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The radiative effects of biomass burning aerosols (BBAs) on low-level atmospheric circulation over southern Africa are investigated on 5 September 2017 during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign. This is conducted using a variety of in situ and remote sensing observations, as well as two 5 d ensemble simulations made with the Meso-NH mesoscale model, one including the direct and semi-direct radiative effects of aerosols and one in which these effects are not included. We show that the radiative impact of BBA building up over a period of 5 d in the Meso-NH simulations can lead to significantly different circulations at low and middle levels, thereby affecting dust emissions over southern Namibia and northwestern South Africa as well as the transport of BBA in a so-called "river of smoke". While most of the regional-scale dynamics, thermodynamics and composition features are convincingly represented in the simulation with BBA radiative effects, neglecting the radiative impact of BBA leads to unrealistic representations of (i) the low-level jet (LLJ) over the plateau, which is the main low-level dynamic feature fostering dust emission, and (ii) the mid-level dynamics pertaining to the transport of BBA from the fire-prone regions in the tropics to the mid-latitudes. For instance, when the BBA radiative impacts are not included, the LLJ is too weak and not well established over night, and the developing convective planetary boundary layer (PBL) is too deep compared to observations. The deeper convective PBL over Etosha and surrounding areas is related to the enhanced anomalous upward motion caused by the eastern displacement of the river of smoke. This eastern displacement is, in turn, related to the weaker southerly African easterly jet. Both ensemble simulations provide clear evidence that the enhanced near-surface extinction coefficient values detected from observations over Etosha are related to the downward mixing of BBA in the developing convective boundary layer rather than dust being emitted as a result of the LLJ breakdown after sunrise. This study suggests that the radiative effect of BBAs needs to be taken into account to properly forecast dust emissions in Namibia. [ABSTRACT FROM AUTHOR]

In West Africa, the zonal band of precipitation is generally located around the southern coast in June before migrating northward towards the Sahel in late June/early July. This gives way to a relative dry season for coastal regions from Côte d'Ivoire to Benin called "little dry season", which lasts until September–October. Previous studies have noted that the coastal rainfall cessation in early July seems to coincide with the emergence of an upwelling along the Guinea coast. The aim of this study is to investigate the mechanisms by which this upwelling impacts precipitation, using a set of numerical simulations performed with the Weather Research and Forecasting regional atmospheric model (WRF v 3.7.1). Sensitivity experiments highlight the response of the atmospheric circulation to an intensification or reduction of the strength of the coastal upwelling. They clearly show that the coastal upwelling emergence is responsible for the cessation of coastal precipitation by weakening the northward humidity transport, thus decreasing the coastal convergence of the humidity transport and inhibiting the deep atmospheric convection. In addition, the diurnal cycle of the low-level circulation plays a critical role: the land breeze controls the seaward convergence of diurnal anomaly of humidity transport, explaining the late night–early morning peak observed in coastal precipitation. The emergence of the coastal upwelling strongly attenuates this peak because of a reduced land–sea temperature gradient in the night and a weaker land breeze. The impact on the inland transport of anthropogenic pollution is also shown with numerical simulations of aerosols using the CHIMERE chemistry-transport model: warmer (colder) sea surface temperature (SST) increases (decreases) the inland transport of pollutants, especially during the night, suggesting an influence of the upwelling intensity on the coastal low-level jet. The mechanisms described have important consequences for inland humidity transport and the predictability of the West African monsoon precipitation in summer. [ABSTRACT FROM AUTHOR]

Naturally available, stable, and heavy water molecules such as HDO and H 218 O have a lower saturation vapour pressure than the most abundant light water molecule H 216 O; therefore, these heavy water molecules preferentially condense and rain out during cloud formation. Stable water isotope observations thus have the potential to provide information on cloud processes in the trade-wind region, in particular when combined with high-resolution model simulations. In order to evaluate this potential, nested COSMO iso (isotope-enabled Consortium for Small Scale Modelling;) simulations with explicit convection and horizontal grid spacings of 10, 5, and 1 km were carried out in this study over the tropical Atlantic for the time period of the EUREC 4 A (Elucidating the role of clouds-circulation coupling in climate;) field experiment. The comparison to airborne in situ and remote sensing observations shows that the three simulations are able to distinguish between different mesoscale cloud organisation patterns as well as between periods with comparatively high and low rain rates. Cloud fraction and liquid water content show a better agreement with aircraft observations with higher spatial resolution, because they show strong spatial variations on the scale of a few kilometres. A low-level cold-dry bias, including too depleted vapour in the subcloud and cloud layer and too enriched vapour in the free troposphere, is found in all three simulations. Furthermore, the simulated secondary isotope variable d -excess in vapour is overestimated compared to observations. Special attention is given to the cloud base level, which is the formation altitude of shallow cumulus clouds. The temporal variability of the simulated isotope variables at cloud base agrees reasonably well with observations, with correlations of the flight-to-flight data as high as 0.7 for δ2 H and d -excess. A close examination of isotopic characteristics under precipitating clouds, non-precipitating clouds, clear-sky and dry-warm patches at the altitude of cloud base shows that these different environments are represented faithfully in the model with similar frequencies of occurrence, isotope signals, and specific-humidity anomalies as found in the observations. Furthermore, it is shown that the δ2 H of cloud base vapour at the hourly timescale is mainly controlled by mesoscale transport and not by local microphysical processes, while the d -excess is mainly controlled by large-scale drivers. Overall, this evaluation of COSMO iso , including the isotopic characterisation of different cloud base environments, suggests that the simulations can be used for investigating the role of atmospheric circulations on different scales for controlling the formation of shallow cumulus clouds in the trade-wind region, as will be done in part 2 of this study. [ABSTRACT FROM AUTHOR]

