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8 results on '"atmospheric sulfuric-acid"'

1. Comprehensive modelling study on observed new particle formation at the SORPES station in Nanjing, China

Author

X. Huang, L. Zhou, A. Ding, X. Qi, W. Nie, M. Wang, X. Chi, T. Petäjä, V.-M. Kerminen, P. Roldin, A. Rusanen, M. Kulmala, M. Boy, Department of Physics, and Aerosol-Cloud-Climate -Interactions (ACCI)

Subjects
Delta, BOREAL FOREST SITE, Atmospheric Science, 010504 meteorology & atmospheric sciences, Chemical transport model, Population, 010501 environmental sciences, GAS-PHASE, 114 Physical sciences, 01 natural sciences, lcsh:Chemistry, Troposphere, SECONDARY ORGANIC AEROSOL, Cloud condensation nuclei, EASTERN CHINA, education, NUMBER SIZE DISTRIBUTION, LOWER TROPOSPHERE, 0105 earth and related environmental sciences, education.field_of_study, BOUNDARY-LAYER, ATMOSPHERIC SULFURIC-ACID, lcsh:QC1-999, Aerosol, POLLUTION-CONTROL, lcsh:QD1-999, YANGTZE-RIVER DELTA, 13. Climate action, Climatology, Weather Research and Forecasting Model, Particle, lcsh:Physics
Abstract

New particle formation (NPF) has been investigated intensively during the last 2 decades because of its influence on aerosol population and the possible contribution to cloud condensation nuclei. However, intensive measurements and modelling activities on this topic in urban metropolitan areas in China with frequent high-pollution episodes are still very limited. This study provides results from a comprehensive modelling study on the occurrence of NPF events in the western part of the Yangtze River Delta (YRD) region, China. The comprehensive modelling system, which combines the WRF-Chem (the Weather Research and Forecasting model coupled with Chemistry) regional chemical transport model and the MALTE-BOX sectional box model (the model to predict new aerosol formation in the lower troposphere), was shown to be capable of simulating atmospheric nucleation and subsequent growth. Here we present a detailed discussion of three typical NPF days, during which the measured air masses were notably influenced by either anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. Overall, simulated NPF events were generally in good agreement with the corresponding measurements, enabling us to get further insights into NPF processes in the YRD region. Based on the simulations, we conclude that biogenic organic compounds, particularly monoterpenes, play an essential role in the initial condensational growth of newly formed clusters through their low-volatility oxidation products. Although some uncertainties remain in this modelling system, this method provides a possibility to better understand particle formation and growth processes.

Published
2016
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2. Measurement–model comparison of stabilized Criegee intermediate and highly oxygenated molecule production in the CLOUD chamber

Author

N. Sarnela, T. Jokinen, J. Duplissy, C. Yan, T. Nieminen, M. Ehn, S. Schobesberger, M. Heinritzi, S. Ehrhart, K. Lehtipalo, J. Tröstl, M. Simon, A. Kürten, M. Leiminger, M. J. Lawler, M. P. Rissanen, F. Bianchi, A. P. Praplan, J. Hakala, A. Amorim, M. Gonin, A. Hansel, J. Kirkby, J. Dommen, J. Curtius, J. N. Smith, T. Petäjä, D. R. Worsnop, M. Kulmala, N. M. Donahue, M. Sipilä, INAR Physics, Institute for Atmospheric and Earth System Research (INAR), and Polar and arctic atmospheric research (PANDA)

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, Hydrogen, Radical, IONIZATION MASS-SPECTROMETRY, Inorganic chemistry, Nucleation, chemistry.chemical_element, VOLATILE ORGANIC-COMPOUNDS, 010402 general chemistry, 01 natural sciences, 114 Physical sciences, 7. Clean energy, lcsh:Chemistry, chemistry.chemical_compound, Criegee intermediate, CHEMICAL-IONIZATION, GAS-PHASE OZONOLYSIS, PARTICLE FORMATION, Cloud condensation nuclei, Nuclear Physics - Experiment, 0105 earth and related environmental sciences, Chemical ionization, Ozonolysis, GROWTH-RATES, Sulfuric acid, ATMOSPHERIC SULFURIC-ACID, OXIDATION-PRODUCTS, lcsh:QC1-999, 0104 chemical sciences, chemistry, lcsh:QD1-999, WATER-VAPOR, 13. Climate action, AEROSOL FORMATION, lcsh:Physics
Abstract

