Articles | Volume 20, issue 12
Atmos. Chem. Phys., 20, 7359–7372, 2020
https://doi.org/10.5194/acp-20-7359-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue: The CERN CLOUD experiment (ACP/AMT inter-journal SI)
Atmos. Chem. Phys., 20, 7359–7372, 2020
https://doi.org/10.5194/acp-20-7359-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 25 Jun 2020
Research article | 25 Jun 2020
Enhanced growth rate of atmospheric particles from sulfuric acid
Dominik Stolzenburg et al.
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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.
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.
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. Discuss., https://doi.org/10.5194/acp-2021-512, https://doi.org/10.5194/acp-2021-512, 2021
Revised manuscript accepted for ACP
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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 °C and −50 °C). We measured particle and gas phase and found that most of the compounds that are 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 °C, 20 % RH.
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.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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.
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.
Peter Josef Wlasits, Dominik Stolzenburg, Christian Tauber, Sophia Brilke, Sebastian Harald Schmitt, Paul Martin Winkler, and Daniela Wimmer
Atmos. Meas. Tech., 13, 3787–3798, https://doi.org/10.5194/amt-13-3787-2020, https://doi.org/10.5194/amt-13-3787-2020, 2020
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In this paper we show that chemical similarities between the seed particle material and the working fluid have an impact on the detection efficiency of commonly used CPCs. A remarkable set of CPCs, including the newly developed V-WCPC 3789, was tested. Among others, reproducibly generated organic seeds based on beta-caryophyllene were used. Theoretical simulations of supersaturation profiles were successfully linked to measured data.
Lukas Pichelstorfer, Dominik Stolzenburg, John Ortega, Thomas Karl, Harri Kokkola, Anton Laakso, Kari E. J. Lehtinen, James N. Smith, Peter H. McMurry, and Paul M. Winkler
Atmos. Chem. Phys., 18, 1307–1323, https://doi.org/10.5194/acp-18-1307-2018, https://doi.org/10.5194/acp-18-1307-2018, 2018
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Quantification of new particle formation as a source of atmospheric aerosol is clearly of importance for climate and health aspects. In our new study we developed two analysis methods that allow retrieval of nanoparticle growth dynamics at much higher precision than it was possible so far. Our results clearly demonstrate that growth rates show much more variation than is currently known and suggest that the Kelvin effect governs growth in the sub-10 nm size range.
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
Dominik Stolzenburg, Gerhard Steiner, and Paul M. Winkler
Atmos. Meas. Tech., 10, 1639–1651, https://doi.org/10.5194/amt-10-1639-2017, https://doi.org/10.5194/amt-10-1639-2017, 2017
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Aerosol particles produced by gas-to-particle conversion in the atmosphere might influence the climate due to their effects on cloud formation. Characterizing the early growth of newly formed particles is extremely challenging. We present the development and characterization of an instrument that measures the evolution of particles smaller than 10 nm with high time resolution and/or high sensitivity to low concentrations. It can help quantify the characteristics of early nanoparticle growth.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Joel Kuula, Hilkka Timonen, Jarkko V. Niemi, Hanna Manninen, Topi Rönkkö, Tareq Hussein, Pak Lung Fung, Sasu Tarkoma, Mikko Laakso, Erkka Saukko, Aino Ovaska, Markku Kulmala, Ari Karppinen, Lasse Johansson, and Tuukka Petäjä
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-854, https://doi.org/10.5194/acp-2021-854, 2021
Preprint under review for ACP
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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 the Ambient Air Quality Directive (2008/50/EC) this manuscript initiates discussion on selected features of the directive that we believe would benefit from a reassessment. Scientific community has the most recent and deepest understanding of air pollution and thus its contribution is essential.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
Heather Guy, Ian M. Brooks, Ken S. Carslaw, Benjamin J. Murray, Von P. Walden, Matthew D. Shupe, Claire Pettersen, David D. Turner, Christopher J. Cox, William D. Neff, Ralf Bennartz, and Ryan R. Neely III
Atmos. Chem. Phys., 21, 15351–15374, https://doi.org/10.5194/acp-21-15351-2021, https://doi.org/10.5194/acp-21-15351-2021, 2021
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We present the first full year of surface aerosol number concentration measurements from the central Greenland Ice Sheet. Aerosol concentrations here have a distinct seasonal cycle from those at lower-altitude Arctic sites, which is driven by large-scale atmospheric circulation. Our results can be used to help understand the role aerosols might play in Greenland surface melt through the modification of cloud properties. This is crucial in a rapidly changing region where observations are sparse.
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.
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. Abbat, 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. Discuss., https://doi.org/10.5194/acp-2021-744, https://doi.org/10.5194/acp-2021-744, 2021
Preprint under review for ACP
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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 infrastructures 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.
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.
Roseline Cutting 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. Discuss., https://doi.org/10.5194/acp-2021-729, https://doi.org/10.5194/acp-2021-729, 2021
Preprint under review for ACP
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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 address the impact of biogenic emissions from these blooms on the gas-vapor concentrations, which in turn could influence new particle formations. This is the first of its kind study, which addresses the chemistry driving the new particle formations (NPF) during a bloom period in this region, highlighting the role of biogenic sulphuric acid and iodic acid.
Irina Mironova, Miriam Sinnhuber, Galina Bazilevskaya, Mark Clilverd, Bernd Funke, Vladimir Makhmutov, Eugene Rozanov, Michelle L. Santee, and Timofei Sukhodolov
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-737, https://doi.org/10.5194/acp-2021-737, 2021
Preprint under review for ACP
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From the 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.