Reflection of solar radiation by tropical low-level clouds has an important cooling effect on climate and leads to decreases in surface temperatures. Still, the effect of pollution on ubiquitous tropical continental low-level clouds and the investigation of the related impact on atmospheric cooling rates are poorly constrained by in situ observations and modeling, in particular during the West African summer monsoon season. Here, we present comprehensive in situ measurements of microphysical properties of low-level clouds over tropical West Africa, measured with the Deutsches Zentrum für Luft- und Raumfahrt (DLR) aircraft Falcon 20 during the DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa) campaign in June and July 2016. Clouds below 1800 m altitude, identified as boundary layer clouds, were classified according to their carbon monoxide (CO) pollution level into pristine and less polluted clouds (CO < 135 ppbv) and polluted low-level clouds (CO > 155 ppbv) as confirmed by the linear CO to accumulation aerosol number concentration correlation. Whereas slightly enhanced aerosol background levels from biomass burning were measured across the entire area, clouds with substantially enhanced aerosol levels were measured in the outflow of major coastal cities, as well as over rural conurbations in the hinterlands. Here we investigate the impact of pollution on cloud droplet number concentration and size during the West African monsoon season. Our results show that the cloud droplet number concentration (CDNC) measured in the size range from 3 to 50 µm around noon increases by 26 % in the elevated aerosol outflow of coastal cities and conurbations with elevated aerosol loadings from median CDNC of 240 cm-3 (52 to 501 cm-3 interquartile range) to 324 cm-3 (60 to 740 cm-3 interquartile range). Higher CDNC resulted in a 17 % decrease in effective cloud droplet diameter from a median deff of 14.8 µm to a deff of 12.4 µm in polluted clouds. Radiative transfer simulations show a non-negligible influence of higher droplet number concentrations and smaller particle sizes on the diurnally averaged (noon) net radiative forcing at the top of atmosphere of - 3.9 Wm-2 (- 16.3 Wm-2) of polluted with respect to less polluted clouds and lead to a change in instantaneous heating rates of - 22.8 Kd-1 (- 17.7 Kd-1) at the top of clouds. Thus, the atmospheric cooling by low-level clouds increases only slightly in the polluted case due to the already elevated background aerosol concentrations. Additionally, the occurrence of mid- and high-level cloud layers atop buffer this effect further, so that the net radiative forcing and instantaneous heating rate of low-level clouds turn out to be less sensitive towards projected future increases in anthropogenic pollution in West Africa. [ABSTRACT FROM AUTHOR]

The direct and semi-direct radiative effects of biomass burning aerosols (BBAs) are investigated over southern Africa and the southeastern Atlantic during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign in September 2017. A reference convection-permitting simulation has been performed using the Meso-NH model with an online dust emission scheme, a strongly absorbing BBA tracer emitted using the daily Global Fire Emissions Database and online-computed backward Lagrangian trajectories. The simulation captures both the aerosol optical depth and the vertical distribution of aerosols as observed from airborne and spaceborne lidars. The occurrence of stratocumulus over the southeastern Atlantic, deep convective clouds over equatorial Africa and the large-scale circulation are all reproduced by the model. If the radiative effects of BBA are omitted in the model, we show that (i) the smoke plume is too low in altitude, (ii) the low-cloud cover is too weak, (iii) the deep convective activity is too frequent but not intense enough, (iv) the Benguela low-level jet is too strong, and (v) the southern African easterly jet is too weak. The Lagrangian analysis indicates that the radiative effect of BBA leads to the transport of BBA to higher altitudes, farther southwest and with a stronger diurnal oscillation. The higher smoke plume altitude can be explained by a combination of three factors: increased upward motion induced by the stronger southern African easterly jet, self-lofting of BBA and reduced subsidence associated with less frequent deep convective activity over western equatorial Africa. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

