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This paper presents the first investigation of the solubility of iron in mineral dust aerosols collected at the Henties Bay Aerosol Observatory (HBAO), in Namibia, from April to December 2017. During the study period, 10 intense dust events occurred. Elemental iron reached peak concentrations as high as 1.5 µg m−3, significantly higher than background levels. These events are attributed to wind erosion of natural soils from the surrounding gravel plains of the Namib desert. The composition of the sampled dust is found to be overall similar to that of aerosols from northern Africa but is characterized by persistent and high concentrations of fluorine which are attributed to local fugitive dust. The fractional solubility of Fe (%SFe) for both the identified dust episodes and background conditions ranged between 1.3 % and 20 % and averaged at 7.9 % (±4.1 %) and 6.8 (±3.3 %), respectively. Even under background conditions, the %SFe was correlated with that of Al and Si. The solubility was lower between June and August and increased from September onwards during the austral spring. The relation to measured concentrations of particulate MSA (methane sulfonic acid), solar irradiance, and wind speed suggests a possible two-way interaction whereby marine biogenic emissions from the coastal Benguela upwelling to the atmosphere would increase the solubility of iron-bearing dust according to the photo-reduction processes. This first investigation points to the western coast of southern Africa as a complex environment with multiple processes and active exchanges between the atmosphere and the Atlantic Ocean, requiring further research.

Aerosol-aware microphysics parameterisation schemes are increasingly being introduced into numerical weather prediction models, allowing for regional and case-specific parameterisation of cloud condensation nuclei (CCN) and cloud droplet interactions. In this paper, the Thompson aerosol-aware microphysics scheme, within the Weather Research and Forecasting (WRF) model, is used for two fog cases during September 2017 over Namibia. Measurements of CCN and fog microphysics were undertaken during the AErosols, RadiatiOn and CLOuds in southern Africa (AEROCLO-sA) field campaign at Henties Bay on the coast of Namibia during September 2017. A key concept of the microphysics scheme is the conversion of water-friendly aerosols to cloud droplets (hereafter referred to as CCN activation), which could be estimated from the observations. A fog monitor 100 (FM-100) provided cloud droplet size distribution, number concentration (Nt), liquid water content (LWC), and mean volumetric diameter (MVD). These measurements are used to evaluate and parameterise WRF model simulations of Nt, LWC, and MVD. A sensitivity analysis was conducted through variations to the initial CCN concentration, CCN radius, and the minimum updraft speed, which are important factors that influence droplet activation in the microphysics scheme of the model. The first model scenario made use of the default settings with a constant initial CCN number concentration of 300 cm−3 and underestimated the cloud droplet number concentration, while the LWC was in good agreement with the observations. This resulted in droplet size being larger than the observations. Another scenario used modelled data as CCN initial conditions, which were an order of magnitude higher than other scenarios. However, these provided the most realistic values of Nt, LWC, MVD, and droplet size distribution. From this, it was concluded that CCN activation of around 10 % in the simulations is too low, while the observed appears to be higher reaching between 20 % and 80 %, with a mean (median) of 0.55 (0.56) during fog events. To achieve this level of activation in the model, the minimum updraft speed for CCN activation was increased from 0.01 to 0.1 m s−1. This scenario provided Nt, LWC, MVD, and droplet size distribution in the range of the observations, with the added benefit of a realistic initial CCN concentration. These results demonstrate the benefits of a dynamic aerosol-aware scheme when parameterised with observations.

