Research article
20 Oct 2020
Research article
| 20 Oct 2020
Molecular understanding of the suppression of new-particle formation by isoprene
Martin Heinritzi et al.
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Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-238, https://doi.org/10.5194/acp-2022-238, 2022
Revised manuscript under review for ACP
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.8 to 9.1E5 cm–3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Joschka Pfeifer, Mario Simon, Martin Heinritzi, Felix Piel, Lena Weitz, Dongyu Wang, Manuel Granzin, Tatjana Müller, Steffen Bräkling, Jasper Kirkby, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 13, 2501–2522, https://doi.org/10.5194/amt-13-2501-2020, https://doi.org/10.5194/amt-13-2501-2020, 2020
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Ammonia is an important atmospheric trace gas that affects secondary aerosol formation and, together with sulfuric acid, the formation of new particles. A measurement technique is presented that uses high-resolution mass spectrometry and protonated water clusters for the ultrasensitive detection of ammonia at single-digit parts per trillion by volume levels. The instrument is further capable of measuring amines and a suite of iodine compounds at sub-parts per trillion by volume levels.
Andrea C. Wagner, Anton Bergen, Sophia Brilke, Claudia Fuchs, Markus Ernst, Jesica Hoker, Martin Heinritzi, Mario Simon, Bertram Bühner, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 11, 5489–5506, https://doi.org/10.5194/amt-11-5489-2018, https://doi.org/10.5194/amt-11-5489-2018, 2018
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Chemical analysis of sub-30 nm aerosol particles is important for understanding aerosol nucleation and early growth, yet it is still an experimental challenge. In this study, we present a novel device for size resolved chemical analysis of nucleation and Aitken mode particles (from ~10 to ~30 nm) while allowing gas phase measurements with the same detector. Particles are charged, size selected, electrostatically collected and then thermally desorbed in a carrier gas.
Anne-Kathrin Bernhammer, Lukas Fischer, Bernhard Mentler, Martin Heinritzi, Mario Simon, and Armin Hansel
Atmos. Meas. Tech., 11, 4763–4773, https://doi.org/10.5194/amt-11-4763-2018, https://doi.org/10.5194/amt-11-4763-2018, 2018
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During new particle formation (NPF) studies from pure isoprene oxidation in the CLOUD chamber at CERN we observed unexpected ion signals. We identified two origins of these signals: first secondary association reactions of protonated isoprene with isoprene within the PTR3 reaction chamber and, second, polymerization of isoprene inside the gas bottle.
In order to study NPF from pure isoprene oxidation we had to install a cryogenic trap in the isoprene inlet line to remove polymerized isoprene.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Andreas Kürten, Anton Bergen, Martin Heinritzi, Markus Leiminger, Verena Lorenz, Felix Piel, Mario Simon, Robert Sitals, Andrea C. Wagner, and Joachim Curtius
Atmos. Chem. Phys., 16, 12793–12813, https://doi.org/10.5194/acp-16-12793-2016, https://doi.org/10.5194/acp-16-12793-2016, 2016
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Field measurements were conducted at a rural site in central Germany close to dairy farms to investigate if there is a connection between new particle formation and the presence of amines. A variety of trace gases were measured in addition to amines, like sulfuric acid, ammonia and highly oxygenated organic molecules (HOM). The results indicate that amines are very likely involved in the growth of aerosol particles and probably also in the nucleation process, although HOM could be relevant, too.
Mario Simon, Martin Heinritzi, Stephan Herzog, Markus Leiminger, Federico Bianchi, Arnaud Praplan, Josef Dommen, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 9, 2135–2145, https://doi.org/10.5194/amt-9-2135-2016, https://doi.org/10.5194/amt-9-2135-2016, 2016
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This study demonstrate the detection of dimethylamine at low mixing ratios by nitrate chemical ionization mass spectrometry (CIMS). Due to simultaneously high-sensitive gas-phase measurements of DMA, sulfuric acid, and extremely low volatile organic compounds (ELVOCs), this technique can be used as a versatile tool for studying new particle formation in the atmosphere.
Martin Heinritzi, Mario Simon, Gerhard Steiner, Andrea C. Wagner, Andreas Kürten, Armin Hansel, and Joachim Curtius
Atmos. Meas. Tech., 9, 1449–1460, https://doi.org/10.5194/amt-9-1449-2016, https://doi.org/10.5194/amt-9-1449-2016, 2016
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An easy-to-use method of estimating the mass-dependent transmission efficiency of a CIMS is presented. It makes use of depleting nitrate primary ions by different perfluorinated acids to obtain the transmission efficiency of these acids relative to the primary ion. Knowledge about the transmission efficiency is crucial for, e.g., quantification of extremely low volatile organic compounds.
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
Preprint under review for ESD
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The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Yishuo Guo, Chao Yan, Yuliang Liu, Xiaohui Qiao, Feixue Zheng, Ying Zhang, Ying Zhou, Chang Li, Xiaolong Fan, Zhuohui Lin, Zemin Feng, Yusheng Zhang, Penggang Zheng, Linhui Tian, Wei Nie, Zhe Wang, Dandan Huang, Kaspar R. Daellenbach, Lei Yao, Lubna Dada, Federico Bianchi, Jingkun Jiang, Yongchun Liu, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 10077–10097, https://doi.org/10.5194/acp-22-10077-2022, https://doi.org/10.5194/acp-22-10077-2022, 2022
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Gaseous oxygenated organic molecules (OOMs) are able to form atmospheric aerosols, which will impact on human health and climate change. Here, we find that OOMs in urban Beijing are dominated by anthropogenic sources, i.e. aromatic (29 %–41 %) and aliphatic (26 %–41 %) OOMs. They are also the main contributors to the condensational growth of secondary organic aerosols (SOAs). Therefore, the restriction on anthropogenic VOCs is crucial for the reduction of SOAs and haze formation.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Markku Kulmala, Jingkun Jiang, Chao Yan, and Jenni Kontkanen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-484, https://doi.org/10.5194/acp-2022-484, 2022
Preprint under review for ACP
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We compare observed survival probabilities of atmospheric particles from Beijing, China to survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower or similar, than theoretical survival probabilities. Uncertainties in condensation sink and growth rate are found unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
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.
Christian Tatzelt, Silvia Henning, André Welti, Andrea Baccarini, Markus Hartmann, Martin Gysel-Beer, Manuela van Pinxteren, Robin L. Modini, Julia Schmale, and Frank Stratmann
Atmos. Chem. Phys., 22, 9721–9745, https://doi.org/10.5194/acp-22-9721-2022, https://doi.org/10.5194/acp-22-9721-2022, 2022
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We present the abundance and origin of cloud-relevant aerosol particles in the preindustral-like conditions of the Southern Ocean (SO) during austral summer. Cloud condensation nuclei (CCN) and ice-nucleating particles (INP) were measured during a circum-Antarctic scientific cruise with in situ instrumentation and offline filter measurements, respectively. Transport processes were found to play an equally important role as local sources for both the CCN and INP population of the SO.
Runlong Cai, Chenjuan Deng, Dominik Stolzenburg, Chenxi Li, Junchen Guo, Veli-Matti Kerminen, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-476, https://doi.org/10.5194/acp-2022-476, 2022
Preprint under review for ACP
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The survival probability of new particles is the key parameter governing their influences on the atmosphere and climate, yet the knowledge of particle survival in the atmosphere is rather limited. We propose methods to compute the size-resolved particle survival probability and validate them using simulations and measurements from diverse environments. Using these methods, we could explain particle survival from the cluster size to the cloud condensation nuclei size.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Suzanne Crumeyrolle, Jenni Kontkanen, Clémence Rose, Alejandra Velasquez Garcia, Eric Bourrianne, Maxime Catalfamo, Véronique Riffault, Emmanuel Tison, Joel Ferreira de Brito, Nicolas Visez, Nicolas Ferlay, Frédérique Auriol, and Isabelle Chiapello
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-436, https://doi.org/10.5194/acp-2022-436, 2022
Preprint under review for ACP
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Ultrafine particles (UFPs) are particles with an aerodynamic diameter of 100 nm or less, has negligible mass concentration but is the dominant contributor to the total particle number concentration. The present study aims to better understand the environmental factors favoring or inhibiting, atmospheric new particle formation (NPF) over Lille a large city North of France and to analyze the impact of such event on urban air quality using a long-term dataset (3 years).
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-472, https://doi.org/10.5194/acp-2022-472, 2022
Preprint under review for ACP
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean, but larger differences in the seasonal consideration.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Karine Sartelet, Youngseob Kim, Florian Couvidat, Maik Merkel, Tuukka Petäjä, Jean Sciare, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 8579–8596, https://doi.org/10.5194/acp-22-8579-2022, https://doi.org/10.5194/acp-22-8579-2022, 2022
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A methodology is defined to estimate number emissions from an inventory providing mass emissions. Number concentrations are simulated over Greater Paris using different nucleation parameterisations (binary, ternary involving sulfuric acid and ammonia, and heteromolecular involving sulfuric acid and extremely low-volatility organics, ELVOCs). The comparisons show that ternary nucleation may not be a dominant process for new particle formation in cities, but they stress the role of ELVOCs.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Juha Sulo, Janne Lampilahti, Xuemeng Chen, Jenni Kontkanen, Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Katrianne Lehtipalo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-392, https://doi.org/10.5194/acp-2022-392, 2022
Preprint under review for ACP
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We measured atmospheric ion concentrations continuously in a boreal forest between 2005 and 2021 and observed an increasing inter-annual trend. The increase in cluster ion concentrations can be largely explained by overall decreasing level of anthropogenic aerosols in the boreal forest. This suggests that the role of ions in atmospheric new particle formation may be more important in the future.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Miska Olin, Magdalena Okuljar, Matti P. Rissanen, Joni Kalliokoski, Jiali Shen, Lubna Dada, Markus Lampimäki, Yusheng Wu, Annalea Lohila, Jonathan Duplissy, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 8097–8115, https://doi.org/10.5194/acp-22-8097-2022, https://doi.org/10.5194/acp-22-8097-2022, 2022
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Atmospheric new particle formation is an important source of the total particle number concentration in the atmosphere. Several parameters for predicting new particle formation events have been suggested before, but the results have been inconclusive. This study proposes an another predicting parameter, related to a specific type of highly oxidized organic molecules, especially for similar locations to the measurement site in this study, which was a coastal agricultural site in Finland.
Markus Leiminger, Lukas Fischer, Sophia Brilke, Julian Resch, Paul Martin Winkler, Armin Hansel, and Gerhard Steiner
Atmos. Meas. Tech., 15, 3705–3720, https://doi.org/10.5194/amt-15-3705-2022, https://doi.org/10.5194/amt-15-3705-2022, 2022
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We developed an axial ion mobility classifier coupled to an atmospheric-pressure interface time-of-flight (APi-TOF) mass spectrometer to measure size-segregated atmospheric ions. We characterize the performance of the novel instrument with bipolar-electrospray-generated ion mobility standards and compare the results with CFD simulations and a simplified numerical particle-tracking model. Ultimately, we report first mass–mobility measurements of atmospheric ions in Innsbruck, Austria.