During the West African summer monsoon, pollutants emitted in urbanized coastal areas modify cloud cover and precipitation patterns. The Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) field campaign provided numerous aircraft-based and ground-based observations, which are used here to evaluate two experiments made with the coupled WRF–CHIMERE model, integrating both the direct and indirect aerosol effect on meteorology. During one well-documented week (1–7 July 2016), the impacts of anthropogenic aerosols on the diurnal cycle of low-level clouds and precipitation are analyzed in detail using high and moderate intensity of anthropogenic emissions in the experiments. Over the continent and close to major anthropogenic emission sources, the breakup time of low-level clouds is delayed by 1 hour, and the daily precipitation rate decreased by 7.5 % with the enhanced anthropogenic emission experiment (with high aerosol load). Despite the small modifications on daily average of low-level cloud cover (+ 2.6 %) with high aerosol load compared to moderate, there is an increase by more than 20 % from 14:00 to 22:00 UTC on hourly average. Moreover, modifications of the modeled low-level cloud and precipitation rate occur far from the major anthropogenic emission sources, to the south over the ocean and to the north up to 11 ∘ N. The present study adds evidence to recent findings that enhanced pollution levels in West Africa may reduce precipitation. [ABSTRACT FROM AUTHOR]

From 23 January to 13 February 2020, 20 ATR-42 scientific flights were conducted in the framework of the EUREC4A field campaign over the tropical Atlantic, off the coast of Barbados (13 ∘ 30 ′ N, - 58 ∘ 30 ′ W). By means of a sideway-pointing lidar, these flights allowed us to retrieve the optical properties of the aerosols found in the sub-cloud layer and below the trade wind inversion. Two distinct periods with significant aerosol contents were identified in relationship with the so-called trade wind and tropical regimes, respectively. For these two regimes, mixings of two air mass types encompassing dust and carbonaceous aerosols have been highlighted. Both were mainly from West Africa with similar optical contributions and linked to dust uptake above Sahara and biomass burning between Guinea-Bissau and Côte d'Ivoire. In the tropical transport regime, the wind within the planetary boundary layer is stronger and favours a contribution of marine aerosols (sulfate and sea salt aerosol components) in shallower aerosol layers than for the trade wind transport regime. The latter is responsible for advecting dust–biomass-burning-aerosol mixtures in the deeper, well-mixed layer, in part due to the complex interactions of the easterly flow from West Africa with mid-latitude dynamics. The aerosol vertical structures appear to be well reproduced using atmospheric composition reanalyses from CAMS when comparing with lidar-derived vertical profiles. The competition between the two types of transport regimes leads to strong heterogeneity in the optical properties of the horizontal aerosol field. Our study highlights the transport regime under which a significant mixture of dust and biomass burning aerosols from West Africa can be observed over the Caribbean and Barbados in particular, namely the trade wind regime. [ABSTRACT FROM AUTHOR]

During austral winter, a compact low cloud deck over the South Atlantic contrasts with clear sky over southern Africa, where forest fires triggered by dry conditions emit large amounts of biomass burning aerosols (BBAs) in the free troposphere. Most of the BBA burden crosses the South Atlantic embedded in the tropical easterly flow. However, midlatitude synoptic disturbances can deflect part of the aerosol from the main transport path towards southern extratropics. In this study, the first objective classification of the synoptic variability controlling the spatial distribution of BBA in southern Africa and the South Atlantic during austral winter (August to October) is presented. By analysing atmospheric circulation data from reanalysis products, a six-class weather regime (WR) classification of the region is constructed. The classification reveals that the synoptic variability is composed of four WRs, representing disturbances travelling at midlatitudes, and two WRs accounting for pressure anomalies in the South Atlantic. The WR classification is then successfully used to characterise the aerosol spatial distribution in the region in the period 2003–2017, in both reanalysis products and station data. Results show that the BBA transport towards southern extratropics is controlled by weather regimes associated with midlatitude synoptic disturbances. In particular, depending on the relative position of the pressure anomalies along the midlatitude westerly flow, the BBA transport is deflected from the main tropical route towards southern Africa or the South Atlantic. Moreover, the WRs accounting for midlatitude disturbances show organised transition sequences, which allow one to illustrate the evolution of the BBA northerly transport across the region in the context of a wave pattern. The skill in characterising the BBA transport shown by the WR classification indicates the potential for using it as a diagnostic/predictive tool for the aerosol dynamics, which is a key component for the full understanding and modelling of the complex radiation–aerosol–cloud interactions controlling the atmospheric radiative budget in the region. [ABSTRACT FROM AUTHOR]

