Megacities are immense sources of air pollutants, with large impacts on air quality and climate. However, emission inventories in many of them still are highly uncertain, particularly in developing countries. Satellite observations allow top-down estimates of emissions to be made for nitrogen oxides (NO(x) = NO + NO(2)), but require poorly quantified a priori information on the NO(x) lifetime. We present a method for the simultaneous determination of megacity NO(x) emissions and lifetimes from satellite measurements by analyzing the downwind patterns of NO(2) separately for different wind conditions. Daytime lifetimes are ~4 hours at low and mid-latitudes, but ~8 hours in wintertime for Moscow. The derived NO(x) emissions are generally in good agreement with existing emission inventories, but are higher by a factor of 3 for the Saudi Arabian capital Riyadh.

[1] The first global simultaneous observations of glyoxal (CHOCHO) and formaldehyde (HCHO) columns retrieved from measurements by the Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) satellite instrument are presented and compared to model calculations. The global pattern of the distribution of CHOCHO is similar to that of HCHO. High values are observed over areas with large biogenic isoprene emissions (Central Africa, parts of South America, and Indonesia). Also regions with biomass burning and anthropogenic pollution exhibit elevated levels of CHOCHO. The ratio of the columns of CHOCHO to HCHO is generally of the order of 0.05 in regions having biogenic emissions, which is in reasonable agreement with the current understanding of the oxidation of hydrocarbons emitted by the biosphere. However and in contrast to our model, high values of both HCHO and CHOCHO are also observed over areas of the tropical oceans. This is tentatively attributed to outflow from the continents and local oceanic biogenic sources of the precursors of HCHO and CHOCHO.

Abstract. Nitrogen oxides (NO+NO 2 =NO x and reservoir species) are important trace gases in the troposphere with impact on human health, atmospheric chemistry and climate. Besides natural sources (lightning, soil emissions) and biomass burning, fossil fuel combustion is estimated to be responsible for about 50% of the total production of NO x . Since human activity in industrialized countries largely follows a seven-day cycle, fossil fuel combustion is expected to be reduced during weekends. This "weekend effect" is well known from local, ground based measurements, but has never been analysed on a global scale before.The Global Ozone Monitoring Experiment (GOME) on board the ESA-satellite ERS-2 allows measurements of NO 2 column densities. By estimating and subtracting the stratospheric column, and considering radiative transfer, vertical column densities (VCD) of tropospheric NO 2 can be determined (e.g. Leue et al., 2001). We demonstrate the statistical analysis of weekly cycles of tropospheric NO 2 VCDs for different regions of the world. In the cycles of the industrialized regions and cities in the US, Europe and Japan a clear Sunday minimum of tropospheric NO 2 VCD can be seen. Sunday NO 2 VCDs are about 25-50% lower than working day levels. Metropolitan areas with other religious and cultural backgrounds (Jerusalem, Mecca) show different weekly patterns corresponding to different days of rest. In China, no weekly pattern can be found.The presence of a weekly cycle in the measured tropospheric NO 2 VCD may help to identify the different anthropogenic source categories. Furthermore, we estimated the lifetime of tropospheric NO 2 by analysing the mean weekly cycle exemplarily over Germany, obtaining a value of about 6 h in summer and 18-24 h in winter.

Abstract. Ground-based measurements of scattered sunlight by the Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) have been carried out at an urban site (39.95° N, 116.32° E) in Beijing megacity since 6 August 2008. In this study, we retrieved the tropospheric NO2 vertical column densities (VCDs) over Beijing from these MAX-DOAS observations from August 2008 to September 2011. Over this period, the daytime (08:00–17:00 Beijing Time (BJT, which equals UTC + 8)) mean tropospheric NO2 VCDs varied from 0.5 to 13.3 with an average of 3.6 during summertime, and from 0.2 to 16.8 with an average of 5.8 during wintertime, all in units of 1016 molecules cm−2. The average diurnal variation patterns of tropospheric NO2 over Beijing appeared to be rather different from one season to another, indicating differences in the emission strength and atmospheric lifetime. In contrast to previous studies, we find a small weekly cycle of the tropospheric NO2 VCD over Beijing. The NO2 VCD in the late afternoon was the largest on Saturday and the lowest on Sunday, and in the morning it reached a clear maximum on Wednesday. We also find a post-Olympic Games effect, with 39–54% decrease in the tropospheric NO2 VCD over Beijing estimated for August of 2008, compared to the following years. The tropospheric NO2 VCDs derived by our ground MAX-DOAS measurements show a good correlation with SCIAMACHY and OMI satellite data. However, compared with the MAX-DOAS measurements, the satellite observations underestimate the tropospheric NO2 VCDs over Beijing systematically, by 43% for SCIAMACHY and 26–38% for OMI (DOMINO v2.0 and DOMINO v1.02). Based on radiative transfer simulations, we show that the aerosol shielding effect can explain this underestimation, while the gradient smoothing effect caused by the coarse spatial resolution of the satellite observations could play an additional role.