Chenjuan Deng, Yiran Li, Chao Yan, Jin Wu, Runlong Cai, Dongbin Wang, Yongchun Liu, Juha Kangasluoma, Veli-Matti Kerminen, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-414, https://doi.org/10.5194/acp-2022-414, 2022
Preprint under review for ACP
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The size distributions of urban atmospheric particles convey important information on their origins and impacts. This study investigates the characteristics of typical particle size distributions together with key gaseous precursors from the long-term perspective in urban Beijing. A fitting function is proposed to represent and help to interpret the size distribution including particles and gaseous precursors. In addition to NPF as the major source, vehicles can emit sub-3 nm particles as well.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Michael S. Diamond, Pablo E. Saide, Paquita Zuidema, Andrew S. Ackerman, Sarah J. Doherty, Ann M. Fridlind, Hamish Gordon, Calvin Howes, Jan Kazil, Takanobu Yamaguchi, Jianhao Zhang, Graham Feingold, and Robert Wood
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-411, https://doi.org/10.5194/acp-2022-411, 2022
Revised manuscript under review for ACP
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Smoke from southern Africa blankets the southeast Atlantic Ocean from June-October, overlying a major low-altitude cloud deck. The smoke affects Earth's radiation budget by absorbing and reflecting sunlight and changing cloud properties. We investigate smoke effects on the transition between overcast and scattered clouds in regional climate and large eddy simulation models and compare our results with observations from three recent international field campaigns.
Anton Rusanen, Kristo Hõrrak, Lauri R. Ahonen, Tuomo Nieminen, Pasi P. Aalto, Pasi Kolari, Markku Kulmala, Tuukka Petäjä, and Heikki Junninen
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-67, https://doi.org/10.5194/amt-2022-67, 2022
Preprint under review for AMT
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We present a framework for setting up SMEAR (Station for Measuring Earth Surface-Atmosphere Relations) type measurement station data flows. This framework, called SMEARcore, consists of modular open-source software components that can be chosen to suit various station configurations. The benefits of using this framework are automation of routine operations, real-time monitoring of measurement results and station status.
Johannes Mikkola, Victoria Sinclair, Marja Bister, and Federico Bianchi
EGUsphere, https://doi.org/10.5194/egusphere-2022-336, https://doi.org/10.5194/egusphere-2022-336, 2022
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Local winds in four valleys located in the Nepal Himalayas are studied by means of high-resolution meteorological modelling. Well defined daytime up-valley winds are simulated in all of the valleys with some variation in the flow depth and strength between the valleys and their parts. Parts of the valleys with steep valley floor inclination (2–5 degrees) are associated with weaker and shallower daytime up-valley winds compared to the parts which have nearly flat valley floors (<1 degrees).
Irina Mironova, Miriam Sinnhuber, Galina Bazilevskaya, Mark Clilverd, Bernd Funke, Vladimir Makhmutov, Eugene Rozanov, Michelle L. Santee, Timofei Sukhodolov, and Thomas Ulich
Atmos. Chem. Phys., 22, 6703–6716, https://doi.org/10.5194/acp-22-6703-2022, https://doi.org/10.5194/acp-22-6703-2022, 2022
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From balloon measurements, we detected unprecedented, extremely powerful, electron precipitation over the middle latitudes. The robustness of this event is confirmed by satellite observations of electron fluxes and chemical composition, as well as by ground-based observations of the radio signal propagation. The applied chemistry–climate model shows the almost complete destruction of ozone in the mesosphere over the region where high-energy electrons were observed.
Marilena Teri, Thomas Müller, Josef Gasteiger, Sara Valentini, Helmuth Horvath, Roberta Vecchi, Paulus Bauer, Adrian Walser, and Bernadett Weinzierl
Atmos. Meas. Tech., 15, 3161–3187, https://doi.org/10.5194/amt-15-3161-2022, https://doi.org/10.5194/amt-15-3161-2022, 2022
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We performed an extensive closure study including laboratory and simulated experiments to evaluate various angular corrections for the Aurora 4000 polar nephelometer, focusing on irregularly shaped aerosols such as mineral dust. We describe the impact of particle size, refractive index, and shape on the determination of the particle scattering coefficient and propose a guideline to establish the most appropriate angular correction depending on the aerosol type and the investigated size range.
Maija Peltola, Clémence Rose, Jonathan V. Trueblood, Sally Gray, Mike Harvey, and Karine Sellegri
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-307, https://doi.org/10.5194/acp-2022-307, 2022
Preprint under review for ACP
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We measured the chemical composition of ambient ions at a coastal New Zealand site and connected these data with aerosol size distribution data to study the chemical precursors of new particle formation at the site. Our results showed that iodine oxides and sulfur species were important for particle formation in marine air while in land-influenced air sulfuric acid and organics were connected to new particle formation events.
Roseline C. Thakur, Lubna Dada, Lisa J. Beck, Lauriane L. J. Quéléver, Tommy Chan, Marjan Marbouti, Xu-Cheng He, Carlton Xavier, Juha Sulo, Janne Lampilahti, Markus Lampimäki, Yee Jun Tham, Nina Sarnela, Katrianne Lehtipalo, Alf Norkko, Markku Kulmala, Mikko Sipilä, and Tuija Jokinen
Atmos. Chem. Phys., 22, 6365–6391, https://doi.org/10.5194/acp-22-6365-2022, https://doi.org/10.5194/acp-22-6365-2022, 2022
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Every year intense cyanobacterial and macroalgal blooms occur in the Baltic Sea and in the coastal areas surrounding Helsinki, yet no studies have addressed the impact of biogenic emissions from these blooms on gas vapor concentrations, which in turn could influence new particle formation. This is the first study of its kind to address the chemistry driving new particle formation (NPF) during a bloom period in this region, highlighting the role of biogenic sulfuric acid and iodic acid.
Ajit Ahlawat, Kay Weinhold, Jesus Marval, Paolo Tronville, Ari Leskinen, Mika Komppula, Holger Gerwig, Lars Gerling, Stephan Weber, Rikke Bramming Jørgensen, Thomas Nørregaard Jensen, Marouane Merizak, Ulrich Vogt, Carla Ribalta, Mar Viana, Andre Schmitz, Maria Chiesa, Giacomo Gerosa, Lothar Keck, Markus Pesch, Gerhard Steiner, Thomas Krinke, Torsten Tritscher, Wolfram Birmili, and Alfred Wiedensohler
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-155, https://doi.org/10.5194/amt-2022-155, 2022
Preprint under review for AMT
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Measurements of ultrafine particles must be done with quality-assured instruments. The performance of portable instruments such as NanoScan SMPS, and GRIMM Mini WRAS spectrometer measuring the particle number size distribution in the range from 10 to 200 nm were investigated. The influence of different aerosol types and maintenance activities on these instruments were explored. The results show that these portable instruments are suitable for mobile UFP measurements for source identification.
Maija Peltola, Clémence Rose, Jonathan V. Trueblood, Sally Gray, Mike Harvey, and Karine Sellegri
Atmos. Chem. Phys., 22, 6231–6254, https://doi.org/10.5194/acp-22-6231-2022, https://doi.org/10.5194/acp-22-6231-2022, 2022
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Despite the importance of marine aerosol measurements for constraining climate models, these measurements are scarce. We measured the aerosol particle number size distribution in coastal New Zealand over a total period of 10 months. This paper analyses the aerosol properties at the site, with a special focus on new particle formation and marine air masses. New particle formation was observed frequently, but in marine air masses it did not follow traditional event criteria.
Matti Kämäräinen, Anna Lintunen, Markku Kulmala, Juha-Pekka Tuovinen, Ivan Mammarella, Juha Aalto, Henriikka Vekuri, and Annalea Lohila
Biogeosciences Discuss., https://doi.org/10.5194/bg-2022-108, https://doi.org/10.5194/bg-2022-108, 2022
Preprint under review for BG
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In this work we present an alternative machine learning approach to model the exchange of carbon between the atmosphere and the study site, located in a boreal forest in Southern Finland. The suggested method produces more accurate results than another which has been widely used previously in this context. Accurate estimations of the exchange of carbon are needed for better understanding of the role of forests in regulating atmospheric carbon and climate change.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-238, https://doi.org/10.5194/acp-2022-238, 2022
Revised manuscript under review for ACP
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.8 to 9.1E5 cm–3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Zijun Li, Angela Buchholz, Luis M. F. Barreira, Arttu Ylisirniö, Liqing Hao, Iida Pullinen, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-285, https://doi.org/10.5194/acp-2022-285, 2022
Preprint under review for ACP
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Interaction between NOx and biogenic emissions can be important in suburban areas. Our study showed that the addition of NOx during α-pinene SOA formation produced considerable amounts of organic nitrates and affected the composition of non-nitrated organic compounds. The compositional difference consequently altered the primary type of aqueous-phase processes during the isothermal particle evaporation.
Jarmo Mäkelä, Laila Melkas, Ivan Mammarella, Tuomo Nieminen, Suyog Chandramouli, Rafael Savvides, and Kai Puolamäki
Biogeosciences, 19, 2095–2099, https://doi.org/10.5194/bg-19-2095-2022, https://doi.org/10.5194/bg-19-2095-2022, 2022
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Causal structure discovery algorithms have been making headway into Earth system sciences, and they can be used to increase our understanding on biosphere–atmosphere interactions. In this paper we present a procedure on how to utilize prior knowledge of the domain experts together with these algorithms in order to find more robust causal structure models. We also demonstrate how to avoid pitfalls such as over-fitting and concept drift during this process.
Zoé Brasseur, Dimitri Castarède, Erik S. Thomson, Michael P. Adams, Saskia Drossaart van Dusseldorp, Paavo Heikkilä, Kimmo Korhonen, Janne Lampilahti, Mikhail Paramonov, Julia Schneider, Franziska Vogel, Yusheng Wu, Jonathan P. D. Abbatt, Nina S. Atanasova, Dennis H. Bamford, Barbara Bertozzi, Matthew Boyer, David Brus, Martin I. Daily, Romy Fösig, Ellen Gute, Alexander D. Harrison, Paula Hietala, Kristina Höhler, Zamin A. Kanji, Jorma Keskinen, Larissa Lacher, Markus Lampimäki, Janne Levula, Antti Manninen, Jens Nadolny, Maija Peltola, Grace C. E. Porter, Pyry Poutanen, Ulrike Proske, Tobias Schorr, Nsikanabasi Silas Umo, János Stenszky, Annele Virtanen, Dmitri Moisseev, Markku Kulmala, Benjamin J. Murray, Tuukka Petäjä, Ottmar Möhler, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 5117–5145, https://doi.org/10.5194/acp-22-5117-2022, https://doi.org/10.5194/acp-22-5117-2022, 2022
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The present measurement report introduces the ice nucleation campaign organized in Hyytiälä, Finland, in 2018 (HyICE-2018). We provide an overview of the campaign settings, and we describe the measurement infrastructure and operating procedures used. In addition, we use results from ice nucleation instrument inter-comparison to show that the suite of these instruments deployed during the campaign reports consistent results.
Meri Räty, Larisa Sogacheva, Helmi-Marja Keskinen, Veli-Matti Kerminen, Tuomo Nieminen, Tuukka Petäjä, Ekaterina Ezhova, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-264, https://doi.org/10.5194/acp-2022-264, 2022
Preprint under review for ACP
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We utilised back-trajectories to identify the source region of air masses arriving in Hyytiälä, Finland, and their travel time over forests. Combined with atmospheric observations, they revealed how air mass transport over the Fennoscandian boreal forest during the growing season produced an accumulation of cloud condensation nuclei and humidity, promoting cloudiness and precipitation. By 60 hours of transport, air masses appeared to reach a balanced state with the forest environment.
