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1. A new optical-based technique for real-time measurements of mineral dust concentration in PM10 using a virtual impactor

Author: Jean Sciare, Spiros Bezantakos, Griša Močnik, Luka Drinovec, Chrysanthos Savvides, Maja Remškar, Bojana Višić, Michael Pikridas, Iasonas Stavroulas, and Florin Unga
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Photometer, 010501 environmental sciences, Mineral dust, Aethalometer, Atmospheric sciences, 01 natural sciences, Aerosol, law.invention, Atmosphere, 13. Climate action, law, Radiative transfer, Environmental science, Absorption (electromagnetic radiation), Air quality index, 0105 earth and related environmental sciences
Abstract: Atmospheric mineral dust influences Earth's radiative budget, cloud formation, and lifetime; has adverse health effects; and affects air quality through the increase of regulatory PM10 concentrations, making its real-time quantification in the atmosphere of strategic importance. Only few near-real-time techniques can discriminate dust aerosol in PM10 samples and they are based on the dust chemical composition. The online determination of mineral dust using aerosol absorption photometers offers an interesting and competitive alternative but remains a difficult task to achieve. This is particularly challenging when dust is mixed with black carbon, which features a much higher mass absorption cross section. We build on previous work using filter photometers and present here for the first time a highly time-resolved online technique for quantification of mineral dust concentration by coupling a high-flow virtual impactor (VI) sampler that concentrates coarse particles with an aerosol absorption photometer (Aethalometer, model AE33). The absorption of concentrated dust particles is obtained by subtracting the absorption of the submicron (PM1) aerosol fraction from the absorption of the virtual impactor sample (VI-PM1 method). This real-time method for detecting desert dust was tested in the field for a period of 2 months (April and May 2016) at a regional background site of Cyprus, in the Eastern Mediterranean. Several intense desert mineral dust events were observed during the field campaign with dust concentration in PM10 up to 45 µg m−3. Mineral dust was present most of the time during the campaign with an average PM10 of about 8 µg m−3. Mineral dust absorption was most prominent at short wavelengths, yielding an average mass absorption cross section (MAC) of 0.24±0.01 m2 g−1 at 370 nm and an absorption Ångström exponent of 1.41±0.29. This MAC value can be used as a site-specific parameter for online determination of mineral dust concentration. The uncertainty of the proposed method is discussed by comparing and validating it with different methods.
Published: 2020

2. Shipborne measurements of ClNO2 in the Mediterranean Sea and around the Arabian Peninsula during summer

Author: John Crowley, Roland Rohloff, Monica Martinez, Justin Shenolikar, Sebastian Tauer, Frank Drewnick, Horst Fischer, Friederike Fachinger, Nils Friedrich, Michael Pikridas, Philipp Eger, James Brooks, Jan Schuladen, Ivan Tadic, Jos Lelieveld, Jean Sciare, Eoghan Darbyshire, and Hartwig Harder
Subjects: Atmospheric Science, geography, Dinitrogen pentoxide, geography.geographical_feature_category, 010504 meteorology & atmospheric sciences, Climate change, 010501 environmental sciences, 01 natural sciences, Aerosol, chemistry.chemical_compound, Oceanography, Mediterranean sea, chemistry, Peninsula, Environmental science, Diel vertical migration, Air quality index, Sulfur dioxide, 0105 earth and related environmental sciences
Abstract: Shipborne measurements of nitryl chloride (ClNO2), hydrogen chloride (HCl) and sulphur dioxide (SO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea, the Suez Canal, the Red Sea, the Gulf of Aden, the Arabian Sea, the Gulf of Oman and the Arabian Gulf (also known as Persian Gulf) with observed ClNO2 mixing ratios ranging from the limit of detection to ≈ 600 pptv. We examined the regional variability in the generation of ClNO2 via the uptake of dinitrogen pentoxide (N2O5) to Cl-containing aerosol and its importance for Cl-atom generation in a marine boundary layer under the (variable) influence of emissions from shipping and oil industry. The yield of ClNO2 formation per NO3 radical generated was generally low (median of ≈ 1–5 % depending on the region), mainly as a result of gas-phase loss of NO3 dominating over heterogeneous loss of N2O5, the latter being disfavoured by the high temperatures found throughout the campaign. The contributions of ClNO2 photolysis and OH-induced HCl oxidation to Cl-radical formation were derived and their relative contributions over the diel cycle compared. The results indicate that over the northern Red Sea, the Gulf of Suez and the Gulf of Oman the formation of Cl-atoms will enhance the oxidation rates of some VOCs, especially in the early morning.
Published: 2019

3. The monitoring nitrous oxide sources (MIN2OS) satellite project

Author: Joël Léonard, Jean-Luc Attié, Hélène Reynal, Christine Groot Zwaaftink, Naoko Saitoh, Laurent Berdeu, Rona Thompson, Jos Lelieveld, Elizabeth Pattey, Z. Zelinger, Audrey Fortems-Cheiney, Frédérick Pasternak, Isabelle Pison, Prabir K. Patra, Václav Nevrlý, Jan Suchánek, Olivier Saint-Pé, Rémi Chalinel, Juying Warner, Laure Brooker, Jean Sciare, Philippe Ricaud, Jérôme Vidot, Michal Dostál, 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), Laboratoire d'aérologie (LAERO), 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), Airbus Defence and Space [Les Mureaux], ASTRIUM, Agroressources et Impacts environnementaux (AgroImpact), Institut National de la Recherche Agronomique (INRA), 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), Institut Pierre-Simon-Laplace (IPSL (FR_636)), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-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)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), Agriculture and Agri-Food (AAFC), Norsk Institutt for Luftforskning (NILU), J. Heyrovský Institute of Physical Chemistry of the ASCR, Czech Academy of Sciences [Prague] (CAS), Max Planck Institute for Chemistry (MPIC), Max-Planck-Gesellschaft, Cyprus Institute (CyI), Chiba University, University of Maryland [Baltimore], Research Institute for Global Change (RIGC), Japan Agency for Marine-Earth Science and Technology (JAMSTEC), AGroécologie, Innovations, teRritoires (AGIR), Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE), The TN2OR project is funded by the Région Occitanie, the University of Toulouse, the Institut National des Sciences de l'Univers (INSU)/Centre National de la Recherche Scientifique (CNRS), Météo-France, the Centre National d'Etudes Spatiales (CNES), Airbus Defense and Space, and Sciences et technologies pour l'Aéronautique et l'Espace (STAE) foundation. RC's PhD has been funded by Région Occitanie and Airbus Defense and Space., Météo France-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), 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, Airbus Defence and Space, Airbus Group, 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), Agriculture and Agri-Food [Ottawa] (AAFC), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National de Recherche pour l’Agriculture, l’Alimentation et l’Environnement (INRAE)
Subjects: Daytime, N2O emissions, 010504 meteorology & atmospheric sciences, Equator, Soil Science, 7. Clean energy, 01 natural sciences, Modelling, Atmosphere, Mixing ratio, Computers in Earth Sciences, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, Remote sensing, Atmospheric sounding, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Nitrous oxide, [SDE.IE]Environmental Sciences/Environmental Engineering, Sources, Geology, 04 agricultural and veterinary sciences, Spectral bands, Atmosphere of Earth, 13. Climate action, 040103 agronomy & agriculture, 0401 agriculture, forestry, and fisheries, Environmental science, Satellite, Space-borne observations
Abstract: International audience; The Monitoring Nitrous Oxide Sources (MIN2OS) satellite project aims at monitoring global-scale nitrous oxide (N2O) sources by retrieving N2O surface fluxes from the inversion of space-borne N2O measurements that are sensitive to the lowermost atmospheric layers under favorable conditions. MIN2OS will provide emission estimates of N2O at a horizontal resolution of 1° × 1° on the global scale and 10 × 10 km2 on the regional scale on a weekly to monthly basis depending on the application (e.g., agriculture, national inventories, policy, scientific research). Our novel approach is based on the development of: 1) a space-borne instrument operating in the Thermal InfraRed domain providing, in clear sky conditions, N2O mixing ratio in the lowermost atmosphere (900 hPa) under favorable conditions (summer daytime) over land and under favorable and unfavorable (winter nighttime) conditions over the ocean and 2) an atmospheric inversion framework to estimate N2O surface fluxes from the atmospheric satellite observations. After studying three N2O spectral bands (B1 at 1240–1350 cm−1, B2 at 2150–2260 cm−1 and B3 at 2400–2600 cm−1), a new TIR instrument will be developed, centered at 1250–1330 cm−1, with a resolution of 0.125 cm−1, a Full Width at Half Maximum of 0.25 cm−1 and a swath of 300 km. To optimally constrain the retrieval of N2O vertical profiles, the instrument will be on-board a platform at ~830 km altitude in a sun-synchronous orbit crossing the Equator in descending node at 09:30 local time in synergy with two other platforms (Metop-SG and Sentinel-2 NG) expected to fly in 2031–32 aiming at detecting surface properties, agricultural information on the field scale and vertical profiles of atmospheric constituents and temperature. The lifetime of the MIN2OS project would be 4–5 years to study the interannual variability of N2O surface fluxes. The spectral noise can be decreased by at least a factor of 5 compared to the lowest noise accessible to date with the Infrared Atmospheric Sounding Interferometer-New Generation (IASI-NG) mission. The N2O total error is expected to be less than ~1% (~3 ppbv) along the vertical. The preliminary design of the MIN2OS project results in a small instrument (payload of 90 kg, volume of 1200 × 600 × 300 mm3) with, in addition to the spectrometer, a wide field and 1-km resolution imager for cloud detection. The instruments could be hosted on a small platform, the whole satellite being largely compatible with a dual launch on VEGA-C. The MIN2OS project has been submitted to the European Space Agency Earth Explorer 11 mission ideas.
Published: 2021

4. Optical, physical and chemical properties of aerosols transported to a coastal site in the Western Mediterranean: Focus on primary marine aerosols

Author: Marine Claeys, Greg Roberts, Marc Mallet, Jovanna Arndt, Karine Sellegri, Jean Sciare, John Wenger, Bastien Sauvage, Scripps Institution of Oceanography (SIO), University of California [San Diego] (UC San Diego), University of California-University of California, Centre national de recherches météorologiques (CNRM), and Météo France-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, 13. Climate action, [SDE]Environmental Sciences, 14. Life underwater, 01 natural sciences, 0105 earth and related environmental sciences
Abstract: As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based in-situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m asl) to characterize the physical, optical and chemical properties of aerosols. During the observation period, three different aerosol regimes have been identified, including a dust outbreak (Dust) originating from Algeria/Tunisia, a primary marine aerosols (PMA) event from both the Gulf of Lion and emissions near the sample site, and a pollution period from Eastern Europe, which includes anthropogenic and biomass burning sources (BBP). The chemical, physical and optical properties of the observed aerosols as well as their local shortwave (SW) direct radiative forcing (DRF) in clear-sky conditions are compared for these three periods in order to assess the direct radiative impact of PMA above the Western Mediterranean Basin. The PMA period is characterized by a mean sea salt mass concentration up to 6.5 μg m−3, representing 40 % of the total PM10 mass concentration, and a relatively low ratio of chloride to sodium (average of 0.57) indicating a generally "aged" sea salt aerosol at Ersa. In this work, an original dataset, obtained from on-line real-time instruments (ATOFMS, PILS-IC) have been used to characterize the ageing of PMA. The majority of PMA had surprisingly undergone chemical reactions and were mostly advected from long-range transport. During PMA period, the mixing between fresh and aged PMA originated from both local and regional (Gulf of Lion) emissions. The aerosol optical properties, obtained for the whole atmospheric column and at the surface, indicate a single scattering albedo (SSA) near unity (at 440 nm), indicating almost purely scattering particles, associated to a relatively low aerosol optical depth (AOD) close to 0.1 (at 500 nm), and an aerosol angstrom extinction exponent (AE) equal to 1.3 ± 0.4 (between 440 and 870 nm), suggesting a possible mixing of the PMA with fine particles (probably of continental origin). AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of −11 ± 4 W m−2 at the surface and −8 ± 3 W m−2 at the top of the atmosphere (TOA). In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3–0.4 at 440 nm and column-integrated SSA of 0.90–0.95), induced a local instantaneous SW DRF nearly three times the forcing calculated during the PMA period, with maximum values up to −40 W m−2 at the surface. On average, the SW DRF was about −21 ± 11 and −14 ± 6 W m−2, at the surface and at TOA, respectively, during this dust outbreak. Finally, the BBP period was characterized by a significant increase of the aerosol PM1 mass concentration (from 3.7 μg m−3 to 7.2 μg m−3) due to the influence of biomass-burning and anthropogenic aerosols transported from Eastern Europe. The influence of polluted/smoke particles led to a significant decrease in SSA (0.90 at 440 nm), showing the important absorbing characteristics of such particles. For this period, the SW DRF at the surface and TOA also exhibit higher mean values compared to the PMA period (with values of −23 ± 6 W m−2 and −15 ± 4 W m−2, respectively) and similar range of values as the Dust period.
Published: 2020

5. Towards understanding the mechanisms of new particle formation in the Eastern Mediterranean

Author: Aliki Christodoulou, Lubna Dada, Elie Bimenyimana, Juha Kangasluoma, Kimmo Neitola, Jean Sciare, Lauri Ahonen, Rima Baalbaki, Anne Maisser, Tuija Jokinen, Katrianne Lehtipalo, George Biskos, Florin Unga, Michael Pikridas, Markku Kulmala, S. Bezantakos, Veli-Matti Kerminen, Chrysanthos Savvides, Tiia Laurila, and Tuukka Petäjä
Subjects: 010504 meteorology & atmospheric sciences, Particle (ecology), Seasonality, Atmospheric sciences, medicine.disease, 01 natural sciences, Trace gas, Aerosol, Eastern mediterranean, 13. Climate action, Ultrafine particle, medicine, Environmental science, Desert dust, 0105 earth and related environmental sciences
Abstract: To quantify the contribution of new particle formation (NPF) to ultrafine particle number and CCN budgets, one has to understand the mechanisms that govern NPF in different environments and its temporal extent. Here, we study NPF in Cyprus, an Eastern Mediterranean country located at the crossroads of three continents. We performed one-year continuous measurements of aerosol particles down to ~ 1 nm in diameter, for the first time in the Eastern Mediterranean and Middle East (EMME) region. These measurements were complemented with trace gas data, meteorological variables and retroplume analysis. We show that NPF is a very frequent phenomenon at this site and has higher frequencies of occurrence during spring and autumn. NPF events were both of local and regional origin, and the local events occurred frequently during the month with the lowest NPF frequency. Some NPF events exhibited multiple onsets, while others exhibited particle apparent shrinkage in size. Additionally, NPF events were observed during the night-time and during episodes of high desert dust loadings. Particle formation rates and growth rates were comparable to those in urban environments, although our site is a rural one. Meteorological variables and trace gases played a role in explaining the intra-monthly variability of NPF events, but did not explain why summer month had the least NPF frequency. Similarly, pre-existing aerosol loading did not explain the observed seasonality. The month with the least NPF frequency were associated with higher H2SO4 concentrations but lower NOx concentration, which is an indicator of anthropogenic influence. Air masses arriving from the Middle East were not observed during these month, which could suggest that precursor vapors important for nucleation and growth are transported to our site from the Middle East. Further comprehensive measurements of precursor vapors are required to prove this hypothesis.
Published: 2020

6. Qualification of the Alphasense Optical Particle Counter for Inline Air Quality Monitoring

Author: Panayiota Antoniou, K. Barmpounis, George Biskos, Jean Sciare, Christos Keleshis, Panagiotis Vouterakos, M. Costi, and S. Bezantakos
Subjects: Air quality monitoring, stomatognathic diseases, 010504 meteorology & atmospheric sciences, Nuclear engineering, Environmental Chemistry, Environmental science, General Materials Science, 010501 environmental sciences, Particulates, 01 natural sciences, Pollution, Particle counter, 0105 earth and related environmental sciences
Abstract: The Alphasense optical particle counter (OPC) provides a low-cost and lightweight solution for measurements of the size and number concentration of airborne particulate matter (PM). The micro fan with which it is originally equipped cannot, however, achieve a high enough pressure differential for maintaining an adequate flow rate when connected to sampling/pretreatment aerosol lines, limiting its use for air quality monitoring. Here, we propose a simple modification on the sample flow system that enables the connection of the Alphasense OPC with sampling/pretreatment lines (e.g., dryers) commonly employed on ground observational sites, as well as its use onboard Unmanned Aerial Systems (UASs). Tests of the modified OPC using monodisperse polystyrene spherical (PS) particles having sizes between 0.8 and 2.5 μm show that both the sizing and counting performance of the modified instrument is in agreement with that of a calibrated reference OPC at concentrations from ca. 50 to 800 #/ml, which are typically encountered in the atmosphere in that size range. For particle number concentrations below or above this range, we observed a concentration-dependent counting efficiency, which can be corrected using a polynomial function derived from our measurements. Tests conducted under reduced pressure and temperature conditions demonstrate the capability of the modified OPC for accurately (i.e., within 13% deviation from the reference measurements) determining the size and number concentration of the sampled particles. The tests reported in this work show that the proposed modification can qualify the Alphasense OPC for use in both ground and aerial observations without affecting its performance, and at the same time maintaining its strongly desired characteristics (i.e., cost effectiveness and high portability). Copyright © 2020 American Association for Aerosol Research
Published: 2020
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7. Spatial and temporal (short and long-term) variability of submicron, fine and sub-10 μm particulate matter (PM1, PM2.5, PM10) in Cyprus

