Articles | Volume 19, issue 4
https://doi.org/10.5194/acp-19-2701-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-19-2701-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
01 Mar 2019
Research article |
| 01 Mar 2019
| 01 Mar 2019
Effect of salt seed particle surface area, composition and phase on secondary organic aerosol mass yields in oxidation flow reactors
Erik Ahlberg
CORRESPONDING AUTHOR
Centre for Environmental and Climate Research, Lund University,
Sölvegatan 37, 223 52 Lund, Sweden
Division of Nuclear Physics, Lund University, Box 118, 221 00 Lund,
Sweden
Axel Eriksson
Ergonomics and Aerosol Technology, Lund University, Box 118, 221 00
Lund, Sweden
William H. Brune
Department of Meteorology, Pennsylvania State University,
University Park, PA, USA
Pontus Roldin
Division of Nuclear Physics, Lund University, Box 118, 221 00 Lund,
Sweden
Birgitta Svenningsson
Division of Nuclear Physics, Lund University, Box 118, 221 00 Lund,
Sweden
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To investigate the properties and origin of black carbon particles in southern Sweden during late summer, we performed measurements both at a rural site and the nearby city of Malmö. We found that local traffic emissions of black carbon led to concentrations around twice as high as those at the rural site. Modeling show that these emissions are not clearly distinguishable at the rural site, unless meteorology was favourable, which shows the importance of long-range transport and processing.
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
Stina Ausmeel, Axel Eriksson, Erik Ahlberg, Moa K. Sporre, Mårten Spanne, and Adam Kristensson
Atmos. Chem. Phys., 20, 9135–9151, https://doi.org/10.5194/acp-20-9135-2020, https://doi.org/10.5194/acp-20-9135-2020, 2020
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Emissions from shipping have an impact on air quality, especially in coastal areas. We have measured properties of the airborne particles in several plumes from ships that are sailing within an Emission Control Area. Individual ships showed large variability in contribution to total particle mass and nitrogen dioxide. Organics and sulfate dominated the particle mass, and most plumes contained very little or no soot. We also present recommendations for future stationary ship plume measurements.
Stina Ausmeel, Axel Eriksson, Erik Ahlberg, and Adam Kristensson
Atmos. Meas. Tech., 12, 4479–4493, https://doi.org/10.5194/amt-12-4479-2019, https://doi.org/10.5194/amt-12-4479-2019, 2019
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We present a method for identifying individual exhaust plumes of air pollution emitted from shipping, by linking these to specific ships using identification information which all ships transmit. We also quantify the contribution of these plumes to local particle levels, which has relevance for health effects. Ships emit a lot of nanometre-sized particles, which proved to be a good indicator of plumes at a distance of about 10 km downwind of a shipping lane in the Baltic Sea.
Hilkka Timonen, Panu Karjalainen, Erkka Saukko, Sanna Saarikoski, Päivi Aakko-Saksa, Pauli Simonen, Timo Murtonen, Miikka Dal Maso, Heino Kuuluvainen, Matthew Bloss, Erik Ahlberg, Birgitta Svenningsson, Joakim Pagels, William H. Brune, Jorma Keskinen, Douglas R. Worsnop, Risto Hillamo, and Topi Rönkkö
Atmos. Chem. Phys., 17, 5311–5329, https://doi.org/10.5194/acp-17-5311-2017, https://doi.org/10.5194/acp-17-5311-2017, 2017
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The effect of fuel ethanol content (10–100 %) on primary emissions and the subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. The emissions were characterized during the New European Driving Cycle (NEDC) using high time-resolution instruments. The chemical composition of the exhaust particulate matter was studied using a soot particle aerosol mass spectrometer (SP-AMS), and the secondary aerosol formation was studied with an oxidation chamber.
Johan Martinsson, Hafiz Abdul Azeem, Moa K. Sporre, Robert Bergström, Erik Ahlberg, Emilie Öström, Adam Kristensson, Erik Swietlicki, and Kristina Eriksson Stenström
Atmos. Chem. Phys., 17, 4265–4281, https://doi.org/10.5194/acp-17-4265-2017, https://doi.org/10.5194/acp-17-4265-2017, 2017
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In this study we have focused our attention on the sources atmospheric carbon particles. More specifically, we evaluate a fast and inexpensive method which determines the source of these particles by utilizing light absorption by the particles. We found that this method is suitable for source estimation by comparing it to another method based on carbon isotopes and chemical tracer molecules. Cheap and fast methods based on light absorption can be utilized widely to deduce particle sources.
Panu Karjalainen, Hilkka Timonen, Erkka Saukko, Heino Kuuluvainen, Sanna Saarikoski, Päivi Aakko-Saksa, Timo Murtonen, Matthew Bloss, Miikka Dal Maso, Pauli Simonen, Erik Ahlberg, Birgitta Svenningsson, William Henry Brune, Risto Hillamo, Jorma Keskinen, and Topi Rönkkö
Atmos. Chem. Phys., 16, 8559–8570, https://doi.org/10.5194/acp-16-8559-2016, https://doi.org/10.5194/acp-16-8559-2016, 2016
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We characterized time-resolved primary particulate emissions and secondary particle formation from a modern gasoline passenger car. In mass terms, the amount of secondary particles was 13 times the amount of primary particles. The highest emissions were observed after a cold start when the engine and catalyst performance were suboptimal. The key parameter for secondary particle formation was the amount of gaseous hydrocarbons in the exhaust.
