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1. Design and evaluation of BOOGIE: a collector for the analysis of cloud composition and processes: Biological, Organics, Oxidants, soluble Gases, inorganic Ions and metal Elements.

Author

Vaitilingom, Mickael, Bernard, Christophe, Ribeiro, Mickael, Berthod, Christophe, Bianco, Angelica, and Deguillaume, Laurent

Subjects
METAL ions, COMPUTATIONAL fluid dynamics, CLOUD droplets, ATMOSPHERIC chemistry, OXIDIZING agents
Abstract

Cloud/fog droplets comprise a myriad of chemical compounds and are living environments in which microorganisms are present and active. These chemical and biological elements can evolve in various ways within the cloud system, and the aqueous transformation of chemicals contributes to atmospheric chemistry. In situ cloud studies are fundamental in this sense, because they enable us to study the variability in cloud chemical composition as a function of environmental conditions and assess their potential for transforming chemical compounds. To achieve this objective, cloud water collectors have been developed in recent decades to recover water from clouds and fogs using different designs and collection methods. In this study, a new active ground-based cloud collector was developed and tested for sampling cloud water to assess the cloud microbiology and chemistry. This new instrument, BOOGIE, is an easy mobile sampler for cloud water collection with the objective of being cleanable and sterilisable, respecting chemical and microbial cloud integrity, and presenting an efficient collection rate of cloud water. Computational fluid dynamics simulations were performed to theoretically assess the capture of cloud droplets by this new sampler. Few turbulences have been observed inside the collector and a 50 % collection efficiency cutoff of 10 µm has been estimated. The collector was deployed at Puy de Dôme station under cloudy conditions for evaluation. The water collection rates were measured at 156 ± 52 mL h-1 for a collection of 17 cloud events; considering the measured liquid water content, the sampling efficiency of this new collector has been estimated at 87.2 ± 8.6 % over the same set of cloud events. BOOGIE was compared with other active cloud collectors commonly used by the scientific community (Cloud Water Sampler and Caltech Active Strand Cloud Collector version 2). Four cloud events were collected; the three samplers presented similar collection efficiencies (between 79 % and 88 % on average). The measured ionic composition was comparable even if differences were highlighted between collectors, the consequence of different designs, and the intrinsic homogeneity in the chemical composition within the cloud system. [ABSTRACT FROM AUTHOR]

Published
2024
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2. Molecular composition of clouds: a comparison between samples collected at tropical (Réunion Island, France) and mid-north (Puy de Dôme, France) latitudes.

Author

Pailler, Lucas, Deguillaume, Laurent, Lavanant, Hélène, Schmitz, Isabelle, Hubert, Marie, Nicol, Edith, Ribeiro, Mickaël, Pichon, Jean-Marc, Vaïtilingom, Mickaël, Dominutti, Pamela, Burnet, Frédéric, Tulet, Pierre, Leriche, Maud, and Bianco, Angelica

Subjects
CARBON content of water, DISSOLVED organic matter, MOLECULAR clouds, CHEMICAL formulas, PRINCIPAL components analysis, TERPENES
Abstract

The composition of dissolved organic matter of cloud water has been investigated through non-targeted high-resolution mass spectrometry on only a few samples that were mostly collected in the Northern Hemisphere in the USA, Europe and China. There remains, therefore, a lack of measurements for clouds located in the Southern Hemisphere, under tropical conditions and influenced by forest emissions. As a matter of fact, the comparison of the composition of clouds collected in different locations is challenging since the methodology for the analysis and data treatment is not standardized. In this work, the chemical composition of three samples collected at Réunion Island (REU) during the BIO-MAÏDO field campaign, in the Indian Ocean, with influences from marine, anthropogenic and biogenic (tropical) emissions, is investigated and compared to the chemical composition of samples collected at the Puy de Dôme (PUY) observatory in France. The same methodology of analysis and data treatment was employed, producing a unique dataset for the investigation of the molecular composition of organic matter in cloud water. Besides the analysis of elemental composition, we investigated the carbon oxidation state (OSC) of dissolved organic matter, finding that overall samples collected at PUY are more oxidized than those collected at REU. Molecular formulas were also classified based on stoichiometric elemental ratios, showing the high frequency and abundance of reduced organic compounds, classified as lipids (LipidC), in this matrix, which led to a search for terpene oxidation products in cloud water samples. To better discriminate between samples collected at PUY and REU, statistical analysis (principal component analysis and agglomerative hierarchical clustering) was performed on the ensemble of molecular formulas and their intensities. Samples collected at REU have a different composition from samples collected at PUY, which is mainly linked to different primary sources, the processing of organic matter in cloud water and the influence of different primary emissions at the two locations. [ABSTRACT FROM AUTHOR]

Published
2024
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4. Measurement report: Bio-physicochemistry of tropical clouds at Maïdo (Réunion, Indian Ocean): overview of results from the BIO-MAÏDO campaign.

Author

Leriche, Maud, Tulet, Pierre, Deguillaume, Laurent, Burnet, Frédéric, Colomb, Aurélie, Borbon, Agnès, Jambert, Corinne, Duflot, Valentin, Houdier, Stéphan, Jaffrezo, Jean-Luc, Vaïtilingom, Mickaël, Dominutti, Pamela, Rocco, Manon, Mouchel-Vallon, Camille, El Gdachi, Samira, Brissy, Maxence, Fathalli, Maroua, Maury, Nicolas, Verreyken, Bert, and Amelynck, Crist

Subjects
TURBULENT boundary layer, MICROBIOLOGICAL aerosols, VOLATILE organic compounds, OXALIC acid, AIR masses, TRADE winds, AIRWAYS (Aeronautics)
Abstract

The BIO-MAÏDO (Bio-physicochemistry of tropical clouds at Maïdo: processes and impacts on secondary organic aerosols formation) campaign was conducted from 13 March to 4 April 2019 on the tropical island of Réunion. The main objective of the project was to improve understanding of cloud impacts on the formation of secondary organic aerosols (SOA) from biogenic volatile organic compound (BVOC) precursors in a tropical environment. Instruments were deployed at five sites: a receptor site, Maïdo Observatory (MO) at 2165 m a.s.l. and four sites along the slope of the Maïdo mountain. Observations include measurements of volatile organic compounds (VOCs) and characterization of the physical, chemical and biological (bacterial diversity and culture-based approaches) properties of aerosols and cloud water. Turbulent parameters of the boundary layer, radiative fluxes and emissions fluxes of BVOCs from the surrounding vegetation were measured to help interpret observed chemical concentrations in the different phases. Dynamical analyses showed two preferred trajectory routes for air masses arriving at MO during the daytime. Both trajectories correspond to return branches of the trade winds associated with upslope thermal breezes, where air masses likely encountered cloud processing. The highest mixing ratios of oxygenated VOCs (OVOCs) were measured above the site located in the endemic forest and the highest contribution of OVOCs to total VOCs at MO. Chemical compositions of particles during daytime showed higher concentrations of oxalic acid, a tracer of cloud processing and photochemical aging, and a more oxidized organic aerosol at MO than at other sites. Approximately 20 % of the dissolved organic compounds were analyzed. Additional analyses by ultra-high-resolution mass spectrometry will explore the complexity of the missing cloud organic matter. [ABSTRACT FROM AUTHOR]

Published
2024
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6. Molecular composition of clouds: a comparison between samples collected at tropical (Réunion Island, France) and mid-north (puy de Dôme, France) latitudes.

