We present a method for deriving the radiative effects of absorbing aerosols in cloudy scenes from satellite retrievals only. We use data of 2005–2007 from various passive sensors aboard satellites of the “A-Train” constellation. The study area is restricted to the tropical- and subtropical Atlantic Ocean. To identify the dependence of the local planetary albedo in cloudy scenes on cloud liquid water path and aerosol optical depth (AOD), we perform a multiple linear regression. The OMI UV-Aerosolindex serves as an indicator for absorbing-aerosol presence. In our method, the aerosol influences the local planetary albedo through direct- (scattering and absorption) and indirect (Twomey) aerosol effects. We find an increase of the local planetary albedo (LPA) with increasing AOD of mostly scattering aerosol and a decrease of the LPA with increasing AOD of mostly absorbing aerosol. These results allow us to derive the direct aerosol effect of absorbing aerosols in cloudy scenes, with the effect of cloudy-scene aerosol absorption in the tropical- and subtropical Atlantic contributing (+21.2±11.1)×10−3 Wm−2 to the global top of the atmosphere radiative forcing.

This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model’s capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation. Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced k-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker incloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher Ångström parameters. Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans in Ångström parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aerosol mass concentrations are very similar to those in the old version. The total aerosol water content in HAM2 is considerably closer to the multi-model average from Phase I of the AeroCom intercomparison project. Model deficiencies that require further efforts in the future include (i) positive biases in AOD over the ocean, (ii) negative biases in AOD and aerosol mass concentration in high-latitude regions, and (iii) negative biases in particle number concentration, especially that of the Aitken mode, in the lower troposphere in heavily polluted regions.

Nucleation from the gas phase is an important source of aerosol particles in the Earth’s atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosolclimate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth’s radiative forcing. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are −1.15 W/m2 for charged H2SO4/H2O nucleation, −0.235 W/m2 for cluster activation, and −0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is −2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with −2.18 W/m2 to total absorbed solar short-wave radiation, compared to −0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth’s radiative forcing over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local measurements: over southern Finland, where cluster activation proceeds efficiently, we find that charged nucleation of sulfuric acid and water contributes on average less than 10% to ultrafine aerosol concentrations, in good agreement with observations.

The impact of aerosols above and around the Tibetan Plateau on the Asian Summer Monsoon during premonsoon seasons March-April-May 2007, 2008, and 2009 is investigated by means of remote sensing and radiative transfer modelling. Four source regions are found to be responsible for the high aerosol loading around the Tibetan Plateau: the Taklamakan Desert, the Ganges Plains, the Indus Plains, and the Arabian Sea. CALIPSO lidar satellite data, providing vertically resolved images of aerosols, shows aerosol concentrations to be highest in the lower 5 km of the atmosphere with only little amounts reaching the Tibetan Plateau altitude. Using a radiative transfer model we find that aerosol plumes reduce shortwave radiation throughout the Monsoon region in the seasonal average by between 20 and 30 W/m2. Peak shortwave heating in the lower troposphere reaches 0.2 K/day. In higher layers this shortwave heating is partly balanced by longwave cooling. Although high-albedo surfaces, such as deserts or the Tibetan Plateau, increase the shortwave heating by around 10%, the overall effect is strongest close to the aerosol sources. A strong elevated heating which could influence large-scale monsoonal circulations as suggested by previous studies is not found.

Uncertainties in aerosol radiative forcings, especially those associated with clouds, contribute to a large extent to uncertainties in the total anthropogenic forcing. The interaction of aerosols with clouds and radiation introduces feedbacks which can affect the rate of precipitation formation. In former assessments of aerosol radiative forcings, these effects have not been quantified. Also, with global aerosol-climate models simulating interactively aerosols and cloud microphysical properties, a quantification of the aerosol forcings in the traditional way is difficult to define properly. Here we argue that fast feedbacks should be included because they act quickly compared with the time scale of global warming. We show that for different forcing agents (aerosols and greenhouse gases) the radiative forcings as traditionally defined agree rather well with estimates from a method, here referred to as radiative flux perturbations (RFP), that takes these fast feedbacks and interactions into account. Based on our results, we recommend RFP as a valid option to compare different forcing agents, and to compare the effects of particular forcing agents in different models.

Statistical analysis of satellite data shows a positive correlation between aerosol optical depth (AOD) and total cloud cover (TCC). Reasons for this relationship have been disputed in recent literature. The aim of this study is to explore how different processes contribute to one model’s analog of the positive correlation between aerosol optical depth and total cloud cover seen in the satellite retrievals. We compare the slope of the linear regression between the logarithm of TCC and the logarithm of AOD, or the strength of the relationship, as derived from three satellite data sets to the ones simulated by a global aerosol-climate model. We analyse model results from two different simulations with and without a parameterisation of aerosol indirect effects, and using dry compared to humidified AOD. Perhaps not surprisingly we find that no single one of the hypotheses discussed in the literature is able to uniquely explain the positive relationship. However the dominant contribution to the model’s AOD-TCC relationship can be attributed to aerosol swelling in regions where humidity is high and clouds are coincidentally found. This finding leads us to hypothesise that much of the AOD-TCC relationship seen in the satellite data is also carried by such a process, rather than the direct effects of the aerosols on the cloud fields themselves.

