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Understanding ocean-cloud interactions and their effect on climate requires that atmospheric new particle formation is characterized. Yet, the process of particle formation from marine biogenic gaz-phase emissions has not been evidenced in the open ocean lower atmosphere, partly due to the naturally low concentrations of these particles in remote oceanic places. Here we show, using new ship-borne air-sea interface enclosures, that new particles are formed in relation to marine micro-biology present in the seawater. The chemical analysis of newly formed clusters with API-ToF-MS shows unexpected results, implicating nucleating coumpounds and pathways that are usually not taken into account in nucleation processes.

The study of marine aerosols size distribution and cloud condensation nuclei (CCN) properties is of major interest as they influence clouds life and clouds radiative properties, particularly in the remote ocean which remains poorly documented. Several short campaigns focusing on specific regions as phytoplankton bloom regions, pristine regions or remote areas influenced by continental air masses took place to address this issue. However, long sampling periods targeting different in-situ conditions had not been realized. In this context, the MAP-IO program was launched with the aim of providing a large new set of marine aerosol observations (size distribution from 10 nm to 10 µm and CCN properties) on different sea state and meteorological conditions. Thus, the Marion Dufresne vessel has been equipped with a set of various instruments described in Tulet et al. (in preparation) or on the website www.mapio.re. Two years after the launch of the program, we now have aerosol observations (about 200 days) over an area covering 50 ° of latitudes and extending from the Tropics to the upper Southern Ocean. These measurements were first used to investigate the size distribution and CCN variability of marine aerosols according to local conditions (sea states and wind speed).The results highlight that at the lowest latitudes (south of 50 °S) the minimum concentration of CCN tends to increase when the wind speed exceeds approximately 12 m s-1, which is consistent with the literature as sea salt emissions are mechanically driven by local conditions and tend to be predominant from 10 m s-1. .When analyzing the size distributions of aerosols according to the wind speed during a 5-day storm that occurred in the Southern Ocean, we found that: (1) the number of particles with a diameter less than 500 nm is predominant and stable over the full range of wind speeds (4 to 33 m s-1), (2) the number of aerosols with diameter greater than 500 nm remains low under 10 m s-1 and increases from 10 m s-1 to 33 m s-1 to finally reach the concentration of the particles with diameter less than 500 nm at 33 m s-1. Taking this first analysis into account, further work will focus on average size distributions per region, season, origin of air masses (from simulated FLEXPART back trajectories) and wind speed conditions. Analysis of these distributions is unique due to the size of the database, the variability of regions encountered and knowing that the measurements were carried out with the same experimental device. Finally, to deepen the study, the activation diameter of marine aerosols will be determined and the hygroscopicity parameter Kappa-Köhler will be calculated (Petters and Kreidenweis, 2007) in this case to distinguish sea salts (Kappa~1.2) from organic matter (0.01

Air-sea fluxes of dimethyl sulphide (DMS) and methanethiol (MeSH) from surface seawater in the remote Southern Pacific Ocean were measured in three Air-Sea Interface Tank (ASIT) experiments during the Sea2Cloud voyage in March 2020. The measured fluxes of 0.78 ± 0.44 ng m-2 s-1 and 0.05 ± 0.03 ng m-2 s-1 for DMS and MeSH, respectively, varied between experiments reflecting the different water mass types investigated, with lowest fluxes with subtropical water and highest with biologically-active water with sub-Tropical water and highest from the sub-Tropical Front. Measured DMS fluxes were consistent with calculated fluxes from a two-layer model using DMS concentration in the ASIT seawater. The experiments also determined the influence of elevated ozone, with one ASIT headspace amended with 10 ppbv ozone while the other provided an unamended control. Elevated ozone resulted in a decrease in DMS flux, corresponding to decreased conversion of dimethylsulfoniopropionate (DMSP) to DMS in the seawater. The MeSH:DMS flux range was 11–18 % across experiments, in line with previous observations, indicating that MeSH represents a significant contribution to the atmospheric sulfur budget. Using the ASIT results in combination with ambient seawater concentrations during Sea2Cloud, significant linear correlations were identified for both DMS and MeSH fluxes with nanophytoplankton cell abundance (rDMS= 0.73 and rMeSH= 0.86), indicating an important role for this phytoplankton size class, and also its potential as a proxy for estimating DMS and MeSH emissions in chemistry-climate models.

