A case study of the radiative effect of aerosols over Europe: EUCAARI-LONGREX

The radiative effect of anthropogenic aerosols over Europe during the 2008 European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions Long Range Experiment (EUCAARI-LONGREX) campaign has been calculated using measurements collected by the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 aircraft and radiative transfer modelling. The aircraft sampled anthropogenically perturbed air masses across north-western Europe under anticyclonic conditions with aerosol optical depths ranging from 0.047 to 0.357. For one specially designed “radiative closure” flight, simulated irradiances have been compared to radiation measurements for a case of aged European aerosol in order to explore the validity of model assumptions and the degree of radiative closure that can be attained given the spatial and temporal variability of the observations and their measurement uncertainties. Secondly, the diurnally averaged aerosol radiative effect throughout EUCAARI-LONGREX has been calculated. The surface radiative effect ranged between −3.9 and −22.8 W m−2 (mean −11 ± 5 W m−2), whilst top-of-the-atmosphere (TOA) values were between −2.1 and −12.0 W m−2 (mean −5 ± 3 W m−2). We have quantified the uncertainties in our calculations due to the way in which aerosols and other parameters are represented in a radiative transfer model. The largest uncertainty in the aerosol radiative effect at both the surface and the TOA comes from the spectral resolution of the information used in the radiative transfer model (∼ 17 %) and the aerosol description (composition and size distribution) used in the Mie calculations of the aerosol optical properties included in the radiative transfer model (∼ 7 %). The aerosol radiative effect at the TOA is also highly sensitive to the surface albedo (∼ 12 %)

Coarse and giant particles are ubiquitous in Saharan dust export regions and are radiatively significant over the Sahara

Mineral dust is an important component of the climate system, interacting with radiation, clouds and biogeochemical systems, and impacting atmospheric circulation, air quality, aviation and solar energy generation. These impacts are sensitive 10 to dust particle size distribution (PSD), yet models struggle or even fail to represent coarse (diameter (d) >2.5 μm) and giant (d>20 μm) dust particles and the evolution of the PSD with transport. Here we examine three state-of-the-art airborne observational datasets, all of which measured the full size range of dust (d=0.1 to >100 μm) at different stages during transport, with consistent instrumentation. We quantify the presence and evolution of coarse and giant particles and their contribution to optical properties using airborne observations over the Sahara (from the Fennec field campaign) and in the Saharan Air Layer 15 (SAL) over the tropical eastern Atlantic (from the AER-D field campaign). Observations show significantly more abundant coarse and giant dust particles over the Sahara compared to the SAL: effective diameters of up to 20 μm were observed over the Sahara, compared to 4 μm in the SAL. Excluding giant particles over the Sahara results in significant underestimation of mass concentration (40%), as well as underestimates of both shortwave and 20 longwave extinction (18 and 26% respectively from scattering calculations), while the effects in the SAL are smaller but non-negligible. The larger impact on longwave extinction compared to shortwave implies a bias towards a radiative cooling effect in dust models, which typically exclude giant particles and underestimate coarse mode concentrations. A compilation of published effective diameters against dust age since uplift time suggests that two regimes of dust transport 25 exist. During the initial 1.5 days, both coarse and giant particles are rapidly deposited. During the subsequent 1.5 to 10 days, PSD barely changes with transport, and the coarse mode is retained to a much greater degree than expected from estimates of gravitational sedimentation alone. The reasons for this are unclear, and warrant further investigation in order to improve dust transport schemes, and the associated radiative effects of coarse and giant particles in models

Studies on mineral dust using airborne lidar, ground-based remote sensing, and in situ instrumentation

© 2018 The Author(s). Published by EDP Sciences. This is an Open Access article distributed under the terms of the Creative Commons Attribution License 4.0, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (http://creativecommons.org/licenses/by/4.0/).In August 2015, the AER-D campaign made use of the FAAM research aircraft based in Cape Verde, and targeted mineral dust. First results will be shown here. The campaign had multiple objectives: (1) lidar dust mapping for the validation of satellite and model products; (2) validation of sunphotometer remote sensing with airborne measurements; (3) coordinated measurements with the CATS lidar on the ISS; (4) radiative closure studies; and (5) the validation of a new model of dustsonde.Peer reviewe

How well do the CMIP6 models simulate dust aerosols?

