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Icelandic dust can impact the radiative budget in high-latitude regions directly by affecting light absorption and scattering and indirectly by changing the surface albedo after dust deposition. This tends to produce a positive radiative forcing. However, the limited knowledge of the spectral optical properties of Icelandic dust prevents an accurate assessment of these radiative effects. Here, the spectral single scattering albedo (SSA) and the complex refractive index (m=n-ik) of Icelandic dust from five major emission hotspots were retrieved between 370–950 nm using online measurements of size distribution and spectral absorption (βabs) and scattering (βsca) coefficients of particles suspended in a large-scale atmospheric simulation chamber. The SSA(λ) estimated from the measured βabs and βsca increased from 0.90–0.94 at 370 nm to 0.94–0.96 at 950 nm in Icelandic dust from the different hotspots, which falls within the range of mineral dust from northern Africa and eastern Asia. The spectral complex refractive index was retrieved by minimizing the differences between the measured βabs and βsca and those computed using the Mie theory for spherical and internally homogeneous particles, using the size distribution data as input. The real part of the complex refractive index (n(λ)) was found to be 1.60–1.61 in the different samples and be independent of wavelength. The imaginary part (k(λ)) was almost constant with wavelength and was found to be around 0.004 at 370 nm and 0.002–0.003 at 950 nm. The estimated complex refractive index was close to the initial estimates based on the mineralogical composition, also suggesting that the high magnetite content observed in Icelandic dust may contribute to its high absorption capacity in the shortwave part of the spectrum. The k(λ) values retrieved for Icelandic dust are at the upper end of the reported range for low-latitude dust (e.g., from the Sahel). Furthermore, Icelandic dust tends to be more absorbing towards the near-infrared. In Icelandic dust, k(λ) between 660–950 nm was 2–8 times higher than most of the dust samples sourced in northern Africa and eastern Asia. This suggests that Icelandic dust may have a stronger positive direct radiative forcing on climate that has not been accounted for in climate predictions.

International audience; Glycolaldehyde (GAld) is a C2 water-soluble aldehyde produced during the atmospheric oxidation of isoprene and many other species and is commonly found in cloudwater. Previous work has established that glycolaldehyde evaporates more readily from drying aerosol droplets containing ammonium sulfate (AS) than does glyoxal, methylglyoxal, or hydroxyacetone, which implies that it does not oligomerize as quickly as these other species. Here, we report NMR measurements of glycolaldehyde’s aqueous-phase reactions with AS, methylamine, and glycine. Reaction rate constants are smaller than those of respective glyoxal and methylglyoxal reactions in the pH range of 3–6. In follow-up cloud chamber experiments, deliquesced glycine and AS seed particles were found to take up glycolaldehyde and methylamine and form brown carbon. At very high relative humidity, these changes were more than 2 orders of magnitude faster than predicted by our bulk liquid NMR kinetics measurements, suggesting that reactions involving surface-active species at crowded air–water interfaces may play an important role. The high-resolution liquid chromatography–electrospray ionization–mass spectrometric analysis of filter extracts of unprocessed AS + GAld seed particles identified sugar-like C6 and C12 GAld oligomers, including proposed product 3-deoxyglucosone, with and without modification by reactions with ammonia to diimine and imidazole forms. Chamber exposure to methylamine gas, cloud processing, and simulated sunlight increased the incorporation of both ammonia and methylamine into oligomers. Many C4–C16 imidazole derivatives were detected in an extract of chamber-exposed aerosol along with a predominance of N-derivatized C6 and C12 glycolaldehyde oligomers, suggesting that GAld is capable of forming brown carbon SOA

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 complex refractive index (CRI) is one of the key parameter driving aerosol spectral optical properties and direct radiative effects (DRE). Its value and spectral variation under different conditions, such as anthropogenic− and biogenic−dominated environments and anthropogenic−biogenic mixing situations, remains not fully understood. As a consequence, oversimplified representations of aerosol optical properties are generally used in climate models. Therefore, measurements of aerosol CRI in different environments and their inclusion in models are needed. The field observations from the ACROSS campaign, performed in June-July 2022 in the Ile de France region, are used in this study to deepen the knowledge of aerosol optical properties, aiming to improve the aerosol representation in the CHIMERE model and provide the best constraint for DRE simulations. Measurements obtained both at the Paris city center and the Rambouilllet rural forest sites during ACROSS are considered, in order to explore the CRI variability from anthropogenic−dominated to biogenic−dominated environments, including anthropogenic−biogenic mixing situations. The CRI retrievals at seven different wavelengths, performed by combining the Mie theory with optical and size distribution measurements, are representative of different atmospheric conditions, aerosol loadings as well as type and chemical compositions. In fact, the June-July 2022 period was characterized by highly diversified weather conditions: 1) two strong heatwaves, promoting SOA build-up and favoring the export of the Paris pollution plume towards the forest site; 2) Saharan dust events transported from the upper atmosphere to the ground; 3) biomass burning episode; 4) periods with reduced anthropogenic influence. The CRI retrievals under these different conditions and their link to particulate chemical composition is investigated. Hence, the CRI dataset presented here constitutes a unique dataset from which models can benefit to validate and constrain simulations and DRE estimations, under both urban and biogenic emissions influence. These data, in conjunction with those from the aircraft observations during ACROSS, are used to initialize and perform sensitivity studies on the aerosol DRE, using the CHIMERE−WRF coupled model, the OPTSIM model for the aerosol optical properties and the Rapid Radiative Transfer Model for GCMs (RRTMG).Keywords: Complex refractive index, direct radiative effect, aerosol mixing, urban, forest

