[1] Understanding the surface O 3 response over a ''receptor'' region to emission changes over a foreign ''source'' region is key to evaluating the potential gains from an international approach to abate ozone (O 3 ) pollution. We apply an ensemble of 21 global and hemispheric chemical transport models to estimate the spatial average surface O 3 response over east Asia (EA), Europe (EU), North America (NA), and south Asia (SA) to 20% decreases in anthropogenic emissions of the O 3 precursors, NO x , NMVOC, and CO (individually and combined), from each of these regions. We find that the ensemble mean surface O 3 concentrations in the base case (year 2001) simulation matches available observations throughout the year over EU but overestimates them by >10 ppb during summer and early fall over the eastern United States and Japan. The sum of the O 3 responses to NO x , CO, and NMVOC decreases separately is approximately equal to that from a simultaneous reduction of all precursors. We define a continental-scale ''import sensitivity'' as the ratio of the O 3 response to the 20% reductions in foreign versus 1 ''domestic'' (i.e., over the source region itself) emissions. For example, the combined reduction of emissions from the three foreign regions produces an ensemble spatial mean decrease of 0.6 ppb over EU (0.4 ppb from NA), less than the 0.8 ppb from the reduction of EU emissions, leading to an import sensitivity ratio of 0.7. The ensemble mean surface O 3 response to foreign emissions is largest in spring and late fall (0.7-0.9 ppb decrease in all regions from the combined precursor reductions in the three foreign regions), with import sensitivities ranging from 0.5 to 1.1 (responses to domestic emission reductions are 0.8-1.6 ppb). High O 3 values are much more sensitive to domestic emissions than to foreign emissions, as indicated by lower import sensitivities of 0.2 to 0.3 during July in EA, EU, and NA when O 3 levels are typically highest and by the weaker relative response of annual incidences of daily maximum 8-h average O 3 above 60 ppb to emission reductions in a foreign region (<10-20% of that to domestic) as compared to the annual mean response (up to 50% of that to domestic). Applying the ensemble annual mean results to changes in anthropogenic emissions from 1996 to 2002, we estimate a Northern Hemispheric increase in background surface O 3 of about 0.1 ppb a À1 , at the low end of the 0.1-0.5 ppb a À1 derived from observations. From an additional simulation in which global atmospheric methane was reduced, we infer that 20% reductions in anthropogenic methane emissions from a foreign source region would yield an O 3 response in a receptor region that roughly equals that produced by combined 20% reductions of anthropogenic NO x , NMVOC, and CO emissions from the foreign source region.

Abstract. We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe, East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosolsCorrespondence to: D. T. Shindell (dshindell@giss.nasa.gov) and CO, European emissions dominate at the Arctic surface but East Asian emissions become progressively more important with altitude, and are dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute ∼40% of total BC deposition to Greenland, with ∼20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by EuroPublished by Copernicus Publications on behalf of the European Geosciences Union. pean emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physical and chemical processing (including removal). Comparison of modeled aerosol concentrations with observations indicates problems in the models, and perhaps, interpretation of the measurements. For gas phase pollutants such as CO and O 3 , which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region and altitude examined. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions, and oxidation are comparable for European and North American sources. At higher levels, modelto-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity, though transport also contributes substantially in the mid-troposphere.