Author

Pailler, Lucas, Deguillaume, Laurent, Lavanant, Hélène, Schmitz, Isabelle, Hubert, Marie, Nicol, Edith, Ribeiro, Mickaël, Pichon, Jean-Marc, Vaïtilingom, Mickaël, Dominutti, Pamela, Burnet, Frédéric, Tulet, Pierre, Leriche, Maud, and Bianco, Angelica

Abstract

The composition of cloud water dissolved organic matter has been investigated through non-targeted high resolution mass spectrometry only on few samples, mostly collected in the Northern hemisphere, in USA, Europe and China. Nevertheless, there is a lack of measurements for clouds located in the Southern Hemisphere, under tropical conditions and influenced by forest emissions. Moreover, the comparison of the composition of cloud samples collected in different locations is not trivial, since the methodology for the analysis and data treatment are not standardized. In this work, the chemical composition of three samples collected at Reunion Island (REU) during the BIO-MAÏDO field campaign, in the Indian Ocean, with influences from marine, anthropogenic and biogenic (tropical) emissions is investigated and compared to the chemical composition of samples collected at the puy de Dôme (PUY) observatory, in France. The same methodology of analysis and data treatment was employed, producing a unique dataset for the investigation of molecular composition of organic matter in cloud water. Besides the analysis of elemental composition, we investigated the carbon oxidation state (OSC) of dissolved organic matter, finding that overall samples collected at PUY are more oxidized than those collected at REU. Molecular formulas were also classified based on stoichiometric elemental ratios, showing the high frequency and abundance of reduced organic compounds, classified as lipids (LipidC), in this matrix, which led to search for terpenes oxidation products in cloud water samples. To better discriminate between samples collected at PUY and at REU, statistical analysis (principal component analysis and agglomerative hierarchical clustering) was performed on the ensemble of molecular formulas and their intensities. Samples collected at REU, have a different composition from samples collected at PUY, mainly linked to the processing of organic matter in cloud water, but also to the influence of different primary emissions at the two locations. [ABSTRACT FROM AUTHOR]

Published
2023
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10. Measurement Report: Bio-physicochemistry of tropical clouds at Maïdo (Réunion Island, Indian Ocean): overview of results from the BIO-MAÏDO campaign.

Author

Leriche, Maud, Tulet, Pierre, Deguillaume, Laurent, Burnet, Frédéric, Colomb, Aurélie, Borbon, Agnès, Jambert, Corinne, Duflot, Valentin, Houdier, Stéphan, Jaffrezo, Jean-Luc, Vaïtilingom, Mickaël, Dominutti, Pamela, Rocco, Manon, Mouchel-Vallon, Camille, El Gdachi, Samira, Brissy, Maxence, Fathalli, Maroua, Maury, Nicolas, Verreyken, Bert, and Amelynck, Crist

Abstract

The BIO-MAÏDO (Bio-physicochemistry of tropical clouds at Maïdo (Réunion Island): processes and impacts on secondary organic aerosols formation) campaign was conducted from the 13th of March to the 4th of April 2019 on the tropical Réunion Island and implied several scientific teams and state-of-the-art instrumentation. The campaign was part of the BIO-MAÏDO project with the main objective is to improve our understanding of cloud impacts on the formation of secondary organic aerosols (SOA) from biogenic volatile organic compounds (BVOC) precursors in a tropical environment. Instruments were deployed at five sites: a receptor site, the Maïdo observatory (MO) at 2165 m asl, and four sites along the slope of the Maïdo mountain. The obtained dataset includes measurements of the gas-phase mixing ratio of volatile organic compounds (VOC), the characterization of the physical, chemical, and biological (bacterial diversity) properties of aerosols and the characterization of the physical, chemical and biological (identification of viable bacteria through culture-based approaches) properties of the cloud water. In addition, the turbulent parameters of the boundary layer, radiative fluxes, and emissions fluxes of BVOC from the surrounding vegetation were measured to help with the interpretation of the observed chemical concentrations in the different phases. Dynamical analyses show two preferred trajectories routes for air masses arriving at MO during the daytime both corresponding to the return branches of the trade winds associated with the up-slopes thermal breezes. These air masses likely encountered cloud processing during transport along the slope. The highest mixing ratio of oxygenated VOC (OVOC) were measured above the site located in the endemic forest and the highest contribution of OVOC to total VOC at MO. Chemical composition of particles during the daytime shows a higher concentration of oxalic acid and a more oxidized organic aerosol at MO than at other sites along the slope. This is a signature of photochemical aerosols aging along the slope potentially influenced by cloud processing. Despite an in-depth analysis of organic compounds in cloud water, around 80% on average of dissolved organic compounds is undefined highlighting the complexity of the cloud organic matter. [ABSTRACT FROM AUTHOR]

Published
2023
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11. Assessing the efficiency of water-soluble organic compound biodegradation in clouds under various environmental conditions

Author

Pailler, Lucas, primary, Wirgot, Nolwenn, additional, Joly, Muriel, additional, Renard, Pascal, additional, Mouchel-Vallon, Camille, additional, Bianco, Angelica, additional, Leriche, Maud, additional, Sancelme, Martine, additional, Job, Aurélie, additional, Patryl, Luc, additional, Armand, Patrick, additional, Delort, Anne-Marie, additional, Chaumerliac, Nadine, additional, and Deguillaume, Laurent, additional

Published
2023
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14. Evaluation of the Sources, Precursors, and Processing of Aerosols at a High-Altitude Tropical Site