Andrea Pozzer, Simon Reifenberg, Vinod Kumar, Bruno Franco, Domenico Taraborrelli, Sergy Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-295, https://doi.org/10.5194/gmd-2021-295, 2021
Preprint under review for GMD
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A newly developed set-up of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is here evaluated; a comprehensive organic degradation mechanism is used and coupled with a volatility base model. The results show that the model is reproducing most of the tracer and aerosols satisfactorily, although with discrepancies for oxygenated organic gases and that this model configuration can be used for further research in atmospheric chemistry.
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 %.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-775, https://doi.org/10.5194/acp-2021-775, 2021
Preprint under review for ACP
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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, while the smallest molecules detected in our experiment were likely products of thermal decomposition.
Lisa Johanna Beck, Siegfried Schobesberger, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-259, https://doi.org/10.5194/amt-2021-259, 2021
Preprint under review for AMT
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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 when detecting it. In our study, we derive the sulfuric acid concentration based on 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.
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. Discuss., https://doi.org/10.5194/acp-2021-735, https://doi.org/10.5194/acp-2021-735, 2021
Preprint under review for ACP
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New particle formation is an important source of cloud condensation nuclei (CCN) and in the arctic, cloud formation is very sensitive to the availability of CCN. Field observations from the are are scarce and long term measurements close to non-existent. In here we report 7 months of CI-APi-TOF measurements of sulfuric acid, iodic acid, MSA and HOM from the Finnish sub-Arctic. The results help us to understand atmospheric chemical processes and aerosol formation in the rapidly changing Arctic.
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. Discuss., https://doi.org/10.5194/acp-2021-771, https://doi.org/10.5194/acp-2021-771, 2021
Preprint under review for ACP
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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.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-694, https://doi.org/10.5194/acp-2021-694, 2021
Preprint under review for ACP
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the earth’s atmosphere including the budget of HOx and the abundance of tropospheric O3. This research presents photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via oxidation of only four VOC precursors, which are CH4, CH3CHO, C5H8 and CH3OH, can well balance the observed loss at all sites.
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.
Jarmo Mäkelä, Laila Melkas, Ivan Mammarella, Tuomo Nieminen, Suyog Chandramouli, Rafael Savvides, and Kai Puolamäki
Biogeosciences Discuss., https://doi.org/10.5194/bg-2021-231, https://doi.org/10.5194/bg-2021-231, 2021
Preprint under review for BG
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Causal structure discovery algorithms have been making headway into Earth system sciences and they can be used to e.g. increase our understanding on biosphere-atmosphere interactions. In this paper we present a procedure on how to utilise 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 such pitfalls as overfitting and concept drift during this process.
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. Discuss., https://doi.org/10.5194/acp-2021-700, https://doi.org/10.5194/acp-2021-700, 2021
Preprint under review for ACP
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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.
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.
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. Discuss., https://doi.org/10.5194/acp-2021-672, https://doi.org/10.5194/acp-2021-672, 2021
Preprint under review for ACP
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. High CHOCHO concentrations were observed over highly populated cities and industrial areas. Aromatics were the most important precursors of CHOCHO production. Loss path to aerosol was the highest sink contributing to ~20 % of SOA formation. CHOCHO uptake rate can be affected by aerosol viscosity and irradiation. Finally, our work highlights the lacking knowledge to explain the CHOCHO solubility.
Timo Vesala, Kukka-Maaria Kohonen, Arnaud P. Praplan, Linda M. J. Kooijmans, Lenka Foltýnová, Pasi Kolari, Markku Kulmala, Jaana Bäck, David Nelson, Dan Yakir, Mark Zahniser, and Ivan Mammarella
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-721, https://doi.org/10.5194/acp-2021-721, 2021
Preprint under review for ACP
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Carbonyl sulfide (COS) provides new insights into carbon cycle research and impacts the climate. We present an easy-to-use flux parameterization and the longest forest-atmosphere COS exchange measurements, allowing to study both seasonal and interannual variability. We observed only uptake of COS by the forest on annual basis, with 37 % variability between years. Upscaling the boreal COS uptake by a biosphere model indicates a significant missing COS sink at high latitudes.
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.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2021-246, https://doi.org/10.5194/essd-2021-246, 2021
Preprint under review for ESSD
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We present a global airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006-2016 in the UTLS. The Copernicus CAMS-GLOB ethane emission inventory coupled with atmospheric model EMAC was optimized by the observational data with 12 ethane sectoral emission sources distinguished. The global ethane emission budget is estimated to be 19.28 Tg/yr for 2006–2016.
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.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Yuqin Liu, Tao Lin, Juan Hong, Yonghong Wang, Lamei Shi, Yiyi Huang, Xian Wu, Hao Zhou, Jiahua Zhang, and Gerrit de Leeuw
Atmos. Chem. Phys., 21, 12331–12358, https://doi.org/10.5194/acp-21-12331-2021, https://doi.org/10.5194/acp-21-12331-2021, 2021
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The four-dimensional variation of aerosol properties over the BTH, YRD and PRD (east China) were investigated using satellite observations from 2007 to 2020. Distinct differences between the aerosol optical depth and vertical distribution of the occurrence of aerosol types over these regions depend on season, aerosol loading and meteorological conditions. Day–night differences between the vertical distribution of aerosol types suggest effects of boundary layer dynamics and aerosol transport.
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.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-654, https://doi.org/10.5194/acp-2021-654, 2021
Preprint under review for ACP
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This paper presents model simulations of stratospheric aerosols with a focus on explosive volcanic eruptions. Using occulation and limb-based satellite instruments with vertical profiles of sulfur dioxide and aerosol extinction, we characterised the influence of volcanic aerosols for the period between 1990–2019. We established a volcanic sulfur emission inventory that includes more than 500 eruptions. Our results show that also smaller eruptions can contribute to the stratospheric aerosol layer.
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.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
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
Preprint 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.