In order to gain understanding on the vertical structure of atmospheric water vapour above mountain lakes and to assess its link with the isotopic composition of the lake water and with small-scale dynamics (i.e. valley winds, thermal convection above complex terrain), the L-WAIVE (Lacustrine-Water vApor Isotope inVentory Experiment) field campaign was conducted in the Annecy valley in the French Alps during 10 d in June 2019. This field campaign was based on an original experimental synergy between a suite of ground-based, boat-borne, and two ultra-light aircraft (ULA) measuring platforms implemented to characterize the thermodynamic and isotopic composition above and in the lake. A cavity ring-down spectrometer and an in-cloud liquid water collector were deployed aboard one of the ULA to characterize the vertical distribution of the main stable water isotopes (H 216 O, H 218 O and H 2 H 16 O) both in the air and in shallow cumulus clouds. The temporal evolution of the meteorological structures of the low troposphere was derived from an airborne Rayleigh–Mie lidar (embarked on a second ULA), a ground-based Raman lidar, and a wind lidar. ULA flight patterns were repeated several times per day to capture the diurnal evolution as well as the variability associated with the different weather events encountered during the field campaign, which influenced the humidity field, cloud conditions, and slope wind regimes in the valley. In parallel, throughout the campaign, liquid water samples of rain, at the air–lake water interface, and at 2 m depth in the lake were taken. A significant variability of the isotopic composition was observed along time, depending on weather conditions, linked to the transition from the valley boundary layer towards the free troposphere, the valley wind intensity, and the vertical thermal stability. Thus, significant gradients of isotopic content have been revealed at the transition to the free troposphere, at altitudes between 2.5 and 3.5 km. The influence of the lake on the atmosphere isotopic composition is difficult to isolate from other contributions, especially in the presence of thermal instabilities and valley winds. Nevertheless, such an effect appears to be detectable in a layer of about 300 m thickness above the lake in light wind conditions. We also noted similar isotopic compositions in cloud drops and rainwater. [ABSTRACT FROM AUTHOR]

We analyse the airborne measurements of above-cloud aerosols from the AErosol, RadiatiOn, and CLOuds in southern Africa (AEROCLO-sA) field campaign performed in Namibia during August and September 2017. The study aims to retrieve the aerosol above-cloud direct radiative effect (DRE) with well-defined uncertainties. To improve the retrieval of the aerosol and cloud properties, the airborne demonstrator of the Multi-Viewing, Multi-Channel, Multi-Polarization (3MI) satellite instrument, called the Observing System Including PolaRisation in the Solar Infrared Spectrum (OSIRIS), was deployed on-board the SAFIRE (Service des Avions Français Instrumentés pour la Rechercheen Environnement) Falcon 20 aircraft during 10 flights performed over land, over the ocean, and along the Namibian coast. The airborne instrument OSIRIS provides observations at high temporal and spatial resolutions for aerosol above clouds (AACs) and cloud properties. OSIRIS was supplemented with the Photomètre Léger Aéroporté pour la surveillance des Masses d'Air version 2 (PLASMA2). The combined airborne measurements allow, for the first time, the validation of AAC algorithms previously developed for satellite measurements. The variations in the aerosol properties are consistent with the different atmospheric circulation regimes observed during the deployment. Airborne observations typically show strong aerosol optical depth (AOD; up to 1.2 at 550 nm) of fine-mode particles from biomass burning (extinction Ångström exponent varying between 1.6 and 2.2), transported above bright stratocumulus decks (mean cloud top around 1 km above mean sea level), with cloud optical thickness (COT) up to 35 at 550 nm. The above-cloud visible AOD retrieved with OSIRIS agrees within 10 % of the PLASMA2 sun photometer measurements in the same environment. The single scattering albedo (SSA) is one of the most influential parameters on the AAC DRE calculation that remains largely uncertain in models. During the AEROCLO-sA campaign, the average SSA obtained by OSIRIS at 550 nm is 0.87, which is in agreement within 3 %, on average, with previous polarimetric-based satellite and airborne retrievals. The strong absorption of the biomass burning plumes in the visible range is generally consistent with the observations from the Aerosol Robotic Network (AERONET) ground-based sun photometers. This, however, shows a significant increase in the particles' absorption at 440 nm in northern Namibia and Angola, which indicates more absorbing organic species within the observed smoke plumes. Biomass burning aerosols are also vertically collocated, with significant amounts of water content up to the top of the plume at around 6 km height in our measurements. The detailed characterization of aerosol and cloud properties, water vapour, and their uncertainties obtained from OSIRIS and PLASMA2 measurements allows us to study their impacts on the AAC DRE. The high-absorbing load of AAC, combined with high cloud albedo, leads to unprecedented DRE estimates, which are higher than previous satellite-based estimates. The average AAC DRE calculated from the airborne measurements in the visible range is +85 Wm-2 (standard deviation of 26 Wm-2), with instantaneous values up to +190 W m -2 during intense events. These high DRE values, associated with their uncertainties, have to be considered as new upper cases in order to evaluate the ability of models to reproduce the radiative impact of the aerosols over the southeastern Atlantic region. [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]