Author

Dominutti, Pamela, Chevassus, Emmanuel, Baray, Jean-Luc, Jaffrezo, Jean-Luc, Borbon, Agnès, Colomb, Aurélie, Deguillaume, Laurent, El Gdachi, Samira, Houdier, Stephan, Leriche, Maud, Metzger, Jean-Marc, Rocco, Manon, Tulet, Pierre, Sellegri, Karine, Freney, Evelyn, Institut des Géosciences de l’Environnement (IGE), Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), 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 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 de l'Atmosphère et des Cyclones (LACy), Institut national des sciences de l'Univers (INSU - CNRS)-Université de La Réunion (UR)-Centre National de la Recherche Scientifique (CNRS)-Météo-France, Centre ESCER, Université du Québec à Montréal = University of Québec in Montréal (UQAM), Observatoire des Sciences de l'Univers de La Réunion (OSU-Réunion), Institut national des sciences de l'Univers (INSU - CNRS)-Université de La Réunion (UR), ANR-18-CE01-0013,BIO-MAIDO,Bio-physicochimie des nuages tropicaux au Maïdo (Île de la Réunion) : processus et impacts sur la formation des aérosols organiques secondaires(2018), and European Project: 654109,H2020,H2020-INFRAIA-2014-2015,ACTRIS-2(2015)

Subjects
Atmospheric Science, Cloud processing, Positive matrix factorization, Space and Planetary Science, Geochemistry and Petrology, ToF-ACSM, [SDE.IE]Environmental Sciences/Environmental Engineering, [CHIM.ANAL]Chemical Sciences/Analytical chemistry, [SDE.MCG]Environmental Sciences/Global Changes, Secondary organic aerosols, Aqueous-phase chemistry, Southern Hemisphere, [SDE.ES]Environmental Sciences/Environmental and Society
Abstract

International audience; This work presents the results from a set of aerosol- and gas-phase measurements collected during the BIO-MAIDÖ field campaign in Reunion ́ between March 8 and April 5, 2019. Several offline and online sampling devices were installed at the Maidö Observatory (MO), a remote high-altitude site in the Southern Hemisphere, allowing the physical and chemical characterization of atmospheric aerosols and gases. The evaluation of short-lived gas-phase measurements allows us to conclude that air masses sampled during this period contained little or no anthropogenic influence. The dominance of sulfate and organic species in the submicron fraction of the aerosol is similar to that measured at other coastal sites.Carboxylic acids on PM10 showed a significant contribution of oxalic acid, a typical tracer of aqueous processed air masses, increasing at the end of the campaign. This result agrees with the positive matrix factorization analysis of the submicron organic aerosol, where more oxidized organic aerosols (MOOAs) dominated the organic aerosol with an increasing contribution toward the end of the campaign. Using a combination of air mass trajectories (model predictions), it was possible to assess the impact of aqueous phase processing on the formation of secondary organic aerosols(SOAs). Our results show how specific chemical signatures and physical properties of air masses, possibly affected by cloud processing, can be identified at Reunion. ́ These changes in properties are represented by a shift in aerosol size distribution to large diameters and an increased contribution of secondary sulfate and organic aerosols after cloud processing.

Published
2022

16. Influence of strong iron-binding ligands on cloud water oxidant capacity

Author

González, Aridane G., Bianco, Angelica, Boutorh, Julia, Cheize, Marie, Mailhot, Gilles, Delort, Nne-marie, Planquette, Helene, Chaumerliac, Nadine, Deguillaume, Laurent, Sarthou, Geraldine, González, Aridane G., Bianco, Angelica, Boutorh, Julia, Cheize, Marie, Mailhot, Gilles, Delort, Nne-marie, Planquette, Helene, Chaumerliac, Nadine, Deguillaume, Laurent, and Sarthou, Geraldine

Abstract

Iron (Fe) plays a dual role in atmospheric chemistry: it is involved in chemical and photochemical reactivity and serves as a micronutrient for microorganisms that have recently been shown to produce strong organic ligands. These ligands control the reactivity, mobility, solubility and speciation of Fe, which have a potential impact on Fe bioavailability and cloud water oxidant capacity. In this work, the concentrations of Fe-binding ligands and the conditional stability constants were experimentally measured for the first time by Competitive Ligand Exchange-Adsorptive Cathodic Stripping Voltammetry (CLE-ACSV) technique in cloud water samples collected at puy de Dôme (France). The conditional stability constants, which indicate the strength of the Fe-ligand complexes, are higher than those considered until now in cloud chemistry (mainly Fe-oxalate). To understand the effect of Fe complexation on cloud water reactivity, we used the CLEPS cloud chemistry model. According to the model results, we found that Fe complexation impacts the hydroxyl radical formation rate: contrary to our expectations, Fe complexation by natural organic ligands led to an increase in hydroxyl radical production. These findings have important impacts on cloud chemistry and the global iron cycle.

Published
2022
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18. Insights into tropical cloud chemistry in Réunion (Indian Ocean): results from the BIO-MAÏDO campaign

Author

Dominutti, Pamela A., primary, Renard, Pascal, additional, Vaïtilingom, Mickaël, additional, Bianco, Angelica, additional, Baray, Jean-Luc, additional, Borbon, Agnès, additional, Bourianne, Thierry, additional, Burnet, Frédéric, additional, Colomb, Aurélie, additional, Delort, Anne-Marie, additional, Duflot, Valentin, additional, Houdier, Stephan, additional, Jaffrezo, Jean-Luc, additional, Joly, Muriel, additional, Leremboure, Martin, additional, Metzger, Jean-Marc, additional, Pichon, Jean-Marc, additional, Ribeiro, Mickaël, additional, Rocco, Manon, additional, Tulet, Pierre, additional, Vella, Anthony, additional, Leriche, Maud, additional, and Deguillaume, Laurent, additional

Published
2022
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23. Cézeaux-Aulnat-Opme-Puy De Dôme: a multi-site for the long-term survey of the tropospheric composition and climate change

