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The ADRIMED campaign provides measurements of all key parameters regarding atmospheric composition in the Mediterranean area during the summer 2013. This is an opportunity to quantify the ability of current models to adequately represent the atmospheric composition in this complex region, which is influenced by anthropogenic emissions from Europe, Africa, the Middle-East and from shipping activities as well as mineral dust emissions mostly from the arid areas in Africa, sea-salt emissions, biomass burning emissions and biogenic emissions from the vegetation. The CHIMERE model in its present version is a chemistry-transport model which takes into account all these processes. We show here by simulating the period from 5 June to 15 July 2013 with the CHIMERE model and comparing the results to both routine and specific ADRIMED measurements that this model allows an adequate representation the atmospheric composition over the western Mediterranean, in terms of ozone concentration, particulate matter (PM) and aerosol optical depth (AOD). It is also shown that the concentrations of PM on all the considered area is dominated by mineral dust, even though local dust emissions in Europe are certainly overestimated by the model. A comparison with sulphate concentrations at Cape Corsica exhibits some discrepancies related to the regridding of shipping emissions.

Aerosols have important effects on both local and global climate, as well as on clouds and precipitations. We present here some original results of the AErosol RadiatiOn and CLOud in Southern Africa (AEROCLO-sA) field campaign led in Namibia in August and September 2017. This region shows a strong response to climate change and is associated with large uncertainties in climate models. Large amounts of biomass burning aerosols emitted by vegetation fires in Central Africa are transported far over the Namibian deserts and are also detected over the stratocumulus clouds covering the South Atlantic Ocean along the coast of Namibia. Absorbing aerosols above clouds are associated with strong positive direct radiative forcing (warming) that are still underestimated in climate models (De Graaf etal.,2021). The absorption of solar radiation by absorbing above clouds may also cause a warming where the aerosol layer is located. This warming would alter the thermodynamic properties of the atmosphere, which would impact the vertical development of low-level clouds impacting the cloud top height and its brightness. The airborne field campaign consisted in ten flights performed with the French F-20 Falcon aircraft in this region of interest. Several instruments were involved: the OSIRIS polarimeter, prototype of the next 3MI spaceborne instrument of ESA (Chauvigné etal.,2021), the LNG lidar, an airborne photometer called PLASMA, as well as fluxmeters and dropsondes used to measure thermodynamical quantities, supplemented with in situ aerosol measurements of particles size distribution.In order to quantify the aerosols radiative impact on the Namibian regional radiative budget, we use an original approach that combines polarimeter and lidar data to derive heating rate of the aerosols. This approach is evaluated during massive transports of biomass burning particles. To calculate this parameter, we use a radiative transfer code and additional meteorological parameters, provided by the dropsondes. We will introduce, the flight of September 8, 2017, aerosol pollution was very important. Emissions and dust were carried along the Namibian coast, and an aerosol plume was observed above a stratocumulus. We will present vertical profiles of heating rates computed in the solar and thermal parts of the spectrum with this technique. Our results indicated particularly strong heating rate values retrieved above clouds due to aerosols, in the order of 8K per day, which is likely to perturbate the dynamic of the below cloud layers.In order to validate and to quantify this new methodology, we used the flux measurements acquired during loop descents performed during dedicated parts of the flights, which provides unique measurements of flux distribution (upwelling and downwelling) and heating rates in function of the altitude.Finally, we will discuss the possibility to apply this method to available spaceborne passive and active observations in order to provide the first estimates of heating rate profiles above clouds at global scale.

The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

International audience; Aerosols interact with clouds through radiative and microphysical mechanisms in addition to their direct radiative effects of scattering and absorbing of solar and thermal radiation. Aerosol indirect effects consist of the modification of cloud droplet number concentrations, cloud albedo, and ice nucleating particle concentrations with ensuing effects on precipitation through aerosol perturbations. Different aerosol types present over the basin, notably dust, sea-salt and anthropogenic contribute to the formation of cloud condensation and ice nucleating particles, thus modifying cloud parameters. These processes notably occur during the frequent dust outbreaks over the Mediterranean Sea. Besides, the semi-direct aerosol effect, namely changes in cloud cover and atmospheric dynamics due to aerosol absorption, is another impact on regional climate. Regional climate simulations including aerosol-cloud interactions highlight the importance of considering aerosols, even if uncertainties are still important notably with regards to effects on cloud microphysics. To date, the direct and semi-direct effects seem to have larger impacts on the average radiative budget over the Mediterranean than the cloud-albedo indirect effect, but the question remains open concerning other indirect effects. Therefore, more observations of these interactions coupled with numerical simulations considering all these processes are needed to reduce uncertainties.

The southeast Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activity that occurs in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AOD) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25°S–0° and 15°W–15°E (excluding land) among the ESMs. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2 and their similarities in the mean AODs are the result of cancellation of high and low AOD biases. GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL compared to aircraft-based observations. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

The impacts of poor air quality on human health are becoming more apparent. Businesses and governments are implementing technologies and policies in order to improve air quality. Despite this the PM10 air quality in the mining town of Moranbah, Australia, has worsened since measurements commenced in 2011. The annual average PM10 concentrations during 2012, 2017, 2018 and 2019 have all exceeded the Australian National Environmental Protection Measure's standard, and there has been an increase in the frequency of exceedances of the daily standard. The average annual increase in PM10 was 1.2 ± 0.5 μg m − 3 per year between 2011 and 2019 and has been 2.5 ± 1.2 μg m − 3 per year since 2014. The cause of this has not previously been established. Here, two machine learning algorithms (gradient boosted regression and random forest) have been implemented to model and then meteorologically normalise PM10 mass concentrations measured in Moranbah. The best performing model, using the random forest algorithm, was able to explain 59% of the variance in PM10 using a range of meteorological, environmental and temporal variables as predictors. An increasing trend after normalising for these factors was found of 0.6 ± 0.5 μg m − 3 per year since 2011 and 1.7 ± 0.3 μg m − 3 per year since 2014. These results indicate that more than half of the increase in PM10 is due to a rise in local emissions in the region. The remainder of the rise in PM10 was found to be due to a decrease of soil water content in the surrounding region, which can facilitate higher dust emissions. Whether the presence of open-cut coal mines exacerbated the role of soil water content is unclear. Although fires can have drastic effects on the local air quality, changes in fire patterns are not responsible for the rising trend. PM10 composition measurements or more detailed data relating to local sources is still needed to better isolate these emissions. Nonetheless, this study highlights the need and potential for action by industry and government to improve the air quality and reduce health risks for the nearby population.

