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1. Seasonal Variations, Origin, and Parameterization of Ice‐Nucleating Particles at a Mountain Station in Central France

Author: Yannick Bras, Evelyn Freney, Antoine Canzi, Pierre Amato, Laetitia Bouvier, Jean‐Marc Pichon, David Picard, María Cruz Minguillón, Noemí Pérez, and Karine Sellegri
Subjects: ice nuclei particles, nucleation, clouds, aerosols, mountain site, Astronomy, QB1-991, Geology, QE1-996.5
Abstract: Abstract Identifying how aerosol particles interact with atmospheric water is critical to understand climate and precipitation. Ice‐nucleating particles (INP) trigger the formation of atmospheric ice crystals at higher temperatures than pure water. They are difficult to characterize because of their scarce occurrence, and variability, in the atmosphere, especially at temperatures above −20°C. It has been demonstrated that at these temperatures, biological aerosol particles can contribute significantly to INP number concentration. This study incorporates a series of offline, size‐segregated measurements of INPs collected at the Puy de Dôme station (PUY, 1,465 m a.s.l.) over a 6 month period from October to May, covering the transitions from autumn, winter, to spring. These measurements show a general trend of decreasing particle number concentrations during the winter months and higher concentration during autumn and spring. INP concentrations measured in the range of −5 and −18°C, had concentrations of 0.001 INP/Lair at the warmest temperatures, and between 0.01 and 0.1 INP/Lair at the coldest temperatures. The majority of INP measured at temperatures warmer than −15°C were heat labile, suggesting a biological or organic origin. The INP variability was compared with collocated aerosol physical and chemical properties, allowing us to associate highest INP concentrations with local and marine origins. Following these comparisons, we use aerosol total number concentration to develop a new parameterization. In addition, this parameterization is specifically optimized for warmer temperature INP measurements, and demonstrated a good performance when tested on independent data sets.
Published: 2024
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2. European aerosol phenomenology − 8: Harmonised source apportionment of organic aerosol using 22 Year-long ACSM/AMS datasets

Author: Gang Chen, Francesco Canonaco, Anna Tobler, Wenche Aas, Andres Alastuey, James Allan, Samira Atabakhsh, Minna Aurela, Urs Baltensperger, Aikaterini Bougiatioti, Joel F. De Brito, Darius Ceburnis, Benjamin Chazeau, Hasna Chebaicheb, Kaspar R. Daellenbach, Mikael Ehn, Imad El Haddad, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Anna Font, Kirsten Fossum, Evelyn Freney, Maria Gini, David C Green, Liine Heikkinen, Hartmut Herrmann, Athina-Cerise Kalogridis, Hannes Keernik, Radek Lhotka, Chunshui Lin, Chris Lunder, Marek Maasikmets, Manousos I. Manousakas, Nicolas Marchand, Cristina Marin, Luminita Marmureanu, Nikolaos Mihalopoulos, Griša Močnik, Jaroslaw Nęcki, Colin O'Dowd, Jurgita Ovadnevaite, Thomas Peter, Jean-Eudes Petit, Michael Pikridas, Stephen Matthew Platt, Petra Pokorná, Laurent Poulain, Max Priestman, Véronique Riffault, Matteo Rinaldi, Kazimierz Różański, Jaroslav Schwarz, Jean Sciare, Leïla Simon, Alicja Skiba, Jay G. Slowik, Yulia Sosedova, Iasonas Stavroulas, Katarzyna Styszko, Erik Teinemaa, Hilkka Timonen, Anja Tremper, Jeni Vasilescu, Marta Via, Petr Vodička, Alfred Wiedensohler, Olga Zografou, María Cruz Minguillón, and André S.H. Prévôt
Subjects: European Overview, Source apportionment, Harmonised Protocol, Organic Aerosol, Long-term Datasets, Rolling PMF, Environmental sciences, GE1-350
Abstract: Organic aerosol (OA) is a key component of total submicron particulate matter (PM1), and comprehensive knowledge of OA sources across Europe is crucial to mitigate PM1 levels. Europe has a well-established air quality research infrastructure from which yearlong datasets using 21 aerosol chemical speciation monitors (ACSMs) and 1 aerosol mass spectrometer (AMS) were gathered during 2013–2019. It includes 9 non-urban and 13 urban sites. This study developed a state-of-the-art source apportionment protocol to analyse long-term OA mass spectrum data by applying the most advanced source apportionment strategies (i.e., rolling PMF, ME-2, and bootstrap). This harmonised protocol was followed strictly for all 22 datasets, making the source apportionment results more comparable. In addition, it enables quantification of the most common OA components such as hydrocarbon-like OA (HOA), biomass burning OA (BBOA), cooking-like OA (COA), more oxidised-oxygenated OA (MO-OOA), and less oxidised-oxygenated OA (LO-OOA). Other components such as coal combustion OA (CCOA), solid fuel OA (SFOA: mainly mixture of coal and peat combustion), cigarette smoke OA (CSOA), sea salt (mostly inorganic but part of the OA mass spectrum), coffee OA, and ship industry OA could also be separated at a few specific sites. Oxygenated OA (OOA) components make up most of the submicron OA mass (average = 71.1%, range from 43.7 to 100%). Solid fuel combustion-related OA components (i.e., BBOA, CCOA, and SFOA) are still considerable with in total 16.0% yearly contribution to the OA, yet mainly during winter months (21.4%). Overall, this comprehensive protocol works effectively across all sites governed by different sources and generates robust and consistent source apportionment results. Our work presents a comprehensive overview of OA sources in Europe with a unique combination of high time resolution (30–240 min) and long-term data coverage (9–36 months), providing essential information to improve/validate air quality, health impact, and climate models.
Published: 2022
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3. Surface ocean microbiota determine cloud precursors

Author: Karine Sellegri, Alessia Nicosia, Evelyn Freney, Julia Uitz, Melilotus Thyssen, Gérald Grégori, Anja Engel, Birthe Zäncker, Nils Haëntjens, Sébastien Mas, David Picard, Alexia Saint-Macary, Maija Peltola, Clémence Rose, Jonathan Trueblood, Dominique Lefevre, Barbara D’Anna, Karine Desboeufs, Nicholas Meskhidze, Cécile Guieu, and Cliff S. Law
Subjects: Medicine, Science
Abstract: Abstract 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.
Published: 2021
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4. A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Author: Martin J. Wolf, Yue Zhang, Maria A. Zawadowicz, Megan Goodell, Karl Froyd, Evelyn Freney, Karine Sellegri, Michael Rösch, Tianqu Cui, Margaux Winter, Larissa Lacher, Duncan Axisa, Paul J. DeMott, Ezra J. T. Levin, Ellen Gute, Jonathan Abbatt, Abigail Koss, Jesse H. Kroll, Jason D. Surratt, and Daniel J. Cziczo
Subjects: Science
Abstract: 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.
Published: 2020
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5. Seasonal Variation of Aerosol Size Distribution Data at the Puy de Dôme Station with Emphasis on the Boundary Layer/Free Troposphere Segregation

Author: Antoine Farah, Evelyn Freney, Aurélien Chauvigné, Jean-Luc Baray, Clémence Rose, David Picard, Aurélie Colomb, Dani Hadad, Maher Abboud, Wehbeh Farah, and Karine Sellegri
Subjects: aerosol size distribution, high altitude site, long-range transport, boundary layer/lower free troposphere, Meteorology. Climatology, QC851-999
Abstract: Aerosol particles are important due to their direct and indirect impacts on climate. Within the planetary boundary layer (BL), these particles have a relatively short lifetime due to their frequent removal process by wet deposition. When aerosols are transported into the free troposphere (FT), their atmospheric lifetime increases significantly, making them representative of large spatial areas. In this work, we use a combination of in situ measurements performed at the high altitude PUY (Puy de Dôme, 45°46′ N, 2°57′ E, 1465 m a.s.l) station, together with LIDAR profiles at Clermont-Ferrand for characterizing FT conditions, and further characterize the physical properties of aerosol in this poorly documented area of the atmosphere. First, a combination of four criteria was used to identify whether the PUY station lies within the FT or within the BL. Results show that the PUY station is located in BL with frequencies ranging from 50% during the winter, up to 97% during the summer. Then, the classification is applied to a year-long dataset (2015) of particle size distribution data to study the differences in particle physical characteristics (size distribution) and black carbon (BC) concentrations between the FT and the BL. Although BC, Aitken, and the accumulation mode particles concentrations were higher in the BL than in the FT in winter and autumn, they were measured to be higher in the FT compared to BL in spring. No significant difference between the BL and the FT concentrations was observed for the nucleation mode particles for all seasons, suggesting a continuous additional source of nucleation mode particles in the FT during winter and autumn. Coarse mode particle concentrations were found higher in the FT than in the BL for all seasons and especially during summer. This indicates an efficient long-range transport of large particles in the FT from distant sources (marine and desert) due to higher wind speeds in the FT compared to BL. For FT air masses, we used 204-h air mass back-trajectories combined with boundary layer height estimations from ECMWF ERA-Interim to assess the time they spent in the FT since their last contact with the BL and to evaluate the impact of this parameter on the aerosol properties. We observed that even after 75 h without any contact with the BL, FT aerosols preserve specific properties of their air mass type.
Published: 2018
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6. Quantified effect of seawater biogeochemistry on the temperature dependence of sea spray aerosol fluxes

Author: Karine Sellegri, Theresa Barthelmeß, Jonathan Trueblood, Antonia Cristi, Evelyn Freney, Clémence Rose, Neill Barr, Mike Harvey, Karl Safi, Stacy Deppeler, Karen Thompson, Wayne Dillon, Anja Engel, and Cliff Law
Abstract: 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.
Published: 2023

7. Measurements of aerosol dimensional distributions and microphysical characteristics: A comparison between Raman lidar and airborne sensors

Author: Igor Veselovskii, Evelyn Freney, Benedetto De Rosa, Paolo Di Girolamo, Donato Summa, and Noemi Franco
Subjects: Raman lidar, Environmental science, Aerosol, Remote sensing
Abstract: This manuscript compares aerosol size distributions and microphysical property measurements from the Raman lidar BASIL and from aircraft sensors during HyMeX-SOP1. The attention was focused on a me...
Published: 2021

8. Evidence of New Particle Formation Within Etna and Stromboli Volcanic Plumes and Its Parameterization From Airborne In Situ Measurements

Author: Jonathan Duplissy, Maher Sahyoun, T. Bourianne, Mathieu Gouhier, Chao Yan, Markku Kulmala, Alfons Schwarzenboeck, Régis Dupuy, Céline Planche, John B. Nowak, Karine Sellegri, Tuukka Petäjä, Joel Brito, Evelyn Freney, Aurélie Colomb, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Helsinki Institute of Physics (HIP), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Laboratoire Magmas et Volcans (LMV), Institut national des sciences de l'Univers (INSU - CNRS)-Université Jean Monnet - Saint-Étienne (UJM)-Institut de Recherche pour le Développement et la société-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS)-Observatoire de Physique du Globe de Clermont-Ferrand (OPGC), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Observatoire de Physique du Globe de Clermont-Ferrand (OPGC), Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), NASA Langley Research Center [Hampton] (LaRC), ANR-10-LABX-0006,CLERVOLC,Clermont-Ferrand centre for research on volcanism(2010), ANR-16-IDEX-0001,CAP 20-25,CAP 20-25(2016), Institute for Atmospheric and Earth System Research (INAR), INAR Physics, Polar and arctic atmospheric research (PANDA), University of Helsinki, Institut national des sciences de l'Univers (INSU - CNRS)-Université Jean Monnet [Saint-Étienne] (UJM)-Institut de Recherche pour le Développement et la société-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS)-Observatoire de Physique du Globe de Clermont-Ferrand (OPGC), Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement et la société-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Physique du Globe de Clermont-Ferrand (OPGC), and Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Université Jean Monnet [Saint-Étienne] (UJM)
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Particle number, volcanic secondary aerosols, 116 Chemical sciences, Mesoscale meteorology, ASH, Atmospheric sciences, 114 Physical sciences, 01 natural sciences, CLOUD CONDENSATION NUCLEI, Troposphere, chemistry.chemical_compound, SULFURIC-ACID, ATMOSPHERIC NUCLEATION, new particle formation, CHEMISTRY, aerosol formation rate parameterization, [SDU.STU.VO]Sciences of the Universe [physics]/Earth Sciences/Volcanology, Earth and Planetary Sciences (miscellaneous), Cloud condensation nuclei, EMISSIONS, Sulfur dioxide, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, geography, geography.geographical_feature_category, sulfuric acid, volcanic plume, AEROSOL, KILAUEA VOLCANO, Aerosol, Boundary layer, Geophysics, chemistry, Volcano, GAS, 13. Climate action, Space and Planetary Science, GROWTH, Etna and Stromboli
Abstract: 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.
Published: 2019

