Description: Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-Ålesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.

Description: The organic mass fraction from sea spray aerosol (SSA) is currently a subject of intense research. The majority of this research is dedicated to measurements in ambient air. However a number of studies have recently started to focus on nascent sea spray aerosol. This work presents measurements collected during a 5-week cruise in May and June 2017 in the central and western Mediterranean Sea, an oligotrophic marine region with low phytoplankton biomass. Surface seawater was continuously pumped into a bubble-bursting apparatus to generate nascent sea spray aerosol. Size distributions were measured with a differential mobility particle sizer (DMPS). Chemical characterization of the submicron aerosol was performed with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) operating with 10 min time resolution and with filter-based chemical analysis on a daily basis. Using positive matrix factorization analysis, the ToF-ACSM non-refractory organic matter (OMNR) was separated into four different organic aerosol types, identified as primary OA (POANR), oxidized OA (OOANR), methanesulfonic acid type OA (MSA-OANR), and mixed OA (MOANR). In parallel, surface seawater biogeochemical properties were monitored providing information on phytoplankton cell abundance and seawater particulate organic carbon (1 h time resolution) and seawater surface microlayer (SML) dissolved organic carbon (DOC) (on a daily basis). Statistically robust correlations (for n〉500) were found between MOANR and nanophytoplankton cell abundance, as well as between POANR, OOANR, and particulate organic carbon (POC). Parameterizations of the contributions of different types of organics to the submicron nascent sea spray aerosol are proposed as a function of the seawater biogeochemical properties for use in models.

Description: The goal of the Sea2Cloud project is to study the interplay between surface ocean biogeochemical and physical properties, fluxes to the atmosphere, and ultimately their impact on cloud formation under minimal direct anthropogenic influence. Here we present an interdisciplinary approach, combining atmospheric physics and chemistry with marine biogeochemistry, during a voyage between 41 degrees and 47 degrees S in March 2020. In parallel to ambient measurements of atmospheric composition and seawater biogeochemical properties, we describe semicontrolled experiments to characterize nascent sea spray properties and nucleation from gas-phase biogenic emissions. The experimental framework for studying the impact of the predicted evolution of ozone concentration in the Southern Hemisphere is also detailed. After describing the experimental strategy, we present the oceanic and meteorological context including provisional results on atmospheric thermodynamics, composition, and flux measurements. In situ measurements and flux studies were carried out on different biological communities by sampling surface seawater from subantarctic, subtropical, and frontal water masses. Air-Sea-Interface Tanks (ASIT) were used to quantify biogenic emissions of trace gases under realistic environmental conditions, with nucleation observed in association with biogenic seawater emissions. Sea spray continuously generated produced sea spray fluxes of 34% of organic matter by mass, of which 4% particles had fluorescent properties, and which size distribution resembled the one found in clean sectors of the Southern Ocean. The goal of Sea2Cloud is to generate realistic parameterizations of emission flux dependences of trace gases and nucleation precursors, sea spray, cloud condensation nuclei, and ice nuclei using seawater biogeochemistry, for implementation in regional atmospheric models.

Description: 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 (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 Mediterranean 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 influence of bulk SSW INPs for the temperatures investigated (T=−18 ∘C for SSAs, T=−15 ∘C for SSW). Results confirmed 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〈−22 ∘C) are correlated with SSA water-insoluble organic carbon (WIOC) and SML dissolved organic carbon (DOC) concentrations. A relationship was also found between cold INPSSA and SSW nano- and microphytoplankton cell abundances, indicating that these species might be a source of water-insoluble organic matter with surfactant properties and specific IN activities. Guided by these results, we formulated and tested multiple parameterizations for the abundance of INPs in marine SSAs, including a single-component model based on POCSSW and a two-component model based on SSA WIOC and OC. We also altered a previous model based on OCSSA content to account for oligotrophy of the Mediterranean Sea. We then compared this formulation with the previous models. This new parameterization should improve attempts to incorporate marine INP emissions into numerical models.

Description: One pathway by which the oceans influence climate is via the emission of sea spray that may subsequently influence cloud properties. Sea spray emissions are known to be dependent on atmospheric and oceanic physicochemical parameters, but the potential role of ocean biology on sea spray fluxes remains poorly characterized. Here we show a consistent significant relationship between seawater nanophytoplankton cell abundances and sea-spray derived Cloud Condensation Nuclei (CCN) number fluxes, generated using water from three different oceanic regions. This sensitivity of CCN number fluxes to ocean biology is currently unaccounted for in climate models yet our measurements indicate that it influences fluxes by more than one order of magnitude over the range of phytoplankton investigated.