The evolution of the vertical distribution and optical properties of aerosols in the free troposphere, above stratocumulus, is characterized for the first time over the Namibian coast, a region where uncertainties on aerosol–cloud coupling in climate simulations are significant. We show the high variability of atmospheric aerosol composition in the lower and middle troposphere during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign (22 August–12 September 2017) around the Henties Bay supersite using a combination of ground-based, airborne and space-borne lidar measurements. Three distinct periods of 4 to 7 d are observed, associated with increasing aerosol loads (aerosol optical thickness at 550 nm ranging from ∼0.2 to ∼0.7), as well as increasing lofted aerosol layer depth and top altitude. Aerosols are observed up to 6 km above mean sea level during the later period. Aerosols transported within the free troposphere are mainly polluted dust (predominantly dust mixed with smoke from fires) for the first two periods (22 August–1 September 2017) and smoke for the last part (3–9 September) of the field campaign. As shown by Lagrangian back-trajectory analyses, the main contribution to the aerosol optical thickness over Henties Bay is shown to be due to biomass burning over Angola. Nevertheless, in early September, the highest aerosol layers (between 5 and 6 km above mean sea level) seem to come from South America (southern Brazil, Argentina and Uruguay) and reach Henties Bay after 3 to 6 d. Aerosols appear to be transported eastward by the midlatitude westerlies and towards southern Africa by the equatorward moving cut-off low originating from within the westerlies. All the observations show a very complex mixture of aerosols over the coastal regions of Namibia that must be taken into account when investigating aerosol radiative effects above stratocumulus clouds in the southeast Atlantic Ocean. [ABSTRACT FROM AUTHOR]

The aerosol direct and indirect effects are studied over west Africa in the summer of 2016 using the coupled WRF-CHIMERE regional model including aerosol–cloud interaction parameterization. First, a reference simulation is performed and compared with observations acquired during the Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) field campaign which took place in June and July 2016. Sensitivity experiments are also designed to gain insights into the impact of the aerosols dominating the atmospheric composition in southern west Africa (one simulation with halved anthropogenic emissions and one with halved mineral dust emissions). The most important effect of aerosol–cloud interactions is found for the mineral dust scenario, and it is shown that halving the emissions of mineral dust decreases the 2 m temperature by 0.5 K and the boundary layer height by 25 m on a monthly average (July 2016) and over the Saharan region. The presence of dust aerosols also increases (decreases) the shortwave (longwave) radiation at the surface by 25 W m -2. It is also shown that the decrease of anthropogenic emissions along the coast has an impact on the mineral dust load over west Africa by increasing their emissions in the Saharan region. It is due to a mechanism where particulate matter concentrations are decreased along the coast, imposing a latitudinal shift of the monsoonal precipitation and, in turn, an increase of the surface wind speed over arid areas, inducing more mineral dust emissions. [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 dynamical context and moisture transport pathways embedded in large-scale flow and associated with a heavy precipitation event (HPE) in southern Italy (SI) are investigated with the help of stable water isotopes (SWIs) based on a purely numerical framework. The event occurred during the Intensive Observation Period (IOP) 13 of the field campaign of the Hydrological Cycle in the Mediterranean Experiment (HyMeX) on 15 and 16 October 2012, and SI experienced intense rainfall of 62.4 mm over 27 h with two precipitation phases during this event. The first one (P1) was induced by convective precipitation ahead of a cold front, while the second one (P2) was mainly associated with precipitation induced by large-scale uplift. The moisture transport and processes responsible for the HPE are analysed using a simulation with the isotope-enabled regional numerical model COSMO iso. The simulation at a horizontal grid spacing of about 7 km over a large domain (about 4300 km ×3500 km) allows the isotopes signal to be distinguished due to local processes or large-scale advection. Backward trajectory analyses based on this simulation show that the air parcels arriving in SI during P1 originate from the North Atlantic and descend within an upper-level trough over the north-western Mediterranean. The descending air parcels reach elevations below 1 km over the sea and bring dry and isotopically depleted air (median δ18O ≤-25 ‰, water vapour mixing ratio q≤2 g kg -1) close to the surface, which induces strong surface evaporation. These air parcels are rapidly enriched in SWIs (δ18O ≥-14 ‰) and moistened (q≥8 g kg -1) over the Tyrrhenian Sea by taking up moisture from surface evaporation and potentially from evaporation of frontal precipitation. Thereafter, the SWI-enriched low-level air masses arriving upstream of SI are convectively pumped to higher altitudes, and the SWI-depleted moisture from higher levels is transported towards the surface within the downdrafts ahead of the cold front over SI, producing a large amount of convective precipitation in SI. Most of the moisture processes (i.e. evaporation, convective mixing) related to the HPE take place during the 18 h before P1 over SI. A period of 4 h later, during the second precipitation phase P2, the air parcels arriving over SI mainly originate from north Africa. The strong cyclonic flow around the eastward-moving upper-level trough induces the advection of a SWI-enriched African moisture plume towards SI and leads to large-scale uplift of the warm air mass along the cold front. This lifts moist and SWI-enriched air (median δ18O ≥-16 ‰, median q≥6 g kg -1) and leads to gradual rain out of the air parcels over Italy. Large-scale ascent in the warm sector ahead of the cold front takes place during the 72 h preceding P2 in SI. This work demonstrates how stable water isotopes can yield additional insights into the variety of thermodynamic mechanisms occurring at the mesoscale and synoptic scale during the formation of a HPE. [ABSTRACT FROM AUTHOR]