9. A two-component parameterization of marine ice-nucleating particles based on seawater biology and sea spray aerosol measurements in the Mediterranean Sea

Author: Jonathan V. Trueblood, Alesia Nicosia, Anja Engel, Birthe Zäncker, Matteo Rinaldi, Evelyn Freney, Melilotus Thyssen, Ingrid Obernosterer, Julie Dinasquet, Franco Belosi, Antonio Tovar-Sánchez, Araceli Rodriguez-Romero, Gianni Santachiara, Cécile Guieu, Karine Sellegri, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA), Helmholtz Centre for Ocean Research [Kiel] (GEOMAR), Istituto di Scienze dell'Atmosfera e del Clima [Bologna] (ISAC), Consiglio Nazionale delle Ricerche (CNR), Institut méditerranéen d'océanologie (MIO), Institut de Recherche pour le Développement (IRD)-Aix Marseille Université (AMU)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Toulon (UTLN)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'océanographie de Villefranche (LOV), Institut national des sciences de l'Univers (INSU - CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de la Mer de Villefranche (IMEV), Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Scripps Institution of Oceanography (SIO), University of California [San Diego] (UC San Diego), University of California-University of California, Instituto de Ciencias Marinas de Andalucia [Cádiz, Espagne] (ICMAN), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Observatoire océanologique de Villefranche-sur-mer (OOVM), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Scripps Institution of Oceanography (SIO - UC San Diego), University of California (UC)-University of California (UC), Centre National de la Recherche Scientifique (France), Institut national des sciences de l'Univers (France), French Alternative Energies and Atomic Energy Commission, Institut Français de Recherche pour l'Exploitation de la Mer, Météo-France, European Commission, NASA Ocean Biology and Biogeochemistry, and Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 0106 biological sciences, 010504 meteorology & atmospheric sciences, 13. Climate action, 010604 marine biology & hydrobiology, [SDE]Environmental Sciences, 14. Life underwater, 01 natural sciences, 0105 earth and related environmental sciences
Abstract: 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.
Published: 2021

10. Altitude Aerosol Measurements in Central France: Seasonality, Sources and Free‐Troposphere/Boundary Layer Segregation

Author: Francesco Canonaco, Karine Sellegri, Wehbeh Farah, André S. H. Prévôt, Evelyn Freney, Marie Abboud, J‐m. Pichon, Antoine Farah, Laboratoire de Météorologie Physique (LaMP), and Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA)
Subjects: 010504 meteorology & atmospheric sciences, lcsh:Astronomy, boundary layer/free troposphere, Environmental Science (miscellaneous), 010502 geochemistry & geophysics, Atmospheric sciences, 01 natural sciences, lcsh:QB1-991, Troposphere, Atmosphere, Altitude, medicine, long range transport, 0105 earth and related environmental sciences, aerosol chemical speciation monitor, Atmospheric models, lcsh:QE1-996.5, organic aerosol sources, 15. Life on land, Seasonality, high altitude site, medicine.disease, Trace gas, Aerosol, lcsh:Geology, 13. Climate action, [SDU]Sciences of the Universe [physics], [SDE]Environmental Sciences, General Earth and Planetary Sciences, Environmental science, Aerosol mass spectrometry
Abstract: 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
Published: 2021

11. Response to reviewers

Author: Evelyn Freney
Published: 2020

12. A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Author: Ellen Gute, Megan Goodell, Tianqu Cui, Karine Sellegri, Maria A. Zawadowicz, Margaux Winter, Michael Rösch, Yue Zhang, Martin J. Wolf, Jason D. Surratt, Jesse H. Kroll, Ezra J. T. Levin, Daniel J. Cziczo, Jonathan P. D. Abbatt, Evelyn Freney, Paul J. DeMott, Abigail R. Koss, Larissa Lacher, Karl D. Froyd, Duncan Axisa, Department of Earth and Planetary Sciences [Cambridge, USA] (EPS), Harvard University [Cambridge], Department of Environmental Sciences & Engineering, University of North Carolina [Chapel Hill] (UNC), University of North Carolina System (UNC)-University of North Carolina System (UNC), Aerodyne Research Incorporated, Center for Aerosol and Cloud Chemistry, Department of Chemistry and Chemical Biology [Boston], Northeastern University [Boston], Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory (PNNL), NOAA Earth System Research Laboratory (ESRL), National Oceanic and Atmospheric Administration (NOAA), Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado [Boulder]-National Oceanic and Atmospheric Administration (NOAA), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Institute for Atmospheric and Climate Science [Zürich] (IAC), Eidgenössische Technische Hochschule - Swiss Federal Institute of Technology [Zürich] (ETH Zürich), Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Department of Chemistry and Chemical Biology [Harvard], Institute of Meteorology and Climate Research – Atmospheric Environmental Research, Karlsruhe Institute of Technology, Partenaires INRAE, Droplet Measurement Technologies, Department of Atmospheric Science, Colorado State University, Department of Chemistry [University of Toronto], University of Toronto, Department of Civil and Environmental Engineering [Cambridge] (CEE), Massachusetts Institute of Technology (MIT), Harvard University, Karlsruhe Institute of Technology (KIT), Department of Atmospheric Science [Fort Collins], and Colorado State University [Fort Collins] (CSU)
Subjects: Atmospheric chemistry, 010504 meteorology & atmospheric sciences, Climate, Science, General Physics and Astronomy, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Article, General Biochemistry, Genetics and Molecular Biology, Physics::Geophysics, Troposphere, Atmosphere, chemistry.chemical_compound, Hemiterpenes, ddc:550, Butadienes, Atmospheric science, Precipitation, lcsh:Science, Physics::Atmospheric and Oceanic Physics, Isoprene, 0105 earth and related environmental sciences, Aerosols, Supersaturation, Multidisciplinary, Ice, General Chemistry, Aerosol, Earth sciences, chemistry, 13. Climate action, [SDE]Environmental Sciences, Ice nucleus, Environmental science, lcsh:Q, Cirrus, Astrophysics::Earth and Planetary Astrophysics
Abstract: 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.
Published: 2020

13. Supplementary material to 'A Two-Component Parameterization of Marine Ice Nucleating Particles Based on Seawater Biology and Sea Spray Aerosol Measurements in the Mediterranean Sea'

Author: Jonathan V. Trueblood, Alesia Nicosia, Anja Engel, Birthe Zäncker, Matteo Rinaldi, Evelyn Freney, Melilotus Thyssen, Ingrid Obernosterer, Julie Dinasquet, Franco Belosi, Antonio Tovar-Sánchez, Araceli Rodriguez-Romero, Gianni Santachiara, Cécile Guieu, and Karine Sellegri
Published: 2020

14. Supplementary material to 'Mediterranean nascent sea spray organic aerosol and relationships with seawater biogeochemistry'

Author: Evelyn Freney, Karine Sellegri, Alessia Nicosia, Jonathan T. Trueblood, Matteo Rinaldi, Leah R. Williams, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van-Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilka Timmonen, and Cécile Guieu
Published: 2020

15. Cézeaux-Aulnat-Opme-Puy De Dôme: a multi-site for the long term survey of the tropospheric composition and climate change

Author: Jean-Luc Baray, Laurent Deguillaume, Aurélie Colomb, Karine Sellegri, Evelyn Freney, Clémence Rose, Joël Van Baelen, Jean-Marc Pichon, David Picard, Patrick Fréville, Laetitia Bouvier, Mickaël Ribeiro, Pierre Amato, Sandra Banson, Angelica Bianco, Agnès Borbon, Laureline Bourcier, Yannick Bras, Marcello Brigante, Philippe Cacault, Aurélien Chauvigné, Tiffany Charbouillot, Nadine Chaumerliac, Anne Marie Delort, Marc Delmotte, Régis Dupuy, Antoine Farah, Guy Febvre, Andrea Flossmann, Christophe Gourbeyre, Claude Hervier, Maxime Hervo, Nathalie Huret, Muriel Joly, Victor Kazan, Morgan Lopez, Gilles Mailhot, Angela Marinoni, Olivier Masson, Nadège Montoux, Marius Parazols, Frédéric Peyrin, Yves Pointin, Michel Ramonet, Manon Rocco, Martine Sancelme, Stéphane Sauvage, Martina Schmidt, Emmanuel Tison, Mickaël Vaïtilingom, Paolo Villani, Miao Wang, Camille Yver-Kwok, and Paolo Laj
Abstract: For the last twenty-five years, CO-PDD (Cézeaux-Aulnat-Opme-puy de Dôme) has evolved to become a full instrumented platform for atmospheric research. It is nationally accredited by CNRS, the French national center for scientific research, and recognized as a global station in the GAW network (Global Atmospheric Watch). It is a reference site of the European and national research infrastructures ACTRIS (Aerosol Cloud and Trace gases Research Infrastructure) and ICOS (Integrated Carbon Observing System). The site located on-top of the puy de Dôme mountain (1465 m a.s.l.) is completed by additional sites located at lower altitudes and adding the vertical dimension to the atmospheric observations: Opme (660 m a.s.l.), Cézeaux (410 m) and Aulnat (330 m). On the sites has been developed a unique combination of in-situ and remote sensing measurements capturing and documenting the variability of particulate and gaseous atmospheric composition, but also the optical, biochemical and physical properties of aerosol particles, clouds and precipitations. Given its location far away from any major emission sources, its altitude and the mountain orography, the puy de Dôme station is ideally situated to sample different air masses in the boundary layer or in the free troposphere depending on time of day and seasons. It is also an ideal place to study cloud properties with frequent presence of clouds at the top in autumn and winter. As a result of the natural conditions prevailing at the site and of the very exhaustive instrumental deployment, scientific studies at puy de Dôme strongly contribute to improving the knowledge in atmospheric sciences including the characterization of trends and variability, the understanding of complex and interconnected processes (microphysical, chemical, biological, chemical and dynamical) and providing a reference point for climate models. In this context, CO-PDD is a pilot site to conduct instrumental development inside its wind tunnel for testing liquid/ice cloud probes in natural conditions, or in-situ systems to collect aerosol and cloud. This paper reviews 25 years (1995–2020) of atmospheric observation at the station, and related scientific research contributing to atmospheric and climate science.
Published: 2019

16. The second ACTRIS inter-comparison (2016) for Aerosol Chemical Speciation Monitors (ACSM): Calibration protocols and instrument performance evaluations

