[1] The IMPACT global chemistry and transport model has been updated to include an aerosol dynamics module. Here it is used to simulate the dynamics of sulfate aerosol and its interaction with nonsulfate aerosol components: carbonaceous aerosol (organic matter (OM) and black carbon (BC)), dust, and sea salt. The sulfate aerosol dynamics is based on the method of modes and moments. In the current implementation, two modes are used for sulfate aerosol (nuclei and accumulation mode), and two moments are predicted within each mode (sulfate aerosol number and mass concentration). The aging of carbonaceous aerosol and dust particles from hydrophobic to hydrophilic depends on the surface coating of sulfate which occurs as a result of the condensation of sulfuric acid gas H 2 SO 4 (g) on their surface, and coagulation with pure sulfate aerosol. The model predicts high sulfate aerosol number concentrations in the nuclei mode (over 10 4 cm À3 ) in the tropical upper troposphere, while accumulation mode sulfate number concentrations are generally within 50-500 cm À3 in most parts of the free troposphere. The model predicted mass concentrations of sulfate, OM, BC, dust, and sea salt, H 2 SO 4 (g) concentration, aerosol number, and size distributions are compared with measurement data. Our model predicts $80% of global sulfate existing as a pure sulfate aerosol (9.7% in nuclei and 69.8% in accumulation mode), with 14.3% on carbonaceous aerosol, 3.3% on dust, and 2.7% on sea salt. In the boundary layer, over 40% of sulfate is associated with nonsulfate aerosols in many regions of the world whereas less than 10% of sulfate is associated with nonsulfate aerosols in the upper troposphere. The model predicted mass fraction of sulfate in the sulfate-carbonaceous aerosol mixture suggests that carbonaceous aerosol in most of the troposphere is internally mixed with sulfate and thus generally hygroscopic except near the source regions where the mass fraction is less than 5%. On the global mean, 54% and 93% of carbonaceous aerosol are coated with sulfate in the boundary layer and in the upper troposphere, respectively. Our result suggests that carbonaceous aerosols have a shorter lifetime (3$4 days) than predicted (4$8 days) using models that treat these aerosols as partly hydrophobic with an arbitrary e-folding time from hydrophobic to hydrophilic.Citation: Liu, X., J. E. Penner, and M. Herzog (2005), Global modeling of aerosol dynamics: Model description, evaluation, and interactions between sulfate and nonsulfate aerosols,

Abstract.The AeroCom exercise diagnoses multicomponent aerosol modules in global modeling. In an initial assessment simulated global distributions for mass and mid-visible aerosol optical thickness (aot) were compared among 20 different modules. Model diversity was also explored in the context of previous comparisons. For the component combined aot general agreement has improved for the annual global mean. At 0.11 to 0.14, simulated aot values are at the lower end of global averages suggested by remote sensing from ground (AERONET ca. 0.135) and space (satellite composite ca. 0.15). More detailed comparisons, however, reveal that larger differences in regional distribution and significant differences in compositional mixture remain. Of Correspondence to: S. Kinne (stefan.kinne@zmaw.de) particular concern are large model diversities for contributions by dust and carbonaceous aerosol, because they lead to significant uncertainty in aerosol absorption (aab). Since aot and aab, both, influence the aerosol impact on the radiative energy-balance, the aerosol (direct) forcing uncertainty in modeling is larger than differences in aot might suggest. New diagnostic approaches are proposed to trace model differences in terms of aerosol processing and transport: These include the prescription of common input (e.g. amount, size and injection of aerosol component emissions) and the use of observational capabilities from ground (e.g. measurements networks) or space (e.g. correlations between aerosol and clouds).

Abstract. Wildland fires in boreal regions have the potential to initiate deep convection, so-called pyro-convection, due to their release of sensible heat. Under favorable atmospheric conditions, large fires can result in pyro-convection that transports the emissions into the upper troposphere and the lower stratosphere. Here, we present three-dimensional model simulations of the injection of fire emissions into the lower stratosphere by pyro-convection. These model simulations are constrained and evaluated with observations obtained from the Chisholm fire in Alberta, Canada, in 2001. The active tracer high resolution atmospheric model (ATHAM) is initialized with observations obtained by radiosonde. Information on the fire forcing is obtained from ground-based observations of the mass and moisture of the burned fuel. Based on radar observations, the pyroconvection reached an altitude of about 13 km, well above the tropopause, which was located at about 11.2 km. The model simulation yields a similarly strong convection with an overshoot of the convection above the tropopause. The main outflow from the pyro-convection occurs at about 10.6 km, but a significant fraction (about 8%) of the emitted mass of the smoke aerosol is transported above the tropopause. In contrast to regular convection, the region with maximum updraft velocity in the pyro-convection is located close to the surface above the fire. This results in high updraft velocities >10 m s −1 at cloud base. The temperature anomaly in the plume decreases rapidly with height from values above 50 K at the fire to about 5 K at about 3000 m above the fire. WhileCorrespondence to: J. Trentmann (jtrent@uni-mainz.de) the sensible heat released from the fire is responsible for the initiation of convection in the model, the release of latent heat from condensation and freezing dominates the overall energy budget. Emissions of water vapor from the fire do not significantly contribute to the energy budget of the convection.