Atmospheric oxidation is an important phenomenon which produces large quantities of low-volatility compounds such as sulfuric acid and oxidized organic compounds. Such species may be involved in the nucleation of particles and enhance their subsequent growth to reach the size of cloud condensation nuclei (CCN). In this study, we investigate α-pinene, the most abundant monoterpene globally, and its oxidation products formed through ozonolysis in the Cosmic Leaving OUtdoor Droplets (CLOUD) chamber at CERN (the European Organization for Nuclear Research). By scavenging hydroxyl radicals (OH) with hydrogen (H2), we were able to investigate the formation of highly oxygenated molecules (HOMs) purely driven by ozonolysis and study the oxidation of sulfur dioxide (SO2) driven by stabilized Criegee intermediates (sCIs). We measured the concentrations of HOM and sulfuric acid with a chemical ionization atmospheric-pressure interface time-of-flight (CI-APi-TOF) mass spectrometer and compared the measured concentrations with simulated concentrations calculated with a kinetic model. We found molar yields in the range of 3.5–6.5 % for HOM formation and 22–32 % for the formation of stabilized Criegee intermediates by fitting our model to the measured sulfuric acid concentrations. The simulated time evolution of the ozonolysis products was in good agreement with measured concentrations except that in some of the experiments sulfuric acid formation was faster than simulated. In those experiments the simulated and measured concentrations met when the concentration reached a plateau but the plateau was reached 20–50 min later in the simulations. The results shown here are consistent with the recently published yields for HOM formation from different laboratory experiments. Together with the sCI yields, these results help us to understand atmospheric oxidation processes better and make the reaction parameters more comprehensive for broader use.

Published
2018
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3. Simulating ultrafine particle formation in Europe using a regional CTM: Contribution of primary emissions versus secondary formation to aerosol number concentrations

Author

Marcel M. Moerman, Ilona Riipinen, Colin D. O'Dowd, H.A.C. Denier van der Gon, Alfred Wiedensohler, J. P. Putaud, P. E. Charalampidis, Christodoulos Pilinis, Christos Fountoukis, and Spyros N. Pandis

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, Particle number, three-dimensional modeling, Nucleation, Balkans, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, ammonia, air-quality, lcsh:Chemistry, Urban Development, emission control, ion-induced nucleation, Ultrafine particle, size distribution, Mass concentration (chemistry), sulfur dioxide, Built Environment, chemical-transport model, concentration (composition), Emission Environment, size distributions, particle size, lcsh:QC1-999, cloud condensation nuclei, Climatology, EELS - Earth, Environmental and Life Sciences, transport process, Chemical transport model, nucleation, Earth & Environment, aerosol formation, wild-land fires, Scanning mobility particle sizer, global scales, 0105 earth and related environmental sciences, Portugal, quality interactions eucaari, CAS - Climate, Air and Sustainability, Aerosol, lcsh:QD1-999, 13. Climate action, Spain, Environmental science, atmospheric sulfuric-acid, Particle size, off-line model, lcsh:Physics
Abstract

A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.

