship between the concentration ratios CHBr 3 /CH 2 Br 2 and CHBr 2 Cl/CH 2 Br 2 suggested a large mixing/ dilution effect on bromomethane ratios in coastal regions and yielded a rough estimate of 9 for the molar emission ratio of CHBr 3 /CH 2 Br 2 and of 0.7 for that of CHBr 2 Cl/CH 2 Br 2 . Using these ratios and an global emission estimate for CH 2 Br 2 (61 Gg/yr (Br)) calculated from its background concentration, the global emission rates of CHBr 3 and CHBr 2 Cl were calculated to be approximately 820(±310) Gg/yr (Br) and 43(±16) Gg/yr (Br), respectively, assuming that the bromomethanes ratios measured in this study are global representative. The estimated CHBr 3 emission is consistent with that estimated in a very recent study by integrating the sea-to-air flux database. Thus the contribution of CHBr 3 and CHBr 2 Cl to inorganic Br in the atmosphere is likely to be more important than previously thought. Citation: Yokouchi, Y., et al. (2005), Correlations and emission ratios among bromoform, dibromochloromethane, and dibromomethane in the atmosphere,
Abstract. In June 2009, 22 spectrometers from 14 institutes measured tropospheric and stratospheric NO 2 from the ground for more than 11 days during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI), at Cabauw, NL (51.97 • N, 4.93 • E). All visible instruments used a common wavelength range and set of cross sections for the spectral analysis. Most of the instruments were of the multi-axis design with analysis by differential spectroscopy software (MAX-DOAS), whose nonzenith slant columns were compared by examining slopes of their least-squares straight line fits to mean values of a selection of instruments, after taking 30-min averages. Zenith slant columns near twilight were compared by fits Correspondence to: H. K. Roscoe (h.roscoe@bas.ac.uk) to interpolated values of a reference instrument, then normalised by the mean of the slopes of the best instruments. For visible MAX-DOAS instruments, the means of the fitted slopes for NO 2 and O 4 of all except one instrument were within 10% of unity at almost all non-zenith elevations, and most were within 5%. Values for UV MAX-DOAS instruments were almost as good, being 12% and 7%, respectively. For visible instruments at zenith near twilight, the means of the fitted slopes of all instruments were within 5% of unity. This level of agreement is as good as that of previous intercomparisons, despite the site not being ideal for zenith twilight measurements. It bodes well for the future of measurements of tropospheric NO 2 , as previous intercomparisons were only for zenith instruments focussing on stratospheric NO 2 , with their longer heritage.Published by Copernicus Publications on behalf of the European Geosciences Union.
Abstract. For the intercomparison of tropospheric nitrogen dioxide (NO 2 ) vertical column density (VCD) data from three different satellite sensors (SCIAMACHY, OMI, and GOME-2), we use a common standard to quantitatively evaluate the biases for the respective data sets. As the standard, a regression analysis using a single set of collocated ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations at several sites in Japan and China from 2006-2011 is adopted. Examinations of various spatial coincidence criteria indicates that the slope of the regression line can be influenced by the spatial distribution of NO 2 over the area considered. While the slope varies systematically with the distance between the MAX-DOAS and satellite observation points around Tokyo in Japan, such a systematic dependence is not clearly seen and correlation coefficients are generally higher in comparisons at sites in China. On the basis of these results, we focus mainly on comparisons over China and estimate the biases in SCIAMACHY, OMI, and GOME-2 data (TM4NO2A and DOMINO version 2 products) against the MAX-DOAS observations to be −5 ± 14 %, −10 ± 14 %, and +1 ± 14 %, respectively, which are all small and insignificant. We suggest that these small biases now allow for analyses combining these satellite data for air quality studies, which are more systematic and quantitative than previously possible.
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