Jena M. Jenkins and William H. Brune
EGUsphere, https://doi.org/10.5194/egusphere-2024-3579, https://doi.org/10.5194/egusphere-2024-3579, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Both the atmosphere’s primary cleaner, the hydroxyl radical, and nitric oxide are generated in extreme amounts by lightning, and laboratory and modelling experiments demonstrate that these molecules are generated in different places in lightning flashes. Thus the hydroxyl radical is not immediately consumed by the nitric oxide and instead is available to remove other pollutants in the atmosphere. Additionally, substantial nitrous acid is also likely generated by lightning.
Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn
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∆3-carene is abundantly emitted from vegetation, but its atmospheric oxidation chemistry has received limited attention. We explored highly oxygenated organic molecule (HOM) formation from ∆3-carene ozonolysis in chambers and investigated the impact of temperature and relative humidity on HOM formation. Our findings provide new insights into ∆3-carene oxidation pathways and their potential to impact atmospheric aerosols.
Dimitri Castarède, Zoé Brasseur, Yusheng Wu, Zamin A. Kanji, Markus Hartmann, Lauri Ahonen, Merete Bilde, Markku Kulmala, Tuukka Petäjä, Jan B. C. Pettersson, Berko Sierau, Olaf Stetzer, Frank Stratmann, Birgitta Svenningsson, Erik Swietlicki, Quynh Thu Nguyen, Jonathan Duplissy, and Erik S. Thomson
Atmos. Meas. Tech., 16, 3881–3899, https://doi.org/10.5194/amt-16-3881-2023, https://doi.org/10.5194/amt-16-3881-2023, 2023
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Erik Ahlberg, Stina Ausmeel, Lovisa Nilsson, Mårten Spanne, Julija Pauraite, Jacob Klenø Nøjgaard, Michele Bertò, Henrik Skov, Pontus Roldin, Adam Kristensson, Erik Swietlicki, and Axel Eriksson
Atmos. Chem. Phys., 23, 3051–3064, https://doi.org/10.5194/acp-23-3051-2023, https://doi.org/10.5194/acp-23-3051-2023, 2023
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To investigate the properties and origin of black carbon particles in southern Sweden during late summer, we performed measurements both at a rural site and the nearby city of Malmö. We found that local traffic emissions of black carbon led to concentrations around twice as high as those at the rural site. Modeling show that these emissions are not clearly distinguishable at the rural site, unless meteorology was favourable, which shows the importance of long-range transport and processing.
Amir H. Souri, Matthew S. Johnson, Glenn M. Wolfe, James H. Crawford, Alan Fried, Armin Wisthaler, William H. Brune, Donald R. Blake, Andrew J. Weinheimer, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Corinne Vigouroux, Bavo Langerock, Sungyeon Choi, Lok Lamsal, Lei Zhu, Shuai Sun, Ronald C. Cohen, Kyung-Eun Min, Changmin Cho, Sajeev Philip, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 23, 1963–1986, https://doi.org/10.5194/acp-23-1963-2023, https://doi.org/10.5194/acp-23-1963-2023, 2023
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We have rigorously characterized different sources of error in satellite-based HCHO / NO2 tropospheric columns, a widely used metric for diagnosing near-surface ozone sensitivity. Specifically, the errors were categorized/quantified into (i) an inherent chemistry error, (ii) the decoupled relationship between columns and the near-surface concentration, (iii) the spatial representativeness error of ground satellite pixels, and (iv) the satellite retrieval errors.
Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Putian Zhou, Tinja Olenius, Pontus Roldin, and Michael Boy
Geosci. Model Dev., 15, 7257–7286, https://doi.org/10.5194/gmd-15-7257-2022, https://doi.org/10.5194/gmd-15-7257-2022, 2022
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Atmospheric chemistry and aerosol processes form a dynamic and sensitively balanced system, and solving problems regarding air quality or climate requires detailed modelling and coupling of the processes. The models involved are often very complex to use. We have addressed this problem with the new ARCA box model. It puts much of the current knowledge of the nano- and microscale aerosol dynamics and chemistry into usable software and has the potential to become a valuable tool in the community.
Carlton Xavier, Metin Baykara, Robin Wollesen de Jonge, Barbara Altstädter, Petri Clusius, Ville Vakkari, Roseline Thakur, Lisa Beck, Silvia Becagli, Mirko Severi, Rita Traversi, Radovan Krejci, Peter Tunved, Mauro Mazzola, Birgit Wehner, Mikko Sipilä, Markku Kulmala, Michael Boy, and Pontus Roldin
Atmos. Chem. Phys., 22, 10023–10043, https://doi.org/10.5194/acp-22-10023-2022, https://doi.org/10.5194/acp-22-10023-2022, 2022
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The focus of this work is to study and improve our understanding of processes involved in the formation and growth of new particles in a remote Arctic marine environment. We run the 1D model ADCHEM along air mass trajectories arriving at Ny-Ålesund in May 2018. The model finds that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation at Ny-Ålesund. The growth of particles is driven via H2SO4 condensation and formation of methane sulfonic acid in the aqueous phase.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
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We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Robin Wollesen de Jonge, Jonas Elm, Bernadette Rosati, Sigurd Christiansen, Noora Hyttinen, Dana Lüdemann, Merete Bilde, and Pontus Roldin
Atmos. Chem. Phys., 21, 9955–9976, https://doi.org/10.5194/acp-21-9955-2021, https://doi.org/10.5194/acp-21-9955-2021, 2021
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This study presents a detailed analysis of the OH-initiated oxidation of dimethyl sulfide (DMS) based on experiments performed in the Aarhus University Research on Aerosol (AURA) smog chamber and the gas- and particle-phase chemistry kinetic multilayer model (ADCHAM). We capture the formation, growth and chemical composition of aerosols in the chamber setup by an improved multiphase oxidation mechanism and utilize our results to reproduce the important role of DMS in the marine boundary layer.
Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Vilhelm B. Malmborg, Axel C. Eriksson, Kimmo Korhonen, Ricardo Luis Carvalho, Christoffer Boman, Joakim Pagels, and Birgitta Svenningsson
Atmos. Chem. Phys., 21, 8023–8044, https://doi.org/10.5194/acp-21-8023-2021, https://doi.org/10.5194/acp-21-8023-2021, 2021
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Residential biomass combustion is a major anthropogenic source of aerosol particles on regional and global scales. Nevertheless, little is known about those aerosol particles' ability to act as cloud condensation nuclei (CCN) and thus influence cloud properties and climate. Our study shows a strong link between the potassium content in the fuel and emissions of CCN for different stove technologies. Previous studies may have underestimated the anthropogenic climate impact of these emissions.
Mona Kurppa, Pontus Roldin, Jani Strömberg, Anna Balling, Sasu Karttunen, Heino Kuuluvainen, Jarkko V. Niemi, Liisa Pirjola, Topi Rönkkö, Hilkka Timonen, Antti Hellsten, and Leena Järvi
Geosci. Model Dev., 13, 5663–5685, https://doi.org/10.5194/gmd-13-5663-2020, https://doi.org/10.5194/gmd-13-5663-2020, 2020
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High-resolution modelling is needed to solve the aerosol concentrations in a complex urban area. Here, the performance of an aerosol module within the PALM model to simulate the detailed horizontal and vertical distribution of aerosol particles is studied. Further, sensitivity to the meteorological and aerosol boundary conditions is assessed using both model and observation data. The horizontal distribution is sensitive to the wind speed and stability, and the vertical to the wind direction.
Jake P. Rowe, Andrew T. Lambe, and William H. Brune
Atmos. Chem. Phys., 20, 13417–13424, https://doi.org/10.5194/acp-20-13417-2020, https://doi.org/10.5194/acp-20-13417-2020, 2020
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We conducted a series of experiments in which the 185 to 254 nm photon flux ratio (I185 : I254) emitted by low-pressure mercury lamps installed in an oxidation flow reactor (OFR) was systematically varied using multiple novel lamp configurations. Integrated OH exposure values achieved for each lamp type were obtained as a function of OFR operating conditions. A photochemical box model was used to develop a generalized OH exposure estimation equation as a function of [H2O], [O3], and OH reactivity.
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
Stina Ausmeel, Axel Eriksson, Erik Ahlberg, Moa K. Sporre, Mårten Spanne, and Adam Kristensson
Atmos. Chem. Phys., 20, 9135–9151, https://doi.org/10.5194/acp-20-9135-2020, https://doi.org/10.5194/acp-20-9135-2020, 2020
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Emissions from shipping have an impact on air quality, especially in coastal areas. We have measured properties of the airborne particles in several plumes from ships that are sailing within an Emission Control Area. Individual ships showed large variability in contribution to total particle mass and nitrogen dioxide. Organics and sulfate dominated the particle mass, and most plumes contained very little or no soot. We also present recommendations for future stationary ship plume measurements.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Ricardo Luis Carvalho, Vilhelm Malmborg, Axel Eriksson, Christoffer Boman, Joakim Pagels, Birgitta Svenningsson, Mika Komppula, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 20, 4951–4968, https://doi.org/10.5194/acp-20-4951-2020, https://doi.org/10.5194/acp-20-4951-2020, 2020
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Ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves were studied using a portable ice nuclei counter in an extensive laboratory experiment campaign. We found that even small changes in combustion conditions may affect the ice-nucleating ability of the emissions significantly. Also six different physico-chemical properties of the emissions were studied, but no clear correlation to their ice-nucleating ability was found.
Dean Chen, Putian Zhou, Tuomo Nieminen, Pontus Roldin, Ximeng Qi, Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Markku Kulmala, Pekka Rantala, Juho Aalto, Nina Sarnela, Pasi Kolari, Petri Keronen, Matti P. Rissanen, Metin Baykara, and Michael Boy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-128, https://doi.org/10.5194/acp-2020-128, 2020
Preprint withdrawn
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
Alexander B. Thames, William H. Brune, David O. Miller, Hannah M. Allen, Eric C. Apel, Donald R. Blake, T. Paul Bui, Roisin Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, Joshua P. DiGangi, James W. Elkins, Samuel R. Hall, Thomas F. Hanisco, Reem A. Hannun, Eric Hintsa, Rebecca S. Hornbrook, Michelle J. Kim, Kathryn McKain, Fred L. Moore, Julie M. Nicely, Jeffrey Peischl, Thomas B. Ryerson, Jason M. St. Clair, Colm Sweeney, Alex Teng, Chelsea R. Thompson, Kirk Ullmann, Paul O. Wennberg, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 4013–4029, https://doi.org/10.5194/acp-20-4013-2020, https://doi.org/10.5194/acp-20-4013-2020, 2020
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Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Otso Peräkylä, Matthieu Riva, Liine Heikkinen, Lauriane Quéléver, Pontus Roldin, and Mikael Ehn
Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, https://doi.org/10.5194/acp-20-649-2020, 2020
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Highly oxygenated organic molecules have been suggested to form a large part of secondary organic aerosol. However, with their exotic structures, their volatilities are not well known, making their exact role in particle formation hard to assess. In laboratory experiments, we found the volatility of HOMs formed in the ozonolysis of the monoterpene alpha-pinene to be in the middle of earlier estimates. The volatilities of HOMs could be well explained in terms of their molecular formulae.
