Ship tracks are regarded as the most obvious manifestations of the effect of anthropogenic aerosol particles on clouds (indirect effect). However, it is not yet fully quantified whether there are climatically relevant effects on large scales beyond the narrow ship tracks visible in selected satellite images. A combination of satellite and reanalysis data is used here to analyze regions in which major shipping lanes cut through otherwise pristine marine environments in subtropical and tropical oceans. We expect the region downwind of a shipping lane is affected by the aerosol produced by shipping emissions but not the one upwind. Thus, differences in microphysical and macrophysical cloud properties are analyzed statistically. We investigate microphysical and macrophysical cloud properties as well as the aerosol optical depth and its fine-mode fraction for the years 2005–2007 as provided for by retrievals of the two Moderate Resolution Imaging Spectroradiometer instruments. Water-cloud properties include cloud optical depth, cloud droplet effective radius, cloud top temperature, and cloud top pressure. Large-scale meteorological parameters are taken from ERA-Interim reanalysis data and microwave remote sensing (sea surface temperature). We analyze the regions of interest in a Eulerian and Lagrangian sense, i.e., sampling along shipping lanes and sampling along wind trajectories, respectively. No statistically significant impacts of shipping emissions on large-scale cloud fields could be found in any of the selected regions close to major shipping lanes. In conclusion, the net indirect effects of aerosols from ship emissions are not large enough to be distinguishable from the natural dynamics controlling cloud presence and formation.

Regimes of tropical low-level clouds are commonly identified according to large-scale subsidence and lower tropospheric stability (LTS). This definition alone is insufficient for the distinction between regimes and limits the comparison of low-level clouds from CloudSat radar observations and the ECHAM5 GCM run with the COSP radar simulator. Comparisons of CloudSat radar cloud altitude-reflectivity histograms for stratocumulus and shallow cumulus regimes, as defined above, show nearly identical reflectivity profiles, because the distinction between the two regimes is dependent upon atmospheric stability below 700 hPa and observations above 1.5 km. Regional subsets, near California and Hawaii, for example, have large differences in reflectivity profiles than the dynamically defined domain; indicating different reflectivity profiles exist under a given large-scale environment. Regional subsets are better for the evaluation of low-level clouds in CloudSat and ECHAM5 as there is less contamination between 2.5 km and 7.5 km from precipitating hydrometeors which obscured cloud reflectivities.

The formation of cloud droplets on aerosol particles, technically known as the activation of cloud condensation nuclei (CCN), is the fundamental process driving the interactions of aerosols with clouds and precipitation. Knowledge of these interactions is foundational to our understanding of weather and climate. The Intergovernmental Panel on Climate Change (IPCC) and the Decadal Survey (NRC 2007) indicate that the uncertainty in how clouds adjust to aerosol perturbations dominates the uncertainty in the overall quantification of the radiative forcing attributable to human activities. The Clouds, Hazards, and Aerosols Survey for Earth Researchers (CHASER) satellite mission concept responds to the IPCC and Decadal Survey concerns by studying the activation of CCN and their interactions with clouds and storms. The CHASER satellite mission was developed to remotely sense quantities necessary for determining the interactions of aerosols with clouds and storms. The links between the Decadal Survey recommendations and the CHASER goals, science objectives, measurements, and instruments are described in Table 1. Measurements by current satellites allow a rough determination of profiles of cloud particle size but not of the activated CCN that seed them. CHASER will use an innovative technique (Freud et al. 2011; Freud and Rosenfeld 2012; Rosenfeld et al. 2012) and high-heritage (flown in a previous spaceflight mission) instruments to produce satellite-based remotely sensed observations of activated CCN and the properties of the clouds associated with them. CHASER will estimate updraft velocities at cloud base to calculate the number density of activated CCN as a function of the water vapor supersaturation. CHASER will determine the CCN concentration and cloud thermodynamic forcing (i.e., forcing caused by changes in the temperature and humidity of the boundary layer air) simultaneously, allowing their effects to be distinguished. Changes in the behavior of a group of weather systems in which only one of the quantities varies (a partial derivative of the intensity of the weather system with respect to the desirable quantity) will allow the determination of each effect statistically.

The Advanced Very High Resolution Radiometer (AVHRR) instruments onboard the series of National Oceanic and Atmospheric Administration (NOAA) satellites offer the longest available meteorological data records from space. These satellites have drifted in orbit resulting in shifts in the local time sampling during the life span of the sensors onboard. Depending upon the amplitude of the diurnal cycle of the geophysical parameters derived, orbital drift may cause spurious trends in their time series. We investigate tropical deep convective clouds, which show pronounced diurnal cycle amplitude, to estimate an upper bound of the impact of orbital drift on their time series. We carry out a rotated empirical orthogonal function analysis (REOF) and show that the REOFs are useful in delineating orbital drift signal and, more importantly, in subtracting this signal in the time series of convective cloud amount. These results will help facilitate the derivation of homogenized data series of cloud amount from NOAA satellite sensors and ultimately analyzing trends from them. However, we suggest detailed comparison of various methods and rigorous testing thereof applying final orbital drift corrections.

