Articles | Volume 21, issue 9
https://doi.org/10.5194/acp-21-7357-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-7357-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement report
| 
17 May 2021
Measurement report |
| 17 May 2021
| 17 May 2021
Measurement report: Effects of NOx and seed aerosol on highly oxygenated organic molecules (HOMs) from cyclohexene ozonolysis
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Otso Peräkylä
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Matthieu Riva
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Univ. Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, 69626, Villeurbanne, France
Lauriane Quéléver
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Olga Garmash
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Matti Rissanen
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Aerosol Physics Laboratory, Physics Unit, Tampere University, Tampere, Finland
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
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Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
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Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
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Shawon Barua, Siddharth Iyer, Avinash Kumar, Prasenjit Seal, and Matti Rissanen
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Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
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Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Meri Räty, Larisa Sogacheva, Helmi-Marja Keskinen, Veli-Matti Kerminen, Tuomo Nieminen, Tuukka Petäjä, Ekaterina Ezhova, and Markku Kulmala
Atmos. Chem. Phys., 23, 3779–3798, https://doi.org/10.5194/acp-23-3779-2023, https://doi.org/10.5194/acp-23-3779-2023, 2023
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We utilised back trajectories to identify the source region of air masses arriving in Hyytiälä, Finland, and their travel time over forests. Combined with atmospheric observations, they revealed how air mass transport over the Fennoscandian boreal forest during the growing season produced an accumulation of cloud condensation nuclei and humidity, promoting cloudiness and precipitation. By 55 h of transport, air masses appeared to reach a balanced state with the forest environment.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
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Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Yiqun Lu, Yingge Ma, Dan Dan Huang, Shengrong Lou, Sheng'ao Jing, Yaqin Gao, Hongli Wang, Yanjun Zhang, Hui Chen, Yunhua Chang, Naiqiang Yan, Jianmin Chen, Christian George, Matthieu Riva, and Cheng Huang
Atmos. Chem. Phys., 23, 3233–3245, https://doi.org/10.5194/acp-23-3233-2023, https://doi.org/10.5194/acp-23-3233-2023, 2023
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N-containing oxygenated organic molecules have been identified as important precursors of aerosol particles. We used an ultra-high-resolution mass spectrometer coupled with an online sample inlet to accurately measure their molecular composition, concentration level and variation patterns. We show their formation process and influencing factors in a Chinese megacity involving various volatile organic compound precursors and atmospheric oxidants, and we highlight the influence of PM2.5 episodes.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
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The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities to but also distinct differences from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Miska Olin, Magdalena Okuljar, Matti P. Rissanen, Joni Kalliokoski, Jiali Shen, Lubna Dada, Markus Lampimäki, Yusheng Wu, Annalea Lohila, Jonathan Duplissy, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 8097–8115, https://doi.org/10.5194/acp-22-8097-2022, https://doi.org/10.5194/acp-22-8097-2022, 2022
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Atmospheric new particle formation is an important source of the total particle number concentration in the atmosphere. Several parameters for predicting new particle formation events have been suggested before, but the results have been inconclusive. This study proposes an another predicting parameter, related to a specific type of highly oxidized organic molecules, especially for similar locations to the measurement site in this study, which was a coastal agricultural site in Finland.
Roseline C. Thakur, Lubna Dada, Lisa J. Beck, Lauriane L. J. Quéléver, Tommy Chan, Marjan Marbouti, Xu-Cheng He, Carlton Xavier, Juha Sulo, Janne Lampilahti, Markus Lampimäki, Yee Jun Tham, Nina Sarnela, Katrianne Lehtipalo, Alf Norkko, Markku Kulmala, Mikko Sipilä, and Tuija Jokinen
Atmos. Chem. Phys., 22, 6365–6391, https://doi.org/10.5194/acp-22-6365-2022, https://doi.org/10.5194/acp-22-6365-2022, 2022
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Every year intense cyanobacterial and macroalgal blooms occur in the Baltic Sea and in the coastal areas surrounding Helsinki, yet no studies have addressed the impact of biogenic emissions from these blooms on gas vapor concentrations, which in turn could influence new particle formation. This is the first study of its kind to address the chemistry driving new particle formation (NPF) during a bloom period in this region, highlighting the role of biogenic sulfuric acid and iodic acid.
Yuanyuan Luo, Olga Garmash, Haiyan Li, Frans Graeffe, Arnaud P. Praplan, Anssi Liikanen, Yanjun Zhang, Melissa Meder, Otso Peräkylä, Josep Peñuelas, Ana María Yáñez-Serrano, and Mikael Ehn
Atmos. Chem. Phys., 22, 5619–5637, https://doi.org/10.5194/acp-22-5619-2022, https://doi.org/10.5194/acp-22-5619-2022, 2022
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Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and we characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Ditte Taipale, Veli-Matti Kerminen, Mikael Ehn, Markku Kulmala, and Ülo Niinemets
Atmos. Chem. Phys., 21, 17389–17431, https://doi.org/10.5194/acp-21-17389-2021, https://doi.org/10.5194/acp-21-17389-2021, 2021
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Larval feeding and fungal infections of leaves can greatly change the emission of volatile compounds from plants and thereby influence aerosol processes in the air. We developed a model that considers the dynamics of larvae and fungi and the dependency of the emission on the severity of stress. We show that the infections can be highly atmospherically relevant during long periods of time and at times more important to consider than the parameters that are currently used in emission models.
