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Low-level stratiform clouds (LLSCs) covering a large area appear frequently during the wet monsoon season in southern West Africa. This region is also a place where different types of aerosols coexist, including biomass burning aerosols coming from central and southern Africa and aerosols emitted by local anthropogenic activities. We investigate the indirect and semi-direct effects of these aerosols on the life cycle of LLSCs by conducting a case study based on airborne and ground-based observations from the field campaign of Dynamic-Aerosol-Chemistry-Cloud-Interaction in West Africa (DACCIWA). This case is modeled using a large-eddy-simulation (LES) model with fine resolution and in situ aerosol measurements, including size distribution and chemical composition. The model has successfully reproduced the observed life cycle of the LLSC, from stratus formation to stabilization during the night and to upward development after sunrise until break-up of the cloud deck in the late afternoon. Additional sensitivity simulations using different measured aerosol profiles also suggest that aerosols can affect the cloud life cycle through both the indirect and semi-direct effects. As expected, modeled cloud microphysical features, including cloud droplet number concentration, mean radius, and thus cloud reflectivity, are all controlled by aerosol concentration. However, it is found that the variation in cloud reflectivity induced by different aerosol profiles is not always the only factor in determining the incoming solar radiation at the ground and thus for the cloud life cycle after sunrise. Instead, the difference in cloud fraction brought by dry-air entrainment from above and thus the speed of consequent evaporation – also influenced by aerosol concentration – is another important factor to consider. Clouds influenced by higher aerosol concentrations and thus with a higher number concentration and smaller sizes of cloud droplets are found to evaporate more easily and thus impose a lower cloud fraction. In addition, our sensitivity runs including versus excluding aerosol direct radiative effects have also demonstrated the impacts specifically of solar absorption by black carbon on the cloud life cycle. The semi-direct effect resulting from an excessive atmospheric heating of up to 12 K d -1 by black carbon in our modeled cases is found to lower the cloud top as well as the liquid water path, reducing surface incoming solar radiation and dry entrainment and increasing the cloud fraction. [ABSTRACT FROM AUTHOR]

Direct and semi‐direct radiative effects of biomass burning aerosols (BBA) from southern and central African fires are still widely debated, in particular because climate models have been unsuccessful in reproducing the low single scattering albedo in BBA over the eastern Atlantic Ocean. Using state‐of‐the‐art airborne in situ measurements and Mie scattering simulations, we demonstrate that low single scattering albedo in well‐aged BBA plumes over southern West Africa results from the presence of strongly absorbing refractory black carbon (rBC), whereas the brown carbon contribution to the BBA absorption is negligible. Coatings enhance light absorption by rBC‐containing particles by up to 210%. Our results show that accounting for the diversity in black carbon mixing state by combining internal and external configurations is needed to accurately estimate the optical properties and henceforth the shortwave direct radiative effect and heating rate of BBA over southern West Africa. Plain Language Summary: Extensive seasonal fires over southern and central Africa result in the transport of massive amounts of biomass burning aerosols over huge areas of the eastern Atlantic Ocean. Recent field observations highlight that biomass burning aerosols transported from the coast of southern Africa to the far north over southern West Africa were characterized by low single scattering albedo. This finding is of paramount interest, because radiative heating within the absorbing aerosol layer is hypothesized to affect the low cloud deck over this specific region and may ultimately influence the large‐scale circulation. However, debate remains about the causes of the low single scattering albedo by biomass burning aerosols, causing ambiguous parameterizations of their optical properties in climate models. Here we present simultaneous airborne measurements of the composition and optical properties of biomass burning aerosols transported over southern West Africa. We show that black carbon particles dominated the light absorption by biomass burning aerosols at mid‐visible wavelengths. Our findings indicate that the black carbon mixing state plays a significant role in the aerosol optical properties and may be an important modulator to be considered in climate models for simulating direct and semi‐direct radiative effects of biomass burning aerosol over southern West Africa. Key Points: The low single scattering albedo in biomass burning aerosol (BBA) over southern West Africa results from the presence of refractory black carbonThe brown carbon contribution to the aerosol absorption is negligible in these well‐aged BBA plumesAccounting for the diversity in black carbon mixing state is needed to accurately estimate BBA optical properties [ABSTRACT FROM AUTHOR]