During the monsoon season, pollutants emitted by large coastal cities and biomass burning plumes originating from central Africa have complex transport pathways over southern West Africa (SWA). The Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa (DACCIWA) field campaign has provided numerous dynamical and chemical measurements in and around the super-site of Savè in Benin (≈185 km away from the coast), which allows quantification of the relative contribution of advected pollutants. Through the combination of in situ ground measurements with aircraft, radio-sounding, satellite, and high-resolution chemistry-transport modeling with the CHIMERE model, the source attribution and transport pathways of pollutants inland (here, NOx and CO) are carefully analyzed for the 1–7 July 2016 period. The relative contributions of different sources (i.e., emissions from several large coastal cities) to the air quality in Savè are characterized. It is shown that a systematic diurnal cycle exists with high surface concentrations of pollutants from 18:00 to 22:00 UTC. This evening peak is attributed to pollution transport from the coastal city of Cotonou (Benin). Numerical model experiments indicate that the anthropogenic pollutants are accumulated during the day close to the coast and transported northward as soon as the daytime convection in the atmospheric boundary layer ceases after 16:00 UTC, reaching 8 ∘ N at 21:00 UTC. When significant biomass burning pollutants are transported into continental SWA, they are mixed with anthropogenic pollutants along the coast during the day, and this mixture is then transported northward. At night, most of the coastal anthropogenic plumes are transported within the planetary boundary layer (below about 500 m above ground level), whereas the biomass burning pollutants are mostly transported above it, thus generally not impacting ground level air quality. [ABSTRACT FROM AUTHOR]

The present study examines the impact of the environmental moisture structure in the lower troposphere (below 2 km above sea level, a.s.l.) on the precipitation development, observed in southern France during Intensive Observation Period (IOP) 13 of the first Special Observation Period of the Hydrological cycle in the Mediterranean Experiment (HyMeX SOP-1), through a series of sensitivity experiments using the non-hydrostatic mesoscale atmospheric numerical model (Meso-NH). The control simulation (CNTL) and all the other 12 sensitivity experiments examined in this study succeed in reproducing a heavy precipitation event (HPE) in the coastal mountainous region of Var in south-eastern France as observed. The sensitivity experiments are designed to investigate the response of the HPE to the variability of the water vapour content upstream in the moist marine atmospheric boundary layer (MABL) and the drier air above. The comparisons between CNTL and the 12 sensitivity experiments show how the life cycle of precipitation associated with the HPE, but also the upstream flow (over the sea), is modified, even for moisture content changes of only 1 g kg -1 below 2 km a.s.l. Within the low-level wind convergence between southerlies and south-westerlies, a small increase of moisture content in the MABL prolongs moderate precipitation (≥5 mm in 15 min) and enlarges the area of weak precipitation (≥1 mm in 15 min). The moistening in the 1–2 km a.s.l. layer, just above the MABL, prolongs the duration of moderate precipitation, for a similar total precipitation amount as in CNTL. The drier MABL and 1–2 km a.s.l. layer shorten the lifetime of precipitation and reduce the total precipitation amount with respect to CNTL. We also found that the moisture in the MABL has a stronger impact on producing enhanced precipitation (both in terms of amount and intensity) than the moisture just above (1–2 km a.s.l.). Also, it is worth noting that adding moisture in the MABL does not necessarily lead to enhanced precipitation amount. In moistening the MABL, the duration of moderate precipitation increases with increasing moisture as does the area covered by weak precipitation, while the area covered by the intense precipitation (≥30 mm) decreases. Despite a simplified moisture-profile modification approach, this study suggests that moisture structure in the lower troposphere is key for accurate prediction at short-term range of the timing and location of precipitation in the coastal mountainous region in southern France. [ABSTRACT FROM AUTHOR]