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. Discuss., https://doi.org/10.5194/acp-2021-562, https://doi.org/10.5194/acp-2021-562, 2021
Preprint under review for ACP
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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.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea 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. Discuss., https://doi.org/10.5194/amt-2021-223, https://doi.org/10.5194/amt-2021-223, 2021
Preprint under review for AMT
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Satellite-derived NOx emissions from biomass burning are derived 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.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
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.
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. Discuss., https://doi.org/10.5194/acp-2021-593, https://doi.org/10.5194/acp-2021-593, 2021
Revised manuscript under review for ACP
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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 insights into the discriminated fates of organics during the formation and evolution processes.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-186, https://doi.org/10.5194/amt-2021-186, 2021
Preprint under review for AMT
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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 has 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.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
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.
Arto Heitto, Kari Lehtinen, Tuukka Petäjä, Felipe Lopez-Hilfiker, Joel A. Thornton, Markku Kulmala, and Taina Yli-Juuti
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-571, https://doi.org/10.5194/acp-2021-571, 2021
Preprint under review for ACP
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When organic molecules condense on atmospheric nano-sized particles, they can combine forming larger molecules (oligomerization) or fragment to smaller molecules (decomposition). We investigated the effects of these reactions with particle growth model MODNAG and found out that they have potential to significantly affect the growth of atmospheric aerosol particles. These reactions are often excluded from growth models and it is important to increase our understanding of them.
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.
Ramiro Checa-Garcia, Yves Balkanski, Samuel Albani, Tommi Bergman, Ken Carslaw, Anne Cozic, Chris Dearden, Beatrice Marticorena, Martine Michou, Twan van Noije, Pierre Nabat, Fiona M. O'Connor, Dirk Olivié, Joseph M. Prospero, Philippe Le Sager, Michael Schulz, and Catherine Scott
Atmos. Chem. Phys., 21, 10295–10335, https://doi.org/10.5194/acp-21-10295-2021, https://doi.org/10.5194/acp-21-10295-2021, 2021
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Thousands of tons of dust are emitted into the atmosphere every year, producing important impacts on the Earth system. However, current global climate models are not yet able to reproduce dust emissions, transport and depositions with the desirable accuracy. Our study analyses five different Earth system models to report aspects to be improved to reproduce better available observations, increase the consistency between models and therefore decrease the current uncertainties.
Shahzad Gani, Lukas Kohl, Rima Baalbaki, Federico Bianchi, Taina M. Ruuskanen, Olli-Pekka Siira, Pauli Paasonen, and Hanna Vehkamäki
Geosci. Commun. Discuss., https://doi.org/10.5194/gc-2021-20, https://doi.org/10.5194/gc-2021-20, 2021
Revised manuscript accepted for GC
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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.
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. Discuss., https://doi.org/10.5194/acp-2021-512, https://doi.org/10.5194/acp-2021-512, 2021
Revised manuscript accepted for ACP
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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 °C and −50 °C). We measured particle and gas phase and found that most of the compounds that are 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 °C, 20 % RH.
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.
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. Discuss., https://doi.org/10.5194/acp-2021-427, https://doi.org/10.5194/acp-2021-427, 2021
Preprint under review for ACP
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We develop an input-adaptive mixed effects model, which is 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 test the model to estimate lung deposited surface area (LDSA), which correlates well with human’s health. The results show the inclusion of time indicators improves the sensitivity and the accuracy of the model so that it could serve as a network of virtual sensors.
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.
Rachel E. Hawker, Annette K. Miltenberger, Jill S. Johnson, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Paul R. Field, Benjamin J. Murray, and Ken S. Carslaw
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-513, https://doi.org/10.5194/acp-2021-513, 2021
Revised manuscript under review for ACP
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Convectively generated anvil cirrus can have large effects on the global radiation budget. We find that ice-nucleating particles (INP), aerosols that can initiate the freezing of cloud droplets, can cause substantial changes to the properties of convective anvils. The number and source of INP were important for the anvil properties indicating that we need INP measurements covering a large temperature range, and that climate models should represent the interaction of INP with cloud glaciation.
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.
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. Discuss., https://doi.org/10.5194/acp-2021-528, https://doi.org/10.5194/acp-2021-528, 2021
Revised manuscript under review for ACP
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn 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 the light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and 4O atoms) and aromatics/nitro-aromatics, respectively.
Stavros Amanatidis, Yuanlong Huang, Buddhi Pushpawela, Benjamin C. Schulze, Christopher M. Kenseth, Ryan X. Ward, John H. Seinfeld, Susanne V. Hering, and Richard C. Flagan
Atmos. Meas. Tech., 14, 4507–4516, https://doi.org/10.5194/amt-14-4507-2021, https://doi.org/10.5194/amt-14-4507-2021, 2021
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We assess the performance of a highly portable mobility analyzer, the Spider DMA, in measuring ambient aerosol particle size distributions, with specific attention to its moderate sizing resolution (R=3). Long-term field testing showed excellent correlation with a conventional mobility analyzer (R=10) over the 17–500 nm range, suggesting that moderate resolution may be sufficient to obtain key properties of ambient size distributions, enabling smaller instruments and better counting statistics.
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.
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. Discuss., https://doi.org/10.5194/gmd-2021-107, https://doi.org/10.5194/gmd-2021-107, 2021
Revised manuscript accepted for GMD
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution showed a good agreement when validated against other simulations and available observations. We also estimated the contribution of iodine to ozone loss 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 to further studies of iodine effect on ozone.
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.
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. Discuss., https://doi.org/10.5194/amt-2021-125, https://doi.org/10.5194/amt-2021-125, 2021
Revised manuscript accepted for AMT
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To understand the sources and fate of particulate matters in the atmosphere, the ability to quantitatively describe their 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 for the firs time the driving factors behind instrument sensitivity variability towards individual components of particulate matters.