Aki Virkkula, Henrik Grythe, John Backman, Tuukka Petäjä, Maurizio Busetto, Christian Lanconelli, Angelo Lupi, Silvia Becagli, Rita Traversi, Mirko Severi, Vito Vitale, Patrick Sheridan, and Elisabeth Andrews
Atmos. Chem. Phys., 22, 5033–5069, https://doi.org/10.5194/acp-22-5033-2022, https://doi.org/10.5194/acp-22-5033-2022, 2022
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Optical properties of surface aerosols at Dome C, Antarctica, in 2007–2013 and their potential source areas are presented. The equivalent black carbon (eBC) mass concentrations were compared with eBC measured at three other Antarctic sites: the South Pole (SPO) and two coastal sites, Neumayer and Syowa. Transport analysis suggests that South American BC emissions are the largest contributor to eBC at Dome C.
Runlong Cai, Ella Häkkinen, Chao Yan, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-262, https://doi.org/10.5194/acp-2022-262, 2022
Revised manuscript accepted for ACP
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The influences of new particle formation on the climate and air quality are governed by particle survival, which has been under debate due to the uncertainties in the coagulation sink. Here we measure the coagulation coefficient of sub-10 nm particles and demonstrate that collisions between the freshly nucleated and background particles can effectively lead to coagulation. We further show that the effective coagulation sink is consistent with the new particle formation measured in urban Beijing.
Silvia Margarita Calderón, Juha Tonttila, Angela Buchholz, Jorma Joutsensaari, Mika Komppula, Ari Leskinen, Liqing Hao, Dmitri Moisseev, Iida Pullinen, Petri Tiitta, Jian Xu, Annele Virtanen, Harri Kokkola, and Sami Romakkaniemi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-273, https://doi.org/10.5194/acp-2022-273, 2022
Revised manuscript under review for ACP
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The spatial and temporal restrictions of observations, and oversimplified aerosol representation in large-eddy-simulations (LES) limit our understanding of aerosol-stratocumulus interactions. In this closure study of in situ and remote sensing observations, and outputs from UCLALES-SALSA, we have assessed the role of convective overturning and aerosol effects in two cloud events observed at the Puijo SMEAR IV station, Finland, a diurnal-high aerosol case and a nocturnal-low aerosol case.
Joel Kuula, Hilkka Timonen, Jarkko V. Niemi, Hanna E. Manninen, Topi Rönkkö, Tareq Hussein, Pak Lun Fung, Sasu Tarkoma, Mikko Laakso, Erkka Saukko, Aino Ovaska, Markku Kulmala, Ari Karppinen, Lasse Johansson, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 4801–4808, https://doi.org/10.5194/acp-22-4801-2022, https://doi.org/10.5194/acp-22-4801-2022, 2022
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Modern and up-to-date policies and air quality management strategies are instrumental in tackling global air pollution. As the European Union is preparing to revise Ambient Air Quality Directive 2008/50/EC, this paper initiates discussion on selected features of the directive that we believe would benefit from a reassessment. The scientific community has the most recent and deepest understanding of air pollution; thus, its contribution is essential.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Svetlana Sofieva, Eija Asmi, Nina S. Atanasova, Aino E. Heikkinen, Emeline Vidal, Jonathan Duplissy, Martin Romantschuk, Rostislav Kouznetsov, Jaakko Kukkonen, Dennis H. Bamford, Antti-Pekka Hyvärinen, and Mikhail Sofiev
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-117, https://doi.org/10.5194/amt-2022-117, 2022
Preprint under review for AMT
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Sea spray aerosols (SSA) emitted from ocean surface are a source of the global aerosols and significantly affect climate. A new bubble-generating glass chamber design with an extensive set of aerosol production experiments is presented to re-evaluate the SSA production as a function of water parameters: bubbling air flow, water salinity, and temperature. Our main findings suggest modest dependence of aerosol production on the water salinity and strong dependence on temperature below ~10 °C.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Lisa J. Beck, Siegfried Schobesberger, Mikko Sipilä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Meas. Tech., 15, 1957–1965, https://doi.org/10.5194/amt-15-1957-2022, https://doi.org/10.5194/amt-15-1957-2022, 2022
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Sulfuric acid is known to be a main compound in atmospheric new particle formation. Yet, its concentration is very low, which leads to challenges in detecting it. In our study, we derive the sulfuric acid concentration from measurements of ambient ions with a mass spectrometer. Our validation shows that the theoretical approach using the bisulfate ion and its clusters with H2SO4 captures the sulfuric acid concentration very well during daytime.
Loïc Gonzalez Carracedo, Katrianne Lehtipalo, Lauri R. Ahonen, Nina Sarnela, Sebastian Holm, Juha Kangasluoma, Markku Kulmala, Paul M. Winkler, and Dominik Stolzenburg
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-234, https://doi.org/10.5194/acp-2022-234, 2022
Preprint under review for ACP
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Fast nanoparticle growth is essential for the survival of new aerosol particles in the atmosphere and hence their contribution to the climate. We show that using naturally charged ions for growth calculations can cause a significant error. During the diurnal cycle, the importance of ion-induced and neutral nucleation vary, causing the ion-population to have a slower measurable apparent growth. Our results suggest that data from ion spectrometers need to be considered with great care below 3 nm.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-188, https://doi.org/10.5194/acp-2022-188, 2022
Preprint under review for ACP
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Sulphate aerosols have a strong influence on climate. Due to the reduction in sulphur-based fossil fuels, natural sulphur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulphur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Sini Isokääntä, Paul Kim, Santtu Mikkonen, Thomas Kühn, Harri Kokkola, Taina Yli-Juuti, Liine Heikkinen, Krista Luoma, Tuukka Petäjä, Zak Kipling, Daniel Partridge, and Annele Virtanen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-147, https://doi.org/10.5194/acp-2022-147, 2022
Revised manuscript accepted for ACP
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This study employs airmass history analysis and observations to investigate how clouds and precipitation affect atmospheric aerosols during their transport to a boreal forest site. The mass concentrations of studied chemical species showed exponential decrease as a function accumulated rain along the airmass route. Our analysis revealed in-cloud sulfate formation, while no major changes in organic concentrations were seen. Most of the sulfate formed were distributed to particle sizes > 200 nm.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-225, https://doi.org/10.5194/acp-2022-225, 2022
Preprint under review for ACP
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We provide the first extensive comparison of detailed aerosol size distribution trends between in-situ observations from Europe and five different earth system models. We investigated commonly used aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. This provides an important addition to earlier aerosol-cloud interaction model evaluation studies.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-78, https://doi.org/10.5194/amt-2022-78, 2022
Preprint under review for AMT
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
Marjan Marbouti, Sehyun Jang, Silvia Becagli, Gabriel Navarro, Rita Traversi, Kitack Lee, Tuomo Nieminen, Lisa J. Beck, Markku Kulmala, Veli-Matti Kerminen, and Mikko Sipilä
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-52, https://doi.org/10.5194/acp-2022-52, 2022
Preprint under review for ACP
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This research was done to understand and investigate the roles of Chl-a, PP and sea ice extent in controlling and producing the in-situ measured MSA, SA, HIO3, HOM and aerosol concentrations over the Greenland and Barents Seas. Our results provide strong support to the hypothesis that MSA, SA and small-particle concentrations in the Svalbard area are directly linked to ocean biological activity and sea ice melting during springtime.
Timo Vesala, Kukka-Maaria Kohonen, Linda M. J. Kooijmans, Arnaud P. Praplan, Lenka Foltýnová, Pasi Kolari, Markku Kulmala, Jaana Bäck, David Nelson, Dan Yakir, Mark Zahniser, and Ivan Mammarella
Atmos. Chem. Phys., 22, 2569–2584, https://doi.org/10.5194/acp-22-2569-2022, https://doi.org/10.5194/acp-22-2569-2022, 2022
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Carbonyl sulfide (COS) provides new insights into carbon cycle research. We present an easy-to-use flux parameterization and the longest existing time series of forest–atmosphere COS exchange measurements, which allow us to study both seasonal and interannual variability. We observed only uptake of COS by the forest on an annual basis, with 37 % variability between years. Upscaling the boreal COS uptake using a biosphere model indicates a significant missing COS sink at high latitudes.
Mykhailo Savenets, Larysa Pysarenko, Svitlana Krakovska, Alexander Mahura, and Tuukka Petäjä
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-103, https://doi.org/10.5194/acp-2022-103, 2022
Preprint under review for ACP
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The paper explores spatio-temporal variability of black carbon during a wildfire episode of August 2010 with focus on Ukraine. As a research tool the seamless Enviro-HIRLAM modelling system used for investigating atmospheric transport of aerosol particles emitted by wildfires from remote and local sources. Results of this study improve our understanding of physical/ chemical processes and interactions of aerosols in the atmosphere.
Tuija Jokinen, Katrianne Lehtipalo, Roseline Cutting Thakur, Ilona Ylivinkka, Kimmo Neitola, Nina Sarnela, Totti Laitinen, Markku Kulmala, Tuukka Petäjä, and Mikko Sipilä
Atmos. Chem. Phys., 22, 2237–2254, https://doi.org/10.5194/acp-22-2237-2022, https://doi.org/10.5194/acp-22-2237-2022, 2022
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New particle formation is an important source of cloud condensation nuclei; however, long-term measurements of aerosol-forming vapors are close to nonexistent in the Arctic. Here, we report 7 months of CI-APi-TOF measurements of sulfuric acid, iodic acid, methane sulfonic acid and the sum of highly oxygenated organic molecules from the SMEAR I station in the Finnish subarctic. The results help us to understand atmospheric chemical processes and aerosol formation in this rapidly changing area.
Pak Lun Fung, Martha A. Zaidan, Jarkko V. Niemi, Erkka Saukko, Hilkka Timonen, Anu Kousa, Joel Kuula, Topi Rönkkö, Ari Karppinen, Sasu Tarkoma, Markku Kulmala, Tuukka Petäjä, and Tareq Hussein
Atmos. Chem. Phys., 22, 1861–1882, https://doi.org/10.5194/acp-22-1861-2022, https://doi.org/10.5194/acp-22-1861-2022, 2022
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We developed an input-adaptive mixed-effects model, which was automatised to select the best combination of input variables, including up to three fixed effect variables and three time indictors as random effect variables. We tested the model to estimate lung-deposited surface area (LDSA), which correlates well with human health. The results show the inclusion of time indicators improved the sensitivity and the accuracy of the model so that it could serve as a network of virtual sensors.
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.
Haochi Che, Philip Stier, Duncan Watson-Parris, Hamish Gordon, and Lucia Deaconu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-43, https://doi.org/10.5194/acp-2022-43, 2022
Revised manuscript accepted for ACP
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The extensive stratocumulus clouds over the South-eastern Atlantic Ocean (SEA) can lead to a cooling effect on the climate, and a key pathway of aerosols affecting cloud properties is by acting as cloud condensation nuclei (CCN). Here we investigated the source attribution of CCN in that region, and the cloud responses. Our results show nucleation contributes most of CCN in the marine boundary layer. In terms of emissions, anthropogenic contributes most of CCN and cloud droplets numbers.