Southern West Africa (SWA) is an African pollution hotspot but a relatively poorly sampled region of the world. We present an overview of in situ aerosol optical measurements collected over SWA in June and July 2016 as part as of the DACCIWA (Dynamics-Aerosol-Chemistry-Clouds Interactions in West Africa) airborne campaign. The aircraft sampled a wide range of air masses, including anthropogenic pollution plumes emitted from the coastal cities, long-range transported biomass burning plumes from central and southern Africa and dust plumes from the Sahara and Sahel region, as well as mixtures of these plumes. The specific objective of this work is to characterize the regional variability of the vertical distribution of aerosol particles and their spectral optical properties (single scattering albedo: SSA, asymmetry parameter, extinction mass efficiency, scattering Ångström exponent and absorption Ångström exponent: AAE). The first findings indicate that aerosol optical properties in the planetary boundary layer were dominated by a widespread and persistent biomass burning loading from the Southern Hemisphere. Despite a strong increase in aerosol number concentration in air masses downwind of urban conglomerations, spectral SSA were comparable to the background and showed signatures of the absorption characteristics of biomass burning aerosols. In the free troposphere, moderately to strongly absorbing aerosol layers, dominated by either dust or biomass burning particles, occurred occasionally. In aerosol layers dominated by mineral dust particles, SSA varied from 0.81 to 0.92 at 550 nm depending on the variable proportion of anthropogenic pollution particles externally mixed with the dust. For the layers dominated by biomass burning particles, aerosol particles were significantly more light absorbing than those previously measured in other areas (e.g. Amazonia, North America), with SSA ranging from 0.71 to 0.77 at 550 nm. The variability of SSA was mainly controlled by variations in aerosol composition rather than in aerosol size distribution. Correspondingly, values of AAE ranged from 0.9 to 1.1, suggesting that lens-coated black carbon particles were the dominant absorber in the visible range for these biomass burning aerosols. Comparison with the literature shows a consistent picture of increasing absorption enhancement of biomass burning aerosol from emission to remote location and underscores that the evolution of SSA occurred a long time after emission. The results presented here build a fundamental basis of knowledge about the aerosol optical properties observed over SWA during the monsoon season and can be used in climate modelling studies and satellite retrievals. In particular and regarding the very high absorbing properties of biomass burning aerosols over SWA, our findings suggest that considering the effect of internal mixing on absorption properties of black carbon particles in climate models should help better assess the direct and semi-direct radiative effects of biomass burning particles. [ABSTRACT FROM AUTHOR]

Vast stretches of agricultural land in southern and central Africa are burnt between June and September each year, which releases large quantities of aerosol into the atmosphere. The resulting smoke plumes are carried west over the Atlantic Ocean at altitudes between 2 and 4 km. As only limited observational data in West Africa have existed until now, whether this pollution has an impact at lower altitudes has remained unclear. The Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) aircraft campaign took place in southern West Africa during June and July 2016, with the aim of observing gas and aerosol properties in the region in order to assess anthropogenic and other influences on the atmosphere. Results presented here show that a significant mass of aged accumulation mode aerosol was present in the southern West African monsoon layer, over both the ocean and the continent. A median dry aerosol concentration of 6.2 µ g m -3 (standard temperature and pressure, STP) was observed over the Atlantic Ocean upwind of the major cities, with an interquartile range from 5.3 to 8.0 µ g m -3. This concentration increased to a median of 11.1 µ g m -3 (8.6 to 15.7 µ g m -3) in the immediate outflow from cities. In the continental air mass away from the cities, the median aerosol loading was 7.5 µ g m -3 (5.9 to 10.5 µ g m -3). The accumulation mode aerosol population over land displayed similar chemical properties to the upstream population, which implies that upstream aerosol is a significant source of aerosol pollution over the continent. The upstream aerosol is found to have most likely originated from central and southern African biomass burning. This demonstrates that biomass burning plumes are being advected northwards, after being entrained into the monsoon layer over the eastern tropical Atlantic Ocean. It is shown observationally for the first time that they contribute up to 80 % to the regional aerosol loading in the monsoon layer over southern West Africa. Results from the COSMO-ART (Consortium for Small-scale Modeling – Aerosol and Reactive Trace gases) and GEOS-Chem models support this conclusion, showing that observed aerosol concentrations over the northern Atlantic Ocean can only be reproduced when the contribution of transported biomass burning aerosol is taken into account. As a result, the large and growing emissions from the coastal cities are overlaid on an already substantial aerosol background. Simulations using COSMO-ART show that cloud droplet number concentrations can increase by up to 27 % as a result of transported biomass burning aerosol. On a regional scale this renders cloud properties and precipitation less sensitive to future increases in anthropogenic emissions. In addition, such high background loadings will lead to greater pollution exposure for the large and growing population in southern West Africa. These results emphasise the importance of including aerosol from across country borders in the development of air pollution policies and interventions in regions such as West Africa. [ABSTRACT FROM AUTHOR]