Author: Nikos Mihalopoulos, E. Vasiliadou, Chrysanthos Savvides, Mihalis Vrekoussis, Michael Pikridas, Savvas Kleanthous, Jean Sciare, and Christos Kizas
Subjects: Pollution, Atmospheric Science, 010504 meteorology & atmospheric sciences, media_common.quotation_subject, Industrial area, 010501 environmental sciences, Particulates, Atmospheric sciences, 01 natural sciences, Eastern mediterranean, Environmental science, Mass concentration (chemistry), East mediterranean, 0105 earth and related environmental sciences, General Environmental Science, media_common
Abstract: Long-term particulate matter (PM) mass concentration measurements have been performed in Cyprus at three major cities, one industrial area and two remote stations covering the entire southern part of the island in an effort to assess; i) the spatial and temporal variability of sub-10 μm (PM10), fine (PM2.5) and submicron (PM1) particulate matter in the eastern Mediterranean, ii) the main source areas contributing to their levels and iii) the relative contribution of regional and local anthropogenic and natural sources to PM levels. It was found that dust is responsible for the 33.6 ± 5.2% or about 10 μg m−3 of the annual PM10 levels reported in background stations; the latter underlines the significant contribution of natural sources on the ambient PM10 amounts in the eastern Mediterranean region. A significant (p
Published: 2018

8. The new TC-BC method and online instrument for the measurement of carbonaceous aerosols

Author: Anthony D. A. Hansen, Irena Kranjc, Judita Burger, Athanasia Vlachou, Martin Rigler, Jean Sciare, Janja Turšič, Jean Luc Jaffrezo, Griša Močnik, André S. H. Prévôt, Luka Drinovec, Gašper Lavrič, and Iasonas Stavroulas
Subjects: Detection limit, 010504 meteorology & atmospheric sciences, Analytical chemistry, chemistry.chemical_element, Carbon black, 010501 environmental sciences, Particulates, Aethalometer, 01 natural sciences, Aerosol, Volumetric flow rate, chemistry, Environmental science, Pyrolytic carbon, Carbon, 0105 earth and related environmental sciences
Abstract: We present the newly developed Total Carbon Analyzer (TCA08), and a new method for online speciation of carbonaceous aerosol with a high time resolution. The total carbon content is determined by flash heating of a sample collected on a quartz-fiber filter with a time base between 20 min and 24 h. The limit of detection is approximately 0.3 μgC, which corresponds to a concentration of 0.3 μgC/m3 at a sample flow rate of 16.7 LPM and a 1-hour sampling time base. The concentration of particulate organic carbon (OC) is determined by subtracting black carbon concentration, concurrently measured optically by an Aethalometer®, from the total carbon concentration measured by the TCA08. The combination of TCA08 and Aethalometer (AE33) is an easy-to-deploy and low maintenance continuous measurement technique for the high time resolution determination of organic and elemental carbon (EC) in different particulate matter size fractions, which avoids pyrolytic correction and need for high purity compressed gases. The equivalence of this new online method to the standardized off-line thermo-optical OC-EC methods was evaluated during a winter field campaign at an urban background location in Ljubljana, Slovenia. The organic matter-to-organic carbon ratio obtained from the comparison with an Aerosol Chemical Speciation Monitor (ACSM) was OM/OC = 1.8, in the expected range.
Published: 2019

9. Large-scale particulate air pollution and chemical fingerprint of volcanic sulfate aerosols from the 2014-2015 Holuhraun flood lava eruption of Bardarbunga volcano (Iceland)

Author: Colette Brogniez, Jean Sciare, Philippe Goloub, Yunjiang Zhang, Emmanuel Tison, Véronique Riffault, Hervé Delbarre, Nathalie Pujol-Söhne, Olivier Favez, Marie Boichu, Isabelle Chiapello, Jean-Eudes Petit, Shouwen Zhang, and Lieven Clarisse
Subjects: Pollution, Atmospheric Science, 010504 meteorology & atmospheric sciences, Lava, media_common.quotation_subject, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, complex mixtures, lcsh:Chemistry, Troposphere, chemistry.chemical_compound, Sulfate, Air quality index, 0105 earth and related environmental sciences, media_common, geography, geography.geographical_feature_category, Particulates, lcsh:QC1-999, Aerosol, lcsh:QD1-999, Volcano, chemistry, 13. Climate action, Environmental science, lcsh:Physics, Sciences exactes et naturelles
Abstract: Volcanic sulfate aerosols play a key role in air quality and climate. However, the rate of oxidation of sulfur dioxide (SO2) precursor gas to sulfate aerosols (SO42-) in volcanic plumes is poorly known, especially in the troposphere. Here we determine the chemical speciation as well as the intensity and temporal persistence of the impact on air quality of sulfate aerosols from the 2014–2015 Holuhraun flood lava eruption of Icelandic volcano Bárðarbunga. To do so, we jointly analyse a set of SO2 observations from satellite (OMPS and IASI) and ground-level measurements from air quality monitoring stations together with high temporal resolution mass spectrometry measurements of an Aerosol Chemical Speciation Monitor (ACSM) performed far from the volcanic source. We explore month/year long ACSM data in France from stations in contrasting environments, close and far from industrial sulfur-rich activities. We demonstrate that volcanic sulfate aerosols exhibit a distinct chemical signature in urban/rural conditions, with NO3:SO4 mass concentration ratios lower than for non-volcanic background aerosols. These results are supported by thermodynamic simulations of aerosol composition, using the ISORROPIA II model, which show that ammonium sulfate aerosols are preferentially formed at a high concentration of sulfate, leading to a decrease in the production of particulate ammonium nitrate. Such a chemical signature is however more difficult to identify at heavily polluted industrial sites due to a high level of background noise in sulfur. Nevertheless, aged volcanic sulfates can be distinguished from freshly emitted industrial sulfates according to their contrasting degree of anion neutralization. Combining AERONET (AErosol RObotic NETwork) sunphotometric data with ACSM observations, we also show a long persistence over weeks of pollution in volcanic sulfate aerosols, while SO2 pollution disappears in a few days at most. Finally, gathering 6-month long datasets from 27 sulfur monitoring stations of the EMEP (European Monitoring and Evaluation Programme) network allows us to demonstrate a much broader large-scale European pollution, in both SO2 and SO4, associated with the Holuhraun eruption, from Scandinavia to France. While widespread SO2 anomalies, with ground-level mass concentrations far exceeding background values, almost entirely result from the volcanic source, the origin of sulfate aerosols is more complex. Using a multi-site concentration-weighted trajectory analysis, emissions from the Holuhraun eruption are shown to be one of the main sources of SO4 at all EMEP sites across Europe and can be distinguished from anthropogenic emissions from eastern Europe but also from Great Britain. A wide variability in SO2:SO4 mass concentration ratios, ranging from 0.8 to 8.0, is shown at several stations geographically dispersed at thousands of kilometres from the eruption site. Despite this apparent spatial complexity, we demonstrate that these mass oxidation ratios can be explained by a simple linear dependency on the age of the plume, with a SO2-to-SO4 oxidation rate of 0.23 h−1. Most current studies generally focus on SO2, an unambiguous and more readily measured marker of the volcanic plume. However, the long persistence of the chemical fingerprint of volcanic sulfate aerosols at continental scale, as shown for the Holuhraun eruption here, casts light on the impact of tropospheric eruptions and passive degassing activities on air quality, health, atmospheric chemistry and climate., info:eu-repo/semantics/published
Published: 2019

10. Field characterization of the PM2.5 Aerosol Chemical Speciation Monitor: insights into the composition, sources, and processes of fine particles in eastern China

Author: André S. H. Prévôt, Yele Sun, Alexandre Albinet, Zhuang Wang, Douglas R. Worsnop, Philip Croteau, Jean Sciare, Lili Tang, Olivier Favez, Manjula R. Canagaratna, Florian Couvidat, Hongliang Zhang, Yunjiang Zhang, and John T. Jayne
Subjects: Atmospheric Science, Haze, 010504 meteorology & atmospheric sciences, Chemistry, 010501 environmental sciences, 01 natural sciences, Aerosol, chemistry.chemical_compound, Nitrate, 13. Climate action, Environmental chemistry, Particle, Relative humidity, Sulfate, Mass fraction, NOx, 0105 earth and related environmental sciences
Abstract: A PM2.5-capable aerosol chemical speciation monitor (ACSM) was deployed in urban Nanjing, China for the first time to measure in-situ non-refractory fine particle (NR-PM2.5) composition from October 20 to November 19, 2015 along with parallel measurements of submicron aerosol (PM1) species by a standard ACSM. Our results show that the NR-PM2.5 species (organics, sulfate, nitrate, and ammonium) measured by the PM2.5-ACSM are highly correlated (r2 > 0.9) with those measured by a Sunset Lab OC/EC Analyzer and a Monitor for AeRosols and GAses (MARGA). The comparisons between the two ACSMs illustrated similar temporal variations in all NR species between PM1 and PM2.5, yet substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm. On average, NR-PM1–2.5 contributed 53 % of the total NR-PM2.5 with sulfate and secondary organic aerosols (SOA) being the two largest contributors (26 % and 27 %, respectively). Rapid formation and thereafter growth of secondary inorganic aerosols (SIA) were observed under fog processing in NH3-rich environments. Positive matrix factorization of organic aerosol showed similar temporal variations in both primary and secondary OA between PM1 and PM2.5 although the mass spectra were slightly different due to more thermal decomposition on the capture vaporizer of PM2.5-ACSM. We observed an enhancement of SOA under high relative humidity conditions, which is associated with simultaneous increases in particle surface area, gas-phase species (NO2, SO2, and NH3) concentrations and aerosol water content driven by anthropogenic SIA. These results likely indicate an enhanced reactive uptake of SOA precursors upon aqueous particles. Therefore, reducing anthropogenic NOx, SO2, and NH3 emissions might not only reduce SIA but also SOA burden during haze episodes in China.
Published: 2017

11. 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

12. Source apportionment of fine PM by combining high time resolution organic and inorganic chemical composition datasets

Author: Jean Sciare, Michael Pikridas, Giulia Calzolai, M. Berico, Ettore Petralia, Franco Lucarelli, Claudio A. Belis, Fabrizia Cavalli, Belis, C. A., Pikridas, M., Lucarelli, F., Petralia, E., Cavalli, F., Calzolai, G., Berico, M., and Sciare, J.
Subjects: Online and offline, Atmospheric Science, Source apportionment, 010504 meteorology & atmospheric sciences, Ammonium nitrate, Analyser, Mineralogy, lcsh:QC851-999, 010501 environmental sciences, Inorganic ions, 01 natural sciences, chemistry.chemical_compound, On-line measurements, Particulate matter, Po valley, Positive matrix factorization, Receptor models, lcsh:Environmental pollution, On-line measurement, 0105 earth and related environmental sciences, General Environmental Science, Inorganic Chemical, Spectrometer, Aerosol, Chemical species, chemistry, lcsh:TD172-193.5, Environmental science, lcsh:Meteorology. Climatology, Receptor model, Source apportionment Particulate matter Po valley Receptor models Positive matrix factorization On-line measurements
Abstract: The use of high time resolution datasets of aerosol organic and inorganic species as input for receptor models poses a number of challenges. The estimation of uncertainties differ between different analytical methods and the number of chemical species may considerably vary among the different techniques. In this study, an approach to harmonise the uncertainties of different online datasets for their combined use in source apportionment with positive matrix factorization (PMF) is presented. The concentration of inorganic ions, organic fragments and trace elements were measured in a Po Valley background site using offline and online methods. Six-hour PM 2.5 samples were collected on filters and chemical analyses were carried out offline. Parallel hourly online measurements were made using the Xact 625 (CES LLC) XRF analyser and the Q-ACSM (Aerodyne Research Inc.) spectrometer.Online and offline methods produced comparable results for the major chemical component and some trace elements, while others (Ba, Ni, As and Se) showed limited comparability between the two methods. To ensure the consistency of the final PMF results, a multistep approach was adopted. In the first step PMF was run with only the offline dataset, in the second step only the online organic data were used and in a third step the PMF run was executed using only the online inorganic species. In the first three steps running PMF with homogeneous data made it possible to identify the main sources and produce chemical profiles to be used as internal reference for the final fourth step in which all the online species (major inorganic ions, m/z of organic fragments and trace elements) were combined. The sources of the final solution were developed using internally consistent chemical profiles and those from the literature and were validated by analysing the source diurnal variations and by comparison with external tracers. The sources identified were: biomass burning, aged biomass burning, secondary ammonium nitrate and ammonium sulphate, traffic, steel industry and waste thermal treatment. The source profiles with a large set of organic and inorganic species (87) and associated source diurnal variations resulting from this study are expected to serve as reference for future studies. Keywords: Source apportionment, Particulate matter, Po valley, Receptor models, Positive matrix factorization, On-line measurements
Published: 2019

13. Evidence of major secondary organic aerosol contribution to lensing effect black carbon absorption enhancement

Author: Francesco Canonaco, Dantong Liu, Alexandre Albinet, Tanguy Amodeo, Yunjiang Zhang, Jean Sciare, André S. H. Prévôt, Olivier Favez, Valérie Gros, Griša Močnik, Institut National de l'Environnement Industriel et des Risques (INERIS), Paul Scherrer Institute, Villigen, School of Earth and Environmental Sciences [Manchester] (SEES), University of Manchester [Manchester], Jozef Stefan Institute [Ljubljana] (IJS), Cyprus International Institute for the Environment and Public Health, 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), 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), and 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)
Subjects: lcsh:GE1-350, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, Global and Planetary Change, 010504 meteorology & atmospheric sciences, Global warming, Carbon black, 010501 environmental sciences, lcsh:QC851-999, Combustion, Atmospheric sciences, 7. Clean energy, 01 natural sciences, Aerosol, 13. Climate action, Environmental Chemistry, Environmental science, Particle, Climate model, lcsh:Meteorology. Climatology, Absorption (electromagnetic radiation), [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Air quality index, lcsh:Environmental sciences, 0105 earth and related environmental sciences
Abstract: Atmospheric black carbon (BC) has a strong positive, but still controversial, effect on global warming. In particular, BC absorption enhancement (Eabs) due to internal mixing with other chemical species—so-called lensing effect—is poorly assessed. This bottleneck partly relies on the lack of long-term in situ measurements of both the optical and chemical properties of BC-containing particles. Here, we present experimental and computational results showing a significant Eabs increase with the aerosol photochemical aging. This was associated with the production of highly oxidized secondary organic aerosols (SOA), especially at summertime. The 3-year-long continuous aerosol chemical and optical measurements used for the present study was obtained in the Paris region, France, which might be representative of near-future air quality within developing countries. These findings suggest that SOA could represent one of the most critical chemical species to be considered within climate models. Tiny remnants of combustion, known as black carbon, absorb solar radiation and warm the atmosphere—an effect that can be doubled by “lensing” from secondary organic aerosols. A multi-institution team led by Olivier Favez at the Institut National de l’Environnement Industriel et des Risques conducted a three-year observational and modeling study near Paris. The researchers tested a range of atmospheric constituents and found that secondary organic aerosols—adhered to black carbon particles—are the most important determinant of the enhanced warming. The aerosols are produced by photochemical reactions with a wide variety of natural and human-produced volatile organic compounds, and act to focus solar radiation to the core of the black carbon particle, especially during the particle aging process during summer. The findings—although specific to Paris—provide insights into the specific compounds leading to enhanced warming, and reveal the most effective targets for remediating their effect.
Published: 2018

14. Spatiotemporal variability and sources of aerosol water-soluble organic nitrogen (WSON), in the Eastern Mediterranean