Carlton Xavier, Anton Rusanen, Putian Zhou, Chen Dean, Lukas Pichelstorfer, Pontus Roldin, and Michael Boy
Atmos. Chem. Phys., 19, 13741–13758, https://doi.org/10.5194/acp-19-13741-2019, https://doi.org/10.5194/acp-19-13741-2019, 2019
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Master Chemical Mechanism (MCM) coupled to peroxy radical autoxidation mechanism (PRAM) was used to simulate secondary organic aerosol mass loadings from oxidation of five selected biogenic volatile organic compounds. The simulations were designed to replicate idealized chamber and oxidative flow-tube setups. The mass yields using MCM + PRAM are in good agreement with the experimental yields, thereby allowing us to highlight a few important compounds which contribute to > 95 % of mass loadings.
Stina Ausmeel, Axel Eriksson, Erik Ahlberg, and Adam Kristensson
Atmos. Meas. Tech., 12, 4479–4493, https://doi.org/10.5194/amt-12-4479-2019, https://doi.org/10.5194/amt-12-4479-2019, 2019
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We present a method for identifying individual exhaust plumes of air pollution emitted from shipping, by linking these to specific ships using identification information which all ships transmit. We also quantify the contribution of these plumes to local particle levels, which has relevance for health effects. Ships emit a lot of nanometre-sized particles, which proved to be a good indicator of plumes at a distance of about 10 km downwind of a shipping lane in the Baltic Sea.
Ingeborg E. Nielsen, Henrik Skov, Andreas Massling, Axel C. Eriksson, Manuel Dall'Osto, Heikki Junninen, Nina Sarnela, Robert Lange, Sonya Collier, Qi Zhang, Christopher D. Cappa, and Jacob K. Nøjgaard
Atmos. Chem. Phys., 19, 10239–10256, https://doi.org/10.5194/acp-19-10239-2019, https://doi.org/10.5194/acp-19-10239-2019, 2019
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Measurements of the chemical composition of sub-micrometer aerosols were carried out in northern Greenland during the Arctic haze (February–May) where concentrations are high due to favorable conditions for long-range transport. Sulfate was the dominant aerosol (66 %), followed by organic matter (24 %). The highest black carbon concentrations where observed in February. Source apportionment yielded three factors: a primary factor (12 %), an Arctic haze factor (64 %) and a marine factor (22 %).
Lauriane L. J. Quéléver, Kasper Kristensen, Louise Normann Jensen, Bernadette Rosati, Ricky Teiwes, Kaspar R. Daellenbach, Otso Peräkylä, Pontus Roldin, Rossana Bossi, Henrik B. Pedersen, Marianne Glasius, Merete Bilde, and Mikael Ehn
Atmos. Chem. Phys., 19, 7609–7625, https://doi.org/10.5194/acp-19-7609-2019, https://doi.org/10.5194/acp-19-7609-2019, 2019
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Highly oxygenated organic molecules (HOMs) form rapidly in oxidation of monoterpenes and have been shown to be crucial for secondary organic aerosol formation. We studied the formation of HOMs under different temperatures, finding a strong dependence on their yields. As temperatures decrease, the isomerization reactions that allow rapid oxidation by molecular oxygen slow down, and competing reaction pathways can suppress the HOM formation almost completely, especially at high VOC loadings.
Mona Kurppa, Antti Hellsten, Pontus Roldin, Harri Kokkola, Juha Tonttila, Mikko Auvinen, Christoph Kent, Prashant Kumar, Björn Maronga, and Leena Järvi
Geosci. Model Dev., 12, 1403–1422, https://doi.org/10.5194/gmd-12-1403-2019, https://doi.org/10.5194/gmd-12-1403-2019, 2019
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This paper describes the implementation of a sectional aerosol module, SALSA, into the PALM model system 6.0. The first evaluation study shows excellent agreements with measurements. Furthermore, we show that ignoring the dry deposition of aerosol particles can overestimate aerosol number concentrations by 20 %, whereas condensation and dissolutional growth increase the total aerosol mass by over 10 % in this specific urban environment.
Nikos Kalivitis, Veli-Matti Kerminen, Giorgos Kouvarakis, Iasonas Stavroulas, Evaggelia Tzitzikalaki, Panayiotis Kalkavouras, Nikos Daskalakis, Stelios Myriokefalitakis, Aikaterini Bougiatioti, Hanna E. Manninen, Pontus Roldin, Tuukka Petäjä, Michael Boy, Markku Kulmala, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 2671–2686, https://doi.org/10.5194/acp-19-2671-2019, https://doi.org/10.5194/acp-19-2671-2019, 2019
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New particle formation (NPF) is an important source of atmospheric aerosols. For the Mediterranean atmosphere, only few studies exist. In this study we present one of the longest series of NPF by analyzing 10 years of data from Crete, Greece. NPF took place on 27 % of the available days; it was more frequent in spring and less so in late summer. Model simulations showed that NPF in the subtropical environment may differ greatly from that in the boreal environment.