There is ample evidence that anthropogenic aerosols have important effects on climate in the Northern Hemisphere but little such evidence in the Southern Hemisphere. Observations of Australian rainfall and cloudiness since 1950 show increases over much of the continent. We show that including anthropogenic aerosol changes in 20th century simulations of a global climate model gives increasing rainfall and cloudiness over Australia during 1951–1996, whereas omitting this forcing gives decreasing rainfall and cloudiness. The pattern of increasing rainfall when aerosols are included is strongest over northwestern Australia, in agreement with the observed trends. The strong impact of aerosols is primarily due to the massive Asian aerosol haze, as confirmed by a sensitivity test in which only Asian anthropogenic aerosols are included. The Asian haze alters the meridional temperature and pressure gradients over the tropical Indian Ocean, thereby increasing the tendency of monsoonal winds to flow toward Australia. Anthropogenic aerosols also make the simulated pattern of surface‐temperature change in the tropical Pacific more like La Niña, since they induce a cooling of the surface waters in the extratropical North Pacific, which are then transported to the tropical eastern Pacific via the deep ocean. Transient climate model simulations forced only by increased greenhouse gases have generally not reproduced the observed rainfall increase over northwestern and central Australia. Our results suggest that a possible reason for this failure was the omission of forcing by Asian aerosols. Further research is essential to more accurately quantify the role of Asian aerosols in forcing Australian climate change.

[1] Explosive eruptions can inject large amounts of volcanic gases into the stratosphere. These gases may be scavenged by hydrometeors within the eruption column, and high uncertainties remain regarding the proportion of volcanic gases, which eventually reach the stratosphere. These are caused by the difficulties of directly sampling explosive volcanic eruption columns and by the lack of laboratory studies in the extreme parameter regime characterizing them. Using the nonhydrostatic nonsteady state plume model Active Tracer High Resolution Atmospheric Model (ATHAM), we simulated an explosive volcanic eruption. We examined the scavenging efficiency for the climatically relevant gases within the eruption column. The low concentration of water in the plume results in the formation of relatively dry aggregates. More than 99% of these are frozen because of their fast ascent to low-temperature regions. Consideration of the salinity effect increases the amount of liquid water by one order of magnitude, but the ice phase is still highly dominant. Consequently, the scavenging efficiency for HCl is very low, and only 1% is dissolved in liquid water. However, scavenging by ice particles via direct gas incorporation during diffusional growth is a significant process. The salinity effect increases the total scavenging efficiency for HCl from about 50% to about 90%. The sulfur-containing gases SO 2 and H 2 S are only slightly soluble in liquid water; however, these gases are incorporated into ice particles with an efficiency of 10 to 30%. Despite scavenging, more than 25% of the HCl and 80% of the sulfur gases reach the stratosphere because most of the particles containing these species are lifted there. Sedimentation of the particles would remove the volcanic gases from the stratosphere. Hence the final quantity of volcanic gases injected in a particular eruption depends on the fate of the particles containing them, which is in turn dependent on the volcanic and environmental conditions.

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A complex thermodynamic-microphysical package has been formulated that is able to deal with the microphysical processes of condensed water vapour in a volcanic plume. The microphysics follows a prognostic bulk approach for cloud water, cloud ice, rain and graupel and the interaction between them. In a standard experiment, this module, applied within a Ž . new nonhydrostatic volcano plume model, Active Tracer High Resolution Atmospheric Model ATHAM , produces reasonable concentrations of different types of hydrometeors. Under tropical conditions, the plume gains three times as much water from the environment through entrainment as from the volcanic source. The formed hydrometeors are dominated by the ice phase. Thermodynamic effects of phase changes contribute about 13% to the plume's total thermal energy and therefore have a considerable effect on the vertical development of the plume.

Abstract. The Chisholm forest fire that burned in Alberta, Canada, in May 2001 resulted in injection of substantial amounts of smoke into the lower stratosphere. We used the cloud-resolving plume model ATHAM (Active Tracer High resolution Atmospheric Model) to investigate the importance of different contributing factors to the severe intensification of the convection induced by the Chisholm fire and the subsequent injection of biomass smoke into the lower stratosphere. The simulations show strong sensitivity of the pyroconvection to background meteorology. This explains the observed coincidence of the convective blow-up of the fire plume and the passage of a synoptic cold front.Furthermore, we performed model sensitivity studies to the rate of release of sensible heat and water vapor from the fire. The release of sensible heat by the fire plays a dominant role for the dynamic development of the pyro-cumulonimbus cloud (pyroCb) and the height to which smoke is transported. The convection is very sensitive to the heat flux from the fire. The emissions of water vapor play a less significant role for the injection height but enhance the amount of smoke transported beyond the tropopause level.The aerosol burden in the plume has a strong impact on the microphysical structure of the resulting convective cloud. The dynamic evolution of the pyroCb, however, is only weakly sensitive to the abundance of cloud condensation nuclei (CCN) from the fire. In contrast to previous findings by other studies of convective clouds, we found that fire CCN have a negative effect on the convection dynamics because they give rise to a delay in the freezing of cloud droplets. Even in a simulation without fire CCN, there is no precipitation formation within the updraft region of the pyroCb. EnCorrespondence to: G. Luderer (gunnar@mpch-mainz.mpg.de) hancement of convection by aerosols as reported from studies of other cases of convection is therefore not found in our study.