Author

Baray, Jean-Luc, primary, Deguillaume, Laurent, additional, Colomb, Aurélie, additional, Sellegri, Karine, additional, Freney, Evelyn, additional, Rose, Clémence, additional, Van Baelen, Joël, additional, Pichon, Jean-Marc, additional, Picard, David, additional, Fréville, Patrick, additional, Bouvier, Laëtitia, additional, Ribeiro, Mickaël, additional, Amato, Pierre, additional, Banson, Sandra, additional, Bianco, Angelica, additional, Borbon, Agnès, additional, Bourcier, Lauréline, additional, Bras, Yannick, additional, Brigante, Marcello, additional, Cacault, Philippe, additional, Chauvigné, Aurélien, additional, Charbouillot, Tiffany, additional, Chaumerliac, Nadine, additional, Delort, Anne-Marie, additional, Delmotte, Marc, additional, Dupuy, Régis, additional, Farah, Antoine, additional, Febvre, Guy, additional, Flossmann, Andrea, additional, Gourbeyre, Christophe, additional, Hervier, Claude, additional, Hervo, Maxime, additional, Huret, Nathalie, additional, Joly, Muriel, additional, Kazan, Victor, additional, Lopez, Morgan, additional, Mailhot, Gilles, additional, Marinoni, Angela, additional, Masson, Olivier, additional, Montoux, Nadège, additional, Parazols, Marius, additional, Peyrin, Frédéric, additional, Pointin, Yves, additional, Ramonet, Michel, additional, Rocco, Manon, additional, Sancelme, Martine, additional, Sauvage, Stéphane, additional, Schmidt, Martina, additional, Tison, Emmanuel, additional, Vaïtilingom, Mickaël, additional, Villani, Paolo, additional, Wang, Miao, additional, Yver-Kwok, Camille, additional, and Laj, Paolo, additional

Published
2020
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25. Cloud Occurrence Frequency at Puy de Dôme (France) Deduced from an Automatic Camera Image Analysis: Method, Validation, and Comparisons with Larger Scale Parameters

Author

Baray, Jean-Luc, primary, Bah, Asmaou, additional, Cacault, Philippe, additional, Sellegri, Karine, additional, Pichon, Jean-Marc, additional, Deguillaume, Laurent, additional, Montoux, Nadège, additional, Noel, Vincent, additional, Seze, Geneviève, additional, Gabarrot, Franck, additional, Payen, Guillaume, additional, and Duflot, Valentin, additional

Published
2019
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26. Preliminary results from the FARCE 2015 campaign: multidisciplinary study of the forest–gas–aerosol–cloud system on the tropical island of La Réunion

Author

Duflot, Valentin, Tulet, Pierre, Flores, Olivier, Barthe, Christelle, Colomb, Aurélie, Deguillaume, Laurent, Vaitilingom, Mickaël, Perring, Anne, Huffman, Alex, Hernandez, Mark, Sellegri, Karine, Robinson, Ellis, O'Connor, David, Gomez, Odessa, Burnet, Frédéric, Bourrianne, Thierry, Strasberg, Dominique, Rocco, Manon, Bertram, Allan, Chazette, Patrick, Totems, Julien, Fournel, Jacques, Stamenoff, Pierre, Metzger, Jean-Marc, Chabasset, Mathilde, Rousseau, Clothilde, Bourrianne, Eric, Sancelme, Martine, Delort, Anne-Marie, Wegener, Rachel, Chou, Cedric, Elizondo, Pablo, Laboratoire de l'Atmosphère et des Cyclones (LACy), Météo France-Université de La Réunion (UR)-Centre National de la Recherche Scientifique (CNRS), Peuplements végétaux et bioagresseurs en milieu tropical (UMR PVBMT), Institut de Recherche pour le Développement (IRD)-Centre de Coopération Internationale en Recherche Agronomique pour le Développement (Cirad)-Université de La Réunion (UR)-Institut National de la Recherche Agronomique (INRA), 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), Synthèse et étude de systèmes à intêret biologique (SEESIB), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-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), University of Wisconsin-Madison, Centre national de recherches météorologiques (CNRM), Météo France-Centre National de la Recherche Scientifique (CNRS), Department of Chemistry [Vancouver], University of British Columbia (UBC), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), 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), Sigma CLERMONT (Sigma CLERMONT), Institut national des sciences de l'Univers (INSU - CNRS)-Université de La Réunion (UR)-Centre National de la Recherche Scientifique (CNRS)-Météo-France, Centre de Coopération Internationale en Recherche Agronomique pour le Développement (Cirad)-Institut de Recherche pour le Développement (IRD)-Institut National de la Recherche Agronomique (INRA)-Université de La Réunion (UR), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 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)-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), Department of Chemistry [Vancouver] (UBC Chemistry), 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), SIGMA Clermont (SIGMA Clermont), Centre National de la Recherche Scientifique (CNRS)-Université de La Réunion (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Météo France, Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), 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 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.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, [SDE.BE]Environmental Sciences/Biodiversity and Ecology
Abstract

International audience; The Forests gAses aeRosols Clouds Exploratory (FARCE) campaign was conducted in March-April 2015 on the tropical island of La Réunion. For the first time, several scientific teams from different disciplines collaborated to provide reference measurements and characterization of La Réunion vegetation, volatile organic compounds (VOCs), biogenic VOCs (BVOCs), (bio)aerosols and composition of clouds, with a strong focus on the Maïdo mountain slope area. The main observations obtained during this 2-month intensive field campaign are summarized. They include characterizations of forest structure, concentrations of VOCs and precursors emitted by forests, aerosol loading and optical properties in the planetary boundary layer (PBL), formation of new particles by nucleation of gas-phase precursors, ice-nucleating particles concentrations, and biological loading in both cloud-free and cloudy conditions. Simulations and measurements confirm that the Maïdo Observatory lies within the PBL from late morning to late evening and that, when in the PBL, the main primary sources impacting the Maïdo Observatory are of marine origin via the Indian Ocean and of bio-genic origin through the dense forest cover. They also show that (i) the marine source prevails less and less while reaching the observatory; (ii) when in the PBL, depending on the lo-calization of a horizontal wind shear, the Maïdo Observatory can be affected by air masses coming directly from the ocean and passing over the Maïdo mountain slope, or coming from inland; (iii) bio-aerosols can be observed in both cloud-free and cloudy conditions at the Maïdo Observatory; (iv) BVOC emissions by the forest covering the Maïdo mountain slope can be transported upslope within clouds and are a potential cause of secondary organic aerosol formation in the aqueous phase at the Maïdo Observatory; and (v) the simulation of dynamics parameters, emitted BVOCs and cloud life cycle in the Meso-NH model are realistic, and more advanced Meso-NH simulations should use an increased horizontal resolution (100 m) to better take into account the orography and improve the simulation of the wind shear front zone within which lies the Maïdo Observatory. Using various observations and simulations, this work draws up an inventory of the in situ studies that could be performed in La Réunion and at the Maïdo Observatory. It also aims to develop scientific collaborations and to support future scientific projects in order to better understand the forest-gas-aerosol-cloud system in an insular tropical environment.