Organic aerosols are predominantly emitted from biomass burning and biofuel use. The fraction of these aerosols that strongly absorbs ultraviolet and short visible light is referred to as brown carbon (BrC). The life cycle and the optical properties of BrC are still highly uncertain, thus contributing to the uncertainty of the total aerosol radiative effect. This study presents the implementation of BrC aerosols in the Tropospheric Aerosols for ClimaTe In CNRM (TACTIC) aerosol scheme of the atmospheric component of the Centre National de Recherches Météorologiques (CNRM) climate model. This implementation has been achieved using a BrC parameterization based on the optical properties of Saleh et al. (2014). Several simulations have been carried out with the CNRM global climate model, over the period of 2000–2014, to analyze the BrC radiative and climatic effects. Model evaluation has been carried out by comparing numerical results of single-scattering albedo (SSA), aerosol optical depth (AOD), and absorption aerosol optical depth (AAOD) to data provided by Aerosol Robotic Network (AERONET) stations, at the local scale, and by different satellite products, at the global scale. The implementation of BrC and its bleaching parameterization has resulted in an improvement of the estimation of the total SSA and AAOD at 350 and 440 nm. This improvement is observed at both the local scale, for several locations of AERONET stations, and the regional scale, over regions of Africa (AFR) and South America (AME), where large quantities of biomass burning aerosols are emitted. The annual global BrC effective radiative forcing (all-sky conditions) has been calculated in terms of both aerosol–radiation interactions (ERFari, 0.029 ± 0.006 W m−2) and aerosol–cloud interactions (ERFaci, −0.024 ± 0.066 W m−2). This study shows, on an annual average, positive values of ERFari of 0.292 ± 0.034 and 0.085 ± 0.032 W m−2 over the AFR and AME regions, respectively, which is in accordance with the BrC radiative effect calculated in previous studies. This work also reveals that the inclusion of BrC in the TACTIC aerosol scheme causes a statistically significant low-level cloud fraction increase over the southeastern Atlantic Ocean during the burning season partially caused by a vertical velocity decrease at 700 hPa (semi-direct aerosol effect). Lastly, this study also highlights that the low-level cloud fraction changes, associated with more absorbing biomass burning aerosols, contribute to an increase in both solar heating rate and air temperature at 700 hPa over this region.

The present work aims at better understanding regional climate–aerosol interactions by studying the relationships between aerosols and synoptic atmospheric circulation over the Euro-Mediterranean region. Two 40-year simulations (1979–2018) have been carried out with version 6.3 of the Centre National de Recherches Météorologiques (National Centre for Meteorological Research) – Aire Limitée Adaptation dynamique Développement InterNational (CNRM-ALADIN) regional climate model, one using interactive aerosols and the other one without any aerosol. The simulation with aerosols has been evaluated in terms of different climate and aerosol parameters. This evaluation shows a good agreement between the model and observations, significant improvements compared to the previous model version and consequently the relevance of using this model for the study of climate–aerosol interactions over this region. A first attempt to explain the climate variability of aerosols is based on the use of the North Atlantic Oscillation (NAO) index. The latter explains a significant part of the interannual variability, notably in winter for the export of dust aerosols over the Atlantic Ocean and the eastern Mediterranean, and in summer for the positive anomalies of anthropogenic aerosols over western Europe. This index is however not sufficient to fully understand the variations of aerosols in this region, notably at daily scale. The use of “weather regimes”, namely persisting meteorological patterns, stable at synoptic scale for a few days, provides a relevant description of atmospheric circulation, which drives the emission, transport and deposition of aerosols. The four weather regimes usually defined in this area in winter and in summer bring significant information to answer this question. The blocking and NAO+ regimes are largely favourable to strong aerosol effects on shortwave surface radiation and near-surface temperature, either because of higher aerosol loads or because of weaker cloud fraction, which reinforces the direct aerosol effect. Inversely, the NAO− and Atlantic Ridge regimes are unfavourable to aerosol radiative effects, because of weaker aerosol concentrations and increased cloud cover. This study thus puts forward the strong dependence of aerosol loads on the synoptic circulation from interannual to daily scales and, as a consequence, the important modulation of the aerosol effects on shortwave surface radiation and near-surface temperature by atmospheric circulation. The role of cloud cover is essential in this modulation as shown by the use of weather regimes.

Description, Underestimates of smoke absorption by climate models limits their ability to reproduce positive forcing and low-cloud feedback., The radiative budget, cloud properties, and precipitation over tropical Africa are influenced by solar absorption by biomass-burning aerosols (BBA) from Central Africa. Recent field campaigns, reinforced by new remote-sensing and aerosol climatology datasets, have highlighted the absorbing nature of the elevated BBA layers over the South-East Atlantic (SEA), indicating that the absorption could be stronger than previously thought. We show that most of the latest generation of general circulation models (GCMs) from the sixth phase of the Coupled Model Intercomparison Project 6 (CMIP6) underestimates the absorption of BBA over the SEA. This underlines why many (~75%) CMIP6 models do not fully capture the intense positive (warming) direct radiative forcing at the top of the atmosphere observed over this region. In addition, underestimating the magnitude of the BBA-induced solar heating could lead to misrepresentations of the low-level cloud responses and fast precipitation feedbacks that are induced by BBA in tropical regions.