Atmospheric aerosols make significant contributions to several atmospheric chemical and physical processes. Aerosols from anthropogenic emissions have negative impact on air quality and human health. In recent years, significant progress has been made in understanding the anthropogenic pollutants. However, it is still not clear how mixtures of anthropogenic and biogenic emissions impact the regional climate and human health. To better understand aerosol physicochemical properties within the Paris urban plume when mixed with biogenic emissions, a comprehensive airborne measurement platform was deployed in the Île-de-France region in summer 2022 as part of the ACROSS (Atmospheric ChemistRy Of the Suburban foreSt) campaign. In this study, the vertical and spatial distributions of aerosol chemical composition, size distributions, and optical properties during urban plume aging are characterized based on couples of in-situ measurement techniques like aerosol mass spectrometer (c-ToF-AMS), Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and AVIRAD staged onboard the Safire ATR 42 research aircraft. Gas phase components are also detailed characterized by Proton-transfer-reaction mass spectrometry (PTR-ToF-MS) to act as tracers of anthropogenic and biogenic emissions. Based on gas and particulate phase organic information provided by laser-induced fluorescence technique (TDLIF), the production rate of particulate organic nitrate (pON) can also be estimated. These detailed airborne measurements of aerosol properties provide data that can contribute to modelling studies of aerosol characteristics.

Global population increase has placed pressure on available resources and has resulted in the emission of a variety of trace gases into the troposphere that includes volatile organic compounds (VOCs). This class of molecules plays major roles in the formation of secondary products such as secondary organic aerosol (SOA) and tropospheric ozone, which adversely affect Earth’s climate and human health. Research has continued to reveal more details of complex atmospheric degradation processes involving VOCs of both anthropogenic and biogenic origins, but relatively few have been directly studied including the possible impacts of mixing of air masses of anthropogenic and biogenic origins. The ACROSS (Atmospheric ChemistRy Of the Suburban foreSt) project aims to improve our knowledge of atmospheric chemical processes that occur in such mixed air masses and their impact on air quality. The experimental strategy of ACROSS is based on ground-based and airborne observations during an international, large-scale, comprehensive, multi-platform, multi-site field campaign that took place in the summer of 2022 in the greater Paris and suburban forested areas.As VOCs are processed in the atmosphere, secondary compounds are produced including highly oxygenated organic molecules (HOMs) that are a subset of low volatility organic compounds characterized by their contribution to formation and ageing of SOA. Nitrate ion chemical ionization (CI), coupled with an Atmospheric Pressure Interface−Time-Of-Flight Mass Spectrometer (API-TOF-MS) is an online analytical technique that detects and quantifies gas-phase HOMs (and other compounds) with high sensitivity and mass resolution in the atmosphere or laboratory systems. This instrument provides measurements that help to fill the observational gap between the aerosol and gas phases.The instrument was deployed at the top of a 40 m tower (above the canopy) in the Rambouillet forest site during the ACROSS field campaign to measure and identify HOMs formed mainly under two different composition regimes: biogenic emissions only, and biogenic air/urban air mixtures. The data collected by the instrument will be presented and used to enhance understanding of the chemical formation pathways of HOMs and their contribution to the composition of aerosols.

The mineralogy of dust aerosols (i.e. the abundance, relative proportions and state of mixing of the different minerals composing the aerosols, including mainly silicates in the form of clays, quartz, and feldspars, carbonates, sulfates, and iron and titanium oxides) is of key relevance in driving its climatic and environmental effects. Ground–based and airborne observations support the evidence that the dust mineralogy is heterogeneous in the atmosphere, varying from local to global scale due to changes in the mineralogical composition of the emitting source soils and atmospheric processing. However, the capability to get regional and global mapping of airborne dust mineralogy is still missing to date. This gap represents a fundamental limitation for properly developing and validating the representation of dust in Earth System Models and constraining its regional and global climate forcing.Because the different minerals composing the fine and coarse fractions of dust show different spectral absorption signatures, remote sensing spectral and hyperspectral observations can be used to fill this gap by detecting the presence of diverse minerals and reconstructing their relative proportions in the dust aerosols. Based on this idea, recent efforts move into this direction, including the EMIT mission (Earth Surface Mineral Dust Source Investigation) started in 2022.In this study we demonstrate, starting from exemplary data acquired in the CESAM simulation chamber on dust aerosols from global sources (Di Biagio et al., 2017), that the extinction signature of suspended dust aerosols in the 740−1475 cm−1 infrared spectral range (6.8−13.5 µm) can be used to derive dust mineralogy in terms of its infrared−active and coarse−sized minerals: quartz, clays, feldspars and calcite. We show that diverse spectral infrared signatures allow to distinguish dust aerosols from different sources worldwide with variable composition, and that following the changes of the dust extinction spectra with time informs on particles size−selective mineralogy changes during atmospheric transport. Results from the present study confirm the major advance that hyperspectral infrared remote sensing observations, as those by IASI (Infrared Atmospheric Sounding Interferometer) and the IASI−NG (Next Generation) instruments, can provide to dust science. Di Biagio, C., Formenti, P., Balkanski, Y., Caponi, L., Cazaunau, M., Pangui, E., Journet, E., Nowak, S., Caquineau, S., Andreae, M. O., Kandler, K., Saeed, T., Piketh, S., Seibert, D., Williams, E., and Doussin, J.-F.: Global scale variability of the mineral dust long-wave refractive index: a new dataset of in situ measurements for climate modeling and remote sensing, Atmos. Chem. Phys., 17, 1901–1929, https://doi.org/10.5194/acp-17-1901-2017, 2017.