Published
2019

28. Preliminary Results from the FARCE 2015 Campaign: Multidisciplinary Study of the Forest–Gas–Aerosol–Cloud System on the Tropical Island of LaRéunion

Author

Duflot, Valentin, Tulet, Pierre, Flores, Olivier, Barthe, Christelle, Colomb, Aurélie, Deguillaume, Laurent, Vaïtilingom, Mickael, Perring, Anne, Huffman, Alex, Hernandez, MarkT., Sellegri, Karine, Robinson, Ellis, O'Connor, David J., Gomez, Odessa M, Burnet, Frédéric, Bourrianne, Thierry, Strasberg, Dominique, Rocco, Manon, Bertram, Allan K, Chazette, Patrick, Totems, Julien, Stamenoff, Pierre, Metzger, Jean-Marc, Chabasset, Mathilde, Rousseau, Clothilde, Bourrianne, Eric, Sancelme, Martine, Delort, Anne-Marie, Wegener, Rachel E., Chou, Cedric, and Elizondo, Pablo

Subjects
Chemistry, FARCE campaign
Abstract

The Forests gAses aeRosols Clouds Exploratory (FARCE) campaign was conducted in March–April 2015 on the tropical island of La Réunion. For the first time, several scientific teams from different disciplines collaborated to provide reference measurements and characterization of LaRéunionvegetation,volatileorganiccompounds(VOCs), biogenic VOCs (BVOCs), (bio)aerosols and composition of clouds, with a strong focus on the Maïdo mountain slope area. The main observations obtained during this 2-month intensivefieldcampaignaresummarized.Theyincludecharacterizations of forest structure, concentrations of VOCs and precursors emitted by forests, aerosol loading and optical properties in the planetary boundary layer (PBL), formation of new particles by nucleation of gas-phase precursors, icenucleatingparticlesconcentrations,andbiologicalloadingin bothcloud-freeandcloudyconditions.SimulationsandmeasurementsconfirmthattheMaïdoObservatorylieswithinthe PBL from late morning to late evening and that, when in the PBL, the main primary sources impacting the Maïdo Observatory are of marine origin via the Indian Ocean and of biogenic origin through the dense forest cover. They also show that(i)themarinesourceprevailslessandlesswhilereaching the observatory; (ii) when in the PBL, depending on the localizationofahorizontalwindshear,theMaïdoObservatory canbeaffectedbyairmassescomingdirectlyfromtheocean and passing over the Maïdo mountain slope, or coming from inland; (iii) bio-aerosols can be observed in both cloud-free and cloudy conditions at the Maïdo Observatory; (iv) BVOC emissions by the forest covering the Maïdo mountain slope can be transported upslope within clouds and are a potential cause of secondary organic aerosol formation in the aqueous phase at the Maïdo Observatory; and (v) the simulation of dynamicsparameters,emittedBVOCsandcloudlifecyclein the Meso-NH model are realistic, and more advanced MesoNH simulations should use an increased horizontal resolution (100m) to better take into account the orography and improve the simulation of the wind shear front zone within which lies the Maïdo

Published
2019

29. Free amino acids quantification in cloud water at the puy de Dôme station (France).

Author

Renard, Pascal, Brissy, Maxence, Rossi, Florent, Leremboure, Martin, Jaber, Saly, Baray, Jean-Luc, Bianco, Angelica, Delort, Anne-Marie, and Deguillaume, Laurent

Abstract

Eighteen free amino acids (FAAs) were quantified in cloud water sampled at the puy de Dome station (PUY - France) during 13 cloud events. This quantification has been performed without concentration neither derivatization, using LC-MS and the standard addition method to avoid matrix effects. Total concentrations of FAAs (TCAAs) vary from 1.2 µM to 7.7 µM, Ser (Serine) being the most abundant AA (23.7 % in average) but with elevated standard deviation, followed by Glycine (Gly) (20.5 %), Alanine (Ala) (11.9 %), Asparagine (Asn) (8.7 %), and Leucine/Isoleucine (Leu/I) (6.4 %). The distribution of AAs among the cloud events reveals high variability. TCAA constitutes between 0.5 and 4.4 % of the dissolved organic carbon measured in the cloud samples. AAs quantification in cloud water is scarce but the results agree with the few studies that investigated AAs in this aqueous medium. The environmental variability is assessed through a statistical analysis. This work shows that AAs are correlated with the time spent by the air masses in the boundary layer, especially over the sea surface before reaching the PUY. The cloud microphysical properties fluctuation does not explain the AAs variability in our samples confirming previous studies at PUY. We finally assessed the sources and the atmospheric processes that potentially explain the prevailing presence of certain AAs in the cloud samples. The initial relative distribution of AAs in biological matrices (proteins extracted from bacterial cells or mammalian cells, for example) could explain the dominance of Ala, Gly and Leu/I. AA composition of aquatic organisms (i.e., diatoms species) could also explain the high concentrations of Ser in our samples. The analysis of the AAs hydropathy also indicates a higher contribution of AAs (80 % in average) that are hydrophilic or neutral revealing the fact that other AAs (hydrophobic) are less favorably incorporated into cloud droplets. Finally, the atmospheric aging of AAs has been evaluated by calculating atmospheric lifetimes considering their potential transformation in the cloud medium by biotic or abiotic (mainly oxidation) processes. The most concentrated AAs encountered in our samples present the longest atmospheric lifetimes and the less dominant are clearly efficiently transformed in the atmosphere, potentially explaining their low concentrations. However, this cannot fully explain the relative contribution of several AAs in the cloud samples. This reveals the high complexity of the bio-physico-chemical processes occurring in the multiphasic atmospheric environment. [ABSTRACT FROM AUTHOR]

Published
2021
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30. Trace Metals in Cloud Water Sampled at the Puy De Dôme Station

Author

Bianco, Angelica, Vaïtilingom, Mickaël, Bridoux, Maxime, Chaumerliac, Nadine, Pichon, Jean-Marc, Piro, Jean-Luc, Deguillaume, Laurent, 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), 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), Laboratoire de Recherche en Géosciences et Energies (LARGE), Université des Antilles (UA), 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), 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), ANR-13-BS06-0004,BIOCAP,Impacts BIOlogiques et photochimiques sur la CAPacité oxydante du nuage(2013), 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 Recherche en Géosciences et Energies [UR2_1] (LARGE), 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), 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)-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, puy de Dôme, principal component analysis, trace metals, cloud, lcsh:Meteorology. Climatology, air mass origin, lcsh:QC851-999
Abstract