Mineral dust impacts key processes in the Earth system, including the radiation budget, clouds, and nutrient cycles. We evaluate dust aerosols in 16 models participating in the sixth phase of the Coupled Model Intercomparison Project (CMIP6) against multiple reanalyses and satellite observations. Most models, and particularly the multi-model ensemble mean (MEM), capture the spatial patterns and seasonal cycles of global dust processes well. However, large uncertainties and inter-model diversity are found. For example, global dust emissions, primarily driven by model-simulated surface winds, vary by a factor of 5 across models, while the MEM estimate is double the amount in reanalyses. The ranges of CMIP6 model-simulated global dust emission, deposition, burden and optical depth (DOD) are larger than previous generations of models. Models present considerable disagreement in dust seasonal cycles over North China and North America. Here, DOD values are overestimated by most CMIP6 models, with the MEM estimate 1.2–1.7 times larger compared to satellite and reanalysis datasets. Such overestimates can reach up to a factor of 5 in individual models. Models also fail to reproduce some key features of the regional dust distribution, such as dust accumulation along the southern edge of the Himalayas. Overall, there are still large uncertainties in CMIP6 models’ simulated dust processes, which feature inconsistent biases throughout the dust lifecycle between models, particularly in the relationship connecting dust mass to DOD. Our results imply that modelled dust processes are becoming more uncertain as models become more sophisticated. More detailed output relating to the dust cycle in future intercomparison projects will enable better constraints of global dust cycles, and enable the potential identification of observationally-constrained links between dust cycles and optical properties

Thermal infrared dust optical depth and coarse-mode effective diameter retrieved from collocated MODIS and CALIOP observations

In this study, we developed a novel algorithm based on the collocated Moderate Resolution Imaging Spectroradiometer (MODIS) thermal infrared (TIR) observations and dust vertical profiles from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) to simultaneously retrieve dust aerosol optical depth at 10 &micro;m (DAOD10&mu;m) and the coarse-mode dust effective diameter (Deff) over global oceans. The accuracy of the Deff retrieval is assessed by comparing retrieved Deff with the in-situ measured dust particle size distributions (PSDs) from the AER-D, SAMUM-2 and SALTRACE field campaigns through case studies. The new DAOD10&mu;m retrievals were evaluated first through comparisons with the collocated DAOD10.6&mu;m retrieved from the combined Imaging Infrared Radiometer (IIR) and CALIOP observations from our previous study (Zheng et al. 2022). The pixel-to-pixel comparison of the two retrievals indicates a good agreement (R~0.7) and a significant reduction of (~50 %) retrieval uncertainties largely thanks to the better constraint on dust size. In a climatological comparison, the seasonal and regional (5&deg;&times;2&deg;) mean DAOD10um retrievals based on our combined MODIS and CALIOP method are in good agreement with the two independent Infrared Atmospheric Sounding Interferometer (IASI) products over three dust transport regions (i.e., North Atlantic (NA; R = 0.9), Indian Ocean (IO; R = 0.8) and North Pacific (NP; R = 0.7)). Using the new retrievals from 2013 to 2017, we performed a climatological analysis of coarse mode dust Deff over global oceans. We found that dust Deff over IO and NP are up to 20 % smaller than that over NA. Over NA in summer, we found a ~50 % reduction of the number of retrievals with Deff &gt; 5 &mu;m from 15&deg; W to 35&deg; W and a stable trend of Deff average at 4.4 &mu;m from 35&deg; W throughout the Caribbean Sea (90&deg; W). Over NP in spring, only ~5 % of retrieved pixels with Deff &gt; 5 &mu;m are found from 150&deg; E to 180&deg;, while the mean Deff remains stable at 4.0 &mu;m throughout eastern NP. To our best knowledge, this study is the first to retrieve both DAOD and coarse-mode dust particle size over global oceans for multiple years. This retrieval dataset provides insightful information for evaluating dust long-wave radiative effects and coarse mode dust particle size in models.</p