Southern Africa, and in particular its western part, Namibia, is considered a climate change hotspot by the IPCC and is at risk of severe temperature-related changes. As examples, models projections suggest by the end of the century: 1) Increase of surface temperature of +4 to +7°C; 2) destruction of the stratocumulus cloud deck along the western coast; and 3) decrease of the fog inland. The role of aerosols in this context is still not completely quantified, due to their high spatial and temporal variability, the many sources responsible for the complex mixture and the lack of continuous observations. Most of the past regional climate modelling (RCM) and intensive field campaigns focussed primarily on constraining the radiative effects of the seasonal biomass burning aerosols generally occurring in the end of the austral winter (August to October). However, the aerosol spectral optical properties, aerosol optical depth and the organic fractions are not studied enough to provide a firm understanding of regional aerosol load, interaction with radiation and interplays in relation to particle chemistry.In this work, we present the first analysis of new long-term ground-based aerosol observations conducted since april 2022 at Gobabeb Namib Research Institue (23°33’40‘’S, 15°02’24’’E) in Namibia. Gobabeb is located in the hyperarid Namib desert and it is under the influence of different air masses, transporting maritime and biomass burning aerosols, amongst others. The measurements of optical and physical properties of the aerosol mixtures are analysed to provide with the aerosol single scattering albedo and mass absorption, scattering and extinction efficiencies which are needed to evaluate the first Africa-based Earth system model by the Global Change Institute at the University of Witwatersrand in South Africa. The in situ surface data are complemented by the analysis of pre-existing observations such as those from the AERONET sunphotometers.

Mineral dust aerosols, which account for about 40% of global annual aerosol emissions, contribute to the persistent and large uncertainties on the global radiative budget and the oxidative capacity of the atmosphere.Indeed, the uptake of atmospheric volatile organic compounds (VOCs) on mineral dust particles can contribute to the formation of secondary organic aerosols (SOA), with consequent modification of the chemical and optical properties of the dust.Glyoxal, one of the most important VOC in the atmosphere, is a precursor of SOA, capable of interacting with mineral dust and forming SOA as a consequence of the interaction.In this experimental study we investigate the formation of SOA by the uptake of glyoxal on mineral dust particles. We present the results of the heterogeneous interaction obtained in the CESAM atmospheric simulation chamber (Chambre Expérimentale de Simulation Atmosphérique Multiphasique), used to conduct aging experiments in various controlled conditions in terms of relative humidity, irradiation, and gas phase composition. Prior entering the chamber, particles from a real soil sample (Gobi Desert) are size-selected using an aerodynamic aerosol classifier (AAC) in order to obtain a monodispersed size distribution centered at 300 nm in mobility diameter, narrow enough to be able to appreciate a dimensional variation from glyoxal condensation.In experiments conducted in humid conditions (RH=80%), a rapid uptake of glyoxal was observed on sub micrometric dust particles. 15 minutes after the injection of 1 ppm of glyoxal into the chamber, the mass of the particles increased by about 10%, with a variation of the modal diameter of the size distribution. As a consequence of glyoxal uptake in humid conditions, an increase of the aerosol organic mass concentration occurred immediately after the interaction, which was not observed in dry conditions. At the same time, the aerosol chemical speciation monitor (ACSM) mass spectra of the organic fraction show the increase in intensity of the glyoxal marker signals at m/z 58 and m/z 29. It is interesting to note also the drop of O/C ratio of the dust organic fraction after the injection of the glyoxal from 1.5 (the one of the dust itself) to a value close to 1, that is the one of the glyoxal.Hence, the first results of the study suggest the presence of a fast glyoxal uptake on submicronic mineral dust particles in high relative humidity conditions. This process modifies the mass and the size distribution of the aerosol, as well as the chemical composition of its organic fraction.

The international ACROSS (Atmospheric ChemistRy Of the Suburban forest) intensive field measurement campaign (supported by the Make Our Planet Great Again initiative) took place from June 13 to July 25 2022 in and around the Ile-de-France during an exceptional hot (more than 3°C above the climatological mean for France) and dry summer season. This work will provide a broad classification of weather conditions that occurred during the campaign, useful for further analysis of observations and simulations. Weather scenarios will be analysed in terms of synoptic weather situations, relating transport patterns (regional advection to the Ile-de-France region, plumes from Paris agglomeration), temperature and relative humidity evolution. During the June-July 2022 period, several distinct weather and pollution patterns occurred, among which: (1) two strong heatwaves, with large photochemical activity promoting secondary pollutants build-up (O3, SOA), (2) advection of relatively clean oceanic air masses, and (3) Saharan dust and intense forest fire events with dust and fire aerosol advection to the Ile-de-France region. The analysis is based on meteorological data from several models (GFS, WRF, ARPEGE, AROME) and observations, pollution forecasts from the French Prev’Air system (http://www2.prevair.org/), and from the AirParif Esmeralda platform (http://www.esmeralda-web.fr/accueil/) that have been used for the airborne campaign support. In addition, dedicated simulations with the CHIMERE model (see companion abstract by Di Antonio et al. for this session), and major pollutant observations by air quality networks, from satellites, or performed within ACROSS will be used to analyse how meteorological conditions and weather patterns impacted the spatial distributions of major primary and secondary chemical species. Especially tracers of anthropogenic and biogenic emissions and photochemical activity (O3, PM2.5, OA, BC, NOx, BVOC) will be analysed. Keywords: Meteorology, pollutant distributions, transport patterns, ACROSS, MOPGA

Mineral dust is an important aerosol specie in the atmosphere that impacts the Earth’s climate system through its interactions with radiation, clouds, hydrology, atmospheric chemistry, and biogeochemistry. Because dust sizes span more than three orders of magnitude in diameter and dust properties are size-dependent, most previous studies separate dust particles into different classes – broadly defined as fine and coarse dust – which could produce distinct impacts on the Earth system. However, there are general inconsistencies in the terminology, the diameter boundaries, and diameter ranges currently attributed to dust size classes across the literature. As part of a comprehensive review of coarse dust recently completed, we propose, with justification, a new uniform classification that defines coarse and super-coarse dust as particles between 2.5 - 10 µm and 10 - 62.5 µm in diameter, respectively. In addition, we will show several lines of observational evidence that indicate coarse and super-coarse dust particles are transported much farther than previously expected and that the abundance of these particles is substantially underestimated in current global models. Despite the limitations of representing coarse and super-coarse dust aerosols in models, we will highlight their unique impacts on several aspects of the Earth's climate system.