Author: Evanthia Vargiakaki, Nikolaos Mihalopoulos, Georgios Grivas, Jean Sciare, Chrysanthos Savvides, Maria Tsagkaraki, and C. Theodosi
Subjects: Total organic carbon, Atmospheric Science, 010504 meteorology & atmospheric sciences, chemistry.chemical_element, 010501 environmental sciences, Mineral dust, Atmospheric sciences, 01 natural sciences, Nitrogen, Aerosol, chemistry.chemical_compound, Eastern mediterranean, Nitrate, chemistry, Total nitrogen, Environmental science, Ammonium, 0105 earth and related environmental sciences, General Environmental Science
Abstract: This study aims to characterize the variability and sources of water-soluble organic nitrogen (WSON) in aerosol over Cyprus in the Eastern Mediterranean. Measurements of PM10 particles were conducted during the calendar year of 2011 at two sites, located at a roadside location in Nicosia (urban traffic) and in the rural area of Agia Marina Xyliatou (regional background). Filter samples were analyzed for water-soluble total nitrogen (WSTN), nitrate and ammonium, to determine WSON. Additional analyses were performed, for water-soluble organic carbon (WSOC), organic and elemental carbon (OC and EC), major ions and trace metals. Annual mean WSON concentrations of 0.20 and 0.16 μgN m−3 were determined at the urban traffic and regional background sites, respectively. The organic fraction of WSTN was about 20%, with limited inter-site and seasonal variability. Distinct seasonal patterns were observed at the two sites, with warm-period concentrations being significantly higher at the regional background site, while the enhanced local emissions during winter at the traffic site smoothed out the observed variability. Mean WSON/WSOC ratios of 0.09–0.12 were calculated at the two sites, with the two parameters being weakly correlated. A roadside WSON enhancement was verified, although moderate on an annual basis (9%). However, concentrations in Nicosia were more than one time higher than the background during winter. The observed temporal and inter-site variability highlighted the necessity of source apportionment, which was performed using Positive Matrix Factorization (PMF) modeling, utilizing the analytical datasets at the two sites. In this way, the estimated contribution of regional transport of processed aerosols was found to be more pronounced at the regional background site (59% vs. 38%), while a sizeable input (35%) was linked to vehicular emissions at the traffic site. An additional anthropogenic impact, probably related to biomass burning, was estimated at both sites (16%), while contributions of natural sources like mineral dust (4–8%) and marine aerosol (2–3%) were smaller.
Published: 2021

15. LOAC: a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles – Part 2: First results from balloon and unmanned aerial vehicle flights

Author: Rony Akiki, Nicolas Verdier, Jean-Charles Dupont, C. Camy-Peyret, Pavla Dagsson-Waldhauserova, Jean Sciare, Haraldur Ólafsson, Eric Hamonou, Tjarda Roberts, Gwenaël Berthet, François Gensdarmes, Damien Vignelles, Vincent Duverger, Matthew Salter, Matthieu Gobbi, Thierry Tonnelier, Martin Piringer, Jean-Baptiste Renard, Matthieu Jeannot, Paul Zieger, Daniel Daugeron, Thierry Elias, Patrick Charpentier, Thibaut Lurton, Thierry Décamps, Jérôme Giacomoni, Benoit Couté, Jérémy Surcin, Samuel Mesmin, Marc Mallet, Vincent Crenn, François Dulac, Christophe Mazel, Fabrice Jégou, 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 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), Environnement SA, Centre National d'Études Spatiales [Toulouse] (CNES), 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), Service du Confinement et de l'Aérodispersion des polluants (IRSN/PSN-RES/SCA), Institut de Radioprotection et de Sûreté Nucléaire (IRSN), MeteoModem, Ury, MeteoModem, 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), HYGEOS (SARL), Stockholm University, Groupe Aerophile, University of Iceland [Reykjavik], Institut Pierre-Simon-Laplace (IPSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS), Fly-n-Sense, Mérignac, Fly-n-Sense, Zentralanstalt für Meteorologie und Geodynamik (ZAMG), ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Laboratoire d'aérologie (LA), Centre National de la Recherche Scientifique (CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Centre National de la Recherche Scientifique (CNRS)-Université Fédérale Toulouse Midi-Pyrénées-Centre National d'Études Spatiales [Toulouse] (CNES)-Météo France-Institut de Recherche pour le Développement (IRD)-Centre National de la Recherche Scientifique (CNRS)-Université Fédérale Toulouse Midi-Pyrénées-Centre National d'Études Spatiales [Toulouse] (CNES)-Météo France-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées, IRSN, PSN-RES, SCA, 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 d’Auvergne/LPC2E, ANR-10-LABX-100-01/10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), 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), 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), Département des Géosciences - 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), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National d'Études Spatiales [Toulouse] (CNES)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, lcsh:TA715-787, lcsh:Earthwork. Foundations, Mineral dust, Balloon, 01 natural sciences, lcsh:Environmental engineering, Aerosol, Troposphere, Ground level, Depth sounding, 13. Climate action, ChArMEx, 0103 physical sciences, Environmental science, Particle, lcsh:TA170-171, 010303 astronomy & astrophysics, Particle counter, 0105 earth and related environmental sciences, Remote sensing
Abstract: International audience; In the companion (Part I) paper, we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosol Counter), based on scattering measurements at angles of 12 and 60 •. That allows for some typology identification of particles (droplets, carbonaceous, salts, and mineral dust) in addition to size-segregated counting in a large diameter range from 0.2 µm up to possibly more than 100 µm depending on sampling conditions (Renard et al., 2016). Its capabilities overpass those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronic-sized absorbing carbonaceous particles in polluted air to very coarse particles (> 10–20 µm in diameter) in desert dust plumes or fog and clouds. LOAC's light and compact design allows measurements under all kinds of balloons , on-board unmanned aerial vehicles (UAVs) and at Published by Copernicus Publications on behalf of the European Geosciences Union. 3674 J.-B. Renard et al.: LOAC: a counter/sizer for ground-based and balloon measurements – Part 2 ground level. We illustrate here the first LOAC airborne results obtained from a UAV and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Vi-enna (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediter-ranean (during the Chemistry-Aerosol Mediterranean Experiment – ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in southwestern France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes.
Published: 2016

16. Long-term variability, source apportionment and spectral properties of black carbon at an urban background site in Athens, Greece

Author: Umesh Chandra Dumka, Evangelos Gerasopoulos, Iasonas Stavroulas, Nikos Mihalopoulos, Dimitris G. Kaskaoutis, K. Oikonomou, Maria Tsagkaraki, Jean Sciare, Aikaterini Bougiatioti, Georgios Grivas, Eleni Liakakou, and Despina Paraskevopoulou
Subjects: Atmospheric Science, Evening, 010504 meteorology & atmospheric sciences, Carbon black, 010501 environmental sciences, Seasonality, Atmospheric sciences, Aethalometer, medicine.disease, 01 natural sciences, Atmosphere, Diurnal cycle, medicine, Environmental science, Precipitation, 0105 earth and related environmental sciences, General Environmental Science, Morning
Abstract: This study aims to delineate the characteristics of Black Carbon (BC) in the atmosphere over Athens, Greece, using 4-year (May 2015–April 2019) Aethalometer (AE-33) measurements. The average BC concentration is 1.9 ± 2.5 μg m−3 (ranging from 0.1 to 32.7 μg m−3; hourly values), with a well-defined seasonality from 1.3 ± 1.1 μg m−3 in summer to 3.0 ± 4.0 μg m−3 in winter. Pronounced morning and evening/night peaks are found in the BC concentrations in winter, while during the rest of the seasons, this diurnal cycle appears to flatten out, with the exception of the morning traffic peak. On an annual basis, the biomass-burning fraction (BB%) of BC accounts for 22 ± 12%, while the fossil-fuel combustion (BCff) component (traffic emissions and domestic heating) dominates during summer (83%) and in the morning hours. BCwb exhibits higher contribution in winter (32%), especially during the night hours (39%). BC levels are effectively reduced by precipitation, while they significantly build-up for wind speeds
Published: 2020

17. Atmospheric Evolution of Molecular Weight Separated Brown Carbon from Biomass Burning

Author: Jenny P. S. Wong, Maria Tsagaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Subjects: 010504 meteorology & atmospheric sciences, 13. Climate action, 010501 environmental sciences, 01 natural sciences, 7. Clean energy, 0105 earth and related environmental sciences
Abstract: Biomass burning is a major source of atmospheric brown carbon (BrC) and through its absorption of UV/VIS radiation, it can play an important role on the planetary radiative balance and atmospheric photochemistry. The considerable uncertainty of BrC impacts is associated with its poorly constrained sources, transformations and atmospheric lifetime. Here we report laboratory experiments that examined changes in the optical properties of the water-soluble BrC fraction of biomass burning particles. Effects of direct UVB photolysis and OH oxidation in the aqueous phase on molecular weight-separated BrC were studied. Results indicated that low molecular weight (MW) BrC ( 10 hours) biomass burning emissions, poor linear correlations were found between light absorptivity and levoglucosan, consistent with other studies suggesting a short atmospheric lifetime for levoglucosan. However, a much stronger correlation between light absorptivity and total hydrous sugars was observed, suggesting that they may serve as more robust tracers for aged biomass burning emissions. Overall, the results from this study suggest that robust model estimates of BrC radiative impacts require consideration of the atmospheric aging of BrC and the stability of high-MW BrC.
Published: 2018

18. 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

19. Retrieval of ice nucleating particle concentrations from lidar observations: Comparison with airborne in-situ measurements from UAVs

Author: Ronny Engelmann, Silke Groβ, Eleni Marinou, Holger Baars, Jean Sciare, Vassilis Amiridis, Kalliopi-Artemis Voudouri, Dimitra Mamali, Michael Pikridas, Albert Ansmann, Matthias Tesche, Alexandra Tsekeri, Athanasios Nenes, Stavros Solomos, and Jann Schrod
Subjects: 010504 meteorology & atmospheric sciences, Particle number, Nucleation, Mineral dust, Atmospheric sciences, 01 natural sciences, Aerosol, Trace gas, Lidar, Deposition (aerosol physics), 13. Climate action, Environmental science, Parametrization (atmospheric modeling), 0105 earth and related environmental sciences
Abstract: Aerosols that are efficient ice nucleating particles (INPs) are crucial for the formation of cloud ice via heterogeneous nucleation in the atmosphere. The distribution of INPs on a large spatial scale and as a function of height determines their impact on clouds and climate. However, in-situ measurements of INPs provide sparse coverage over space and time. A promising approach to address this gap is to retrieve INP concentration profiles by combining particle concentration profiles derived by lidar measurements with INP efficiency parametrization for different freezing mechanisms (immersion freezing, deposition nucleation). Here, we assess the feasibility of this new method for both ground-based and space-borne lidar measurements, using airborne in-situ observations from an experimental campaign at Cyprus in April 2016. Analyzing five case studies we calculated the particle number concentrations using lidar measurements (with an uncertainty of 20 to 100 %) and we assessed the suitability of the different INP parameterizations with respect to the temperature range and the type of particles considered. Specifically, our analysis suggests that the parametrization of Ullrich et al. (2017) (applicable for the temperature range −50 °C to −33 °C) agree within 1 order of magnitude with the in-situ observations of nINP and can efficiently address the deposition nucleation pathway in dust-dominated environments. Additionally, the combination of the parameterizations of DeMott et al. (2015) and DeMott et al. (2010) (applicable 15 for the temperature range −35 °C to −9 °C) agree within 2 orders of magnitude with the in-situ observations of nINP and can efficiently address the immersion/condensation pathway of dust and continental/anthropogenic particles. The same conclusion is derived from the compilation of the parameterizations of DeMott et al. (2015) for dust and Ullrich et al. (2017) for soot. Furthermore, we applied this methodology to estimate the INP concentration profiles before and after a cloud formation, indicating the seeding role of the particles and their subsequent impact on cloud formation and characteristics. More synergistic data-sets are expected to become available in the future from EARLINET (European Aerosol Research Lidar NETwork) and in the frame of the European ACTRIS-RI (Aerosols, Clouds and Trace gases Research Infrastructure). Our analysis shown that the developed techniques, when applied on CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) space-born lidar observations, are in very good agreement with the in-situ measurements. This study give us confidence for the production of global 3D products of n250,dry, Sdry and nINP using the CALIPSO 13-yrs dataset. This could provide valuable insight into global height-resolved distribution of INP concentrations related to mineral dust, and possibly other aerosol types.
Published: 2018
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20. Driving parameters of biogenic volatile organic compounds and consequences on new particle formation observed at an eastern Mediterranean background site

Author: Isabelle Fronval, Thierry Léonardis, Valérie Gros, Karine Sellegri, Roland Sarda-Esteve, Jean Sciare, Stéphane Sauvage, Michael Pikridas, Mihalis Vrekoussis, Vincent Gaudion, Laurence Depelchin, Iasonas Stavroulas, Nadine Locoge, Dominique Baisnée, Bernard Bonsang, Chrysanthos Savvides, Cécile Debevec, Centre for Energy and Environment (CERI EE - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), 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), 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), Energy, Environment and Water Research Center (EEWRC), Cyprus Institute (CyI), Air Quality Section, Institute of Environmental Physics [Bremen] (IUP), University of Bremen, Centre for Energy and Environment (CERI EE), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), 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), and Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, Pinene, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, 01 natural sciences, lcsh:QC1-999, Aerosol, lcsh:Chemistry, chemistry.chemical_compound, lcsh:QD1-999, chemistry, 13. Climate action, TRACER, Environmental chemistry, ChArMEx, Environmental science, Relative humidity, Particle size, Precipitation, Sulfate, lcsh:Physics, Isoprene, 0105 earth and related environmental sciences
Abstract: As a part of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) and Cyprus Aerosols and Gas Precursors (ENVI-Med CyAr) programs, this study aims primarily to provide an improved understanding of the sources and the fate of volatile organic compounds (VOCs) in the eastern Mediterranean. More than 60 VOCs, including biogenic species (isoprene and eight monoterpenes) and oxygenated VOCs, were measured during a 1-month intensive field campaign performed in March 2015 at the Cyprus Atmospheric Observatory (CAO), a regional background site in Cyprus. VOC measurements were conducted using complementary online and offline techniques. Biogenic VOCs (BVOCs) were principally imputed to local sources and characterized by compound-specific daily cycles such as diurnal maximum for isoprene and nocturnal maximum for α- and β-pinenes, in connection with the variability of emission sources. The simultaneous study of pinene and isoprene temporal evolution and meteorological parameters has shown that BVOC emissions were mainly controlled by ambient temperature, precipitation and relative humidity. It was found that isoprene daytime emissions at CAO depended on temperature and solar radiation changes, whereas nocturnal BVOC concentrations (e.g., from oak and pine forests) were more prone to the relative humidity and temperature changes. Significant changes in monoterpene mixing ratios occurred during and after rainfall. The second part of the study focused on new particle formation (NPF) events at CAO. BVOCs are known to potentially play a role in the growth as well as in the early stages of formation of new atmospheric particles. Based on observations of the particle size distribution performed with a differential mobility particle sizer (DMPS) and the total number concentrations of particles larger than 1 nm diameter measured by particle size magnifier (PSM), NPF events were found on 14 out of 20 days of the field campaign. For all possible proxy parameters (meteorological parameters, calculated H2SO4 and measured gaseous compounds) having a role in NPF, we present daily variations of different classes during nucleation event and non-event days. NPF can occur at various condensational sink (CS) values and both under polluted and clean atmospheric conditions. High H2SO4 concentrations coupled with high BVOC concentrations seemed to be one of the most favorable conditions to observe NPF at CAO in March 2015. NPF event days were characterized by either (1) a predominant anthropogenic influence (high concentrations of anthropogenic source tracers observed), (2) a predominant biogenic influence (high BVOC concentrations coupled with low anthropogenic tracer concentrations), (3) a mixed influence (high BVOC concentrations coupled with high anthropogenic tracer concentrations) and (4) a marine influence (both low BVOC and anthropogenic tracer concentrations). More pronounced NPF events were identified during mixed anthropogenic–biogenic conditions compared to the pure anthropogenic or biogenic ones, for the same levels of precursors. Analysis of a specific NPF period of the mixed influence type highlighted that BVOC interactions with anthropogenic compounds enhanced nucleation formation and growth of newly formed particles. During this period, the nucleation-mode particles may be formed by the combination of high H2SO4 and isoprene amounts, under favorable meteorological conditions (high temperature and solar radiation and low relative humidity) along with low CS. During the daytime, growth of the newly formed particles, not only sulfate but also oxygen-like organic aerosol (OOA) mass contributions, increased in the particle phase. High BVOC concentrations were observed during the night following NPF events, accompanied by an increase in CS and in semi-volatile OOA contributions, suggesting further BVOC contribution to aerosol nighttime growth by condensing onto pre-existing aerosols.
Published: 2018