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. Discuss., https://doi.org/10.5194/acp-2021-277, https://doi.org/10.5194/acp-2021-277, 2021
Revised manuscript under review for ACP
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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.
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.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
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.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Zijun Li, Angela Buchholz, Arttu Ylisirniö, Luis Barreira, Liqing Hao, Siegfried Schobesberger, Taina Yli-Juuti, and Annele Virtanen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-367, https://doi.org/10.5194/acp-2021-367, 2021
Revised manuscript under review for ACP
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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.
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
Preprint under review 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.
Hanna Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Michael Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Ye Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Koster, Elena Lapsina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenko, Dimitry Orlov, Jean-Daniel Paris, Robertta 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 Qui, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergey Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-341, https://doi.org/10.5194/acp-2021-341, 2021
Preprint under review for ACP
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We summarize results during the last five years in the Northern Eurasian region, especially from Russia, and introduce recent observations on 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.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
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 under review 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.
Peng Zhang, Tianzeng Chen, Jun Liu, Guangyan Xu, Qingxin Ma, Biwu Chu, Wanqi Sun, and Hong He
Atmos. Chem. Phys., 21, 7099–7112, https://doi.org/10.5194/acp-21-7099-2021, https://doi.org/10.5194/acp-21-7099-2021, 2021
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This work highlights the opposing effects of primary and secondary H2SO4 on both secondary organic aerosol (SOA) formation and constitutes. Our findings revealed that a substantial increase in secondary H2SO4 particles promoted the SOA formation of ethyl methacrylate with increasing SO2 in the absence of seed particles. However, increased primary H2SO4 with seed acidity enhanced ethyl methacrylate uptake but reduced its SOA formation in the presence of seed particles.
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. Discuss., https://doi.org/10.5194/acp-2021-266, https://doi.org/10.5194/acp-2021-266, 2021
Revised manuscript under review for ACP
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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 200 km away from it. Due to the substantial contribution of NPF to the global aerosol budget, identifying the conditions that promote the occurrence of regional events could help understand their participation on a large scale and would improve their implementation in global models.
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. Discuss., https://doi.org/10.5194/amt-2021-117, https://doi.org/10.5194/amt-2021-117, 2021
Preprint under review for AMT
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Ecosystems emit biogenic volatile organic compounds (BVOC), which are then oxidized in the atmosphere contributing to ozone and secondary aerosol formation. While flux measurements of BVOC 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.
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. Discuss., https://doi.org/10.5194/acp-2021-333, https://doi.org/10.5194/acp-2021-333, 2021
Revised manuscript under review for ACP
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Between July and October, biomass burning smoke is advected over the southeast 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 how these biases propagate to biases in forcing.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-304, https://doi.org/10.5194/acp-2021-304, 2021
Revised manuscript accepted for ACP
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We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radical (OH) and the OH reactivity around the Arabian Peninsula, which were used to perform a comparison between local HCHO production and the related OH chemistry. This regression analysis revealed the regional HCHO yield alpha, which was elevated in the Arabian Gulf (also known as the Persion Gulf) and highlights the area as a hotspot of photochemical air pollution.
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. Discuss., https://doi.org/10.5194/esd-2021-16, https://doi.org/10.5194/esd-2021-16, 2021
Revised manuscript accepted for ESD
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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 “hotspots” of interaction. Code and data are open-access.
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.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
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. Discuss., https://doi.org/10.5194/acp-2021-251, https://doi.org/10.5194/acp-2021-251, 2021
Revised manuscript under review for ACP
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We employ a combination of models for gas-phase chemical reactions and equilibrium gas-particle partitioning of isoprene-derived secondary organic aerosols (SOA) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RH) 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 semivolatile organics.
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.
Shuping Zhang, Golam Sarwar, Jia Xing, Biwu Chu, Chaoyang Xue, Arunachalam Sarav, Dian Ding, Haotian Zheng, Yujing Mu, Fengkui Duan, Tao Ma, and Hong He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-47, https://doi.org/10.5194/acp-2021-47, 2021
Revised manuscript accepted for ACP
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Six heterogeneous HONO chemistry updates in CMAQ significantly improves HONO concentration. HONO production is primarily controlled by the heterogeneous reactions on ground and aerosol surfaces during haze. Additional HONO chemistry updates increase OH and production of secondary aerosols: sulfate, nitrate, and SOA.
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.
Ditte Taipale, Veli-Matti Kerminen, Mikael Ehn, Markku Kulmala, and Ülo Niinemets
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-141, https://doi.org/10.5194/acp-2021-141, 2021
Revised manuscript under review for ACP
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Larval feeding and fungal infections of leaves can change the emission of volatile compounds from plants a lot and thereby influence aerosol processes in the air. We developed a model which 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 be more important to consider than the parameters which are currently used in emission models.
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. Discuss., https://doi.org/10.5194/acp-2021-104, https://doi.org/10.5194/acp-2021-104, 2021
Revised manuscript accepted for ACP
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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.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
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.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
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.
Kamalika Sengupta, Kirsty Pringle, Jill S. Johnson, Carly Reddington, Jo Browse, Catherine E. Scott, and Ken Carslaw
Atmos. Chem. Phys., 21, 2693–2723, https://doi.org/10.5194/acp-21-2693-2021, https://doi.org/10.5194/acp-21-2693-2021, 2021
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Global models consistently underestimate atmospheric secondary organic aerosol (SOA), which has significant climatic implications. We use a perturbed parameter model ensemble and ground-based observations to reduce the uncertainty in modelling SOA formation from oxidation of volatile organic compounds. We identify plausible parameter spaces for the yields of extremely low-volatility, low-volatility, and semi-volatile organic compounds based on model–observation match for three key model outputs.
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.
