Using aircraft measurements to determine the refractive index of Saharan dust during the DODO Experiments

Much uncertainty in the value of the imaginary part of the refractive index of mineral dust contributes to uncertainty in the radiative effect of mineral dust in the atmosphere. A synthesis of optical, chemical and physical in-situ aircraft measurements from the DODO experiments during February and August 2006 are used to calculate the refractive index mineral dust encountered over West Africa. Radiative transfer modeling and measurements of broadband shortwave irradiance at a range of altitudes are used to test and validate these calculations for a specific dust event on 23 August 2006 over Mauritania. Two techniques are used to determine the refractive index: firstly a method combining measurements of scattering, absorption, size distributions and Mie code simulations, and secondly a method using composition measured on filter samples to apportion the content of internally mixed quartz, calcite and iron oxide-clay aggregates, where the iron oxide is represented by either hematite or goethite and clay by either illite or kaolinite. The imaginary part of the refractive index at 550 nm (ni550) is found to range between 0.0001 i to 0.0046 i, and where filter samples are available, agreement between methods is found depending on mineral combination assumed. The refractive indices are also found to agree well with AERONET data where comparisons are possible. ni550 is found to vary with dust source, which is investigated with the NAME model for each case. The relationship between both size distribution and ni550 on the accumulation mode single scattering albedo at 550 nm (ω0550) are examined and size distribution is found to have no correlation to ω0550, while ni550 shows a strong linear relationship with ω0550. Radiative transfer modeling was performed with different models (Mie-derived refractive indices, but also filter sampling composition assuming both internal and external mixing). Our calculations indicate that Mie-derived values of ni550 and the externally mixed dust where the iron oxide-clay aggregate corresponds to the goethite-kaolinite combination result in the best agreement with irradiance measurements. The radiative effect of the dust is found to be very sensitive to the mineral combination (and hence refractive index) assumed, and to whether the dust is assumed to be internally or externally mixed

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

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NO<sub>x</sub>) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NO<sub>x</sub> and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9–0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations

Direct radiative effect of aerosols emitted by transport from road, shipping and aviation

Aerosols and their precursors are emitted abundantly by transport activities. Transportation constitutes one of the fastest growing activities and its growth is predicted to increase significantly in the future. Previous studies have estimated the aerosol direct radiative forcing from one transport sub-sector, but only one study to our knowledge estimated the range of radiative forcing from the main aerosol components (sulphate, black carbon (BC) and organic carbon) for the whole transportation sector. In this study, we compare results from two different chemical transport models and three radiation codes under different hypothesis of mixing: internal and external mixing using emission inventories for the year 2000. The main results from this study consist of a positive direct radiative forcing for aerosols emitted by road traffic of +20±11 mW m−2 for an externally mixed aerosol, and of +32±13 mW m−2 when BC is internally mixed. These direct radiative forcings are much higher than the previously published estimate of +3±11 mW m−2. For transport activities from shipping, the net direct aerosol radiative forcing is negative. This forcing is dominated by the contribution of the sulphate. For both an external and an internal mixture, the radiative forcing from shipping is estimated at −26±4 mW m−2. These estimates are in very good agreement with the range of a previously published one (from −46 to −13 mW m−2) but with a much narrower range. By contrast, the direct aerosol forcing from aviation is estimated to be small, and in the range −0.9 to +0.3 mW m−2

Can explicit convection improve modelled dust in summertime West Africa?

Global and regional models have large systematic errors in their modelled dust fields over West Africa. It is well established that cold-pool outflows from moist convection (haboobs) can raise over 50% of the dust over parts of the Sahara and Sahel in summer, but parameterised moist convection tends to give a very poor representation of this in models. Here, we test the hypothesis that an explicit representation of convection in the Met Office Unified Model (UM) improves haboob winds and so may reduce errors in modelled dust fields. The results show that despite varying both grid spacing and the representation of convection there are only minor changes in dust aerosol optical depth (AOD) and dust mass loading fields between simulations. In all simulations there is an AOD deficit over the observed central Saharan dust maximum and a high bias in AOD along the west coast: both features are consistent with many climate (CMIP5) models. Cold-pool outflows are present in the explicit simulations and do raise dust. Consistent with this, there is an improved diurnal cycle in dust-generating winds with a seasonal peak in evening winds at locations with moist convection that is absent in simulations with parameterised convection. However, the explicit convection does not change the AOD field in the UM significantly for several reasons. Firstly, the increased windiness in the evening from haboobs is approximately balanced by a reduction in morning winds associated with the breakdown of the nocturnal low-level jet (LLJ). Secondly, although explicit convection increases the frequency of the strongest winds, they are still weaker than observed, especially close to the observed summertime Saharan dust maximum: this results from the fact that, although large mesoscale convective systems (and resultant cold pools) are generated, they have a lower frequency than observed and haboob winds are too weak. Finally, major impacts of the haboobs on winds occur over the Sahel, where, although dust uplift is known to occur in reality, uplift in the simulations is limited by a seasonally constant bare-soil fraction in the model, together with soil moisture and clay fractions which are too restrictive of dust emission in seasonally varying vegetated regions. For future studies, the results demonstrate (1) the improvements in behaviour produced by the explicit representation of convection, (2) the value of simultaneously evaluating both dust and winds and (3) the need to develop parameterisations of the land surface alongside those of dust-generating winds

The effect of South American biomass burning aerosol emissions on the regional climate