Terrestrial volcanism is known to emit mercury (Hg) into the atmosphere. However, despite many years of investigation, its net impact on the atmospheric Hg budget remains insufficiently constrained, in part because the transformations of Hg in volcanic plumes as they age and mix with background air are poorly understood. Here we report the observation of complete gaseous elemental mercury (GEM) depletion events in dilute and moderately aged (~3-7 hours) volcanic plumes from Piton de la Fournaise on Réunion Island. While it has been suggested that co-emitted bromine could, once photochemically activated, deplete GEM in a volcanic plume, we measured low bromine concentrations in both the gas- and particle phase and observed complete GEM depletion even before sunrise, ruling out a leading role of bromine chemistry here. Instead, we hypothesize that the GEM depletions were mainly caused by gas-particle interactions with sulfate-rich volcanic particles (mostly of submicron size), abundantly present in the dilute plume. We consider heterogeneous GEM oxidation and GEM uptake by particles as plausible manifestations of such a process and derive empirical rate constants. By extrapolation, we estimate that volcanic aerosols may scavenge 210 Mg y-1 (67 – 480 Mg y-1) of Hg from the atmosphere globally, acting effectively as atmospheric mercury sink. While this estimate is subject to large uncertainties, it highlights that Hg transformations in aging volcanic plumes must be better understood to determine the net impact of volcanism on the atmospheric Hg budget and Hg deposition pathways.

The sea surface microlayer (SSML) is critical to air-sea exchanges of gases and primary aerosols. However, despite the extent of this boundary layer, little is known about its specific bacterial community (bacterioneuston) and how it may affect ocean-atmosphere exchanges. Here, we studied the bacterial community composition in the surface waters of three different basins of the Western Mediterranean Sea and assessed the selective air-sea transfer of marine bacteria through experimental nascent sea spray aerosol production in a 10 L tank with plunging jets. In situ, the bacterioneuston harbored basin-specific enriched taxa and followed a similar spatial pattern as the underlying bacterioplankton community. Aerosolization potential showed that sea spray taxa might be recruited from both the underlying water and the SSML, and that taxa enriched in the bacterioneuston were not always aerosolized. Our results suggest that the Mediterranean nutrient gradient, as well as pulse events such as dust deposition, affect the distribution of the bacterial community at the ocean-atmosphere interface, which may impact biogeochemical processes, climate regulation and bacterial dispersal through aerosolization.

Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at Chacaltaya Global Atmosphere Watch station in Bolivia (5240 m a.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign . The simulations showed that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modelled and measured particle growth rates. This study gives an insight on the key factors affecting the particle growth on the site. Low volatile organic compounds were found to be the main contributor to the particle growth, covering on average 65 % of simulated particle mass in particle with diameter of 40 nm In addition, sulfuric acid had a major contribution to the particle growth, covering at maximum 39 % of simulated particle mass in 40 nm particle during periods when volcanic activity was detected on the area, suggesting that volcanic emissions can greatly enhance the particle growth.

Future change in sea surface temperature may influence climate via various air-sea feedbacks and pathways. In this study, we investigate the influence of surface seawater biogeochemical composition on the temperature dependence of sea spray number emission fluxes. Dependence of sea spray fluxes was investigated in different water masses (i.e. subantarctic, subtropical and frontal bloom) with contrasting biogeochemical properties across a temperature range from ambient (13–18 °C) to 2 °C, using seawater circulating in a plunging jet sea spray generator. We observed sea spray total concentration to increase significantly at temperatures below 8 °C, with an average 4-fold increase at 2 °C relative to initial concentration at ambient temperatures. This temperature dependence was more pronounced for smaller size sea spray particles (i.e. nucleation and Aitken modes). Moreover, temperature dependence varied with water mass type and so biogeochemical properties. While the sea spray flux at moderate temperatures (8–11 °C) was highest in frontal bloom waters, the effect of low temperature on the sea spray flux was highest with subtropical seawaters. The temperature dependence of sea spray flux was also inversely proportional to the seawater cell abundance of the cyanobacterium Synechococcus, which facilitated parameterization of temperature dependence of sea spray emission fluxes as a function of Synechococcus for future implementation in modelling exercises.

Benzene, toluene, ethylbenzene and xylenes can contribute to hydroxyl reactivity and secondary aerosol formation in the atmosphere. These aromatic hydrocarbons are typically classified as anthropogenic air pollutants, but there is growing evidence of biogenic sources, such as emissions from plants and phytoplankton. Here we use a series of shipborne measurements of the remote marine atmosphere, seawater mesocosm incubation experiments and phytoplankton laboratory cultures to investigate potential marine biogenic sources of these compounds in the oceanic atmosphere. Laboratory culture experiments confirmed marine phytoplankton are a source of benzene, toluene, ethylbenzene, xylenes and in mesocosm experiments their sea-air fluxes varied between seawater samples containing differing phytoplankton communities. These fluxes were of a similar magnitude or greater than the fluxes of dimethyl sulfide, which is considered to be the key reactive organic species in the marine atmosphere. Benzene, toluene, ethylbenzene, xylenes fluxes were observed to increase under elevated headspace ozone concentration in the mesocosm incubation experiments, indicating that phytoplankton produce these compounds in response to oxidative stress. Our findings suggest that biogenic sources of these gases may be sufficiently strong to influence atmospheric chemistry in some remote ocean regions. A group of aromatic hydrocarbons in the remote marine atmosphere, typically classified as anthropogenic pollutants, are attributable to local biogenic sources, according to shipborne observations and mesocosm experiments.