Published
2012

4. Primary versus secondary contributions to particle number concentrations in the European boundary layer

Author

Karine Sellegri, Nadezda Zikova, Kenneth S. Carslaw, Ernest Weingartner, Angela Marinoni, Thomas Hamburger, Thomas Tuch, Paolo Bonasoni, Joonas Merikanto, Urs Baltensperger, A. Sonntag, Marcel M. Moerman, M. G. Frontoso, Colin D. O'Dowd, Vladimír Ždímal, Pasi Aalto, Pontus Roldin, J. Boulon, L. Collins, Carly Reddington, Birgit Wehner, Hugh Coe, Wolfram Birmili, J. P. Putaud, Andreas Minikin, R. Duchi, Christian Plass-Dülmer, Hans-Christen Hansson, Régis Dupuy, Carsten Gruening, Paolo Laj, Markku Kulmala, Peter Tunved, J. S. Henzing, Dominick V. Spracklen, Alfred Wiedensohler, Nikos Mihalopoulos, Erik Swietlicki, S. G. Jennings, Giorgos Kouvarakis, Harald Flentje, Institute for Climate and Atmospheric Science [Leeds] (ICAS), School of Earth and Environment [Leeds] (SEE), University of Leeds-University of Leeds, C2SM, Department of Physics [Helsinki], Falculty of Science [Helsinki], Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki, DLR Institut für Physik der Atmosphäre (IPA), Deutsches Zentrum für Luft- und Raumfahrt [Oberpfaffenhofen-Wessling] (DLR), School of Earth, Atmospheric and Environmental Sciences [Manchester] (SEAES), University of Manchester [Manchester], Deutscher Wetterdienst [Offenbach] (DWD), Leibniz Institute for Tropospheric Research (TROPOS), Centre for Climate and Air Pollution Studies [Galway] (C-CAPS), National University of Ireland [Galway] (NUI Galway), School of Physics [NUI Galway], Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Institute for Applied Environmental Research [Stockholm], Stockholm University, Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), JRC Institute for Environment and Sustainability (IES), European Commission - Joint Research Centre [Ispra] (JRC), Division of Nuclear Physics, Lund University [Lund], Netherlands Organization for Applied Scientific Research (TNO), TNO Science and Industry, Environmental Chemical Processes Laboratory [Heraklion] (ECPL), Department of Chemistry [Heraklion], University of Crete [Heraklion] (UOC)-University of Crete [Heraklion] (UOC), Institute of Chemical Process Fundamentals of the AS CR, CNR Institute of Atmospheric Sciences and Climate (ISAC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), NERC ADIENT, University of Helsinki-University of Helsinki, Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Consiglio Nazionale delle Ricerche (CNR), 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), 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
Atmospheric Science, Particle number, 010504 meteorology & atmospheric sciences, aerosol particles, Aerosol radiative forcing, Earth & Environment, Nucleation, [SDU.STU]Sciences of the Universe [physics]/Earth Sciences, boundary layer, Environment, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, resolved aerosol microphysics, lcsh:Chemistry, Primary (astronomy), ion-induced nucleation, instrumental development, Cloud condensation nuclei, 0105 earth and related environmental sciences, particulate matter, size distributions, Atmosphärische Spurenstoffe, Particulates, lcsh:QC1-999, Aerosol, on-road, Europe, Boundary layer, carbonaceous aerosol, lcsh:QD1-999, 13. Climate action, UES - Urban Environment & Safety, Environmental science, emission factors, atmospheric sulfuric-acid, off-line model, EELS - Earth, Environmental and Life Sciences, lcsh:Physics
Abstract

It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models., JRC.H.2-Air and Climate

Published
2011
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5. General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI)-integrating aerosol research from nano to global scales