Michael Boy, Erik S. Thomson, Juan-C. Acosta Navarro, Olafur Arnalds, Ekaterina Batchvarova, Jaana Bäck, Frank Berninger, Merete Bilde, Zoé Brasseur, Pavla Dagsson-Waldhauserova, Dimitri Castarède, Maryam Dalirian, Gerrit de Leeuw, Monika Dragosics, Ella-Maria Duplissy, Jonathan Duplissy, Annica M. L. Ekman, Keyan Fang, Jean-Charles Gallet, Marianne Glasius, Sven-Erik Gryning, Henrik Grythe, Hans-Christen Hansson, Margareta Hansson, Elisabeth Isaksson, Trond Iversen, Ingibjorg Jonsdottir, Ville Kasurinen, Alf Kirkevåg, Atte Korhola, Radovan Krejci, Jon Egill Kristjansson, Hanna K. Lappalainen, Antti Lauri, Matti Leppäranta, Heikki Lihavainen, Risto Makkonen, Andreas Massling, Outi Meinander, E. Douglas Nilsson, Haraldur Olafsson, Jan B. C. Pettersson, Nønne L. Prisle, Ilona Riipinen, Pontus Roldin, Meri Ruppel, Matthew Salter, Maria Sand, Øyvind Seland, Heikki Seppä, Henrik Skov, Joana Soares, Andreas Stohl, Johan Ström, Jonas Svensson, Erik Swietlicki, Ksenia Tabakova, Throstur Thorsteinsson, Aki Virkkula, Gesa A. Weyhenmeyer, Yusheng Wu, Paul Zieger, and Markku Kulmala
Atmos. Chem. Phys., 19, 2015–2061, https://doi.org/10.5194/acp-19-2015-2019, https://doi.org/10.5194/acp-19-2015-2019, 2019
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The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date and aimed to strengthen research and innovation regarding climate change issues in the Nordic region. The paper presents an overview of the main scientific topics investigated and provides a state-of-the-art comprehensive summary of what has been achieved in CRAICC.
Nathan J. Janechek, Rachel F. Marek, Nathan Bryngelson, Ashish Singh, Robert L. Bullard, William H. Brune, and Charles O. Stanier
Atmos. Chem. Phys., 19, 1649–1664, https://doi.org/10.5194/acp-19-1649-2019, https://doi.org/10.5194/acp-19-1649-2019, 2019
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Cyclic volatile methyl siloxanes (cVMSs) are widely used chemicals in personal care products which can undergo oxidation to generate secondary organic aerosol. In this work, cVMS oxidation aerosols were generated using a photochemical chamber and the physical properties characterized. The aerosol yield, volatility, hygroscopicity, morphology, elemental composition, and proposed parameters for treatment as secondary organic aerosol in atmospheric models are provided.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Ximeng Qi, Aijun Ding, Pontus Roldin, Zhengning Xu, Putian Zhou, Nina Sarnela, Wei Nie, Xin Huang, Anton Rusanen, Mikael Ehn, Matti P. Rissanen, Tuukka Petäjä, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 18, 11779–11791, https://doi.org/10.5194/acp-18-11779-2018, https://doi.org/10.5194/acp-18-11779-2018, 2018
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In this study we simulate the HOM concentrations and discuss their roles in NPF at a remote boreal forest site in Finland and a suburban site in eastern China. We found that sulfuric acid and HOM organonitrate concentrations in the gas phase are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower in eastern China. This study highlights the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas.
Luciana Varanda Rizzo, Pontus Roldin, Joel Brito, John Backman, Erik Swietlicki, Radovan Krejci, Peter Tunved, Tukka Petäjä, Markku Kulmala, and Paulo Artaxo
Atmos. Chem. Phys., 18, 10255–10274, https://doi.org/10.5194/acp-18-10255-2018, https://doi.org/10.5194/acp-18-10255-2018, 2018
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Aerosols are tiny particles suspended in the air that can interact with sunlight and form clouds, which in turn affect the climate. They can also recycle nutrients in forest environments. Aerosols are naturally emitted at the surface in the Amazon forest, in addition to being brought down from above the boundary layer by intense air movements. In this work, we describe how the particle size number concentrations of aerosols change over hours, days and seasons in a multi-year study in Amazonia.
Xiangyu Pei, Mattias Hallquist, Axel C. Eriksson, Joakim Pagels, Neil M. Donahue, Thomas Mentel, Birgitta Svenningsson, William Brune, and Ravi Kant Pathak
Atmos. Chem. Phys., 18, 9845–9860, https://doi.org/10.5194/acp-18-9845-2018, https://doi.org/10.5194/acp-18-9845-2018, 2018
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The findings in this study show that morphological transformation of soot occurs via two key complementary and sequential processes, i.e., void filling in the particle and its diameter growth. To quantify the state of morphological transformation, i.e., the utilization of material for filling and growth during the condensation processes, a framework was developed which can further be utilized to quantify the effect of condensed material on the optical and hygroscopic properties of soot.
Eunha Kang, Meehye Lee, William H. Brune, Taehyoung Lee, Taehyun Park, Joonyoung Ahn, and Xiaona Shang
Atmos. Chem. Phys., 18, 6661–6677, https://doi.org/10.5194/acp-18-6661-2018, https://doi.org/10.5194/acp-18-6661-2018, 2018
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A potential aerosol mass (PAM) reactor expedites slow atmospheric oxidation reactions and enables the observation of chemical aging processes and the determination of the aerosol-forming power of an air mass. A PAM reactor was deployed at Baengnyeong Island in the Yellow Sea. Experimental results confirm the key role of SO2 in generating secondary aerosols in northeast Asia, and the contribution of organics to secondary aerosols is more variable during transport in the atmosphere.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Kenneth E. Christian, William H. Brune, Jingqiu Mao, and Xinrong Ren
Atmos. Chem. Phys., 18, 2443–2460, https://doi.org/10.5194/acp-18-2443-2018, https://doi.org/10.5194/acp-18-2443-2018, 2018
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We applied a global sensitivity analysis to the GEOS-Chem chemical transport model analyzing some well-studied tropospheric oxidants for a time period corresponding to an aircraft field campaign. We find modeled results generally agree with measurements when uncertainties in both the model and measurements are taken into account. While model results were largely sensitive to emissions, chemical reaction rates also represented a large source of uncertainty.
