A risk-based framework for assessing the effectiveness of stratospheric aerosol geoengineering

Geoengineering by stratospheric aerosol injection has been proposed as a policy response to warming from human emissions of greenhouse gases, but it may produce unequal regional impacts. We present a simple, intuitive risk-based framework for classifying these impacts according to whether geoengineering increases or decreases the risk of substantial climate change, with further classification by the level of existing risk from climate change from increasing carbon dioxide concentrations. This framework is applied to two climate model simulations of geoengineering counterbalancing the surface warming produced by a quadrupling of carbon dioxide concentrations, with one using a layer of sulphate aerosol in the lower stratosphere, and the other a reduction in total solar irradiance. The solar dimming model simulation shows less regional inequality of impacts compared with the aerosol geoengineering simulation. In the solar dimming simulation, 10% of the Earth’s surface area, containing 10% of its population and 11% of its gross domestic product, experiences greater risk of substantial precipitation changes under geoengineering than under enhanced carbon dioxide concentrations. In the aerosol geoengineering simulation the increased risk of substantial precipitation change is experienced by 42% of Earth’s surface area, containing 36% of its population and 60% of its gross domestic product.

Impacts of 20th century aerosol emissions on the South Asian monsoon in the CMIP5 models

Comparison of single-forcing varieties of 20th century historical experiments in a subset of models from the Fifth Coupled Model Intercomparison Project (CMIP5) reveals that South Asian summer monsoon rainfall increases towards the present day in Greenhouse Gas (GHG)-only experiments with respect to pre-industrial levels, while it decreases in anthropogenic aerosol-only experiments. Comparison of these single-forcing experiments with the all-forcings historical experiment suggests aerosol emissions have dominated South Asian monsoon rainfall trends in recent decades, especially during the 1950s to 1970s. The variations in South Asian monsoon rainfall in these experiments follows approximately the time evolution of inter-hemispheric temperature gradient over the same period, suggesting a contribution from the large-scale background state relating to the asymmetric distribution of aerosol emissions about the equator. By examining the 24 available all-forcings historical experiments, we show that models including aerosol indirect effects dominate the negative rainfall trend. Indeed, models including only the direct radiative effect of aerosol show an increase in monsoon rainfall, consistent with the dominance of increasing greenhouse gas emissions and planetary warming on monsoon rainfall in those models. For South Asia, reduced rainfall in the models with indirect effects is related to decreased evaporation at the land surface rather than from anomalies in horizontal moisture flux, suggesting the impact of indirect effects on local aerosol emissions. This is confirmed by examination of aerosol loading and cloud droplet number trends over the South Asia region. Thus, while remote aerosols and their asymmetric distribution about the equator play a role in setting the inter-hemispheric temperature distribution on which the South Asian monsoon, as one of the global monsoons, operates, the addition of indirect aerosol effects acting on very local aerosol emissions also plays a role in declining monsoon rainfall. The disparity between the response of monsoon rainfall to increasing aerosol emissions in models containing direct aerosol effects only and those also containing indirect effects needs to be urgently investigated since the suggested future decline in Asian anthropogenic aerosol emissions inherent to the representative concentration pathways (RCPs) used for future climate projection may turn out to be optimistic. In addition, both groups of models show declining rainfall over China, also relating to local aerosol mechanisms. We hypothesize that aerosol emissions over China are large enough, in the CMIP5 models, to cause declining monsoon rainfall even in the absence of indirect aerosol effects. The same is not true for India.

Intercomparison of shortwave radiative transfer schemes in global aerosol modeling: results from the AeroCom Radiative Transfer Experiment

In this study we examine the performance of 31 global model radiative transfer schemes in cloud-free conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scattering-only aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multi-angular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly −10 to 20%, with over- and underestimates of radiative cooling at lower and higher solar zenith angle, respectively. Inter-model diversity (relative standard deviation) increases from ~10 to 15% as solar zenith angle decreases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

Optical properties of Saharan dust aerosol and contribution from the coarse mode as measured during the Fennec 2011 aircraft campaign