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1079, https://doi.org/10.5194/acp-2021-1079, 2022
Revised manuscript accepted for ACP
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In the urban environment, traffic emission is a major source of primary pollutants, but its contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine its relevance to NPF. Based on our comprehensive measurements, we demonstrate an insignificant role of traffic emission in NPF.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Peifeng Su, Jorma Joutsensaari, Lubna Dada, Martha Arbayani Zaidan, Tuomo Nieminen, Xinyang Li, Yusheng Wu, Stefano Decesari, Sasu Tarkoma, Tuukka Petäjä, Markku Kulmala, and Petri Pellikka
Atmos. Chem. Phys., 22, 1293–1309, https://doi.org/10.5194/acp-22-1293-2022, https://doi.org/10.5194/acp-22-1293-2022, 2022
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We regarded the banana shapes in the surface plots as a special kind of object (similar to cats) and applied an instance segmentation technique to automatically identify the new particle formation (NPF) events (especially the strongest ones), in addition to their growth rates, start times, and end times. The automatic method generalized well on datasets collected in different sites, which is useful for long-term data series analysis and obtaining statistical properties of NPF events.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Arto Heitto, Kari Lehtinen, Tuukka Petäjä, Felipe Lopez-Hilfiker, Joel A. Thornton, Markku Kulmala, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 155–171, https://doi.org/10.5194/acp-22-155-2022, https://doi.org/10.5194/acp-22-155-2022, 2022
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For atmospheric aerosol particles to take part in cloud formation, they need to be at least a few tens of nanometers in diameter. By using a particle condensation model, we investigated how two types of chemical reactions, oligomerization and decomposition, of organic molecules inside the particle may affect the growth of secondary aerosol particles to these sizes. We show that the effect is potentially significant, which highlights the importance of increasing understanding of these processes.
Sarah J. Doherty, Pablo E. Saide, Paquita Zuidema, Yohei Shinozuka, Gonzalo A. Ferrada, Hamish Gordon, Marc Mallet, Kerry Meyer, David Painemal, Steven G. Howell, Steffen Freitag, Amie Dobracki, James R. Podolske, Sharon P. Burton, Richard A. Ferrare, Calvin Howes, Pierre Nabat, Gregory R. Carmichael, Arlindo da Silva, Kristina Pistone, Ian Chang, Lan Gao, Robert Wood, and Jens Redemann
Atmos. Chem. Phys., 22, 1–46, https://doi.org/10.5194/acp-22-1-2022, https://doi.org/10.5194/acp-22-1-2022, 2022
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Between July and October, biomass burning smoke is advected over the southeastern Atlantic Ocean, leading to climate forcing. Model calculations of forcing by this plume vary significantly in both magnitude and sign. This paper compares aerosol and cloud properties observed during three NASA ORACLES field campaigns to the same in four models. It quantifies modeled biases in properties key to aerosol direct radiative forcing and evaluates how these biases propagate to biases in forcing.
Dina Alfaouri, Monica Passananti, Tommaso Zanca, Lauri Ahonen, Juha Kangasluoma, Jakub Kubečka, Nanna Myllys, and Hanna Vehkamäki
Atmos. Meas. Tech., 15, 11–19, https://doi.org/10.5194/amt-15-11-2022, https://doi.org/10.5194/amt-15-11-2022, 2022
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To study what is happening in the atmosphere, it is important to be able to measure the molecules and clusters present in it. In our work, we studied an artifact that happens inside a mass spectrometer, in particular the fragmentation of clusters. We were able to quantify the fragmentation and retrieve the correct concentration and composition of the clusters using our dual (experimental and theoretical) approach.
Lukas Fischer, Martin Breitenlechner, Eva Canaval, Wiebke Scholz, Marcus Striednig, Martin Graus, Thomas G. Karl, Tuukka Petäjä, Markku Kulmala, and Armin Hansel
Atmos. Meas. Tech., 14, 8019–8039, https://doi.org/10.5194/amt-14-8019-2021, https://doi.org/10.5194/amt-14-8019-2021, 2021
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Ecosystems emit biogenic volatile organic compounds (BVOCs), which are then oxidized in the atmosphere, contributing to ozone and secondary aerosol formation. While flux measurements of BVOCs are state of the art, flux measurements of the less volatile oxidation products are difficult to achieve due to inlet losses. Here we present first flux measurements, utilizing a novel PTR3 instrument in combination with a specially designed wall-less inlet we put on top of the Hyytiälä tower in Finland.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Zijun Li, Angela Buchholz, Arttu Ylisirniö, Luis Barreira, Liqing Hao, Siegfried Schobesberger, Taina Yli-Juuti, and Annele Virtanen
Atmos. Chem. Phys., 21, 18283–18302, https://doi.org/10.5194/acp-21-18283-2021, https://doi.org/10.5194/acp-21-18283-2021, 2021
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We compared the evolution of two types of secondary organic aerosol (SOA) particles during isothermal evaporation. The sesquiterpene SOA particles demonstrated higher resilience to evaporation than α-pinene SOA particles generated under comparable conditions. In-depth analysis showed that under high-relative-humidity conditions, particulate water drove the evolution of particulate constituents by reducing the particle viscosity and initiating chemical aqueous-phase processes.
Simon Felix Reifenberg, Anna Martin, Matthias Kohl, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna Holanda, Ovid O. Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1005, https://doi.org/10.5194/acp-2021-1005, 2021
Revised manuscript accepted for ACP
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissionsare located in the upper troposphere, around the aircraft cruise altitude, while largest absolute changes are present at the surface.
Qi En Zhong, Chunlei Cheng, Zaihua Wang, Lei Li, Mei Li, Dafeng Ge, Lei Wang, Yuanyuan Li, Wei Nie, Xuguang Chi, Aijun Ding, Suxia Yang, Duohong Chen, and Zhen Zhou
Atmos. Chem. Phys., 21, 17953–17967, https://doi.org/10.5194/acp-21-17953-2021, https://doi.org/10.5194/acp-21-17953-2021, 2021
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Particulate amines play important roles in new particle formation, aerosol acidity, and hygroscopicity. Most of the field observations did not distinguish the different behavior of each type amine under the same ambient influencing factors. In this study, two amine-containing single particles exhibited different mixing states and disparate enrichment of secondary organics, which provide insight into the discriminated fates of organics during the formation and evolution processes.
Ying Zhou, Simo Hakala, Chao Yan, Yang Gao, Xiaohong Yao, Biwu Chu, Tommy Chan, Juha Kangasluoma, Shahzad Gani, Jenni Kontkanen, Pauli Paasonen, Yongchun Liu, Tuukka Petäjä, Markku Kulmala, and Lubna Dada
Atmos. Chem. Phys., 21, 17885–17906, https://doi.org/10.5194/acp-21-17885-2021, https://doi.org/10.5194/acp-21-17885-2021, 2021
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We characterized the connection between new particle formation (NPF) events in terms of frequency, intensity and growth at a near-highway location in central Beijing and at a background mountain site 80 km away. Due to the substantial contribution of NPF to the global aerosol budget, identifying the conditions that promote the occurrence of regional NPF events could help understand their contribution on a large scale and would improve their implementation in global models.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
Ditte Taipale, Veli-Matti Kerminen, Mikael Ehn, Markku Kulmala, and Ülo Niinemets
Atmos. Chem. Phys., 21, 17389–17431, https://doi.org/10.5194/acp-21-17389-2021, https://doi.org/10.5194/acp-21-17389-2021, 2021
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Larval feeding and fungal infections of leaves can greatly change the emission of volatile compounds from plants and thereby influence aerosol processes in the air. We developed a model that considers the dynamics of larvae and fungi and the dependency of the emission on the severity of stress. We show that the infections can be highly atmospherically relevant during long periods of time and at times more important to consider than the parameters that are currently used in emission models.
Sebastian Landwehr, Michele Volpi, F. Alexander Haumann, Charlotte M. Robinson, Iris Thurnherr, Valerio Ferracci, Andrea Baccarini, Jenny Thomas, Irina Gorodetskaya, Christian Tatzelt, Silvia Henning, Rob L. Modini, Heather J. Forrer, Yajuan Lin, Nicolas Cassar, Rafel Simó, Christel Hassler, Alireza Moallemi, Sarah E. Fawcett, Neil Harris, Ruth Airs, Marzieh H. Derkani, Alberto Alberello, Alessandro Toffoli, Gang Chen, Pablo Rodríguez-Ros, Marina Zamanillo, Pau Cortés-Greus, Lei Xue, Conor G. Bolas, Katherine C. Leonard, Fernando Perez-Cruz, David Walton, and Julia Schmale
Earth Syst. Dynam., 12, 1295–1369, https://doi.org/10.5194/esd-12-1295-2021, https://doi.org/10.5194/esd-12-1295-2021, 2021
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The Antarctic Circumnavigation Expedition surveyed a large number of variables describing the dynamic state of ocean and atmosphere, freshwater cycle, atmospheric chemistry, ocean biogeochemistry, and microbiology in the Southern Ocean. To reduce the dimensionality of the dataset, we apply a sparse principal component analysis and identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and
hotspotsof interaction. Code and data are open access.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Sharmine Akter Simu, Yuzo Miyazaki, Eri Tachibana, Henning Finkenzeller, Jérôme Brioude, Aurélie Colomb, Olivier Magand, Bert Verreyken, Stephanie Evan, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 17017–17029, https://doi.org/10.5194/acp-21-17017-2021, https://doi.org/10.5194/acp-21-17017-2021, 2021
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The tropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic carbon (WSOC), which is relevant to cloud formation. Our study showed that marine secondary organic formation dominantly contributed to the aerosol WSOC mass at the high-altitude observatory in the southwest IO in the wet season in both marine boundary layer and free troposphere (FT). This suggests that the effect of marine secondary sources is important up to FT, a process missing in climate models.