21. In situ formation and spatial variability of particle number concentration in a European megacity

Author: G. J. Engelhart, S.-L. von der Weiden-Reinmüller, Tuukka Petäjä, Agnès Borbon, Evangelia Kostenidou, André S. H. Prévôt, A. Wiedensohler, Matthias Beekmann, Monica Crippa, Lea Hildebrandt, Maik Merkel, Spyros N. Pandis, Markku Kulmala, Magda Psichoudaki, Frank Drewnick, Michael Pikridas, Suzanne Crumeyrolle, Alfons Schwarzenboeck, F. Freutel, Jean Sciare, Urs Baltensperger, 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), Max-Planck-Institut für Chemie (MPIC), Max-Planck-Gesellschaft, 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), 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), FOCUS GmbH, D-65510 Hunstetten, Germany, Paul Scherrer Institute (PSI), Department of Physics [Helsinki], Falculty of Science [Helsinki], Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Département d'Anatomo-pathologie, AP-HP - Hôpital Antoine Béclère [Clamart], Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP)-Assistance publique - Hôpitaux de Paris (AP-HP) (AP-HP), Max Planck Institute for Chemistry (MPIC), Leibniz Institute for Tropospheric Research (TROPOS), 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), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), University of Helsinki-University of Helsinki, Department of Physics, 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)-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), and Hôpital Antoine Béclère
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, Particle number, FORMATION EVENTS, LONG-TERM MEASUREMENTS, Atmospheric pollution, 010501 environmental sciences, Atmospheric sciences, 114 Physical sciences, 01 natural sciences, Climate effects, Sink (geography), TRACE GAS MEASUREMENTS, lcsh:Chemistry, SIZE-DISTRIBUTION DATA, LUNG-CANCER, ATMOSPHERIC PARTICLES, SECONDARY ORGANIC AEROSOL, 11. Sustainability, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, NUCLEATION MODE PARTICLES, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, geography, geography.geographical_feature_category, PARTICULATE AIR-POLLUTION, Particulate air pollution, lcsh:QC1-999, Plume, Megacity, lcsh:QD1-999, 13. Climate action, Environmental science, Spatial variability, PARIS METROPOLITAN-AREA, lcsh:Physics
Abstract: Ambient particle number size distributions were measured in Paris, France, during summer (1–31 July 2009) and winter (15 January to 15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation (MEGAPOLI) project. New particle formation (NPF) was observed only during summer on approximately 50 % of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10−3 s−1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from the Paris center during summer. The number concentration of particles with diameters exceeding 2.5 nm measured on the surface at the Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm−3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer, one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of 3 when it was downwind of Paris.
Published: 2015

22. Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols

Author: Bastien Sauvage, Marc Mallet, M Claeys, Jovanna Arndt, John C. Wenger, Karine Sellegri, Greg Roberts, Jean Sciare, Scripps Institution of Oceanography (SIO), University of California [San Diego] (UC San Diego), University of California-University of California, Centre national de recherches météorologiques (CNRM), 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)-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), Scripps Institution of Oceanography (SIO - UC San Diego), University of California (UC)-University of California (UC), Laboratoire d'aérologie (LAERO), 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), Environmental Research Institute [Cork] (ERI), University College Cork (UCC), Department of Chemistry [Cork], 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), Cyprus Institute (CyI), 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), Ohio State University [Columbus] (OSU), Laboratoire des sciences de l'ingénieur, de l'informatique et de l'imagerie (ICube), École Nationale du Génie de l'Eau et de l'Environnement de Strasbourg (ENGEES)-Université de Strasbourg (UNISTRA)-Institut National des Sciences Appliquées - Strasbourg (INSA Strasbourg), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut National de Recherche en Informatique et en Automatique (Inria)-Les Hôpitaux Universitaires de Strasbourg (HUS)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-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), 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), Aptel, Florence, 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), 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), Institut National des Sciences Appliquées - Strasbourg (INSA Strasbourg), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-École Nationale du Génie de l'Eau et de l'Environnement de Strasbourg (ENGEES)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), 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 Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)
Subjects: Mediterranean climate, Pollution, Atmospheric Science, 010504 meteorology & atmospheric sciences, media_common.quotation_subject, 010501 environmental sciences, 01 natural sciences, Mediterranean Basin, lcsh:Chemistry, Atmosphere, Mass concentration (chemistry), [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Sea salt aerosol, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, media_common, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.ENVI] Sciences of the Universe [physics]/Continental interfaces, environment, lcsh:QC1-999, AERONET, Aerosol, lcsh:QD1-999, 13. Climate action, ChArMEx, Climatology, Environmental science, lcsh:Physics
Abstract: As part of the ChArMEx-ADRIMED campaign (summer 2013), ground-based in situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m a.s.l.) to characterise the optical, physical and chemical properties of aerosols. During the observation period, a major influence of primary marine aerosols was detected (22–26 June), with a mass concentration reaching up to 6.5 µg m−3 and representing more than 40 % of the total PM10 mass concentration. Its relatively low ratio of chloride to sodium (average of 0.57) indicates a fairly aged sea salt aerosol at Ersa. In this work, an original data set, obtained from online real-time instruments (ATOFMS, PILS-IC) has been used to characterise the ageing of primary marine aerosols (PMAs). During this PMA period, the mixing of fresh and aged PMAs was found to originate from both local and regional (Gulf of Lion) emissions, according to local wind measurements and FLEXPART back trajectories. Two different aerosol regimes have been identified: a dust outbreak (dust) originating from Algeria/Tunisia, and a pollution period with aerosols originating from eastern Europe, which includes anthropogenic and biomass burning sources (BBP). The optical, physical and chemical properties of the observed aerosols, as well as their local shortwave (SW) direct radiative effect (DRE) in clear-sky conditions, are compared for these three periods in order to assess the importance of the direct radiative impact of PMAs compared to other sources above the western Mediterranean Basin. As expected, AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of −11 ± 4 at the surface and −8 ± 3 W m−2 at the top of the atmosphere (TOA). In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3–0.4 at 440 nm and column-integrated SSA of 0.90–0.95), induced a local instantaneous SW DRF that is nearly 3 times the effect calculated during the PMA period, with maximum values up to −40 W m−2 at the surface. A similar range of values were found for the BBP period to those during the dust period (SW DRF at the surface and TOA of −23 ± 6 and −15 ± 4 W m−2 respectively). The multiple sources of measurements at Ersa allowed the detection of a PMA-dominant period and their characterisation in terms of ageing, origin, transport, optical and physical properties and direct climatic impact.
Published: 2017

23. Aerosol Vertical Profiling Utilizing the Synergy of Lidar, Sunphotometry and In-Situ Measurements in the Framework of the ACTRIS-2 Campaign in Athens

Author: Evangelos Gerasopoulos, Alexandra Tsekeri, Stavros Solomos, Oleg Dubovik, Eleni Marinou, Ulla Wandinger, Ronny Engelmann, Nikos Mihalopoulos, I. P. Raptis, P. Kokkalis, Jean Sciare, Michael Kottas, Michael Pikridas, Holger Baars, Eleni Liakakou, Ioannis Binietoglou, Athanasios Nenes, Anton Lopatin, Albert Ansmann, and V. Amiridis
Subjects: Radiometer, 010504 meteorology & atmospheric sciences, Meteorology, Single-scattering albedo, 010501 environmental sciences, 7. Clean energy, 01 natural sciences, Trace gas, AERONET, Aerosol, Geography, Lidar, 13. Climate action, 11. Sustainability, Radiative transfer, Cloud condensation nuclei, 0105 earth and related environmental sciences, Remote sensing
Abstract: The importance of studying the aerosol vertical distribution is prominent in regional and climate studies. Aerosol profiling can contribute to the estimation of the cloud condensation nuclei (CCN) and ice nuclei (IN) concentrations, thus reducing the uncertainty in describing aerosol/cloud interactions. Aerosol absorption profiling contributes in defining the thermodynamic stability of the atmosphere while single scattering albedo profiling is crucial for radiative transfer calculations and climate modelling. The new Generalized Aerosol Retrieval from Radiometer and Lidar Combined data algorithm (GARRLiC) provides the opportunity to derive vertical profiles of aerosol microphysical properties combining active and passive ground-based remote sensing from lidar and sunphotometer measurements. GARRLiC has been developed in the frame of Aerosols, Clouds, and Trace gases Research InfraStructure Network (ACTRIS) to utilize the capabilities of combined European stations of the AErosol RObotic NETwork (AERONET) and the European Aerosol Research Lidar Network (EARLINET). Here, we utilize GARRLiC with measurements acquired during the Athens ACTRIS-2 campaign held during the winter months on 2016. The campaign focuses on the characterization of the alterations of the man-made aerosol pollution in the urban environment of Athens due to the economic crisis. Along with the remote sensing techniques, in situ measurements are performed providing absorption coefficients employing a micro-Aethalometer on board an Unmanned Aerial Vehicle (UAV). This detailed information is compared with GARRLiC profile products for an effective characterization of the aerosol properties along the atmospheric column.
Published: 2017
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24. Ice nucleating particles over the Eastern Mediterranean measured by unmanned aircraft systems

Author: Mihalis Vrekoussis, Albert Ansmann, Jaqueline Drücke, Joachim Curtius, Eleni Marinou, Jean Sciare, Christos Keleshis, Michael Pikridas, Nikos Mihalopoulos, Martin Ebert, Slobodan Nickovic, Daniel Weber, Bojan Cvetkovic, Jann Schrod, Heinz Bingemer, Holger Baars, and Ervens, B.
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, QC1-999, Mineral dust, 010502 geochemistry & geophysics, Atmospheric sciences, 01 natural sciences, complex mixtures, lcsh:Chemistry, Troposphere, Altitude, ddc:550, QD1-999, 0105 earth and related environmental sciences, Physics, Particulates, lcsh:QC1-999, Aerosol, Chemistry, Lidar, Deposition (aerosol physics), lcsh:QD1-999, 13. Climate action, Ice nucleus, Environmental science, lcsh:Physics
Abstract: During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from −20 to −30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L−1 were measured at −30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.
Published: 2017
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25. Sources and mixing state of summertime background aerosol in the north-western Mediterranean basin

Author: Jean Sciare, Karine Sellegri, Greg Roberts, Nicolas Marchand, Jovanna Arndt, John C. Wenger, Robert M. Healy, Marc Mallet, François Dulac, Karine Sartelet, Environmental Research Institute [Cork] (ERI), University College Cork (UCC), Department of Chemistry [Cork], Cyprus Institute (CyI), 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), 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), Scripps Institution of Oceanography (SIO - UC San Diego), University of California [San Diego] (UC San Diego), University of California (UC)-University of California (UC), Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-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), 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), Environmental Monitoring and Reporting Branch, Ontario Ministry of the Environment and Climate Change, 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), Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS), Scripps Institution of Oceanography (SIO), University of California-University of California, Météo France-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC), 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: Fine particulate matter, Atmospheric Science, Source apportionment, food.ingredient, 010504 meteorology & atmospheric sciences, Particle number, Fired power station, Chemical composition, Particle mass spectrometry, Secondary organic aerosol, 010501 environmental sciences, Combustion, complex mixtures, 01 natural sciences, lcsh:Chemistry, chemistry.chemical_compound, food, Methanesulfonic acid water, Laser desorption ionization, Mass concentration (chemistry), Sulfate, Sea salt aerosol, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Chemistry, Sea salt, lcsh:QC1-999, Aerosol, Long range transport, Real time, lcsh:QD1-999, 13. Climate action, Environmental chemistry, ChArMEx, [SDE]Environmental Sciences, Particle, lcsh:Physics
Abstract: International audience; An aerosol time-of-flight mass spectrometer (ATOFMS) was employed to provide real-time single particle mixing state and thereby source information for aerosols impacting the western Mediterranean basin during the ChArMEx-ADRIMED and SAF-MED campaigns in summer 2013. The ATOFMS measurements were made at a ground-based remote site on the northern tip of Corsica. Twenty-seven distinct ATOFMS particle classes were identified and subsequently grouped into eight general categories: EC-rich (elemental carbon), K-rich, Na-rich, amines, OC-rich (organic carbon), V-rich, Fe-rich and Ca-rich particles. Mass concentrations were reconstructed for the ATOFMS particle classes and found to be in good agreement with other co-located quantitative measurements (PM 1 , black carbon (BC), organic carbon, sulfate mass and am-monium mass). Total ATOFMS reconstructed mass (PM 2.5) accounted for 70–90 % of measured PM 10 mass and was comprised of regionally transported fossil fuel (EC-rich) and biomass burning (K-rich) particles. The accumulation of these transported particles was favoured by repeated and extended periods of air mass stagnation over the western Mediterranean during the sampling campaigns. The single particle mass spectra proved to be valuable source markers, allowing the identification of fossil fuel and biomass burning combustion sources, and was therefore highly complementary to quantitative measurements made by Particle into Liquid Sampler ion chromatography (PILS-IC) and an aerosol chemical speciation monitor (ACSM), which have demonstrated that PM 1 and PM 10 were comprised predominantly of sulfate, ammonium and OC. Good temporal agreement was observed between ATOFMS EC-rich and K-rich particle mass concentrations and combined mass concentrations of BC, sulfate, ammonium and low volatility oxygenated organic aerosol (LV-OOA). This combined information suggests that combustion of fossil fuels and biomass produced primary EC-and OC-containing particles, which then accumulated ammonium, sulfate and alkylamines during regional transport. Three other sources were also identified: local biomass burning, marine and shipping. Local combustion particles Published by Copernicus Publications on behalf of the European Geosciences Union. 6976 J. Arndt et al.: Sources and mixing state of summertime background aerosol (emitted in Corsica) contributed little to PM 2.5 particle number and mass concentrations but were easily distinguished from regional combustion particles. Marine emissions comprised fresh and aged sea salt: the former was detected mostly during a 5-day event during which it accounted for 50–80 % of sea salt aerosol mass, while the latter was detected throughout the sampling period. Dust was not efficiently detected by the ATOFMS, and support measurements showed that it was mainly in the PM 2.5–10 fraction. Shipping particles, identified using markers for heavy fuel oil combustion , were associated with regional emissions and represented only a small fraction of PM 2.5 particle number and mass concentration at the site.
Published: 2017

26. Multi-tracer approach to characterize domestic wood burning in Athens (Greece) during wintertime

Author: Pavlos Zarmpas, K. Bairachtari, Th. Maggos, Iasonas Stavroulas, Basil E. Psiloglou, Roland Sarda-Esteve, Nikos Mihalopoulos, Evangelos Gerasopoulos, L. Fourtziou, C. Theodosi, Jean Sciare, Eleni Liakakou, Nicolas Bonnaire, Aikaterini Bougiatioti, 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), 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, Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, Chemistry, Levoglucosan, Athens greece, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, 7. Clean energy, Atmosphere, chemistry.chemical_compound, Deposition (aerosol physics), 13. Climate action, TRACER, 11. Sustainability, Wood burning, Precipitation, Biomass burning, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, General Environmental Science
Abstract: During the last years the atmosphere of the Great Athens Area (GAA) and other Greek cities is burdened from extended residential biomass burning for heating purposes. In this work, a series of near real-time and off-line biomass burning tracers are analyzed during intense wood burning events in Athens. The measurements were conducted at an urban background site located in the center of Athens, and in the heart of wood burning activities (winter 2013–2014). The measured tracers include high resolution measurements of non-sea salt potassium (nss-K+), wood burning black carbon (BCwb), the m/z 60 fragment associated with levoglucosan and monosaccharide anhydrides (levoglucosan, mannosan and galactosan) determined on selected filter samples. The suitability of these tracers was evaluated when the prevailing meteorological conditions with low dispersion and deposition mechanisms (low wind speed, absence of precipitation) were associated with high biomass burning emissions at nighttime. During the severe smog periods, the levels of K+, BCwb, m/z 60 and levoglucosan were up to 2.2 μg m−3, 12.5 μg m−3, 3.4 μg m−3 and 8.6 μg m−3, respectively, higher by a factor of at least two, relatively to the non smog periods due to biomass burning. Correlations between biomass burning tracers as well as between monosaccharide anhydrides provided information about the type of material and wood being burned.
Published: 2017

27. Characterising an intense PM pollution episode in March 2015 in France from multi-site approach and near real time data : Climatology, variabilities, geographical origins and model evaluation

Author: Jean-Eudes Petit, Alexandre Ockler, Olivier Favez, Yann Pellan, Jean Sciare, Benoit Rocq, Tanguy Amodeo, Didier Grenier, Laurent Menut, Valérie Gros, Bertrand Bessagnet, Frédérik Meleux, 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), Air Lorraine, Institut National de l'Environnement Industriel et des Risques (INERIS), 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), ATMO Picardie, Cyprus Institute (CyI), 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), 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), and 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)
Subjects: Pollution, Atmospheric Science, 010504 meteorology & atmospheric sciences, media_common.quotation_subject, FRANCE, 010501 environmental sciences, Aethalometer, 01 natural sciences, chemistry.chemical_compound, Nitrate, POLLUTION, Urban background, 11. Sustainability, AETHALOMETER, 0105 earth and related environmental sciences, General Environmental Science, media_common, Advection, Multi site, AEROSOL, Particulates, AEROSOL CHEMICAL SPECIATION MONITOR, Aerosol, MODEL, chemistry, 13. Climate action, Climatology, ACSM, [SDE]Environmental Sciences, Environmental science
Abstract: International audience; During March 2015, a severe and large-scale particulate matter (PM) pollution episode occurred in France. Measurements in near real-time of the major chemical composition at four different urban background sites across the country (Paris, Creil, Metz and Lyon) allowed the investigation of spatiotemporal variabilities during this episode. A climatology approach showed that all sites experienced clear unusual rain shortage, a pattern that is also found on a longer timescale, highlighting the role of synoptic conditions over Wester-Europe. This episode is characterized by a strong predominance of secondary pollution, and more particularly of ammonium nitrate, which accounted for more than 50% of submicron aerosols at all sites during the most intense period of the episode. Pollution advection is illustrated by similar variabilities in Paris and Creil (distant of around 100 km), as well as trajectory analyses applied on nitrate and sulphate. Local sources, especially wood burning, are however found to contribute to local/ regional sub-episodes, notably in Metz. Finally, simulated concentrations from Chemistry-Transport model CHIMERE were compared to observed ones. Results highlighted different patterns depending on the chemical components and the measuring site, reinforcing the need of such exercises over other pollution episodes and sites.
Published: 2017