While the most extensive and active sources of mineral dust are found at mid-latitudes (Sahara, East Asia and the Arabic peninsula), source areas at high latitudes both in northern and the southern Hemispheres, are gaining attention because of their distinct characteristics and impacts at the appropriate regional and semi-hemispheric scales.Southern Africa is estimated to account for approximately 5% of the global annual emissions of mineral dust and the long-range transport of dust emitted from these regions are shown to head towards the South Atlantic, the southern Oceans, and across the subcontinent by both observations and modelling.In particular, hundreds distinct point sources have been identified in Namibia, including the topographical lows of the Etosha pan alluvial basin, the dry lands (Kalahari Desert, gravel plains bordering the Namib Deserts), but mostly the numerous ephemeral riverbeds, pans, wetlands and possibly mines along the coastline. By deposition, this windblown dust could impact to the productivity of the waters offshore, but also the formation and the chemical composition of the fog and low marine clouds. Through the fog, the dust emitted has the potential of redistributing nutrients not only to the marine but also to the continental ecosystems. Likewise, the strong and almost omnipresent southerly trade winds driven by the temperature contrast between the cold Benguela current and warm and dry continental desert air masses also provide an opportunity to transport sediment influenced by the nutrient rich aerosols of the ocean further onto land to nourish the nearshore ecosystems. To date, the majority of dust emissions observations from this region have relied heavily on the improved ability of satellite platforms to optically isolate dust aerosols over the ocean surface and despite the consistent high winds from the south, have excluded the potential for dust emission transport processes towards the interior.This presentation illustrates the new results of recent coordinated research exploring the emissions, the transport, and properties of net transported mineral dust from Namibia sources. These new results rely on model simulations at different spatial resolution, on the analysis of local and regional wind regimes, on field observations, and on laboratory-based experiments on airborne dust generated from natural soils. Our results demonstrate that the frequency of emission might be higher than expected by only easterly berg winds. We also suggest that the Namibian dust may be transported to Antartica and that its processing by marine biogenic emissions could be responsible for the seasonal increase in the dust iron solubility observed in the Austral fall.

In the context of climate change with increasingly pronounced impacts, year 2022 in France has been the warmest year ever observed. It has been the case more specifically during July, when a severe heatwave occurred across North-Western Europe. Sea-level temperature anomalies jumped over +12°C, especially in the Western half of France, pushing back all-time records. Associated to extreme temperature occurred a severe drought, with long-lasting precipitation deficit throughout the year, which was amplified during July. With around 80% deficit, July 2022 in France has also been the driest ever recorded. These singular meteorological conditions were therefore a fertile ground for forest fires. Around 70 000 ha of forest have burned in France during 2022. The South-West region has been particularly impacted during July 2022, as well as other areas which are not usually subject to this kind of events (Brittany, Center, Paris region). During July 2022 occurred the ACROSS field campaign within the Paris region, where several sites following a South-West to North-East transect provided comprehensive characterization of atmospheric composition. Namely Rambouillet station (forest, SW of Paris), SIRTA (peri-urban, SW of Paris), PRG (urban, Paris center) and Chatelet Les Halles (urban, Paris center). These sites were equiped with state-of-the-art instrumentations to characterize aerosols and reactive gases. On July 19th, an intense biomass burning plume went through the Paris region, with PM10 concentrations reaching more than 150µg/m3. The experimental effort during that period is therefore a unique asset in order to characterize the composition of this episode. Most of the sites, during that episode, record high concentrations of carbonaceous aerosols (organic matter and black carbon) and Volatile Organic Compounds tracers of biomass burning (eg acetonitrile, benzene, toluene). Temporality of the episode, atmospheric dynamics and air mass pathways, suggest the transport of a biomass burning plume from South-Western France, more than 600km away from Paris. However, aerosol size distribution surpringly reveals the influence of local fires occuring near some of the sites, at almost the same time. This work is therefore focusing on the different properties of different plumes mixing at the same time over a densely urbanized region. These differences can be highlighted by source apportionment, combined with size distribution, as well as oxydation state of organic aerosols.

ACROSS is an extensive field campaign that was conducted over the greater Paris region in summer 2022 to study the interaction between the urban pollution plume and biogenic volatile organic compounds emitted from the surrounding forests. This is mainly done by synergism of in-situ ground-based and airborne observations of the composition of the atmosphere (Cantrell and Michoud, 2022). Satellite observations are complementary to these measurements, providing a regional and continental framework of the atmospheric composition.In this study, we present new satellite observations of the 3D distribution of anthropogenic and natural atmospheric aerosols over France during the ACROSS campaign. For this, we use a so-called AEROS5P approach which derives vertical profiles of aerosol extinction for each cloud free TROPOspheric Monitoring Instrument (TROPOMI) pixel using hyperspectral top of atmosphere (TOA) reflectance measurements in the visible and near infrared. This method uses a priori knowledge on particle properties, such as their size and refractive index, along with meteorological parameters from meteorological analyses (ECMWF), surface albedo properties, and a unique a priori aerosol vertical profile. The initial version of AEROS5P was able to monitor the 3D distribution of biomass burning aerosols over Australia, which is a single aerosol type (Lemmouchi et al., 2022).In this study, we present a new version of AEROS5P for deriving the 3D distribution of several aerosol types present in the same atmospheric scene, from both anthropogenic and natural origins. This is done by taking for each TROPOMI pixel the co-localised aerosol type from the VIIRS aerosol product and then processing it with an associated aerosol model of microphysical and optical properties. These aerosol properties are taken from an AERONET sun photometer inversion climatology (Dubovik et al., 2002). This new multi aerosol type AEROS5P method is used for studying dust transport from North Africa, urban pollution from the Paris region, and smoke aerosol transport from South France during the ACROSS campaign. These results are compared against total aerosol extinction from MODIS, vertical aerosol backscatter from CALIOP, airborne and ground-based measurements of aerosol composition, optical and microphysical properties performed in the framework of ACROSS.ReferencesCantrell, Christopher, and Vincent Michoud. "An Experiment to Study Atmospheric Oxidation Chemistry and Physics of Mixed Anthropogenic–Biogenic Air Masses in the Greater Paris Area." Bulletin of the American Meteorological Society 103.8 (2022): 599-603.Dubovik, Oleg, et al. "Variability of absorption and optical properties of key aerosol types observed in worldwide locations." Journal of the atmospheric sciences 59.3 (2002): 590-608Lemmouchi, Farouk, et al. "Three-Dimensional Distribution of Biomass Burning Aerosols from Australian Wildfires Observed by TROPOMI Satellite Observations." Remote Sensing 14.11 (2022): 2582.