To reduce uncertainties in climate predictions, we need to better understand aerosol formation in different environments. An important part of this is studying which chemical species are responsible for particle formation. While many advances have been made in this field, measurements are especially lacking from marine environments. Here, we measured the chemical composition of ambient anions over 7 months at Baring Head station, located in coastal New Zealand. This adds to our previous work which reported the aerosol size distribution measurements and investigated new particle formation and environmental conditions favouring new particle formation at the station. By combining the information on ion chemical composition with our previous work, we were able to study the chemical precursors of new particle formation. Our results showed that while over land new particle formation is likely driven by sulfuric acid and organic species, in clean marine air iodine oxoacids and sulfur species are likely important drivers of particle formation processes. These data were also used to characterise the diurnal and seasonal cycles of the most important anion groups and their geographical source regions. Bisulfate anions displayed a clear daytime maximum where as iodine oxoacids had morning and evening maximums. Highly oxygenated organic molecules, on the other hand, were most abundant during the night when the air was land-influenced. This data set is highly valuable and our results provide important information on the chemical species driving new particle formation at a remote Southern Hemisphere coastal site.

Climate model simulations of cloud radiative properties over the Southern Ocean (SO) show that clouds reflect too little solar radiation compared with observations. This results in large errors in the modelled sea surface temperature, atmospheric circulation and climate sensitivity. Low-level (LL) mixed-phase clouds (MPCs) in the cold sectors of extratropical cyclones are identified as the main contributor to the SO radiation bias.In this study, LL clouds are investigated between 40°S and 82° S to provide a new insight into their geographical distribution, as well as their spatial and temporal variabilities. The methodology relies on DARDAR products which exploits the synergy of CALIPSO's lidar and CloudSat's radar space-borne remote sensing observations. Based on DARDAR cloud-type products, a cloud classification program was developed to establish cloud spatial and temporal distributions. This study concerns all types of cloud, including MPCs and supercooled-water containing clouds. The mean seasonal LL cloud cover for 2007-2010 over oceans (including sea-ice) varies from 64.4% in winter to 68.4% in fall. Larger cloud covers are observed between 50°S and 65°S where clouds are present more than 80% of the time. Dividing the studied area into smaller regions allowed to extract homogeneous sectors in term of cloud coverage. This analysis draw attention on some regions, such as the Tasman Sea sector that undergoes the highest seasonal variations for MPC and USLC occurrence, and the Argentinian coasts that presents important differences with other regions at the same latitudes. Over the Southern Ocean, the Weddell Sea sector stands out with a relatively low LL cloud occurrence.Statistical analyses were carried out to determine the influence of the meteorological and biological conditions on cloud occurrence. Even though air temperature drives all cloud-type occurrences, it was found that the lower-tropospheric stability (LTS) is a good predictor of ice-cloud occurrence between 40°S and 50°S, particularly. With biological activity, first results indicate strong correlations with cloud occurrence, where chlorophyll-a, nanophytoplankton and particulate organic carbon concentrations are investigated between 40°S and 60°S.

We investigated the role of the passive volcanic plume of Mount Etna (Italy) in the formation of new particles in the size range of 2.5–10 nm through the gas-to-particle nucleation of sulfuric acid (H2SO4) precursors, formed from the oxidation of SO2, and their evolution to particles with diameters larger than 100 nm. Two simulations were performed using the Weather Research and Forecasting Model coupled with chemistry (WRF-Chem) under the same configuration, except for the nucleation parameterization implemented in the model: the activation nucleation parameterization (JS1 = 2.0 × 10−6 × (H2SO4)) in the first simulation (S1) and a new parameterization for nucleation (NPN) (JS2 = 1.844 × 10−8 × (H2SO4)1.12) in the second simulation (S2). The comparison of the numerical results with the observations shows that, on average, NPN improves the performance of the model in the prediction of the H2SO4 concentrations, newly-formed particles (~2.5–10 nm), and their growth into larger particles (10–100 nm) by decreasing the rates of H2SO4 consumption and nucleation relative to S1. In addition, particles formed in the plume do not grow into cloud condensation nuclei (CCN) sizes (100–215 nm) within a few hours of the vent (tens of km). However, tracking the size evolution of simulated particles along the passive plume indicates the downwind formation of particles larger than 100 nm more than 100 km far from the vent with relatively high concentrations relative to the background (more than 1500 cm−3) in S2. These particles, originating in the volcanic source, could affect the chemical and microphysical properties of clouds and exert regional climatic effects over time.

