Emissions of sulfur gases from both natural and anthropogenic sources strongly influence the chemistry of the atmosphere. To assess the relative importance of these sources we have combined the measurements of sulfur gases and fluxes during the past decade to create a global emission inventory. The inventory, which is divided into 12 latitude belts, takes into account the seasonal dependence of sulfur emissions from biogenic sources. The total emissions of sulfur gases from natural sources are approximately 0.79 Tmol S/a. These emissions are 16% of the total sulfur emissions in the Northern Hemisphere and 58% in the Southern Hemisphere. The inventory clearly shows the impact of anthropogenic sulfur emissions in the region between 35 ° and 50°N.

Two sets of global inventories of anthropogenic emissions of both oxides of sulfur and oxides of nitrogen for circa 1985 have been produced under the umbrella of the Global Emissions Inventory Activity (GEIA) of the International Global Atmospheric Chemistry Program. The two sets of inventories have different temporal, sectoral, and vertical resolution. Both were compiled using the same data sets; default data sets of global emissions have been refined via the use of more detailed regional data sets. This article reports on the compilation of the annual, one‐vertical‐level inventories, called version 1A; the inventory files are available to the scientific community via anonymous file transform protocol (FTP). Existing global inventories and regional inventories have been updated and combined on a 1° × 1° longitude/latitude grid. The resulting global anthropogenic emissions are 65 Tg S yr−1 and 21 Tg N yr−1; qualitative uncertainty estimates have been assigned on a regional basis. Emissions of both SOx and NOx are strongly localized in the highly populated and industrialized areas of eastern North America and across Europe; other smaller regions of large emissions are associated with densely populated areas with developed industries or in connection with exploitation of fuels or mineral reserves. The molar ratio of nitrogen to sulfur emissions reflects the overall character of sources; its value is generally between 0.33 and 10 for industrialized and heavily populated areas but varies over a wide range for other areas. We suggest that those requiring sulfur or nitrogen emission inventories standardize on the GEIA inventories, which we believe are authoritative and which are freely available to all users by anonymous FTP.

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[1] We present a global chemical transport model called the Integrated Massively Parallel Atmospheric Chemical Transport (IMPACT) model. This model treats chemical and physical processes in the troposphere, the stratosphere, and the climatically critical tropopause region, allowing for physically based simulations of past, present, and future ozone and its precursors. The model is driven by meteorological fields from general circulation models (GCMs) or assimilated fields representing particular time periods. It includes anthropogenic and natural emissions, advective and convective transport, vertical diffusion, dry deposition, wet scavenging, and photochemistry. Simulations presented here use meteorological fields from the National Center for Atmospheric Research (NCAR) Middle Atmospheric Community Climate Model, Version 3 (MACCM3). IMPACT simulations of radon/lead are compared to observed vertical profiles and seasonal cycles. IMPACT results for a full chemistry simulation, with approximately 100 chemical species and 300 reactions representative of a mid-1990s atmosphere, are presented. The results are compared with surface, satellite, and ozonesonde observations. The model calculates a total annual flux from the stratosphere of 663 Tg O 3 /year, and a net in situ tropospheric photochemical source (that is, production minus loss) of 161 Tg O 3 /year, with 826 Tg O 3 /year dry deposited. NO x is overpredicted in the lower midlatitude stratosphere, perhaps because model aerosol surface densities are lower than actual values or the NO x to NO y conversion rate is underpredicted. Analysis of the free radical budget shows that ozone and NO y abundances are simulated satisfactorily, as are HO x catalytic cycles and total production and removal rates for ozone.

We simulate the global cycle of reactive nitrogen in a three‐dimensional model of chemistry, transport, and deposition. Our model is based on the Lagrangian tracer model described by Walton et al. [1988] and uses winds and precipitation fields calculated by the Livermore version of the NCAR Community Climate Model. The model includes the basic chemical reactions of NO, NO2, and HNO3. For this study, we use prescribed OH and O3 concentrations and calculate the concentrations of NO, NO2, and HNO3 for a perpetual January and a perpetual July. The sources of reactive nitrogen due to fossil‐fuel combustion (22 Mt N/yr), lightning discharges (3 Mt N/yr), soil microbial activity (10 Mt N/yr), biomass burning (6 Mt N/yr), and the oxidation of N2O in the stratosphere (1 Mt N/yr) are included. Model‐predicted concentrations of NO, NO2, and HNO3 are compared to available measurements. In general, we find reasonable agreement between model predictions and measurements except for concentrations of HNO3 in the remote Pacific. At these latter locations, we require a larger source of reactive nitrogen to fit the observations. This may be supplied by lightning discharges, although increasing this source degrades our agreement with measured HNO3 abundances in the free troposphere. Alternatively, a local marine source could contribute to the measured abundances. Predictions for nitrate deposition by precipitation are within a factor of 2 of measured deposition rates in the northern hemisphere in the summer and in both seasons at remote locations. The model underpredicts nitrate deposition in winter in Europe, due primarily to the excessively strong winds generated by the general circulation model. Model simulations for NOx and HNO3 surface mixing ratios from calculations including only the fossil‐fuel source, only natural sources, and all sources acting together, are compared. Anthropogenic sources have substantially increased the concentrations of NOx and HNO3 throughout all continents during both January and July. Fossil‐fuel sources are responsible for most of this increase in the northern hemisphere, while both biomass burning and fossil‐fuel combustion contribute in the southern hemisphere.