28. The filter-loading effect by ambient aerosols in filter absorption photometers depends on the coating of the sampled particles

Author: Ágnes Filep, Emily A. Bruns, Griša Močnik, Rajan K. Chakrabarty, Jean-Eudes Petit, Jean Sciare, Luka Drinovec, Robert Wolf, Ian J. Arnold, André S. H. Prévôt, Hans Moosmüller, Asta Gregorič, Olivier Favez, Peter Zotter, Aerosol D.O.O, Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Institut National de l'Environnement Industriel et des Risques (INERIS), 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), Energy, Environment and Water Research Center (EEWRC), Cyprus Institute (CyI), 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: Atmospheric Science, Ammonium sulfate, Materials science, 010504 meteorology & atmospheric sciences, Infrared, Analytical chemistry, 010501 environmental sciences, engineering.material, Aethalometer, Combustion, 01 natural sciences, law.invention, chemistry.chemical_compound, Coating, law, lcsh:TA170-171, 0105 earth and related environmental sciences, lcsh:TA715-787, lcsh:Earthwork. Foundations, Carbon black, Photometer, Aerosol, lcsh:Environmental engineering, chemistry, 13. Climate action, [SDE]Environmental Sciences, engineering
Abstract: Black carbon is a primary aerosol tracer for high-temperature combustion emissions and can be used to characterize the time evolution of its sources. It is correlated with a decrease in public health and contributes to atmospheric warming. Black carbon measurements are usually conducted with absorption filter photometers, which are prone to several artifacts, including the filter-loading effect – a saturation of the instrumental response due to the accumulation of the sample in the filter matrix. In this paper, we investigate the hypothesis that this filter-loading effect depends on the optical properties of particles present in the filter matrix, especially on the black carbon particle coating. We conducted field campaigns in contrasting environments to determine the influence of source characteristics, particle age and coating on the magnitude of the filter-loading effect. High-time-resolution measurements of the filter-loading parameter in filter absorption photometers show daily and seasonal variations of the effect. The variation is most pronounced in the near-infrared region, where the black carbon mass concentration is determined. During winter, the filter-loading parameter value increases with the absorption Ångström exponent. It is suggested that this effect is related to the size of the black carbon particle core as the wood burning (with higher values of the absorption Ångström exponent) produces soot particles with larger diameters. A reduction of the filter-loading effect is correlated with the availability of the coating material. As the coating of ambient aerosols is reduced or removed, the filter-loading parameter increases. Coatings composed of ammonium sulfate and secondary organics seem to be responsible for the variation of the loading effect. The potential source contribution function analysis shows that high values of the filter-loading parameter in the infrared are indicative of local pollution, whereas low values of the filter-loading parameter result from ageing and coating during long-range transport. Our results show that the filter-loading parameter can be used as a proxy for determination of the particle coating, thus allowing for differentiation between local/fresh and transported/aged particles.
Published: 2017

29. Stable isotopes measurements reveal dual carbon pools contributing to organic matter enrichment in marine aerosol

Author: Agne Masalaite, Willy Maenhaut, Colin D. O'Dowd, Vidmantas Remeikis, Jurgita Ovadnevaite, Andrius Garbaras, Darius Ceburnis, Jean Sciare, Magda Claeys, Dominique Baisnée, 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), 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), and 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)
Subjects: 010504 meteorology & atmospheric sciences, 010501 environmental sciences, 01 natural sciences, Article, Carbon cycle, PHYTOPLANKTON, Dissolved organic carbon, sea spray aerosol, origin, Organic matter, 14. Life underwater, fractionation, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, chemistry.chemical_classification, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Multidisciplinary, photosynthesis, Stable isotope ratio, Ecology, ORIGIN, PHOTOSYNTHESIS, FRACTIONATION, Particulates, Sea spray, ATMOSPHERE, Equilibrium fractionation, Chemistry, chemistry, 13. Climate action, Isotopes of carbon, Environmental chemistry, Earth and Environmental Sciences, SEA SPRAY AEROSOL, atmosphere, phytoplankton, Engineering sciences. Technology
Abstract: Stable carbon isotope ratios in marine aerosol collected over the Southern Indian Ocean revealed δ13C values ranging from −20.0‰ to −28.2‰. The isotope ratios exhibited a strong correlation with the fractional organic matter (OM) enrichment in sea spray aerosol. The base-level isotope ratio of −20.0‰ is characteristic of an aged Dissolved Organic Matter (DOM) pool contributing a relatively homogeneous background level of DOM to oceanic waters. The range of isotope ratios, extending down to −28.2‰, is characteristic of more variable, stronger, and fresher Particulate Organic Matter (POM) pool driven by trophic level interactions. We present a conceptual dual-pool POM-DOM model which comprises a ‘young’ and variable POM pool which dominates enrichment in sea-spray and an ‘aged’ but invariant DOM pool which is, ultimately, an aged end-product of processed ‘fresh’ POM. This model is harmonious with the preferential enrichment of fresh colloidal and nano-gel lipid-like particulate matter in sea spray particles and the observed depleted δ13C ratio resulting from isotope equilibrium fractionation coupled with enhanced plankton photosynthesis in cold water (−2 °C to +8 °C). These results re-assert the hypothesis that OM enrichment in sea-spray is directly linked to primary production and, consequently, can have implications for climate-aerosol-cloud feedback systems.
Published: 2016

30. Maïdo observatory: a new high-altitude station facility at Reunion Island (21° S, 55° E) for long-term atmospheric remote sensing and in situ measurements

Author: Françoise Posny, Yann Courcoux, F. Desmet, Karine Sellegri, Robert Delmas, M. De Mazière, Thierry Portafaix, Alain Hauchecorne, Jean Sciare, J. Leclair de Bellevue, Franck Gabarrot, S. Godin Beekmann, Guillaume Payen, Jean-Luc Baray, Aurélie Colomb, C. Vuillemin, Davide Dionisi, Valentin Duflot, Jacques Porteneuve, Jean-Pierre Cammas, T. Gaudo, Christelle Barthe, Philippe Ricaud, Pierre Tulet, Jean-Marc Metzger, Hélène Vérèmes, Abdel Abchiche, Michel Ramonet, Christian Hermans, Philippe Keckhut, Christophe Hoareau, 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, 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), 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), STRATO - 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), Belgian Institute for Space Aeronomy / Institut d'Aéronomie Spatiale de Belgique (BIRA-IASB), Spectroscopie de l'atmosphère, Service de Chimie Quantique et Photophysique, Université libre de Bruxelles (ULB), 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), 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), ICOS-RAMCES (ICOS-RAMCES), 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), Chimie Atmosphérique Expérimentale (CAE), 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), Division technique INSU/SDU (DTI), Institut national des sciences de l'Univers (INSU - CNRS)-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), Centre National de la Recherche Scientifique (CNRS)-Université de La Réunion (UR)-Institut national des sciences de l'Univers (INSU - CNRS)-Météo France, 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)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - 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), 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), 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), Groupe d'étude de l'atmosphère météorologique (CNRM-GAME), and Institut national des sciences de l'Univers (INSU - 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], Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, lcsh:TA715-787, lcsh:Earthwork. Foundations, Climate change, Subtropics, 01 natural sciences, lcsh:Environmental engineering, 010309 optics, Troposphere, Lidar, Observatory, 0103 physical sciences, Environmental science, 14. Life underwater, lcsh:TA170-171, Sociologie politique, Southern Hemisphere, Stratosphere, Sea level, 0105 earth and related environmental sciences, Remote sensing
Abstract: Since the nineties, atmospheric measurement systems have been deployed at Reunion Island, mainly for monitoring the atmospheric composition in the framework of NDSC/NDACC (Network for the Detection of Stratospheric< /i> Change/Network for the Detection of Atmospheric Composition Change). The location of Reunion Island presents a great interest because there are very few multi-instrumented stations in the tropics and particularly in the southern hemisphere. In 2012, a new observatory was commissioned in Maïdo at 2200 m above sea level: it hosts various instruments for atmospheric measurements, including lidar systems, spectro-radiometers and in situ gas and aerosol measurements. This new high-altitude Maïdo station provides an opportunity: 1. to improve the performance of the optical instruments above the marine boundary layer, and to open new perspectives on upper troposphere and lower stratosphere studies; 2. to develop in situ measurements of the atmospheric composition for climate change surveys, in a reference site in the tropical/subtropical region of the southern hemisphere; 3. to offer trans-national access to host experiments or measurement campaigns for focused process studies. © 2013 Author(s)., SCOPUS: ar.j, info:eu-repo/semantics/published
Published: 2013

31. Identification of marine and continental aerosol sources in Paris using high resolution aerosol mass spectrometry

Author: R. Chirico, Monica Crippa, André S. H. Prévôt, Jean Sciare, Urs Baltensperger, Claudia Mohr, M. F. Heringa, Peter F. DeCarlo, Imad El Haddad, Nicolas Marchand, and Jay G. Slowik
Subjects: chemistry.chemical_classification, Atmospheric Science, 010504 meteorology & atmospheric sciences, Resolution (mass spectrometry), Mineralogy, Salt (chemistry), 010501 environmental sciences, Aethalometer, Mass spectrometry, 01 natural sciences, 7. Clean energy, Methanesulfonic acid, Aerosol, chemistry.chemical_compound, Geophysics, chemistry, 13. Climate action, Space and Planetary Science, Environmental chemistry, Earth and Planetary Sciences (miscellaneous), Environmental science, Aerosol mass spectrometry, Sulfate, 0105 earth and related environmental sciences
Abstract: [1] Major summertime aerosol emission sources in Paris were assessed using a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The application of positive matrix factorization (PMF) to the highly mass and time-resolved AMS measurements allowed the identification of primary and secondary sources of organic (OA) and sulfate aerosols. Primary anthropogenic emissions contributed on average ~27% (14.7% cooking, 12% traffic) to the total organic mass, while the major contribution to the organic fraction was associated with secondary formation products. Low-volatility oxygenated OA (LV-OOA, 25.2%) and semi-volatile oxygenated OA (SV-OOA, 32.4%) factors were classified as SOA. An additional component with high S : C and O : C ratios was identified and attributed to marine emissions (marine organic aerosol, MOA), owing to its high correlation with methanesulfonic acid (R2 = 0.84) and contributing on average 15.7% to the total OA mass, even in the continental megacity of Paris. Non-sea salt sulfate was apportioned by including both organic and sulfate ions in the PMF data matrix. This allowed apportionment of submicron sulfate to continental versus marine sources. A detailed source apportionment of PM1 combining AMS, aethalometer, and filter data is presented.
Published: 2013

32. Geochemistry of pm10 over europe during the emep intensive measurement periods in summer 2012 and winter 2013

Author: Anna Ripoll, Noemí Pérez, Hans Areskoug, Gerald Spindler, Violeta Balan, Darius Ceburnis, Wenche Aas, Jean Philippe Putaud, Sébastien Conil, Kornélia Imre, Marta Mitosinkova, Colin D. O'Dowd, Nikolaos Mihalopoulos, Franco Lucarelli, Jean Sciare, Teresa Moreno, Jean Luc Jaffrezo, Andrés Alastuey, Sarah Leeson, Véronique Riffault, Maria Catrambone, Jorge Pey, Karine Sellegri, Christoph Hueglin, Xavier Querol, José Carlos Cerro, Lusine Gevorgyan, Fabrizia Cavalli, and Karl Espen Yttri
Subjects: Mediterranean climate, Atmospheric Science, 010504 meteorology & atmospheric sciences, atmospheric aerosols, mediterranean basin, 010501 environmental sciences, Mineral dust, Spatial distribution, 01 natural sciences, Mediterranean Basin, complex mixtures, industrial sites, saharan dust, size distribution, african dust transport, 0105 earth and related environmental sciences, particulate matter, daily mortality, source apportionment, Particulates, Eastern european, Eastern mediterranean, 13. Climate action, Climatology, mineral-dust, Period (geology), Environmental science, Physical geography
Abstract: The third intensive measurement period (IMP) organised by the European Monitoring and Evaluation Programme (EMEP) under the UNECE CLTRAP took place in summer 2012 and winter 2013, with PM10 filter samples concurrently collected at 20 (16 EMEP) regional background sites across Europe for subsequent analysis of their mineral dust content. All samples were analysed by the same or a comparable methodology. Higher PM10 mineral dust loadings were observed at most sites in summer (0.5–10 µg m−3) compared to winter (0.2–2 µg m−3), with the most elevated concentrations in the southern- and easternmost countries, accounting for 20–40 % of PM10. Saharan dust outbreaks were responsible for the high summer dust loadings at western and central European sites, whereas regional or local sources explained the elevated concentrations observed at eastern sites. The eastern Mediterranean sites experienced elevated levels due to African dust outbreaks during both summer and winter. The mineral dust composition varied more in winter than in summer, with a higher relative contribution of anthropogenic dust during the former period. A relatively high contribution of K from non-mineral and non-sea-salt sources, such as biomass burning, was evident in winter at some of the central and eastern European sites. The spatial distribution of some components and metals reveals the influence of specific anthropogenic sources on a regional scale: shipping emissions (V, Ni, and SO42−) in the Mediterranean region, metallurgy (Cr, Ni, and Mn) in central and eastern Europe, high temperature processes (As, Pb, and SO42−) in eastern countries, and traffic (Cu) at sites affected by emissions from nearby cities.
Published: 2016

33. Size-Resolved Identification, Characterization, and Quantification of Primary Biological Organic Aerosol at a European Rural Site

Author: Timor Shuster-Meiseles, Paola Fermo, Adéla Křepelová, Yinon Rudich, André S. H. Prévôt, Imad El Haddad, Robert Wolf, Jay G. Slowik, Mario El Kazzi, Francesco Canonaco, Jean Sciare, Christoph Hueglin, Kaspar R. Daellenbach, Mira Flasch, Yinon Mazar, Jürgen Schnelle-Kreis, A. Kasper-Giebl, Raquel Gonzalez, Carlo Bozzetti, Gülcin Abbaszade, Urs Baltensperger, Ralf Zimmermann, 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), 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: Rural Population, 010504 meteorology & atmospheric sciences, Air Microbiology, Carbohydrates, 010501 environmental sciences, Mass spectrometry, 01 natural sciences, Polymerase Chain Reaction, Gas Chromatography-Mass Spectrometry, Mass Spectrometry, Environmental Chemistry, Humans, Organic matter, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, chemistry.chemical_classification, Aerosols, Spores, Bacterial, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Primary (chemistry), General Chemistry, Particulates, Spores, Fungal, Characterization (materials science), Aerosol, chemistry, 13. Climate action, Environmental chemistry, Environmental science, Particulate Matter, Gas chromatography, Seasons, Gas chromatography–mass spectrometry, Switzerland, Environmental Monitoring
Abstract: Primary biological organic aerosols (PBOA) represent a major component of the coarse organic matter (OMCOARSE, aerodynamic diameter2.5 μm). Although this fraction affects human health and the climate, its quantification and chemical characterization currently remain elusive. We present the first quantification of the entire PBOACOARSE mass and its main sources by analyzing size-segregated filter samples collected during the summer and winter at the rural site of Payerne (Switzerland), representing a continental Europe background environment. The size-segregated water-soluble OM was analyzed by a newly developed offline aerosol mass spectrometric technique (AMS). Collected spectra were analyzed by three-dimensional positive matrix factorization (3D-PMF), showing that PBOA represented the main OMCOARSE source during summer and its contribution to PM10 was comparable to that of secondary organic aerosol. We found substantial cellulose contributions to OMCOARSE, which in combination with gas chromatography mass spectrometry molecular markers quantification, underlined the predominance of plant debris. Quantitative polymerase chain reaction (qPCR) analysis instead revealed that the sum of bacterial and fungal spores mass represented only a minor OMCOARSE fraction (0.1%). X-ray photoelectron spectroscopic (XPS) analysis of C and N binding energies throughout the size fractions revealed an organic N increase in the PM10 compared to PM1 consistent with AMS observations.
Published: 2016

34. A Modelling Perspective of the Summer 2013 and 2014 ChArMEx/SAFMED Chemistry Intensive Campaigns: Origin of Photo-Oxidant and Aerosol Formation over the Western Mediterranean