Anna Franck, Dmitri Moisseev, Ville Vakkari, Matti Leskinen, Janne Lampilahti, Veli-Matti Kerminen, and Ewan O'Connor
Atmos. Meas. Tech., 14, 7341–7353, https://doi.org/10.5194/amt-14-7341-2021, https://doi.org/10.5194/amt-14-7341-2021, 2021
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We proposed a method to derive a convective boundary layer height, using insects in radar observations, and we investigated the consistency of these retrievals among different radar frequencies (5, 35 and 94 GHz). This method can be applied to radars at other measurement stations and serve as additional way to estimate the boundary layer height during summer. The entrainment zone was also observed by the 5 GHz radar above the boundary layer in the form of a Bragg scatter layer.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Diego Aliaga, Victoria A. Sinclair, Marcos Andrade, Paulo Artaxo, Samara Carbone, Evgeny Kadantsev, Paolo Laj, Alfred Wiedensohler, Radovan Krejci, and Federico Bianchi
Atmos. Chem. Phys., 21, 16453–16477, https://doi.org/10.5194/acp-21-16453-2021, https://doi.org/10.5194/acp-21-16453-2021, 2021
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We investigate the origin of air masses sampled at Mount Chacaltaya, Bolivia. Three-quarters of the measured air has not been influenced by the surface in the previous 4 d. However, it is rare that, at any given time, the sampled air has not been influenced at all by the surface, and often the sampled air has multiple origins. The influence of the surface is more prevalent during day than night. Furthermore, during the 6-month study, one-third of the air masses originated from Amazonia.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Marcel Zauner-Wieczorek, Joachim Curtius, and Andreas Kürten
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-795, https://doi.org/10.5194/acp-2021-795, 2021
Revised manuscript under review for ACP
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We reviewed different theories of the ion-ion recombination coefficient α, which describes the reaction and mutual neutralisation of two oppositely charged ions. We focussed on temperature and pressure dependencies and the atmospheric altitude range between 0 and 20 km. We compared the theories for atmospheric conditions and identified the most favourable value for standard conditions, 1.7 · 10–6 cm3 s–1, and recommend the parameterisation by Brasseur and Chatel (1983) for higher altitudes.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Shahzad Gani, Lukas Kohl, Rima Baalbaki, Federico Bianchi, Taina M. Ruuskanen, Olli-Pekka Siira, Pauli Paasonen, and Hanna Vehkamäki
Geosci. Commun., 4, 507–516, https://doi.org/10.5194/gc-4-507-2021, https://doi.org/10.5194/gc-4-507-2021, 2021
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In this article, we present authorship guidelines which also include a novel authorship form along with the documentation of the formulation process for a multidisciplinary and interdisciplinary center with more than 250 researchers. Our practical approach promotes fair authorship practices and, by focusing on clear, transparent, and timely communication, helps avoid late-stage authorship conflict.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Zhe Wang, Yee Jun Tham, Jianmin Chen, Hui Chen, Yujing Mu, Chenglong Zhang, Pengfei Liu, Likun Xue, Xinfeng Wang, Jian Gao, Hong Li, and Tao Wang
Atmos. Chem. Phys., 21, 15985–16000, https://doi.org/10.5194/acp-21-15985-2021, https://doi.org/10.5194/acp-21-15985-2021, 2021
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ClNO2 is an important precursor of chlorine radical that affects photochemistry. However, its production and impact are not well understood. Our study presents field observations of ClNO2 at three sites in northern China. These observations provide new insights into nighttime processes that produce ClNO2 and the significant impact of ClNO2 on secondary pollutions during daytime. The results improve the understanding of photochemical pollution in the lower part of the atmosphere.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Krista Luoma, Aki Virkkula, Pasi Aalto, Katrianne Lehtipalo, Tuukka Petäjä, and Markku Kulmala
Atmos. Meas. Tech., 14, 6419–6441, https://doi.org/10.5194/amt-14-6419-2021, https://doi.org/10.5194/amt-14-6419-2021, 2021
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The study presents a comparison of three absorption photometers that measured ambient aerosol particles at a boreal forest site. The study aims to better understand problems related to filter-based measurements. Results show how different correction algorithms, which are used to produce the data, affect the derived optical properties of aerosol particles.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Haoran Li, Ottmar Möhler, Tuukka Petäjä, and Dmitri Moisseev
Atmos. Chem. Phys., 21, 14671–14686, https://doi.org/10.5194/acp-21-14671-2021, https://doi.org/10.5194/acp-21-14671-2021, 2021
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In natural clouds, ice-nucleating particles are expected to be rare above –10 °C. In the current paper, we found that the formation of ice columns is frequent in stratiform clouds and is associated with increased precipitation intensity and liquid water path. In single-layer shallow clouds, the production of ice columns was attributed to secondary ice production, despite the rime-splintering process not being expected to take place in such clouds.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Maxim Philippov, Vladimir Makhmutov, Galina Bazilevskaya, Fedor Zagumennov, Vladimir Fomenko, Yuri Stozhkov, and Andrey Orlov
Geosci. Instrum. Method. Data Syst., 10, 219–226, https://doi.org/10.5194/gi-10-219-2021, https://doi.org/10.5194/gi-10-219-2021, 2021
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This paper presents a brief description of the ground-based installation for the study of cosmic rays
CARPET. Today there is a network of such installations located in different parts of the world. For ground-based installations, meteorological effects must be considered as they affect the data. This paper shows a technique for eliminating barometric and temperature dependences based on data for 2019–2020.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Helmi Uusitalo, Jenni Kontkanen, Ilona Ylivinkka, Ekaterina Ezhova, Anastasiia Demakova, Mikhail Arshinov, Boris Denisovich Belan, Denis Davydov, Nan Ma, Tuukka Petäjä, Alfred Wiedensohler, Markku Kulmala, and Tuomo Nieminen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-530, https://doi.org/10.5194/acp-2021-530, 2021
Preprint under review for ACP
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Characteristics of formation of atmospheric aerosol at four boreal forest sites in Finland and Russian Siberia was analyzed. Our results provide information on the governing processes of atmospheric aerosol formation in the boreal forest area, which a substantial part of the continental biosphere. Aerosol formation was occurring less frequently at Siberian than in Finnish sites, which was affected by the lower particle growth rates and higher loss rates in Siberia.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Nahid Atashi, Dariush Rahimi, Victoria A. Sinclair, Martha A. Zaidan, Anton Rusanen, Henri Vuollekoski, Markku Kulmala, Timo Vesala, and Tareq Hussein
Hydrol. Earth Syst. Sci., 25, 4719–4740, https://doi.org/10.5194/hess-25-4719-2021, https://doi.org/10.5194/hess-25-4719-2021, 2021
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Dew formation potential during a long-term period (1979–2018) was assessed in Iran to identify dew formation zones and to investigate the impacts of long-term variation in meteorological parameters on dew formation. Six dew formation zones were identified based on cluster analysis of the time series of the simulated dew yield. The distribution of dew formation zones in Iran was closely aligned with topography and sources of moisture. The dew formation trend was significantly negative.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
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We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Matthew Ozon, Dominik Stolzenburg, Lubna Dada, Aku Seppänen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 21, 12595–12611, https://doi.org/10.5194/acp-21-12595-2021, https://doi.org/10.5194/acp-21-12595-2021, 2021
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Measuring the rate at which aerosol particles are formed is of importance for understanding climate change. We present an analysis method based on Kalman smoothing, which retrieves new particle formation and growth rates from size-distribution measurements. We apply it to atmospheric simulation chamber experiments and show that it agrees well with traditional methods. In addition, it provides reliable uncertainty estimates, and we suggest instrument design optimisation for signal processing.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
Pak Lun Fung, Martha Arbayani Zaidan, Ola Surakhi, Sasu Tarkoma, Tuukka Petäjä, and Tareq Hussein
Atmos. Meas. Tech., 14, 5535–5554, https://doi.org/10.5194/amt-14-5535-2021, https://doi.org/10.5194/amt-14-5535-2021, 2021
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Aerosol size distribution measurements rely on a variety of techniques to classify the aerosol size and measure the size distribution. However, due to the instrumental insufficiency and inversion limitations, the raw dataset contains missing gaps or negative values, which hinder further analysis. With a merged particle size distribution in Jordan, this paper suggests a neural network method to estimate number concentrations at a particular size bin by the number concentration at other size bins.
Dimitrios Bousiotis, Francis D. Pope, David C. S. Beddows, Manuel Dall'Osto, Andreas Massling, Jakob Klenø Nøjgaard, Claus Nordstrøm, Jarkko V. Niemi, Harri Portin, Tuukka Petäjä, Noemi Perez, Andrés Alastuey, Xavier Querol, Giorgos Kouvarakis, Nikos Mihalopoulos, Stergios Vratolis, Konstantinos Eleftheriadis, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Thomas Tuch, and Roy M. Harrison
Atmos. Chem. Phys., 21, 11905–11925, https://doi.org/10.5194/acp-21-11905-2021, https://doi.org/10.5194/acp-21-11905-2021, 2021
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Formation of new particles is a key process in the atmosphere. New particle formation events arising from nucleation of gaseous precursors have been analysed in extensive datasets from 13 sites in five European countries in terms of frequency, nucleation rate, and particle growth rate, with several common features and many differences identified. Although nucleation frequencies are lower at roadside sites, nucleation rates and particle growth rates are typically higher.
Weimeng Kong, Stavros Amanatidis, Huajun Mai, Changhyuk Kim, Benjamin C. Schulze, Yuanlong Huang, Gregory S. Lewis, Susanne V. Hering, John H. Seinfeld, and Richard C. Flagan
Atmos. Meas. Tech., 14, 5429–5445, https://doi.org/10.5194/amt-14-5429-2021, https://doi.org/10.5194/amt-14-5429-2021, 2021
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We present the design, modeling, and experimental characterization of the nano-scanning electrical mobility spectrometer (nSEMS), a recently developed instrument that probes particle physical properties in the 1.5–25 nm range. The nSEMS has proven to be extremely powerful in examining atmospheric nucleation and the subsequent growth of nanoparticles in the CERN CLOUD experiment, which provides a valuable asset to study atmospheric nanoparticles and to evaluate their impact on climate.
Matti Räsänen, Mika Aurela, Ville Vakkari, Johan P. Beukes, Juha-Pekka Tuovinen, Pieter G. Van Zyl, Miroslav Josipovic, Stefan J. Siebert, Tuomas Laurila, Markku Kulmala, Lauri Laakso, Janne Rinne, Ram Oren, and Gabriel Katul
Hydrol. Earth Syst. Sci. Discuss., https://doi.org/10.5194/hess-2021-292, https://doi.org/10.5194/hess-2021-292, 2021
Revised manuscript under review for HESS
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The productivity of semi-arid grazed grasslands is linked to the variation in rainfall and transpiration. By combining carbon dioxide and water flux measurements, we show that the annual transpiration is nearly constant during wet years while grasses react quickly to dry spells and drought, which reduce transpiration. The planning of annual grazing strategies could take into account the early-season rainfall frequency that was linked to the portion of annual transpiration.
Luis M. F. Barreira, Arttu Ylisirniö, Iida Pullinen, Angela Buchholz, Zijun Li, Helina Lipp, Heikki Junninen, Urmas Hõrrak, Steffen M. Noe, Alisa Krasnova, Dmitrii Krasnov, Kaia Kask, Eero Talts, Ülo Niinemets, Jose Ruiz-Jimenez, and Siegfried Schobesberger
Atmos. Chem. Phys., 21, 11781–11800, https://doi.org/10.5194/acp-21-11781-2021, https://doi.org/10.5194/acp-21-11781-2021, 2021
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We present results from PM1 atmospheric composition and concentration measurements performed in a springtime hemiboreal forest. Sesquiterpene mixing ratios and particle-phase concentrations of corresponding oxidation products were rapidly increasing on some early mornings. The particle volatility suggested that condensable sesquiterpene oxidation products are rapidly formed in the atmosphere. The results revealed the importance of sesquiterpenes for secondary organic aerosol particulate mass.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Michael P. Adams, Nina S. Atanasova, Svetlana Sofieva, Janne Ravantti, Aino Heikkinen, Zoé Brasseur, Jonathan Duplissy, Dennis H. Bamford, and Benjamin J. Murray
Biogeosciences, 18, 4431–4444, https://doi.org/10.5194/bg-18-4431-2021, https://doi.org/10.5194/bg-18-4431-2021, 2021
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The formation of ice in clouds is critically important for the planet's climate. Hence, we need to know which aerosol types nucleate ice and how effectively they do so. Here we show that virus particles, with a range of architectures, nucleate ice when immersed in supercooled water. However, we also show that they only make a minor contribution to the ice-nucleating particle population in the terrestrial atmosphere, but we cannot rule them out as being important in the marine environment.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
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Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
Barbara Bertozzi, Robert Wagner, Junwei Song, Kristina Höhler, Joschka Pfeifer, Harald Saathoff, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 10779–10798, https://doi.org/10.5194/acp-21-10779-2021, https://doi.org/10.5194/acp-21-10779-2021, 2021
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Internally mixed particles composed of sulfate and organics are among the most abundant aerosol types. Their ice nucleation (IN) ability influences the formation of cirrus and, thus, the climate. We show that the presence of a thin organic coating suppresses the heterogeneous IN ability of crystalline ammonium sulfate particles. However, the IN ability of the same particle can substantially change if subjected to atmospheric processing, mainly due to differences in the resulting morphology.