The optical spectrograph and infrared imager system (OSIRIS) on board the Odin spacecraft is designed to retrieve altitude profiles of terrestrial atmospheric minor species by observing limb-radiance profiles. The grating optical spectrograph (OS) obtains spectra of scattered sunlight over the range 280-800 nm with a spectral resolution of approximately 1 nm. The Odin spacecraft performs a repetitive vertical limb scan to sweep the OS 1 km vertical field of view over selected altitude ranges from approximately 10 to 100 km. The terrestrial absorption features that are superimposed on the scattered solar spectrum are monitored to derive the minor species altitude profiles. The spectrograph also detects the airglow, which can be used to study the mesosphere and lower thermosphere. The other part of OSIRIS is a three-channel infrared imager (IRI) that uses linear array detectors to image the vertical limb radiance over an altitude range of approximately 100 km. The IRI observes both scattered sunlight and the airglow emissions from the oxygen infrared atmospheric band at 1.27 µm and the OH (3-1) Meinel band at 1.53 µm. A tomographic inversion technique is used with a series of these vertical images to derive the two-dimensional distribution of the emissions within the orbit plane.Résumé : Le système de spectrographie optique et d'imagerie infrarouge (OSIRIS) à bord du satellite Odin est conçu pour enregistrer les profils en altitude des éléments mineurs de l'atmosphère en observant les profils de radiance du limbe. Le spectrographe optique à réseau (OS) obtient les spectres de la lumière solaire diffusée sur le domaine entre 280-800 nm, avec une résolution spatiale approximative de 1 nm. Le satellite Odin balaye verticalement le limbe de façon répétée, de telle sorte que l'ouverture verticale de 1 km du OS parcoure les domaines voulus entre 10 et 100 km. Nous analysons les spectres solaires diffusés en superposition avec les caractéristiques terrestres d'absorption, afin de déterminer les profils en altitude des éléments mineurs de l'atmosphère. Le spectrographe détecte aussi la luminescence nocturne atmosphérique qui peut être utilisé pour étudier la mésosphère et la thermosphère. L'autre partie d'OSIRIS est un imageur infrarouge (IRI) à trois canaux qui utilise une banque linéaire de détecteurs pour imager la radiance du limbe sur un domaine d'altitude d'approximativement 100 km. L'IRI observe à la fois la lumière solaire diffusée et les émissions de luminescence nocturne atmospérique provenant de la bande infrarouge de l'oxygène atmosphérique à 1.27 µm et la bande de Meinel de l'OH (3-1) à 1.53 µm. Nous utilisons une technique d'inversion tomographique avec une série de ces images verticales pour obtenir la distribution bidimensionnelle des émissions à l'intérieur de l'orbite.[Traduit par la Rédaction] Can.

Episodes of high bromine levels and surface ozone depletion in the springtime Arctic are simulated by an online air-quality model, GEM-AQ, with gas-phase and heterogeneous reactions of inorganic bromine species and a simple scheme of air-snowpack chemical interactions implemented for this study. Snowpack on sea ice is assumed to be the only source of bromine to the atmosphere and to be capable of converting relatively stable bromine species to photolabile Br₂ via air-snowpack interactions. A set of sensitivity model runs are performed for April 2001 at a horizontal resolution of approximately 100 km&times;100 km in the Arctic, to provide insights into the effects of temperature and the age (first-year, FY, versus multi-year, MY) of sea ice on the release of reactive bromine to the atmosphere. The model simulations capture much of the temporal variations in surface ozone mixing ratios as observed at stations in the high Arctic and the synoptic-scale evolution of areas with enhanced BrO column amount ("BrO clouds") as estimated from satellite observations. The simulated "BrO clouds" are in modestly better agreement with the satellite measurements when the FY sea ice is assumed to be more efficient at releasing reactive bromine to the atmosphere than on the MY sea ice. Surface ozone data from coastal stations used in this study are not sufficient to evaluate unambiguously the difference between the FY sea ice and the MY sea ice as a source of bromine. The results strongly suggest that reactive bromine is released ubiquitously from the snow on the sea ice during the Arctic spring while the timing and location of the bromine release are largely controlled by meteorological factors. It appears that a rapid advection and an enhanced turbulent diffusion associated with strong boundary-layer winds drive transport and dispersion of ozone to the near-surface air over the sea ice, increasing the oxidation rate of bromide (Br^&minus;) in the surface snow. Also, if indeed the surface snowpack does supply most of the reactive bromine in the Arctic boundary layer, it appears to be capable of releasing reactive bromine at temperatures as high as −10 °C, particularly on the sea ice in the central and eastern Arctic Ocean. Dynamically-induced BrO column variability in the lowermost stratosphere appears to interfere with the use of satellite BrO column measurements for interpreting BrO variability in the lower troposphere but probably not to the extent of totally obscuring "BrO clouds" that originate from the surface snow/ice source of bromine in the high Arctic. A budget analysis of the simulated air-surface exchange of bromine compounds suggests that a "bromine explosion" occurs in the interstitial air of the snowpack and/or is accelerated by heterogeneous reactions on the surface of wind-blown snow in ambient air, both of which are not represented explicitly in our simple model but could have been approximated by a parameter adjustment for the yield of Br₂...

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