Author: David C. Green, Jean Sciare, Evelyn Freney, François Truong, Jean-Eudes Petit, Roland Sarda-Esteve, Olivier Favez, Harald Flentje, Philip Croteau, Vincent Crenn, Nicola Zanca, Minna Aurela, C. Carbone, André S. H. Prévôt, Iasonas Stavroulas, Yunjiang Zhang, Aikaterini Bougiatioti, Max Priestman, Marek Maasikmets, Valérie Gros, Tarvo Arumae, Esther Coz, Leah R. Williams, Alfred Wiedensohler, Nikolaos Mihalopoulos, Tanguy Amodeo, Jeni Vasilescu, Thomas Elste, Anna Tobler, Manjula R. Canagaratna, María Cruz Minguillón, Begoña Artíñano, Hartmut Herrmann, Andrés Alastuey, Nicolas Bonnaire, Laurent Poulain, Liine Heikkinen, Luminita Marmureanu, John T. Jayne, Ministerio de Economía y Competitividad (España), Alastuey, Andrés [0000-0002-5453-5495], Minguillón, María Cruz [0000-0002-5464-0391], Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Institut National de l'Environnement Industriel et des Risques (INERIS), Aerodyne Research Inc., Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Finnish Meteorological Institute (FMI), Institute for Environmental Research and Sustainable Development (IERSD), National Observatory of Athens (NOA), Centro de Investigaciones Energéticas Medioambientales y Tecnológicas [Madrid] (CIEMAT), Deutscher Wetterdienst [Offenbach] (DWD), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Leibniz-Institut für Troposphärenforschung (TROPOS), Leibniz Institute for Tropospheric Research (TROPOS), King‘s College London, Institute of Environmental Assessment and Water Research (IDAEA), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Cyprus Institute (CyI), Paul Scherrer Institute (PSI), National Institute of Research and Development for Optoelectronics (INOE), Consiglio Nazionale delle Ricerche [Bologna] (CNR), Estonian Environmental Research Center, Tallinn, Estonia, Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Alastuey, Andrés, Minguillón, María Cruz, Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), University of Helsinki, Department of Chemistry, and INAR Physics
Subjects: Research program, SUBMICRON AEROSOLS, 010504 meteorology & atmospheric sciences, EFFICIENCIES, 116 Chemical sciences, Library science, 010501 environmental sciences, 114 Physical sciences, 01 natural sciences, 7. Clean energy, Data treatment, Air quality monitoring, CHEMISTRY, Political science, Environmental Chemistry, media_common.cataloged_instance, General Materials Science, Cost action, Environmental impact assessment, AMS, FIELD, European union, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, media_common, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Aerosols, Chemical speciation, Water-soluble ions, Pollution, 13. Climate action, ORIGINS, [SDE]Environmental Sciences, Jim Smith, Christian ministry, Haze, Particulate matter
Abstract: This work describes results obtained from the 2016 Aerosol Chemical Speciation Monitor (ACSM) intercomparison exercise performed at the Aerosol Chemical Monitor Calibration Center (ACMCC, France). Fifteen quadrupole ACSMs (Q_ACSM) from the European Research Infrastructure for the observation of Aerosols, Clouds and Trace gases (ACTRIS) network were calibrated using a new procedure that acquires calibration data under the same operating conditions as those used during sampling and hence gets information representative of instrument performance. The new calibration procedure notably resulted in a decrease in the spread of the measured sulfate mass concentrations, improving the reproducibility of inorganic species measurements between ACSMs as well as the consistency with co-located independent instruments. Tested calibration procedures also allowed for the investigation of artifacts in individual instruments, such as the overestimation of m/z 44 from organic aerosol. This effect was quantified by the m/z (mass-to-charge) 44 to nitrate ratio measured during ammonium nitrate calibrations, with values ranging from 0.03 to 0.26, showing that it can be significant for some instruments. The fragmentation table correction previously proposed to account for this artifact was applied to the measurements acquired during this study. For some instruments (those with high artifacts), this fragmentation table adjustment led to an “overcorrection” of the f44 (m/z 44/Org) signal. This correction based on measurements made with pure NH4NO3, assumes that the magnitude of the artifact is independent of chemical composition. Using data acquired at different NH4NO3 mixing ratios (from solutions of NH4NO3 and (NH4)2SO4) we observe that the magnitude of the artifact varies as a function of composition. Here we applied an updated correction, dependent on the ambient NO3 mass fraction, which resulted in an improved agreement in organic signal among instruments. This work illustrates the benefits of integrating new calibration procedures and artifact corrections, but also highlights the benefits of these intercomparison exercises to continue to improve our knowledge of how these instruments operate, and assist us in interpreting atmospheric chemistry. © 2019, © 2019 Author(s). Published with license by Taylor & Francis Group, LLC., Funding text #1 aLaboratoire de Météorologie Physique (LaMP), Aubiere, France; bInstitut National de l’Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, France; cLaboratoire des Sciences du Climat et de l’Environnement (LSCE), CNRS-CEA-UVSQ, Gif-sur-Yvette, France; dAerodyne Research, Inc, Billerica, Massachusetts, USA; eEnvironment Energy and Water Research Center, The Cyprus Institute, Nicosia, Cyprus; fEstonian Environmental Research Center (EERC), Tallinn, Estonia; gFinnish meteorological institute (FMI), Helsinki, Finland; hIERSD, National Observatory of Athens, Athens, Greece; iDepartment of the Environment, Centre for Energy, Environment and Technology Research (CIEMAT), Madrid, Spain; jDeutscher Wetterdienst, Meteorologisches Observatorium Hohenpeißenberg, Hohenpeißenberg, Germany; kInstitute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland; lLeibniz Institute for Tropospheric Research, Leipzig, Germany; mEnvironmental Research Group, MRC-HPA Centre for Environment and Health, King’s College London, London, United Kingdom; nInstitute of Environmental Assessment and Water Research (IDAEA-CSIC), Barcelona, Spain; oLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen PSI, Switzerland; pNational Institute of R&D for Optoelectronics (INOE), Ilfov, Romania; qProambiente S.c.r.l CNR Research Area, Bologna, Italy Funding text #2 This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 654109. The US Department of Energy Small Business Innovative Research program (award number DE-SC0017041) provided support for development of ACSM calibration procedures. CNRS, CEA, and INERIS are acknowledged for financial support of the ACMCC. The intercomparison campaign and the following data treatment have been conducted in collaboration with the French reference laboratory for air quality monitoring (LCSQA), funded by the French Ministry of Environment. COST action CA16109 Chemical On-Line cOmpoSition and Source Apportionment of fine aerosoLs COLOSSAL grant is gratefully acknowledged for the support of data workshops. M.C. Minguillón acknowledges the Ramón y Cajal fellowship awarded by the Spanish Ministry of Economy, Industry and Competitiveness. The CIEMAT participation has been partially funded by MINECO/AEI/FEDER, UE (CGL2017-85344-R and CGL2017-90884-REDT) and TIGAS-CM (Y2018/EMT- 5177) Project. PSI is grateful for financial support by the Federal Office for the Environment in Switzerland.
Published: 2019

17. Volcanic plume aging during passive degassing and low eruptive events of Etna and Stromboli volcanoes

Author: Karine Sellegri, Evelyn Freney, Aurélie Colomb, G. Salerno, Marco Liuzzo, Maud Leriche, Pierre Tulet, Brice Foucart, Joris Pianezze, Laboratoire de l'Atmosphère et des Cyclones (LACy), Centre National de la Recherche Scientifique (CNRS)-Université de La Réunion (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Météo France, Laboratoire d'aérologie (LAERO), Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées, Université du Québec à Montréal = University of Québec in Montréal (UQAM), Istituto Nazionale di Geofisica e Vulcanologia - Sezione di Palermo (INGV), Istituto Nazionale di Geofisica e Vulcanologia, Istituto Nazionale di Geofisica e Vulcanologia - Sezione di Catania (INGV), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Université de La Réunion (UR)-Centre National de la Recherche Scientifique (CNRS)-Météo-France, Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS)
Subjects: event.disaster_type, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, geography, geography.geographical_feature_category, 010504 meteorology & atmospheric sciences, Planetary boundary layer, Atmospheric sciences, 01 natural sciences, Strombolian eruption, Plume, Aerosol, Volcanic Gases, Troposphere, Geophysics, Volcano, 13. Climate action, Space and Planetary Science, Earth and Planetary Sciences (miscellaneous), Cloud condensation nuclei, event, 0105 earth and related environmental sciences
Abstract: International audience; 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.
Published: 2019

18. Novel insights on new particle formation derived from a pan-european observing system

Author: Karine Sellegri, F. Bianchi, Monica Crippa, André S. H. Prévôt, Claire Granier, Annele Virtanen, Axel Eriksson, Roy M. Harrison, G. de Leeuw, James Allan, J. P. Putaud, J. S. Henzing, Liqing Hao, Erik Swietlicki, Rafel Simó, Manuel Dall'Osto, Hans-Christen Hansson, Paolo Laj, Colin D. O'Dowd, Laurent Poulain, Maria Vidal, Timothy B. Onasch, Manjula R. Canagaratna, David C. S. Beddows, Ari Asmi, Douglas R. Worsnop, Markku Kulmala, K. Zemankova, Evelyn Freney, Spanish National Research Council (CSIC), National Centre for Atmospheric Science, University of Birmingham [Birmingham], Finnish Meteorological Institute (FMI), Leibniz Institute for Tropospheric Research (TROPOS), University of Eastern Finland, Laboratoire de météorologie physique (LaMP), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), European Commission - Joint Research Centre [Petten], University of Helsinki, Lund University [Lund], Laboratoire d'aérologie (LAERO), Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées, Department of Applied Mathematics and Institute of Theoretical Computer Science (Charles University), Charles University [Prague] (CU), Institut des Géosciences de l’Environnement (IGE), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Recherche pour le Développement (IRD)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Aerodyne Research Inc., European Project: 36071,EUCAARI, European Project: 624680,EC:FP7:PEOPLE,FP7-PEOPLE-2013-IOF,MANU(2014), Department of Physics, Polar and arctic atmospheric research (PANDA), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Laboratoire d'aérologie (LA), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Charles University [Prague], Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Universitat de Barcelona, Federal Office for the Environment (Switzerland), Ministerio de Economía y Competitividad (España), European Commission, and Natural Environment Research Council (UK)
Subjects: Statistical cluster, 010504 meteorology & atmospheric sciences, BIOGENIC EMISSIONS, Growth phase, Earth science, Seasonal variation, education, AIR-QUALITY, lcsh:Medicine, Urbanisation, 010501 environmental sciences, Environment, VOLATILE ORGANIC-COMPOUNDS, CHEMICAL-COMPOSITION, 01 natural sciences, 7. Clean energy, 114 Physical sciences, Article, CLOUD CONDENSATION NUCLEI, Cluster analysis, Pan european, Growth curve, SULFURIC-ACID, ATMOSPHERIC NUCLEATION, Contaminació atmosfèrica, Ozó atmosfèric, Cloud condensation nuclei, lcsh:Science, Aerosol, POSITIVE MATRIX FACTORIZATION, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Multidisciplinary, Atmospheric pollution, SIZE DISTRIBUTIONS, Biogenic emissions, lcsh:R, AEROSOL MASS-SPECTROMETER, Atmospheric ozone, Europe, 13. Climate action, [SDU]Sciences of the Universe [physics], Atmospheric chemistry, Particle, Environmental science, lcsh:Q, Environment & Sustainability
Abstract: Dall'Osto, Manuel ... et al.-- 11 pages, 4 figures, supplementary material https://dx.doi.org/10.1038/s41598-017-17343-9, The formation of new atmospheric particles involves an initial step forming stable clusters less than a nanometre in size (~10 nm). Although at times, the same species can be responsible for both processes, it is thought that more generally each step comprises differing chemical contributors. Here, we present a novel analysis of measurements from a unique multi-station ground-based observing system which reveals new insights into continental-scale patterns associated with new particle formation. Statistical cluster analysis of this unique 2-year multi-station dataset comprising size distribution and chemical composition reveals that across Europe, there are different major seasonal trends depending on geographical location, concomitant with diversity in nucleating species while it seems that the growth phase is dominated by organic aerosol formation. The diversity and seasonality of these events requires an advanced observing system to elucidate the key processes and species driving particle formation, along with detecting continental scale changes in aerosol formation into the future, We gratefully acknowledge support by the German Federal Environment Agency (Umweltbundesamt), grants no. 351 03 031 and 351 01 038, and UFOPLAN grant 3703 43 200 (title “Erfassung der Zahl feiner und ultrafeiner Partikel in der Außenluft”). [...] The study was funded by the Spanish Ministry of Economy through projects BIO-NUC (CGL2013-49020-R), and by the EU though the FP7-PEOPLE-2013-IOF programme (Project number 624680, MANU – Marine Aerosol NUcleations) and the Ramon y Cajal fellowship (RYC-2012-11922).The National Centre for Atmospheric Science NCAS Birmingham group is funded by the UK Natural Environment Research Council
Published: 2018