The complex vertical distribution of aerosols over coastal southernWest Africa (SWA) is investigated using airborne observations and numerical simulations. Observations were gathered on 2 July 2016 offshore of Ghana and Togo, during the field phase of the Dynamics-Aerosol-Chemistry- Cloud Interactions in West Africa project. This was the only flight conducted over the ocean during which a downwardlooking lidar was operational. The aerosol loading in the lower troposphere includes emissions from coastal cities (Accra, Lomé, Cotonou, and Lagos) as well as biomass burning aerosol and dust associated with long-range transport from central Africa and the Sahara, respectively. Our results indicate that the aerosol distribution on this day is impacted by subsidence associated with zonal and meridional regionalscale overturning circulations associated with the land-sea surface temperature contrast and orography over Ghana and Togo, as typically observed on hot, cloud-free summer days such as 2 July 2016. Furthermore, we show that the zonal circulation evidenced on 2 July is a persistent feature over the Gulf of Guinea during July 2016. Numerical tracer release experiments highlight the dominance of aged emissions from Accra on the observed pollution plume loadings over the ocean, in the area of aircraft operation. The contribution of aged emission from Lomé and Cotonou is also evident above the marine boundary layer. Given the general direction of the monsoon flow, the tracer experiments indicate no contribution from Lagos emissions to the atmospheric composition of the area west of Cotonou, where our airborne observations were gathered. The tracer plume does not extend very far south over the ocean (i.e. less than 100 km from Accra), mostly because emissions are transported northeastward near the surface over land and westward above the marine atmospheric boundary layer. The latter is possible due to interactions between the monsoon flow, complex terrain, and land-sea breeze systems, which support the vertical mixing of the urban pollution. This work sheds light on the complex - and to date undocumented - mechanisms by which coastal shallow circulations can distribute atmospheric pollutants over the densely populated SWA region. [ABSTRACT FROM AUTHOR]

In the framework of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, the tropospheric chemical composition in large cities along the Gulf of Guinea is studied using the Weather and Research Forecast and CHIMERE regional models. Simulations are performed for the May-July 2014 period, without and with biomass burning emissions. Model results are compared to satellite data and surface measurements. Using numerical tracer release experiments, it is shown that the biomass burning emissions in Central Africa are impacting the surface aerosol and gaseous species concentrations in Gulf of Guinea cities such as Lagos (Nigeria) and Abidjan (Ivory Coast). Depending on the altitude of the injection of these emissions, the pollutants follow different pathways: directly along the coast or over land towards the Sahel before being vertically mixed in the convective boundary layer and transported to the south-west and over the cities. In July 2014, the maximum increase in surface concentrations due to fires in Central Africa is ≈ 150 µg m-3 for CO, ≈ 10 to 20 µg m-3 for O3 and ≈ 5 µg m-3 for PM10. The analysis of the PM-3 chemical composition shows that this increase is mainly related to an increase in particulate primary and organic matter. [ABSTRACT FROM AUTHOR]

As part of the Dynamics-Aerosol-Chemistry- Cloud Interactions in West Africa (DACCIWA) project, an airborne campaign was designed to measure a large range of atmospheric constituents, focusing on the effect of anthropogenic emissions on regional climate. The presented study details results of the French ATR42 research aircraft, which aimed to characterize gas-phase, aerosol and cloud properties in the region during the field campaign carried out in June/July 2016 in combination with the German Falcon 20 and the British Twin Otter aircraft. The aircraft flight paths covered large areas of Benin, Togo, Ghana and Côte d'Ivoire, focusing on emissions from large urban conurbations such as Abidjan, Accra and Lomé, as well as remote continental areas and the Gulf of Guinea. This paper focuses on aerosol particle measurements within the boundary layer .< 2000 m), in particular their sources and chemical composition in view of the complex mix of both biogenic and anthropogenic emissions, based on measurements from a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) and ancillary instrumentation. Background concentrations (i.e. outside urban plumes) observed from the ATR42 indicate a fairly polluted region during the time of the campaign, with average concentrations of carbon monoxide of 131 ppb, ozone of 32 ppb, and aerosol particle number concentration (>15 nm) of 735 cm-3 stp. Regarding submicron aerosol composition (considering nonrefractory species and black carbon, BC), organic aerosol (OA) is the most abundant species contributing 53 %, followed by SO4 (27 %), NH4 (11 %), BC (6 %), NO3 (2 %) and minor contribution of Cl (<0.5 %). Average background PM1 in the region was 5.9 μgm-3 stp. During measurements of urban pollution plumes, mainly focusing on the outflow of Abidjan, Accra and Lomé, pollutants are significantly enhanced (e.g. average concentration of CO of 176 ppb, and aerosol particle number concentration of 6500 cm-3 stp), as well as PM1 concentration (11.9 μgm-3 stp). Two classes of organic aerosols were estimated based on C-ToF-AMS: particulate organic nitrates (pONs) and isoprene epoxydiols secondary organic aerosols (IEPOX-SOA). Both classes are usually associated with the formation of particulate matter through complex interactions of anthro-pogenic and biogenic sources. During DACCIWA, pONs have a fairly small contribution to OA (around 5 %) and are more associated with long-range transport from central Africa than local formation. Conversely, IEPOX-SOA provides a significant contribution to OA (around 24 and 28% under background and in-plume conditions). Furthermore, the fractional contribution of IEPOX-SOA is largely unaffected by changes in the aerosol composition (particularly the SO4 concentration), which suggests that IEPOX-SOA concentration is mainly driven by pre-existing aerosol surface, instead of aerosol chemical properties. At times of large in-plume SO4 enhancements (above 5 μgm-3/, the fractional contribution of IEPOX-SOA to OA increases above 50 %, suggesting only then a change in the IEPOX-SOAcontrolling mechanism. It is important to note that IEPOX- SOA constitutes a lower limit to the contribution of biogenic OA, given that other processes (e.g. non-IEPOX isoprene, monoterpene SOA) are likely in the region. Given the significant contribution to aerosol concentration, it is crucial that such complex biogenic-anthropogenic interactions are taken into account in both present-day and future scenario models of this fast-changing, highly sensitive region. [ABSTRACT FROM AUTHOR]

