Summary for policymakers Technical summary 1. The climate system - an overview 2. Observed climate variability and change 3. The carbon cycle and atmospheric CO2 4. Atmospheric chemistry and greenhouse gases 5. Aerosols, their direct and indirect effects 6. Radiative forcing of climate change 7. Physical climate processes and feedbacks 8. Model evaluation 9. Projections of future climate change 10. Regional climate simulation - evaluation and projections 11. Changes in sea level 12. Detection of climate change and attribution of causes 13. Climate scenario development 14. Advancing our understanding Glossary Index Appendix.

Climate change 2001: the scientific basis

We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.

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Global modeling of tropospheric chemistry with assimilated meteorology : Model description and evaluation

This paper reviews the many developments in estimates of the direct and indirect global annual mean radiative forcing due to present-day concentra- tions of anthropogenic tropospheric aerosols since Inter- governmental Panel on Climate Change (1996). The range of estimates of the global mean direct radiative forcing due to six distinct aerosol types is presented. Addition- ally, the indirect effect is split into two components corresponding to the radiative forcing due to modifica- tion of the radiative properties of clouds (cloud albedo effect) and the effects of anthropogenic aerosols upon the lifetime of clouds (cloud lifetime effect). The radia- tive forcing for anthropogenic sulphate aerosol ranges from 20.26 to 20.82 W m 22 . For fossil fuel black carbon the radiative forcing ranges from 10.16 W m 22 for an external mixture to 10.42 W m 22 for where the black carbon is modeled as internally mixed with sulphate aerosol. For fossil fuel organic carbon the two estimates of the likely weakest limit of the direct radiative forcing are 20.02 and 20.04 W m 22 . For biomass-burning sources of black carbon and organic carbon the com-

https://agupubs.onlinelibrary.wiley.com/doi/pdf/10.1029/1999RG000078

Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review

Simulation results of global aerosol models have been assembled in the framework of the AeroCom intercomparison exercise. In this paper, we analyze the life cycles of dust, sea salt, sulfate, black carbon and particulate organic matter as simulated by sixteen global aerosol models. The differences among the results (model diversities) for sources and sinks, burdens, particle sizes, water uptakes, and spatial dispersals have been established. These diversities have large consequences for the calculated radiative forcing and the aerosol concentrations at the surface. Processes and parameters are identified which deserve further research. The AeroCom all-models-average emissions are dominated by the mass of sea salt (SS), followed by dust (DU), sulfate (SO 4 ), particulate organic matter (POM), and finally black carbon (BC). Interactive parameterizations of the emissions and contrasting particles sizes of SS and DU lead generally to higher diversities of these species, and for total aerosol. The lower diversity of the emissions of the fine aerosols, BC, POM, and SO 4 , is due to the use of similar emission inventories, and does therefore not necessarily indicate a better understanding of their sources. The diversity of SO 4 -sources is mainly caused by the disagreement on depositional loss of precursor gases and on chemical production. The diversities of the emissions are passed on to the burdens, but the latter are also strongly affected by the model-specific treatments of transport and aerosol processes. The burdens of dry masses decrease from largest to smallest: DU, SS, SO 4 , POM, and BC. The all-models-average residence time is shortest for SS with about half a day, followed by SO 4 and DU with four days, and POM and BC with six and seven days, respectively. The wet deposition rate is controlled by the solubility and increases from DU, BC, POM to SO 4 and SS. It is the dominant sink for SO 4 , BC, and POM, and contributes about one third to the total removal of SS and DU species. For SS and DU we find high diversities for the removal rate coefficients and deposition pathways. Models do neither agree on the split between wet and dry deposition, nor on that between sedimentation and other dry deposition processes. We diagnose an extremely high diversity for the uptake of ambient water vapor that influences the particle size and thus the sink rate coefficients. Furthermore, we find little agreement among the model results for the partitioning of wet removal into scavenging by convective and stratiform rain. Large differences exist for aerosol dispersal both in the vertical and in the horizontal direction. In some models, a minimum of total aerosol concentration is simulated at the surface. Aerosol dispersal is most pronounced for SO 4 and BC and lowest for SS. Diversities are higher for meridional than for vertical dispersal, they are similar for the individual species and highest for SS and DU. For these two components we do not find a correlation between vertical and meridional aerosol dispersal. In addition the degree of dispersals of SS and DU is not related to their residence times. SO 4 , BC, and POM, however, show increased meridional dispersal in models with larger vertical dispersal, and dispersal is larger for longer simulated residence times.

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Analysis and quantification of the diversities of aerosol life cycles within AeroCom

A global three-dimensional model of the troposphere is used to simulate the sources, abundances, and sinks of mineral aerosol and the species involved in the photochemical oxidant, nitrogen, and sulfur cycles. Although the calculated heterogeneous removal rates on mineral aerosol are highly uncertain, mainly due to poorly known heterogeneous reaction rates, the reaction of SO2 on calcium-rich mineral aerosol is likely to play an important role downwind of arid source regions. This is especially important for regions in Asia, which are important and increasing emitters of sulfur compounds. Our results indicate that the assumption that sulfate aerosol follows an accumulation mode size distribution, is particularly in Asia likely to overestimate the sulfate aerosol climate-cooling effect. An even larger fraction of gas phase nitric acid may be associated with and neutralized by mineral aerosol. Interactions of N2O5, O3, and HO2-radicals with dust are calculated to affect the photochemical oxidant cycle, causing ozone decreases up to 10% in and nearby the dust source areas. Comparison of these results with limited available measurements indicates that the proposed reactions can indeed take place, although due to a lack of measurements a rigorous evaluation is not possible at this time.

Role of mineral aerosol as a reactive surface in the global troposphere

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.

Global gridded inventories of anthropogenic emissions of sulfur and nitrogen

Global emission inventories, being the key information for the global budgets of trace metals, have become available only recently. The latest information on emissions and sources of trace metals o...

M. Trevor Scholtz

Papers

Global gridded inventories of anthropogenic emissions of sulfur and nitrogen

Global budget of trace metal sources