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.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
Tianzeng Chen, Jun Liu, Qingxin Ma, Biwu Chu, Peng Zhang, Jinzhu Ma, Yongchun Liu, Cheng Zhong, Pengfei Liu, Yafei Wang, Yujing Mu, and Hong He
Atmos. Chem. Phys., 21, 1341–1356, https://doi.org/10.5194/acp-21-1341-2021, https://doi.org/10.5194/acp-21-1341-2021, 2021
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Effects of photochemical aging on the formation and evolution of summertime secondary aerosol were systematically investigated in a suburb of Beijing. Higher PM1 concentration accompanied longer photochemical age (ta). Sulfate and more-oxidized OOA formation were significantly sensitive to the increase in ta, and their contributions were greatly enhanced at elevated ta levels. Our results suggested that photochemical aging process played a crucial role in PM1 and O3 pollution in summertime.
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.
Benjamin J. Murray, Kenneth S. Carslaw, and Paul R. Field
Atmos. Chem. Phys., 21, 665–679, https://doi.org/10.5194/acp-21-665-2021, https://doi.org/10.5194/acp-21-665-2021, 2021
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The balance between the amounts of ice and supercooled water in clouds over the world's oceans strongly influences how much these clouds can dampen or amplify global warming. Aerosol particles which catalyse ice formation can dramatically reduce the amount of supercooled water in clouds; hence we argue that we need a concerted effort to improve our understanding of these ice-nucleating particles if we are to improve our predictions of climate change.
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.
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. Discuss., https://doi.org/10.5194/acp-2020-1202, https://doi.org/10.5194/acp-2020-1202, 2021
Revised manuscript accepted for ACP
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulphur dioxide emissions from the ore smelters are transported to wide areas. We investigated sulphur dioxide and its transformation to sulphuric 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.
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, A. 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. Discuss., https://doi.org/10.5194/acp-2020-1311, https://doi.org/10.5194/acp-2020-1311, 2021
Revised manuscript accepted for ACP
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Aerosol particles are a complex component of the atmospheric system which effects 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.
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.
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.
Jane P. Mulcahy, Colin Johnson, Colin G. Jones, Adam C. Povey, Catherine E. Scott, Alistair Sellar, Steven T. Turnock, Matthew T. Woodhouse, Nathan Luke Abraham, Martin B. Andrews, Nicolas Bellouin, Jo Browse, Ken S. Carslaw, Mohit Dalvi, Gerd A. Folberth, Matthew Glover, Daniel P. Grosvenor, Catherine Hardacre, Richard Hill, Ben Johnson, Andy Jones, Zak Kipling, Graham Mann, James Mollard, Fiona M. O'Connor, Julien Palmiéri, Carly Reddington, Steven T. Rumbold, Mark Richardson, Nick A. J. Schutgens, Philip Stier, Marc Stringer, Yongming Tang, Jeremy Walton, Stephanie Woodward, and Andrew Yool
Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, https://doi.org/10.5194/gmd-13-6383-2020, 2020
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Aerosols are an important component of the Earth system. Here, we comprehensively document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 and UKESM1. This study provides a useful characterisation of the aerosol climatology in both models, facilitating the understanding of the numerous aerosol–climate interaction studies that will be conducted for CMIP6 and beyond.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 20, 15681–15724, https://doi.org/10.5194/acp-20-15681-2020, https://doi.org/10.5194/acp-20-15681-2020, 2020
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Particles arising from human activity interact with clouds and affect how much of the Sun's energy is reflected away. Lack of understanding about how to represent this in models leads to large uncertainties in climate predictions. We quantify cloud responses to particles in the latest UK Met Office climate model over the North Atlantic Ocean, showing that, in contrast to suggestions elsewhere, increases in cloud coverage and thickness are important over large areas.
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
Revised manuscript has not been submitted
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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.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
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.
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.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
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.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
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.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
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.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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.
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.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
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.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
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.
Miao Yu, Guiqian Tang, Yang Yang, Qingchun Li, Yonghong Wang, Shiguang Miao, Yizhou Zhang, and Yuesi Wang
Atmos. Chem. Phys., 20, 9855–9870, https://doi.org/10.5194/acp-20-9855-2020, https://doi.org/10.5194/acp-20-9855-2020, 2020
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.
Jill S. Johnson, Leighton A. Regayre, Masaru Yoshioka, Kirsty J. Pringle, Steven T. Turnock, Jo Browse, David M. H. Sexton, John W. Rostron, Nick A. J. Schutgens, Daniel G. Partridge, Dantong Liu, James D. Allan, Hugh Coe, Aijun Ding, David D. Cohen, Armand Atanacio, Ville Vakkari, Eija Asmi, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 9491–9524, https://doi.org/10.5194/acp-20-9491-2020, https://doi.org/10.5194/acp-20-9491-2020, 2020
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We use over 9000 monthly aggregated grid-box measurements of aerosol to constrain the uncertainty in the HadGEM3-UKCA climate model. Measurements of AOD, PM2.5, particle number concentrations, sulfate and organic mass concentrations are compared to 1 million
variantsof the model using an implausibility metric. Despite many compensating effects in the model, the procedure constrains the probability distributions of many parameters, and direct radiative forcing uncertainty is reduced by 34 %.