Author: Agnès Borbon, Evelyne Freney, Nicolas Marchand, Matthias Beekmann, Guillaume Siour, Jean-Pierre Kervern, Sébastien Sauvage, Jean Sciare, Corinne Jambert, Valérie Gros, Paola Formenti, Karine Sellegri, François Dulac, Hervé Petetin, Pierre Durand, Eric Hamonou, Arineh Cholakian, 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), 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), and 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)
Subjects: Mediterranean climate, Pollution, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 010504 meteorology & atmospheric sciences, Chemistry, media_common.quotation_subject, 010502 geochemistry & geophysics, Atmospheric sciences, 01 natural sciences, 7. Clean energy, Mediterranean Basin, Aerosol, Geography, 13. Climate action, Climatology, Emission inventory, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, Dust emission, media_common
Abstract: During summers 2013 and 2014, two three weeks intensive campaign took place over the western Mediterranean basin in order to investigate photo-oxidant and aerosol sources over the region. Within the frame of the MISTRALS/ChArMEx (Chemistry-Aerosol Mediterranean Experiment) program and the ANR/SAFMED (Secondary Aerosol Formation in the MEDiterranean) project, this campaign included an extensive experimental set-up based on ground-based, balloon-borne, aircraft and satellite measurements. In this paper, a modeling perspective of the campaign is given, based on simulations with the regional chemistry-transport model, CHIMERE, in a configuration shaped for the Mediterranean region. Major sources of photo-oxidants, and aerosols are addressed: long range transport from continental Europe, pollution build-up from shipping emissions, marine emissions, organic aerosol formation from biogenic and anthropogenic VOC emissions, dust emissions.
Published: 2016

35. LOAC: a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles – Part 1: Principle of measurements and instrument evaluation

Author: Tjarda Roberts, Fabrice Jégou, Matthew Salter, Eric Hamonou, Jérémy Surcin, Matthieu Gobbi, Matthieu Jeannot, Samuel Mesmin, Marc Mallet, Daniel Daugeron, François Gensdarmes, Thierry Décamps, Gwenaël Berthet, Thierry Tonnelier, Jérôme Giacomoni, Vincent Crenn, Benoit Couté, Nicolas Verdier, Paul Zieger, Jean-Baptiste Renard, Damien Vignelles, Vincent Duverger, François Dulac, Thierry Elias, Rony Akiki, Jean-Charles Dupont, Claude Camy-Peyret, Pavla Dagsson-Waldhauserova, Christophe Mazel, Haraldur Ólafsson, Jean Sciare, Martin Piringer, Patrick Charpentier, Thibaut Lurton, 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 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), Environnement SA, Groupe Aerophile, Centre National d'Études Spatiales [Toulouse] (CNES), 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), Service du Confinement et de l'Aérodispersion des polluants (IRSN/PSN-RES/SCA), Institut de Radioprotection et de Sûreté Nucléaire (IRSN), MeteoModem, Ury, MeteoModem, 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), HYGEOS (SARL), Stockholm University, University of Bergen (UiB), University of Iceland [Reykjavik], Institut Pierre-Simon-Laplace (IPSL (FR_636)), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-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 Diderot - Paris 7 (UPD7)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Fly-n-Sense, Mérignac, Fly-n-Sense, Zentralanstalt für Meteorologie und Geodynamik (ZAMG), Université d'Auvergne - Clermont-Ferrand I (UdA), 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), 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, IRSN, PSN-RES, SCA, 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), 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), 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 d'aérologie (LA), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), École normale supérieure - Paris (ENS Paris)-École normale supérieure - Paris (ENS Paris), University of Bergen (UIB), École normale supérieure - Paris (ENS Paris)-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 Diderot - Paris 7 (UPD7)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique et chimie de l'environnement et de l'Espace (LPC2E), UMR 7328 CNRS/Université d'Orléans, and Université d'Orléans (UO)
Subjects: Atmospheric Science, Materials science, 010504 meteorology & atmospheric sciences, Particle number, [SDU.STU.ME]Sciences of the Universe [physics]/Earth Sciences/Meteorology, 01 natural sciences, 010309 optics, Troposphere, Optics, 11. Sustainability, 0103 physical sciences, [PHYS.PHYS.PHYS-INS-DET]Physics [physics]/Physics [physics]/Instrumentation and Detectors [physics.ins-det], lcsh:TA170-171, Stratosphere, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Range (particle radiation), Scattering, business.industry, lcsh:TA715-787, lcsh:Earthwork. Foundations, Sea spray, Aerosol, lcsh:Environmental engineering, 13. Climate action, ChArMEx, Particle, business
Abstract: The study of aerosols in the troposphere and in the stratosphere is of major importance both for climate and air quality studies. Among the numerous instruments available, optical aerosol particles counters (OPCs) provide the size distribution in diameter range from about 100 nm to a few tens of µm. Most of them are very sensitive to the nature of aerosols, and this can result in significant biases in the retrieved size distribution. We describe here a new versatile optical particle/sizer counter named LOAC (Light Optical Aerosol Counter), which is light and compact enough to perform measurements not only at the surface but under all kinds of balloons in the troposphere and in the stratosphere. LOAC is an original OPC performing observations at two scattering angles. The first one is around 12°, and is almost insensitive to the refractive index of the particles; the second one is around 60° and is strongly sensitive to the refractive index of the particles. By combining measurement at the two angles, it is possible to retrieve the size distribution between 0.2 and 100 µm and to estimate the nature of the dominant particles (droplets, carbonaceous, salts and mineral particles) when the aerosol is relatively homogeneous. This typology is based on calibration charts obtained in the laboratory. The uncertainty for total concentrations measurements is ±20 % when concentrations are higher than 1 particle cm−3 (for a 10 min integration time). For lower concentrations, the uncertainty is up to about ±60 % for concentrations smaller than 10−2 particle cm−3. Also, the uncertainties in size calibration are ±0.025 µm for particles smaller than 0.6 µm, 5 % for particles in the 0.7–2 µm range, and 10 % for particles greater than 2 µm. The measurement accuracy of submicronic particles could be reduced in a strongly turbid case when concentration of particles > 3 µm exceeds a few particles cm−3. Several campaigns of cross-comparison of LOAC with other particle counting instruments and remote sensing photometers have been conducted to validate both the size distribution derived by LOAC and the retrieved particle number density. The typology of the aerosols has been validated in well-defined conditions including urban pollution, desert dust episodes, sea spray, fog, and cloud. Comparison with reference aerosol mass monitoring instruments also shows that the LOAC measurements can be successfully converted to mass concentrations.
Published: 2016

36. Role of the boundary layer dynamics effects on an extreme air pollution event in Paris

Author: Olivier Favez, Jordi Badosa, Jean-Charles Dupont, Vincent Crenn, Jean-Eudes Petit, Jean-Louis Bonne, Jean Sciare, Martial Haeffelin, Frédérik Meleux, Thierry Elias, Institut Pierre-Simon-Laplace (IPSL), École normale supérieure - Paris (ENS Paris), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Météorologie Dynamique (UMR 8539) (LMD), Département des Géosciences - 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), Institut National de l'Environnement Industriel et des Risques (INERIS), 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), 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), Cyprus Institute (CyI), Agropole, Capgènes, École normale supérieure - Paris (ENS-PSL), 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, 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), 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), and 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)
Subjects: DYNAMICS, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, Irradiance, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Aerosol, Boundary layer, POLLUTION, 13. Climate action, Diurnal cycle, Wind shear, Turbulence kinetic energy, Radiative transfer, Environmental science, BOUNDARY LAYER DEPTH, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Optical depth, 0105 earth and related environmental sciences, General Environmental Science
Abstract: International audience; The physical and chemical aerosol properties are explored here based on ground-based observations in the Paris region to better understand the role of clouds, radiative fluxes and dynamics on aerosol loading during a heavy regional air pollution that occurred in March 2014 over North-Western Europe. This event is primarily characterized by a fine particle mass (PM2.5) increase from 10 to more than 120 μg m−3 and a simultaneous decrease of the horizontal visibility from 40 to 1 km, mainly due to significant formation of ammonium nitrate particles. The aerosol optical depth (AOD) at 550 nm increased steadily from about 0.06 on March 6 to more than 0.9 five days later. The scattering of the solar radiation by polluted particles induced, at the peak of the heavy pollution event, an instantaneous shortwave flux decrease of about 300 W m−2 for direct irradiance and an increase of about 150 W m−2 for diffuse irradiance (only scattering). The mean surface aerosol effect efficiency (effect per unit optical depth) is of about −80 W m−2 with a mean aerosol direct radiative effect of −23 W m−2. The dynamical and radiative processes that can be responsible for the diurnal cycle of PM2.5 in terms of amplitude and timing are investigated. A comparative analysis is performed for 4 consecutive days (between March 11 and 14), showing that the PM2.5 diurnal cycle can be modulated in time and amplitude by local processes such as the boundary layer depth development (ranging from 100 m to 1350 m), surface relative humidity (100%–35%), thermal structure (10 °C–16 °C for day/night amplitude), dynamics (wind speed ranging from 4 m s−1 to 1.5 m s−1) and turbulence (turbulent kinetic energy reaching 2 m2 s−2) near the surface and wind shear along the vertical. Finally, modeled and measured surface PM2.5 loadings are also compared here, notably illustrating the need of accurate boundary layer depth data for efficient air quality forecasts.
Published: 2016

37. Diagnostic Evaluations of the CHIMERE Model: Local Versus Advected Contributions of Fine Particles and Nitrate Formation Regime in the Paris Megacity

Author: Roland Sarda-Esteve, Hervé Petetin, Jean Sciare, Jean-Eudes Petit, Véronique Ghersi, Olivier Sanchez, M. Bressi, Amandine Rosso, Matthias Beekmann, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité), 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), 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), AIRPARIF - Surveillance de la qualité de l'air en Île-de-France, Douw G. Steyn, Nadine Chaumerliac, 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), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), 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), 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, Pollution, 010504 meteorology & atmospheric sciences, Meteorology, Economies of agglomeration, Advection, Chemistry, media_common.quotation_subject, Ammonium nitrate, Particulates, Atmospheric sciences, 01 natural sciences, Aerosol, chemistry.chemical_compound, Nitrate, 13. Climate action, 11. Sustainability, Sulfate, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, 0105 earth and related environmental sciences, media_common
Abstract: International audience; Chemistry transport models (CTMs) are a powerful tool to investigate various features of the aerosol pollution in megacities, including its geographical origin or its sensitivity to anthropogenic emissions changes (scenario analysis). However, due to the numerous uncertainties still at stake in CTMs, assessing the reliability of the results obtained in these two common exercises remains a challenging task that usually requires specific observations and methodologies. In our work, we have taken advantage of some recent campaigns in the Paris region—PARTICULES and FRANCIPOL—to run a diagnostic evaluation of the CHIMERE model regarding these two issues. The first substantive point is to assess in what extent the model is able to retrieve the correct share between local production and regional advection of aerosol pollution in the Paris agglomeration. During a whole year, daily measurements of the fine particulate matter (PM$_{2.5}$) and its main chemical constituents (elemental and organic carbon, nitrate, sulfate and ammonium) are available at various stations both in and around Paris (PARTICULES project). Based on back-trajectory data, we can locate the upwind station, from which the concentration is identified as the import, the local production being deduced from the urban concentration by subtraction. Uncertainties on these contributions are quantified. Small biases in urban background PM$_{2.5}$ simulations (+16 %) hide significant error compensations between local and advected contributions, as well as in PM$_{2.5}$ chemical compounds. In particular, wintertime OM imports appear strongly underestimated (potentially explained by uncertain continental woodburning emissions and missing SOA pathways) while local OM and EC production are overestimated all along the year (likely to be related to uncertainties in emissions and dynamics). A statistically significant local formation of nitrate is also highlighted from observations, but missed by the model. Together with the overestimation of nitrate imports, it leads to a bias of +51 % on the local PM$_{2.5}$ contribution. In parallel to inorganic aerosols measurements, gaseous nitrate precursors (nitric acid and ammonia) have also been measured (FRANCIPOL project), which offers the opportunity to investigate the regime of nitrate formation in Paris and its sensitivity to precursor changes and to assess, again, the ability of the CHIMERE model to retrieve the observed sensitivity. Experimental data clearly point to NH3-rich conditions in the city (as indicated by high gas ratio values), but a quite similar sensitivity of nitrate concentrations to changes in nitric acid and ammonia. However, simulation results indicate that the model highly overestimates the sensitivity of nitrate to ammonia changes. Thus, while overall particulate matter levels are well reproduced by the model, differences with observations are much larger for local versus advected contributions, and the sensitivity of nitrate formation with respect to gaseous precursors.
Published: 2016

38. A new methodology to assess the performance and uncertainty of source apportionment models II: The results of two European intercomparison exercises

Author: E. Cuccia, Jean-Eudes Petit, Marco Pandolfi, Franco Lucarelli, Xavier Querol, Matthias Karl, D. Mooibroek, Marcelo Pinho Almeida, Eduardo Yubero, Pentti Paatero, Jakob Klenø Nøjgaard, Olivier Favez, Silvia Nava, Daniele Contini, Konstantinos Eleftheriadis, Evangelia Diapouli, Gianluigi Valli, A. Pietrodangelo, Paulo Artaxo, V. Bernardoni, Claudio A. Belis, Maria Chiara Bove, André S. H. Prévôt, Paolo Prati, Federico Karagulian, Philip K. Hopke, Daniela Cesari, Jan Hovorka, I. El Haddad, Petra Pokorná, Fulvio Amato, David C. S. Beddows, Héctor Jorquera, Dikaia Saraga, Athanasios Sfetsos, Maria Grazia Perrone, Roy M. Harrison, Mika Vestenius, Eunhwa Jang, Samara Carbone, Ulrich Quass, Roberta Vecchi, T. Kammermeier, Jean Sciare, Stig Hellebust, JRC Institute for Environment and Sustainability (IES), European Commission - Joint Research Centre [Ispra] (JRC), Institute of Environmental Assessment and Water Research (IDAEA), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Universidade Nova de Lisboa = NOVA University Lisbon (NOVA), Institute for Physics, National Centre for Atmospheric Science, University of Birmingham [Birmingham], Department of Physics, Università degli Studi di Milano = University of Milan (UNIMI), Departement of Experimental Medicine, Section of Human Physiology, Università degli studi di Genova = University of Genoa (UniGe), Istituto di Scienze dell'Atmosfera e del Clima (ISAC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Dipartimento di Fisica, ICT Institute of Politecnico di Milano, Institute of Nuclear Technology & Radiation Protection, National Center for Scientific Research 'Demokritos' (NCSR), 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), Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Tasmanian Institute of Agriculture (TIA), University of Tasmania [Hobart, Australia] (UTAS), Norwegian Institute for Air Research (NILU), Università degli Studi di Napoli 'Parthenope' = University of Naples (PARTHENOPE), INTA - Instituto Nacional de Tecnología Agropecuaria, Università degli Studi di Milano-Bicocca = University of Milano-Bicocca (UNIMIB), Environmental Research Laboratory, National Centre for Scientific Research Demokritos, 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), University of Rochester Medical Center, Universita degli Studi di Milano & National Institute of Nuclear Physics, University of Genoa (UNIGE), Consiglio Nazionale delle Ricerche [Roma] (CNR), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), Universita degli studi di Napoli 'Parthenope' [Napoli], Università degli Studi di Milano-Bicocca [Milano] (UNIMIB), 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), Belis, C, Karagulian, F, Amato, F, Almeida, M, Artaxo, P, Beddows, D, Bernardoni, V, Bove, M, Carbone, S, Cesari, D, Contini, D, Cuccia, E, Diapouli, E, Eleftheriadis, K, Favez, O, El Haddad, I, Harrison, R, Hellebust, S, Hovorka, J, Jang, E, Jorquera, H, Kammermeier, T, Karl, M, Lucarelli, F, Mooibroek, D, Nava, S, Nøjgaard, J, Paatero, P, Pandolfi, M, Perrone, M, Petit, J, Pietrodangelo, A, Pokorná, P, Prati, P, Prevot, A, Quass, U, Querol, X, Saraga, D, Sciare, J, Sfetsos, A, Valli, G, Vecchi, R, Vestenius, M, Yubero, E, and Hopke, P
Subjects: Atmospheric Science, Source apportionment, 010504 meteorology & atmospheric sciences, Meteorology, AIR-QUALITY, Intercomparison exercise, Source apportionment Receptor models Intercomparison exercise Model performance indicators Model uncertainty Particulate matter, 010501 environmental sciences, 114 Physical sciences, 01 natural sciences, complex mixtures, Receptor models, POLLUTION, AEROSOLS, Time windows, Apportionment, Environmental Science(all), Statistics, Air quality management, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Air quality index, 1172 Environmental sciences, 0105 earth and related environmental sciences, General Environmental Science, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, PM SOURCE APPORTIONMENT, Time trends, AREA, respiratory system, Objective quality, Model performance indicator, CHIM/12 - CHIMICA DELL'AMBIENTE E DEI BENI CULTURALI, 13. Climate action, Model uncertainty, Model performance indicators, Environmental science, Receptor model, Standard uncertainty, Particulate matter
Abstract: The performance and the uncertainty of receptor models (RMs) were assessed in intercomparison exercises employing real-world and synthetic input datasets. To that end, the results obtained by different practitioners using ten different RMs were compared with a reference. In order to explain the differences in the performances and uncertainties of the different approaches, the apportioned mass, the number of sources, the chemical profiles, the contribution-to-species and the time trends of the sources were all evaluated using the methodology described in Bells et al. (2015). In this study, 87% of the 344 source contribution estimates (SCEs) reported by participants in 47 different source apportionment model results met the 50% standard uncertainty quality objective established for the performance test. In addition, 68% of the SCE uncertainties reported in the results were coherent with the analytical uncertainties in the input data. The most used models, EPA-PMF v.3, PMF2 and EPA-CMB 8.2, presented quite satisfactory performances in the estimation of SCEs while unconstrained models, that do not account for the uncertainty in the input data (e.g. APCS and FA-MLRA), showed below average performance. Sources with well-defined chemical profiles and seasonal time trends, that make appreciable contributions (>10%), were those better quantified by the models while those with contributions to the PM mass close to 1% represented a challenge. The results of the assessment indicate that RMs are capable of estimating the contribution of the major pollution source categories over a given time window with a level of accuracy that is in line with the needs of air quality management. (C) 2015 The Authors. Published by Elsevier Ltd.
Published: 2015