Massive amounts of desert dust uplifted over the Sahara are exported over the North Atlantic. They play a major environmental role over this region, impacting the Earth radiative budget, atmospheric dynamics and thermodynamics, cloud properties, atmospheric composition, and biogeochemistry. These multiple impacts of Saharan dust can also affect the evolution of mesoscale convective systems (MCS) formed over West Africa that may lead to the formation of tropical cyclones over the North Atlantic. A better understanding of these aspects, also influenced by African Easterly waves, is the primary objective of the “Clouds-Atmospheric Dynamics-Dust Interactions in West Africa - CADDIWA ” field experiment that took place on September 2021. The current presentation will provide a comprehensive description of the three-dimensional (3D) distribution of Saharan dust and its pathways of export over the North Atlantic during CADDIWA. This will be analysed with respect to the location and evolution of the MCS travelling over the region. This characterisation will be done using a suite of observations which will be compared with dust simulations. The objective is to analyse the difference in terms of abundance and 3D distribution of dust between the cases where MCSs lead to cyclogenesis and those not evolving that way.The ensemble of datasets describing the Saharan dust distribution will be inter-compared and their consistency verified. Twice-daily satellite thermal infrared hyperspectral measurements from IASI will be used to document the 3D distribution of desert dust for cloud-free conditions using the AEROIASI approach (Cuesta et al., 2015; 2020). Further details will be provided by nadir-pointing lidar measurements from AEOLUS and CALIOP space sensors, and from the RALI airborne instruments, in terms of transects of aerosol profiles and winds. In addition to aerosol backscatter profiles, AEOLUS and LNG-RALI will provide aerosol extinction profiles, provided their high spectral resolution capabilities. Observations from MODIS and VIIRS of aerosol optical depth will inform on the horizontal distribution of desert dust. Airborne in situ measurements of the size distribution and intensive optical properties of desert dust, such as the angstrom exponent, will be compared to those used as a priori properties of dust within the satellite dust retrievals (particularly for IASI). These satellite and airborne measurements will be confronted with simulations from the Meso-NH and WRF-CHIMERE, contributing with an all-sky and hourly 3D description.

Organic aerosol (OA) from natural or anthropogenic origin can be directly emitted into the atmosphere (primary organic aerosols, POA) or formed by secondary processes via the oxidation of volatile organic compounds (VOC). However, the formation pathways and their chemical composition of these secondary organic aerosols (SOA), which may contribute up to 90% of the OA mass, are not well understood to date, which is problematic due to the relevance of SOA on climate. To address this issue, this study uses a tracer-based approach to identify and quantify the contribution of different anthropogenic/biogenic VOCs precursors to the SOA formation. To do so, we combine experiments in a large scale atmospheric simulations chamber, CESAM (which means Multiphase Atmospheric Experimental Simulation Chamber), and field measurements during the ACROSS (Atmospheric ChemistRy Of the Suburban foreSt) campaign conducted in the Paris area in summer 2022. This approach provides both a mechanistic study of the oxidation of targeted VOCs in simulated and controlled rural/urban atmospheres and the identification of targeted tracers in the real atmosphere, to quantify their concentrations in ambient air.The ACROSS dataset consists in atmospheric samples of submicron aerosols collected twice a day (day and night) in the urban area of Paris and the Rambouillet forest on the south-west of Paris, as well as samples collected onboard the Safire ATR-42 research aircraft on low-level flights targeting the evolution and dilution of the Paris urban plume. The CESAM chamber dataset consists in samples of SOA generated by the OH oxidation of toluene/ m-xylene in various conditions.Filters are analyzed to provide with the chemical composition at the molecular scale by SFE-GC-MS (Supercritical Fluid Extraction Gas Chromatography- Mass Spectrometry) and UPLC-QTOF-MS (Ultra Performance Liquid Chromatography Time of Flight Mass Spectrometry). The organic mass and chemical speciation are obtained by aerosol mass spectrometry and the organic carbon (OC) concentrations by thermal-optical analysis.The first results of the ambient samples of Paris revealed that the OC concentration varied between 0.69 ± 0.07 and 9.48 ± 0.51 µgC/m3, which correspond to the 28% and 53% of the total mass of the submicron aerosols, for background and polluted (fire) conditions, respectively. These diverse conditions are favorable to trace the compounds identified during the simulation chamber experiments, such as benzoic acid, succinic acid, and 2-methyl-4-nitrophenol. These attempts will be presented and discussed in order to determine the contribution of specific precursors to SOA formation.