International audience; This article presents the results of the AEROMARINE field campaign which took place between February and April 2019 off the coast of Reunion Island in the South West Indian Ocean basin. The Southern Indian Ocean is of major interest for the study of marine aerosols, their distribution and variability. Six instrumented light plane flights and a ground-based microwave radiometer were used during the field campaign. These measurements were compared with the long-term measurements of the AERONET sun-photometer (based in St Denis, Reunion Island) and various instruments of the high altitude Maïdo Observatory (2.2 km above sea level, Reunion Island). These results were also analyzed using different model outputs: (i) the AROME mesoscale weather forecast model to work on the thermodynamics of the boundary layer, (ii) the FLEXPART-AROME Lagrangian particle dispersion model to assess the geographical and vertical origin of air masses, and (iii) the chemical transport model CAMS (Copernicus Atmosphere Monitoring Service) to work on the aerosol chemical composition of air masses. This allowed to highlight two points: (1) the atmospheric layer above 1.5 km is mainly composed of aerosols from the regional background; (2) the local environment (ocean or island) has little impact on the measured concentrations. Marine aerosols emitted locally are mostly measured below 0.5 km. The daytime marine aerosol distributions in the free troposphere measured by the aircraft were compared to the night-time aerosol distributions measured at the high altitude Maïdo Observatory when the Observatory is located in the free troposphere. The results indicate that this high altitude site of measurements is representative of the marine aerosol concentrations in the free troposphere. We also found that the CAMS reanalyses overestimated the aerosol optical depth in this region. Finally, our study strongly suggests that the AERONET station in St Denis (Reunion Island) can be considered as a representative marine station under the Tropics.

Even though oceans cover the majority of the Earth, most aerosol measurements are from continental sites. We measured aerosol particle number size distribution at Baring Head, in coastal New Zealand, over a total period of 10 months to study aerosol properties and new particle formation, with a special focus on aerosol formation in open ocean air masses. Particle concentrations were higher in land-influenced air compared to clean marine air in all size classes from sub-10 nm to cloud condensation nuclei sizes. When classifying the particle number size distributions with traditional methods designed for continental sites, new particle formation was observed at the station throughout the year with an average event frequency of 23 %. While most of these traditional event days had some land-influence, we also observed particle growth starting from nucleation mode during 16 % of the data in clean marine air and at least part of this growth was connected to nucleation in the marine boundary layer. Sub-10 nm particles accounted for 29 % of the total aerosol number concentration of particles larger than 1 nm in marine air during the spring. This shows that nucleation in marine air is frequent enough to influence the total particle concentration. Particle formation in land-influenced air was more intense and had on average higher growth rates than what was found for marine air. Particle formation and primary emissions increased particle number concentrations as a function of time spent over land during the first 1–2 days spent over land. After this, nucleation seems to start getting suppressed by the pre-existing particle population, but accumulation mode particle concentration keeps increasing, likely due to primary particle emissions. Further work showed that traditional NPF events were favoured by sunny conditions with low relative humidity and wind speeds. In marine air, formation of sub-10 nm particles was favoured by low temperatures, relative humidity, and wind speeds and could happen even during the night. Our future work will study the mechanisms responsible for particle formation at Baring Head with a focus on different chemical precursor species. This study sheds light on both new particle formation in open ocean air masses coming from the Southern Ocean and local aerosol properties in New Zealand.

Co-auteur étranger; International audience; Volcanic emissions can significantly affect the Earth's radiation budget by emitting aerosol particles and gas‐phase species that can result in the new particle formation (NPF). These particles can scatter solar radiation or modify cloud properties, with consequences on health, weather, and climate. To our knowledge, this is the first dedicated study detailing how gas‐phase precursors emitted from volcanic plumes can influence the NPF. A series of airborne measurements were performed around the Etna and Stromboli volcanoes within the framework of the CLerVolc and STRAP projects. The ATR‐42 aircraft was equipped with a range of instrumentation allowing the measurement of particle number concentration in diameter range above 2.5 nm, and gaseous species to investigate the aerosol dynamics and the processes governing the NPF and their growth within the volcanic plumes. We demonstrate that NPF occurs within the volcanic plumes in the Free Troposphere (FT) and Boundary Layer (BL). Typically, the NPF events were more pronounced in the FT, where the condensational sink was up to two orders of magnitude smaller and the temperature was ~20°C lower than in the BL. Within the passive volcanic plume, the concentration of sulfur dioxide, sulfuric acid, and N2.5 were as high as 92 ppbV, 5.65×108 and 2.4×105 cm–3, respectively. Using these measurements, we propose a new parameterization for NPF rate (J2.5) within the passive volcanic plume in the FT. These results can be incorporated into mesoscale models to better assess the impact of the particle formed by natural processes, i.e. volcanic plumes, on climate.