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.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Magdalena Okuljar, Heino Kuuluvainen, Jenni Kontkanen, Olga Garmash, Miska Olin, Jarkko V. Niemi, Hilkka Timonen, Juha Kangasluoma, Yee Jun Tham, Rima Baalbaki, Mikko Sipilä, Laura Salo, Henna Lintusaari, Harri Portin, Kimmo Teinilä, Minna Aurela, Miikka Dal Maso, Topi Rönkkö, Tuukka Petäjä, and Pauli Paasonen
Atmos. Chem. Phys., 21, 9931–9953, https://doi.org/10.5194/acp-21-9931-2021, https://doi.org/10.5194/acp-21-9931-2021, 2021
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To estimate the relative contribution of different sources to the particle population in an urban environment, we conducted simultaneous measurements at a street canyon and an urban background station in Helsinki. We investigated the contribution of traffic and new particle formation to particles with a diameter between 1 and 800 nm. We found that during spring traffic does not dominate the particles smaller than 3 nm at either of the stations.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Rima Baalbaki, Michael Pikridas, Tuija Jokinen, Tiia Laurila, Lubna Dada, Spyros Bezantakos, Lauri Ahonen, Kimmo Neitola, Anne Maisser, Elie Bimenyimana, Aliki Christodoulou, Florin Unga, Chrysanthos Savvides, Katrianne Lehtipalo, Juha Kangasluoma, George Biskos, Tuukka Petäjä, Veli-Matti Kerminen, Jean Sciare, and Markku Kulmala
Atmos. Chem. Phys., 21, 9223–9251, https://doi.org/10.5194/acp-21-9223-2021, https://doi.org/10.5194/acp-21-9223-2021, 2021
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This study investigates new particle formation (NPF) in the less represented region of the Mediterranean basin using 1-year measurements of aerosol particles down to ~ 1 nm in diameter. We report a high frequency of NPF and give examples of interesting NPF features. We quantify the strength of NPF events by calculating formation rates and growth rates. We further unveil the atmospheric conditions and variables considered important for the intra-monthly and inter-monthly occurrence of NPF.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
Jose Ruiz-Jimenez, Magdalena Okuljar, Outi-Maaria Sietiö, Giorgia Demaria, Thanaporn Liangsupree, Elisa Zagatti, Juho Aalto, Kari Hartonen, Jussi Heinonsalo, Jaana Bäck, Tuukka Petäjä, and Marja-Liisa Riekkola
Atmos. Chem. Phys., 21, 8775–8790, https://doi.org/10.5194/acp-21-8775-2021, https://doi.org/10.5194/acp-21-8775-2021, 2021
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Altogether, 84 size-segregated aerosol samples from four particle size fractions were collected at the Station for Measuring Forest Ecosystem-Atmosphere Relations, Hyytiälä, Finland, in autumn 2017 for the clarification of the complex interrelationships between airborne and particulate chemical traces, amino acids and saccharides, gene copy numbers (16S and 18S for bacteria and fungi, respectively), gas-phase chemistry, and the particle size distribution.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Markku Kulmala, Tom V. Kokkonen, Juha Pekkanen, Sami Paatero, Tuukka Petäjä, Veli-Matti Kerminen, and Aijun Ding
Atmos. Chem. Phys., 21, 8313–8322, https://doi.org/10.5194/acp-21-8313-2021, https://doi.org/10.5194/acp-21-8313-2021, 2021
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The eastern part of China as a whole is practically a gigacity with 650 million inhabitants. The gigacity, with its emissions, processes in the pollution cocktail and numerous feedbacks and interactions, has a crucial and big impact on regional air quality and on global climate. A large-scale research and innovation program is needed to meet the interlinked grand challenges in this gigacity and to serve as a platform for finding pathways for sustainable development of the globe.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Janne Lampilahti, Katri Leino, Antti Manninen, Pyry Poutanen, Anna Franck, Maija Peltola, Paula Hietala, Lisa Beck, Lubna Dada, Lauriane Quéléver, Ronja Öhrnberg, Ying Zhou, Madeleine Ekblom, Ville Vakkari, Sergej Zilitinkevich, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 21, 7901–7915, https://doi.org/10.5194/acp-21-7901-2021, https://doi.org/10.5194/acp-21-7901-2021, 2021
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Using airborne measurements we observed increased number concentrations of sub-25 nm particles in the upper residual layer. These particles may be entrained into the well-mixed boundary layer and observed at the surface. We attribute our observations to new particle formation in the topmost part of the residual layer.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Benjamin Foreback, Lubna Dada, Kaspar Dällenbach, Chao Yan, Lili Wang, Biwu Chu, Ying Zhou, Tom V. Kokkonen, Mona Kurppa, Rosaria E. Pileci, Yonghong Wang, Tommy Chan, Juha Kangasluoma, Lin Zhuohui, Yishou Guo, Chang Li, Rima Baalbaki, Joni Kujansuu, Xiaolong Fan, Zemin Feng, Pekka Rantala, Shahzad Gani, Federico Bianchi, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, Yongchun Liu, and Pauli Paasonen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-192, https://doi.org/10.5194/acp-2021-192, 2021
Revised manuscript accepted for ACP
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This study analysed air quality in Beijing during the Chinese New Year over seven years, including data from a new in-depth measurement station. This is one of few studies to look at long-term impacts, including the outcome of firework restrictions starting in 2018. Results show that firework pollution has gone down since 2016, indicating a positive result from the restrictions. Results of this study may be useful in making future decisions about the use of fireworks to improve air quality.
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys., 21, 7357–7372, https://doi.org/10.5194/acp-21-7357-2021, https://doi.org/10.5194/acp-21-7357-2021, 2021
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Cyclohexene resembles certain relatively complex compounds in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOMs) formed in cyclohexene ozonolysis, the relationship between their chemical composition and their tendency to condense onto seed aerosol, as well as the effect of NOx pollutants on their signals. Two existing models were also tested for their ability to predict the volatility of the HOMs.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-379, https://doi.org/10.5194/acp-2021-379, 2021
Revised manuscript accepted for ACP
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using an oxidant found at night (NO3). The chemical composition steadily changed from its initial composition through different chemical reactions taking place inside of the aerosol. These results show the composition of organic aerosol is steadily changing during its lifetime in the atmosphere.
Yishuo Guo, Chao Yan, Chang Li, Wei Ma, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 5499–5511, https://doi.org/10.5194/acp-21-5499-2021, https://doi.org/10.5194/acp-21-5499-2021, 2021
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Fog, cloud and haze are very common natural phenomena. Sulfuric acid (SA) is one of the key compounds forming those suspended particles, technically called aerosols, through gas-to-particle conversion. Therefore, the concentration level, source and sink of SA is very important. Our results show that ozonolysis of alkenes plays a major role in nighttime SA formation under unpolluted conditions in urban Beijing, and nighttime cluster mode particles are probably driven by SA in urban environments.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev., 14, 1821–1839, https://doi.org/10.5194/gmd-14-1821-2021, https://doi.org/10.5194/gmd-14-1821-2021, 2021
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Atmospheric particle formation, emissions, and growth process rates are significant sources of uncertainty in predicting climate change. We aim to reduce that uncertainty by using measurements from several ground-based sites across Europe. We developed an estimation technique to adapt the governing process rates so model–measurement bias decays. The estimation framework developed has potential to improve model predictions while providing insight into the underlying atmospheric particle physics.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys., 21, 3899–3918, https://doi.org/10.5194/acp-21-3899-2021, https://doi.org/10.5194/acp-21-3899-2021, 2021
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By triggering the formation of ice crystals, ice-nucleating particles (INP) strongly influence cloud formation. Continuous, long-term measurements are needed to characterize the atmospheric INP variability. Here, a first long-term time series of INP spectra measured in the boreal forest for more than 1 year is presented, showing a clear seasonal cycle. It is shown that the seasonal dependency of INP concentrations and prevalent INP types is driven by the abundance of biogenic aerosol.
Naser G. A. Mahfouz and Neil M. Donahue
Atmos. Chem. Phys., 21, 3827–3832, https://doi.org/10.5194/acp-21-3827-2021, https://doi.org/10.5194/acp-21-3827-2021, 2021
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In this technical note, we show that the limit of the coagulation scavenging enhancement of charged particles is asymptotically 2; that is, at the limit, charged particles are lost at twice the rate of their neutral counterparts. This has serious implications for aerosol particle survivability where ions play a role in nucleation and growth. Such cases can happen readily in experiments and cannot be neglected in the atmosphere.
Florian Ungeheuer, Dominik van Pinxteren, and Alexander L. Vogel
Atmos. Chem. Phys., 21, 3763–3775, https://doi.org/10.5194/acp-21-3763-2021, https://doi.org/10.5194/acp-21-3763-2021, 2021
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We analysed the chemical composition of ultrafine particles from 10–56 nm near Frankfurt Airport based on cascade impactor samples. We used an offline non-target screening to determine size-resolved molecular fingerprints. Unambiguous attribution of two homologous ester series to jet engine oils enables a new strategy of source attribution and explains the majority of the detected compounds. In addition, we identified additives of jet oils and a detrimental thermal transformation product.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Dimitrios Bousiotis, James Brean, Francis D. Pope, Manuel Dall'Osto, Xavier Querol, Andrés Alastuey, Noemi Perez, Tuukka Petäjä, Andreas Massling, Jacob Klenø Nøjgaard, Claus Nordstrøm, Giorgos Kouvarakis, Stergios Vratolis, Konstantinos Eleftheriadis, Jarkko V. Niemi, Harri Portin, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Thomas Tuch, and Roy M. Harrison
Atmos. Chem. Phys., 21, 3345–3370, https://doi.org/10.5194/acp-21-3345-2021, https://doi.org/10.5194/acp-21-3345-2021, 2021
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New particle formation events from 16 sites over Europe have been studied, and the influence of meteorological and atmospheric composition variables has been investigated. Some variables, like solar radiation intensity and temperature, have a positive effect on the occurrence of these events, while others have a negative effect, affecting different aspects such as the rate at which particles are formed or grow. This effect varies depending on the site type and magnitude of these variables.
Imre Salma, Wanda Thén, Pasi Aalto, Veli-Matti Kerminen, Anikó Kern, Zoltán Barcza, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 21, 2861–2880, https://doi.org/10.5194/acp-21-2861-2021, https://doi.org/10.5194/acp-21-2861-2021, 2021
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The distribution of the monthly mean nucleation frequency possessed a characteristic pattern. Its shape was compared to those of environmental variables, including vegetation-derived properties. The spring maximum in the occurrence frequency often overlapped with the positive T anomaly. The link between the heat stress and the occurrence minimum in summer could not be proven, whereas an association between the occurrence frequency and vegetation growth dynamics was clearly identified in spring.
