Guy P. Brasseur

Radiative forcing in the 21st century due to ozone changes in the troposphere and the lower stratosphere

ranging from 0.40 to 0.78 W m 2 on a global and annual average. The lower stratosphere contributes an additional 7.5–9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15–0.17 W m 2 . The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change. INDEX TERMS: 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0341 Atmospheric Composition and Structure: Middle atmosphere—constituent transport and chemistry (3334) Citation: Gauss, M., et al., Radiative forcing in the 21st century due to ozone changes in the troposphere and the lower stratosphere, J. Geophys. Res., 108(D9), 4292, doi:10.1029/2002JD002624, 2003.

IMAGES: A three‐dimensional chemical transport model of the global troposphere

A new three-dimensional chemical transport model of the troposphere is presented. This model, named intermediate model of global evolution of species, has been developed to study the global distributions, budgets, and trends of 41 chemical compounds, including the most important species that determine the oxidation capacity of the atmosphere. The chemical mechanism is made of approximately 125 chemical reactions and 26 photodissociations. The model accounts for surface emissions, chemical transformations, dry and wet deposition, and aerosol reactions of trace constituents. The model is formulated in σ coordinates and includes 25 layers in the vertical. Its horizontal resolution is 5° in longitude and 5° in latitude. To keep the requirements in computer time limited, a simplified representation of the transport is adopted: the advection, solved by a semi-Lagrangian scheme, is driven by monthly mean climatological winds provided by an European Center for Medium-Range Weather Forecasts analysis. The effect of wind variability at timescales smaller than a month is taken into account by an eddy diffusion parameterization. Convection in cumulonimbus clouds is also represented. All input field, such as the distribution of winds, clouds, eddy diffusion coefficients, and the boundary conditions, are monthly means constrained by observational data. The modeled global distributions of species such as methane, carbon monoxide, nitrogen oxides, and ozone are generally in good agreement with observations. The lifetime of methane, which can be regarded as a measure of the oxidizing capacity of the atmosphere, is found to be equal to 11 years, in agreement with recent estimates. The model also shows that the deposition of ozone at the Earths surface (1100 Tg/yr) balances the sum of the net photochemical production (550 Tg/yr) and the flux from the stratosphere (550 Tg/yr). In the case of carbon monoxide, surface emissions (1400 Tg/yr) are approximately 50% larger than in situ production by hydrocarbon oxidation (900 Tg/yr).

Variations in the predicted spatial distribution of atmospheric nitrogen deposition and their impact on carbon uptake by terrestrial ecosystems

Widespread mobilization of nitrogen into the atmosphere from industry, agriculture, and biomass burning and its subsequent deposition have the potential to alleviate nitrogen limitation of productivity in terrestrial ecosystems, and may contribute to enhanced terrestrial carbon uptake. To evaluate the importance of the spatial distribution of nitrogen deposition for carbon uptake and to better quantify its magnitude and uncertainty NO y -N deposition fields from five different three-dimensional chemical models, GCTM, GRANTOUR, IMAGES, MOGUNTIA, and ECHAM were used to drive NDEP, a perturbation model of terrestrial carbon uptake. Differences in atmospheric sources of NO x -N, transport, resolution, and representation of chemistry, contribute to the distinct spatial patterns of nitrogen deposition on the global land surface; these differences lead to distinct patterns of carbon uptake that vary between 0.7 and 1.3 Gt C yr -1 globally. Less than 10% of the nitrogen was deposited on forests which were most able to respond with increased carbon storage because of the wide C:N ratio of wood as well as its long lifetime. Addition of NH x -N to NO y -N deposition, increased global terrestrial carbon storage to between 1.5 and 2.0 Gt C yr -1 , while the missing terrestrial sink is quite similar in magnitude. Thus global air pollution appears to be an important influence on the global carbon cycle. If N fertilization of the terrestrial biosphere accounts for the missing C sink or a substantial portion of it, we would expect significant reductions in its magnitude over the next century as terrestrial ecosystems become N saturated and O 3 pollution expands.