Aerosols act as cloud condensation nuclei (CCN) for cloud water droplets, and changes in aerosol concentrations have significant microphysical impacts on the corresponding cloud properties. Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol and cloud properties are combined with NCEP Reanalysis data for six different regions around the globe between March 2000 and December 2005 to study the effects of different aerosol, cloud, and atmospheric conditions on the aerosol indirect effect (AIE). Emphasis is placed in examining the relative importance of aerosol concentration, type, and atmospheric conditions (mainly vertical motion) to AIE from region to region. Results show that in most regions, AIE has a distinct seasonal cycle, though the cycle varies in significance and period from region to region. In the Arabian Sea (AS), the sixyear mean anthropogenic + dust AIE is −0.27Wm−2 and is greatest during the summer months (<−2.0Wm−2) during which aerosol concentrations (from both dust and anthropogenic sources) are greatest. Comparing AIE as a function of thin (LWP<20 gm−2) vs. thick (LWP≥20 gm−2) clouds under conditions of large scale ascent or decent at 850 hPa showed that AIE is greatest for thick clouds during periods of upward vertical motion. In the Bay of Bengal, AIE is negligible owing to less favorable atmospheric conditions, a lower concentration of aerosols, and a non-alignment of aerosol and cloud layers. In the eastern North Atlantic, AIE is weakly positive (+0.1Wm−2) with dust aerosol concentration being much greater than the anthropogenic or sea salt components. However, elevated dust in this region exists above the maritime cloud layers and does not have a hygroscopic coating, which occurs in AS, preventing the dust from acting as CCN and limiting AIE. The Western Atlantic has a large anthropogenic aerosol concentration transported from the eastern United States producing a modest anthropogenic AIE (−0.46Wm−2). Anthropogenic AIE is also present off the West African coast corresponding to aerosols produced from seasonal biomass burning (both natural and man-made). Interestingly, atmospheric conditions are not particularly favorable for cloud formation compared to the other regions during the times where AIE is observed; however, clouds are generally thin (LWP<20 gm−2) and concentrated very near the surface. Overall, we conclude that vertical motion, aerosol type, and aerosol layer heights do make a significant contribution to AIE and that these factors are often more important than total aerosol concentration alone and that the relative importance of each differs significantly from region to region.

Aerosol indirect effects are considered to be the most uncertain yet important anthropogenic forcing of climate change. The goal of the present study is to reduce this uncertainty by constraining two different general circulation models (LMDZ and ECHAM4) with satellite data. We build a statistical relationship between cloud droplet number concentration and the optical depth of the fine aerosol mode as a measure of the aerosol indirect effect using MODerate Resolution Imaging Spectroradiometer (MODIS) satellite data, and constrain the model parameterizations to match this relationship. We include here “empirical” formulations for the cloud albedo effect as well as parameterizations of the cloud lifetime effect. When fitting the model parameterizations to the satellite data, consistently in both models, the radiative forcing by the combined aerosol indirect effect is reduced considerably, down to −0.5 and −0.3Wm−2, for LMDZ and ECHAM4, respectively.

A weekly cycle in aerosol pollution and some meteorological quantities is observed over Europe. In the present study we exploit this effect to analyse aerosol-cloudradiation interactions. A weekly cycle is imposed on anthropogenic emissions in two general circulation models that include parameterizations of aerosol processes and cloud microphysics. It is found that the simulated weekly cycles in sulfur dioxide, sulfate, and aerosol optical depth in both models agree reasonably well with those observed indicating model skill in simulating the aerosol cycle. A distinct weekly cycle in cloud droplet number concentration is demonstrated in both observations and models. For other variables, such as cloud liquid water path, cloud cover, top-of-the-atmosphere radiation fluxes, precipitation, and surface temperature, large variability and contradictory results between observations, model simulations, and model control simulations without a weekly cycle in emissions prevent us from reaching any firm conclusions about the potential aerosol impact on meteorology or the realism of the modelled second aerosol indirect effects.

Modeled differences in predicted effects are increasingly used to help quantify the uncertainty of these effects. Here, we examine modeled differences in the aerosol indirect effect in a series of experiments that help to quantify how and why model-predicted aerosol indirect forcing varies between models. The experiments start with an experiment in which aerosol concentrations, the parameterization of droplet concentrations and the autoconversion scheme are all specified and end with an experiment that examines the predicted aerosol indirect forcing when only aerosol sources are specified. Although there are large differences in the predicted liquid water path among the models, the predicted aerosol first indirect effect for the first experiment is rather similar, about −0.6Wm−2 to −0.7Wm−2. Changes to the autoconversion scheme can lead to large changes in the liquid water path of the models and to the response of the liquid water path to changes in aerosols. Adding an autoconversion scheme that depends on the droplet concentration caused a larger (negative) change in net outgoing shortwave radiation compared to the 1st indirect effect, and the increase varied from only 22% to more than a factor of three. The change in net shortwave forcing in the models due to varying the autoconversion scheme depends on the liquid water content of the clouds as well as their predicted droplet concentrations, and both increases and decreases in the net shortwave forcing can occur when autoconversion schemes are changed. The parameterization of cloud fraction within models is not sensitive to the aerosol concentration, and, therefore, the response of the modeled cloud fraction within the present models appears to be smaller than that which would be associated with model “noise”. The prediction of aerosol concentrations, given a fixed set of sources, leads to some of the largest differences in the predicted aerosol indirect radiative forcing among the models, with values of cloud forcing ranging from −0.3Wm−2 to −1.4Wm−2. Thus, this aspect of modeling requires significant improvement in order to improve the prediction of aerosol indirect effects.