39. Comparison between simulated and observed chemical composition of fine aerosols in Paris (France) during springtime: contribution of regional versus continental emissions

Author: Roland Sarda-Esteve, Cécile Gaimoz, Valérie Gros, Olivier Sanchez, Matthias Beekmann, Odile d'Argouges, Qijie Zhang, Jean Sciare, 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), 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), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP), AIRPARIF - Surveillance de la qualité de l'air en Île-de-France, Conventions Industrielles de Formation par la REcherche CIFRE ANR 2016/403, The publication of this article is financed by CNRS-INSU, ANR-05-JCJC-0106,AEROCOV,Etude expérimentale des aérosols et des composés organiques volatils dans les mégapoles: Quantification des interactions et des impacts(2005), 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 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), and Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, 010504 meteorology & atmospheric sciences, Secondary organic aerosols, 010501 environmental sciences, complex mixtures, 01 natural sciences, lcsh:QC1-999, Ion, Aerosol, lcsh:Chemistry, chemistry.chemical_compound, Inorganic salts, Above ground, lcsh:QD1-999, chemistry, 13. Climate action, Environmental chemistry, Aerodynamic diameter, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Chemical composition, lcsh:Physics, 0105 earth and related environmental sciences
Abstract: Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. 2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5 > 15 μg m−3 were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM2.5 concentrations (typically of about 10 μg m−3); carbonaceous aerosols contributing for most of this mass (typically 75%). In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM2.5 over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM2.5 and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.
Published: 2010

40. MEGAPOLI: concept of multi-scale modelling of megacity impact on air quality and climate

Author: Urs Baltensperger, L. Gomes, Agnès Borbon, A. Wiedensholer, Markku Kulmala, Spyros N. Pandis, Sergey Zilitinkevich, W. B. Rossow, John A. Pyle, Alexander Mahura, H. D. van der Gon, Tim Butler, Jean-Luc Jaffrezo, Paolo Laj, Bruce Denby, Rainer Friedrich, Stefano Galmarini, Sue Grimmond, Jaakko Kukkonen, B. Collins, Jean Sciare, Peter J. H. Builtjes, Thomas Wagner, Andreas Stohl, D. van den Hout, Valérie Gros, Ranjeet S. Sokhi, H. Schluenzen, F. Giorgi, Isabelle Coll, Tomas Halenka, Alexander Baklanov, Igor Esau, Matthias Beekmann, Sandro Finardi, L. Jalkinen, Nicolas Moussiopoulos, J. Theloke, U. Kummer, and Mark Lawrence
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, Atmospheric pollution, lcsh:QC851-999, 010501 environmental sciences, 7. Clean energy, 01 natural sciences, 11. Sustainability, lcsh:Science, Temporal scales, Air quality index, 0105 earth and related environmental sciences, Scientific instrument, business.industry, Ecological Modeling, Scale (chemistry), European research, Environmental resource management, Pollution, lcsh:QC1-999, Geophysics, Megacity, 13. Climate action, Atmospheric chemistry, Environmental science, lcsh:Q, lcsh:Meteorology. Climatology, business, lcsh:Physics
Abstract: The EU FP7 Project MEGAPOLI: "Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation" (http://megapoli.info) brings together leading European research groups, state-of-the-art scientific tools and key players from non-European countries to investigate the interactions among megacities, air quality and climate. MEGAPOLI bridges the spatial and temporal scales that connect local emissions, air quality and weather with global atmospheric chemistry and climate. The suggested concept of multi-scale integrated modelling of megacity impact on air quality and climate and vice versa is discussed in the paper. It requires considering different spatial and temporal dimensions: time scales from seconds and hours (to understand the interaction mechanisms) up to years and decades (to consider the climate effects); spatial resolutions: with model down- and up-scaling from street- to global-scale; and two-way interactions between meteorological and chemical processes.
Published: 2010

41. Aerosol chemistry above an extended archipelago of the eastern Mediterranean basin during strong northern winds

Author: Maria Tombrou, E Athanasopoulou, George Biskos, A. Dandou, E. Bossioli, J. Kalogiros, James Allan, Nikos Mihalopoulos, Jean Sciare, Asan Bacak, Anna P. Protonotariou, Hugh Coe, Department of Environmental Physics and Meteorology [Zografou campus], Faculty of Physics [Zografou campus], National and Kapodistrian University of Athens (NKUA)-National and Kapodistrian University of Athens (NKUA), Laboratoire de recherche en Hydrodynamique, Énergétique et Environnement Atmosphérique (LHEEA), École Centrale de Nantes (ECN)-Centre National de la Recherche Scientifique (CNRS), University of Manchester [Manchester], School of Earth, Atmospheric and Environmental Sciences [Manchester] (SEAES), Environmental Chemical Processes Laboratory [Heraklion] (ECPL), Department of Chemistry [Heraklion], University of Crete [Heraklion] (UOC)-University of Crete [Heraklion] (UOC), 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), Harvard John A. Paulson School of Engineering and Applied Sciences (SEAS), Harvard University, 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), and Harvard University [Cambridge]
Subjects: Atmospheric Science, Chemical transport model, 010504 meteorology & atmospheric sciences, Structural basin, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Troposphere, lcsh:Chemistry, chemistry.chemical_compound, Sulfate, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, geography, geography.geographical_feature_category, Particulates, lcsh:QC1-999, Aerosol, chemistry, lcsh:QD1-999, 13. Climate action, Weather Research and Forecasting Model, Climatology, Archipelago, lcsh:Physics
Abstract: Detailed aerosol chemical predictions by a comprehensive model system (i.e. PMCAMx, WRF, GEOS-CHEM), along with airborne and ground-based observations, are presented and analysed over a wide domain covering the Aegean Archipelago. The studied period is 10 successive days in 2011, characterized by strong northern winds, which is the most frequently prevailing synoptic pattern during summer. The submicron aerosol load in the lower troposphere above the archipelago is homogenously enriched in sulfate (average modelled and measured submicron sulfate of 5.5 and 5.8 μg m−3, respectively), followed by organics (2.3 and 4.4 μg m−3) and ammonium (1.5 and 1.7 μg m−3). Aerosol concentrations smoothly decline aloft, reaching lower values (< 1 μg m−3) above 4.2 km altitude. The evaluation criteria rate the model results for sulfate, ammonium, chloride, elemental carbon, organic carbon and total PM10 mass concentrations as "good", indicating a satisfactory representation of the aerosol chemistry and precursors. Higher model discrepancies are confined to the highest (e.g. peak sulfate values) and lowest ends (e.g. nitrate) of the airborne aerosol mass size distribution, as well as in airborne organic aerosol concentrations (model underestimation ca. 50 %). The latter is most likely related to the intense fire activity at the eastern Balkan area and the Black Sea coastline, which is not represented in the current model application. The investigation of the effect of local variables on model performance revealed that the best agreement between predictions and observations occurs during high winds from the northeast, as well as for the area confined above the archipelago and up to 2.2 km altitude. The atmospheric ageing of biogenic particles is suggested to be activated in the aerosol chemistry module, when treating organics in a sufficient nitrogen and sulfate-rich environment, such as that over the Aegean basin. More than 70 % of the predicted aerosol mass over the Aegean Archipelago during a representative Etesian episode is related to transport of aerosols and their precursors from outside the modelling domain.
Published: 2015

42. Atmospheric water-soluble organic nitrogen (WSON) over marine environments: a global perspective

Author: Manuela Martino, Jonathan Williams, Nikos Mihalopoulos, Kalliopi Violaki, Alex R. Baker, Jean Sciare, University of Crete [Heraklion] (UOC), 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), Environmental Chemical Processes Laboratory [Heraklion] (ECPL), Department of Chemistry [Heraklion], University of Crete [Heraklion] (UOC)-University of Crete [Heraklion] (UOC), 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: 010504 meteorology & atmospheric sciences, lcsh:Life, chemistry.chemical_element, 010501 environmental sciences, Spatial distribution, 01 natural sciences, Atmosphere, lcsh:QH540-549.5, 14. Life underwater, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Southern Hemisphere, Ecology, Evolution, Behavior and Systematics, 0105 earth and related environmental sciences, Earth-Surface Processes, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric water, lcsh:QE1-996.5, Northern Hemisphere, Nitrogen, lcsh:Geology, Indian ocean, Eastern mediterranean, lcsh:QH501-531, Oceanography, chemistry, 13. Climate action, Environmental chemistry, Environmental science, lcsh:Ecology
Abstract: To obtain a comprehensive picture on the spatial distribution of water soluble organic nitrogen (WSON) in marine aerosols, samples were collected during research cruises in the tropical and south Atlantic Ocean and during a one year period (2005) over the southern Indian Ocean (Amsterdam island). Samples have been analyzed for both organic and inorganic forms of nitrogen and the factors controlling their levels have been examined. Fine mode WSON was found to play a significant role in the remote marine atmosphere with enhanced biogenic activity, with concentrations of WSON (11.3 ± 3.3 nmol N m–3) accounting for about 84% of the total dissolved nitrogen (TDN). Such levels are similar to those observed in the polluted marine atmosphere of the eastern Mediterranean (11.6 ± 14.0 nmol N m–3). Anthropogenic activities were found to be an important source of atmospheric WSON as evidenced by the ten times higher levels in the Northern Hemisphere (NH) than in the remote Southern Hemisphere (SH). Furthermore, the higher contribution of WSON to TDN (40%) in the SH, compared to the NH (20%), underlines the important role of organic nitrogen in remote marine areas. Finally, Sahara dust was also identified as a significant source of WSON in the coarse mode aerosols of the NH.
Published: 2015

43. ECOC comparison exercise with identical thermal protocols after temperature offset correction - Instrument diagnostics by in-depth evaluation of operational parameters

Author: J. Schwarz, Willy Maenhaut, Paola Fermo, Martina Giannoni, A.C. John, T. Hafkenscheid, Regina Hitzenberger, P. Panteliadis, Jean Sciare, Olivier Favez, Paul Quincey, Roberta Vecchi, Jean-Luc Jaffrezo, Evangelia Diapouli, Angeliki Karanasiou, Dikaia Saraga, Andrea Fischer, J. Novak, B. Cary, Mar Viana, National Center for Scientific Research 'Demokritos' (NCSR), Laboratoire de Probabilités et Modèles Aléatoires (LPMA), Université Pierre et Marie Curie - Paris 6 (UPMC)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Institut National de l'Environnement Industriel et des Risques (INERIS), Environmental Measurements Group, National Physical Laboratory [Teddington] (NPL), Institute of Environmental Assessment and Water Research (IDAEA), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), Faculty of Physics [Vienna], Universität Wien, Environmental Research Laboratory, National Centre for Scientific Research Demokritos, 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), Università degli Studi di Milano = University of Milan (UNIMI), Universiteit Gent = Ghent University (UGENT), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Pierre et Marie Curie - Paris 6 (UPMC), 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), Università degli Studi di Milano [Milano] (UNIMI), and Universiteit Gent = Ghent University [Belgium] (UGENT)
Subjects: Atmospheric Science, THERMAL/OPTICAL CARBON ANALYSIS, Offset (computer science), 010504 meteorology & atmospheric sciences, AIR-QUALITY, Analytical chemistry, 010501 environmental sciences, Standard score, 01 natural sciences, LOW-EMISSION ZONE, Standard deviation, IMPLEMENTATION, Calibration, lcsh:TA170-171, ELEMENTAL CARBON, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Protocol (science), Reproducibility, DIESEL EXHAUST, lcsh:TA715-787, [SDE.IE]Environmental Sciences/Environmental Engineering, Chemistry, lcsh:Earthwork. Foundations, AEROSOL, Repeatability, QUANTIFICATION, lcsh:Environmental engineering, Aerosol, Earth and Environmental Sciences, BLACK CARBON, OPTICAL METHOD
Abstract: A comparison exercise on thermal-optical elemental carbon/organic carbon (ECOC) analysers was carried out among 17 European laboratories. Contrary to previous comparison exercises, the 17 participants made use of an identical instrument set-up, after correcting for temperature offsets with the application of a recently developed temperature calibration kit (Sunset Laboratory Inc, OR, US). Temperature offsets reported by participants ranged from −93 to +100 °C per temperature step. Five filter samples and two sucrose solutions were analysed with both the EUSAAR2 and NIOSH870 thermal protocols. z scores were calculated for total carbon (TC); nine outliers and three stragglers were identified. Three outliers and eight stragglers were found for EC. Overall, the participants provided results between the warning levels with the exception of two laboratories that showed poor performance, the causes of which were identified and corrected through the course of the comparison exercise. The TC repeatability and reproducibility (expressed as relative standard deviations) were 11 and 15% for EUSAAR2 and 9.2 and 12% for NIOSH870; the standard deviations for EC were 15 and 20% for EUSAAR2 and 20 and 26% for NIOSH870. TC was in good agreement between the two protocols, TCNIOSH870 = 0.98 × TCEUSAAR2 (R2 = 1.00, robust means). Transmittance (TOT) calculated EC for NIOSH870 was found to be 20% lower than for EUSAAR2, ECNIOSH870 = 0.80 × ECEUSAAR2 (R2 = 0.96, robust means). The thermograms and laser signal values were compared and similar peak patterns were observed per sample and protocol for most participants. Notable deviations from the typical patterns indicated either the absence or inaccurate application of the temperature calibration procedure and/or pre-oxidation during the inert phase of the analysis. Low or zero pyrolytic organic carbon (POC), as reported by a few participants, is suggested as an indicator of an instrument-specific pre-oxidation. A sample-specific pre-oxidation effect was observed for filter G, for all participants and both thermal protocols, indicating the presence of oxygen donors on the suspended particulate matter. POC (TOT) levels were lower for NIOSH870 than for EUSAAR2, which is related to the heating profile differences of the two thermal protocols.
Published: 2015

44. Ozone and aerosol tropospheric concentrations variability analyzed using the ADRIMED measurements and the WRF and CHIMERE models

Author: Laurent Menut, Paola Formenti, Marc Mallet, F. Meleux, Jean Sciare, Bertrand Bessagnet, Sylvain Mailler, R. Briant, G. Rea, Guillaume Siour, S. Turquety, Laboratoire de Météorologie Dynamique (UMR 8539) (LMD), 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), 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), Institut National de l'Environnement Industriel et des Risques (INERIS), 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, Energy, Environment and Water Research Center (EEWRC), Cyprus Institute (CyI), 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), 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 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 Paris)-École normale supérieure - Paris (ENS Paris), 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), 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), 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 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), 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 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 Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), 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: Atmospheric Science, food.ingredient, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Mineral dust, Atmospheric sciences, 01 natural sciences, complex mixtures, Troposphere, lcsh:Chemistry, food, Precipitation, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Sea salt, lcsh:QC1-999, Aerosol, AERONET, Deposition (aerosol physics), lcsh:QD1-999, 13. Climate action, Climatology, Weather Research and Forecasting Model, ChArMEx, Environmental science, lcsh:Physics
Abstract: During the months of June and July 2013, over the Euro–Mediterranean area, the ADRIMED (Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) project was dedicated to characterize the ozone and aerosol concentrations in the troposphere. It is first shown that this period was not highly polluted compared to previous summers in this region, with a moderate ozone production, no significant vegetation fire events and several precipitation periods scavenging the aerosol. The period is modeled with the WRF (Weather Research and Forecasting) and CHIMERE models, and their ability to quantify the observed pollution transport events is presented. The CHIMERE model simulating all kinds of sources (anthropogenic, biogenic, mineral dust, vegetation fires); the aerosol speciation, not available with the measurements, is presented: during the whole period, the aerosol was mainly constituted by mineral dust, sea salt and sulfates close to the surface and mainly by mineral dust in the troposphere. Compared to the AERONET (Aerosol Robotic Network) size distribution, it is shown that the model underestimates the coarse mode near mineral dust sources and overestimates the fine mode in the Mediterranean area, highlighting the need to improve the model representation of the aerosol size distribution both during emissions, long-range transport and deposition.
Published: 2015