Carbon monoxide, CO, and fine atmospheric particulate matter, PM2:5, are analyzed over the Guinean Gulf coastal region using the WRF-CHIMERE modeling system and observations during the beginning of the monsoon 2006 (from May to July), corresponding to the Africa Multidisciplinary Monsoon Analysis (AMMA) campaign period. Along the Guinean Gulf coast, the contribution of longrange pollution transport to CO or PM2:5 concentrations is important. The contribution of desert dust PM2:5 concentration decreases from ↑38% in May to ~5% in July. The contribution of biomass burning PM2:5 concentration from Central Africa increases from ~10% in May to ~52% in July. The anthropogenic contribution is ~30% for CO and ~10% for PM2:5 during the whole period. When focusing only on anthropogenic pollution, frequent northward transport events from the coast to the Sahel are associated with periods of low wind and no precipitation. In June, anthropogenic PM2:5 and CO concentrations are higher than in May or July over the Guinean coastal region. Air mass dynamics concentrate pollutants emitted in the Sahel due to a meridional atmospheric cell. Moreover, a part of the pollution emitted remotely at the coast is transported and accumulated over the Sahel. Focusing the analysis on the period 8-15 June, anthropogenic pollutants emitted along the coastline are exported toward the north especially at the beginning of the night (18:00 to 00:00 UTC) with the establishment of the nocturnal low level jet. Plumes originating from different cities are mixed for some hours at the coast, leading to high pollution concentration, because of specific disturbed meteorological conditions. [ABSTRACT FROM AUTHOR]

The isotopic composition of water vapour in the North Atlantic free troposphere is investigated with Infrared Atmospheric Sounding Interferometer (IASI) measurements of the D=H ratio (δD) above the ocean. We show that in the vicinity of West Africa, the seasonality of δD is particularly strong (130‰), which is related with the influence of the Saharan heat low (SHL) during summertime. The SHL indeed largely influences the dynamic in that region by producing deep turbulent mixing layers, yielding a specific water vapour isotopic footprint. The influence of the SHL on the isotopic budget is analysed on various time and space scales and is shown to be large, highlighting the importance of the SHL dynamics on the moistening and the HDO enrichment of the free troposphere over the North Atlantic. The potential influence of the SHL is also investigated on the inter-annual scale as we also report important variations in δD above the Canary archipelago region. We interpret the variability in the enrichment, using backward trajectory analyses, in terms of the ratio of air masses coming from the North Atlantic and air masses coming from the African continent. Finally, the interest of IASI high sampling capabilities is further illustrated by presenting spatial distributions of δD and humidity above the North Atlantic from which we show that the different sources and dehydration pathways controlling the humidity can be disentangled thanks to the added value of δD observations. More generally, our results demonstrate the utility of δD observations obtained from the IASI sounder to gain insight into the hydrological cycle processes in the West African region. [ABSTRACT FROM AUTHOR]

In the framework of the Fennec international programme, a field campaign was conducted in June 2011 over the western Sahara. It led to the first observational data set ever obtained that documents the dynamics, thermodynamics and composition of the Saharan atmospheric boundary layer (SABL) under the influence of the heat low. In support to the aircraft operation, four dust forecasts were run daily at low and high resolutions with convection-parameterizing and convection-permitting models, respectively. The unique airborne and ground-based data sets allowed the first ever intercomparison of dust forecasts over the western Sahara. At monthly scale, large aerosol optical depths (AODs) were forecast over the Sahara, a feature observed by satellite retrievals but with different magnitudes. The AOD intensity was correctly predicted by the high-resolution models, while it was underestimated by the low-resolution models. This was partly because of the generation of strong near-surface wind associated with thunderstorm-related density currents that could only be reproduced by models representing convection explicitly. Such models yield emissions mainly in the afternoon that dominate the total emission over the western fringes of the Adrar des Iforas and the Aïr Mountains in the high-resolution forecasts. Over the western Sahara, where the harmattan contributes up to 80% of dust emission, all the models were successful in forecasting the deep wellmixed SABL. Some of them, however, missed the large nearsurface dust concentration generated by density currents and low-level winds. This feature, observed repeatedly by the airborne lidar, was partly forecast by one high-resolution model only. [ABSTRACT FROM AUTHOR]