International audience; Concentrations of 33 metal elements were determined by ICP-MS (Inductively Coupled Plasma Mass Spectrometry) analysis for 24 cloud water samples (corresponding to 10 cloud events) collected at the puy de Dôme station. Clouds present contrasted chemical composition with mainly marine and continental characteristics; for some cloud events, a further anthropogenic source can be superimposed on the background level. In this context, measurements of trace metals may help to evaluate the impact of anthropogenic and natural sources on the cloud and to better discriminate the origin of the air masses. The metal concentrations in the samples are low (between 16.4 µg L$^{−1}$ and 1.46 mg L$^{−1}$). This could be explained by the remoteness of the puy de Dôme site from local sources. Trace metals are then used to confirm and refine a previous sample classification. A principal component analysis (PCA) using the pH value and the concentrations of Cl$^−$, NO${_3}^−$, SO${_4}^{2−}$, Na$^+$ and NH${_4}^+$ is performed considering 24 cloud samples. This first analysis shows that 18 samples are of marine origin and 6 samples are classified as continental. The same statistical approach is used adding trace metal concentration. Zn and Mg elements are the most abundant trace metals for all clouds. A higher concentration of Cd is mainly associated to clouds from marine origins. Cu, As, Tl and Sb elements are rather found in the continental samples than in the marine ones. Mg, V, Mn and Rb elements mainly found in soil particles are also more concentrated in the samples from continental air mass. This new PCA including trace metal confirms the classification between marine and continental air masses but also indicates that one sample presenting low pH and high concentrations of SO${_4}^{2−}$, Fe, Pb and Cu could be rather attributed to a polluted event.

Published
2017

31. Active microorganisms thrive among extremely diverse communities in cloud water

Author

Amato, Pierre, Joly, Muriel, Besaury, Ludovic, Oudart, Anne, Taib, Najwa, Moné, Anne I., Deguillaume, Laurent, Delort, Anne-Marie, Debroas, Didier, Synthèse et étude de systèmes à intêret biologique (SEESIB), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Clermont-Ferrand (ICCF), SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Microorganismes : Génome et Environnement (LMGE), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Université d'Auvergne - Clermont-Ferrand I (UdA)-Centre National de la Recherche Scientifique (CNRS), 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), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), and Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Centre National de la Recherche Scientifique (CNRS)-Université d'Auvergne - Clermont-Ferrand I (UdA)

Subjects
Atmospheric Science, Molecular biology, Atmospheric clouds, [SDV]Life Sciences [q-bio], lcsh:Medicine, Microbiology, Polymerase Chain Reaction, Meteorology, Extraction techniques, Sequencing techniques, Prokaryotic cells, Clouds, [CHIM]Chemical Sciences, Atmospheric Dynamics, Archaean Biology, lcsh:Science, Principal Component Analysis, Bacteria, Atmosphere, Physics, Altitude, lcsh:R, Organisms, Fungi, Biology and Life Sciences, High-Throughput Nucleotide Sequencing, Eukaryota, RNA sequencing, Cell Biology, Atmospheric Physics, RNA extraction, Community structure, Research and analysis methods, Geophysics, Molecular biology techniques, Physical Sciences, [SDE]Environmental Sciences, Earth Sciences, lcsh:Q, France, Cellular Types, Water Microbiology, Research Article
Abstract

International audience; Clouds are key components in Earth’s functioning. In addition of acting as obstacles to light radiations and chemical reactors, they are possible atmospheric oases for airborne microorganisms, providing water, nutrients and paths to the ground. Microbial activity was previously detected in clouds, but the microbial community that is active in situ remains unknown. Here, microbial communities in cloud water collected at puy de Dôme Mountain’s meteorological station (1465 m altitude, France) were fixed upon sampling and examined by high-throughput sequencing from DNA and RNA extracts, so as to identify active species among community members. Communities consisted of ~103−104 bacteria and archaea mL-1 and ~102−103 eukaryote cells mL-1. They appeared extremely rich, with more than 28 000 distinct species detected in bacteria and 2 600 in eukaryotes. Proteobacteria and Bacteroidetes largely dominated in bacteria, while eukaryotes were essentially distributed among Fungi, Stramenopiles and Alveolata. Within these complex communities, the active members of cloud microbiota were identified as Alpha- (Sphingomonadales, Rhodospirillales and Rhizobiales), Beta- (Burkholderiales) and Gamma-Proteobacteria (Pseudomonadales). These groups of bacteria usually classified as epiphytic are probably the best candidates for interfering with abiotic chemical processes in clouds, and the most prone to successful aerial dispersion.

Published
2017

32. CLEPS 1.0: A new protocol for cloud aqueous phase oxidation of VOC mechanisms

Author

Mouchel-Vallon, Camille, Deguillaume, Laurent, Monod, Anne, Perroux, Hélène, Rose, Clémence, Ghigo, Giovanni, Long, Yoann, Leriche, Maud, Aumont, Bernard, Patryl, Luc, Armand, Patrick, Chaumerliac, Nadine, 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 Chimie de l'environnement (LCE), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU), Dipartimento di Chimica (Dipartimento di Chimica - Università di Torino), Università degli studi di Torino (UNITO), 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 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), 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), ANR-10-BLAN-0617,CUMULUS,Chimie organiqUe MULtiphasique des nUages troposphériqueS(2010), ANR-13-BS06-0004,BIOCAP,Impacts BIOlogiques et photochimiques sur la CAPacité oxydante du nuage(2013), 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), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Dipartimento di Chimica [Torino], Università degli studi di Torino = University of Turin (UNITO), Laboratoire d'aérologie (LAERO), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), 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 -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 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), 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), 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), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), and 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)

Subjects
lcsh:Geology, Modeling and Simulation, Earth and Planetary Sciences (all), Isoprene oxidation, Cloud Explicit Physico-chemical Scheme (CLEPS 1.0), Monoacids, lcsh:QE1-996.5, Oxidation, [SDE]Environmental Sciences, GROMHE SAR, Water, [CHIM]Chemical Sciences
Abstract

A new detailed aqueous phase mechanism named the Cloud Explicit Physico-chemical Scheme (CLEPS 1.0) is proposed to describe the oxidation of water soluble organic compounds resulting from isoprene oxidation. It is based on structure activity relationships (SARs) which provide global rate constants together with branching ratios for HO⋅ abstraction and addition on atmospheric organic compounds. The GROMHE SAR allows the evaluation of Henry's law constants for undocumented organic compounds. This new aqueous phase mechanism is coupled with the MCM v3.3.1 gas phase mechanism through a mass transfer scheme between gas phase and aqueous phase. The resulting multiphase mechanism has then been implemented in a model based on the Dynamically Simple Model for Atmospheric Chemical Complexity (DSMACC) using the Kinetic PreProcessor (KPP) that can serve to analyze data from cloud chamber experiments and field campaigns. The simulation of permanent cloud under low-NOx conditions describes the formation of oxidized monoacids and diacids in the aqueous phase as well as a significant influence on the gas phase chemistry and composition and shows that the aqueous phase reactivity leads to an efficient fragmentation and functionalization of organic compounds.

