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There is growing interest in the formation of secondary organic aerosol (SOA) through condensed aqueous-phase reactions. In this study, we use a global model (IMPACT) to investigate the potential formation of SOA in the aqueous phase. We compare results from several multiphase process schemes with detailed aqueous-phase reactions to schemes that use a first-order gas-to-particle formation rate based on uptake coefficients. The predicted net global SOA production rate in cloud water ranges from 13.1 Tg yr−1 to 46.8 Tg yr−1 while that in aerosol water ranges from −0.4 Tg yr−1 to 12.6 Tg yr−1. The predicted global burden of SOA formed in the aqueous phase ranges from 0.09 Tg to 0.51 Tg. A sensitivity test to investigate two representations of cloud water content from two global models shows that increasing cloud water by an average factor of 2.7 can increase the net SOA production rate in cloud water by a factor of 4 at low altitudes (below approximately 900 hPa). We also investigated the importance of including dissolved Fe chemistry in cloud water aqueous reactions. Adding these reactions increases the formation rate of aqueous-phase OH by a factor of 2.6 and decreases the amount of global aqueous SOA formed by 31%. None of the mechanisms discussed here is able to provide a best fit for all observations. Rather, the use of an uptake coefficient method for aerosol water and a multi-phase scheme for cloud water provides the best fit in the Northern Hemisphere and the use of multiphase process scheme for aerosol and cloud water provides the best fit in the tropics. The model with Fe chemistry underpredicts oxalate measurements in all regions. Finally, the comparison of oxygen-to-carbon (O / C) ratios estimated in the model with those estimated from measurements shows that the modeled SOA has a slightly higher O / C ratio than the observed SOA for all cases.

We use a single aerosol model to explore the effects of the differing meteorological fields from the NCAR CAM5 and GFDL AM3 models. We simulate the global distributions of sulfate, black carbon, organic matter, dust and sea salt using the University of Michigan IMPACT model and use these fields to calculate aerosol direct and indirect forcing, thereby isolating the impacts of the differing meteorological fields. Over all, the IMPACT-AM3 model predicts larger burdens and longer aerosol lifetimes than the IMPACT-CAM5 model. However, the IMPACT-CAM5 simulations transport more black carbon to the polar regions and more dust from Asia towards North America. These differences can mainly be attributed to differences in: (1) the vertical cloud mass flux and large-scale precipitation fields which determine the wet deposition of aerosols; (2) the in-cloud liquid water content and the cloud coverage which determine the wet aqueous phase production of sulfate. The burden, lifetime and global distribution, especially black carbon in polar regions, are strongly affected by choice of the parameters used for wet deposition. The total annual mean aerosol optical depth (AOD) at 550 nm ranges from 0.087 to 0.122 for the IMPACT-AM3 model and from 0.138 to 0.186 for the IMPACT-CAM5 model (range is due to different parameters used for wet deposition). Even though IMPACT-CAM5 has smaller aerosol burdens, its AOD is larger due to the much higher relative humidity in CAM5 which leads to more hygroscopic growth. The corresponding global annual average anthropogenic and all-sky aerosol direct forcing at the top of the atmosphere ranges from −0.25 W m−2 to −0.30 W m−2 for IMPACT-AM3 and from −0.48 W m−2 to −0.64 W m−2 for IMPACT-CAM5. The global annual average anthropogenic 1st aerosol indirect effect at the top of the atmosphere ranges from −1.26 W m−2 to −1.44 W m−2 for IMPACT-AM3 and from −1.74 W m−2 to −1.77 W m−2 for IMPACT-CAM5.

It is well-known that aerosols affect clouds and that the effect of aerosols on clouds is critical for understanding human-induced climate change. Most climate model studies have focused on the effect of aerosols on warm stratiform clouds (e.g., stratocumulus clouds) for the prediction of climate change. However, systems like the Asian and Indian Monsoon, storm tracks, and the intertropical convergence zone, play important roles in the global hydrological cycle and in the circulation of energy and are driven by thunderstorm-type convective clouds. Here, we show that the different morphologies of these two cloud types lead to different aerosol-cloud interactions. Increasing aerosols are known to suppress the conversion of droplets to rain (i.e., so-called autoconversion). This increases droplets as a source of evaporative cooling, leading to an increased intensity of downdrafts. The acceleration of the intensity of downdrafts is larger in convective clouds due to their larger cloud depths (providing longer paths for downdrafts to follow to the surface) than in stratiform clouds. More accelerated downdrafts intensify the gust front, leading to significantly increased updrafts, condensation and thus the collection of cloud liquid by precipitation, which offsets the suppressed autoconversion. This leads to an enhancement of precipitation with increased aerosols in convective clouds. However, the downdrafts are less accelerated in stratiform clouds due to their smaller cloud depths, and they are not able to induce changes in updrafts as large as those in convective clouds. Thus, the offset is not as effective, and this allows the suppression of precipitation with increased aerosols. Thus aerosols affect these cloud systems differently. The dependence of the effect of aerosols on clouds on the morphology of clouds should be taken into account for a more complete assessment of climate change.