Aerosol heating due to shortwave absorption has implications for local atmospheric stability and regional dynamics. The derivation of heating rate profiles from space-based observations is challenging because it requires the vertical profile of relevant properties such as the aerosol extinction coefficient and single scattering albedo (SSA). In the southeast Atlantic, this challenge is amplified by the presence of stratocumulus clouds below the biomass burning plume advected from Africa, since the cloud properties affect the magnitude of the aerosol heating aloft, which may in turn lead to changes in the cloud properties and life cycle. The combination of spaceborne lidar data with passive imagers shows promise for future derivations of heating rate profiles and curtains, but new algorithms require careful testing with data from aircraft experiments where measurements of radiation, aerosol and cloud parameters are better collocated and readily available. In this study, we derive heating rate profiles and curtains from aircraft measurements during the NASA ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES) project in the southeastern Atlantic. Spectrally resolved irradiance measurements and the derived column absorption allow for the separation of total heating rates into aerosol and gas (primarily water vapor) absorption. The nine cases we analyzed capture some of the co-variability of heating rate profiles and their primary drivers, leading to the development of a new concept: The Heating Rate Efficiency (HRE; the heating rate per unit aerosol extinction). The HRE, which accounts for the overall aerosol loading as well as vertical distribution of the aerosol layer, varies little with altitude as opposed to the standard heating rate. The large case-to-case variability for ORACLES is significantly reduced after converting from heating rate to HRE, allowing us to quantify its dependence on SSA, cloud albedo, and solar zenith angle.

Biomass burning smoke is advected over the southeast Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly, in both magnitude and sign. The NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project deployed for field campaigns off the west coast of Africa in three consecutive years (Sept., 2016; Aug., 2017; and Oct., 2018) with the goal of better characterizing this plume as a function of the monthly evolution, by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect, and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models the simulated plume is too vertically diffuse, has smaller vertical gradients, and, in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate under-estimates in modeled plume concentrations, leading in general to under-estimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2018) and September (2017). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (

The Euro-Mediterranean region is subject to numerous and various aerosol loads, which interact with radiation, clouds and atmospheric dynamics, with ensuing impact on regional climate. However up to now, aerosol variations are hardly taken into account in most regional climate simulations, although anthropogenic emissions have been dramatically reduced in Europe since the 1980s. Moreover, inconsistencies between regional climate models (RCMs) and their driving global model (GCM) have recently been identified in terms of future radiation and temperature evolution, which could be related to the differences in aerosol forcing. The present study aims at assessing the role of aerosols in the future evolution of the Euro-Mediterranean climate, using a specific multi-model protocol carried out in the Flagship Pilot Study "Aerosol" of the CORDEX program. This protocol relies on three simulations for each RCM: a historical run (1971-2000) and two future RCP8.5 simulations (2021-2050), a first one with evolving aerosols, and a second one with the same aerosols as in the historical period. Six modeling groups have taken part in this protocol, providing nine triplets of simulations. The analysis of these simulations will be presented here. First results show that the future evolution of aerosols has a significant impact on the evolution of surface radiation and surface temperature. In addition RCM runs taking into account the evolution of aerosols are simulating climate change signal closer to the one of their driving GCM than those with constant aerosols.

The Tropical Atlantic is facing a massive proliferation of Sargassum since 2011, with severe environmental and socioeconomic impacts. The development of Sargassum modelling is essential to clarify the link between Sargassum distribution and environmental conditions, and to lay the groundwork for a seasonal forecast on the scale of the Tropical Atlantic basin. We present here a modelling framework based on the NEMO ocean model which integrates transport by currents and waves, stranding at the coast, and physiology of Sargassum with varying internal nutrients quota. The model is initialized from basin scale satellite observations and performance was assessed over the Sargassum year 2017. Model parameters are calibrated through the analysis of large ensembles of simulations, and the sensitivity to forcing fields like riverine nutrients inputs, atmospheric deposition, and waves is investigated. Overall, results demonstrate the ability of the model to reproduce the seasonal cycle and large-scale distribution of Sargassum biomass.

Weather and climate models are challenged by uncertainties and biases in simulating Southern Ocean (SO) radiative fluxes that trace to a poor understanding of cloud, aerosol, precipitation, and radiative processes, and their interactions. Projects between 2016 and 2018 used in situ probes, radar, lidar, and other instruments to make comprehensive measurements of thermodynamics, surface radiation, cloud, precipitation, aerosol, cloud condensation nuclei (CCN), and ice nucleating particles over the SO cold waters, and in ubiquitous liquid and mixed-phase clouds common to this pristine environment. Data including soundings were collected from the NSF–NCAR G-V aircraft flying north–south gradients south of Tasmania, at Macquarie Island, and on the R/V Investigator and RSV Aurora Australis. Synergistically these data characterize boundary layer and free troposphere environmental properties, and represent the most comprehensive data of this type available south of the oceanic polar front, in the cold sector of SO cyclones, and across seasons. Results show largely pristine environments with numerous small and few large aerosols above cloud, suggesting new particle formation and limited long-range transport from continents, high variability in CCN and cloud droplet concentrations, and ubiquitous supercooled water in thin, multilayered clouds, often with small-scale generating cells near cloud top. These observations demonstrate how cloud properties depend on aerosols while highlighting the importance of dynamics and turbulence that likely drive heterogeneity of cloud phase. Satellite retrievals confirmed low clouds were responsible for radiation biases. The combination of models and observations is examining how aerosols and meteorology couple to control SO water and energy budgets.