The ACROSS campaign (Atmospheric chemistry of the suburban forest) is a collaborative effort to better understand how the mixing between urban and biogenic air masses impacts atmospheric composition and reactivity. A main objective is to provide a detailed description of physico-chemical processes involved in atmospheric transformations of biogenic Volatile Organic Compounds (VOCs), and the myriad of intermediate species formed as a consequence, which have yet to be characterized. This multi-platform campaign took place during summer 2022 for a duration of 6 weeks and included a supersite in the Rambouillet forest located on the path of pollution plumes from Paris. An unprecedented suite of analytical instruments was deployed at this site to probe air masses at the ground level and above the forest canopy using a 40-m tower.This presentation will focus on trace gas observations, including VOCs, ROx (OH+HO2+RO2) and selected inorganic species (O3, NOx – NO+NO2), both above and below the forest canopy. A descriptive analysis will be presented to highlight biogenic VOC oxidation regimes taking place under unpolluted (oceanic air masses) and polluted (Paris plumes) conditions, with a focus on primary/secondary species. Chemical compositions observed above and below-canopy will also be contrasted. On the basis of these observations, this presentation will highlight scientific questions related to ROx, VOC and NOx budgets that will be further investigated to fill important gaps in our understanding of biogenic VOC transformations and secondary organic aerosol formation. Acknowledgments. This work is supported by the French national research agency (ANR-20-CE01-0010) & LABEX-CaPPA (ANR-11-LABX-005-01) and the French national program LEFE/CHAT INSU.

Atmospheric simulation chambers are often utilized to study the physical properties and chemical reactivity of particles suspended in air. In this chapter, the various approaches employed for the addition of particles to simulation chambers are described in detail. Procedures for the generation of monodispersed seed aerosols, mineral dust, soot particles and bioaerosols are all presented using illustrative examples from chamber experiments. Technical descriptions of the methods used for the addition of whole emissions (gases and particles) from real-world sources such as wood-burning stoves, automobile engines and plants are also included, along with an outline of experimental approaches for investigating the atmospheric processing of these emissions.

The Mediterranean atmosphere is impacted by a variety of natural and anthropogenic aerosols which exert a complex and variable pressure on the regional climate and air quality. This study focuses on the Western Mediterranean Sea (west of longitude 20∘ E) using the full POLarization and Directionality of the Earth's Reflectances version 3 (POLDER-3)/Polarization & Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL) aerosol data record derived from the operational clear-sky ocean algorithm (collection 3) available from March 2005 to October 2013. This 8.5-year satellite data set includes retrievals at 865 nm of the total, fine-, and coarse-mode aerosol optical depth (AOD, AODF, and AODC, respectively), Ångström exponent (AE), and the spherical/non-spherical partition of the coarse-mode AOD (AODCS and AODCNS, respectively), that have been carefully validated over the study region (Formenti et al., 2018). Here, we analyze the spatial distribution, the seasonal cycle, and interannual variability of this ensemble of advanced aerosol products in three latitude bands (34–38, 38–42, and > 42∘ N) and for three sites (Ersa, Barcelona, Lampedusa) distributed on the western basin. POLDER-3 retrieves the high influence of north African desert dust over the region, which largely controls the spatial distributions (south-to-north decreasing gradient) and seasonal cycles (spring/summer maximum) of both AOD and coarse AOD, including its non-spherical component. In contrast, the coarse spherical component of AOD remains relatively homogenously low all year long over the region, whereas fine-mode AODs are generally more elevated in the eastern part of the region of study, especially north of the Adriatic Sea. From 2005 to 2013, annual POLDER-3 AOD evolution shows a decreasing trend of 0.0030 yr−1 in absolute value at 865 nm (0.0060 yr−1 at 550 nm). Such a downward evolution is much more pronounced and spatially extended for AODF (−0.0020 yr−1 at 865 nm) than for AODC. Our analysis also suggests that the North Atlantic Oscillation (NAO) index explains a significant part of the interannual variability of POLDER-3 AODC, reflecting its role on the frequency of Saharan dust transport over the region. Finally, the POLDER-3 data set highlights an improvement of air quality related to the fine aerosol component, with a marked evolution toward more frequent occurrence of clean conditions (≥ 75 % of daily AODF-865 nm.05) at the end of the period of study (2010–2013) over most of the Western Mediterranean Sea, and much less evidence of such a large-scale evolution for the coarse fraction. Therefore, despite the high and variable influence of mostly natural north African dust over the region, the POLDER-3 advanced aerosol data set appears sufficiently accurate to successfully resolve the concurrent downward trend of fine, primarily anthropogenic particles, most likely related to reduced emissions in the surrounding European countries.

Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that are chemically complex, thus making it difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models, utilizing a suite of airborne measurements from the ORACLES 2018 campaign. An effective refractive index of black carbon (BC), meBC=1.95+ikeBC, that characterizes the absorptivity of all absorbing components at 660 nm wavelength was introduced to facilitate the attribution of absorption at shorter wavelengths, i.e. 470 nm. Most values of the imaginary part of the effective refractive index, keBC, were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers besides BC at 660 nm. The TEM-EDX single-particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of keBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (RBrC,470) ranges from ∼8 %–22 %, with the organic aerosol mass absorption coefficient (MACOA,470) at this wavelength ranging from 0.30±0.27 to 0.68±0.08 m2 g−1. The core–shell model yielded much higher estimates of MACOA,470 and RBrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Absorption attribution using the Bruggeman mixing Mie model suggests a minor BrC contribution of 4 % at 530 nm, while its removal would triple the BrC contribution to the total absorption at 470 nm obtained using the AAE (absorption Ångström exponent) attribution method. Thus, it is recommended that the application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC and to account for potential contributions from other absorbing materials.