Rosaria E. Pileci, Robin L. Modini, Michele Bertò, Jinfeng Yuan, Joel C. Corbin, Angela Marinoni, Bas Henzing, Marcel M. Moerman, Jean P. Putaud, Gerald Spindler, Birgit Wehner, Thomas Müller, Thomas Tuch, Arianna Trentini, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Meas. Tech., 14, 1379–1403, https://doi.org/10.5194/amt-14-1379-2021, https://doi.org/10.5194/amt-14-1379-2021, 2021
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Black carbon (BC), which is an important constituent of atmospheric aerosols, remains difficult to quantify due to various limitations of available methods. This study provides an extensive comparison of co-located field measurements, applying two methods based on different principles. It was shown that both methods indeed quantify the same aerosol property – BC mass concentration. The level of agreement that can be expected was quantified, and some reasons for discrepancy were identified.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
Runlong Cai, Chenxi Li, Xu-Cheng He, Chenjuan Deng, Yiqun Lu, Rujing Yin, Chao Yan, Lin Wang, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 21, 2287–2304, https://doi.org/10.5194/acp-21-2287-2021, https://doi.org/10.5194/acp-21-2287-2021, 2021
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Growth rate determines the survival probability of atmospheric new particles and hence their impacts. We clarify the impacts of coagulation on the values retrieved by the appearance time method, which is widely used for growth rate evaluation. A new formula with coagulation correction is proposed based on derivation and tested using both models and atmospheric data. We show that the sub-3 nm particle growth rate in polluted environments may be overestimated without the coagulation correction.
Antti Ruuskanen, Sami Romakkaniemi, Harri Kokkola, Antti Arola, Santtu Mikkonen, Harri Portin, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, and Ari Leskinen
Atmos. Chem. Phys., 21, 1683–1695, https://doi.org/10.5194/acp-21-1683-2021, https://doi.org/10.5194/acp-21-1683-2021, 2021
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The study focuses mainly on cloud-scavenging efficiency of absorbing particulate matter (mainly black carbon) but additionally covers cloud-scavenging efficiency of scattering particles and statistics of cloud condensation nuclei. The main findings give insight into how black carbon is distributed in different particle sizes and the sensitivity to cloud scavenged. The main findings are useful for large-scale modelling for evaluating cloud scavenging.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943, https://doi.org/10.5194/amt-14-923-2021, https://doi.org/10.5194/amt-14-923-2021, 2021
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Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Krista Luoma, Jarkko V. Niemi, Minna Aurela, Pak Lun Fung, Aku Helin, Tareq Hussein, Leena Kangas, Anu Kousa, Topi Rönkkö, Hilkka Timonen, Aki Virkkula, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 1173–1189, https://doi.org/10.5194/acp-21-1173-2021, https://doi.org/10.5194/acp-21-1173-2021, 2021
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This study combined black carbon measurements from 15 Finnish sites that represented different environments (traffic, detached housing area, urban background, and regional background). The seasonal and diurnal variations in the black carbon concentration were associated with local emissions from traffic and residential wood burning. The study observed decreasing trends in the black carbon concentration and associated them with decreases in traffic emissions.
Jim M. Haywood, Steven J. Abel, Paul A. Barrett, Nicolas Bellouin, Alan Blyth, Keith N. Bower, Melissa Brooks, Ken Carslaw, Haochi Che, Hugh Coe, Michael I. Cotterell, Ian Crawford, Zhiqiang Cui, Nicholas Davies, Beth Dingley, Paul Field, Paola Formenti, Hamish Gordon, Martin de Graaf, Ross Herbert, Ben Johnson, Anthony C. Jones, Justin M. Langridge, Florent Malavelle, Daniel G. Partridge, Fanny Peers, Jens Redemann, Philip Stier, Kate Szpek, Jonathan W. Taylor, Duncan Watson-Parris, Robert Wood, Huihui Wu, and Paquita Zuidema
Atmos. Chem. Phys., 21, 1049–1084, https://doi.org/10.5194/acp-21-1049-2021, https://doi.org/10.5194/acp-21-1049-2021, 2021
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Every year, the seasonal cycle of biomass burning from agricultural practices in Africa creates a huge plume of smoke that travels many thousands of kilometres over the Atlantic Ocean. This study provides an overview of a measurement campaign called the cloud–aerosol–radiation interaction and forcing for year 2017 (CLARIFY-2017) and documents the rationale, deployment strategy, observations, and key results from the campaign which utilized the heavily equipped FAAM atmospheric research aircraft.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Juha Sulo, Nina Sarnela, Jenni Kontkanen, Lauri Ahonen, Pauli Paasonen, Tiia Laurila, Tuija Jokinen, Juha Kangasluoma, Heikki Junninen, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Katrianne Lehtipalo
Atmos. Chem. Phys., 21, 695–715, https://doi.org/10.5194/acp-21-695-2021, https://doi.org/10.5194/acp-21-695-2021, 2021
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In this study, we analyzed over 5 years of sub-3 nm particle concentrations and their precursor vapors, identifying atmoshperic vapors important to the formation of these particles in the boreal forest. We also observed seasonal differences in both particle and precursor vapor concentrations and the formation pathways of these particles. Our results confirm the importance of organic vapors in atmospheric aerosol formation and highlight key seasonal differences that require further study.
Jinfeng Yuan, Robin Lewis Modini, Marco Zanatta, Andreas B. Herber, Thomas Müller, Birgit Wehner, Laurent Poulain, Thomas Tuch, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 21, 635–655, https://doi.org/10.5194/acp-21-635-2021, https://doi.org/10.5194/acp-21-635-2021, 2021
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Black carbon (BC) aerosols contribute substantially to climate warming due to their unique light absorption capabilities. We performed field measurements at a central European background site in winter and found that variability in the absorption efficiency of BC particles is driven mainly by their internal mixing state. Our results suggest that, at this site, knowing the BC mixing state is sufficient to describe BC light absorption enhancements due to the lensing effect in good approximation.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Oleg Sizov, Ekaterina Ezhova, Petr Tsymbarovich, Andrey Soromotin, Nikolay Prihod'ko, Tuukka Petäjä, Sergej Zilitinkevich, Markku Kulmala, Jaana Bäck, and Kajar Köster
Biogeosciences, 18, 207–228, https://doi.org/10.5194/bg-18-207-2021, https://doi.org/10.5194/bg-18-207-2021, 2021
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In changing climate, tundra is expected to turn into shrubs and trees, diminishing reindeer pasture and increasing risks of tick-borne diseases. However, this transition may require a disturbance. Fires in Siberia are increasingly widespread. We studied wildfire dynamics and tundra–forest transition over 60 years in northwest Siberia near the Arctic Circle. Based on satellite data analysis, we found that transition occurs in 40 %–85 % of burned tundra compared to 5 %–15 % in non-disturbed areas.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Haochi Che, Philip Stier, Hamish Gordon, Duncan Watson-Parris, and Lucia Deaconu
Atmos. Chem. Phys., 21, 17–33, https://doi.org/10.5194/acp-21-17-2021, https://doi.org/10.5194/acp-21-17-2021, 2021
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The south-eastern Atlantic is semi-permanently covered by some of the largest stratocumulus clouds and is influenced by one-third of the biomass burning emissions from African fires. A UKEMS1 model simulation shows that the absorption effect of biomass burning aerosols is the most significant on clouds and radiation. The dominate cooling and rapid adjustments induced by the radiative effects of biomass burning aerosols result in an overall cooling in the south-eastern Atlantic.
André Welti, Kimmo Korhonen, Pasi Miettinen, Ana A. Piedehierro, Yrjö Viisanen, Annele Virtanen, and Ari Laaksonen
Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, https://doi.org/10.5194/amt-13-7059-2020, 2020
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We describe a modification of the SPectrometer for Ice Nuclei (SPIN) chamber to study ice nucleation at low temperatures, relevant for ice formation in cirrus clouds. Validation experiments of homogeneous freezing of aqueous ammonium sulfate droplets and heterogeneous ice nucleation on silver iodide particles are included to demonstrate the advantages of the modified SPIN chamber for the investigation of ice nucleation in the extended temperature range.
Jann Schrod, Erik S. Thomson, Daniel Weber, Jens Kossmann, Christopher Pöhlker, Jorge Saturno, Florian Ditas, Paulo Artaxo, Valérie Clouard, Jean-Marie Saurel, Martin Ebert, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 20, 15983–16006, https://doi.org/10.5194/acp-20-15983-2020, https://doi.org/10.5194/acp-20-15983-2020, 2020
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Long-term ice-nucleating particle (INP) data are presented from four semi-pristine sites located in the Amazon, the Caribbean, Germany and the Arctic. Average INP concentrations did not differ by orders of magnitude between the sites. For all sites short-term variability dominated the time series, which lacked clear trends and seasonalities. Common drivers to explain the INP levels and their variations could not be identified, illustrating the complex nature of heterogeneous ice nucleation.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
Helmi-Marja Keskinen, Ilona Ylivinkka, Liine Heikkinen, Pasi P. Aalto, Tuomo Nieminen, Katrianne Lehtipalo, Juho Aalto, Janne Levula, Jutta Kesti, Lauri R. Ahonen, Ekaterina Ezhova, Markku Kulmala, and Tuukka Petäjä
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-447, https://doi.org/10.5194/amt-2020-447, 2020
Publication in AMT not foreseen
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Long-term (2005–2017) aerosol particulate matter (PM) concentration measurements at Finland at Station for Measuring Ecosystem-Atmosphere Relations (SMEAR II, Hyytiälä) have been measured with three different measurement equipment. The comparison revealed an equivalence among the three methods. Mass concentrations were generally highest in summer. The descending trend was visible here in spring, summer and winter. This might have resulted at least partly from air quality legislation.
Bert Verreyken, Crist Amelynck, Jérôme Brioude, Jean-François Müller, Niels Schoon, Nicolas Kumps, Aurélie Colomb, Jean-Marc Metzger, Christopher F. Lee, Theodore K. Koenig, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 20, 14821–14845, https://doi.org/10.5194/acp-20-14821-2020, https://doi.org/10.5194/acp-20-14821-2020, 2020
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Biomass burning (BB) plumes arriving at the Maïdo observatory located in the south-west Indian Ocean during August 2018 and August 2019 are studied using trace gas measurements, Lagrangian transport models and the CAMS near-real-time atmospheric composition service. We investigate (i) secondary production of volatile organic compounds during transport, (ii) efficacy of the CAMS model to reproduce the chemical makeup of BB plumes and (iii) the impact of BB on the remote marine boundary layer.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Juan Andrés Casquero-Vera, Hassan Lyamani, Lubna Dada, Simo Hakala, Pauli Paasonen, Roberto Román, Roberto Fraile, Tuukka Petäjä, Francisco José Olmo-Reyes, and Lucas Alados-Arboledas
Atmos. Chem. Phys., 20, 14253–14271, https://doi.org/10.5194/acp-20-14253-2020, https://doi.org/10.5194/acp-20-14253-2020, 2020
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New particle formation was investigated at two stations located close to each other but at different altitudes: urban and high-altitude sites. Results show that sulfuric acid is able to explain a minimal fraction contribution to the observed growth rates and point to the availability of volatile organic compounds as the main factor controlling NPF events at both sites. A closer analysis of the NPF events that were observed at high-altitude sites during a Saharan dust episode was carried out.