New in-situ aircraft measurements of Saharan dust originating from Mali, Mauritania and Algeria taken during the Fennec 2011 aircraft campaign over a remote part of the Sahara Desert are presented. Size distributions extending to 300 μm are shown, representing measurements extending further into the coarse mode than previously published for airborne Saharan dust. A significant coarse mode was present in the size distribution measurements with effective diameter (deff) from 2.3 to 19.4 μm and coarse mode volume median diameter (dvc) from 5.8 to 45.3 μm. The mean size distribution had a larger relative proportion of coarse mode particles than previous aircraft measurements. The largest particles (with deff >12 μm, or dvc >25 μm) were only encountered within 1 km of the ground. Number concentration, mass loading and extinction coefficient showed inverse relationships to dust age since uplift. Dust particle size showed a weak exponential relationship to dust age. Two cases of freshly uplifted dust showed quite different characteristics of size distribution and number concentration. Single Scattering Albed (SSA) values at 550 nm calculated from the measured size distributions revealed high absorption ranging from 0.70 to 0.97 depending on the refractive index. SSA was found to be strongly related to deff. New instrumentation revealed that direct measurements, behind Rosemount inlets, overestimate SSA by up to 0.11 when deff is greater than 2 μm. This is caused by aircraft inlet inefficiencies and sampling losses. Previous measurements of SSA from aircraft measurements may also have been overestimates for this reason. Radiative transfer calculations indicate that the range of SSAs during Fennec 2011 can lead to underestimates in shortwave atmospheric heating rates by 2.0 to 3.0 times if the coarse mode is neglected. This will have an impact on Saharan atmospheric dynamics and circulation,which should be taken into account by numerical weather prediction and climate models.

A study on the sensitivities of simulated aerosol optical properties to composition and size distribution using airborne measurements

We present a flexible framework to calculate the optical properties of atmospheric aerosols at a given relative humidity based on their composition and size distribution. The similarity of this framework to climate model parameterisations allows rapid and extensive sensitivity tests of the impact of uncertainties in data or of new measurements on climate relevant aerosol properties. The data collected by the FAAM BAe-146 aircraft during the EUCAARI-LONGREX and VOCALS-REx campaigns have been used in a closure study to analyse the agreement between calculated and measured aerosol optical properties for two very different aerosol types. The agreement achieved for the EUCAARI-LONGREX flights is within the measurement uncertainties for both scattering and absorption. However, there is poor agreement between the calculated and the measured scattering for the VOCALS-REx flights. The high concentration of sulphate, which is a scattering aerosol with no absorption in the visible spectrum, made the absorption measurements during VOCALS-REx unreliable, and thus no closure study was possible for the absorption. The calculated hygroscopic scattering growth factor overestimates the measured values during EUCAARI-LONGREX and VOCALS-REx by ∼30% and ∼20%, respectively. We have also tested the sensitivity of the calculated aerosol optical properties to the uncertainties in the refractive indices, the hygroscopic growth factors and the aerosol size distribution. The largest source of uncertainty in the calculated scattering is the aerosol size distribution (∼35%), followed by the assumed hygroscopic growth factor for organic aerosol (∼15%), while the predominant source of uncertainty in the calculated absorption is the refractive index of organic aerosol (28–60%), although we would expect the refractive index of black carbon to be important for aerosol with a higher black carbon fraction.

Regional and monthly and clear-sky aerosol direct radiative effect (and forcing) derived from the GlobAEROSOL-AATSR satellite aerosol product

Using the GlobAEROSOL-AATSR dataset, estimates of the instantaneous, clear-sky, direct aerosol radiative effect and radiative forcing have been produced for the year 2006. Aerosol Robotic Network sun-photometer measurements have been used to characterise the random and systematic error in the GlobAEROSOL product for 22 regions covering the globe. Representative aerosol properties for each region were derived from the results of a wide range of literature sources and, along with the de-biased GlobAEROSOL AODs, were used to drive an offline version of the Met Office unified model radiation scheme. In addition to the mean AOD, best-estimate run of the radiation scheme, a range of additional calculations were done to propagate uncertainty estimates in the AOD, optical properties, surface albedo and errors due to the temporal and spatial averaging of the AOD fields. This analysis produced monthly, regional estimates of the clear-sky aerosol radiative effect and its uncertainty, which were combined to produce annual, global mean values of (−6.7±3.9)Wm−2 at the top of atmosphere (TOA) and (−12±6)Wm−2 at the surface. These results were then used to give estimates of regional, clear-sky aerosol direct radiative forcing, using modelled pre-industrial AOD fields for the year 1750 calculated for the AEROCOM PRE experiment. However, as it was not possible to quantify the uncertainty in the pre-industrial aerosol loading, these figures can only be taken as indicative and their uncertainties as lower bounds on the likely errors. Although the uncertainty on aerosol radiative effect presented here is considerably larger than most previous estimates, the explicit inclusion of the major sources of error in the calculations suggest that they are closer to the true constraint on this figure from similar methodologies, and point to the need for more, improved estimates of both global aerosol loading and aerosol optical properties.

Aerosol scattering and absorption during the EUCAARI-LONGREX flights of the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146: can measurements and models agree?