Ice-nucleating particles (INPs) have a large impact on the climate-relevant properties of clouds over the oceans. Studies have shown that sea spray aerosols (SSAs), produced upon bursting of bubbles at the ocean surface, can be an important source of marine INPs, particularly during periods of enhanced biological productivity. Recent mesocosm experiments using natural seawater spiked with nutrients have revealed that marine INPs are derived from two separate classes of organic matter in SSAs. Despite this finding, existing parameterizations for marine INP abundance are based solely on single variables such as SSA organic carbon (OC) or SSA surface area, which may mask specific trends in the separate classes of INP. The goal of this paper is to improve the understanding of the connection between ocean biology and marine INP abundance by reporting results from a field study and proposing a new parameterization of marine INPs that accounts for the two associated classes of organic matter. The PEACETIME cruise took place from 10 May to 10 June 2017 in the Mediterranean Sea. Throughout the cruise, INP concentrations in the surface microlayer r (INPSML) and in SSAs (INPSSA) produced using a plunging aquarium apparatus were continuously monitored while surface seawater (SSW) and SML biological properties were measured in parallel. The organic content of artificially generated SSAs was also evaluated. INPSML concentrations were found to be lower than those reported in the literature, presumably due to the oligotrophic nature of the Mediter ranean Sea. A dust wet deposition event that occurred during the cruise increased the INP concentrations measured in the SML by an order of magnitude, in line with increases in iron in the SML and bacterial abundances. Increases in INPSSA were not observed until after a delay of 3 days compared to increases in the SML and are likely a result of a strong in fluence of bulk SSW INPs for the temperatures investigated (T =-18 °C for SSAs, T =-15 °C for SSW). Results con firmed that INPSSA are divided into two classes depending on their associated organic matter. Here we find that warm (T ≥-22 °C) INPSSA concentrations are correlated with water soluble organic matter (WSOC) in the SSAs, but also with SSW parameters (particulate organic carbon, POCSSW and INPSSW,-16C) while cold INPSSA (T, CHARMEX and MERMEX are supported by CNRS-INSU, IFREMER, CEA, and Météo-France as part of the programme MISTRALS coordinated by INSU. The Sea2Cloud project is funded by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Sea2Cloud grant agreement no. 771369). Emmanuel Boss's group is funded by NASA Ocean Biology and Biogeochemistry.

Volcanic eruption is one of the main natural sources of atmospheric particles. In particular, evidence of New Particle Formation (NPF) from volcanic emission is reported in previous studies (Boulon et al., 2011; Sahyoun et al., 2019), which also suggests an essential role of sulfuric acid in this process. In addition, Rose et al. (2019) highlighted a significant contribution of the particles formed in the volcanic plume of the piton de la Fournaise to the budget of potential CCN at the Maïdo observatory, located ~40 km from the vent of the volcano. Therefore, it is predicted that the number and size of the cloud droplets, cloud growing and precipitation processes might be affected by the frequency of occurrence and characteristics of volcanically induced NPF in both local and regional scales, because volcanic plumes can extend far from the vent and even lower heights under the influence of the wind field and atmospheric dispersion. Following the study of Planche et al. (2020), the effect of using the New Parameterization of Nucleation (NPN) derived from the measurements performed in the passive volcanic emission plume of Etna (37.748˚ N, 14.99˚ E; Italy) (Sahyoun et al., 2019) in the WRF-Chem model (Weather Research and Forecasting Model coupled with Chemistry) is assessed, with a specific focus on the cluster formation rate and particle number concentration including CCN. In particular, results obtained with the NPN are compared to the predictions obtained with the default model settings, and further with observations.In the next step, the resulting aerosol fields will be used to further evaluate the influence of the newly formed and grown particles on cloud formation and properties in a 3D cloud-scale model using a detailed microphysics scheme (DESCAM; Flossmann and Wobrock, 2010; Planche et al. 2010; 2014) .