In this study, we employ the global aerosol-climate model ECHAM-HAM to globally assess aerosol indirect effects (AIEs) resulting from shipping emissions of aerosols and aerosol precursor gases. We implement shipping emissions of sulphur dioxide (SO2), black carbon (BC) and particulate organic matter (POM) for the year 2000 into the model and quantify the model’s sensitivity towards uncertainties associated with the emission parameterisation as well as with the shipping emissions themselves. Sensitivity experiments are designed to investigate (i) the uncertainty in the size distribution of emitted particles, (ii) the uncertainty associated with the total amount of emissions, and (iii) the impact of reducing carbonaceous emissions from ships. We use the results from one sensitivity experiment for a detailed discussion of shipping-induced changes in the global aerosol system as well as the resulting impact on cloud properties. From all sensitivity experiments, we find AIEs from shipping emissions to range from −0.32±0.01Wm−2 to −0.07±0.01Wm−2 (global mean value and inter-annual variability as a standard deviation). The magnitude of the AIEs depends much more on the assumed emission size distribution and subsequent aerosol microphysical interactions than on the magnitude of the emissions themselves. It is important to note that although the strongest estimate of AIEs from shipping emissions in this study is relatively large, still much larger estimates have been reported in the literature before on the basis of modelling studies. We find that omitting just carbonaceous particle emissions from ships favours new particle formation in the boundary layer. These newly formed particles contribute just about as much to the CCN budget as the carbonaceous particles would, leaving the globally averaged AIEs nearly unaltered compared to a simulation including carbonaceous particle emissions from ships.

Cloud drop condensation nuclei (CCN) and ice nuclei (IN) particles determine to a large extent cloud microstructure and, consequently, cloud albedo and the dynamic response of clouds to aerosol-induced changes to precipitation. This can modify the reflected solar radiation and the thermal radiation emitted to space. Measurements of tropospheric CCN and IN over large areas have not been possible and can be only roughly approximated from satellite-sensor-based estimates of optical properties of aerosols. Our lack of ability to measure both CCN and cloud updrafts precludes disentangling the effects ofmeteorology fromthose of aerosols and represents the largest component in our uncertainty in anthropogenic climate forcing.Ways to improve the retrieval accuracy include multiangle and multipolarimetric passive measurements of the optical signal and multispectral lidar polarimetric measurements. Indirect methods include proxies of trace gases, as retrieved by hyperspectral sensors. Perhaps the most promising emerging direction is retrieving the CCN properties by simultaneously retrieving convective cloud drop number concentrations and updraft speeds, which amounts to using clouds as natural CCN chambers. These satellite observations have to be constrained by in situ observations of aerosol-cloud-precipitation-climate (ACPC) interactions, which in turn constrain a hierarchy of model simulations of ACPC. Since the essence of a general circulation model is an accurate quantification of the energy and mass fluxes in all forms between the surface, atmosphere and outer space, a route to progress is proposed here in the form of a series of box flux closure experiments in the various climate regimes. A roadmap is provided for quantifying the ACPC interactions and thereby reducing the uncertainty in anthropogenic climate 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.

We use global models to explore the microphysical effects of carbonaceous aerosols on liquid clouds. Although absorption of solar radiation by soot warms the atmosphere, soot may cause climate cooling due to its contribution to cloud condensation nuclei (CCN) and therefore cloud brightness. Six global models conducted three soot experiments; four of the models had detailed aerosol microphysical schemes. The average cloud radiative response to biofuel soot (black and organic carbon), including both indirect and semi-direct effects, is −0.11Wm−2, comparable in size but opposite in sign to the respective direct effect. In a more idealized fossil fuel black carbon experiment, some models calculated a positive cloud response because soot provides a deposition sink for sulfuric and nitric acids and secondary organics, decreasing nucleation and evolution of viable CCN. Biofuel soot particles were also typically assumed to be larger and more hygroscopic than for fossil fuel soot and therefore caused more negative forcing, as also found in previous studies. Diesel soot (black and organic carbon) experiments had relatively smaller cloud impacts with five of the models <±0.06Wm−2 from clouds. The results are subject to the caveats that variability among models, and regional and interrannual variability for each model, are large. This comparison together with previously published results stresses the need to further constrain aerosol microphysical schemes. The non-linearities resulting from the competition of opposing effects on the CCN population make it difficult to extrapolate from idealized experiments to likely impacts of realistic potential emission changes.

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 POLDER-1 instrument was able to measure aerosol and cloud properties for eight months in 1996–1997. We use these observational data for aerosol concentration (the aerosol index), cloud optical thickness, and cloud droplet effective radius to establish statistical relationships among these parameters in order to analyze the first and second aerosol indirect effects. We also evaluate the representation of these effects as parameterized in the Laboratoire de Météorologie Dynamique–Zoom (LMDZ) general circulation model. We find a decrease in cloud top droplet radius with increasing aerosol index in both the model and the observations. Our results are only slightly changed if the analysis is done at fixed cloud liquid water path (LWP) instead of considering all LWP conditions. We also find a positive correlation between aerosol index and cloud liquid water path, which is particularly pronounced over the Northern Hemisphere midlatitudes. This may be interpreted as observational evidence for the second aerosol indirect effect on a large scale. The model-simulated relationship agrees well with that derived from POLDER data. Model simulations show a rather small change in the two relationships if preindustrial rather than present-day aerosol distributions are used. However, when entirely switching off the second aerosol indirect effect in our model, we find a much steeper slope than we do when including it.