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

Iceland is a highly active source of natural dust. Icelandic dust has the potential to directly affect the climate via dust–radiation interaction and indirectly via dust–cloud interaction, the snow/ice albedo effect and impacts on biogeochemical cycles. The impacts of Icelandic dust depend on its mineralogical and chemical composition. However, a lack of data has prevented an accurate assessment of the role of Icelandic dust in the Earth system. Here, we collected surface sediment samples from five major Icelandic dust hotspots. Dust aerosols were generated and suspended in atmospheric chambers, and PM10 and PM20 fractions were collected for further analysis. We found that the dust samples primarily consist of amorphous basaltic materials ranging from 8 wt % (from the Hagavatn hotspot) to 60 wt %–90 wt % (other hotspots). Samples had relatively high total Fe content (10 wt %–13 wt %). Sequential extraction of Fe to determine its chemical form shows that dithionite Fe (Fe oxides such as hematite and goethite) and ascorbate Fe (amorphous Fe) contribute respectively 1 %–6 % and 0.3 %–1.4 % to the total Fe in Icelandic dust. The magnetite fraction is 7 %–15 % of total Fe and 1 %–2 wt % of PM10, which is orders of magnitude higher than in mineral dust from northern Africa. Nevertheless, about 80 %–90% of the Fe is contained in pyroxene and amorphous glass. The initial Fe solubility (ammonium acetate extraction at pH 4.7) is from 0.08 % to 0.6 %, which is comparable to low-latitude dust such as that from northern Africa. The Fe solubility at low pH (i.e. pH 2) is significantly higher than typical low-latitude dust (up to 30 % at pH 2 after 72 h). Our results revealed the fundamental differences in composition and mineralogy of Icelandic dust from low-latitude dust. We attribute these differences to the low degree of chemical weathering, the basaltic composition of the parent sediments and glacial processes. Icelandic dust contributes to the atmospheric deposition of soluble Fe and can impact primary productivity in the North Atlantic Ocean. The distinct chemical and mineralogical composition, particularly the high magnetite content (1 wt %–2 wt %), indicates a potentially significant impact of Icelandic dust on the radiation balance in the subpolar and polar regions.

EUFAR (EUropean Facility for Airborne Research, https://www.eufar.net) was born out of the necessity to create a central network for the airborne research community in Europe with the principal aim of supporting scientists, by granting them access to research aircraft and instruments otherwise not accessible in their home countries. With time EUFAR has grown, introducing new activities and objectives to place itself as the unique network and portal of airborne research for the environmental and geosciences in Europe. From serving as an interactive and dynamic hub of information, to maintaining a central data archive, and developing tools and standards to collect, process and analyse data, EUFAR continues to improve the operational environment for conducting airborne research. EUFAR's data archive activity seeks to improve access to and use of the data collected by instrumented aircraft in Europe, providing a unique portal to the data along with supporting metadata. AERIS, the French Data and Services Cluster for Atmosphere (https://en.aeris-data.fr) has implemented a new Data and Metadata Catalogue for EUFAR that in the longer term is intended to become a principal data portal for the European airborne science community. All EUFAR datasets are following the FAIR principles. The main features of the catalogue, i.e. data and metadata discovery and download, have been improved. Advanced services have been implemented such as the discovery of external datasets from EUFAR partners starting with the French Research Airborne Data Portal SAFIRE+. This will be extended to other databases in 2022 such as DLR, NERC-ARF, FAAM, Met Office, etc. New advanced features are currently under development: discovery of datasets from other airborne Research Infrastructures (IAGOS, HEMERA, etc.); data visualization services; integration of the EUFAR products and services in EOSC (European Open Science Cloud); tools for the management of campaigns metadata, etc.

Aerosol aware microphysics parameterisation schemes are increasingly being introduced into numerical weather prediction models, allowing for regional and case specific parameterisation of cloud condensation nuclei (CCN) and cloud droplet interactions. In this paper, the Thompson aerosol aware microphysics scheme, within the Weather, Research and Forecasting (WRF) model, is parameterised for two fog cases during September 2017 over Namibia. Measurements of CCN and fog microphysics were undertaken during the Aerosol, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign at Henties Bay on the coast of Namibia during September 2017. A key concept of the microphysics scheme is the conversion of water friendly aerosols to cloud droplets (hereafter referred to as CCN activation), which could be estimated from the observations. A fog monitor 100 (FM100) provided cloud droplet size distribution, number concentration (Nt), liquid water content (LWC) and mean volumetric diameter (MVD). These measurements are used to evaluate and parameterise WRF model simulations of Nt, LWC and MVD. A sensitivity analysis was conducted through variations to the initial CCN concentration, CCN radius and the minimum updraft speed, important factors that influence droplet activation in the microphysics scheme of the model. The first model scenario made use of the default settings with a constant initial CCN number concentration of 300 cm-3 and underestimated the cloud droplet number concentration while the LWC was in good agreement with the observations. This resulted in droplet size being larger than the observations. Another scenario used modelled data as CCN initial conditions which were an order of magnitude higher than other scenarios. However, these provided the most realistic values of Nt, LWC, MVD and droplet size distribution. From this it was concluded that CCN activation of around 10 % in the simulations is too low, while the observed appears to be higher reaching between with a mean (median) of 0.55 (0.56) during fog events. To achieve this level of activation in the model, the minimum updraft speed for CCN activation was increased from 0.01 to 0.1 ms-1. This scenario provided Nt, LWC, MVD and droplet size distribution in the range of the observations with the added benefit of a realistic initial CCN concentration. These results demonstrate the benefits of a dynamic aerosol aware scheme when parameterised with observations.