19. Experimental Evidence of the Feeding of the Free Troposphere with Aerosol Particles from the Mixing Layer

Author: Montoux Nadege, Evelyn Freney, Bouvier Laeticia, Sellegri Karine, Colomb Aurelie, Hervo Maxime, Asmi Eija, Rose Clemence, Chauvigne Aurelien, Picard David, Baray Jean-Luc, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Finnish Meteorological Institute (FMI), MeteoSwiss, Federal Office of Meteorology and Climatology MeteoSwiss, and Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, 010501 environmental sciences, Sedimentation, Air mass (solar energy), Atmospheric sciences, 01 natural sciences, Pollution, High altitude site, Aerosol, Trace gas, Troposphere, Lidar, 13. Climate action, Radiative transfer, Environmental Chemistry, Aerosol mass spectrometry, Environmental science, Long-range transport, Aerosol Mass Spectrometry, 0105 earth and related environmental sciences
Abstract: International audience; Aerosol particles emitted by both natural and anthropogenic sources have direct and indirect radiative impacts. Within the planetary mixing layer (ML), these particles are subjected to a large number of removal processes, e.g., rain, sedimentation, coagulation, and thus have a relatively short lifetime. Once aerosols are transported into the free troposphere (FT), their atmospheric lifetime increases significantly and they tend to be representative of large spatial areas. The work presented here shows evidence of anthropogenic emissions being transported from the ML to the FT during a cold period in February 2012. Using a wide range of in-situ measurements of aerosol chemical and physical properties at the Puy de Dome (PUY) station, as well as LIDAR measurements (at the Cezeaux site) of atmospheric back scattering we studied the exchange between the ML and the FT. Criteria used to identify when the PUY station was sampling in the ML or in the FT included mixing layer height estimates from LIDAR measurements, trace gas measurements, and air mass trajectories. Within the FT, we observed a gradual change in aerosol physical properties with increases in aerosol mass concentrations of up to 2 times the starting concentration, as well as increases in the number of larger particles (particle diameter >150 nm). Aerosol chemical properties showed increases in organic and nitrate particles. A series of linear fits were made through the data providing information on how different parameters change as a function of time. The impact of these changing aerosol properties are discussed in relation to the potential influence on aerosol direct and indirect effects. This work presents a unique combination of observations, and provide valuable data for future model validation.
Published: 2016

20. Aerosol sources in the western Mediterranean during summertime: a model-based approach

Author: Mounir Chrit, Karine Sartelet, Jean Sciare, Jorge Pey, José B. Nicolas, Nicolas Marchand, Evelyn Freney, Karine Sellegri, Matthias Beekmann, François Dulac, Centre d'Enseignement et de Recherche en Environnement Atmosphérique (CEREA), École des Ponts ParisTech (ENPC)-EDF R&D (EDF R&D), EDF (EDF)-EDF (EDF), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Laboratoire Chimie de l'environnement (LCE), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Laboratoire de Météorologie Physique - Clermont Auvergne (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, 13. Climate action, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, ChArMEx, [SDE.MCG]Environmental Sciences/Global Changes, 14. Life underwater, 01 natural sciences, [SDE.ES]Environmental Sciences/Environmental and Society, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences
Abstract: International audience; In the framework of ChArMEx (the Chemistry-Aerosol Mediterranean Experiment), the air quality model Polyphemus is used to understand the sources of inorganic and organic particles in the western Mediterranean and evaluate the uncertainties linked to the model parameters (mete-orological fields, anthropogenic and sea-salt emissions and hypotheses related to the model representation of conden-sation/evaporation). The model is evaluated by comparisons to in situ aerosol measurements performed during three consecutive summers (2012, 2013 and 2014). The model-to-measurement comparisons concern the concentrations of PM 10 , PM 1 , organic matter in PM 1 (OM 1) and inorganic aerosol concentrations monitored at a remote site (Ersa) on Corsica Island, as well as airborne measurements performed above the western Mediterranean Sea. Organic particles are mostly from biogenic origin. The model parameterization of sea-salt emissions has been shown to strongly influence the concentrations of all particulate species (PM 10 , PM 1 , OM 1 and inorganic concentrations). Although the emission of organic matter by the sea has been shown to be low, organic concentrations are influenced by sea-salt emissions; this is owing to the fact that they provide a mass onto which gaseous hydrophilic organic compounds can condense. PM 10 , PM 1 , OM 1 are also very sensitive to meteorology, which affects not only the transport of pollutants but also natural emissions (biogenic and sea salt). To avoid large and unrealistic sea-salt concentrations, a parameterization with an adequate wind speed power law is chosen. Sulfate is shown to be strongly influenced by anthropogenic (ship) emissions. PM 10 , PM 1 , OM 1 and sulfate concentrations are better described using the emission inventory with the best spatial description of ship emissions (EDGAR-HTAP). However, this is not true for nitrate, ammonium and chloride concentrations, which are very dependent on the hypotheses used in the model regarding condensation/evaporation. Model simulations show that sea-salt aerosols above the sea are not mixed with background transported aerosols. Taking the mixing state of particles with a dynamic approach to condensation/evaporation into account may be necessary to accurately represent inorganic aerosol concentrations.
Published: 2018

21. Response to reviewer 1

Author: Evelyn Freney
Published: 2018

22. Response to reviewer 3

Author: Evelyn Freney
Published: 2018

23. Aerosol composition and the contribution of SOA formation over Mediterranean forests

Author: Evelyn Freney, Karine Sellegri, Mounir Chrit, Kouji Adachi, Joel Brito, Antoine Waked, Agnès Borbon, Aurélie Colomb, Régis Dupuy, Jean-Marc Pichon, Laetitia Bouvier, Claire Delon, Corinne Jambert, Pierre Durand, Thierry Bourianne, Cécile Gaimoz, Sylvain Triquet, Anaïs Féron, Matthias Beekmann, François Dulac, Karine Sartelet, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre d'Enseignement et de Recherche en Environnement Atmosphérique (CEREA), École des Ponts ParisTech (ENPC)-EDF R&D (EDF R&D), EDF (EDF)-EDF (EDF), Japan Meteorological Agency (JMA), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'aérologie (LAERO), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique - Clermont Auvergne (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'aérologie (LA), Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées, Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique - Clermont Auvergne ( LaMP ), Institut national des sciences de l'Univers ( INSU - CNRS ) -Université Clermont Auvergne ( UCA ) -Centre National de la Recherche Scientifique ( CNRS ), Laboratoire de météorologie physique ( LaMP ), Centre National de la Recherche Scientifique ( CNRS ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Université Blaise Pascal - Clermont-Ferrand 2 ( UBP ), Centre d'Enseignement et de Recherche en Environnement Atmosphérique ( CEREA ), École des Ponts ParisTech ( ENPC ) -EDF R&D ( EDF R&D ), EDF ( EDF ) -EDF ( EDF ), Japan Meteorological Agency ( JMA ), Laboratoire inter-universitaire des systèmes atmosphèriques ( LISA ), Centre National de la Recherche Scientifique ( CNRS ) -Université Paris-Est Créteil Val-de-Marne - Paris 12 ( UPEC UP12 ) -Université Paris Diderot - Paris 7 ( UPD7 ) -Institut national des sciences de l'Univers ( INSU - CNRS ), Laboratoire d'aérologie - LA ( LA ), Université Paul Sabatier - Toulouse 3 ( UPS ) -Institut national des sciences de l'Univers ( INSU - CNRS ) -Observatoire Midi-Pyrénées ( OMP ) -Centre National de la Recherche Scientifique ( CNRS ), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] ( LSCE ), Université de Versailles Saint-Quentin-en-Yvelines ( UVSQ ) -Commissariat à l'énergie atomique et aux énergies alternatives ( CEA ) -Université Paris-Saclay-Centre National de la Recherche Scientifique ( CNRS ), Centre National de la Recherche Scientifique ( CNRS ), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), and Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)
Subjects: [ SDU.OCEAN ] Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, 13. Climate action, ChArMEx, [ SDU.ENVI ] Sciences of the Universe [physics]/Continental interfaces, environment, 010501 environmental sciences, 15. Life on land, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, 01 natural sciences, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences
Abstract: International audience; As part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx), a series of aerosol and gas-phase measurements were deployed aboard the SAFIRE ATR42 research aircraft in summer 2014. The present study focuses on the four flights performed in late June early July over two forested regions in the south of France. We combine in situ observations and model simulations to aid in the understanding of secondary organic aerosol (SOA) formation over these forested areas in the Mediterranean and to highlight the role of different gas-phase precursors. The non-refractory particulate species measured by a compact aerosol time-of-flight mass spectrometer (cToF-AMS) were dominated by organ-ics (60 to 72 %) followed by a combined contribution of 25 % by ammonia and sulfate aerosols. The contribution from nitrate and black carbon (BC) particles was less than 5 % of the total PM 1 mass concentration. Measurements of non-refractory species from off-line transmission electron mi-croscopy (TEM) showed that particles have different mixing states and that large fractions (35 %) of the measured particles were organic aerosol containing C, O, and S but without inclusions of crystalline sulfate particles. The organic aerosol measured using the cToF-AMS contained only evidence of oxidized organic aerosol (OOA), without a contribution of fresh primary organic aerosol. Positive matrix factorization (PMF) on the combined organic-inorganic matrices separated the oxidized organic aerosol into a more-oxidized organic aerosol (MOOA), and a less-oxidized organic aerosol (LOOA). The MOOA component is associated with inorganic species and had higher contributions of m/z 44 than the LOOA factor. The LOOA factor is not associated with inorganic species and correlates well with biogenic volatile organic species measured with a proton-transfer-reaction mass spectrometer, such as isoprene and its oxidation products (methyl vinyl ketone, MVK; methacroleine, MACR; and iso-prene hydroxyhydroperoxides, ISOPOOH). Despite a significantly high mixing ratio of isoprene (0.4 to 1.2 ppbV) and its oxidation products (0.2 and 0.8 ppbV), the contribution of specific signatures for isoprene epoxydiols SOA (IEPOX-SOA) within the aerosol organic mass spectrum (m/z 53 and m/z 82) were very weak, suggesting that the presence of Published by Copernicus Publications on behalf of the European Geosciences Union. 7042 E. Freney et al.: Aerosol composition and the contribution of SOA formation isoprene-derived SOA was either too low to be detected by the cToF-AMS, or that SOA was not formed through IEPOX. This was corroborated through simulations performed with the Polyphemus model showing that although 60 to 80 % of SOA originated from biogenic precursors, only about 15 to 32 % was related to isoprene (non-IEPOX) SOA; the remainder was 10 % sesquiterpene SOA and 35 to 40 % monoter-pene SOA. The model results show that despite the zone of sampling being far from industrial or urban sources, a total contribution of 20 to 34 % of the SOA was attributed to purely anthropogenic precursors (aromatics and intermediate or semi-volatile compounds). The measurements obtained during this study allow us to evaluate how biogenic emissions contribute to increasing SOA concentrations over Mediterranean forested areas. Directly comparing these measurements with the Polyphemus model provides insight into the SOA formation pathways that are prevailing in these forested areas as well as processes that need to be implemented in future simulations.
Published: 2018

24. Supplementary material to 'Assessing the role of anthropogenic and biogenic sources on PM1 over Southern West Africa using aircraft measurements'

Author: Joel Brito, Evelyn Freney, Pamela Dominutti, Agnes Borbon, Sophie L. Haslett, Aurelie Colomb, Regis Dupuy, Cyrielle Denjean, Frederic Burnet, Thierry Bourrianne, Adrien Deroubaix, Karine Sellegri, Hugh Coe, Cyrille Flamant, Peter Knippertz, and Alfons Schwarzenboeck
Published: 2017

25. Supplementary material to 'Aerosol composition and the contribution of SOA formation over Mediterranean forests'

Author: Evelyn Freney, Karine Sellegri, Mounir Chrit, Kouji Adachi, Joel Brito, Antoine Waked, Agnès Borbon, Aurélie Colomb, Régis Dupuy, Jean-Marc Pichon, Laetitia Bouvier, Claire Delon, Corinne Jambert, Pierre Durand, Thierry Bourianne, Cécile Gaimoz, Sylvain Triquet, Anaïs Féron, Matthias Beekmann, François Dulac, and Karine Sartelet
Published: 2017