Author

Urmas Hõrrak, Olivier Boucher, J. L. Brenguier, Hanna Lappalainen, Merete Bilde, Antoon Visschedijk, Jón Egill Kristjánsson, Sander Mirme, Zbigniew Klimont, Maria Kanakidou, Michael Schulz, Risto Makkonen, Astrid Kiendler-Scharr, Casimiro Pio, Marc Fischer, J. P. Veefkind, Andreas Stohl, Øyvind Seland, Simon Woodward, Christian George, Daniel Rosenfeld, Thomas Hamburger, T. S. Panwar, Célia Alves, Øystein Hov, Andreas Petzold, Barbara D'Anna, Ari Asmi, Miroslav Josipovic, Birgit Wehner, Maria Cristina Facchini, Gyula Kiss, Heikki Lihavainen, David C. S. Beddows, G. de Leeuw, Elisabetta Vignati, Johan P. Beukes, Min Hu, V. A. Lanz, Karine Sellegri, Holger Siebert, Kari E. J. Lehtinen, A. A. Zardini, Paul R. Halloran, R. Vuolo, Erik Swietlicki, André S. H. Prévôt, Jacobus J. Pienaar, Eiko Nemitz, Hugh Coe, Pekka Kolmonen, Manabu Shiraiwa, Andreas Minikin, Petri Vaattovaara, Thomas F. Mentel, J. Y. Sun, Ulrike Lohmann, Gordon McFiggans, J. Wildt, Ari Laaksonen, David Topping, Christodoulos Pilinis, David Simpson, Joshua P. Schwarz, Stefano Decesari, Urs Baltensperger, Sylwester Arabas, Colin D. O'Dowd, Markus Amann, Alf Kirkevåg, Markus Ammann, Markku Kulmala, Spyros N. Pandis, Antti-Pekka Hyvärinen, G. Roberts, Paulo Artaxo, Joonas Merikanto, Radovan Krejci, Hartmut Herrmann, D. O'Donnell, Ville Vakkari, G.-J. van Zadelhoff, R. Boers, Peter Tunved, Kai Zhang, Gavin R. McMeeking, Alfred Wiedensohler, H. A. C. Denier van der Gon, Yoshiteru Iinuma, Simon L. Clegg, Veli-Matti Kerminen, Kenneth S. Carslaw, Hanna E. Manninen, Hanna Pawlowska, B. Sierau, C. Plass-Duelmer, Johann Feichter, Ilona Riipinen, D. R. Worsnop, Suzanne Crumeyrolle, P. G. van Zyl, Carly Reddington, Roy M. Harrison, Laurent C.-Labonnote, Lauri Laakso, Holger Baars, John F. Burkhart, Henri Vuollekoski, Luciana V. Rizzo, Stefania Gilardoni, Thorsten Hoffmann, Corinna Hoose, Trond Iversen, L. Gomes, Hans-Christen Hansson, Robert Bergström, A. M. Fjaeraa, Francesco Canonaco, Ulrich Pöschl, Mika Komppula, Sara C. Pryor, X. J. Shen, William T. Morgan, Christos Fountoukis, Paolo Laj, INGENIERIE (INGENIERIE), 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)-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 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), RAFFINAGE (RAFFINAGE), AIR (AIR), AIR:EAU+JMH, Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), 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)

Subjects
Atmospheric Science, European aerosol, 010504 meteorology & atmospheric sciences, aerosol, Aerosol radiative forcing, Climate, clouds, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, lcsh:Chemistry, Aerosol cloud, 11. Sustainability, SDG 13 - Climate Action, ddc:550, particle properties, Environmental policy, saturation vapor-pressures, chemical-transport model, Miljövetenskap, air quality, lcsh:QC1-999, General Circulation Model, EUCAARI, EELS - Earth, Environmental and Life Sciences, ION-INDUCED NUCLEATION, Chemical transport model, Meteorology, Earth & Environment, Energy / Geological Survey Netherlands, SIMULATION CHAMBER SAPHIR, nuclei number concentration, SECONDARY ORGANIC AEROSOL, pure component properties, Air quality index, Environmental quality, 0105 earth and related environmental sciences, PARTICLE FORMATION EVENTS, Atmosphärische Spurenstoffe, [CHIM.CATA]Chemical Sciences/Catalysis, CAS - Climate, Air and Sustainability, [SDE.ES]Environmental Sciences/Environmental and Society, Falcon, Aerosol, lcsh:QD1-999, 13. Climate action, mixed-phase clouds, Environmental science, atmospheric sulfuric-acid, Environmental Sciences, lcsh:Physics
Abstract

In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies. Main part of the work in this paper has been funded with FP6 project EUCAARI (Contract 34684). This work was performed in the framework of the Research Infrastructure Action under the FP6 “Structuring the European Research Area” Programme, EUSAAR Contract No. RII3-CT-2006-026140. The financial support by the Academy of Finland Centre of Excellence program (project No. 1118615) is gratefully acknowledged. CNRS and Métófrance partners acknowledge the financial support of Agence Nationale de la Recherche under the AEROCLOUDS proposal. This research has received funding from ERC Advanced Grant ATMNUCLE No. 227463. published