Naturally and anthropogenically emitted aerosols, which are determined by their physical and chemical properties, have an impact on both air quality and the radiative properties of the earth. An important source of atmospheric particulate matter (PM) in South Africa is household combustion for space heating and cooking, which predominantly occurs in low-income urban settlements. The aim of this study was to conduct a detailed size-resolved assessment of chemical characteristics of aerosols associated with household combustion through the collection of particulates in low-income urban settlements in South Africa to quantify the extent of the impacts of atmospheric pollution. Outdoor (ambient) and indoor aerosols in different size fractions were collected during summer and winter in four low-income urban settlements located in the north-eastern interior on the South African Highveld, i.e. Kwadela, Kwazamokuhle, Zamdela, and Jouberton. Mass concentration and chemical composition was determined for three size fractions, namely, PM1, PM2.5, and PM2.5−10. The highest concentrations of particulates were measured indoors with the highest mass concentration determined in the indoor PM2.5−10 (coarse) size fraction. However, the highest mass concentrations were determined in PM1 in all outdoor aerosol samples collected during winter and summer, and in indoor samples collected during summer. Significantly higher concentrations were determined for SO4-2 in outdoor and indoor particulates compared to other ionic species, with NH4+ and NO3- being the second most abundant. SO4-2 and NH4+ almost exclusively occurred in the PM1 size fraction, while NO3- was the major constituent in the larger size fractions. The highest SO4-2 levels were recorded for the winter and summer outdoor campaigns conducted at Zamdela, while NO3- and NH4+ concentrations were higher during the winter outdoor campaign. The combined concentrations of trace elements were higher for indoor particulates compared to outdoor aerosols, while the total trace element concentrations in PM1 were substantially higher than levels thereof in the two larger size fractions of particulates collected during all sampling campaigns. No distinct seasonal trend was observed for the concentrations of trace elements. Na, Ca, and Cr had the highest concentrations in particulates collected during outdoor and indoor sampling campaigns. Ni concentrations in outdoor and indoor aerosols exceeded the annual average European standard. PM1 collected during all sampling campaigns in low-income urban settlements had the highest organic carbon (OC) and elemental carbon (EC) concentrations. The highest OC and EC levels were determined in PM1 collected during the winter indoor campaign. OC and EC concentrations were highest during winter, which can be attributed to changes in meteorological patterns and increased household combustion during winter. Low OC/EC ratios determined for particulates collected in low-income urban settlements are indicative of OC and EC being mainly associated with local sources of these species. OC concentrations determined in this study were an order of magnitude lower than OC concentrations determined for ambient aerosols collected in the north-eastern interior of South Africa, while similar EC levels were measured. According to estimated dust concentrations, it was indicated that dust is the major constituent in all size ranges of particulates collected in this study, while trace elements were the second most abundant. However, trace elements made the highest contribution to indoor PM1 and PM1−2.5 mass. Mass concentrations and chemical concentrations determined for aerosols collected in low-income settlements reflect the regional impacts of anthropogenic sources in the north-eastern interior of South Africa and the influence of local sources.

The formation of a river of smoke crossing southern Africa was investigated during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) campaign in September 2017. A complementary set of global and mesoscale numerical simulations as well as ground-based, airborne and space-borne observations of the dynamics, thermodynamics and composition of the atmosphere are used to characterize the river of smoke in terms of timing and vertical extent of the biomass burning aerosol (BBA) layer. The study area was under the synoptic influence of a coastal low rooted in a tropical easterly wave and a high-pressure system over the continent and westerly waves at mid latitudes, one of which had an embedded cut-off low (CoL). The coastal low interacted with the second of two approaching westerly waves and ultimately formed a mid-level tropical temperate trough (TTT). The TTT created the fast-moving air mass transported to the southwestern Indian Ocean as a river of smoke. The CoL, which developed and intensified in the upper levels associated with the first (easternmost) westerly wave, remained stationary above northern Namibia prior to the formation of the TTT and was responsible for the thickening of the BBA layer. This shows that the evolution of the river of smoke is very much tied to the evolution of the TTT, while its vertical extent is related to the presence of the CoL. The mechanisms by which the CoL, observed over Namibia in the entrance region of the river of smoke, influences the vertical structure of the BBA layer is mainly associated with the ascending motion above the BBA layer. In the presence of the CoL, the top of the BBA layer over northern Namibia reaches altitudes above 8 km. This is much higher than the average height of the top of the BBA layer over the regions where the smoke comes from (Angola, Zambia, Zimbabwe, Mozambique), which is 5 to 6 km. The results suggest that the interaction between the TTTs and the CoLs which form during the winter may have a role in promoting the transport of BBA from fire-prone regions in the tropical band to the temperate mid latitudes and the southwestern Indian Ocean.