45. The 'dual-spot' Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation

Author: Peter Zotter, C. Ruckstuhl, Griša Močnik, A. Wiedensohler, Jean Sciare, Luka Drinovec, André S. H. Prévôt, Maheswar Rupakheti, Thomas Müller, Anthony D. A. Hansen, Esther Coz, 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), Leibniz Institute for Tropospheric Research (TROPOS), 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: Atmospheric Science, 010504 meteorology & atmospheric sciences, Meteorology, Air pollution, 010501 environmental sciences, black carbon, medicine.disease_cause, Combustion, Atmospheric sciences, Aethalometer, 01 natural sciences, Compensation (engineering), law.invention, Atmosphere, law, medicine, lcsh:TA170-171, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Absorption (electromagnetic radiation), 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, algorithm, real time, lcsh:TA715-787, Chemistry, lcsh:Earthwork. Foundations, aerosol composition, anthropogenic effect, Photometer, tracer, air quality, lcsh:Environmental engineering, Aerosol, climate change, 13. Climate action
Abstract: Aerosol black carbon is a unique primary tracer for combustion emissions. It affects the optical properties of the atmosphere and is recognized as the second most important anthropogenic forcing agent for climate change. It is the primary tracer for adverse health effects caused by air pollution. For the accurate determination of mass equivalent black carbon concentrations in the air and for source apportionment of the concentrations, optical measurements by filter-based absorption photometers must take into account the "filter loading effect". We present a new real-time loading effect compensation algorithm based on a two parallel spot measurement of optical absorption. This algorithm has been incorporated into the new Aethalometer model AE33. Intercomparison studies show excellent reproducibility of the AE33 measurements and very good agreement with post-processed data obtained using earlier Aethalometer models and other filter-based absorption photometers. The real-time loading effect compensation algorithm provides the high-quality data necessary for real-time source apportionment and for determination of the temporal variation of the compensation parameter k.
Published: 2015

46. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

Author: Jean Sciare, Astrid Manders, Hannele Korhonen, Jurgita Ovadnevaite, G. de Leeuw, Colin D. O'Dowd, Tommi Bergman, Harri Kokkola, Anton Laakso, Dominique Baisnée, Antti-Ilari Partanen, Larisa Sogacheva, Eimear M. Dunne, Finnish Meteorological Institute (FMI), National University of Ireland [Galway] (NUI Galway), Chimie Atmosphérique Expérimentale (CAE), 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)-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, 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), and Helsingin yliopisto = Helsingfors universitet = University of Helsinki
Subjects: Atmospheric Science, food.ingredient, 010504 meteorology & atmospheric sciences, a-train, Flux, Environment, 010501 environmental sciences, Atmospheric sciences, climate model, data sets, 01 natural sciences, lcsh:Chemistry, food, Urban Development, organic-matter enrichment, Radiative transfer, Cloud condensation nuclei, Built Environment, Sea salt aerosol, 0105 earth and related environmental sciences, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Sea salt, Earth / Environmental, CAS - Climate, Air and Sustainability, Radiative forcing, Sea spray, parameterization, lcsh:QC1-999, Aerosol, cloud condensation nuclei, lcsh:QD1-999, 13. Climate action, Climatology, primary marine aerosol, salt aerosol, mass-spectrometer, Environmental science, mixed-phase clouds, ELSS - Earth, Life and Social Sciences, lcsh:Physics
Abstract: Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol–climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr−1 (uncertainty range 378–1233 Tg yr−1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias −13% for particles with vacuum aerodynamic diameter Dva < 1 μm), Point Reyes (−29% for particles with aerodynamic diameter Da < 2.5 μm) and Amsterdam Island (−52% for particles with Da < 1 μm) but the larger sizes were overestimated (899% for particles with 2.5 μm < Da < 10 μm) at Amsterdam Island. This suggests that at least the high end of the previous estimates of sea spray mass emissions is unrealistic. On the other hand, the model clearly underestimated the observed concentrations of organic or total carbonaceous aerosol at Mace Head (−82%) and Amsterdam Island (−68%). The large overestimation (212%) of organic matter at Point Reyes was due to the contribution of continental sources. At the remote Amsterdam Island site, the organic concentration was underestimated especially in the biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m−2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to suppress both the in-cloud supersaturation and the formation of cloud condensation nuclei from sulfate. These effects can be accounted for only in models with sufficiently detailed aerosol microphysics and physics-based parameterizations of cloud activation. However, due to a strong negative direct effect, the simulated effective radiative forcing (total radiative) effect was −0.2 W m−2. The simulated radiative effects of the primary marine organic emissions were small, with a direct effect of 0.03 W m−2 and an indirect effect of −0.07 W m−2.
Published: 2014

47. DMS atmospheric concentrations and sulphate aerosol indirect radiative forcing: a sensitivity study to the DMS source representation and oxidation

Author: Olivier Boucher, Mark Lawrence, Cyril Moulin, M. S. Reddy, Jean Sciare, Chandra Venkataraman, R. von Kuhlmann, Maï Pham, Laurent Bopp, Emmanuel Cosme, Sauveur Belviso, Olivier Aumont, 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), 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), Laboratoire d'océanographie dynamique et de climatologie (LODYC), Institut de Recherche pour le Développement (IRD)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des Écoulements Géophysiques et Industriels [Grenoble] (LEGI), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS), Max Planck Institute for Chemistry (MPIC), Max-Planck-Gesellschaft, Max-Planck-Institut für Chemie (MPIC), Service d'aéronomie (SA), 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), Centre for Environmental Science and Engineering [Bombay] (CESE), Indian Institute of Technology Bombay (IIT Bombay), Correspondant HAL 2, LEGI, Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut de Recherche pour le Développement (IRD), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble [1985-2015] (OSUG [1985-2015]), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology [2007-2019] (Grenoble INP [2007-2019])-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 [2007-2019] (Grenoble INP [2007-2019])-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), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), ICOS-RAMCES (ICOS-RAMCES), 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), 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), 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)-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), 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), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Lille, 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), and 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)
Subjects: Atmospheric Science, Seasonal-Variation, 010504 meteorology & atmospheric sciences, [PHYS.PHYS.PHYS-GEO-PH]Physics [physics]/Physics [physics]/Geophysics [physics.geo-ph], [SPI.MECA.MEFL] Engineering Sciences [physics]/Mechanics [physics.med-ph]/Fluids mechanics [physics.class-ph], 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, [SPI.MECA.MEFL]Engineering Sciences [physics]/Mechanics [physics.med-ph]/Fluids mechanics [physics.class-ph], Atmosphere, lcsh:Chemistry, chemistry.chemical_compound, [PHYS.MECA.MEFL] Physics [physics]/Mechanics [physics]/Fluid mechanics [physics.class-ph], 14. Life underwater, [PHYS.MECA.MEFL]Physics [physics]/Mechanics [physics]/Fluid mechanics [physics.class-ph], Sulfate, 0105 earth and related environmental sciences, Dimethyl Sulfide, Climate Model, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Sulfur cycle, Radiative forcing, Sulfur Cycle, Global Distributions, lcsh:QC1-999, Aerosol, Bromine Oxide, chemistry, lcsh:QD1-999, 13. Climate action, Cloud albedo, Environmental science, Dimethyl sulfide, Climate model, Amsterdam-Island, lcsh:Physics, Southern Indian-Ocean, Cloud Albedo
Abstract: PAR00002853; International audience; The global sulphur cycle has been simulated using a general circulation model with a focus on the source and oxidation of atmospheric dimethylsulphide (DMS). The sensitivity of atmospheric DMS to the oceanic DMS climatology, the parameterisation of the sea-air transfer and to the oxidant fields have been studied. The importance of additional oxidation pathways (by O3 in the gas- and aqueous-phases and by BrO in the gas phase) not incorporated in global models has also been evaluated. While three different climatologies of the oceanic DMS concentration produce rather similar global DMS fluxes to the atmosphere at 24-27 Tg S yr -1, there are large differences in the spatial and seasonal distribution. The relative contributions of OH and NO3 radicals to DMS oxidation depends critically on which oxidant fields are prescribed in the model. Oxidation by O3 appears to be significant at high latitudes in both hemispheres. Oxidation by BrO could be significant even for BrO concentrations at sub-pptv levels in the marine boundary layer. The impact of such refinements on the DMS chemistry onto the indirect radiative forcing by anthropogenic sulphate aerosols is also discussed.
Published: 2003

48. Interannual variability of methanesulfonate in rainwater at Amsterdam Island (Southern Indian Ocean)

Author: Nikos Mihalopoulos, Jean Sciare, E. Baboukas, Department of Chemistry [Heraklion], University of Crete [Heraklion] (UOC), 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), 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, Atmospheric Science, Biogeochemical cycle, 010504 meteorology & atmospheric sciences, Sulfur cycle, 010501 environmental sciences, Seasonality, medicine.disease, 01 natural sciences, Methanesulfonic acid, Rainwater harvesting, chemistry.chemical_compound, Oceanography, chemistry, 13. Climate action, Atmospheric chemistry, medicine, Environmental science, Dimethyl sulfide, 14. Life underwater, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Chemical composition, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences, General Environmental Science
Abstract: Methanesulfonate (MS − ), an exclusive oxidation product of dimethylsulfide (DMS), has been analyzed in rainwater at Amsterdam Island (37°50′S 77°32′E) in the Southern Indian Ocean from 1991 to 1999. Rainwater MS − concentrations range from 0.004 to 4.59 μmol l −1 with a volume weighted mean value of 0.24 μmol l −1 and present a well distinguished seasonal variation with higher values in summer, in line with the seasonal variation of its gaseous precursor (DMS), which was measured on a daily basis since 1990. The interannual variability of MS − in rainwater follows closely that of DMS, indicating that MS − in rainwater can be used as a surrogate to study long-term variations of atmospheric DMS, and further confirms the findings of Sciare et al. (J. Geophys. Res. 105 (2000a) 26 369), that large-scale anomalies occurred in the biogenic sulfur cycle in the Southern Indian Ocean during the studied period. Furthermore, on a monthly basis, the MS − anomalies in the rainwater were found to be closely related to sea-surface temperature (SST) anomalies. The correlation between MS − and SST is consistent with that observed between gaseous DMS and SST in the area and indicates an important coupling between the oceanic and the atmospheric compartments of the biogeochemical sulfur cycle.
Published: 2002

49. Two years of near real-time chemical composition of submicron aerosols in the region of Paris using an Aerosol Chemical Speciation Monitor (ACSm) and a multi-wavelength Aethalometer

Author: Roland Sarda-Esteve, Martial Haeffelin, Olivier Favez, Eva Leoz-Garziandia, Jean Sciare, Nicolas Bonnaire, Vincent Crenn, Jean-Charles Dupont, Jean-Eudes Petit, Griša Močnik, Institut National de l'Environnement Industriel et des Risques (INERIS), 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), 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), Aerosol D.O.O, Laboratoire de Météorologie Dynamique (UMR 8539) (LMD), 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), 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 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 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), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)
Subjects: Pollution, Atmospheric Science, Ammonium sulfate, 010504 meteorology & atmospheric sciences, media_common.quotation_subject, Real-time computing, 010501 environmental sciences, Aethalometer, Combustion, 01 natural sciences, lcsh:QC1-999, Aerosol, lcsh:Chemistry, chemistry.chemical_compound, chemistry, Nitrate, lcsh:QD1-999, 13. Climate action, [SDE]Environmental Sciences, Environmental science, Sulfate, Chemical composition, lcsh:Physics, media_common, 0105 earth and related environmental sciences
Abstract: Aerosol mass spectrometer (AMS) measurements have been successfully used towards a better understanding of non-refractory submicron (PM1) aerosol chemical properties based on short-term campaigns. The recently developed Aerosol Chemical Speciation Monitor (ACSM) has been designed to deliver quite similar artifact-free chemical information but for low cost, and to perform robust monitoring over long-term periods. When deployed in parallel with real-time black carbon (BC) measurements, the combined data set allows for a quasi-comprehensive description of the whole PM1 fraction in near real time. Here we present 2-year long ACSM and BC data sets, between mid-2011 and mid-2013, obtained at the French atmospheric SIRTA supersite that is representative of background PM levels of the region of Paris. This large data set shows intense and time-limited (a few hours) pollution events observed during wintertime in the region of Paris, pointing to local carbonaceous emissions (mainly combustion sources). A non-parametric wind regression analysis was performed on this 2-year data set for the major PM1 constituents (organic matter, nitrate, sulfate and source apportioned BC) and ammonia in order to better refine their geographical origins and assess local/regional/advected contributions whose information is mandatory for efficient mitigation strategies. While ammonium sulfate typically shows a clear advected pattern, ammonium nitrate partially displays a similar feature, but, less expectedly, it also exhibits a significant contribution of regional and local emissions. The contribution of regional background organic aerosols (OA) is significant in spring and summer, while a more pronounced local origin is evidenced during wintertime, whose pattern is also observed for BC originating from domestic wood burning. Using time-resolved ACSM and BC information, seasonally differentiated weekly diurnal profiles of these constituents were investigated and helped to identify the main parameters controlling their temporal variations (sources, meteorological parameters). Finally, a careful investigation of all the major pollution episodes observed over the region of Paris between 2011 and 2013 was performed and classified in terms of chemical composition and the BC-to-sulfate ratio used here as a proxy of the local/regional/advected contribution of PM. In conclusion, these first 2-year quality-controlled measurements of ACSM clearly demonstrate their great potential to monitor on a long-term basis aerosol sources and their geographical origin and provide strategic information in near real time during pollution episodes. They also support the capacity of the ACSM to be proposed as a robust and credible alternative to filter-based sampling techniques for long-term monitoring strategies.
Published: 2014

50. Clues for a standardised thermal-optical protocol for the assessment of organic and elemental carbon within ambient air particulate matter

Author: Jean-Luc Jaffrezo, Robin Aujay, Corinne Galy-Lacaux, Laurent Y. Alleman, Olivier Favez, Laura Chiappini, Catherine Liousse, S Verlhac, Willy Maenhaut, E Leoz, Jean Sciare, P. Panteliadis, J. P. Putaud, Institut National de l'Environnement Industriel et des Risques (INERIS), CERCHAR, JRC Institute for Environment and Sustainability (IES), European Commission - Joint Research Centre [Ispra] (JRC), 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), 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 d'aérologie (LA), 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 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 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 Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Université Toulouse III - Paul Sabatier (UT3), 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), Service de Radiologie [Créteil], CHI Créteil, Department of Analytical Chemistry, Institute for Nuclear Sciences, 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), Laboratoire d'aérologie (LAERO), 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), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), 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), 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: Atmospheric Science, EUROPE, 010504 meteorology & atmospheric sciences, Meteorology, Optical correction, 010501 environmental sciences, ACE-ASIA, 01 natural sciences, AEROSOLS, Statistics, lcsh:TA170-171, TEMPERATURE, 0105 earth and related environmental sciences, Protocol (science), Chemistry, lcsh:TA715-787, Comparability, lcsh:Earthwork. Foundations, Particulates, [SDE.ES]Environmental Sciences/Environmental and Society, Aerosol, Ambient air, lcsh:Environmental engineering, REFLECTANCE, Data quality, BIOMASS COMBUSTION, BLACK CARBON, TRANSMITTANCE, [SDE]Environmental Sciences, Elemental carbon
Abstract: Along with some research networking programmes, the European Directive 2008/50/CE requires chemical speciation of fine aerosol (PM2.5), including elemental (EC) and organic carbon (OC), at a few rural sites in European countries. Meanwhile, the thermal-optical technique is considered by the European and US networking agencies and normalisation bodies as a reference method to quantify EC–OC collected on filters. Although commonly used for many years, this technique still suffers from a lack of information on the comparability of the different analytical protocols (temperature protocols, type of optical correction) currently applied in the laboratories. To better evaluate the EC–OC data set quality and related uncertainties, the French National Reference Laboratory for Ambient Air Quality Monitoring (LCSQA) organised an EC–OC comparison exercise for French laboratories using different thermal-optical methods (five laboratories only). While there is good agreement on total carbon (TC) measurements among all participants, some differences can be observed on the EC / TC ratio, even among laboratories using the same thermal protocol. These results led to further tests on the influence of the optical correction: results obtained from different European laboratories confirmed that there were higher differences between OCTOT and OCTOR measured with NIOSH 5040 in comparison to EUSAAR-2. Also, striking differences between ECTOT / ECTOR ratios can be observed when comparing results obtained for rural and urban samples, with ECTOT being 50% lower than ECTOR at rural sites whereas it is only 20% lower at urban sites. The PM chemical composition could explain these differences but the way it influences the EC–OC measurement is not clear and needs further investigation. Meanwhile, some additional tests seem to indicate an influence of oven soiling on the EC–OC measurement data quality. This highlights the necessity to follow the laser signal decrease with time and its impact on measurements. Nevertheless, this should be confirmed by further experiments, involving more samples and various instruments, to enable statistical processing. All these results provide insights to determine the quality of EC–OC analytical methods and may contribute to the work toward establishing method standardisation.
Published: 2014

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