This study investigates, through regional climate modelling, the surface mass concentration and AOD (aerosol optical depth) evolution of the various (anthropogenic and natural) aerosols over the Euro-Mediterranean region between the end of the 20th century and the mid-21st century. The direct aerosol radiative forcing (DRF) as well as the future Euro-Mediterranean climate sensitivity to aerosols have also been analysed. Different regional climate simulations were carried out with the CNRM-ALADIN63 regional climate model, driven by the global CNRM-ESM2-1 Earth system model (used in CMIP6) and coupled to the TACTIC (Tropospheric Aerosols for ClimaTe In CNRM) interactive aerosol scheme. These simulations follow several future scenarios called shared socioeconomic pathways (SSP 1-1.9, SSP 3-7.0 and SSP 5-8.5), which have been chosen to analyse a wide range of possible future scenarios in terms of aerosol or particle precursor emissions. Between the historical and the future period, results show a total AOD decrease between 30 % and 40 % over Europe for the three scenarios, mainly due to the sulfate AOD decrease (between −85 and −93 %), that is partly offset by the nitrate and ammonium particles AOD increase (between +90 and +120 %). According to these three scenarios, nitrate aerosols become the largest contributor to the total AOD during the future period over Europe, with a contribution between 43.5 % and 47.5 %. It is important to note that one of the precursors of nitrate and ammonium aerosols, nitric acid, has been implemented in the model as a constant climatology over time. Concerning natural aerosols, their contribution to the total AOD increases slightly between the two periods. The different evolution of aerosols therefore impacts their DRF, with a significant sulfate DRF decrease between 2.4 and 2.8 W m−2 and a moderate nitrate and ammonium DRF increase between 1.3 and 1.5 W m−2, depending on the three scenarios over Europe. These changes, which are similar under the different scenarios, explain about 65 % of the annual shortwave radiation change but also about 6 % (in annual average) of the warming expected over Europe by the middle of the century. This study shows, with SSP 5-8.5, that the extra warming attributable to the anthropogenic aerosol evolution over Central Europe and the Iberian Peninsula during the summer period is due to “aerosol–radiation” as well as “aerosol–cloud” interaction processes. The extra warming of about 0.2 ∘C over Central Europe is explained by a surface radiation increase of 5.8 W m−2 over this region, due to both a surface aerosol DRF decrease of 4.4 W m−2 associated with a positive effective radiative forcing due to aerosol–radiation interactions (ERFari) of 2.7 W m−2 at the top of the atmosphere (TOA) and a cloud optical depth (COD) decrease of 1.3. In parallel, the simulated extra warming of 0.2∘C observed over the Iberian Peninsula is due to a COD decrease of 1.3, leading to a positive effective radiative forcing due to aerosol–cloud interactions (ERFaci) of 2.6 W m−2 at the TOA but also to an atmospheric dynamics change leading to a cloud cover decrease of about 1.7 % and drier air in the lower layers, which is a signature of the semi-direct forcing. This study thus highlights the necessity of taking into account the evolution of aerosols in future regional climate simulations.

We analyse of the airborne measurements of above-cloud aerosols from the AEROCLO-sA field campaign performed in Namibia during August and September 2017. 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 OSIRIS, was deployed on-board the Safire 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 AAC and cloud properties, with well-defined uncertainties. OSIRIS was supplemented with the airborne multi-wavelength sun-photometer PLASMA2. The application of the algorithm developed for the POLDER spaceborne instrument in the visible range to the OSIRIS measurements allowed to characterise the Aerosol Above Cloud (AAC) properties. The variations of the aerosol properties are consistent with the different atmospheric circulation regimes observed during the deployment. Airborne observations typically a show strong Aerosol Optical Depth (AOD, up to 1.2 at 550 nm) of fine mode particles from biomass burning (extinction Angström exponent varying between 1.6 and 2.2), transported above a stratocumulus deck (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 % with the PLASMA2 sun-photometer measured in the same environment. The AEROCLO-sA campaign-average Single Scattering Albedo (SSA) obtained by OSIRIS at 550 nm is 0.87. The strong absorption of the biomass burning plumes in the visible is consistent with the observations from the AERONET ground-based sun-photometers. The latter indicate a significant increase of the absorption at 440 nm, showing possible additional presence of absorbing organic species within the smoke plumes. Biomass burning aerosols are also vertically collocated with significant amounts of water content up to the top of the plume around 6 km height. The average AAC Direct Radiative Effect (DRE) calculated from the airborne measurements in the visible range is +85 W m−2 (standard deviation of 26 W m−2) with instantaneous values up to +200 W m−2 during intense events. Combination between water vapour and the strong positive aerosol forcing over the region explains possible feedbacks on cloud development. This new set of data represents a new opportunity to better constrain climate models and to study aerosol–cloud–radiation interactions over the South-East Atlantic region.

As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based in-situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m asl) to characterize the physical, optical and chemical properties of aerosols. During the observation period, three different aerosol regimes have been identified, including a dust outbreak (Dust) originating from Algeria/Tunisia, a primary marine aerosols (PMA) event from both the Gulf of Lion and emissions near the sample site, and a pollution period from Eastern Europe, which includes anthropogenic and biomass burning sources (BBP). The chemical, physical and optical properties of the observed aerosols as well as their local shortwave (SW) direct radiative forcing (DRF) in clear-sky conditions are compared for these three periods in order to assess the direct radiative impact of PMA above the Western Mediterranean Basin. The PMA period is characterized by a mean sea salt mass concentration up to 6.5 μg m−3, representing 40 % of the total PM10 mass concentration, and a relatively low ratio of chloride to sodium (average of 0.57) indicating a generally "aged" sea salt aerosol at Ersa. In this work, an original dataset, obtained from on-line real-time instruments (ATOFMS, PILS-IC) have been used to characterize the ageing of PMA. The majority of PMA had surprisingly undergone chemical reactions and were mostly advected from long-range transport. During PMA period, the mixing between fresh and aged PMA originated from both local and regional (Gulf of Lion) emissions. The aerosol optical properties, obtained for the whole atmospheric column and at the surface, indicate a single scattering albedo (SSA) near unity (at 440 nm), indicating almost purely scattering particles, associated to a relatively low aerosol optical depth (AOD) close to 0.1 (at 500 nm), and an aerosol angstrom extinction exponent (AE) equal to 1.3 ± 0.4 (between 440 and 870 nm), suggesting a possible mixing of the PMA with fine particles (probably of continental origin). AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of −11 ± 4 W m−2 at the surface and −8 ± 3 W m−2 at the top of the atmosphere (TOA). In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3–0.4 at 440 nm and column-integrated SSA of 0.90–0.95), induced a local instantaneous SW DRF nearly three times the forcing calculated during the PMA period, with maximum values up to −40 W m−2 at the surface. On average, the SW DRF was about −21 ± 11 and −14 ± 6 W m−2, at the surface and at TOA, respectively, during this dust outbreak. Finally, the BBP period was characterized by a significant increase of the aerosol PM1 mass concentration (from 3.7 μg m−3 to 7.2 μg m−3) due to the influence of biomass-burning and anthropogenic aerosols transported from Eastern Europe. The influence of polluted/smoke particles led to a significant decrease in SSA (0.90 at 440 nm), showing the important absorbing characteristics of such particles. For this period, the SW DRF at the surface and TOA also exhibit higher mean values compared to the PMA period (with values of −23 ± 6 W m−2 and −15 ± 4 W m−2, respectively) and similar range of values as the Dust period.