Low-level clouds (LLCs) cover a wide area of southern West Africa (SWA) during the summer monsoon months and have an important cooling effect on the regional climate. Previous studies of these clouds have focused on modelling and remote sensing via satellite. We present the first comprehensive set of in situ measurements of cloud microphysics from the region, taken during June–July 2016, as part of the DACCIWA (Dynamics–aerosol–chemistry–cloud interactions in West Africa) campaign. This novel dataset allows us to assess spatial, diurnal, and day-to-day variation in the properties of these clouds over the region. LLCs developed overnight and mean cloud cover peaked a few hundred kilometres inland around 10:00 local solar time (LST), before clouds began to dissipate and convection intensified in the afternoon. Regional variation in LLC cover was largely orographic, and no lasting impacts in cloud cover related to pollution plumes were observed downwind of major population centres. The boundary layer cloud drop number concentration (CDNC) was locally variable inland, ranging from 200 to 840 cm-3 (10th and 90th percentiles at standard temperature and pressure), but showed no systematic regional variations. Enhancements were seen in pollution plumes from the coastal cities but were not statistically significant across the region. A significant fraction of accumulation mode aerosols, and therefore cloud condensation nuclei, were from ubiquitous biomass burning smoke transported from the Southern Hemisphere. To assess the relative importance of local and transported aerosol on the cloud field, we isolated the local contribution to the aerosol population by comparing inland and offshore size and composition measurements. A parcel model sensitivity analysis showed that doubling or halving local emissions only changed the calculated cloud drop number concentration by 13 %–22 %, as the high background meant local emissions were a small fraction of total aerosol. As the population of SWA grows, local emissions are expected to rise. Biomass burning smoke transported from the Southern Hemisphere is likely to dampen any effect of these increased local emissions on cloud–aerosol interactions. An integrative analysis between local pollution and Central African biomass burning emissions must be considered when predicting anthropogenic impacts on the regional cloud field during the West African summer monsoon. [ABSTRACT FROM AUTHOR]

The western coast of southern Africa off Namibia is characterized by a semi-permanent and widespread stratocumulus (Sc) cloud deck, very frequent coastal fog, and the oceanic northern Benguela upwelling system (nBUS). It is also the crossroad of large quantities of natural and anthropogenic aerosols of distant and local origins (biogenic, anthropogenic, biomass burning, sea salt and mineral dust) from continental and marine sources, with significant differences in terms of physico-chemical and optical properties, water affinity, scale and height of transport, which are not well represented in climate models. The overarching objective of the AErosol, RadiatiOn and CLOuds in southern Africa (AEROCLO-sA) is to improve our knowledge about the role of aerosols on this regional climate with new observations and new climate model exercises. AEROCLO-sA is based on a ground-based and airborne field campaign that was conducted in Namibia between 22 August and 12 September, 2017. Here we present the results of synergetic filter sampling, optical counting, scattering, absorption, extinction and hygroscopicity measurements that were conducted by the ground-based mobile PEGASUS at the coastal Henties Bay experimental site (22°6' S, 14°17' E) to characterize the marine boundary layer aerosols. We illustrate examples of the numerous new particle formation events were observed during the field campaign in link with marine biogenic emissions. We illustrate the chemical composition of the submicron and total aerosols. We discuss the apportionment of maritime sulfate aerosols, and quantify their biogenic fraction, which we link with their cloud condensation nuclei and optical properties. [ABSTRACT FROM AUTHOR]