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.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Yuan Yang, Yonghong Wang, Putian Zhou, Dan Yao, Dongsheng Ji, Jie Sun, Yinghong Wang, Shuman Zhao, Wei Huang, Shuanghong Yang, Dean Chen, Wenkang Gao, Zirui Liu, Bo Hu, Renjian Zhang, Limin Zeng, Maofa Ge, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Yuesi Wang
Atmos. Chem. Phys., 20, 8181–8200, https://doi.org/10.5194/acp-20-8181-2020, https://doi.org/10.5194/acp-20-8181-2020, 2020
Peter Josef Wlasits, Dominik Stolzenburg, Christian Tauber, Sophia Brilke, Sebastian Harald Schmitt, Paul Martin Winkler, and Daniela Wimmer
Atmos. Meas. Tech., 13, 3787–3798, https://doi.org/10.5194/amt-13-3787-2020, https://doi.org/10.5194/amt-13-3787-2020, 2020
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In this paper we show that chemical similarities between the seed particle material and the working fluid have an impact on the detection efficiency of commonly used CPCs. A remarkable set of CPCs, including the newly developed V-WCPC 3789, was tested. Among others, reproducibly generated organic seeds based on beta-caryophyllene were used. Theoretical simulations of supersaturation profiles were successfully linked to measured data.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Alexander B. MacDonald, Ali Hossein Mardi, Hossein Dadashazar, Mojtaba Azadi Aghdam, Ewan Crosbie, Haflidi H. Jonsson, Richard C. Flagan, John H. Seinfeld, and Armin Sorooshian
Atmos. Chem. Phys., 20, 7645–7665, https://doi.org/10.5194/acp-20-7645-2020, https://doi.org/10.5194/acp-20-7645-2020, 2020
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Understanding how humans affect Earth's climate requires understanding of how particles in the air affect the number concentration of droplets in a cloud (Nd). We use the air-equivalent mass concentration of different chemical species contained in cloud water to predict Nd. In this study we found that the prediction of Nd is (1) best described by total sulfate; (2) improved when considering up to five species; and (3) dependent on factors like turbulence, smoke presence, and in-cloud height.
Sini Isokääntä, Eetu Kari, Angela Buchholz, Liqing Hao, Siegfried Schobesberger, Annele Virtanen, and Santtu Mikkonen
Atmos. Meas. Tech., 13, 2995–3022, https://doi.org/10.5194/amt-13-2995-2020, https://doi.org/10.5194/amt-13-2995-2020, 2020
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Online mass spectrometry produces large amounts of data. These data can be interpreted with statistical methods, enabling scientists to more easily understand the underlying processes. We compared these techniques on car exhaust measurements. We show differences and similarities between the methods and give recommendations on applicability of the methods on certain types of data. We show that applying multiple methods leads to more robust results, thus increasing reliability of the findings.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Mikhail Paramonov, Saskia Drossaart van Dusseldorp, Ellen Gute, Jonathan P. D. Abbatt, Paavo Heikkilä, Jorma Keskinen, Xuemeng Chen, Krista Luoma, Liine Heikkinen, Liqing Hao, Tuukka Petäjä, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 6687–6706, https://doi.org/10.5194/acp-20-6687-2020, https://doi.org/10.5194/acp-20-6687-2020, 2020
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Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland in the winter–spring of 2018. It was found that no single parameter could be used to predict the INP number concentration at the measurement location during the examined time period. It was also not possible to identify physical and chemical properties of ambient INPs despite the complexity of the instrumental set-up. Therefore, this paper addresses the necessity for future INP measurements.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Men Xia, Xiang Peng, Weihao Wang, Chuan Yu, Peng Sun, Yuanyuan Li, Yuliang Liu, Zhengning Xu, Zhe Wang, Zheng Xu, Wei Nie, Aijun Ding, and Tao Wang
Atmos. Chem. Phys., 20, 6147–6158, https://doi.org/10.5194/acp-20-6147-2020, https://doi.org/10.5194/acp-20-6147-2020, 2020
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ClNO2 and Cl2 can be photolyzed by sunlight to produce a highly reactive Cl atom which affects air quality and climate. We observed high ClNO2 and Cl2 concentrations during a recent field study in east China. We analyzed the data and proposed a new hypothesis on the Cl2 production mechanism. Yields of ClNO2 and Cl2 from N2O2 uptake were parameterized using observational constraints, and they can be used in air quality models to improve simulations of atmospheric photochemistry and air quality.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
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.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Sophia Brilke, Nikolaus Fölker, Thomas Müller, Konrad Kandler, Xianda Gong, Jeff Peischl, Bernadett Weinzierl, and Paul M. Winkler
Atmos. Chem. Phys., 20, 5645–5656, https://doi.org/10.5194/acp-20-5645-2020, https://doi.org/10.5194/acp-20-5645-2020, 2020
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Atmospheric particle size distributions with the focus on freshly nucleated particles were measured during the A-LIFE field experiment in Cyprus. A DMA-train was set up for the first time in an atmospheric environment and captures the sub-10 nm particle dynamics. Several new particle formation (NPF) events are studied in detail, of which some did not show particle growth beyond 10 nm indicating that NPF may occur more frequently than estimated when the sub-10 nm size range is not covered.
Karin Kreher, Michel Van Roozendael, Francois Hendrick, Arnoud Apituley, Ermioni Dimitropoulou, Udo Frieß, Andreas Richter, Thomas Wagner, Johannes Lampel, Nader Abuhassan, Li Ang, Monica Anguas, Alkis Bais, Nuria Benavent, Tim Bösch, Kristof Bognar, Alexander Borovski, Ilya Bruchkouski, Alexander Cede, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Caroline Fayt, Henning Finkenzeller, David Garcia-Nieto, Clio Gielen, Laura Gómez-Martín, Nan Hao, Bas Henzing, Jay R. Herman, Christian Hermans, Syedul Hoque, Hitoshi Irie, Junli Jin, Paul Johnston, Junaid Khayyam Butt, Fahim Khokhar, Theodore K. Koenig, Jonas Kuhn, Vinod Kumar, Cheng Liu, Jianzhong Ma, Alexis Merlaud, Abhishek K. Mishra, Moritz Müller, Monica Navarro-Comas, Mareike Ostendorf, Andrea Pazmino, Enno Peters, Gaia Pinardi, Manuel Pinharanda, Ankie Piters, Ulrich Platt, Oleg Postylyakov, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Alfonso Saiz-Lopez, Anja Schönhardt, Stefan F. Schreier, André Seyler, Vinayak Sinha, Elena Spinei, Kimberly Strong, Frederik Tack, Xin Tian, Martin Tiefengraber, Jan-Lukas Tirpitz, Jeroen van Gent, Rainer Volkamer, Mihalis Vrekoussis, Shanshan Wang, Zhuoru Wang, Mark Wenig, Folkard Wittrock, Pinhua H. Xie, Jin Xu, Margarita Yela, Chengxin Zhang, and Xiaoyi Zhao
Atmos. Meas. Tech., 13, 2169–2208, https://doi.org/10.5194/amt-13-2169-2020, https://doi.org/10.5194/amt-13-2169-2020, 2020
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In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants during an instrument intercomparison campaign (CINDI-2) at Cabauw, the Netherlands. Here we report on the outcome of this intercomparison exercise. The three major goals were to characterise the differences between the participating instruments, to define a robust methodology for performance assessment, and to contribute to the harmonisation of the measurement settings and retrieval methods.