This study investigates, through regional climate modelling, the surface mass concentration and AOD (Aerosol Optical Depth) evolution of the various (anthropogenic and natural) aerosols over the Euro-Mediterranean region between the end of the 20th century and the mid-21st century. The direct aerosol radiative forcing (DRF) as well as the future Euro-Mediterranean climate sensitivity to aerosols have been also analysed. Different regional climate simulations were carried out with the CNRM-ALADIN63 regional climate model, driven by the global CNRM-ESM2-1 Earth System Model (used in CMIP6) and coupled to the TACTIC (Tropospheric Aerosols for ClimaTe In CNRM) interactive aerosol scheme. These simulations follow several future scenarios called Shared Socioeconomic Pathways (SSP 1-1.9, SSP 3-7.0 and SSP 5-8.5), which have been chosen to analyse a wide range of possible future scenarios in terms of aerosol or particles precursors emissions. Between the historical and the future period, results show a total AOD decrease between 30 and 40 % over Europe for the three scenarios mainly due to the sulfate AOD decrease (between −85 and −93 %), that is partly offset by the nitrate and ammonium particles AOD increase (between +90 and +120 %). According to these three scenarios, nitrate aerosols become the largest contributor to the total AOD during the future period over Europe, with a contribution between 43.5 and 47.5 %. Concerning natural aerosols, their contribution to the total AOD increases slightly between the two periods. The different evolution of aerosols therefore impacts their DRF, with a significant sulfate DRF decrease by 2.6 W m−2 and a moderate nitrate and ammonium DRF increase by 1.4 W m−2, on average according to the three scenarios over Europe. These changes, which are similar under the different scenarios, explain about 65 % of the annual shortwave radiation change but also about 6 % (in annual average) of the warming expected over Europe by the middle of the century. This study shows, with the SSP 5-8.5, that the extra-warming attributable to the anthropogenic aerosols evolution over Central Europe and the Iberian Peninsula during the summer period is due to aerosol-radiation as well as aerosol-cloud interactions processes. The extra-warming of about 0.2 °C over Central Europe is explained by a surface radiation increase of 5.8 W m−2 over this region, due to both a surface aerosol DRF decrease of 4.4 W m−2 and cloud optical depth (COD) decrease of 1.3. In parallel, the simulated extra-warming of 0.2 °C observed over the Iberian Peninsula is due, as for it, to a COD decrease of 1.3 but also to an atmospheric dynamics change leading to a cloud cover decrease of about 2 % and a drier air in the lower layers, signature of the semi-direct forcing. This study thus highlights the necessity of taking into account the evolution of aerosols in future regional climate simulations.

The Tropical Atlantic is facing a massive proliferation of Sargassum since 2011, with severe environmental and socioeconomic impacts. The development of Sargassum modelling is essential to clarify the link between Sargassum distribution and environmental conditions, and to lay the groundwork for a seasonal forecast on the scale of the Tropical Atlantic basin. We developed a modelling framework based on the NEMO ocean model, which integrates transport by currents and waves, physiology of Sargassum with varying internal nutrients quota, and considers stranding at the coast. The model is initialized from basin scale satellite observations and performance was assessed over the Sargassum year 2017. Model parameters are calibrated through the analysis of a large ensemble of simulations, and the sensitivity to forcing fields like riverine nutrients inputs, atmospheric deposition, and waves is discussed. Overall, results demonstrate the ability of the model to reproduce and forecast the seasonal cycle and large-scale distribution of Sargassum biomass.

In spring, the Mediterranean Sea, a well-stratified low nutrient low chlorophyll region, receives atmospheric deposition both desert dust from the Sahara and airborne particles from anthropogenic sources. Such deposition translates into a supply of new nutrients and trace metals for the surface waters that likely impact biogeochemical cycles. However, the quantification of the impacts and the processes involved are still far from being assessed in situ. In this paper, we provide a state of the art regarding dust deposition and its impact on the Mediterranean Sea biogeochemistry and we describe in this context the objectives and strategy of the PEACETIME project and cruise, entirely dedicated to filling this knowledge gap. Our strategy to go a step forward than in previous approaches in understanding these impacts by catching a real deposition event at sea is detailed. The PEACETIME oceanographic campaign took place in May–June 2017 and we describe how we were able to successfully adapt the planned transect in order to sample a Saharan dust deposition event, thanks to a dedicated strategy, so-called Fast Action. That was successful, providing, for the first time in our knowledge, a coupled atmospheric and oceanographic sampling before, during and after an atmospheric deposition event. Atmospheric and marine in situ observations and process studies have been conducted in contrasted area and we summarize the work performed at sea, the type of data acquired and their valorization in the papers published in the special issue.