Scattering and absorption by aerosol in anthropogenically perturbed air masses over Europe has been measured using instrumentation flown on the UK’s BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM) on 14 flights during the EUCAARI-LONGREX campaign in May 2008. The geographical and temporal variations of the derived shortwave optical properties of aerosol are presented. Values of single scattering albedo of dry aerosol at 550 nm varied considerably from 0.86 to near unity, with a campaign average of 0.93 ± 0.03. Dry aerosol optical depths ranged from 0.030 ± 0.009 to 0.24 ± 0.07. An optical properties closure study comparing calculations from composition data and Mie scattering code with the measured properties is presented. Agreement to within measurement uncertainties of 30% can be achieved for both scattering and absorption,but the latter is shown to be sensitive to the refractive indices chosen for organic aerosols, and to a lesser extent black carbon, as well as being highly dependent on the accuracy of the absorption measurements. Agreement with the measured absorption can be achieved either if organic carbon is assumed to be weakly absorbing, or if the organic aerosol is purely scattering and the absorption measurement is an overestimate due to the presence of large amounts of organic carbon. Refractive indices could not be inferred conclusively due to this uncertainty, despite the enhancement in methodology compared to previous studies that derived from the use of the black carbon measurements. Hygroscopic growth curves derived from the wet nephelometer indicate moderate water uptake by the aerosol with a campaign mean f (RH) value (ratio in scattering) of 1.5 (range from 1.23 to 1.63) at 80% relative humidity. This value is qualitatively consistent with the major chemical components of the aerosol measured by the aerosol mass spectrometer, which are primarily mixed organics and nitrate and some sulphate.

Atmospheric electric field measurements in urban environment and the pollutant aerosol weekly dependence

The weekly dependence of pollutant aerosols in the urban environment of Lisbon (Portugal) is inferred from the records of atmospheric electric field at Portela meteorological station (38°47′N,9°08′W). Measurements were made with a Bendorf electrograph. The data set exists from 1955 to 1990, but due to the contaminating effect of the radioactive fallout during 1960 and 1970s, only the period between 1980 and 1990 is considered here. Using a relative difference method a weekly dependence of the atmospheric electric field is found in these records, which shows an increasing trend between 1980 and 1990. This is consistent with a growth of population in the Lisbon metropolitan area and consequently urban activity, mainly traffic. Complementarily, using a Lomb–Scargle periodogram technique the presence of a daily and weekly cycle is also found. Moreover, to follow the evolution of theses cycles, in the period considered, a simple representation in a colour surface plot representation of the annual periodograms is presented. Further, a noise analysis of the periodograms is made, which validates the results found. Two datasets were considered: all days in the period, and fair-weather days only.

Sources, sinks, and transatlantic transport of North African dust aerosol: a multimodel analysis and comparison with remote sensing data

This study evaluates model-simulated dust aerosols over North Africa and the North Atlantic from five global models that participated in the Aerosol Comparison between Observations and Models phase II model experiments. The model results are compared with satellite aerosol optical depth (AOD) data from Moderate Resolution Imaging Spectroradiometer (MODIS), Multiangle Imaging Spectroradiometer (MISR), and Sea-viewing Wide Field-of-view Sensor, dust optical depth (DOD) derived from MODIS and MISR, AOD and coarse-mode AOD (as a proxy of DOD) from ground-based Aerosol Robotic Network Sun photometer measurements, and dust vertical distributions/centroid height from Cloud Aerosol Lidar with Orthogonal Polarization and Atmospheric Infrared Sounder satellite AOD retrievals. We examine the following quantities of AOD and DOD: (1) the magnitudes over land and over ocean in our study domain, (2) the longitudinal gradient from the dust source region over North Africa to the western North Atlantic, (3) seasonal variations at different locations, and (4) the dust vertical profile shape and the AOD centroid height (altitude above or below which half of the AOD is located). The different satellite data show consistent features in most of these aspects; however, the models display large diversity in all of them, with significant differences among the models and between models and observations. By examining dust emission, removal, and mass extinction efficiency in the five models, we also find remarkable differences among the models that all contribute to the discrepancies of model-simulated dust amount and distribution. This study highlights the challenges in simulating the dust physical and optical processes, even in the best known dust environment, and stresses the need for observable quantities to constrain the model processes.

Intercomparison and evaluation of global aerosol microphysical properties among AeroCom models of a range of complexity

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

The AeroCom evaluation and intercomparison of organic aerosol in global models

This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.

Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.

Impacts of increasing the aerosol complexity in the Met Office global numerical weather prediction model.

