Abstract. The April-May, 2010 volcanic eruptions of Eyjafjallajökull, Iceland caused significant economic and social disruption in Europe whilst state of the art measurements and ash dispersion forecasts were heavily criticized by the aviation industry. Here we demonstrate for the first time that large improvements can be made in quantitative predictions of the fate of volcanic ash emissions, by using an inversion scheme that couples a priori source information and the output of a Lagrangian dispersion model with satellite data to estimate the volcanic ash source strength as a function of altitude and time. From the inversion, we obtain a total fine ash emission of the eruption of 8.3±4.2 Tg for particles in the size range of 2.8-28 µm diameter. We evaluate the results of our model results with a posteriori ash emissions using independent ground-based, airborne and space-borne measurements both in case studies and statistically. Subsequently, we estimate the area over Europe affected by volcanic ash above certain concentration thresholds relevant for the aviation industry. We find that during three episodes in April and May, volcanic ash concentrations at some altitude in the atmosphere exceeded the limits for the "Normal" flying zone in up to 14 % (6-16 %), 2 % (1-3 %) and 7 % (4-11 %), respecCorrespondence to: A. Stohl (ast@nilu.no) tively, of the European area. For a limit of 2 mg m −3 only two episodes with fractions of 1.5 % (0.2-2.8 %) and 0.9 % (0.1-1.6 %) occurred, while the current "No-Fly" zone criterion of 4 mg m −3 was rarely exceeded. Our results have important ramifications for determining air space closures and for real-time quantitative estimations of ash concentrations. Furthermore, the general nature of our method yields better constraints on the distribution and fate of volcanic ash in the Earth system.

Abstract. Atmospheric remote sounding from satellites is an essential component of the observational strategy deployed to monitor atmospheric pollution and changing composition. The IASI nadir looking thermal infrared sounder onboard MetOp will provide 15 years of global scale observations for a series of key atmospheric species, with unprecedented spatial sampling and coverage. This paper gives an overview of the instrument's capability for measuring atmospheric composition in the perspective of chemistry and air quality. The assessment is made in terms of species, accuracy and vertical information. Global distributions are presented for CO, CH 4 , O 3 (total and tropospheric), HNO 3 , NH 3 , and volcanic SO 2 . Local distributions of organic species measured during fire events, such as C 2 H 4 , CH 3 OH, HCOOH, and PAN are also shown. For each species or process, the link is made to specialized papers in this issue.

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Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

International audienceExisting descriptions of bi-directional ammonia (NH3) land-atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH3 emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH3 emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH3 monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH3 emission-deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28-67%). Together with increased anthropogenic activity, global NH3 emissions may increase from 65 (45-85) Tg N in 2008 to reach 132 (89-179) Tg by 2100

International audienc

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Through its important role in the formation of particulate matter, atmospheric ammonia affects air quality and has implications for human health and life expectancy 1,2. Excess ammonia in the environment also contributes to the acidification and eutrophication of ecosystems 3-5 and to climate change 6. Anthropogenic emissions dominate natural ones and mostly originate from agricultural, domestic and industrial activities 7. However, the total ammonia budget and the attribution of emissions to specific sources remain highly uncertain across different spatial scales 7-9. Here we identify, categorize and quantify the world's ammonia emission hotspots using a high-resolution map of atmospheric ammonia obtained from almost a decade of daily IASI satellite observations. We report 248 hotspots with diameters smaller than 50 kilometres, which we associate with either a single point source or a cluster of agricultural and industrial point sources-with the exception of one hotspot, which can be traced back to a natural source. The state-of-the-art EDGAR emission inventory 10 mostly agrees with satellitederived emission fluxes within a factor of three for larger regions. However, it does not adequately represent the majority of point sources that we identified and underestimates the emissions of two-thirds of them by at least one order of magnitude. Industrial emitters in particular are often found to be displaced or missing. Our results suggest that it is necessary to completely revisit the emission inventories of anthropogenic ammonia sources and to account for the rapid evolution of such sources over time. This will lead to better health and environmental impact assessments of atmospheric ammonia and the implementation of suitable nitrogen management strategies. Considerable effort goes into establishing spatially and temporally resolved ammonia (NH 3) bottom-up emission inventories, as these are critical drivers of models that are used to assess NH 3 distributions and impacts on the environment. Bottom-up inventories are built from activity data coupled with estimated emission factors. The correctness of these input data is their Achilles' heel, as activity data can be absent or outdated and estimated emission factors are based on specific case studies and may not be representative of either local or global conditions 11,12. When they are available, global measured atmospheric distributions of trace gas concentrations allow us to retrieve source emissions. In the past few years, satellite sounders have offered (bi) daily global NH 3 measurements 13-17 , which have a huge potential to improve our knowledge of the NH 3 emission budget 18. The first global distributions 13 and inverse modelling efforts 19 have confirmed the correctness of the location of the large source regions in the inventories, but have also revealed likely underestimates in the magnitude of their emissions, especially in the Northern Hemisphere. A regional study 20 has highlighted the advantage of averaging data to reveal smaller, localized NH 3 point...