MOZART, a global chemical transport model for ozone and related chemical tracers: 2. Model results and evaluation

In this second of two companion papers, we present results from a new global three-dimensional chemical transport model, called MOZART (model for ozone and related chemical tracers). MOZART is developed in the framework of the National Center for Atmospheric Research (NCAR) Community Climate Model (CCM) and includes a detailed representation of tropospheric chemistry. The model provides the distribution of 56 chemical species at a spatial resolution of 2.8° in both latitude and longitude, with 25 levels in the vertical (from the surface to level of 3 mbar) and a time step of 20 min. The meteorological information is supplied from a 2-year run of the NCAR Community Climate Model. The simulated distributions of ozone (O 3 ) and its precursors are evaluated by comparison with observational data. The distribution of methane, nonmethane hydrocarbons (NMHCs), and CO are generally well simulated by the model. The model evaluation in the tropics stresses the need for a better representation of biomass burning emissions in order to evaluate the budget of carbon monoxide, nitrogen species, and ozone with more accuracy in these regions. MOZART reproduces the NO observations in most parts of the troposphere. Nitric acid, however, is overestimated over the Pacific by up to a factor of 10 and over continental regions by a factor of 2-3. Discrepancies are also found in the simulation of PAN in the upper troposphere and in biomass burning regions. These results highlight shortcomings in our understanding of the nitrogen budget in the troposphere. The seasonal cycle of ozone in the troposphere is generally well reproduced by the model in comparison with ozone soundings. MOZART tends, however, to underestimate O 3 at higher latitudes, and specifically above 300 mbar. The global photochemical production and destruction of ozone in the troposphere are 3018 Tg/yr and 2511 Tg/yr, respectively (net ozone production of 507 Tg/yr). The stratospheric influx of O 3 is estimated to be 391 Tg/yr and the surface dry deposition 898 Tg/yr. The calculated global lifetime of methane is 9.9 years in the annual average.

A three-dimensional study of the tropospheric sulfur cycle

The global tropospheric distributions of seven important sulfur species were simulated with a global three-dimensional chemistry-transport model (IMAGES). Surface emission and deposition velocity maps were established for use as lower boundary conditions in the model. While anthropogenic SO2 emissions are by far the largest sulfur source in the northern midlatitudes, reduced sulfur compounds, notably dimethyl sulfide (DMS) predominate over most remote areas. Simulations were performed for the present-day (∼ 1985) atmosphere. The calculated distributions are compared with available observations. The model results are found to be generally within a factor of (at most) 2–3 of long-term observations. Comparison with campaign measurements is more difficult, mostly due to the strong dependence of sulfur species concentrations on local meteorological conditions. The results, however, indicate the need for future model refinements, especially with respect to biogenic emission estimates and parameterization of cloud processes. A sensitivity study is presented to discuss the uncertainties of the results related to several parameters (the decoupling of wet scavenging and convective transport for soluble species, volcanoes emission and deposition velocities). Results are also discussed in terms of global budgets and related variables and processes. Around 125 Tg S/yr of non-sea-salt (nss) sulfur compounds (DMS, CS2, H2S, COS, and SO2) are injected into the atmosphere. The balance is mainly maintained by nss-sulfates wet and dry deposition, and by SO2 dry deposition (94% of total sulfur deposition). It is found that DMS oxidation represents the main contribution to SO2 chemical production (80% of the chemical sources), and that the major sink of SO2 is provided by in-cloud oxidation (90% of the chemical sinks), under the assumption that all SO2 incorporated into clouds is oxidized. The calculated annual wet deposition of sulfates reaches 3 g S m−2 yr−1 over Europe and North America, while it is usually lower than 0.5 g S m−2 yr−1 in remote parts of the world. Estimations for the global lifetimes are 0.9 day for DMS, 4 days for CS2, 2.2 days for H2S, 0.6 day for SO2, 0.18 day for DMSO, 6.1 days for MSA, and 4.7 days for nss-sulfates.

Chemistry of the 1991–1992 stratospheric winter: Three-dimensional model simulations

A three-dimensional chemistry-transport model of the stratosphere is used to simulate the evolution of trace constituents during the 1991–1992 Arctic winter. It is shown that heterogeneous reactions on polar stratospheric clouds led in early January to almost complete activation of atmospheric chlorine inside the polar vortex, in remarkable coincidence with observations by the ER-2 aircraft (Toohey et al., 1993) and the microwave limb sounder on the Upper Atmosphere Research Satellite (Waters et al., 1993). Sulfate aerosols resulting from the eruption of Mount Pinatubo also produced a significant increase in chlorine monoxide (ClO) concentrations at middle and high latitudes. The net chemical destruction of ozone found in the vortex at the end of the simulation (25% at 50 hPa and 25 DU), although substantial, was limited by available sunlight and the short period during which stratospheric clouds occurred.