The inclusion of the direct and indirect radiative effects of aerosols in high-resolution global numerical weather prediction (NWP) models is being increasingly recognised as important for the improved accuracy of short-range weather forecasts. In this study the impacts of increasing the aerosol complexity in the global NWP configuration of the Met Office Unified Model (MetUM) are investigated. A hierarchy of aerosol representations are evaluated including three-dimensional monthly mean speciated aerosol climatologies, fully prognostic aerosols modelled using the CLASSIC aerosol scheme and finally, initialised aerosols using assimilated aerosol fields from the GEMS project. The prognostic aerosol schemes are better able to predict the temporal and spatial variation of atmospheric aerosol optical depth, which is particularly important in cases of large sporadic aerosol events such as large dust storms or forest fires. Including the direct effect of aerosols improves model biases in outgoing long-wave radiation over West Africa due to a better representation of dust. However, uncertainties in dust optical properties propagate to its direct effect and the subsequent model response. Inclusion of the indirect aerosol effects improves surface radiation biases at the North Slope of Alaska ARM site due to lower cloud amounts in high-latitude clean-air regions. This leads to improved temperature and height forecasts in this region. Impacts on the global mean model precipitation and large-scale circulation fields were found to be generally small in the short-range forecasts. However, the indirect aerosol effect leads to a strengthening of the low-level monsoon flow over the Arabian Sea and Bay of Bengal and an increase in precipitation over Southeast Asia. Regional impacts on the African Easterly Jet (AEJ) are also presented with the large dust loading in the aerosol climatology enhancing of the heat low over West Africa and weakening the AEJ. This study highlights the importance of including a more realistic treatment of aerosol–cloud interactions in global NWP models and the potential for improved global environmental prediction systems through the incorporation of more complex aerosol schemes.

The importance of vertical velocity variability for estimates of the indirect aerosol effects

The activation of aerosols to form cloud droplets is dependent upon vertical velocities whose local variability is not typically resolved at the GCM grid scale. Consequently, it is necessary to represent the subgrid-scale variability of vertical velocity in the calculation of cloud droplet number concentration. This study uses the UK Chemistry and Aerosols community model (UKCA) within the Hadley Centre Global Environmental Model (HadGEM3), coupled for the first time to an explicit aerosol activation parameterisation, and hence known as UKCA-Activate. We explore the range of uncertainty in estimates of the indirect aerosol effects attributable to the choice of parameterisation of the subgrid-scale variability of vertical velocity in HadGEM-UKCA. Results of simulations demonstrate that the use of a characteristic vertical velocity cannot replicate results derived with a distribution of vertical velocities, and is to be discouraged in GCMs. This study focuses on the effect of the variance (σw2) of a Gaussian pdf (probability density function) of vertical velocity. Fixed values of σw (spanning the range measured in situ by nine flight campaigns found in the literature) and a configuration in which σw depends on turbulent kinetic energy are tested. Results from the mid-range fixed σw and TKE-based configurations both compare well with observed vertical velocity distributions and cloud droplet number concentrations. The radiative flux perturbation due to the total effects of anthropogenic aerosol is estimated at −1.9 W m−2 with σw = 0.1 m s−1, −2.1 W m−2 with σw derived from TKE, −2.25 W m−2 with σw = 0.4 m s−1, and −2.3 W m−2 with σw = 0.7 m s−1. The breadth of this range is 0.4 W m−2, which is comparable to a substantial fraction of the total diversity of current aerosol forcing estimates. Reducing the uncertainty in the parameterisation of σw would therefore be an important step towards reducing the uncertainty in estimates of the indirect aerosol effects. Detailed examination of regional radiative flux perturbations reveals that aerosol microphysics can be responsible for some climate-relevant radiative effects, highlighting the importance of including microphysical aerosol processes in GCMs.

Aerosol direct radiative effect of smoke over clouds over the southeast Atlantic Ocean from 2006 to 2009

The aerosol direct radiative effect (DRE) of African smoke was analyzed in cloud scenes over the southeast Atlantic Ocean, using Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) satellite observations and Hadley Centre Global Environmental Model version 2 (HadGEM2) climate model simulations. The observed mean DRE was about 30–35 W m−2 in August and September 2006–2009. In some years, short episodes of high-aerosol DRE can be observed, due to high-aerosol loadings, while in other years the loadings are lower but more prolonged. Climate models that use evenly distributed monthly averaged emission fields will not reproduce these high-aerosol loadings. Furthermore, the simulated monthly mean aerosol DRE in HadGEM2 is only about 6 W m−2 in August. The difference with SCIAMACHY mean observations can be partly explained by an underestimation of the aerosol absorption Ångström exponent in the ultraviolet. However, the subsequent increase of aerosol DRE simulation by about 20% is not enough to explain the observed discrepancy between simulations and observations.