Airborne measurements of trace gases and aerosols over the London metropolitan region

The Emissions around the M25 motorway (EM25) campaign took place over the megacity of London in the United Kingdom in June 2009 with the aim of characterising trace gas and aerosol composition and properties entering and emitted from the urban region. It featured two mobile platforms, the UK BAe-146 Facility for Airborne Atmospheric Measurements (FAAM) research aircraft and a ground-based mobile lidar van, both travelling in circuits around London, roughly following the path of the M25 motorway circling the city. We present an overview of findings from the project, which took place during typical UK summertime pollution conditions. Emission ratios of volatile organic compounds (VOCs) to acetylene and carbon monoxide emitted from the London region were consistent with measurements in and downwind of other large urban areas and indicated traffic and associated fuel evaporation were major sources. Sub-micron aerosol composition was dominated by secondary species including sulphate (24% of sub-micron mass in the London plume and 29% in the non-plume regional aerosol), nitrate (24% plume; 20% regional) and organic aerosol (29% plume; 31% regional). The primary sub-micron aerosol emissions from London were minor compared to the larger regional background, with only limited increases in aerosol mass in the urban plume compared to the background (~12% mass increase on average). Black carbon mass was the major exception and more than doubled in the urban plume, leading to a decrease in the single scattering albedo from 0.91 in the regional aerosol to 0.86 in the London plume, on average. Our observations indicated that regional aerosol plays a major role on aerosol concentrations around London, at least during typical summertime conditions, meaning future efforts to reduce PM levels in London must account for regional as well as local aerosol sources

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

Quantifying particle size and turbulent scale dependence of dust uplift in the Sahara using aircraft measurements

The first size-resolved airborne measurements of dust fluxes and the first dust flux measurements from the central Sahara are presented and compared with a parameterization by Kok (2011a). High-frequency measurements of dust size distribution were obtained from 0.16 to 300 µm diameter, and eddy covariance fluxes were derived. This is more than an order of magnitude larger size range than previous flux estimates. Links to surface emission are provided by analysis of particle drift velocities. Number flux is described by a −2 power law between 1 and 144 µm diameter, significantly larger than the 12 µm upper limit suggested by Kok (2011a). For small particles, the deviation from a power law varies with terrain type and the large size cutoff is correlated with atmospheric vertical turbulent kinetic energy, suggesting control by vertical transport rather than emission processes. The measured mass flux mode is in the range 30–100 µm. The turbulent scales important for dust flux are from 0.1 km to 1–10 km. The upper scale increases during the morning as boundary layer depth and eddy size increase. All locations where large dust fluxes were measured had large topographical variations. These features are often linked with highly erodible surface features, such as wadis or dunes. We also hypothesize that upslope flow and flow separation over such features enhance the dust flux by transporting large particles out of the saltation layer. The tendency to locate surface flux measurements in open, flat terrain means these favored dust sources have been neglected in previous studies

Aircraft and ground measurements of dust aerosols over the west African coast in summer 2015 during ICE-D and AER-D