Published
2011
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6. Nanoparticles in boreal forest and coastal environment: a comparison of observations and implications of the nucleation mechanism

Author

Marko Vana, Markku Kulmala, Darius Ceburnis, Tuukka Petäjä, Colin D. O'Dowd, Mikko Sipilä, Katrianne Lehtipalo, and Régis Dupuy

Subjects
Limiting factor, Atmospheric Science, Meteorology, 010504 meteorology & atmospheric sciences, Nucleation, Nanoparticle, aerosol formation, 010501 environmental sciences, growth-rates, 01 natural sciences, Atmosphere, lcsh:Chemistry, size distribution, Cloud condensation nuclei, particle formation events, smear-ii, 0105 earth and related environmental sciences, mediated nucleation, Chemistry, Taiga, tropospheric aerosols, lcsh:QC1-999, air ion spectrometer, lcsh:QD1-999, Chemical physics, 13. Climate action, mode particles, Particle, Particle size, atmospheric sulfuric-acid, lcsh:Physics
Abstract

The detailed mechanism of secondary new particle formation in the atmosphere is still under debate. It is proposed that particle formation happens via activation of 1–2 nm atmospheric neutral molecular clusters and/or large molecules. Since traditional instrumentation does not reach these sizes, the hypothesis has not yet been verified. By directly measuring particle size distributions down to mobility diameters of about 1.3 nm with a pulse-height CPC, we provide evidence of the nucleation mechanism in a coastal environment (Mace Head, Ireland) and in a boreal forest (Hyytiälä, Finland). In both places neutral sub-3 nm condensation nuclei (nano-CN) were continuously present, even when no new particle formation was detected. In Mace Head, however, the concentration of the nano-CN was far too low to account for the particle formation rates during particle bursts. Thus the results imply that at coastal sites new particle formation initiates, as previously proposed, via homogenous nucleation from biogenic iodine vapors. In contrast, activation of pre-existing nano-CN remains a possible explanation in the boreal forest, but the observed concentrations are not the limiting factor for the particle formation events.

Published
2010

7. Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

Author

Dominick V. Spracklen, Nikos Mihalopoulos, Robert W. Talbot, S. G. Jennings, Niku Kivekäs, Graham Mann, J. Sun, Robert A. Weller, Radovan Krejci, Colin D. O'Dowd, Wolfram Birmili, Boris Bonn, Ari Laaksonen, John A. Ogren, Heikki Lihavainen, S. J. Pickering, Andreas Minikin, John L. Gras, Karine Sellegri, Urs Baltensperger, Elisabeth Andrews, Ernest Weingartner, A. Wiedensohler, Kenneth S. Carslaw, Carly Reddington, Roy M. Harrison, Lauri Laakso, Mika Komppula, Paolo Laj, Michael Boy, Markku Kulmala, A. Hamed, Giorgos Kouvarakis, Joonas Merikanto, Institute for Atmospheric Science [Leeds], School of Earth and Environment [Leeds] (SEE), University of Leeds-University of Leeds, ESRL Global Monitoring Laboratory [Boulder] (GML), NOAA Earth System Research Laboratory (ESRL), National Oceanic and Atmospheric Administration (NOAA)-National Oceanic and Atmospheric Administration (NOAA), Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Univ. of Helsinki, Dept. of Physics, Finnish Meteorological Institute (FMI), Kuopio Unit [FMI], Environmental Chemistry Laboratory [Crete], University of Crete [Heraklion] (UOC), Department of Experimental Physics, Leibniz Institute for Tropospheric Research (TROPOS), Leibniz-Institut für Troposphärenforschung (TROPOS), Department of Bentho-pelagic processes, Alfred-Wegener-Institut, Helmholtz-Zentrum für Polar- und Meeresforschung (AWI), CSIRO Marine and Atmospheric Research, Commonwealth Scientific and Industrial Research Organisation [Canberra] (CSIRO), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), 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), Laboratoire de Météorologie Physique (LaMP), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institute for Atmospheric and Environmental Sciences [Frankfurt/Main] (IAU), Goethe-University Frankfurt am Main, Department of Meteorology, Stockholm University, Department of Physics, University of Kuopio, DLR Institut für Physik der Atmosphäre (IPA), Deutsches Zentrum für Luft- und Raumfahrt [Oberpfaffenhofen-Wessling] (DLR), School of Geography, Earth and Environmental Sciences [Birmingham], University of Birmingham [Birmingham], Climate Change Research Center [Durham], University of New Hampshire (UNH), Centre for Atmosphere Watch and Services [Beijing] (CAWAS), Chinese Academy of Meteorological Sciences (CAMS), NERC Advanced Fellowship NERC APPRAISE NERC AEROFORM NE/D01395X/1 EUCAARI, ESRL Global Monitoring Division [Boulder] (GMD), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), 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), National Centre for Atmospheric Science, School of Geography, Climate Change Research Center, 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), and Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS)