Claire F. Fortenberry, Michael J. Walker, Yaping Zhang, Dhruv Mitroo, William H. Brune, and Brent J. Williams
Atmos. Chem. Phys., 18, 2199–2224, https://doi.org/10.5194/acp-18-2199-2018, https://doi.org/10.5194/acp-18-2199-2018, 2018
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In these laboratory studies, two types of biomass burning organic aerosol (BBOA) were generated in a combustion chamber and treated in a flow reactor to mimic atmospheric oxidation. Complementary bulk and molecular chemical measurements show that while many species deplete with oxidation, oxidized BBOA markers are enhanced. The results provide insight into the complex chemical evolution of BBOA over nearly 10 days of atmospheric photochemistry, informing future laboratory and field studies.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Bianca C. Baier, William H. Brune, David O. Miller, Donald Blake, Russell Long, Armin Wisthaler, Christopher Cantrell, Alan Fried, Brian Heikes, Steven Brown, Erin McDuffie, Frank Flocke, Eric Apel, Lisa Kaser, and Andrew Weinheimer
Atmos. Chem. Phys., 17, 11273–11292, https://doi.org/10.5194/acp-17-11273-2017, https://doi.org/10.5194/acp-17-11273-2017, 2017
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Ozone production rates were measured using the Measurement of Ozone Production Sensor (MOPS). Measurements are compared to modeled ozone production rates using two different chemical mechanisms. At high nitric oxide levels, observed rates are higher than those modeled, prompting the need to revisit current model photochemistry. These direct measurements can add to our understanding of the ozone chemistry within air quality models and can be used to guide government regulatory strategies.
Georgios Tsagkogeorgas, Pontus Roldin, Jonathan Duplissy, Linda Rondo, Jasmin Tröstl, Jay G. Slowik, Sebastian Ehrhart, Alessandro Franchin, Andreas Kürten, Antonio Amorim, Federico Bianchi, Jasper Kirkby, Tuukka Petäjä, Urs Baltensperger, Michael Boy, Joachim Curtius, Richard C. Flagan, Markku Kulmala, Neil M. Donahue, and Frank Stratmann
Atmos. Chem. Phys., 17, 8923–8938, https://doi.org/10.5194/acp-17-8923-2017, https://doi.org/10.5194/acp-17-8923-2017, 2017
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The H2SO4 vapour pressure plays key role in Earth's and Venus' atmospheres. In regions where RH is low and stabilising bases are scarce, H2SO4 can evaporate from particles; however the H2SO4 vapour pressure at low RH is uncertain. To address this, we measured H2SO4 evaporation versus T and RH in the CLOUD chamber and constrained the equilibrium constants for dissociation and dehydration of H2SO4. This study is important for nucleation, particle growth and H2SO4 formation occurring in atmosphere.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
Hilkka Timonen, Panu Karjalainen, Erkka Saukko, Sanna Saarikoski, Päivi Aakko-Saksa, Pauli Simonen, Timo Murtonen, Miikka Dal Maso, Heino Kuuluvainen, Matthew Bloss, Erik Ahlberg, Birgitta Svenningsson, Joakim Pagels, William H. Brune, Jorma Keskinen, Douglas R. Worsnop, Risto Hillamo, and Topi Rönkkö
Atmos. Chem. Phys., 17, 5311–5329, https://doi.org/10.5194/acp-17-5311-2017, https://doi.org/10.5194/acp-17-5311-2017, 2017
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The effect of fuel ethanol content (10–100 %) on primary emissions and the subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. The emissions were characterized during the New European Driving Cycle (NEDC) using high time-resolution instruments. The chemical composition of the exhaust particulate matter was studied using a soot particle aerosol mass spectrometer (SP-AMS), and the secondary aerosol formation was studied with an oxidation chamber.
Johan Martinsson, Hafiz Abdul Azeem, Moa K. Sporre, Robert Bergström, Erik Ahlberg, Emilie Öström, Adam Kristensson, Erik Swietlicki, and Kristina Eriksson Stenström
Atmos. Chem. Phys., 17, 4265–4281, https://doi.org/10.5194/acp-17-4265-2017, https://doi.org/10.5194/acp-17-4265-2017, 2017
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In this study we have focused our attention on the sources atmospheric carbon particles. More specifically, we evaluate a fast and inexpensive method which determines the source of these particles by utilizing light absorption by the particles. We found that this method is suitable for source estimation by comparing it to another method based on carbon isotopes and chemical tracer molecules. Cheap and fast methods based on light absorption can be utilized widely to deduce particle sources.