Even though oceans cover over 70% of the Earth’s surface, the ways in which oceans interact with climate are not fully known. Marine micro-organisms such as phytoplankton can play an important role in regulating climate by releasing different chemical species into air. In air these chemical species can react and form new aerosol particles. If grown to large enough sizes, aerosols can influence climate by acting as cloud condensation nuclei which influence the formation and properties of clouds. Even though a connection of marine biology and climate through aerosol formation was first proposed already over 30 years ago, the processes related to this connection are still uncertain.To unravel how seawater properties affect aerosol formation and to identify which chemical species are responsible for aerosol formation, we built two Air-Sea-Interaction Tanks (ASIT) that isolate 1000 l of seawater and 1000 l of air directly above the water. The used seawater was collected from different locations during a ship campaign on board the R/V Tangaroa in the South West Pacific Ocean, close to Chatham Rise, east of New Zealand. Seawater from one location was kept in the tanks for 2-3 days and then changed. By using seawater collected from different locations, we could obtain water with different biological populations. To monitor the seawater, we took daily samples to determine its chemical and biological properties.The air in the tanks was continuously flushed with particle filtered air. This way the air had on average 40 min to interact with the seawater surface before being sampled. Our air sampling was continuous and consisted of aerosol and air chemistry measurements. The instrumentation included measurements of aerosol number concentration from 1 to 500 nm and chemical species ranging from ozone and sulphur dioxide to volatile organic compounds and chemical composition of molecular clusters.Joining the seawater and atmospheric data together can give us an idea of what chemical species are emitted from the water into the atmosphere and whether these species can form new aerosol particles. Our preliminary results show a small number of particles in the freshly nucleated size range of 1-3 nm in the ASIT headspaces, indicating that new aerosol particles can form in the ASIT headspaces. In this presentation, we will also explore which chemical species could be responsible for aerosol formation and which plankton groups could be related to the emissions of these species. Combining these results with ambient data and modelling work can shed light on how important new particle formation from marine sources is for climate.Acknowledgements: Sea2Cloud project is funded by European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Grant agreement No. 771369).

We present the results of the AEROMARINE field campaign which took place in the boreal spring 2019 off the coast of Reunion island in the South West Indian Ocean basin. The southern Indian Ocean is of major interest for the study of marine aerosols, their distribution and variability [1]. Nine instrumented light plane flights and a ground-based microwave radiometer were used during the AEROMARINE field campaign. These measurements were compared with the long-term measurements of the AERONET sun-photometer (based in Saint Denis, Reunion Island) and various instruments of the high altitude Maido Observatory (2200m above sea level, Reunion island). These results were analyzed using different model outputs: (i) the AROME mesoscale weather forecast model to work on the thermodynamics of the boundary layer, (ii) the FLEXPART-AROME Lagrangian particle dispersion model to assess the geographical and vertical origin of air masses, and (iii) the chemical transport model CAMS (Copernicus Atmosphere Monitoring Service) to work on the aerosol chemical composition of air masses. These measurements allowed us to determine the background concentration of natural marine aerosols and to highlight that (1) the atmospheric layers above 1500m are in the free troposphere and are mainly composed of aerosols from the regional background and (2) that the local environment (ocean or island) has little impact on the measured concentrations. Marine aerosols emitted locally are mostly measured in the lower atmospheric layers (below 500m). The daytime marine aerosol distributions in the free troposphere measured by the aircraft were compared to the aerosol distribution measured at the high altitude Maido observatory at night when the observatory is located in the free troposphere. We also found that the CAMS reanalyses overestimated the aerosol optical depth in this region. Finally, our study confirms, with no ambiguity, that the AERONET station in Saint Denis (Reunion island) can be considered as a representative marine station in the tropics [2]. References[1] I. Koren, G. Dagan, and O. Altaratz. From aerosol-limited to invigoration of warm convective clouds. Science, 344 (6188) : 1143–1146, 2014.[2] P. Hamill, M. Giordano, C. Ward, D. Giles, and B. Holben. An aeronet-based aerosol classification using the mahalanobis distance. Atmospheric Environment, 140 : 213–233,2016.