26. On the impact of anthropogenic emissions on biogenic SOA formation above West Africa: results from DACCIWA aircraft field campaign

Author: Joel Brito, Evelyn Freney, Aurélie Colomb, Régis Dupuy, Jonathan Duplissy, Cyrielle Denjean, Pamela Dominutti, Anneke Batenburg, Sophie Haslett, Christiane Schulz, Thierry Bourrianne, Frédéric Burnet, Agnès Borbon, Johannes Schneider, Stephan Borrmann, Hugh Coe, Karine Sellegri, Cyrille Flamant, Peter Knippertz, Alfons Schwarzenboeck, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Department of Physics [Helsinki], Falculty of Science [Helsinki], Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Instituto de Astronomia, Geofísica e Ciências Atmosféricas [São Paulo] (IAG), Universidade de São Paulo = University of São Paulo (USP), Max-Planck-Institut für Chemie (MPIC), Max-Planck-Gesellschaft, School of Earth and Environmental Sciences [Manchester] (SEES), University of Manchester [Manchester], Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institute for Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology (KIT), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Cardon, Catherine, University of Helsinki-University of Helsinki, Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Universidade de São Paulo (USP), Laboratoire de Météorologie Physique - Clermont Auvergne (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), Météo France-Centre National de la Recherche Scientifique (CNRS), Instituto de Astronomia, Geofisica e Ciencias Atmosfericas [Sao Paulo] (IAG), and Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDE] Environmental Sciences, [SDE]Environmental Sciences
Abstract: International audience; As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, airborne campaigns were designed to measure a large range of atmospheric constituents focusing on the improvement of our current understanding on the effect of anthropogenic emissions on regional climate. The targeted region, Southern West Africa, holds currently a population of over 340 million people, and is predicted by the United Nations to reach about 800 million by 2050. The climate in the region is characterized by a large-scale atmospheric circulation system which controls precipitation over a land area of about 6 million km2, directly impacting the water resources, agriculture and power generation of hundreds of millions of people. Besides its large natural variability, the West African monsoon system is also expected to be significantly affected by global and regional climate change, with large uncertainties on the role of local pollution. An important aspect assessing the impact of human activities on the local climate is thereby the understanding of aerosol sources and properties. The presented study details results of the DACCIWA measurement campaign using the French ATR42 research aircraft, which in combination with the German Falcon 20 and British Twin Otter aircraft, aimed to characterize physico-chemical properties of aerosols in the region using a suite of aerosol measurement techniques (e.g. C-TOF AMS, APITOF, SMPS, etc.) and supporting information from simultaneous trace gas measurements (e.g. PTRMS). This large dataset has been used to assess how anthropogenic emission (NOx, SO2, SO4) is impacting formation of biogenic secondary organic aerosol formation, in particular through the formation of isoprene epoxydiols (IEPOX). The recently collected data will certainly help understanding the coupling between human activities and regional climate in a sensitive, highly populated area.
Published: 2017

27. Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments

Author: Giancarlo Ciarelli, Emily A. Bruns, Colin D. O'Dowd, Urs Baltensperger, Evelyn Freney, André S. H. Prévôt, Monica Crippa, Samara Carbone, Mikko Äijälä, Imad El Haddad, Sebnem Aksoyoglu, Laurent Poulain, Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Department of Biology, Northern Arizona University [Flagstaff], JRC Institute for Environment and Sustainability (IES), European Commission - Joint Research Centre [Ispra] (JRC), Leibniz Institute for Tropospheric Research (TROPOS), University of Helsinki, Universidade de São Paulo (USP), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), National University of Ireland [Galway] (NUI Galway), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Universidade de São Paulo = University of São Paulo (USP), and Department of Physics
Subjects: biomass burning, Atmospheric Science, rethinking, 010504 meteorology & atmospheric sciences, aerosol, Fraction (chemistry), Scale (descriptive set theory), 010501 environmental sciences, Combustion, 7. Clean energy, 01 natural sciences, 114 Physical sciences, CAMX, experimental study, air-quality, Atmosphere, lcsh:Chemistry, volatility basis-set, multilinear engine, london, Apportionment, framework, 11. Sustainability, Air quality index, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Chemistry, emissions, modeling, source apportionment, parameterization, winter, lcsh:QC1-999, Aerosol, lcsh:QD1-999, 13. Climate action, Environmental chemistry, mass, smog, lcsh:Physics, performance, combustion
Abstract: International audience; We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was param-eterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from −61 to −29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64 % of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40 % to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were Published by Copernicus Publications on behalf of the European Geosciences Union. 7654 G. Ciarelli et al.: Modelling winter organic aerosol at the European scale with CAMx also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38 % with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still under-predicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.
Published: 2017

28. Spatial Extent of New Particle Events over the Mediterranean basin from multiple ground-based and airborne measurements

Author: Kevin Berland, Clémence Rose, Jorge Pey, Anais Culot, Evelyn Freney, Nikos Kalivitis, Giorgos Kouvaratis, José Carlos Cerro, Marc Mallet, Karine Sartelet, Matthias Beckmann, Thierry Bourriane, Greg Roberts, Nicolas Marchand, Nikolaos Mihalopoulos, and Karine Sellegri
Abstract: Over the last two decades, new particle formation (NPF), i.e. the formation of new particle clusters from gas-phase compounds followed by their growth to the 10–50 nm size range, has been extensively observed in the atmosphere at a given location, but their spatial extent rarely assessed. In this work, we use aerosol size distribution measurements performed simultaneously at Ersa (Corsica) and Finokalia (Crete) over a one-year period for analyzing the occurrence of NPF events in the Mediterranean area. The geographical location of these two sites, as well as the extended sampling period allow us to assess the spatial and temporal variability of atmospheric nucleation at a regional scale. Globally, Finokalia and Ersa show similar seasonalities in the monthly average nucleation frequencies, growth rates, and nucleation rates although the two stations are located more than 1000 km away from each other. Within this extended period, aerosol size distribution measurements were performed during an intensive campaign (July 3rd to August 12th 2013) from a ground based station on the island of Mallorca, as well as onboard the ATR-42 research aircraft. This unique combination of stationary and mobile measurements provides us with detailed insights into the horizontal and vertical development of the NPF process on the daily scale. During the intensive campaign, nucleation events occurred simultaneously both at Ersa and Mallorca over delimited time slots of several days, but different features were observed at Finokalia. The results highlight that the spatial extent of the NPF events over the Mediterranean Sea might be as large as several hundreds of kilometers, mainly determined by synoptic conditions. Airborne measurements gave additional information regarding the origin of the clusters detected above the sea. The selected cases depicted contrasting situations, with clusters formed in the marine boundary layer or initially nucleated above the continent or in the Free Troposphere (FT) and further transported above the sea.
Published: 2016

29. Interactions of mineral dust with pollution and clouds: An individual-particle TEM study of atmospheric aerosol from Saudi Arabia

Author: Evelyn Freney, Mihály Pósfai, Éva Tompa, Peter R. Buseck, Duncan Axisa, and Roelof Bruintjes
Subjects: Calcite, Atmospheric Science, Ammonium sulfate, Drop (liquid), Mineralogy, Mineral dust, medicine.disease_cause, complex mixtures, Soot, Aerosol, chemistry.chemical_compound, chemistry, medicine, Sulfate, Clay minerals, Geology
Abstract: Aerosol particles from desert dust interact with clouds and influence climate on regional and global scales. The Riyadh (Saudi Arabia) aerosol campaign was initiated to study the effects of dust particles on cloud droplet nucleation and cloud properties. Here we report the results of individual-particle studies of samples that were collected from an aircraft in April 2007. We used analytical transmission electron microscopy, including energy-dispersive X-ray spectrometry, electron diffraction, and imaging techniques for the morphological, chemical, and structural characterization of the particles. Dust storms and regional background conditions were encountered during four days of sampling. Under dusty conditions, the coarse (supermicrometer) fraction resembles freshly crushed rock. The particles are almost exclusively mineral dust grains and include common rock-forming minerals, among which clay minerals, particularly smectites, are most abundant. Unaltered calcite grains also occur, indicating no significant atmospheric processing. The particles have no visible coatings but some contain traces of sulfur. The fine (submicrometer) fraction is dominated by particles of anthropogenic origin, primarily ammonium sulfate (with variable organic coating and some with soot inclusions) and combustion-derived particles (mostly soot). In addition, submicrometer, iron-bearing clay particles also occur, many of which are internally mixed with ammonium sulfate, soot, or both. We studied the relationships between the properties of the aerosol and the droplet microphysics of cumulus clouds that formed above the aerosol layer. Under dusty conditions, when a large concentration of coarse-fraction mineral particles was in the aerosol, cloud drop concentrations were lower and droplet diameters larger than under regional background conditions, when the aerosol was dominated by submicrometer sulfate particles.
Published: 2013

30. Aerosol cloud activation in summer and winter at puy-de-Dôme high altitude site in France

Author: Clémence Rose, Evelyn Freney, Aurélie Colomb, Eija Asmi, Karine Sellegri, David Picard, Maxime Hervo, Laboratoire de Météorologie Physique (LaMP), and Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, Supersaturation, Particle number, 010504 meteorology & atmospheric sciences, Chemistry, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, Effects of high altitude on humans, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, complex mixtures, lcsh:QC1-999, Aerosol, lcsh:Chemistry, lcsh:QD1-999, 13. Climate action, Volume fraction, Cloud condensation nuclei, Particle, Particle size, lcsh:Physics, 0105 earth and related environmental sciences
Abstract: Cloud condensation nuclei (CCN) size distributions and numbers were measured for the first time at Puy-de-Dôme high altitude (1465 m a.s.l) site in Central France. Majority of the measurements were done at constant supersaturation (SS) of 0.24%, which was also deduced to be representative of the typical in-cloud SS at the site. CCN numbers during summer ranged from about 200 up to 2000 cm−3 and during winter from 50 up to 3000 cm−3. Variability of CCN number was explained by both particle chemistry and size distribution variability. The higher CCN concentrations were measured in continental, in contrast to marine, air masses. Aerosol CCN activity was described with a single hygroscopicity parameter κ. Range of this parameter was 0.29 ± 0.13 in summer and 0.43 ± 0.19 in winter. When calculated using SS of 0.51% during summer, κ of 0.22 ± 0.07 was obtained. The decrease with increasing SS is likely explained by the particle size dependent chemistry with smaller particles containing higher amounts of freshly emitted organic species. Higher κ values during winter were for the most part explained by the observed aged organics (analysed from organic m/z 44 ratio) rather than from aerosol organic to inorganic volume fraction. The obtained κ values also fit well within the range of previously proposed global continental κ of 0.27 ± 0.21. During winter, the smallest κ values and the highest organic fractions were measured in marine air masses. CCN closure using bulk AMS chemistry led to positive bias of 5% and 2% in winter and summer, respectively. This is suspected to stem from size dependent aerosol organic fraction, which is underestimated by using AMS bulk mass composition. Finally, the results were combined with size distributions measured from interstitial and whole air inlets to obtain activated droplet size distributions. Cloud droplet number concentrations were shown to increase with accumulation mode particle number, while the real in-cloud SS correspondingly decreased. These results provide evidence on the effects of aerosol particles on maximum cloud supersaturations. Further work with detailed characterisation of cloud properties is proposed in order to provide more quantitative estimates on aerosol effects on clouds.
Published: 2012

31. Supplementary material to 'Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments og'

Author: Giancarlo Ciarelli, Sebnem Aksoyoglu, Imad El Haddad, Emily A. Bruns, Monica Crippa, Laurent Poulain, Mikko Äijälä, Samara Carbone, Evelyn Freney, Colin O'Dowd, Urs Baltensperger, and André S. H. Prévôt
Published: 2016

32. Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments og

Author: Giancarlo Ciarelli, Sebnem Aksoyoglu, Imad El Haddad, Emily A. Bruns, Monica Crippa, Laurent Poulain, Mikko Äijälä, Samara Carbone, Evelyn Freney, Colin O'Dowd, Urs Baltensperger, and André S. H. Prévôt
Abstract: We evaluated a modified VBS (Volatility Basis Set) scheme to treat biomass burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework that accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from −61 % to −29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass burning-like aerosol (BBOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBOA fractions was found to represent 12 to 64 % of the total residential heating related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and transportation precursors contributed about 30–40 % to SOA formation (with increasing contributions at urban and near industrialized sites) whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60–70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semi-volatile range contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, higher volatility residential combustion precursors contributed from 15 to 38 % with no specific gradient among the stations. The new retrieved parameterization, although leading to a better agreement between model and observations, still under-predicts the SOA fraction suggesting remaining uncertainties in the new scheme or that other sources and/or formation mechanisms need to be elucidated.
Published: 2016

33. Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol

Author: Axel Eriksson, James Allan, Lea Hildebrandt, Alex Vermeulen, Jurgita Ovadnevaite, Claudia Mohr, Karine Sellegri, Andreas Wahner, Mikko Äijälä, Colin D. O'Dowd, Eiko Nemitz, Liqing Hao, Hendrik Elbern, Erik Swietlicki, Gordon McFiggans, Jose L. Jimenez, Risto Hillamo, René Otjes, C. Di Marco, E. Friese, Ari Laaksonen, Samara Carbone, Astrid Kiendler-Scharr, Monica Crippa, Hartmut Herrmann, Spyros N. Pandis, Evelyn Freney, André S. H. Prévôt, M. Dall Osto, Amewu A. Mensah, P. F. De Carlo, Patrick Schlag, Laurent Poulain, Manjula R. Canagaratna, Petri Tiitta, David Topping, Douglas R. Worsnop, H. C. Wu, Francesco Canonaco, Douglas A. Day, Observatoire de Physique du Globe de Clermont-Ferrand (OPGC), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique (LaMP), and Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA)
Subjects: atmospheric chemistry, 010504 meteorology & atmospheric sciences, southeastern united-states, Fraction (chemistry), organic nitrate, 010501 environmental sciences, high-resolution, 01 natural sciences, Atmospheric Sciences, Atmosphere, chemistry.chemical_compound, Nitrate, no3 oxidation, NOx, 0105 earth and related environmental sciences, particulate matter, model, isoprene oxidation, Particulates, Aerosol, Chemistry, Geophysics, field study, chemistry, mass-spectrometer data, 13. Climate action, [SDU]Sciences of the Universe [physics], Environmental chemistry, Atmospheric chemistry, General Earth and Planetary Sciences, Particle, anthropogenic emissions, chemical-composition, secondary
Abstract: International audience; In the atmosphere nighttime removal of volatile organic compounds is initiated to a large extent by reaction with the nitrate radical (NO3) forming organic nitrates which partition between gas and particulate phase. Here we show based on particle phase measurements performed at a suburban site in the Netherlands that organic nitrates contribute substantially to particulate nitrate and organic mass. Comparisons with a chemistry transport model indicate that most of the measured particulate organic nitrates are formed by NO3 oxidation. Using aerosol composition data from three intensive observation periods at numerous measurement sites across Europe, we conclude that organic nitrates are a considerable fraction of fine particulate matter (PM1) at the continental scale. Organic nitrates represent 34% to 44% of measured submicron aerosol nitrate and are found at all urban and rural sites, implying a substantial potential of PM reduction by NOx emission control.
Published: 2016

34. Regional Modeling of Aerosol Chemical Composition at the Puy de Dôme (France)

Author: Luc Patryl, Evelyn Freney, Aurélie Colomb, Nadine Chaumerliac, Alexandre Berger, Laurent Deguillaume, Christelle Barbet, Patrick Armand, Karine Sellegri, and Maud Leriche
Subjects: chemistry.chemical_compound, chemistry, Secondary organic aerosols, Biogenic emissions, Environmental science, Aerosol chemical composition, Particulates, Mass spectrometry, Atmospheric sciences, Aerosol
Abstract: Organic aerosols (OA) represent a large fraction (from 20 to 90 %) of the submicron particulate mass and it is mainly composed of secondary organic aerosols (SOA). Despite the ubiquity of OA in the atmosphere, there are still large uncertainties in understanding the formation pathways of SOA. Consequently, OA sources and physico-chemical transformations during their transport are poorly represented in chemistry-transport models and large gaps still remain between simulated and measured OA concentrations. The ability of the WRF-CHEM model to reproduce the organic aerosol mass concentration originated from anthropogenic or/and biogenic emissions is evaluated. From this perspective, simulations for two contrasted air masses are performed with WFR-Chem using the Volatility Basis Set (VBS) approach dedicated to the formation of SOA. Simulations results are compared to aerosol measurements performed at the puy de Dome station with a compact Time-of-Flight Aerosol Mass Spectrometer for two episodes in autumn 2008 and in summer 2010. Moreover, measurements of both anthropogenic and biogenic VOCs are used to access the capacity of the WRF-Chem model to correctly simulate the concentrations levels of the gas precursors of the SOA.
Published: 2016

35. Size distribution and optical properties of mineral dust aerosols transported in the western Mediterranean

Author: G. Momboisse, Paola Formenti, Sylvain Triquet, Andrea Mazzino, Karine Sellegri, Servanne Chevaillier, Noël Grand, A. Schwarzenbock, Marc Mallet, T. Bourrianne, Federico Cassola, Evelyn Freney, C. Denjean, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Istituto di Scienze dell'Atmosfera e del Clima [Lecce] (ISAC), Consiglio Nazionale delle Ricerche [Roma] (CNR), Centre national de recherches météorologiques (CNRM), Météo France-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique - Clermont Auvergne (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'aérologie (LA), Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées, Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique (LaMP), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d'aérologie (LAERO), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS)
Subjects: Mediterranean climate, Angstrom exponent, Atmospheric Science, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Mineral dust, Atmospheric sciences, 01 natural sciences, Mediterranean Basin, complex mixtures, lcsh:Chemistry, Radiative transfer, 0105 earth and related environmental sciences, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Single-scattering albedo, turbulence, particle dispersion, lcsh:QC1-999, Aerosol, Deposition (aerosol physics), lcsh:QD1-999, 13. Climate action, [SDU]Sciences of the Universe [physics], Climatology, Environmental science, Atmospheric Science, particle dispersion, turbulence, lcsh:Physics
Abstract: This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational data set necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin and understanding their atmospheric transport at global scale.
Published: 2016

36. Evaluation of Aerosol Chemical Composition Simulations by the WRF-Chem Model at the Puy de Dôme Station (France)

Author: Maud Leriche, Christelle Barbet, Karine Sellegri, Patrick Armand, Nadine Chaumerliac, Evelyn Freney, Aurélie Colomb, Laurent Deguillaume, Luc Patryl, Service de néphrologie et immunologie clinique [CHRU Tours], Centre Hospitalier Régional Universitaire de Tours (CHRU Tours)-Hôpital Bretonneau-Université de Tours (UT), Laboratoire de météorologie physique (LaMP), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Laboratoire d'aérologie (LAERO), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Détection et de Géophysique (CEA) (LDG), DAM Île-de-France (DAM/DIF), Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Service de néphrologie et immunologie clinique, Hôpital Bretonneau-Université de Tours-Centre Hospitalier Régional Universitaire de Tours (CHRU Tours), Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université Fédérale Toulouse Midi-Pyrénées
Subjects: High concentration, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, Meteorology, Dome, Aerosol chemical composition, 010501 environmental sciences, 7. Clean energy, 01 natural sciences, Pollution, Aerosol, 13. Climate action, Weather Research and Forecasting Model, Environmental Chemistry, Environmental science, Mass concentration (chemistry), ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, Oxidation rate
Abstract: The high altitude Puy de Dome (PUY) research station, located at 1465 m a.s.l. in central France, hosts many instruments allowing continuous measurements and intensive campaigns to measure meteorological parameters, gas-phase species, aerosol and cloud properties. Aerosol chemical composition measurements provided by a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS) are used to evaluate the WRF-Chem model and more precisely its ability to simulate organic aerosol (OA) for a particular event in summer 2010. Using the Volatility Basis Set approach (VBS), dedicated to the formation of secondary organic aerosol (SOA), the WRF-Chem model strongly underestimates the high concentration levels of OA observed at the PUY station: 12.5 µg m–3 were observed and only 2.6 µg m–3 were simulated. By means of several measurements of gas-phase volatile organic compounds (VOCs), the robustness of both emissions and SOA formation processes in the WRF-Chem model was tested. The underestimation of the OA mass concentration appears to be mainly due to a misrepresentation of the oxidation rate of the organic condensable vapours (OCVs) and the SOA yields of both anthropogenic and biogenic VOCs in the VBS parameterization.
Published: 2016

37. The Queensland Cloud Seeding Research Program

Author: Matthew Pocernich, Peter R. Buseck, Roger Stone, Scott Collis, Roelof Bruintjes, Steven T. Siems, Charles A. Knight, Louise Wilson, Merhala Thurai, Acacia Pepler, Courtney Weeks, Peter T. May, V. N. Bringi, Lynne Turner, Sarah A. Tessendorf, Harald Richter, Michael J. Manton, James W. Wilson, Evelyn Freney, Stuart Piketh, Rita D. Roberts, Roelof Burger, David McRae, Michael Dixon, Kyoko Ikeda, Duncan Axisa, Eric Nelson, Don R. Collins, and Justin R. Peter
Subjects: Atmospheric Science, Research program, education.field_of_study, Meteorology, Population, Cloud seeding, Environmental science, Seeding, Economic shortage, Precipitation, education
Abstract: As a response to extreme water shortages in southeast Queensland, Australia, brought about by reduced rainfall and increasing population, the Queensland government decided to explore the potential for cloud seeding to enhance rainfall. The Queensland Cloud Seeding Research Program (QCSRP) was conducted in the southeast Queensland region near Brisbane during the 2008/09 wet seasons. In addition to conducting an initial exploratory, randomized (statistical) cloud seeding study, multiparameter radar measurements and in situ aircraft microphysical data were collected. This comprehensive set of observational platforms was designed to improve the physical understanding of the effects of both ambient aerosols and seeding material on precipitation formation in southeast Queensland clouds. This focus on gaining physical understanding, along with the unique combination of modern observational platforms utilized in the program, set it apart from previous cloud seeding research programs. The overarching goals of the ...
Published: 2012

38. Seasonal variations in aerosol particle composition at the puy-de-Dôme research station in France

Author: Francesco Canonaco, J. Boulon, Paolo Laj, Ralf Weigel, Karine Sellegri, Jean-Marc Pichon, Maxime Hervo, André S. H. Prévôt, Evelyn Freney, Aurélie Colomb, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA), and CNRS-INSU
Subjects: Atmospheric Science, Planetary boundary layer, Atmospheric sciences, Mass spectrometry, lcsh:QC1-999, Aerosol, Troposphere, lcsh:Chemistry, chemistry.chemical_compound, Nitrate, chemistry, lcsh:QD1-999, [SDU]Sciences of the Universe [physics], [SDE]Environmental Sciences, Mass spectrum, Particle, Equivalent potential temperature, lcsh:Physics
Abstract: Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD) research station (1465 m) in autumn (September and October 2008), winter (February and March 2009), and summer (June 2010) using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m−3 up to 27 μg m−3. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA) and a semi-volatile organic aerosol particle (SV-OOA). Correlations of the LV-OOA components with fragments of m/z 60 and m/z 73 (mass spectral markers of wood burning) during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL) or in the free troposphere (FT)/residual layer (RL). We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL/FT airmasses contain high mass fractions of sulphate and LV-OOA. This study provides unique insights into the effects of season and airmass variability on regional aerosol particles measured at an elevated site.
Published: 2011