Simulations are performed for the period 2000–2015 by two different regional climate models, ALADIN and RegCM, to quantify the direct and semi-direct radiative effects of biomass-burning aerosols (BBAs) in the southeast Atlantic (SEA) region. Different simulations have been performed using strongly absorbing BBAs in accordance with recent in situ observations over the SEA. For the July–August–September (JAS) season, the single scattering albedo (SSA) and total aerosol optical depth (AOD) simulated by the ALADIN and RegCM models are consistent with the MACv2 climatology and MERRA-2 and CAMS-RA reanalyses near the biomass-burning emission sources. However, the above-cloud AOD is slightly underestimated compared to satellite (MODIS and POLDER) data during the transport over the SEA. The direct radiative effect exerted at the continental and oceanic surfaces by BBAs is significant in both models and the radiative effects at the top of the atmosphere indicate a remarkable regional contrast over SEA (in all-sky conditions), with a cooling (warming) north (south) of 10 ∘S, which is in agreement with the recent MACv2 climatology. In addition, the two models indicate that BBAs are responsible for an important shortwave radiative heating of ∼0.5–1 K per day over SEA during JAS with maxima between 2 and 4 km a.m.s.l. (above mean sea level). At these altitudes, BBAs increase air temperature by ∼0.2–0.5 K, with the highest values being co-located with low stratocumulus clouds. Vertical changes in air temperature limit the subsidence of air mass over SEA, creating a cyclonic anomaly. The opposite effect is simulated over the continent due to the increase in lower troposphere stability. The BBA semi-direct effect on the lower troposphere circulation is found to be consistent between the two models. Changes in the cloud fraction are moderate in response to the presence of smoke, and the models differ over the Gulf of Guinea. Finally, the results indicate an important sensitivity of the direct and semi-direct effects to the absorbing properties of BBAs. Over the stratocumulus (Sc) region, DRE varies from +0.94 W m−2 (scattering BBAs) to +3.93 W m−2 (most absorbing BBAs).

International audience; 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.

The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29 May until 30 June 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, speciated atmospheric mercury and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS.Biomass burning emissions dominated the gas and aerosol concentrations in this region. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north-west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. Here we present characteristics of the biomass burning observed at the sampling site and provide an overview of the more specific outcomes of the SAFIRED campaign.

Savanna fires contribute significantly to global aerosol loading and hence to the earth's radiative budget. Modelling of the climatic impact of these aerosols is made difficult due to a lack of knowledge of their size distribution. Australia is the third largest source of global carbon emissions from biomass burning, with emissions dominated by tropical savanna fires. Despite this, only a few previous studies have reported emission factors of trace gases from this important ecosystem and there are no previous published emission factors for the aerosol properties reported here for Australian savanna fires. In June 2014, the SAFIRED campaign (Savanna Fires in the Early Dry season) took place in the northern territory of Australia, with the purpose of investigating emissions and aging of aerosols from Australian savanna fires. This paper presents observed enhancement ratios and inferred emission factors of trace gases (CO2, CO, CH4, N2O and gaseous elemental mercury), particles over different size modes (Aitken and accumulation) and speciated aerosols components (organics, sulfate, nitrate, ammonium and chloride). Nine smoke events were identified from the data using large enhancements in CO and/or aerosol data to indicate biomass burning event. The results reported in this paper include the first emission factors for Aitken and accumulation mode aerosols from savanna fires, providing useful size information to enable better modelling of the climatic impact of this important source of global aerosols.

The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm−3 when frequent and close fires were burning – up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ = 0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to ∼ 100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large variations in the activation diameters. Trade winds carry the smoke generated from these fires over the Timor Sea, where aerosol–cloud interactions are likely to be sensitive to changes in CCN concentrations, perturbing cloud albedo and lifetime. Dry season fires in northern Australia are therefore potentially very important in cloud processes in this region.

There is a lack of knowledge of how biomass burning aerosols in the tropics age, including those in the fire-prone Northern Territory in Australia. This paper reports chemical characterization of fresh and aged aerosols monitored during the 1-month-long SAFIRED (Savannah Fires in the Early Dry Season) field study, with an emphasis on the chemical signature and aging of organic aerosols. The campaign took place in June 2014 during the early dry season when the surface measurement site, the Australian Tropical Atmospheric Research Station (ATARS), located in the Northern Territory, was heavily influenced by thousands of wild and prescribed bushfires. ATARS was equipped with a wide suite of instrumentation for gaseous and aerosol characterization. A compact time-of-flight aerosol mass spectrometer was deployed to monitor aerosol chemical composition. Approximately 90 % of submicron non-refractory mass was composed of organic material. Ozone enhancement in biomass burning plumes indicated increased air mass photochemistry. The diversity in biomass burning emissions was illustrated through variability in chemical signature (e.g. wide range in f44, from 0.06 to 0.18) for five intense fire events. The background particulate loading was characterized using positive matrix factorization (PMF). A PMF-resolved BBOA (biomass burning organic aerosol) factor comprised 24 % of the submicron non-refractory organic aerosol mass, confirming the significance of fire sources. A dominant PMF factor, OOA (oxygenated organic aerosol), made up 47 % of the sampled aerosol, illustrating the importance of aerosol aging in the Northern Territory. Biogenic isoprene-derived organic aerosol factor was the third significant fraction of the background aerosol (28 %).

The emission factors (EFs) for a broad range of semivolatile organic chemicals (SVOCs) from subtropical eucalypt forest and tropical savannah fires were determined for the first time from in situ investigations. Significantly higher (t test, P < 0.01) EFs (μg kg–1 dry fuel, gas + particle-associated) for polycyclic aromatic hydrocarbons (∑13 PAHs) were determined from the subtropical forest fire (7,000 ± 170) compared to the tropical savannah fires (1,600 ± 110), due to the approximately 60-fold higher EFs for 3-ring PAHs from the former. EF data for many PAHs from the eucalypt forest fire were comparable with those previously reported from pine and fir forest combustion events. EFs for other SVOCs including polychlorinated biphenyl (PCB), polychlorinated naphthalene (PCN), and polybrominated diphenyl ether (PBDE) congeners as well as some pesticides (e.g., permethrin) were determined from the subtropical eucalypt forest fire. The highest concentrations of total suspended particles, PAHs, PCBs, PCNs, and ...