This study reports the only recent characterization of two contrasted wet deposition events collected during the PEACETIME (ProcEss studies at the Air–sEa Interface after dust deposition in the MEditerranean Sea) cruise in the open Mediterranean Sea (Med Sea) and their impact on trace metal (TM) marine stocks. Rain samples were analysed for Al, 12 TMs (Co, Cd, Cr, Cu, Fe, Mn, Mo, Ni, Pb, Ti, V and Zn) and nutrient (N, P, dissolved organic carbon) concentrations. The first rain sample collected in the Ionian Sea (Rain ION) was a typical regional background wet deposition event, whereas the second rain sample collected in the Algerian Basin (Rain FAST) was a Saharan dust wet deposition event. Even in the remote Med Sea, all background TM inputs presented an anthropogenic signature, except for Fe, Mn and Ti. The concentrations of TMs in the two rain samples were significantly lower compared to concentrations in rains collected at coastal sites reported in the literature, due to the decrease in anthropogenic emissions during the preceding decades. The atmospheric TM inputs were mainly dissolved forms, even in dusty Rain FAST. The TM stocks in the mixed layer (ML, 0–20 m) at the FAST station before and after the event showed that the atmospheric inputs were a significant supply of particulate TMs and dissolved Fe and Co for surface seawater. Even if the wet deposition delivers TMs mainly in soluble form, the post-deposition aerosol dissolution could to be a key additional pathway in the supply of dissolved TMs. At the scale of the western and central Mediterranean, the atmospheric inputs were of the same order of magnitude as ML stocks for dissolved Fe, Co and Zn, highlighting the role of the atmosphere in their biogeochemical cycles in the stratified Med Sea. In case of intense dust-rich wet deposition events, the role of atmospheric inputs as an external source was extended to dissolved Co, Fe, Mn, Pb and Zn. Our results suggest that the wet deposition constitutes only a source of some of dissolved TMs for Med Sea surface waters. The contribution of dry deposition to the atmospheric TM inputs needs to be investigated., This study is a contribution to the PEACETIME project (http://peacetime-project.org; last access: 5 April 2021), a joint initiative of the MERMEX and ChArMEx programmes supported by CNRS-INSU, IFREMER, CEA and Météo-France as part of the decadal meta-programme MISTRALS coordinated by CNRS-INSU.

This study characterizes single-particle aerosol composition from filters collected during the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) and CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017 (CLARIFY-2017) campaigns. In particular the study describes aged biomass burning aerosol (BBA), its interaction with the marine boundary layer and the influence of biomass burning (BB) air on marine aerosol. The study finds evidence of BBA influenced by marine boundary layer processing as well as sea salt influenced by BB air. Secondary chloride aerosols were observed in clean marine air as well as in BB-influenced air in the free troposphere. Higher-volatility organic aerosol appears to be associated with increased age of biomass burning plumes, and photolysis or oxidation may be a mechanism for the apparent increased volatility. Aqueous processing and interaction with the marine boundary layer air may be a mechanism for the presence of sodium on many aged potassium salts. By number, biomass burning potassium salts and modified sea salts are the most observed particles on filter samples. The most commonly observed BC coatings are inorganic salts. These results suggest that atmospheric processes such as photolysis, oxidation and cloud processing are key drivers in the elemental composition and morphology of aged BBA. Fresh BBA inorganic salt content, as it has an important role in the particles' ability to uptake water, may be a key driver in how aqueous processing and atmospheric aging proceed.

International audience; This commentary paper from the recently formed International Global Atmospheric Chemistry (IGAC) Southern Hemisphere Working Group outlines key issues in atmospheric composition research that particularly impact the Southern Hemisphere. In this article, we present a broad overview of many of the challenges for understanding atmospheric chemistry in the Southern Hemisphere, before focusing in on the most significant factors that differentiate it from the Northern Hemisphere. We present sections on the importance of biogenic emissions and fires in the Southern Hemisphere, showing that these emissions often dominate over anthropogenic emissions in many regions. We then describe how these and other factors influence air quality in different parts of the Southern Hemisphere. Finally, we describe the key role of the Southern Ocean in influencing atmospheric chemistry and conclude with a description of the aims and scope of the newly formed IGAC Southern Hemisphere Working Group.

Mineral dust particles suspended in the atmosphere span more than three orders of magnitude in diameter, from

Optical particle counters (OPC) are widely used to measure the aerosol particle number size distribution at atmospheric ambient conditions and over a large size range. Their measurement principle is based on the dependence of light scattering on particle size. However, this dependence is not monotonic at all sizes and light scattering also depends on the particle composition (i.e., the complex refractive index, CRI) and morphology. Therefore, the conversion of the measured scattered intensity to the desired particle size depends on the microphysical properties of the sampled aerosol population and might not be unique at all sizes. While these complexities have been addressed before, corrections are typically applied ad-hoc and are not standardised. This paper addresses this issue by providing a consistent and extended database of pre−computed correction factors for a wide range of complex refractive index values representing the composition variability of atmospheric aerosols. These correction factors are calculated for five different commercial OPCs (USHAS, PCASP, FSSP, GRIMM and its airborne version Sky− GRIMM, CDP) by assuming Mie theory for homogeneous spherical particles, and by varying the real part of the CRI between 1.33 and 1.75 in steps of 0.01 and the imaginary part between 0.0 and 0.4 in steps of 0.001. Correction factors for mineral dust are provided at the CRI of 1.53 – 0.003i and account for the asphericity of these particles. The datasets described in this paper are distributed at open-access repository: https://doi.org/10.25326/234 (license CC BY, Formenti et al., 2021) maintained by the French national center for Atmospheric data and services AERIS to data users/geophysicists who number size distribution measurements from OPC for their research on atmospheric aerosols. Application and caveats of the CRI-corrections factors are presented and discussed. The dataset presented in this paper is not only useful for correcting the size distribution from an OPC when the particle refractive index is known, but even when only assumptions can be made. Furthermore, this dataset can be useful in calculating uncertainties or sensitivities of aerosol volume/mass/extinction from OPCs given no or limited knowledge of refractive index.

The formation of a river of smoke crossing southern Africa is 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, a high-pressure system over the continent and westerly waves in 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 temperate tropical 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 southwestern Indian Ocean.