Description: Significance Oceans represent 70% of our planet’s surface, housing a large spectrum of microorganisms that interact with the above atmosphere. Ocean microorganisms were proposed in the late 80’s to be at the center of a climate feedback loop involving dimethyl sulfide (DMS) that would form aerosols and modify cloud properties (CLAW hypothesis). In the present paper, we report observational evidence from semicontrolled experiments in the South Pacific that nitrate ions, yet hitherto not considered, is a key species involved in aerosol nucleation in the pristine marine atmosphere and which precursors are coemitted with DMS. Our results further indicate that nitrate ion formation would be related to short-term microbial processes, sensitive to environmental stressors, therefore potentially “closing the loop”. Abstract Our understanding of ocean–cloud interactions and their effect on climate lacks insight into a key pathway: do biogenic marine emissions form new particles in the open ocean atmosphere? Using measurements collected in ship-borne air–sea interface tanks deployed in the Southwestern Pacific Ocean, we identified new particle formation (NPF) during nighttime that was related to plankton community composition. We show that nitrate ions are the only species for which abundance could support NPF rates in our semicontrolled experiments. Nitrate ions also prevailed in the natural pristine marine atmosphere and were elevated under higher sub-10 nm particle concentrations. We hypothesize that these nucleation events were fueled by complex, short-term biogeochemical cycling involving the microbial loop. These findings suggest a new perspective with a previously unidentified role of nitrate of marine biogeochemical origin in aerosol nucleation.

Description: 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.

Description: The STRAP (Synergie Transdisciplinaire pour Répondre aux Aléas liés aux Panaches volcaniques) campaign was conducted in 2015 to investigate the volcanic plumes of Piton de La Fournaise (La Réunion, France). For the first time, measurements at the local (near the vent) and at the regional scales around the island were conducted. The STRAP 2015 campaign has become possible thanks to a strong cross-disciplinary collaboration between volcanologists and meteorologists. The main observations during four eruptive 5 periods (85 days) are summarized. They include the estimates of SO2, CO2 and H2O emissions, the altitude of the plume at the vent and over different areas of La Réunion Island, the evolution of the SO2 concentration, the aerosol size distribution, and the aerosol extinction profile. A climatology of the volcanic plume dispersion is also reported. Simulations and measurements showed that the plume formed by weak eruption has a stronger interaction with the surface of the island. Strong SO2 and particles concentrations above 1000 ppb and 50,000 cm−3, respectively, are 10 frequently measured over 20 km of distance from the Piton de la Fournaise. The measured aerosol size distribution shows the predominance of small particles in the volcanic plume. A particular emphasis is placed on the gas-particle conversion with several cases of strong nucleation of sulfuric acid observed within the plume and at the distal site of the Maïdo observatory. The STRAP 2015 campaign gave a unique set of multi-disciplinary data that can now be used by modellers to improve the numerical paramameterizations of the physical and chemical evolution of the volcanic plumes.

Description: Published

Description: 5355-5378

Description: 5V. Dinamica dei processi eruttivi e post-eruttivi

Description: JCR Journal

Description: 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.

Description: Volcanic gases and aerosols emissions from passive degassing or low eruptive events are now included in most climate models despite large uncertainties still exist about their injection height and their temporal and spatial variability. The aim of this study is to quantify the evolution of the gas and aerosols inside volcanic plumes with high kilometric-resolution simulations. With online chemistry and aerosols, these simulations are carried out together with in situ measurements of aerosol and gas-phase properties to assess the impact of Etna and Stromboli volcanic plumes produced by passive degassing and regular Strombolian activity, respectively. Comparison between simulation and observations show that the simulation reproduces the main characteristics of the volcanic plume evolution and confirms that volcanic plumes produced by passive degassing or low eruptive events have a strong impact on cloud condensation nuclei (CCN) formation increasing the number of CCN by a factor of 5. It was also shown that depending on the plume location, the aerosols will act as CCN at different distance from the vent. In the marine atmospheric boundary layer, the aerosols will act as CCN at proximity to the vent (less than 50 km) because of strong condensation sink inhibiting nucleation. In comparison, in the free troposphere, aerosols will act as CCN far from the vent, at more than 200 km. To the best of our knowledge, this study using in situ measurements as well as subkilometric simulations is unique

Description: Published

Description: 11389-11405

Description: 4V. Processi pre-eruttivi

Description: JCR Journal