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ∼350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ∼100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

The chemical composition of aerosols is of particular importance to assess their interactions with radiation, clouds and trace gases in the atmosphere and consequently their effects on air quality and the regional climate. In this study, we present the results of the first long-term dataset of the aerosol chemical composition at an observatory on the coast of Namibia, facing the south-eastern Atlantic Ocean. Aerosol samples in the mass fraction of particles smaller than 10 µm in aerodynamic diameter (PM10) were collected during 26 weeks between 2016 and 2017 at the ground-based Henties Bay Aerosol Observatory (HBAO; 22∘6′ S, 14∘30′ E; 30 m above mean sea level). The resulting 385 filter samples were analysed by X-ray fluorescence and ion chromatography for 24 inorganic elements and 15 water-soluble ions. Statistical analysis by positive matrix factorisation (PMF) identified five major components, sea salt (mass concentration: 74.7±1.9 %), mineral dust (15.7±1.4 %,), ammonium neutralised (6.1±0.7 %), fugitive dust (2.6±0.2 %) and industry (0.9±0.7 %). While the contribution of sea salt aerosol was persistent, as the dominant wind direction was south-westerly and westerly from the open ocean, the occurrence of mineral dust was episodic and coincided with high wind speeds from the south-south-east and the north-north-west, along the coastline. Concentrations of heavy metals measured at HBAO were higher than reported in the literature from measurements over the open ocean. V, Cd, Pb and Nd were attributed to fugitive dust emitted from bare surfaces or mining activities. As, Zn, Cu, Ni and Sr were attributed to the combustion of heavy oils in commercial ship traffic across the Cape of Good Hope sea route, power generation, smelting and other industrial activities in the greater region. Fluoride concentrations up to 25 µg m−3 were measured, as in heavily polluted areas in China. This is surprising and a worrisome result that has profound health implications and deserves further investigation. Although no clear signature for biomass burning could be determined, the PMF ammonium-neutralised component was described by a mixture of aerosols typically emitted by biomass burning, but also by other biogenic activities. Episodic contributions with moderate correlations between NO3-, nss-SO42- (higher than 2 µg m−3) and nss-K+ were observed, further indicative of the potential for an episodic source of biomass burning. Sea salt accounted for up to 57 % of the measured mass concentrations of SO42-, and the non-sea salt fraction was contributed mainly by the ammonium-neutralised component and small contributions from the mineral dust component. The marine biogenic contribution to the ammonium-neutralised component is attributed to efficient oxidation in the moist marine atmosphere of sulfur-containing gas phase emitted by marine phytoplankton in the fertile waters offshore in the Benguela Upwelling System. The data presented in this paper provide the first ever information on the temporal variability of aerosol concentrations in the Namibian marine boundary layer. This data also provide context for intensive observations in the area.

Continuous measurements between July 2012 and December 2015 at the Henties Bay Aerosol Observatory (HBAO; 22∘ S, 14∘05′ E), Namibia, show that, during the austral wintertime, transport of light-absorbing black carbon aerosols occurs at low level into the marine boundary layer. The average of daily concentrations of equivalent black carbon (eBC) over the whole sampling period is 53 (±55) ng m−3. Peak values above 200 ng m−3 and up to 800 ng m−3 occur seasonally from May to August, ahead of the dry season peak of biomass burning in southern Africa (August to October). Analysis of 3-day air mass back-trajectories show that air masses from the South Atlantic Ocean south of Henties Bay are generally cleaner than air having originated over the ocean north of Henties Bay, influenced by the outflow of the major biomass burning plume, and from the continent, where wildfires occur. Additional episodic peak concentrations, even for oceanic transport, indicate that pollution from distant sources in South Africa and maritime traffic along the Atlantic ship tracks could be important. While we expect the direct radiative effect to be negligible, the indirect effect on the microphysical properties of the stratocumulus clouds and the deposition to the ocean could be significant and deserve further investigation, specifically ahead of the dry season.

In many investigations of tropospheric chemistry information about the two dimensional distribution of trace gases on a small scale (e.g. tens to hundreds of metres) is highly desirable. An airborne instrument based on imaging Differential Optical Absorption Spectroscopy has been built to map the two dimensional distribution of a series of relevant trace gases including NO2, HCHO, C2H2O2, H2O, O4, SO2, and BrO on a scale of 100 m. Here we report on the first tests of the novel aircraft instrument over the industrialised South African Highveld, where large variations in NO2 column densities in the immediate vicinity of several sources e.g. power plants or steel works, were measured. The observed patterns in the trace gas distribution are interpreted with respect to flux estimates, and it is seen that the fine resolution of the measurements allows separate sources in close proximity to one another to be distinguished.