Global Wildland Fire Emission Model (GWEM): Evaluating the use of global area burnt satellite data

[1] The new Global Wildland Fire Emission Model (GWEM) has been developed on the basis of data from the European Space Agency’s monthly Global Burnt Scar satellite product (GLOBSCAR) and results from the Lund-Potsdam-Jena Dynamic Global Vegetation Model (LPJ-DGVM). GWEM computes monthly emissions of more than 40 chemical compounds and aerosols from forest and savanna fires. This study focuses on an evaluation of the GLOBSCAR data set. The GWEM version presented here makes use of the Moderate-Resolution Imaging Spectroradiometer (MODIS) land cover map. Emission totals for the year 2000 are 1741 Tg C, 5716 Tg CO2, 271 Tg CO, 12.52 Tg CH4, 9.09 Tg C (as nonmethane hydrocarbons), 8.08 Tg NOx (as NO), 24.30 Tg PM2.5, 15.80 Tg OC, and 1.84 Tg black carbon. These emissions are lower than other estimates found in literature. An evaluation assesses the uncertainties of the individual input data. The GLOBSCAR product yields reasonable estimates of burnt area for large wildland fires in most parts of the globe but experiences problems in some regions where small fires dominate. The seasonality derived from GLOBSCAR differs from other satellite products detecting active fires owing to the different algorithms applied. Application of the presented GWEM results in global chemistry transport modeling will require additional treatment of small deforestation fires in the tropical rain forest regions and small savanna fires, mainly in subequatorial Africa. Further improvements are expected from a more detailed description of the carbon pools and the inclusion of anthropogenic disturbances in the LPJ model. INDEX TERMS: 0315 Atmospheric Composition and Structure: Biosphere/atmosphere interactions; 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry; 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 1615 Global Change: Biogeochemical processes (4805); KEYWORDS: vegetation fire emissions, global area burnt satellite products, tropospheric chemistry

Assessing future nitrogen deposition and carbon cycle feedback using a multimodel approach: Analysis of nitrogen deposition

n this study, we present the results of nitrogen deposition on land from a set of 29 simulations from six different tropospheric chemistry models pertaining to present-day and 2100 conditions. Nitrogen deposition refers here to the deposition (wet and dry) of all nitrogen-containing gas phase chemical species resulting from NOx (NO + NO2) emissions. We show that under the assumed IPCC SRES A2 scenario the global annual average nitrogen deposition over land is expected to increase by a factor of ∼2.5, mostly because of the increase in nitrogen emissions. This will significantly expand the areas with annual average deposition exceeding 1 gN/m2/year. Using the results from all models, we have documented the strong linear relationship between models on the fraction of the nitrogen emissions that is deposited, regardless of the emissions (present day or 2100). On average, approximately 70% of the emitted nitrogen is deposited over the landmasses. For present-day conditions the results from this study suggest that the deposition over land ranges between 25 and 40 Tg(N)/year. By 2100, under the A2 scenario, the deposition over the continents is expected to range between 60 and 100 Tg(N)/year. Over forests the deposition is expected to increase from 10 Tg(N)/year to 20 Tg(N)/year. In 2100 the nitrogen deposition changes from changes in the climate account for much less than the changes from increased nitrogen emissions.

Mount Pinatubo Aerosols, Chlorofluorocarbons, and Ozone Depletion

The injection into the stratosphere of large quantities of sulfur during the June 1991 eruption of Mount Pinatubo (Philippines) and the subsequent formation of sulfate aerosol particles have generated a number of perturbations in the atmosphere with potential effects on the Earths climate. Changes in the solar and infrared radiation budget caused by the eruption should produce a cooling of the troposphere and a warming of the lower stratosphere. These changes could affect atmospheric circulation. In addition, heterogeneous chemical reactions on the surface of sulfate aerosol particles render the ozone molecules more vulnerable to atmospheric chlorine and hence to man-made chlorofluorocarbons.

The HAMMONIA Chemistry Climate Model: Sensitivity of the Mesopause Region to the 11-Year Solar Cycle and CO2 Doubling

Abstract This paper introduces the three-dimensional Hamburg Model of the Neutral and Ionized Atmosphere (HAMMONIA), which treats atmospheric dynamics, radiation, and chemistry interactively for the height range from the earth’s surface to the thermosphere (approximately 250 km). It is based on the latest version of the ECHAM atmospheric general circulation model of the Max Planck Institute for Meteorology in Hamburg, Germany, which is extended to include important radiative and dynamical processes of the upper atmosphere and is coupled to a chemistry module containing 48 compounds. The model is applied to study the effects of natural and anthropogenic climate forcing on the atmosphere, represented, on the one hand, by the 11-yr solar cycle and, on the other hand, by a doubling of the present-day concentration of carbon dioxide. The numerical experiments are analyzed with the focus on the effects on temperature and chemical composition in the mesopause region. Results include a temperature response to the...