Subjects
Atmospheric Science, nucleation mode particles, 010504 meteorology & atmospheric sciences, Particle number, aerosol, Analytical chemistry, Nucleation, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Troposphere, lcsh:Chemistry, size-resolved aerosol, free troposphere, ddc:550, Cloud condensation nuclei, boreal forest, [SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology, 0105 earth and related environmental sciences, Microphysics, Chemistry, particle formation, remote troposphere, Atmosphärische Spurenstoffe, boundary-layer, lcsh:QC1-999, Aerosol, Boundary layer, CN, cloud condensation nuclei, coastal environment, troposphere, lcsh:QD1-999, 13. Climate action, Particle, atmospheric sulfuric-acid, off-line model, lcsh:Physics
Abstract

We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.

Published
2010
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8. Iodine dioxide nucleation simulations in coastal and remote marine environments

Author

Mikael Ehn, Hannele Korhonen, Tatu Anttila, V.-M. Kerminen, Marko Vana, Markku Kulmala, Gordon McFiggans, Henri Vuollekoski, Colin D. O'Dowd, and S.-L. Sihto

Subjects
Atmospheric Science, homogeneous nucleation, Materials science, 010504 meteorology & atmospheric sciences, Nucleation, Soil Science, Mineralogy, aerosol formation, 010501 environmental sciences, Aquatic Science, Oceanography, Kinetic energy, 01 natural sciences, Geochemistry and Petrology, size distribution, Earth and Planetary Sciences (miscellaneous), Cloud condensation nuclei, molecular-iodine, Scavenging, 0105 earth and related environmental sciences, Earth-Surface Processes, Water Science and Technology, Ecology, particle formation, organic contribution, Photodissociation, Condensation, Paleontology, tropospheric aerosols, Forestry, boundary-layer, Aerosol, cloud condensation nuclei, Geophysics, 13. Climate action, Space and Planetary Science, Chemical physics, Particle, atmospheric sulfuric-acid
Abstract

Aerosol dynamical box model simulations of coastal new particle formation were performed in order to investigate the nucleation and growth mechanisms in this environment. In the simulations the nucleating vapor was assumed to be iodine dioxide (OIO). Both Eulerian and Lagrangian type simulations were made and compared with observations. We tested three nucleation mechanisms: kinetic nucleation of OIO (K x [OIO](2)), activation of clusters by OIO (A x [OIO]) and sulphuric acid-induced activation of clusters containing OIO (B x [OIO] x [H2SO4]). All the nucleation mechanisms provided reasonable results, although the growth of particles due to condensation is inadequate in kinetic nucleation cases as compared with experimental measurements. Growth of newly formed particles could be assisted by any low-volatility vapors should their concentration exceed 10(9) cm(-3). Using the obtained values of coefficients K, A, and B we found that nucleation driven by iodine compounds in remote marine areas is possible, but by OIO and H2SO4 alone, only a minor fraction of newly formed particles is likely to reach detectable sizes. Owing to the scavenging by coagulation with background aerosol particles, few of them will likely reach climatically relevant sizes by acting as seed particles for other low-volatility vapors. In order to elucidate the significance of our results, more detailed measurements of OIO source and photolysis rates, dimensions of precursor areas, and particle chemical composition are needed.

Published
2009

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