Dust transported from north African source region toward the Mediterranean basin and Europe is a ubiquitous phenomenon in the Mediterranean region. Winds formed by large-scale pressure gradients foster dust entrainment into the atmosphere over north African dust source regions and advection of dust downwind. The constellation of centers of high and low pressure determines wind speed and direction, and thus the chance for dust emission over northern Africa and transport toward the Mediterranean. We present characteristics of the atmospheric dust life cycle determining dust transport toward the Mediterranean basin with focus on the ChArMEx (Chemistry-Aerosol Mediterranean Experiment) special observation period in June and July 2013 using the atmosphere–dust model COSMO-MUSCAT (COSMO: COnsortium for Small-scale MOdeling; MUSCAT: MUltiScale Chemistry Aerosol Transport Model). Modes of atmospheric circulation are identified from empirical orthogonal function (EOF) analysis of the geopotential height at 850 hPa and compared to EOFs calculated from 1979–2015 ERA-Interim reanalysis. Two different phases are identified from the first EOF, which in total explain 45 % of the variance. They are characterized by the propagation of the subtropical ridge into the Mediterranean basin, the position of the Saharan heat low and the predominant Iberian heat low, and discussed illustrating a dipole pattern for enhanced (reduced) dust emission fluxes, stronger (weaker) meridional dust transport, and consequent increased (decreased) atmospheric dust concentrations and deposition fluxes. In the event of a predominant high-pressure zone over the western and central Mediterranean (positive phase), a hot spot in dust emission flux is evident over the Grand Erg Occidental, and a reduced level of atmospheric dust loading occurs over the western Mediterranean basin. The meridional transport in northward direction is reduced due to prevailing northerly winds. In case of a predominant heat low trough linking the Iberian and the Saharan heat low (negative phase), meridional dust transport toward the western Mediterranean is increased due to prevailing southerly winds resulting in an enhanced atmospheric dust loading over the western Mediterranean. Altogether, results from this study illustrate the relevance of knowing dust source location and characteristics in concert with atmospheric circulation. The study elaborates on the question of the variability of summertime dust transport toward the Mediterranean and Europe with regard to atmospheric circulation conditions controlling dust emission and transport routes of Saharan dust, exemplarily for the 2-month period of June–July 2013. Ultimately, outcomes from this study contribute to the understanding of the variance in dust transport into a populated region.

The aerosol-driven radiative effects on marine low-level cloud represent a large uncertainty in climate simulations, in particular over the Southern Ocean, which is also an important region for sea spray aerosol production. Observations of sea spray aerosol organic enrichment and the resulting impact on water uptake over the remote Southern Hemisphere are scarce, and therefore the region is under-represented in existing parameterisations. The Surface Ocean Aerosol Production (SOAP) voyage was a 23 d voyage which sampled three phytoplankton blooms in the highly productive water of the Chatham Rise, east of New Zealand. In this study we examined the enrichment of organics to nascent sea spray aerosol and the modifications to sea spray aerosol water uptake using in situ chamber measurements of seawater samples taken during the SOAP voyage. Primary marine organics contributed up to 23 % of the sea spray mass for particles with diameter less than approximately 1 µm and up to 79 % of the particle volume for 50 nm diameter sea spray. The composition of the submicron organic fraction was consistent throughout the voyage and was largely composed of a polysaccharide-like component, characterised by very low alkane-to-hydroxyl-concentration ratios of approximately 0.1–0.2. The enrichment of organics was compared to the output from the chlorophyll-a-based sea spray aerosol parameterisation suggested by Gantt et al. (2011) and the OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) models. OCEANFILMS improved on the representation of the organic fraction predicted using chlorophyll a, in particular when the co-adsorption of polysaccharides was included; however, the model still under-predicted the proportion of polysaccharides by an average of 33 %. Nascent 50 nm diameter sea spray aerosol hygroscopic growth factors measured at 90 % relative humidity averaged 1.93±0.08 and did not decrease with increasing sea spray aerosol organic fractions. The observed hygroscopicity was greater than expected from the assumption of full solubility, particularly during the most productive phytoplankton bloom (B1), during which organic fractions were greater than approximately 0.4. The water uptake behaviour observed in this study is consistent with that observed for other measurements of phytoplankton blooms and can be partially attributed to the presence of sea salt hydrates, which lowers the sea spray aerosol hygroscopicity when the organic enrichment is low. The inclusion of surface tension effects only marginally improved the modelled hygroscopicity, and a significant discrepancy between the observed and modelled hygroscopicity at high organic volume fractions remained. The findings from the SOAP voyage highlight the influence of biologically sourced organics on sea spray aerosol composition; these data improve the capacity to parameterise sea spray aerosol organic enrichment and water uptake.

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 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). 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 of 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. Biomass burning 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 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 assessing the direct and semi-direct radiative effects of biomass burning particles.