39. The Dynamic Shape Factor of Sodium Chloride Nanoparticles as Regulated by Drying Rate

Author: Zhe Wang, M. L. Smith, Ernie R. Lewis, Evelyn Freney, Stephen M. King, Ulrich Pöschl, Scot T. Martin, Peter R. Buseck, Mikinori Kuwata, Qi Chen, W. Wang, and Thomas Rosenoern
Subjects: Supersaturation, Aqueous solution, Chemistry, Analytical chemistry, Evaporation, Mineralogy, Nanoparticle, Humidity, Pollution, Efflorescence, Environmental Chemistry, General Materials Science, Relative humidity, Shape factor
Abstract: The influence of drying rate on the dynamic shape factor χ of NaCl particles was investigated. The drying rate at the efflorescence relative humidity (ERH) of 45% was controlled in a laminar flow tube and varied from 5.5 ± 0.9 to 101 ± 3 RH s–1 at ERH, where RH represents one percent unit of relative humidity. Dry particles having mobility diameters of 23–84 nm were studied, corresponding to aqueous particles of 37–129 nm at the RH (57%) prior to drying. At each mobility diameter and drying rate, the critical supersaturation of cloud-condensation activation was also measured. The mobility diameter and the critical supersaturation were combined in an analysis to determine the value of χ. The measured values varied from 1.02 to 1.26. For fixed particle diameter the χ value decreased with increasing drying rate. For fixed drying rate, a maximum occurred in χ between 35- and 40-nm dry mobility diameter, with a lower χ for both smaller and larger particles. The results of this study, in conjunction with the in...
Published: 2010

40. Growth and single-crystal refinement of phase-III potassium nitrate, KNO3

Author: Laurence A. J. Garvie, Thomas L. Groy, Peter R. Buseck, and Evelyn Freney
Subjects: Inorganic chemistry, Stacking, Potassium nitrate, General Medicine, Ferroelectricity, General Biochemistry, Genetics and Molecular Biology, Crystallography, chemistry.chemical_compound, Temperature and pressure, Planar, chemistry, Polymorphism (materials science), Atom, Single crystal
Abstract: Oriented single crystals of the high-temperature phase of KNO3 (phase III), a ferroelectric compound that may also occur as an atmospheric aerosol particle, were grown at room temperature and pressure by atomizing a solution of KNO3 in water and allowing droplets to dry on a glass substrate. The crystals are up to 1 mm across and are stable unless mechanically disturbed. There is no evidence of the spontaneous transformation of phase III to the room-temperature stable phase (phase II), even after several months. Single-crystal structure determinations of phase III were obtained at 295 and 123 K. The unit cell regained its room-temperature dimensions after warming from 123 K. The phase-III KNO3 structure can be viewed as the stacking parallel to the c axis of alternating K atoms and planar NO3 groups. The NO3 groups connect the planes of K atoms, where each O is fourfold coordinated to one N and three K. Each K atom has nine O nearest neighbors, with three bonds at 2.813 and six at 2.9092 Å. The interatomic K—N—K distance alternates from 5.051 to 3.941 along the c axis. The N—O distances increase from 1.245 (2) Å at 295 K to 1.2533 (15) Å at 123 K. The nitrate group has a slight non-planarity, with the N atoms 0.011 Å above the O plane and directed toward the more distant K of the K—N—K chain.
Published: 2009

41. Deliquescence and Efflorescence of Potassium Salts Relevant to Biomass-Burning Aerosol Particles

Author: Evelyn Freney, Scot T. Martin, and Peter R. Buseck
Subjects: Scanning electron microscope, Potassium, Inorganic chemistry, food and beverages, Humidity, chemistry.chemical_element, Pollution, humanities, Aerosol, Efflorescence, chemistry, Environmental Chemistry, Particle, General Materials Science, Relative humidity, Environmental scanning electron microscope
Abstract: Particles containing potassium salts are common in biomass burning plumes and include compounds such as KCl, KNO 3 , and K 2 SO 4 . We determined the deliquescence and efflorescence relative humidities of single- and multi-component potassium salts using an environmental transmission electron microscope and an environmental scanning electron microscope. KCl particles deliquesced at a relative humidity (RH) of 85% and effloresced at 56%. K 2 SO 4 particles deliquesced at 96% and effloresced at 60%. KNO 3 particles grew continuously with increasing humidity. If KNO 3 particles were heat-treated at 104°C overnight, they deliquesced at an RH above 90%. Atomized solutions of multi-component potassium compounds (KCl & KNO 3 and KCl & K 2 SO 4 ) formed particles that contained distinct grains of each compound upon drying. Particles formed from the KCl & KNO 3 mixtures grew continuously with increasing humidity until deliquescence occurred at an RH of 82% and efflorescence occurred at 58%. Particles from the KCl ...
Published: 2009

42. Major contribution of neutral clusters to new particle formation at the interface between the boundary layer and the free troposphere

Author: Jonathan Duplissy, Jenni Kontkanen, Katrianne Lehtipalo, Clémence Rose, Karine Sellegri, Markku Kulmala, Heikki Junninen, Eija Asmi, Maxime Hervo, Mikko Sipilä, Evelyn Freney, Aurélie Colomb, Department of Physics, Aerosol-Cloud-Climate -Interactions (ACCI), Polar and arctic atmospheric research (PANDA), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Finnish Meteorological Institute (FMI), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, and University of Helsinki
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, LONG-TERM, SEASONAL-VARIATION, Population, Nucleation, ATMOSPHERIC AEROSOL NUCLEATION, 010501 environmental sciences, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, Atmospheric sciences, 01 natural sciences, 114 Physical sciences, DOME RESEARCH STATION, lcsh:Chemistry, Atmosphere, Troposphere, BOREAL FOREST, SULFURIC-ACID, Cluster (physics), education, 0105 earth and related environmental sciences, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, education.field_of_study, SIZE DISTRIBUTIONS, GROWTH-RATES, Chemistry, lcsh:QC1-999, Aerosol, Boundary layer, lcsh:QD1-999, 13. Climate action, Chemical physics, Particle, HIGH-ALTITUDE SITE, lcsh:Physics, AIR ION SPECTROMETER
Abstract: The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular at high altitude, where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around high-altitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to ~ 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report day-time concentrations of charged and neutral clusters (1 to 2.5 nm mobility diameter) recorded at the interface between the boundary layer (BL) and the FT as well as in the FT at the altitude site of Puy de Dôme (1465 m a.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the FT, and especially at the interface between the BL and the FT, the formation of 1.5 nm neutral clusters significantly exceeds the one of ionic clusters during NPF events, clearly indicating that they dominate in the nucleation process. We also observe that the total cluster concentration significantly increases during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. During the studied period, the nucleation process does not seem to be sulfuric acid-limited and could be promoted by the transport of pollutants to the upper troposphere, coupled with low temperatures.
Published: 2015

43. Interactions aérosols- rayonnement-climat en région méditerranéenne Impact de l'effet radiatif direct sur le cycle de l'eau

Author: Pierre Nabat, Hélène Ferré, Frédéric Auriol, G. Momboisse, Anaïs Féron, Nicolas Verdier, Karine Sellegri, Julien Totems, Jean-François Léon, Gérard Ancellet, Evelyn Freney, Pierre Durand, Luc Blarel, Matthieu Jeannot, I. Jankowiak, Cyrielle Denjean, Aurélie Colomb, Philippe Goloub, Patrick Chazette, Eric Hamonou, Marc Mallet, Sylvain Triquet, Michaël Sicard, Jacques Pelon, Benjamin Torres, Samuel Somot, L. Roblou, Didier Tanré, Véronique Pont, Gérard Brogniez, Laurence Fleury, Servanne Chevaillier, M Claeys, Noël Grand, Jean-Baptiste Renard, Thierry Podvin, T. Bourrianne, Laurent Menut, Jean Sciare, Yevgeny Derimian, Jean-François Doussin, Damien Vignelles, Sylvain Mailler, Dominique Lambert, Frédéric Parol, G. Rea, Paola Formenti, José Nicolas, François Dulac, Gregory Roberts, Alfons Schwarzenboeck, Fabien Solmon, Karine Desboeufs, Christian Verwaerde, Barbara D'Anna, Laboratoire d'aérologie (LAERO), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire d’Optique Atmosphérique - UMR 8518 (LOA), Institut national des sciences de l'Univers (INSU - CNRS)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Energy, Environment and Water Research Center (EEWRC), Cyprus Institute (CyI), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de recherches sur la catalyse et l'environnement de Lyon (IRCELYON), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), SEDOO, OMP Data Service, Observatoire Midi-Pyrénées (OMP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France, Interactions Aérosols Rayonnement (IAR), Institut national des sciences de l'Univers (INSU - CNRS)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Laboratoire de Météorologie Dynamique (UMR 8539) (LMD), Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-École polytechnique (X)-École des Ponts ParisTech (ENPC)-Centre National de la Recherche Scientifique (CNRS)-Département des Géosciences - ENS Paris, École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL), Météo-France, Universitat Politècnica de Catalunya [Barcelona] (UPC), Abdus Salam International Centre for Theoretical Physics [Trieste] (ICTP), Centre National d'Études Spatiales [Toulouse] (CNES), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France, Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées, Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Groupe d'étude de l'atmosphère météorologique (CNRM-GAME), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD), Département des Géosciences - ENS Paris, École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National de la Recherche Scientifique (CNRS)-École des Ponts ParisTech (ENPC)-École polytechnique (X)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC), Météo-France [Paris], Météo France, Laboratoire d'aérologie (LA), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille, Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées, Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille, Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), and École normale supérieure - Paris (ENS Paris)-École normale supérieure - Paris (ENS Paris)
Subjects: Earth's energy budget, Mediterranean climate, Méditerranée, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], forçage radiatif, Meteorology, télédétection par lidar, mesure aéroportée, Stratification (water), influence des aérosols, campagne de mesure, Atmospheric sciences, simulation climatique, SST, climat régional, Geography, bilan radiatif, 13. Climate action, [SDU.STU.CL]Sciences of the Universe [physics]/Earth Sciences/Climatology, précipitations
Abstract: International audience; Une grande campagne expérimentale a été réalisée en Méditerranée occidentale pendant l'été 2013 afin d'étudier l'impact des aérosols sur le bilan radiatif et le climat régional. Les observations obtenues dans plusieurs stations de surface, à bord de deux avions de recherche, sous ballons sondes plafonnants et par satellite ont documenté la distribution et les propriétés physicochimiques et optiques des particules. Cette campagne a vu se succéder des transports d'aérosols désertiques d'intensité modérée, absorbant modérément le rayonnement solaire et stratifiés verticalement. Les premières simulations climatiques indiquent un impact significatif des aérosols notamment sur la température de surface de la mer, les flux océan-atmosphère et les précipitations saisonnières.; An experimental campaign, coupled with three-dimensional modeling, was conducted in the western Mediterranean during the summer of 2013 to study the impact of aerosols on the radiative balance and climate of this region. In situ observations were obtained on the ground, aboard two research aircraft and balloons to characterize the physico-chemical and optical properties of particles and their vertical stratification. This campaign was mainly characterized by moderate events of desert aerosols. During these episodes, strong vertical stratification was observed and the measurements of the optical properties reveal moderate absorbing particles in the visible spectrum. Climate simulations indicate a significant impact of aerosols in particular by changing the surface temperature of the sea, the ocean-atmosphere fluxes and consequently seasonal precipitation.
Published: 2015

44. Airborne measurements of new particle formation in the free troposphere above the Mediterranean Sea during the HYMEX campaign