During the summertime, dust from the Sahara can be efficiently transported westwards within the Saharan air layer (SAL). This can lead to high aerosol loadings being observed above a relatively clean marine boundary layer (MBL) in the tropical Atlantic Ocean. These dust layers can impart significant radiative effects through strong visible and IR light absorption and scattering, and can also have indirect impacts by altering cloud properties. The processing of the dust aerosol can result in changes in both direct and indirect radiative effects, leading to significant uncertainty in climate prediction in this region. During August 2015, measurements of aerosol and cloud properties were conducted off the coast of west Africa as part of the Ice in Cloud Experiment - Dust (ICE-D) and AERosol properties - Dust (AER-D) campaigns. Observations were obtained over a 4-week period using the UK Facility for Atmospheric Airborne Measurements (FAAM) BAe 146 aircraft based on Santiago Island, Cabo Verde. Ground-based observations were collected from Praia (14∘57′ N, 23∘29′ W; 100 m a.s.l.), also located on Santiago Island. The dust in the SAL was mostly sampled in situ at altitudes of 2-4 km, and the potential dust age was estimated by backward trajectory analysis. The particle mass concentration (at diameter d = 0.1-20 µm) decreased with transport time. Mean effective diameter (Deff) for supermicron SAL dust (d = 1-20 µm) was found to be 5-6 µm regardless of dust age, whereas submicron Deff (d = 0.1-1 µm) showed a decreasing trend with longer transport. For the first time, an airborne laser-induced incandescence instrument (the single particle soot photometer - SP2) was deployed to measure the hematite content of dust. For the Sahel-influenced dust in the SAL, the observed hematite mass fraction of dust (FHm) was found to be anti-correlated with the single scattering albedo (SSA, λ = 550 nm, for particles d < 2.5 µm); as potential dust age increased from 2 to 7 days, FHm increased from 2.5 to 4.5 %, SSA decreased from 0.97 to 0.93 and the derived imaginary part (k) of the refractive index at 550 nm increased from 0.0015 to 0.0035. However, the optical properties of Sahara-influenced plumes (not influenced by the Sahel) were independent of dust age and hematite content with SSA ∼ 0.95 and k ∼ 0.0028. This indicates that the absorbing component of dust may be source dependent, or that gravitational settling of larger particles may lead to a higher fraction of more absorbing clay-iron aggregates at smaller sizes. Mie calculation using the measured size distribution and size-resolved refractive indices of the absorbing components (black carbon and hematite) reproduces the measured SSA to within ±0.02 for SAL dust by assuming a goethite ∕ hematite mass ratio of 2. Overall, hematite and goethite constituted 40-80 % of the absorption for particles d < 2.5 µm, and black carbon (BC) contributed 10-37 %. This highlights the importance of size-dependent composition in determining the optical properties of dust and also the contribution from BC within dust plumes

Saharan dust plume charging observed over the UK

A plume of Saharan dust and Iberian smoke was carried across the southern UK on 16th October 2017, entrained into an Atlantic cyclone which had originated as Hurricane Ophelia. The dust plume aloft was widely noticed as it was sufficiently dense to redden the visual appearance of the sun. Time series of backscatter from ceilometers at Reading and Chilbolton show two plumes: one carried upwards to 2.5 km, and another below 800m into the boundary layer, with a clear slot between. Steady descent of particles at about 50 cms−1 continued throughout the morning, and coarse mode particles reached the surface. Plumes containing dust are frequently observed to be strongly charged,often through frictional effects. This plume passed over atmospheric electric field sensors at Bristol, Chilbolton and Reading. Consistent measurements at these three sites indicated negative plume charge. The lower edge plume charge density was (−8.0±3.3) nCm−2, which is several times greater than that typical for stratiform water clouds, implying an active in situ charge generation mechanism such as turbulent triboelectrification. A meteorological radiosonde measuring temperature and humidity was launched into the plume at 1412 UTC, specially instrumented with charge and turbulence sensors. This detected charge in the boundary layer and in the upper plume region, and strong turbulent mixing was observed throughout the atmosphere’s lowest 4 km. The clear slot region, through which particles sedimented, was anomalously dry compared with modelled values, with water clouds forming intermittently in the air beneath. Electrical aspects of dust should be included in numerical models, particularly the charge-related effects on cloud microphysical properties, to accurately represent particle behaviour and transport