Published
2017

33. H2O2 modulates the energetic metabolism of the cloud microbiome

Author

Wirgot, Nolwenn, Vinatier, Virginie, Deguillaume, Laurent, Sancelme, Martine, Delort, Anne-Marie, Institut de Chimie de Clermont-Ferrand (ICCF), SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-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), 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
lcsh:Chemistry, inorganic chemicals, lcsh:QD1-999, [CHIM]Chemical Sciences, sense organs, complex mixtures, lcsh:Physics, lcsh:QC1-999
Abstract

Chemical reactions in clouds lead to oxidation processes driven by radicals (mainly HO⚫, NO3⚫, or HO2⚫) or strong oxidants such as H2O2, O3, nitrate, and nitrite. Among those species, hydrogen peroxide plays a central role in the cloud chemistry by driving its oxidant capacity. In cloud droplets, H2O2 is transformed by microorganisms which are metabolically active. Biological activity can therefore impact the cloud oxidant capacity. The present article aims at highlighting the interactions between H2O2 and microorganisms within the cloud system. First, experiments were performed with selected strains studied as a reference isolated from clouds in microcosms designed to mimic the cloud chemical composition, including the presence of light and iron. Biotic and abiotic degradation rates of H2O2 were measured and results showed that biodegradation was the most efficient process together with the photo-Fenton process. H2O2 strongly impacted the microbial energetic state as shown by adenosine triphosphate (ATP) measurements in the presence and absence of H2O2. This ATP depletion was not due to the loss of cell viability. Secondly, correlation studies were performed based on real cloud measurements from 37 cloud samples collected at the PUY station (1465 m a.s.l., France). The results support a strong correlation between ATP and H2O2 concentrations and confirm that H2O2 modulates the energetic metabolism of the cloud microbiome. The modulation of microbial metabolism by H2O2 concentration could thus impact cloud chemistry, in particular the biotransformation rates of carbon compounds, and consequently can perturb the way the cloud system is modifying the global atmospheric chemistry.

Published
2017

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

Author

Baray, Jean-Luc, Deguillaume, Laurent, Colomb, Aurélie, Sellegri, Karine, Freney, Evelyn, Rose, Clémence, Van Baelen, Joël, Pichon, Jean-Marc, Picard, David, Fréville, Patrick, Bouvier, Laetitia, Ribeiro, Mickaël, Amato, Pierre, Banson, Sandra, Bianco, Angelica, Borbon, Agnès, Bourcier, Laureline, Bras, Yannick, Brigante, Marcello, and Cacault, Philippe

Subjects
*ATMOSPHERIC sciences, *CLIMATE change, *WIND tunnel testing, *CLIMATOLOGY, *TRACE gases, *AIR masses
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. [ABSTRACT FROM AUTHOR]

Published
2019
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35. Potential for phenol biodegradation in cloud waters

Author

Lallement, Audrey, primary, Besaury, Ludovic, additional, Tixier, Elise, additional, Sancelme, Martine, additional, Amato, Pierre, additional, Vinatier, Virginie, additional, Canet, Isabelle, additional, Polyakova, Olga V., additional, Artaev, Viatcheslay B., additional, Lebedev, Albert T., additional, Deguillaume, Laurent, additional, Mailhot, Gilles, additional, and Delort, Anne-Marie, additional

Published
2018
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38. Classification of clouds sampled at the puy de Dôme (France) from 10-year monitoring: Mean features of their physico-chemical properties

Author

Deguillaume, Laurent, Charbouillot, T., Joly, M., Vaïtilingom, M., Parazols, M., Marinoni, A., Amato, Pierre, Delort, A.M., Vinatier, V., Flossmann, Andrea, Chaumerliac, N., Pichon, J. M., Houdier, S., Laj, Paolo, Sellegri, K., Colomb, Aurélie, Brigante, M., Mailhot, Gilles, 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), Institut de Chimie de Clermont-Ferrand (ICCF), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Sigma CLERMONT (Sigma CLERMONT), CNR Institute of Atmospheric Sciences and Climate (ISAC), Consiglio Nazionale delle Ricerche (CNR), SEESIB, Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Sigma CLERMONT (Sigma CLERMONT)-Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Sigma CLERMONT (Sigma CLERMONT), 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), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-SIGMA Clermont (SIGMA Clermont)-Institut de Chimie du CNRS (INC)-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), 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), The publication of this article isfinanced by CNRS-INSU, Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), 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 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)

Subjects
[CHIM]Chemical Sciences
Abstract

International audience; Long-term monitoring of the chemical composition of clouds (73 cloud events representing 199 individual samples) sampled at the puy de Dôme (pdD) station (France) was performed between 2001 and 2011. Physicochemical parameters, as well as the concentrations of the major organic and inorganic constituents, were measured and analyzed by multicomponent statistical analysis. Along with the corresponding back-trajectory plots, this allowed for distinguishing four different categories of air masses reaching the summit of the pdD: polluted, continental, marine and highly marine. The statistical analysis led to the determination of criteria (concentrations of inorganic compounds, pH) that differentiate each category of air masses. Highly marine clouds exhibited high concentrations of Na+ and Cl−; the marine category presented lower concentration of ions but more elevated pH. Finally, the two remaining clusters were classified as "continental" and "polluted"; these clusters had the second-highest and highest levels of NH4+, NO3−, and SO24−, respectively. This unique data set of cloud chemical composition is then discussed as a function of this classification. Total organic carbon (TOC) is significantly higher in polluted air masses than in the other categories, which suggests additional anthropogenic sources. Concentrations of carboxylic acids and carbonyls represent around 10% of the organic matter in all categories of air masses and are studied for their relative importance. Iron concentrations are significantly higher for polluted air masses and iron is mainly present in its oxidation state (+II) in all categories of air masses. Finally, H2O2 concentrations are much more varied in marine and highly marine clouds than in polluted clouds, which are characterized by the lowest average concentration of H2O2. This data set provides concentration ranges of main inorganic and organic compounds for modeling purposes on multiphase cloud chemistry.

