Emissions from fossil fuel combustion and biomass burning reduce local air quality and affect global tropospheric chemistry. Nitrogen oxides are emitted by all combustion processes and play a key part in the photochemically induced catalytic production of ozone, which results in summer smog and has increased levels of tropospheric ozone globally. Release of nitrogen oxide also results in nitric acid deposition, and--at least locally--increases radiative forcing effects due to the absorption of downward propagating visible light. Nitrogen oxide concentrations in many industrialized countries are expected to decrease, but rapid economic development has the potential to increase significantly the emissions of nitrogen oxides in parts of Asia. Here we present the tropospheric column amounts of nitrogen dioxide retrieved from two satellite instruments GOME and SCIAMACHY over the years 1996-2004. We find substantial reductions in nitrogen dioxide concentrations over some areas of Europe and the USA, but a highly significant increase of about 50 per cent-with an accelerating trend in annual growth rate-over the industrial areas of China, more than recent bottom-up inventories suggest.

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Gaseous elemental mercury (Hg0) is a globally distributed air toxin with a long atmospheric residence time. Any process that reduces its atmospheric lifetime increases its potential accumulation in the biosphere. Our data from Barrow, AK, at 71 degrees N show that rapid, photochemically driven oxidation of boundary-layer Hg0 after polar sunrise, probably by reactive halogens, creates a rapidly depositing species of oxidized gaseous mercury in the remote Arctic troposphere at concentrations in excess of 900 pg m(-3). This mercury accumulates in the snowpack during polar spring at an accelerated rate in a form that is bioavailable to bacteria and is released with snowmelt during the summer emergence of the Arctic ecosystem. Evidence suggests that this is a recent phenomenon that may be occurring throughout the earth's polar regions.

Abstract. We present an improved tropospheric nitrogen dioxide column retrieval algorithm (DOMINO v2.0) for OMI based on better air mass factors (AMFs) and a correction for across-track stripes resulting from calibration errors in the OMI backscattered reflectances. Since October 2004, NO 2 retrievals from the Ozone Monitoring Instrument (OMI), a UV/Vis nadir spectrometer onboard NASA's EOSAura satellite, have been used with success in several scientific studies focusing on air quality monitoring, detection of trends, and NO x emission estimates. Dedicated evaluations of previous DOMINO tropospheric NO 2 retrievals indicated their good quality, but also suggested that the tropospheric columns were susceptible to high biases (by 0-40 %), probably because of errors in the air mass factor calculations. Here we update the DOMINO air mass factor approach. We calculate a new look-up table (LUT) for altitude-dependent AMFs based on more realistic atmospheric profile parameters, and include more surface albedo and surface pressure reference points than before. We improve the sampling of the TM4 model, resulting in a priori NO 2 profiles that are better mixed throughout the boundary layer. We evaluate the NO 2 profiles simulated with the improved TM4 sampling as used in the AMF calculations and show that they are highly consistent with in situ NO 2 measurements from aircraft during the INTEX-A and INTEX-B campaigns in 2004 and 2006. Our air mass factor calculations are furCorrespondence to: Folkert Boersma (boersma@knmi.nl) ther updated by the implementation of a high-resolution terrain height and a high-resolution surface albedo climatology based on OMI measurements. Together with a correction for across-track stripes, the overall impact of the improved terrain height and albedo descriptions is modest (<5 %) on average over large polluted areas, but still causes significant changes locally. The main changes in the DOMINO v2.0 algorithm follow from the new LUT and the improved TM4 sampling that results in more NO 2 simulated aloft, where sensitivity to NO 2 is higher, and amount to reductions in tropospheric NO 2 columns of up to 20 % in winter, and 10 % in summer over extended polluted areas. We investigate the impact of aerosols on the NO 2 retrieval, and based on a comparison of concurrent retrievals of clouds from OMI and aerosols from MODIS Aqua, we find empirical evidence that OMI cloud retrievals are sensitive to the presence of scattering aerosols. It follows that an implicit correction for the effects of aerosols occurs through the aerosol-induced cloud parameters in DOMINO, and we show that such an empirical correction amounts to a 20 % AMF reduction in summer and ±10 % changes in winter over the eastern United States.

[1] A rapid increase of NO 2 columns over China has been observed by satellite instruments in recent years. We present a 10-a regional trend of NO x emissions in China from 1995 to 2004 using a bottom-up methodology and compare the emission trends with the NO 2 column trends observed from GOME and SCIAMACHY, the two spaceborne instruments. We use a dynamic methodology to reflect the dramatic change in China's NO x emissions caused by energy growth and technology renewal. We use a scenario analysis approach to identify the possible sources of uncertainties in the current bottom-up inventory, in comparison with the satellite observation data. Our best estimates for China's NO x emissions are 10.9 Tg in 1995 and 18.6 Tg in 2004, increasing by 70% during the period considered. NO x emissions and satellite-based NO 2 columns show broad agreement in temporal evolution and spatial distribution. Both the emission inventory data and the satellite observations indicate a continuous and accelerating growth rate between 1996 and 2004 over east central China. However, the growth rate from the emission inventory is lower than that from the satellite observations. From 1996 to 2004, NO x emissions over the region increased by 61% according to the inventory, while a 95% increase in the NO 2 columns measured by satellite was observed during the same period. We found good agreement during summertime but a large discrepancy during wintertime. The consistency between the summertime trends suggests that the bias cannot be due to systematic error of activity data or emission factors. The reasons for the discrepancy cannot yet be fully identified, but possible explanations include an underestimation in seasonal emission variations, variability of meteorology, NO x injection height, and the increasing trend of sulfate aerosols.

During springtime in the polar regions, unique photochemistry converts inert halide salt ions (e.g. Br⁻) into reactive halogen species (e.g. Br atoms and BrO) that deplete ozone in the boundary layer to near zero levels. Since their discovery in the late 1980s, research on ozone depletion events (ODEs) has made great advances; however many key processes remain poorly understood. In this article we review the history, chemistry, dependence on environmental conditions, and impacts of ODEs. This research has shown the central role of bromine photochemistry, but how salts are transported from the ocean and are oxidized to become reactive halogen species in the air is still not fully understood. Halogens other than bromine (chlorine and iodine) are also activated through incompletely understood mechanisms that are probably coupled to bromine chemistry. The main consequence of halogen activation is chemical destruction of ozone, which removes the primary precursor of atmospheric oxidation, and generation of reactive halogen atoms/oxides that become the primary oxidizing species. The different reactivity of halogens as compared to OH and ozone has broad impacts on atmospheric chemistry, including near complete removal and deposition of mercury, alteration of oxidation fates for organic gases, and export of bromine into the free troposphere. Recent changes in the climate of the Arctic and state of the Arctic sea ice cover are likely to have strong effects on halogen activation and ODEs; however, more research is needed to make meaningful predictions of these changes

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Elemental stoichiometry constitutes an inherent link between biogeochemistry and the structure and processes within food webs, and thus is at the core of ecosystem functioning.