Abstract. We present a new method to quantify NOx emissions and corresponding atmospheric lifetimes from OMI NO2 observations together with ECMWF wind fields without further model input for sources located in a polluted background. NO2 patterns under calm wind conditions are used as proxy for the spatial patterns of NOx emissions, and the effective atmospheric NOx lifetime is determined from the change of spatial patterns measured at larger wind speeds. Emissions are subsequently derived from the NO2 mass above the background, integrated around the source of interest. Lifetimes and emissions are estimated for 17 power plants and 53 cities located in non-mountainous regions across China and the USA. The derived lifetimes for the ozone season (May–September) are 3.8 ± 1.0 h (mean ± standard deviation) with a range of 1.8 to 7.5 h. The derived NOx emissions show generally good agreement with bottom-up inventories for power plants and cities. Regional inventory shows better agreement with top-down estimates for Chinese cities compared to global inventory, most likely due to different downscaling approaches adopted in the two inventories.

Abstract. In May 2003, severe forest fires in southeast Russia resulted in smoke plumes extending widely across the Northern Hemisphere. This study combines satellite data from a variety of platforms (Moderate Resolution Imaging Spectroradiometer (MODIS), Sea-viewing Wide Field-of-view Sensor (SeaWiFS), Earth Probe Total Ozone Mapping Spectrometer (TOMS) and Global Ozone Monitoring Experiment (GOME)) and vertical aerosol profiles derived with Raman lidar measurements with results from a Lagrangian particle dispersion model to understand the transport processes that led to the large haze plumes observed over North America and Europe. The satellite images provided a unique opportunity for validating model simulations of tropospheric transport on a truly hemispheric scale. Transport of the smoke occurred in two directions: Smoke travelling northwestwards towards Scandinavia was lifted over the Urals and arrived over the Norwegian Sea. Smoke travelling eastwards to the Okhotsk Sea was also lifted, it then crossed the Bering Sea to Alaska from where it proceeded to Canada and was later even observed over Scandinavia and Eastern Europe on its way back to Russia. Not many events of this kind, if any, have been observed, documented and simulated with a transport model comprehensively. The total transport time was about 17 days. We compared transport model simulations using meteorological analysis data from both the European Centre for Medium-Range Weather Forecast (ECMWF) and the National Center for Environmental Prediction (NCEP) in order to find out how well this event could be simulated using these two datasets. Although differences between the two simulations are found on small scales, both agree remarkably well with each other and with the observations on large scales. On the basis of the available observations, it cannot be decided which simulation was more realistic.

Power plant exhausts can be identified and quantified from satellite observations.

Abstract. Global observations of tropospheric nitrogen dioxide (NO2) columns have been shown to be feasible from space, but consistent multi-sensor records do not yet exist, nor are they covered by planned activities at the international level. Harmonised, multi-decadal records of NO2 columns and their associated uncertainties can provide crucial information on how the emissions and concentrations of nitrogen oxides evolve over time. Here we describe the development of a new, community best-practice NO2 retrieval algorithm based on a synthesis of existing approaches. Detailed comparisons of these approaches led us to implement an enhanced spectral fitting method for NO2, a 1°  ×  1° TM5-MP data assimilation scheme to estimate the stratospheric background and improve air mass factor calculations. Guided by the needs expressed by data users, producers, and WMO GCOS guidelines, we incorporated detailed per-pixel uncertainty information in the data product, along with easily traceable information on the relevant quality aspects of the retrieval. We applied the improved QA4ECV NO2 algorithm to the most current level-1 data sets to produce a complete 22-year data record that includes GOME (1995–2003), SCIAMACHY (2002–2012), GOME-2(A) (2007 onwards) and OMI (2004 onwards). The QA4ECV NO2 spectral fitting recommendations and TM5-MP stratospheric column and air mass factor approach are currently also applied to S5P-TROPOMI. The uncertainties in the QA4ECV tropospheric NO2 columns amount to typically 40 % over polluted scenes. The first validation results of the QA4ECV OMI NO2 columns and their uncertainties over Tai'an, China, in June 2006 suggest a small bias (−2 %) and better precision than suggested by uncertainty propagation. We conclude that our improved QA4ECV NO2 long-term data record is providing valuable information to quantitatively constrain emissions, deposition, and trends in nitrogen oxides on a global scale.