Author: Evelyn Freney, Alfons Schwarzenboeck, Aurélie Colomb, Karine Sellegri, Régis Dupuy, Mickael Ribeiro, T. Bourianne, Frédéric Burnet, J. M. Pichon, Clémence Rose, Laboratoire de Météorologie Physique (LaMP), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Groupe d'étude de l'atmosphère météorologique (CNRM-GAME), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, Atmospheric sciences, 01 natural sciences, lcsh:QC1-999, Aerosol, lcsh:Chemistry, Troposphere, Mediterranean sea, Altitude, lcsh:QD1-999, 13. Climate action, Scanning mobility particle sizer, Particle, Environmental science, Outflow, 14. Life underwater, lcsh:Physics, Air mass, 0105 earth and related environmental sciences
Abstract: While atmospheric new particle formation (NPF) has been observed in various environments and was found to contribute significantly to the total aerosol particle concentration, the production of new particles over open seas is poorly documented in the literature. Nucleation events were detected and analysed over the Mediterranean Sea using two condensation particle counters and a scanning mobility particle sizer on board the ATR-42 research aircraft during flights conducted between 11 September and 4 November 2012 in the framework of the HYMEX (HYdrological cycle in Mediterranean EXperiment) project. The main purpose of the present work was to characterize the spatial extent of the NPF process, both horizontally and vertically. Our findings show that nucleation is occurring over large areas above the Mediterranean Sea in all air mass types. Maximum concentrations of particles in the size range 5–10 nm (N5–10) do not systematically coincide with lower fetches (time spent by the air mass over the sea before sampling), and significant N5–10 values are found for fetches between 0 and 60 h depending on the air mass type. These observations suggest that nucleation events could be more influenced by local precursors originating from emission processes occurring above the sea, rather than linked to synoptic history. Vertical soundings were performed, giving the opportunity to examine profiles of the N5–10 concentration and to analyse the vertical extent of NPF. Our observations demonstrate that the process could be favoured above 1000 m, i.e. frequently in the free troposphere, and more especially between 2000 and 3000 m, where the NPF frequency is close to 50 %. This vertical distribution of NPF might be favoured by the gradients of several atmospheric parameters, together with the mixing of two air parcels, which could also explain the occurrence of the process at preferential altitudes. In addition, increased condensation sinks collocated with high concentrations of small particles suggest the occurrence of NPF events promoted by inputs from the boundary layer, most probably associated with convective clouds and their outflow. After their formation, particles slowly grow at higher altitudes to diameters of at least 30 nm while not being greatly depleted or affected by coagulation. Our analysis of the particle size distributions suggests that particle growth could decrease with increasing altitude.
Published: 2015

45. Major contribution of neutral clusters to new particle formation in the free troposphere

Author: Jonathan Duplissy, Jenni Kontkanen, Karine Sellegri, Evelyn Freney, Mikko Sipilä, Heikki Junninen, Katrianne Lehtipalo, Clémence Rose, Eija Asmi, M. Kulmala, and Maxime Hervo
Subjects: Troposphere, Chemistry, Chemical physics, Particle, Atmospheric sciences
Abstract: The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular in the free troposphere (FT) where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around high altitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to ~ 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report observations of charged and neutral clusters (1 to 2.5 nm mobility diameter) during day-time free tropospheric conditions at the altitude site of Puy de Dôme (1465 m a.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the free troposphere, the formation of 1.5 nm neutral clusters is about 40 times higher than the one of ionic clusters during NPF events, indicating that they dominate in the nucleation process. We also observe that the total cluster concentration increases by a factor of 5.5 during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. In the FT, the nucleation process does not seem to be sulphuric acid-limited, as previously suggested, and could be promoted by the transport of pollutants to the upper troposphere.
Published: 2014

46. Organic aerosol components derived from 25 ams data sets across europe using a consistent me-2 based source apportionment approach

Author: D. R. Worsnop, Evelyn Freney, Samara Carbone, Petri Tiitta, L. Hildebrandt Ruiz, Tuukka Petäjä, Amewu A. Mensah, Markku Kulmala, Peter F. DeCarlo, Darius Ceburnis, Colin D. O'Dowd, André S. H. Prévôt, Astrid Kiendler-Scharr, Heikki Junninen, Jose L. Jimenez, Karine Sellegri, Mikael Ehn, Laurent Poulain, Urs Baltensperger, Risto Hillamo, Eiko Nemitz, Gerard Capes, V. A. Lanz, Monica Crippa, A. Kortelainen, Jurgita Ovadnevaite, Axel Eriksson, James Allan, Erik Swietlicki, Mikko Äijälä, Manuel Dall'Osto, Spyros N. Pandis, Francesco Canonaco, Douglas A. Day, Sanna Saarikoski, Claudia Mohr, and Ari Laaksonen
Subjects: Atmospheric Science, new-york-city, Atmospheric sciences, high-resolution, 7. Clean energy, Atmospheric Sciences, lcsh:Chemistry, multilinear engine, Apportionment, Aerosol cloud, particle composition, 11. Sustainability, ddc:550, Biomass burning, Air quality index, quality interactions eucaari, 15. Life on land, Particulates, lcsh:QC1-999, factor-analytic models, Aerosol, Time resolved data, integrated project, lcsh:QD1-999, mass-spectrometer data, 13. Climate action, Environmental chemistry, positive matrix factorization, Environmental science, chemical-composition, Ambient data, lcsh:Physics
Abstract: Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May–June and September–October) and 2009 (February–March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.
Published: 2014

47. Secondary organic aerosol formation during June 2010 in Central Europe: measurements and modelling studies with a mixed thermodynamic-kinetic approach

Author: Evelyn Freney, Baerbel Langmann, Karine Sellegri, Laboratoire de Météorologie Physique (LaMP), and Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA)
Subjects: chemistry.chemical_classification, Atmospheric Science, Chemistry, Nucleation, medicine.disease, complex mixtures, lcsh:QC1-999, Aerosol, lcsh:Chemistry, Troposphere, lcsh:QD1-999, Chemical physics, [SDU]Sciences of the Universe [physics], Environmental chemistry, Particle-size distribution, [SDE]Environmental Sciences, medicine, Cloud condensation nuclei, Mass concentration (chemistry), Volatile organic compound, lcsh:Physics, Vapours
Abstract: Until recently secondary organic carbon aerosol (SOA) mass concentrations have been systematically underestimated by three-dimensional atmospheric-chemistry-aerosol models. With a newly proposed concept of aging of organic vapours, more realistic model results for organic carbon aerosol mass concentrations can be achieved. Applying a mixed thermodynamic-kinetic approach for SOA formation shifted the aerosol size distribution towards particles in the cloud condensation nuclei size range, thereby emphasising the importance of SOA formation schemes for modelling realistic cloud and precipitation formation. The additional importance of hetero-molecular nucleation between H2SO4 and organic vapours remains to be evaluated in three-dimensional atmospheric-chemistry-aerosol models. Here a case study is presented focusing on Puy-de-Dôme, France in June 2010. The measurements indicate a considerable increase in SOA mass concentration during the measurement campaign, which could be reproduced by modelling using a simplified thermodynamic-kinetic approach for SOA formation and increased biogenic volatile organic compound (VOC) precursor emissions. Comparison with a thermodynamic SOA formation approach shows a huge improvement in modelled SOA mass concentration with the thermodynamic-kinetic approach for SOA formation. SOA mass concentration increases by a factor of up to 6 accompanied by a slight improvement of modelled particle size distribution. Even though nucleation events at Puy-de-Dôme were rare during the chosen period of investigation, a weak event in the boundary layer could be reproduced by the model in a sensitivity study when nucleation of low-volatile secondary organic vapour is included. Differences in the model results with and without nucleation of organic vapour are visible in the lower free troposphere over several days. Taking into account the nucleation of organic vapour leads to an increase in accumulation mode particles due to coagulation and condensational growth of nucleation and Aitken mode particles.
Published: 2014

48. Characterizing the impact of urban emissions on regional aerosol particles: airborne measurements during the MEGAPOLI experiment

Author: Karine Sellegri, Agnès Borbon, Francesco Canonaco, Alfons Schwarzenboeck, Matthias Beekmann, André S. H. Prévôt, Jean-François Doussin, Evelyn Freney, Aurélie Colomb, Vincent Michoud, L. Gomes, Jean-Marc Pichon, Nadir Amarouche, T. Bourianne, Suzanne Crumeyrolle, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Clermont Auvergne (UCA), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Paul Scherrer Institute (PSI), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Division technique INSU/SDU (DTI), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), The publication of this article is financed by CNRS-INSU, Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Laboratoire de Météorologie Physique - Clermont Auvergne (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Groupe d'étude de l'atmosphère météorologique (CNRM-GAME), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences de l'Univers (INSU/SPU), Centre National de la Recherche Scientifique (CNRS), Laboratoire Inter-Université des Systèmes Atmosphériques, Université Paris-Est (UPE), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS)
Subjects: Pollution, Atmospheric Science, 010504 meteorology & atmospheric sciences, media_common.quotation_subject, 010501 environmental sciences, medicine.disease_cause, 01 natural sciences, 7. Clean energy, lcsh:Chemistry, chemistry.chemical_compound, Nitrate, 11. Sustainability, medicine, Mass concentration (chemistry), ComputingMilieux_MISCELLANEOUS, NOx, 0105 earth and related environmental sciences, media_common, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Soot, lcsh:QC1-999, Plume, Aerosol, chemistry, lcsh:QD1-999, 13. Climate action, [SDU]Sciences of the Universe [physics], Environmental chemistry, [SDE]Environmental Sciences, Particle, Environmental science, lcsh:Physics
Abstract: The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation yields, we were able to predict ~50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA and have an impact on aerosol composition on a regional scale.
Published: 2014

49. Hygroscopic properties and mixing state of aerosol measured at the high-altitude site Puy de Dôme (1465 m a.s.l.), France

Author: Maxime Hervo, P. Villani, Karine Sellegri, Evelyn Freney, H. Holmgren, Clémence Rose, Paolo Laj, Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Physique - Clermont Auvergne (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne (UCA)-Centre National de la Recherche Scientifique (CNRS), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), and Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, 010504 meteorology & atmospheric sciences, Chemistry, Planetary boundary layer, 010501 environmental sciences, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, Atmospheric sciences, 01 natural sciences, lcsh:QC1-999, Degree (temperature), Aerosol, lcsh:Chemistry, Troposphere, Boundary layer, lcsh:QD1-999, 13. Climate action, Particle, Particle size, lcsh:Physics, Air mass, 0105 earth and related environmental sciences
Abstract: A Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France, periodically from September 2008 to January 2010, and almost continuously from October 2010 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values, GFs, are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of oceanic aerosol can be explained by large proportions of inorganic aerosol and sea salts. Aerosols measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less-hygroscopic mode (GF < 1.3), a hygroscopic mode (GF~1.3–1.7) and a more-hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less-hygroscopic mode or the hygroscopic mode, and only few of them have more-hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when the aerosol is found with two or more aerosol populations with different hygroscopic properties, increases with particle size (average yearly values are 20, 28 and 45 {%} for 25, 50, and 165 nm particles, respectively). The degree of external mixing is more sensitive to season than to air mass type, and it is higher in the cold seasons than in the warm seasons. With more than two years of nearly continuous measurements, this study gathers the results from one of the longest data sets of hygroscopic growth factor measurements to date, allowing a statistically relevant hygroscopic growth parameterization to be determined as a function of both air mass type and season.
Published: 2014

50. Charged and Neutral Binary Nucleation of Sulfuric Acid in Free Troposphere Conditions

Author: Jonathan Duplissy, Joonas Merikanto, Karine Sellegri, Clemence Rose, Eija Asmi, Evelyn Freney, Heikki Juninen, Mikko Sipilä, Hanna Vehkamaki, Markku Kulmala, null CLOUD collaboration, DeMott, Paul J., and ODowd, C. D.
Subjects: Chemistry, Nucleation, Analytical chemistry, 020206 networking & telecommunications, Sulfuric acid, 02 engineering and technology, Atmospheric sciences, 7. Clean energy, Ion, Troposphere, chemistry.chemical_compound, 13. Climate action, Atmospheric chemistry, 0202 electrical engineering, electronic engineering, information engineering, 020201 artificial intelligence & image processing, Relative humidity, Classical nucleation theory, Tropopause
Abstract: We present a data set of binary nucleation of sulfuric acid and water, measured in the CLOUD chamber at CERN during the CLOUD3 and CLOUD5 campaigns. Four parameters have been varied to cover neutral and ion-induced binary nucleation processes: Sulfuric acid concentration (1e5 to 1e8 molecules per cm^(−3)), relative humidity (10% to 80%), temperature (208-293K) and ion concentration (0-4000 ions per cm^(−3)). In addition, classical nucleation theory implemented with hydrates and ion induced nucleation is compared with the data set. Our model and data are also compared with nucleation rates measured at Puy de Dome in the tropopause.
Published: 2013

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