Published
2014

41. H2O2 modulates the energetic metabolism of the cloud microbiome.

Author

Wirgot, Nolwenn, Vinatier, Virginie, Deguillaume, Laurent, Sancelme, Martine, and Delort, Anne-Marie

Subjects
RADICALS (Chemistry), CLOUDS & the environment, CLOUD dynamics, OXIDATION, HYDROGEN peroxide
Abstract

Chemical reactions in clouds lead to oxidation processes driven by radicals (mainly HO•, NO3•, or HO2•) or strong oxidants such as H2O2, O3, nitrate, and nitrite. Among those species, hydrogen peroxide plays a central role in the cloud chemistry by driving its oxidant capacity. In cloud droplets, H2O2 is transformed by microorganisms which are metabolically active. Biological activity can therefore impact the cloud oxidant capacity. The present article aims at highlighting the interactions between H2O2 and microorganisms within the cloud system. First, experiments were performed with selected strains studied as a reference isolated from clouds in microcosms designed to mimic the cloud chemical composition, including the presence of light and iron. Biotic and abiotic degradation rates of H2O2 were measured and results showed that biodegradation was the most efficient process together with the photo-Fenton process. H2O2 strongly impacted the microbial energetic state as shown by adenosine triphosphate (ATP) measurements in the presence and absence of H2O2. This ATP depletion was not due to the loss of cell viability. Secondly, correlation studies were performed based on real cloud measurements from 37 cloud samples collected at the PUY station (1465 ma.s.l., France). The results support a strong correlation between ATP and H2O2 concentrations and confirm that H2O2 modulates the energetic metabolism of the cloud microbiome. The modulation of microbial metabolism by H2O2 concentration could thus impact cloud chemistry, in particular the biotransformation rates of carbon compounds, and consequently can perturb the way the cloud system is modifying the global atmospheric chemistry. [ABSTRACT FROM AUTHOR]

Published
2017
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42. Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1).

Author

Rose, Clémence, Chaumerliac, Nadine, Deguillaume, Laurent, Perroux, Hélène, Mouchel-Vallon, Camille, Leriche, Maud, Patryl, Luc, and Armand, Patrick

Abstract

The new detailed aqueous phase mechanism Cloud Explicit Physico-chemical Scheme (CLEPS 1.0), which describes the oxidation of isoprene-derived water-soluble organic compounds, is coupled with a warm microphysical module simulating the activation of aerosol particles into cloud droplets. CLEPS 1.0 was then extended to CLEPS 1.1 to include the chemistry of the newly added di-carboxylic acids dissolved from the particulate phase. The resulting coupled model allows for predicting the aqueous phase concentrations of chemical compounds originating from particle dissolution, mass transfer from the gas phase and in-cloud aqueous chemical reactivity. The aim of the present study was more particularly to investigate the effect of particle dissolution on cloud chemistry. Several simulations were performed to assess the influence of various parameters on model predictions and to interpret long-term measurements conducted at the top of the puy de Dôme (PUY, France) in marine air masses. Specific attention was paid to carboxylic acids, whose predicted concentrations are on average in the lower range of the observations, with the exception of formic acid, which is rather overestimated in the model. The different sensitivity runs highlight the fact that formic and acetic acids mainly originate from the gas phase and have highly variable aqueous-phase reactivity depending on the cloud acidity, whereas C3-C4 carboxylic acids mainly originate from the particulate phase and are supersaturated in the cloud. [ABSTRACT FROM AUTHOR]

Published
2017
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45. CLEPS: A new protocol for cloud aqueous phase oxidation of VOC mechanisms.

Author

Mouchel-Vallon, Camille, Deguillaume, Laurent, Monod, Anne, Perroux, Hélène, Rose, Clémence, Ghigo, Giovanni, Yoann Long, Leriche, Maud, Aumont, Bernard, Patryl, Luc, Armand, Patrick, and Chaumerliac, Nadine

Subjects
*OXIDATION of volatile organic compounds, *TROPOSPHERE, *AIR quality, *GAS phase reactions, *STRUCTURE-activity relationships, *CLOUDS
Abstract

Organic compounds of both anthropogenic and natural origin are ubiquitous in the multiphasic atmospheric medium. Their transformation in the atmosphere affects air quality and the global climate. Modelling provides a useful tool to investigate the chemistry of organic compounds in the tropospheric multiphase system. While several comprehensive explicit mechanisms exist in the gas phase, explicit mechanisms are much more limited in the aqueous phase. Recently, new empirical methods have been developed to estimate HO• reaction rates in the aqueous phase: structure-activity relationships (SARs) provide global rate constants and branching ratios for HO• abstraction from and addition to atmospheric organic compounds. Based on these SARs, a new detailed aqueous-phase mechanism, named the cloud explicit physico-chemical scheme (CLEPS), to describe the oxidation of hydrosoluble organic compounds resulting from isoprene oxidation is proposed. In this paper, a protocol based on reviewed experimental data and evaluated prediction methods is described in detail. The current version of the mechanism includes approximately 850 aqueous reactions and 465 equilibria. Inorganic reactivity is described for 67 chemical species (e.g., transition metal ions, HxOy, sulphur species, nitrogen species, and chlorine). For organic compounds, 87 chemical species are considered in the mechanism, corresponding to 657 chemical forms that are individually followed (e.g., hydrated forms, anionic forms). This new aqueous-phase mechanism is coupled with the detailed gas phase mechanism MCM v3.3.1 through mass transfer parameterization for the exchange between the gas phase and aqueous phase. The GROMHE SAR enables the evaluation of the Henry's law constants for undocumented organic compounds. The resulting multiphase mechanism is implemented in a model based on the Dynamically Simple Model for Atmospheric Chemical Complexity (DSMACC) using the Kinetic PreProcessor (KPP). This model allows simulation of the time evolution of the concentrations of each individual chemical species in addition to detailed time-resolved flux analyses. The variable photolysis in both phases is calculated using the TUV 4.5 radiative transfer model. To evaluate our chemical mechanism, an idealized cloud event with fixed microphysical cloud parameters is simulated. The simulation is performed for a low-NOx situation. The results indicate the formation of oxidized mono- and diacids in the aqueous phase, as well as a significant influence on the gas phase chemistry and composition. For this particular simulation, the aqueous phase mechanism is responsible for the efficient fragmentation and functionalization of organic compounds. This new cloud chemistry model allows for the analysis of individual aqueous sub systems and can be used to analyze the results from cloud chamber experiments and field campaigns. [ABSTRACT FROM AUTHOR]

Published
2016
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