[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 present a new model for the global tropospheric chemistry of inorganic bromine (Br y ) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Br y include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by < 1-8 nmol mol −1 (6.5 % globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4 %. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40 % higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

[1] A global three-dimensional chemical transport model has been used to simulate atmospheric bromoform using a variety of prescribed surface emission scenarios and a simple atmospheric chemistry scheme. Model simulations indicate that global emissions of bromoform calculated previously using top-down methods are too low, and emissions are likely to be significantly larger than suggested in the World Meteorological Organization's reports on the Scientific Assessment of Ozone Depletion of 1998 and 2002. Our simulations suggest that global emissions of bromoform are in the range of 400-600 GgCHBr 3 /yr and that a large proportion of emissions are situated in tropical regions. Both these factors are likely to have an important influence on estimates of the quantity of bromine transported from the surface to the lower stratosphere by short-lived bromocarbon species and its subsequent impact on ozone in this region. Further simulations including methyl bromide, bromoform and the other major short-lived bromocarbons emitted from the ocean (CH 2 Br 2 , CH 2 BrCl, CHBr 2 Cl, CHBrCl 2 ) provide estimates on the amount of reactive bromine in the troposphere and lower stratosphere derived from these compounds.