Yonghong Wang, Matthieu Riva, Hongbin Xie, Liine Heikkinen, Simon Schallhart, Qiaozhi Zha, Chao Yan, Xu-Cheng He, Otso Peräkylä, and Mikael Ehn
Atmos. Chem. Phys., 20, 5145–5155, https://doi.org/10.5194/acp-20-5145-2020, https://doi.org/10.5194/acp-20-5145-2020, 2020
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Chamber experiments were conducted with alpha-pinene and chlorine under low- and high-nitrogen-oxide (NOX) conditions. We estimated the HOM yields from chlorine-initiated oxidation of alpha-pinene under low-NOX conditions to be around 1.8 %, though with a uncertainty range (0.8 %–4 %) due to lack of suitable calibration methods. Our study clearly demonstrates that the chlorine-atom-initiated oxidation of alpha-pinene can produce low-volatility organic compounds.
Dean Chen, Putian Zhou, Tuomo Nieminen, Pontus Roldin, Ximeng Qi, Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Markku Kulmala, Pekka Rantala, Juho Aalto, Nina Sarnela, Pasi Kolari, Petri Keronen, Matti P. Rissanen, Metin Baykara, and Michael Boy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-128, https://doi.org/10.5194/acp-2020-128, 2020
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
Chuan Yu, Zhe Wang, Men Xia, Xiao Fu, Weihao Wang, Yee Jun Tham, Tianshu Chen, Penggang Zheng, Hongyong Li, Ye Shan, Xinfeng Wang, Likun Xue, Yan Zhou, Dingli Yue, Yubo Ou, Jian Gao, Keding Lu, Steven S. Brown, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 20, 4367–4378, https://doi.org/10.5194/acp-20-4367-2020, https://doi.org/10.5194/acp-20-4367-2020, 2020
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This study provides a holistic picture of N2O5 heterogeneous uptake on ambient aerosols and the influencing factors under various climatic and chemical conditions in China, and it proposes an observation-based empirical parameterization. The empirical parameterization can be used in air quality models to improve the prediction of PM2.5 and photochemical pollution in China and similar polluted regions of the world.
Daniel T. McCoy, Paul Field, Hamish Gordon, Gregory S. Elsaesser, and Daniel P. Grosvenor
Atmos. Chem. Phys., 20, 4085–4103, https://doi.org/10.5194/acp-20-4085-2020, https://doi.org/10.5194/acp-20-4085-2020, 2020
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Incomplete understanding of how aerosol affects clouds degrades our ability to predict future climate. In particular, it is unclear how aerosol affects the lifetime of clouds. Does it increase or decrease it? This confusion is partially because causality flows from aerosol to clouds and clouds to aerosol, and it is hard to tell what is happening in observations. Here, we use simulations to tell us about how clouds affect aerosol and use this to interpret observations, showing increased lifetime.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Jinpei Yan, Jinyoung Jung, Miming Zhang, Federico Bianchi, Yee Jun Tham, Suqing Xu, Qi Lin, Shuhui Zhao, Lei Li, and Liqi Chen
Atmos. Chem. Phys., 20, 3259–3271, https://doi.org/10.5194/acp-20-3259-2020, https://doi.org/10.5194/acp-20-3259-2020, 2020
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Methanesulfonic acid (MSA) is important to the CCN in the MBL. The uptake of MSA on particles is lacking in knowledge. The characteristics of MSA uptake on different particles were studied in the Southern Ocean. The MSA uptake on different particles was associated with particle properties. Uptake of MSA on sea salt particles was favored, while acidic and hydrophobic particles suppressed the MSA uptake. The results extend the knowledge of MSA formation and behavior in the atmosphere.
Liine Heikkinen, Mikko Äijälä, Matthieu Riva, Krista Luoma, Kaspar Dällenbach, Juho Aalto, Pasi Aalto, Diego Aliaga, Minna Aurela, Helmi Keskinen, Ulla Makkonen, Pekka Rantala, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 3151–3180, https://doi.org/10.5194/acp-20-3151-2020, https://doi.org/10.5194/acp-20-3151-2020, 2020
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Atmospheric aerosols are solid or liquid particles suspended in the air. They are known as a health risk, but they also influence the Earth's climate. The composition of aerosols becomes important when predicting their effect on climate. We show both seasonal and year-to-year variability of aerosol chemical composition in the boreal forest of Finland. We observed a consistent bimodal seasonal trend: a biogenic summertime maximum and an anthropogenic wintertime maximum in the mass concentration.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
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We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
Constanze Wellmann, Andrew I. Barrett, Jill S. Johnson, Michael Kunz, Bernhard Vogel, Ken S. Carslaw, and Corinna Hoose
Atmos. Chem. Phys., 20, 2201–2219, https://doi.org/10.5194/acp-20-2201-2020, https://doi.org/10.5194/acp-20-2201-2020, 2020
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Severe hailstorms may cause damage to buildings and crops. Thus, the forecast of numerical weather prediction (NWP) models should be as reliable as possible.
