[1] Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing ''optimistic,'' ''likely,'' and ''pessimistic'' options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of À50, 180, and 300 mW m À2, compared to a CO 2 forcing over the same time period of 800-1100 mW m À2 . These values indicate the importance of air pollution emissions in short-to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%.
[1] An off-line three-dimensional tropospheric chemical transport model, parallelTropospheric Off-Line Model of Chemistry and Transport (p-TOMCAT), has been extended by incorporating a detailed bromine chemistry scheme that contains gas-phase reactions and heterogeneous reactions on both cloud particles and background aerosols. Bromine emission from bromocarbon photo-oxidation and from sea-salt bromine depletion and bromine removal through dry and wet deposition are included. Using this model, tropospheric bromine chemistry and ozone budgets are studied. The zonal mean of the inorganic gas-phase bromine compounds (Br x ) is calculated to be high (4-8 pptv) in the lower troposphere of the midlatitudes to high latitudes in each hemisphere, with decreasing trends with altitude (down to $2-3 pptv in the upper troposphere). The lowest Br x (<2 pptv) is over low latitudes, corresponding to small sea-salt Br emission and a high rate of precipitation scavenging. A mean lifetime of $5 days is obtained for the tropospheric Br x . Sea-salt emission plays the dominant role in total Br x in the lower troposphere while organic Br-containing compounds are important in upper layers. High daytime BrO mixing ratios (>1 pptv) are found over the high-latitude ocean surface, corresponding to high tropospheric column BrO values of up to 1.6 Â 10 13 molecules/cm 2 in the monthly mean. The addition of bromine chemistry to the model leads to a reduction in tropospheric ozone amounts by 4-6% in the Northern Hemisphere and up to $30% in the Southern Hemisphere high latitudes. The net ozone loss depends not only on total Br x , but also on solar irradiance, especially at high latitudes. The hydrolysis reaction of bromine nitrate, which occurs on cloud and aerosol surfaces (BrONO 2 + H 2 O aq ! HOBr + HNO 3 ), has a significant influence on ozone chemistry through its effect on NO x as well as on reactive BrO and Br.
[1] We analyze present-day and future carbon monoxide (CO) simulations in 26 state-ofthe-art atmospheric chemistry models run to study future air quality and climate change. In comparison with near-global satellite observations from the MOPITT instrument and local surface measurements, the models show large underestimates of Northern Hemisphere (NH) extratropical CO, while typically performing reasonably well elsewhere. The results suggest that year-round emissions, probably from fossil fuel burning in east Asia and seasonal biomass burning emissions in south-central Africa, are greatly underestimated in current inventories such as IIASA and EDGAR3.2. Variability among models is large, likely resulting primarily from intermodel differences in representations and emissions of nonmethane volatile organic compounds (NMVOCs) and in hydrologic cycles, which affect OH and soluble hydrocarbon intermediates. Global mean projections of the 2030 CO response to emissions changes are quite robust. Global mean midtropospheric (500 hPa) CO increases by 12.6 ± 3.5 ppbv (16%) for the high-emissions (A2) scenario, by 1.7 ± 1.8 ppbv (2%) for the midrange (CLE) scenario, and decreases by 8.1 ± 2.3 ppbv (11%) for the low-emissions (MFR) scenario. Projected 2030 climate changes decrease global 500 hPa CO by 1.4 ± 1.4 ppbv. Local changes can be much larger. In response to climate change, substantial effects are seen in the tropics, but intermodel variability is quite large. The regional CO responses to emissions changes are robust across models, however. These range from decreases of 10-20 ppbv over much of the industrialized NH for the CLE scenario to CO increases worldwide and year-round under A2, with the 1 of 24 largest changes over central , southern Brazil (20-35 ppbv) and south and east Asia (30-70 ppbv). The trajectory of future emissions thus has the potential to profoundly affect air quality over most of the world's populated areas.Citation: Shindell, D. T., et al. (2006), Multimodel simulations of carbon monoxide: Comparison with observations and projected near-future changes,
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