Kenneth E. Christian, William H. Brune, and Jingqiu Mao
Atmos. Chem. Phys., 17, 3769–3784, https://doi.org/10.5194/acp-17-3769-2017, https://doi.org/10.5194/acp-17-3769-2017, 2017
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To better understand the sources of uncertainty in modeled Arctic tropospheric oxidants, we created and analyzed an ensemble of chemical transport model runs with inputs perturbed according to their respective uncertainties. Ozone and OH were most sensitive to various emissions and chemical factors. HO2 was overwhelmingly sensitive to aerosol particle uptake. When compared to airborne measurements, better agreement was found when the model used lower aerosol particle uptake rates.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Panu Karjalainen, Hilkka Timonen, Erkka Saukko, Heino Kuuluvainen, Sanna Saarikoski, Päivi Aakko-Saksa, Timo Murtonen, Matthew Bloss, Miikka Dal Maso, Pauli Simonen, Erik Ahlberg, Birgitta Svenningsson, William Henry Brune, Risto Hillamo, Jorma Keskinen, and Topi Rönkkö
Atmos. Chem. Phys., 16, 8559–8570, https://doi.org/10.5194/acp-16-8559-2016, https://doi.org/10.5194/acp-16-8559-2016, 2016
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We characterized time-resolved primary particulate emissions and secondary particle formation from a modern gasoline passenger car. In mass terms, the amount of secondary particles was 13 times the amount of primary particles. The highest emissions were observed after a cold start when the engine and catalyst performance were suboptimal. The key parameter for secondary particle formation was the amount of gaseous hydrocarbons in the exhaust.
Luping Su, Edward G. Patton, Jordi Vilà-Guerau de Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong-Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, and John E. Mak
Atmos. Chem. Phys., 16, 7725–7741, https://doi.org/10.5194/acp-16-7725-2016, https://doi.org/10.5194/acp-16-7725-2016, 2016
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Hannah M. Allen, Benjamin R. Ayres, Steven S. Brown, William H. Brune, John D. Crounse, Joost de Gouw, Danielle C. Draper, Philip A. Feiner, Juliane L. Fry, Allen H. Goldstein, Abigail Koss, Pawel K. Misztal, Tran B. Nguyen, Kevin Olson, Alex P. Teng, Paul O. Wennberg, Robert J. Wild, Li Zhang, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 7623–7637, https://doi.org/10.5194/acp-16-7623-2016, https://doi.org/10.5194/acp-16-7623-2016, 2016
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The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the southeastern United States. At warm temperatures in the daytime boundary layer, NOx interconverts rapidly with both PAN and alkyl and multifunctional nitrates (RONO2), and the relevant lifetime is the combined lifetime of these three classes. We find that the production of RONO2, followed by hydrolysis to produce nitric acid, is the dominant pathway for NOx removal in an isoprene dominated forest.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Zhe Peng, Douglas A. Day, Amber M. Ortega, Brett B. Palm, Weiwei Hu, Harald Stark, Rui Li, Kostas Tsigaridis, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, https://doi.org/10.5194/acp-16-4283-2016, 2016
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Oxidation flow reactors (OFRs) are promising tools of studying atmospheric oxidation processes. Elevated concentrations of both OH and non-OH oxidants in OFRs leave room for speculation that non-OH chemistry can play a major role. Through systematic modeling, we find conditions where non-OH VOC fate is significant and show that, in most field studies of SOA using OFRs, non-OH VOC fate in OFRs was insignificant. We also provide guidelines helping OFR users avoid significant non-OH VOC oxidation.
Brett B. Palm, Pedro Campuzano-Jost, Amber M. Ortega, Douglas A. Day, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, James F. Hunter, Eben S. Cross, Jesse H. Kroll, Zhe Peng, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 2943–2970, https://doi.org/10.5194/acp-16-2943-2016, https://doi.org/10.5194/acp-16-2943-2016, 2016
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Ambient pine forest air was oxidized by OH radicals in a PAM oxidation flow reactor during the BEACHON-RoMBAS campaign to study secondary organic aerosol formation. Approximately 4.4 times more secondary organic aerosol was formed in the reactor than could be explained by the volatile organic gases (VOCs) measured in ambient air. The organic aerosol formation can be explained by including an SOA yield from typically unmeasured semivolatile and intermediate-volatility organic gases (S/IVOCs).
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
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We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
Z. Peng, D. A. Day, H. Stark, R. Li, J. Lee-Taylor, B. B. Palm, W. H. Brune, and J. L. Jimenez
Atmos. Meas. Tech., 8, 4863–4890, https://doi.org/10.5194/amt-8-4863-2015, https://doi.org/10.5194/amt-8-4863-2015, 2015
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
P. Roldin, L. Liao, D. Mogensen, M. Dal Maso, A. Rusanen, V.-M. Kerminen, T. F. Mentel, J. Wildt, E. Kleist, A. Kiendler-Scharr, R. Tillmann, M. Ehn, M. Kulmala, and M. Boy
Atmos. Chem. Phys., 15, 10777–10798, https://doi.org/10.5194/acp-15-10777-2015, https://doi.org/10.5194/acp-15-10777-2015, 2015
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We used the ADCHAM model to study new particle formation events in the JPAC chamber. The model results show that the new particles may be formed by a kinetic type of nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of volatile organic compounds (VOCs). The observed particle growth may either be controlled by the condensation of semi- and low-volatililty organic compounds or by the formation of low-volatility compounds (oligomers) at the particle surface.
E. A. Bruns, I. El Haddad, A. Keller, F. Klein, N. K. Kumar, S. M. Pieber, J. C. Corbin, J. G. Slowik, W. H. Brune, U. Baltensperger, and A. S. H. Prévôt
Atmos. Meas. Tech., 8, 2315–2332, https://doi.org/10.5194/amt-8-2315-2015, https://doi.org/10.5194/amt-8-2315-2015, 2015
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
A. T. Lambe, P. S. Chhabra, T. B. Onasch, W. H. Brune, J. F. Hunter, J. H. Kroll, M. J. Cummings, J. F. Brogan, Y. Parmar, D. R. Worsnop, C. E. Kolb, and P. Davidovits
Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, https://doi.org/10.5194/acp-15-3063-2015, 2015
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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 2014
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
E. Hermansson, P. Roldin, A. Rusanen, D. Mogensen, N. Kivekäs, R. Väänänen, M. Boy, and E. Swietlicki
Atmos. Chem. Phys., 14, 11853–11869, https://doi.org/10.5194/acp-14-11853-2014, https://doi.org/10.5194/acp-14-11853-2014, 2014
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Secondary organic aerosols (SOA), produced through oxidation processes, constitute a large part of the global organic aerosol load and affect the climate. We found that the modeled mass of SOA was highly dependent on how the oxidation processes were explained in models. The results indicated that it was especially important to get the volatility distribution of the products from the first oxidation step right and that fragmentation during the oxidation process played an important role.