Estimates of the direct radiative effect (DRE) from absorbing smoke aerosols over the southeast Atlantic Ocean (SAO) require simulation of the microphysical and optical properties of stratocumulus clouds as well as of the altitude and shortwave (SW) optical properties of biomass burning aerosols (BBAs). In this study, we take advantage of the large number of observations acquired during the ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES-2016) and Layered Atlantic Smoke Interactions with Clouds (LASIC) projects during September 2016 and compare them with datasets from the ALADIN-Climate (Aire Limitée Adaptation dynamique Développement InterNational) regional model. The model provides a good representation of the liquid water path but the low cloud fraction is underestimated compared to satellite data. The modeled total-column smoke aerosol optical depth (AOD) and above-cloud AOD are consistent (∼0.7 over continental sources and ∼0.3 over the SAO at 550 nm) with the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Ozone Monitoring Instrument (OMI) or Moderate Resolution Imaging Spectroradiometer (MODIS) data. The simulations indicate smoke transport over the SAO occurs mainly between 2 and 4 km, consistent with surface and aircraft lidar observations. The BBA single scattering albedo is slightly overestimated compared to the Aerosol Robotic Network (AERONET) and more significantly when compared to Ascension Island surface observations. The difference could be due to the absence of internal mixing treatment in the ALADIN-Climate model. The SSA overestimate leads to an underestimation of the simulated SW radiative heating compared to ORACLES data. ALADIN-Climate simulates a positive (monthly mean) SW DRE of about +6 W m−2 over the SAO (20∘ S–10∘ N and 10∘ W–20∘ E) at the top of the atmosphere and in all-sky conditions. Over the continent, the presence of BBA is shown to significantly decrease the net surface SW flux, through direct and semi-direct effects, which is compensated by a decrease (monthly mean) in sensible heat fluxes (−25 W m−2) and surface land temperature (−1.5 ∘C) over Angola, Zambia and the Democratic Republic of the Congo, notably. The surface cooling and the lower tropospheric heating decrease the continental planetary boundary layer height by about ∼200 m.

International audience This study introduces CNRM‐ESM2‐1, the Earth system (ES) model of second generation developed by CNRM‐CERFACS for the sixth phase of the Coupled Model Intercomparison Project (CMIP6). CNRM‐ESM2‐1 offers a higher model complexity than the Atmosphere‐Ocean General Circulation Model CNRM‐CM6‐1 by adding interactive ES components such as carbon cycle, aerosols, and atmospheric chemistry. As both models share the same code, physical parameterizations, and grid resolution, they offer a fully traceable framework to investigate how far the represented ES processes impact the model performance over present‐day, response to external forcing and future climate projections. Using a large variety of CMIP6 experiments, we show that represented ES processes impact more prominently the model response to external forcing than the model performance over present‐day. Both models display comparable performance at replicating modern observations although the mean climate of CNRM‐ESM2‐1 is slightly warmer than that of CNRM‐CM6‐1. This difference arises from land cover‐aerosol interactions where the use of different soil vegetation distributions between both models impacts the rate of dust emissions. This interaction results in a smaller aerosol burden in CNRM‐ESM2‐1 than in CNRM‐CM6‐1, leading to a different surface radiative budget and climate. Greater differences are found when comparing the model response to external forcing and future climate projections. Represented ES processes damp future warming by up to 10% in CNRM‐ESM2‐1 with respect to CNRM‐CM6‐1. The representation of land vegetation and the CO2‐water‐stomatal feedback between both models explain about 60% of this difference. The remainder is driven by other ES feedbacks such as the natural aerosol feedback.

The Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) project investigates the role of aerosols on the regional climate of southern Africa. This is a unique environment where natural and anthropogenic aerosols and a semipermanent and widespread stratocumulus (Sc) cloud deck are found. The project aims to understand the dynamical, chemical, and radiative processes involved in aerosol–cloud–radiation interactions over land and ocean and under various meteorological conditions. The AEROCLO-sA field campaign was conducted in August and September of 2017 over Namibia. An aircraft equipped with active and passive remote sensors and aerosol in situ probes performed a total of 30 research flight hours. In parallel, a ground-based mobile station with state-of-the-art in situ aerosol probes and remote sensing instrumentation was implemented over coastal Namibia, and complemented by ground-based and balloonborne observations of the dynamical, thermodynamical, and physical properties of the lower troposphere. The focus laid on mineral dust emitted from salty pans and ephemeral riverbeds in northern Namibia, the advection of biomass-burning aerosol plumes from Angola subsequently transported over the Atlantic Ocean, and aerosols in the marine boundary layer at the ocean–atmosphere interface. This article presents an overview of the AEROCLO-sA field campaign with results from the airborne and surface measurements. These observations provide new knowledge of the interactions of aerosols and radiation in cloudy and clear skies in connection with the atmospheric dynamics over southern Africa. They will foster new advanced climate simulations and enhance the capability of spaceborne sensors, ultimately allowing a better prediction of future climate and weather in southern Africa.

In Eastern Boundary Upwelling Systems (EBUS), the upwelling favorable wind speeds decrease toward the coast in the so-called wind drop-off coastal strip, which has been shown to be influential on the coastal upwelling dynamics, particularly in terms of the relative contributions of Ekman drift and Ekman suction to coastal upwelling. Currently, the wind drop-off length scale is not properly resolved by the atmospheric forcing of regional ocean models in EBUS, featuring a smoother cross-shore wind profile that results in stronger near-shore speeds that could partly explain the coastal cold bias often found in those model simulations. Here, as a case study for the upwelling system off Central Chile, the sensitivity of upwelling dynamics to the coastal wind reduction is investigated using a Regional Ocean Modeling System (ROMS). Coastal wind profiles at different resolutions are first generated using a regional atmospheric model, validated from altimeter data, and then used to correct the coarse atmospheric wind forcing used for sensitivity experiments with ROMS. It is shown that the wind drop-off correction induces a reduction in the oceanic coastal jet intensity, a stronger poleward undercurrent and a coherent offshore Ekman drift. It also yields a significant reduction of the cold bias along the coast compared to the simulation with uncorrected winds. Such reduction cannot be solely explained by the reduced Ekman transport only partially compensated by increase in Ekman suction. The analysis of the surface heat budget reveals in fact that an important contributor to the cooling reduction along the coast in the presence of coastal wind drop-off is the heat flux term mediated by the reduction in the mixed-layer depth. Overall, our results illustrate the nonlinear response of the upwelling dynamics to the coastal wind profiles in this region.