International audience; Long-term and continuous measurements of aerosol chemical composition is essential to improve our understanding of the formation and transformation of aerosol particles in the atmosphere. Thanks to the recent developments of aerosol mass spectrometry, notably with the Aerosol Chemical Speciation Monitor (ACSM, Aerodyne; Fröhlich et al., 2013; Ng et al., 2011), this information can be acquired over long periods of time with minimal intervention from the user. The ACSM is a robust tool that measures aerosol chemical properties of the aerosol with time resolutions ranging from 10 to 30 min. Global long-term ACSM data sets have recently been presented in the literature, including a 6-year study near Paris (France; Petit et al., 2015; Zhang et al., 2019), a 2-year study in the megacity of Beijing (China; Sun et al., 2018), and a 5-year study from Leipzig (Germany; Poulain et al., 2020). The measurements within Europe are mostly being performed within the framework of the ACTRIS infrastructure (Aerosols, Clouds, and Trace gases Research InfraStructure), and a growing database of these measurements is available via the EBAS database (http://ebas.nilu. no/). Pluri-annuel and multi seasonal studies provide an opportunity to study how aerosol particles concentrations and chemical signature evolves over time in response to different airmass sources and atmospheric changes. This information is useful for understanding transport and aging patterns and can also be used for the validation of atmospheric models. Similar to worldwide measurements at low altitudes (Jimenez et al., 2009; Zhang et al., 2007), organic species also dominate the PM1 mass concentrations at high altitudes (Zhou et al., 2019). Fröhlich et al. (2015) at the Jungfraujoch station (JFJ, 3,580 m a.s.l), showed that organics were the dominant species, making

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.

High-quality data of atmospheric mercury (Hg) is rare for South America, especially for its tropical part. In consequence, mercury dynamics are still highly uncertain in this region, a significant deficiency, as South America appears to play a major role in the global budget of this toxic pollutant. To address this issue, we performed nearly two years (July 2014–February 2016) of continuous high resolution total gaseous mercury (TGM) measurements at the Chacaltaya (CHC) mountain site in the Bolivian Andes, which is subject to a diverse mix of air masses coming predominantly from the Altiplano and the Amazon rainforest. For the first eleven months of measurements, we obtained a mean TGM concentration of 0.89±0.01 ng m−3, in good agreement with the sparse amount of data available from the continent. For the remaining nine months, we obtained a significantly higher TGM concentration of 1.34±0.01 ng m−3, a difference which we tentatively attribute to the strong El Niño event of 2015–2016. Based on HYSPLIT back-trajectories and clustering techniques, we show that lower mean TGM concentrations were linked to either westerly Altiplanic air masses or those originating from the lowlands to the south-east of CHC. Elevated TGM concentrations were related to northerly air masses of Amazonian or southerly air masses of Altiplanic origin, the former possibly linked to artisanal and small scale gold mining (ASGM), while the latter might be explained by volcanic activity. We observed a marked seasonal pattern, with low TGM concentrations in the dry season (austral winter), rising concentrations during biomass burning (BB) season, and highest concentrations at the beginning of the wet season (austral summer). With the help of simultaneously sampled equivalent black carbon (eBC) and carbon monoxide (CO) data, we use the clearly BB influenced signal during BB season (August to October) to derive a mean TGM/CO emission ratio of (2.3±0.6)·10−7 ppbvTGM ppbvCO−1, which could be used to constrain South American BB emissions. Through the link with in-situ measured CO2 and remotely sensed solar-induced fluorescence (SIF) as proxies for vegetation activity, we detect signs of a vegetation sink effect in Amazonian air masses and derive a best guess TGM/CO2 uptake ratio of 0.058±0.017 (ng m−3)TGM ppmCO2−1. Finally, significantly higher Hg concentrations in western Altiplanic air masses during the wet season as compared to the dry season point towards the modulation of atmospheric Hg by the Eastern Pacific Ocean.

Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L–1. Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties., Ice nucleating particles impact the global climate by altering cloud formation and properties, but the sources of these emissions are not completely characterized. Here, the authors show that secondary organic aerosols formed from the oxidation of organic gases in the atmosphere can be a source of ice nucleating particles.

Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation (NPF). However, direct measurements of [H2SO4] remain challenging, thus preventing the determination of this important quantity, and, consequently, a complete understanding of its contribution to the NPF process. Several proxies have been developed to bridge the gaps, but their ability to predict [H2SO4] in very specific conditions such as those encountered in volcanic plumes (including in particular high sulphur dioxide mixing ratios) has not been evaluated so far. In this context, the main objective of the present study was to develop new proxies for daytime [H2SO4] in volcanic plume conditions and compare their performance to that of the proxies available in the literature. In specific, the data collected at Maïdo during the OCTAVE 2018 campaign, in the volcanic eruption plume of the Piton de la Fournaise, were first used to derive seven proxies based on the knowledge of sulphur dioxide (SO2) mixing ratio, global radiation, condensation sink (CS) and relative humidity (RH). In three of the seven proxies (F1–F3), all variables were given equal weight in the prediction of [H2SO4], while adjusted powers were allowed for the different variables in the other four proxies (A1–A4). Proxies A1–A4 were overall found to perform better compared to F1–F3, with, in specific, improved predictive ability for [H2SO4] > 2 × 108 cm−3. The CS was observed to play an important role in regulating [H2SO4], while, in contrast, the inclusion of RH did not improve the predictions. A last expression accounting for an additional sink term related to cluster formation, S1, was also tested and showed a very good predictive ability over the whole range of measured [H2SO4]. The newly developed proxies were in a second step further evaluated using airborne measurements performed in the passive degassing plume of Etna during the STRAP 2016 campaign. Increased correlations between observed and predicted [H2SO4] were obtained when the dependence of predicted [H2SO4] over CS was the lowest, and when the dependence over [SO2] was concurrently the highest. The best predictions were finally retrieved by the simple formulation of F2 (in which [SO2] and radiation alone were assumed to explain the variations of [H2SO4] with equal contributions), with a pre factor adapted to the STRAP data. All in all, our results illustrate the fairly good capacity of the proxy available in the literature to describe [H2SO4] in volcanic plume conditions, but highlight at the same time the benefit of the newly developed proxies for the prediction of the highest concentrations ([H2SO4] > 2–3 × 108 cm−3). Also, the contrasting behaviours of the new proxies in the two investigated datasets indicate that in volcanic plumes like in other environments, the relevance of a proxy can be affected by changes in environmental conditions, and that location specific coefficients do logically improve the predictions.

In order to assess the global evolution of aerosol parameters affecting climate change, a long-term trend analyses of aerosol optical properties were performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several prewhitening methods and with the Sen's slope were used as main trend analysis methods. Comparisons with General Least Mean Square associated with Autoregressive Bootstrap (GLS/ARB) and with standard Least Mean Square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficients trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficients time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, Eastern/Northern Europe and Arctic, 18 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 30 % of sites have trends, which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10 year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10 year trends are primarily found for earlier periods (10 year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10 year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10 year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10 year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2010–2011 for all stations in the eastern and central US. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage enables a better global view of potential aerosol effects on climate changes.

New particle formation (NPF) is an important source of aerosol particles at global scale, including, in particular, cloud condensation nuclei (CCN). NPF has been observed worldwide in a broad variety of environments, but some specific conditions, such as those encountered in volcanic plumes, remain poorly documented in the literature. Yet, these conditions could promote the occurrence of the process, as recently evidenced in the volcanic eruption plume of the Piton de la Fournaise (Rose at al. 2019); a dominant fraction of the volcanic particles was moreover found to be of secondary origin in the plume, further highlighting the importance of the particle formation and growth processes associated to the volcanic plume eruption. A deeper comprehension of such natural processes is thus essential to assess their climate-related effects at present days but also to better define pre-industrial conditions and their variability in climate model simulations.Sulfuric acid (SA) is commonly accepted as one of the main precursors for atmospheric NPF, and its role could be even more important in volcanic plume conditions, as recently evidenced by the airborne measurements conducted in the passive volcanic plumes of Etna and Stromboli (Sahyoun et al., 2019). Indeed, the flights performed in the frame of the STRAP campaign have allowed direct measurement of SA in such conditions for the first time, and have highlighted a strong connection between the cluster formation rate and SA concentration. Following these observations, the objective of the present work was to further quantify the formation of new particles in a volcanic plume and assess the effects of the process at a regional scale. For that purpose, the new parameterisation of nucleation derived by Sahyoun et al. (2019) was introduced in the model WRF-Chem, further optimized for the description of NPF. The flight ETNA13 described in detail in Sahyoun et al. (2019) was used as a case study to evaluate the effect of the new parameterisation on the cluster formation rate and particle number concentration in various size ranges, including CCN (i.e. climate-relevant) sizes.References: Sahyoun, M., Freney, E., Brito, J., Duplissy, J., Gouhier, M., Colomb, A., Dupuy, R., Bourianne, T., Nowak, J. B., Yan, C., Petäjä, T., Kulmala, M., Schwarzenboeck, A., Planche, C., and Sellegri, K.: Evidence of new particle formation within Etna and Stromboli volcanic plumes and its parameterization from airborne in-situ measurements, J. Geophys. Res.-Atmos., 124, 5650–5668, https://doi.org/10.1029/2018JD028882, 2019.Rose, C., Foucart, B., Picard, D., Colomb, A., Metzger, J.-M., Tulet, P., and Sellegri, K.: New particle formation in the volcanic eruption plume of the Piton de la Fournaise: specific features from a long-term dataset, Atmos. Chem. Phys., 19, 13243–13265, https://doi.org/10.5194/acp-19-13243-2019, 2019.