Using statistical emulation, we identify those model input parameters describing environmental conditions and cloud microphysics which lead to large uncertainties in the prediction of deep convection. We find that the impact of the input parameters on the uncertainty depends on the considered output variable.
Haiyan Li, Matthieu Riva, Pekka Rantala, Liine Heikkinen, Kaspar Daellenbach, Jordan E. Krechmer, Pierre-Marie Flaud, Douglas Worsnop, Markku Kulmala, Eric Villenave, Emilie Perraudin, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 20, 1941–1959, https://doi.org/10.5194/acp-20-1941-2020, https://doi.org/10.5194/acp-20-1941-2020, 2020
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We deployed the recently developed Vocus PTR-TOF in the French Landes forest during summertime to gain insights into terpene chemistry. In addition to isoprene, monoterpenes, sesquiterpenes, and the low-volatility diterpenes, various terpene reaction products are characterized. Through the analysis of terpene chemistry, we demonstrate the capability of the Vocus PTR-TOF for the detection of oxidized reaction products, highlighting its importance in investigating atmospheric oxidation processes.
Pragati Rai, Markus Furger, Jay G. Slowik, Francesco Canonaco, Roman Fröhlich, Christoph Hüglin, María Cruz Minguillón, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 1657–1674, https://doi.org/10.5194/acp-20-1657-2020, https://doi.org/10.5194/acp-20-1657-2020, 2020
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A source apportionment study of hourly resolved elements in PM10 measured at a traffic-influenced site in Härkingen, Switzerland, using positive matrix factorization (PMF) and multilinear engine-2 (ME-2) offered resolution of robust and unambiguous factor profiles and contributions. We show that the rotational control available in ME-2 provides a means for treating extreme events such as fireworks within a PMF analysis.
Ditte Taipale, Juho Aalto, Pauliina Schiestl-Aalto, Markku Kulmala, and Jaana Bäck
Biogeosciences Discuss., https://doi.org/10.5194/bg-2019-502, https://doi.org/10.5194/bg-2019-502, 2020
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Ying Zhou, Lubna Dada, Yiliang Liu, Yueyun Fu, Juha Kangasluoma, Tommy Chan, Chao Yan, Biwu Chu, Kaspar R. Daellenbach, Federico Bianchi, Tom V. Kokkonen, Yongchun Liu, Joni Kujansuu, Veli-Matti Kerminen, Tuukka Petäjä, Lin Wang, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 20, 1201–1216, https://doi.org/10.5194/acp-20-1201-2020, https://doi.org/10.5194/acp-20-1201-2020, 2020
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In this study, we focus on explaining the concentration variations in the observed particle modes, by relating them to the potential aerosol sources and sinks, and on understanding the connections between these modes. Interestingly, even in the atmospheric cocktail in urban Beijing, secondary new particle formation (NPF) drives the particle number concentration, especially in the sub-3 nm range. We found that the total number concentration is ~ 4 times higher on NPF days than on haze days.
Meredith Schervish and Neil M. Donahue
Atmos. Chem. Phys., 20, 1183–1199, https://doi.org/10.5194/acp-20-1183-2020, https://doi.org/10.5194/acp-20-1183-2020, 2020
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Gas-phase autoxidation of organics can generate highly oxygenated organic molecules (HOMs) and thus increase secondary organic aerosol production and enable new-particle formation. Here we explicitly represent the generation of HOMs via peroxy radical chemistry and resolve the products based on volatility and O : C. Using experimentally constrained assumptions about autoxidation and dimerization reactions, we see suppression of HOM formation under low-temperature and high-NOx conditions.
Carmen Dameto de España, Anna Wonaschuetz, Gerhard Steiner, Harald Schuh, Constantinos Sioutas, and Regina Hitzenberger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-21, https://doi.org/10.5194/amt-2020-21, 2020
Preprint withdrawn
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Marja Hemmilä, Ulla Makkonen, Aki Virkkula, Georgia Panagiotopoulou, Juho Aalto, Markku Kulmala, Tuukka Petäjä, Hannele Hakola, and Heidi Hellén
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1157, https://doi.org/10.5194/acp-2019-1157, 2020
Publication in ACP not foreseen
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Amines are atmospheric bases, which can affect to nucleation of aerosols. Lately, a computational study showed that guanidine could be even more effective to stabilize sulphuric acid clusters. In this paper we used a a dynamic flow-through chamber with an online ion chromatograph MARGA coupled with a mass spectrometer (MARGA-MS). We studied amine and guanidine emission from a boreal forest floor in Finland, and find out, that the boreal forest floor is a source of amines and guanidine.
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-2019-651, https://doi.org/10.5194/hess-2019-651, 2020
Revised manuscript not accepted
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The annual ET is approximately equal to precipitation during six measured years for grazed savanna grassland. The computed annual transpiration was highly constrained when rainfall was near or above the long-term mean but was reduced during severe drought year. The developed methodologies can be used in a wide range of arid and semi-arid ecosystems.
Yonghong Wang, Miao Yu, Yuesi Wang, Guiqian Tang, Tao Song, Putian Zhou, Zirui Liu, Bo Hu, Dongsheng Ji, Lili Wang, Xiaowan Zhu, Chao Yan, Mikael Ehn, Wenkang Gao, Yuepeng Pan, Jinyuan Xin, Yang Sun, Veli-Matti Kerminen, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 20, 45–53, https://doi.org/10.5194/acp-20-45-2020, https://doi.org/10.5194/acp-20-45-2020, 2020
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Shor