C. Wittbom, A. C. Eriksson, J. Rissler, J. E. Carlsson, P. Roldin, E. Z. Nordin, P. T. Nilsson, E. Swietlicki, J. H. Pagels, and B. Svenningsson
Atmos. Chem. Phys., 14, 9831–9854, https://doi.org/10.5194/acp-14-9831-2014, https://doi.org/10.5194/acp-14-9831-2014, 2014
P. Roldin, A. C. Eriksson, E. Z. Nordin, E. Hermansson, D. Mogensen, A. Rusanen, M. Boy, E. Swietlicki, B. Svenningsson, A. Zelenyuk, and J. Pagels
Atmos. Chem. Phys., 14, 7953–7993, https://doi.org/10.5194/acp-14-7953-2014, https://doi.org/10.5194/acp-14-7953-2014, 2014
E. Z. Nordin, A. C. Eriksson, P. Roldin, P. T. Nilsson, J. E. Carlsson, M. K. Kajos, H. Hellén, C. Wittbom, J. Rissler, J. Löndahl, E. Swietlicki, B. Svenningsson, M. Bohgard, M. Kulmala, M. Hallquist, and J. H. Pagels
Atmos. Chem. Phys., 13, 6101–6116, https://doi.org/10.5194/acp-13-6101-2013, https://doi.org/10.5194/acp-13-6101-2013, 2013
E. C. Browne, K.-E. Min, P. J. Wooldridge, E. Apel, D. R. Blake, W. H. Brune, C. A. Cantrell, M. J. Cubison, G. S. Diskin, J. L. Jimenez, A. J. Weinheimer, P. O. Wennberg, A. Wisthaler, and R. C. Cohen
Atmos. Chem. Phys., 13, 4543–4562, https://doi.org/10.5194/acp-13-4543-2013, https://doi.org/10.5194/acp-13-4543-2013, 2013
L. V. Rizzo, P. Artaxo, T. Müller, A. Wiedensohler, M. Paixão, G. G. Cirino, A. Arana, E. Swietlicki, P. Roldin, E. O. Fors, K. T. Wiedemann, L. S. M. Leal, and M. Kulmala
Atmos. Chem. Phys., 13, 2391–2413, https://doi.org/10.5194/acp-13-2391-2013, https://doi.org/10.5194/acp-13-2391-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photochemical reactions: remarkably enhancing effects of seeds and ammonia
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
The lifetimes and potential change in planetary albedo owing to the oxidation of organic films extracted from atmospheric aerosol by hydroyxl (OH) radical oxidation at the air-water interface of aerosol particles
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement Report: Changes of ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice core record
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Si Zhang, Yining Gao, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 14177–14190, https://doi.org/10.5194/acp-24-14177-2024, https://doi.org/10.5194/acp-24-14177-2024, 2024
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Secondary organic aerosols (SOAs) from acetone photooxidation in the presence of various seeds were studied to illustrate SOA formation kinetics under ammonia-rich conditions. The oxidation mechanism of acetone was investigated using an observation-based model incorporating a Master Chemical Mechanism model. A higher SOA yield of acetone was observed compared to methylglyoxal due to an enhanced uptake of the small photooxidation products of acetone.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
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We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
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This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Rosalie Shepherd, Martin King, Andrew Ward, Edward Stuckey, Rebecca Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2367, https://doi.org/10.5194/egusphere-2024-2367, 2024
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Thin film formation at the air-water interface from material extracted from atmospheric aerosol was demonstrated, supporting core-shell morphology. The film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 hour. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top of the atmosphere albedo for urban films.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
EGUsphere, https://doi.org/10.5194/egusphere-2024-1381, https://doi.org/10.5194/egusphere-2024-1381, 2024
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A record of ammonium covering the years 1750 to 2008 was extracted from a 182-meter-long ice core drilled in 2009 at Mt. Elbrus in the Caucasus, Russia. Changes in ammonia emissions in southeastern Europe during the pre-industrial and industrial periods were investigated. The level of ammonium in 1750 indicates a significant contribution of natural sources to the ammonia budget, contrasting with present-day conditions, where agricultural emissions outweigh those from biogenic sources in Europe.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
EGUsphere, https://doi.org/10.5194/egusphere-2024-1880, https://doi.org/10.5194/egusphere-2024-1880, 2024
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The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolite and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
Short summary
Short summary
Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
Short summary
Short summary
Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
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Short summary
The effects of wet or dry salt seed particle concentration (ammonium nitrate and ammonium sulphate) on secondary organic aerosol mass yields from a mixture of m-xylene and α-pinene were examined in an oxidation flow reactor. The experiments confirmed that increasing the condensation sink significantly increases the particle mass yields in oxidation flow reactors. Further, wet seed particles increased the particle mass yield by 60 % more than dry particles.
The effects of wet or dry salt seed particle concentration (ammonium nitrate and ammonium...
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