The response of a case of thin, warm marine-boundary-layer (MBL) clouds to preindustrial (PI) and present-day (PD) conditions is simulated by a cloud-system resolving model (CSRM). Here, both the aerosol conditions and environmental conditions match those of a general circulation model (GCM). The environmental conditions are characterized by the initial condition and the large-scale forcings of humidity and temperature, as well as the surface fluxes. The response of the CSRM is compared to that simulated by the GCM. The percentage increase of liquid-water path (LWP) due to a change from the PI to PD conditions is ~3 times larger in the CSRM than that in the GCM due to the formation of cumulus clouds. The formation of cumulus clouds is controlled by a larger increase in the surface latent-heat (LH) flux in the PD environment than in the PI environment rather than by the change in aerosols. However, the aerosol increase from the PI to PD level determines the LWP response in the stratocumulus clouds, while the impacts of changes in environmental conditions are negligible for stratocumulus clouds. The conversion of cloud liquid to rain through autoconversion and accretion plays a negligible role in the CSRM in the response to aerosols, whereas it plays a role that is as important as condensation in the GCM. Also, it is notable that the explicit simulation of microphysics in the CSRM leads to a smaller LWP in the CSRM than that in the GCM using heavily parameterized microphysics for stratocumulus clouds. The smaller LWP in the CSRM is closer to an observed LWP than the LWP in the GCM for stratocumulus clouds. Supplementary simulations show that increasing aerosols increase the sensitivity of the cloud responses to the PI and PD environmental conditions. They also show that aerosol effects on clouds depend on the cloud type. The LWP of warm cumulus clouds is more sensitive to aerosols than that of stratocumulus clouds.

We present an intercomparison of several aerosol modules, sectional and modal, in a global 2-D model in order to differentiate their behavior for tropospheric and stratospheric applications. We model only binary sulfuric acid-water aerosols in this study. Three versions of the sectional model and three versions of the modal model are used to test the sensitivity of background aerosol mass and size distribution to the number of bins or modes and to the prescribed width of the largest mode. We find modest sensitivity to the number of bins (40 vs. 150) used in the sectional model. Aerosol mass is found to be reduced in a modal model if care is not taken in selecting the width of the largest lognormal mode, reflecting differences in sedimentation in the middle stratosphere. The size distributions calculated by the sectional model can be better matched by a modal model with four modes rather than three modes in most but not all situations. A simulation of aerosol decay following the 1991 eruption of Mt. Pinatubo shows that the representation of the size distribution can have a signficant impact on model-calculated aerosol decay rates in the stratosphere. Between 1991 and 1995, aerosol extinction and surface area density calculated by two versions of the modal model adequately match results from the sectional model. Calculated effective radius for the same time period shows more intermodel variability, with a 20-bin sectional model performing much better than any of the modal models.

International audience; The Active Tracer High-resolution Atmospheric Model (ATHAM) has been adopted to examine the aerosol indirect effect in contrasting clean and polluted cloudy boundary layers during the Second Aerosol Characterization Experiment (ACE-2). Model results are in good agreement with available in-situ observations, which provides confidence in the results of ATHAM. Sensitivity tests have been conducted to examine the response of the cloud fraction (CF), cloud liquid water path (LWP), and cloud optical depth (COD) to changes in aerosols in the clean and polluted cases. It is shown for two cases that CF and LWP would decrease or remain nearly constant with an increase in aerosols, a result which shows that the second aerosol indirect effect is positive or negligibly small in these cases. Further investigation indicates that the background meteorological conditions play a critical role in the response of CF and LWP to aerosols. When large-scale subsidence is weak as in the clean case, the dry overlying air above the cloud is more efficiently entrained into the cloud, and in so doing, removes cloud water more efficiently, and results in lower CF and LWP when aerosol burden increases. However, when the large-scale subsidence is strong as in the polluted case, the growth of the cloud top is suppressed and the entrainment drying makes no significant difference when aerosol burden increases. Therefore, the CF and LWP remain nearly constant. In both the clean and polluted cases, the COD tends to increase with aerosols, and the total aerosol indirect effect (AIE) is negative even when the CF and LWP decrease with an increase in aerosols. Therefore, the first AIE dominates the response of the cloud to aerosols.