Christian Tauber, David Schmoll, Johannes Gruenwald, Sophia Brilke, Peter Josef Wlasits, Paul Martin Winkler, and Daniela Wimmer
Atmos. Meas. Tech., 13, 5993–6006, https://doi.org/10.5194/amt-13-5993-2020, https://doi.org/10.5194/amt-13-5993-2020, 2020
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In this paper we show that a commercially available plasma charger with nitrogen as the working gas can enhance the charging probability for sub-12 nm particles. In addition, the charger ion mobilities and the chemical composition have been examined using an atmospheric pressure interface time-of-flight mass spectrometer (APi-TOF MS), and comparison of the experimental results revealed that the generated neutralizer ions are not dependent on the charging mechanism.
Yongchun Liu, Yusheng Zhang, Chaofan Lian, Chao Yan, Zeming Feng, Feixue Zheng, Xiaolong Fan, Yan Chen, Weigang Wang, Biwu Chu, Yonghong Wang, Jing Cai, Wei Du, Kaspar R. Daellenbach, Juha Kangasluoma, Federico Bianchi, Joni Kujansuu, Tuukka Petäjä, Xuefei Wang, Bo Hu, Yuesi Wang, Maofa Ge, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 20, 13023–13040, https://doi.org/10.5194/acp-20-13023-2020, https://doi.org/10.5194/acp-20-13023-2020, 2020
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Understanding of the chemical and physical processes leading to atmospheric aerosol particle formation is crucial to devising effective mitigation strategies to protect the public and reduce uncertainties in climate predictions. We found that the photolysis of nitrous acid could promote the formation of organic and nitrate aerosol and that traffic-related emission is a major contributor to ambient nitrous acid on haze days in wintertime in Beijing.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Jann Schrod, Dominik Kleinhenz, Maria Hörhold, Tobias Erhardt, Sarah Richter, Frank Wilhelms, Hubertus Fischer, Martin Ebert, Birthe Twarloh, Damiano Della Lunga, Camilla M. Jensen, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 20, 12459–12482, https://doi.org/10.5194/acp-20-12459-2020, https://doi.org/10.5194/acp-20-12459-2020, 2020
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Ice-nucleating particle (INP) concentrations of the last 6 centuries are presented from an ice core in Greenland. The data are accompanied by physical and chemical aerosol data. INPs are correlated to the dust signal from the ice core and seem to follow the annual input of mineral dust. We find no clear trend in the INP concentration. However, modern-day concentrations are higher and more variable than the concentrations of the past. This might have significant atmospheric implications.
Ilona Ylivinkka, Santeri Kaupinmäki, Meri Virman, Maija Peltola, Ditte Taipale, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Ekaterina Ezhova
Atmos. Meas. Tech., 13, 5595–5619, https://doi.org/10.5194/amt-13-5595-2020, https://doi.org/10.5194/amt-13-5595-2020, 2020
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In this study, we developed a new algorithm for cloud classification using solar radiation and cloud base height measurements. Our objective was to develop a simple and inexpensive but effective algorithm for the needs of studies related to ecosystem and atmosphere interactions. In the present study, we used the algorithm for obtaining cloud statistics at a measurement station in southern Finland, and we discuss the advantages and shortcomings of the algorithm.
Janne Lampilahti, Hanna Elina Manninen, Katri Leino, Riikka Väänänen, Antti Manninen, Stephany Buenrostro Mazon, Tuomo Nieminen, Matti Leskinen, Joonas Enroth, Marja Bister, Sergej Zilitinkevich, Juha Kangasluoma, Heikki Järvinen, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 20, 11841–11854, https://doi.org/10.5194/acp-20-11841-2020, https://doi.org/10.5194/acp-20-11841-2020, 2020
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In this work, by using co-located airborne and ground-based measurements, we show that counter-rotating horizontal circulations in the planetary boundary layer (roll vortices) frequently enhance regional new particle formation or induce localized bursts of new particle formation. These observations can be explained by the ability of the rolls to efficiently lift low-volatile vapors emitted from the surface to the top of the boundary layer where new particle formation is more favorable.
Lubna Dada, Ilona Ylivinkka, Rima Baalbaki, Chang Li, Yishuo Guo, Chao Yan, Lei Yao, Nina Sarnela, Tuija Jokinen, Kaspar R. Daellenbach, Rujing Yin, Chenjuan Deng, Biwu Chu, Tuomo Nieminen, Yonghong Wang, Zhuohui Lin, Roseline C. Thakur, Jenni Kontkanen, Dominik Stolzenburg, Mikko Sipilä, Tareq Hussein, Pauli Paasonen, Federico Bianchi, Imre Salma, Tamás Weidinger, Michael Pikridas, Jean Sciare, Jingkun Jiang, Yongchun Liu, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 20, 11747–11766, https://doi.org/10.5194/acp-20-11747-2020, https://doi.org/10.5194/acp-20-11747-2020, 2020
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We rely on sulfuric acid measurements in four contrasting environments, Hyytiälä, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment, and heavily polluted megacity, respectively, in order to define the sources and sinks of sulfuric acid in these environments and to derive a new sulfuric acid proxy to be utilized in locations and during periods when it is not measured.
Yohei Shinozuka, Pablo E. Saide, Gonzalo A. Ferrada, Sharon P. Burton, Richard Ferrare, Sarah J. Doherty, Hamish Gordon, Karla Longo, Marc Mallet, Yan Feng, Qiaoqiao Wang, Yafang Cheng, Amie Dobracki, Steffen Freitag, Steven G. Howell, Samuel LeBlanc, Connor Flynn, Michal Segal-Rosenhaimer, Kristina Pistone, James R. Podolske, Eric J. Stith, Joseph Ryan Bennett, Gregory R. Carmichael, Arlindo da Silva, Ravi Govindaraju, Ruby Leung, Yang Zhang, Leonhard Pfister, Ju-Mee Ryoo, Jens Redemann, Robert Wood, and Paquita Zuidema
Atmos. Chem. Phys., 20, 11491–11526, https://doi.org/10.5194/acp-20-11491-2020, https://doi.org/10.5194/acp-20-11491-2020, 2020
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In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
Jenni Kontkanen, Chenjuan Deng, Yueyun Fu, Lubna Dada, Ying Zhou, Jing Cai, Kaspar R. Daellenbach, Simo Hakala, Tom V. Kokkonen, Zhuohui Lin, Yongchun Liu, Yonghong Wang, Chao Yan, Tuukka Petäjä, Jingkun Jiang, Markku Kulmala, and Pauli Paasonen
Atmos. Chem. Phys., 20, 11329–11348, https://doi.org/10.5194/acp-20-11329-2020, https://doi.org/10.5194/acp-20-11329-2020, 2020
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To estimate the impacts of atmospheric aerosol particles on air quality, knowledge of size distributions of particles emitted from anthropogenic sources is needed. We introduce a new method for determining size-resolved particle number emissions from measured particle size distributions. We apply our method to data measured in Beijing, China. We find that particle number emissions at our site are dominated by emissions of particles smaller than 30 nm, originating mainly from traffic.
Yang Wang, Arnoud Apituley, Alkiviadis Bais, Steffen Beirle, Nuria Benavent, Alexander Borovski, Ilya Bruchkouski, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Henning Finkenzeller, Martina M. Friedrich, Udo Frieß, David Garcia-Nieto, Laura Gómez-Martín, François Hendrick, Andreas Hilboll, Junli Jin, Paul Johnston, Theodore K. Koenig, Karin Kreher, Vinod Kumar, Aleksandra Kyuberis, Johannes Lampel, Cheng Liu, Haoran Liu, Jianzhong Ma, Oleg L. Polyansky, Oleg Postylyakov, Richard Querel, Alfonso Saiz-Lopez, Stefan Schmitt, Xin Tian, Jan-Lukas Tirpitz, Michel Van Roozendael, Rainer Volkamer, Zhuoru Wang, Pinhua Xie, Chengzhi Xing, Jin Xu, Margarita Yela, Chengxin Zhang, and Thomas Wagner
Atmos. Meas. Tech., 13, 5087–5116, https://doi.org/10.5194/amt-13-5087-2020, https://doi.org/10.5194/amt-13-5087-2020, 2020
Hamish Gordon, Paul R. Field, Steven J. Abel, Paul Barrett, Keith Bower, Ian Crawford, Zhiqiang Cui, Daniel P. Grosvenor, Adrian A. Hill, Jonathan Taylor, Jonathan Wilkinson, Huihui Wu, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10997–11024, https://doi.org/10.5194/acp-20-10997-2020, https://doi.org/10.5194/acp-20-10997-2020, 2020
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The Met Office's Unified Model is widely used both for weather forecasting and climate prediction. We present the first version of the model in which both aerosol and cloud particle mass and number concentrations are allowed to evolve separately and independently, which is important for studying how aerosols affect weather and climate. We test the model against aircraft observations near Ascension Island in the Atlantic, focusing on how aerosols can "activate" to become cloud droplets.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
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Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Tommy Chan, Runlong Cai, Lauri R. Ahonen, Yiliang Liu, Ying Zhou, Joonas Vanhanen, Lubna Dada, Yan Chao, Yongchun Liu, Lin Wang, Markku Kulmala, and Juha Kangasluoma
Atmos. Meas. Tech., 13, 4885–4898, https://doi.org/10.5194/amt-13-4885-2020, https://doi.org/10.5194/amt-13-4885-2020, 2020
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Using a particle size magnifier (PSM; Airmodus, Finland), we determined the particle size distribution using four inversion methods and compared each method to the others to establish their strengths and weaknesses. Furthermore, we provided a step-by-step procedure on how to invert measured data using the PSM. Finally, we provided recommendations, code and data related to the data inversion. This is an important paper, as no operating procedure exists regarding how to process measured PSM data.
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
Leighton A. Regayre, Julia Schmale, Jill S. Johnson, Christian Tatzelt, Andrea Baccarini, Silvia Henning, Masaru Yoshioka, Frank Stratmann, Martin Gysel-Beer, Daniel P. Grosvenor, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10063–10072, https://doi.org/10.5194/acp-20-10063-2020, https://doi.org/10.5194/acp-20-10063-2020, 2020
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The amount of energy reflected back into space because of man-made particles is highly uncertain. Processes related to naturally occurring particles cause most of the uncertainty, but these processes are poorly constrained by present-day measurements. We show that measurements over the Southern Ocean, far from pollution sources, efficiently reduce climate model uncertainties. Our results pave the way to designing experiments and measurement campaigns that reduce this uncertainty even further.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Liwei Wang, Jay G. Slowik, Nidhi Tripathi, Deepika Bhattu, Pragati Rai, Varun Kumar, Pawan Vats, Rangu Satish, Urs Baltensperger, Dilip Ganguly, Neeraj Rastogi, Lokesh K. Sahu, Sachchida N. Tripathi, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 9753–9770, https://doi.org/10.5194/acp-20-9753-2020, https://doi.org/10.5194/acp-20-9753-2020, 2020
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.