The impact of biomass burning aerosol (BBA) on the regional climate in South America is assessed using 30-year simulations with a global atmosphere-only configuration of the Met Office Unified Model. We compare two simulations of high and low emissions of biomass burning aerosol based on realistic interannual variability. The aerosol scheme in the model has hygroscopic growth and optical properties for BBA informed by recent observations, including those from the recent South American Biomass Burning Analysis (SAMBBA) intensive aircraft observations made during September 2012. We find that the difference in the September (peak biomass emissions month) BBA optical depth between a simulation with high emissions and a simulation with low emissions corresponds well to the difference in the BBA emissions between the two simulations, with a 71.6 % reduction from high to low emissions for both the BBA emissions and the BB AOD in the region with maximum emissions (defined by a box of extent 5–25° S, 40–70° W, used for calculating mean values given below). The cloud cover at all altitudes in the region of greatest BBA difference is reduced as a result of the semi-direct effect, by heating of the atmosphere by the BBA and changes in the atmospheric stability and surface fluxes. Within the BBA layer the cloud is reduced by burn-off, while the higher cloud changes appear to be responding to stability changes. The boundary layer is reduced in height and stabilized by increased BBA, resulting in reduced deep convection and reduced cloud cover at heights of 9–14 km, above the layer of BBA. Despite the decrease in cloud fraction, September downwelling clear-sky and all-sky shortwave radiation at the surface is reduced for higher emissions by 13.77 ± 0.39 W m−2 (clear-sky) and 7.37 ± 2.29 W m−2 (all-sky), whilst the upwelling shortwave radiation at the top of atmosphere is increased in clear sky by 3.32 ± 0.09 W m−2, but decreased by −1.36±1.67 W m−2 when cloud changes are included. Shortwave heating rates increase in the aerosol layer by 18 % in the high emissions case. The mean surface temperature is reduced by 0.14 ± 0.24 °C and mean precipitation is reduced by 14.5 % in the peak biomass region due to both changes in cloud cover and cloud microphysical properties. If the increase in BBA occurs in a particularly dry year, the resulting reduction in precipitation may exacerbate the drought. The position of the South Atlantic high pressure is slightly altered by the presence of increased BBA, and the strength of the southward low-level jet to the east of the Andes is increased. There is some evidence that some impacts of increased BBA persist through the transition into the monsoon, particularly in precipitation, but the differences are only statistically significant in some small regions in November. This study therefore provides an insight into how variability in deforestation, realized through variability in biomass burning emissions, may contribute to the South American climate, and consequently on the possible impacts of future changes in BBA emissions

Quantifying sources of inter-model diversity in the cloud albedo effect

There is large diversity in simulated aerosol forcing among models that participated in the fifth Coupled Model Intercomparison Project (CMIP5), particularly related to aerosol interactions with clouds. Here we use the reported model data and fitted aerosol-cloud relations to separate the main sources of inter-model diversity in the magnitude of the cloud albedo effect. There is large diversity in the global load and spatial distribution of sulfate aerosol, as well as in global-mean cloud-top effective radius. The use of different parameterizations of aerosol-cloud interactions makes the largest contribution to diversity in modeled radiative forcing (up to -39%, +48% about the mean estimate). Uncertainty in pre-industrial sulfate load also makes a substantial contribution (-15%, +61% about the mean estimate), with smaller contributions from inter-model differences in the historical change in sulfate load and in mean cloud fraction

The influence of anthropogenic aerosol on multi-decadal variations of historical global climate

Analysis of single forcing runs from CMIP5 (the fifth Coupled Model Intercomparison Project) simulations shows that the mid-twentieth century temperature hiatus, and the coincident decrease in precipitation, is likely to have been influenced strongly by anthropogenic aerosol forcing. Models that include a representation of the indirect effect of aerosol better reproduce inter-decadal variability in historical global-mean near-surface temperatures, particularly the cooling in the 1950s and 1960s, compared to models with representation of the aerosol direct effect only. Models with the indirect effect also show a more pronounced decrease in precipitation during this period, which is in better agreement with observations, and greater inter-decadal variability in the inter-hemispheric temperature difference. This study demonstrates the importance of representing aerosols, and their indirect effects, in general circulation models, and suggests that inter-model diversity in aerosol burden and representation of aerosol–cloud interaction can produce substantial variation in simulations of climate variability on multi decadal timescales

Black carbon measurements in the boundary layer over western and northern Europe

Europe is a densely populated region that is a significant global source of black carbon (BC) aerosol, but there is a lack of information regarding the physical properties and spatial/vertical distribution of rBC in the region. We present the first aircraft observations of sub-micron refractory BC (rBC) aerosol concentrations and physical properties measured by a single particle soot photometer (SP2) in the lower troposphere over Europe. The observations spanned a region roughly bounded by 50° to 60° N and from 15° W to 30° E. The measurements, made between April and September 2008, showed that average rBC mass concentrations ranged from about 300 ng m−3 near urban areas to approximately 50 ng m−3 in remote continental regions, lower than previous surface-based measurements. rBC represented between 0.5 and 3% of the sub-micron aerosol mass. Black carbon mass size distributions were log-normally distributed and peaked at approximately 180 nm, but shifted to smaller diameters (~160 nm) near source regions. rBC was correlated with carbon monoxide (CO) but had different ratios to CO depending on location and air mass. Light absorption coefficients were measured by particle soot absorption photometers on two separate aircraft and showed similar geographic patterns to rBC mass measured by the SP2. We summarize the rBC and light absorption measurements as a function of longitude and air mass age and also provide profiles of rBC mass concentrations and size distribution statistics. Our results will help evaluate model-predicted regional rBC concentrations and properties and determine regional and global climate impacts from rBC due to atmospheric heating and surface dimming

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