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.
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.
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.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Magdalena Okuljar, Heino Kuuluvainen, Jenni Kontkanen, Olga Garmash, Miska Olin, Jarkko V. Niemi, Hilkka Timonen, Juha Kangasluoma, Yee Jun Tham, Rima Baalbaki, Mikko Sipilä, Laura Salo, Henna Lintusaari, Harri Portin, Kimmo Teinilä, Minna Aurela, Miikka Dal Maso, Topi Rönkkö, Tuukka Petäjä, and Pauli Paasonen
Atmos. Chem. Phys., 21, 9931–9953, https://doi.org/10.5194/acp-21-9931-2021, https://doi.org/10.5194/acp-21-9931-2021, 2021
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To estimate the relative contribution of different sources to the particle population in an urban environment, we conducted simultaneous measurements at a street canyon and an urban background station in Helsinki. We investigated the contribution of traffic and new particle formation to particles with a diameter between 1 and 800 nm. We found that during spring traffic does not dominate the particles smaller than 3 nm at either of the stations.
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.
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.
Runlong Cai, Yihao Li, Yohann Clément, Dandan Li, Clément Dubois, Marlène Fabre, Laurence Besson, Sebastien Perrier, Christian George, Mikael Ehn, Cheng Huang, Ping Yi, Yingge Ma, and Matthieu Riva
Atmos. Meas. Tech., 14, 2377–2387, https://doi.org/10.5194/amt-14-2377-2021, https://doi.org/10.5194/amt-14-2377-2021, 2021
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Orbitool is an open-source software tool, mainly coded in Python, with a graphical user interface (GUI), specifically developed to facilitate the analysis of online Orbitrap mass spectrometric data. It is notably optimized for long-term atmospheric measurements and laboratory studies.
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.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
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.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 5945–5961, https://doi.org/10.5194/acp-20-5945-2020, https://doi.org/10.5194/acp-20-5945-2020, 2020
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By utilizing a new analysis approach, we investigated atmospheric oxidation of biogenic volatile emissions in a Finnish forest, measured by chemical ionization mass spectrometry. We identified several new compound groups, including low-volatility accretion products and their formation pathways. Results from this study are important for understanding atmospheric aerosol formation, as well as providing new perspectives on future lab studies and data analysis of short-lived species.
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
Preprint withdrawn
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
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.
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.
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.
Otso Peräkylä, Matthieu Riva, Liine Heikkinen, Lauriane Quéléver, Pontus Roldin, and Mikael Ehn
Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, https://doi.org/10.5194/acp-20-649-2020, 2020
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Highly oxygenated organic molecules have been suggested to form a large part of secondary organic aerosol. However, with their exotic structures, their volatilities are not well known, making their exact role in particle formation hard to assess. In laboratory experiments, we found the volatility of HOMs formed in the ozonolysis of the monoterpene alpha-pinene to be in the middle of earlier estimates. The volatilities of HOMs could be well explained in terms of their molecular formulae.
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.
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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We found a positive particle matter-mixing layer height feedback at three observation platforms at the 325 m Beijing meteorology tower, which is characterized by a shallower mixing layer height and a higher particle matter concentration. Measurements of solar radiation, aerosol chemical composition, meteorology parameters, trace gases and turbulent kinetic energy (TKE) could explain the feedback mechanism to some extent.
Matti P. Rissanen, Jyri Mikkilä, Siddharth Iyer, and Jani Hakala
Atmos. Meas. Tech., 12, 6635–6646, https://doi.org/10.5194/amt-12-6635-2019, https://doi.org/10.5194/amt-12-6635-2019, 2019
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A novel chemical ionization methodology for rapid gas–phase environmental monitoring is presented. The usefulness of the new inlet design is demonstrated by measuring various aerosol precursor compounds that are present at very low concentrations by using two consecutive ionization schemes. This new inlet enables the detection of a wide range of compounds of interest with a minimum of effort and at a fast repetition rate.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Jonathan Liebmann, Nicolas Sobanski, Jan Schuladen, Einar Karu, Heidi Hellén, Hannele Hakola, Qiaozhi Zha, Mikael Ehn, Matthieu Riva, Liine Heikkinen, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 10391–10403, https://doi.org/10.5194/acp-19-10391-2019, https://doi.org/10.5194/acp-19-10391-2019, 2019
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The formation of alkyl nitrates in the boreal forest was dominated by reactions of the NO3 radical with terpenes, both during the day and the night, with fewer contributions from OH and ozone. The alkyl nitrates formed had lifetimes on the order of 2 h, reflecting efficient loss via uptake to aerosol and deposition.
Yanjun Zhang, Otso Peräkylä, Chao Yan, Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Qiaozhi Zha, Matthieu Riva, Olga Garmash, Heikki Junninen, Pentti Paatero, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 3761–3776, https://doi.org/10.5194/amt-12-3761-2019, https://doi.org/10.5194/amt-12-3761-2019, 2019
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Recent advancements in atmospheric mass spectrometry provide large amounts of new information but at the same time present considerable challenges for the data analysis, for example, in high-resolution peak identification and separation. To address these problems, this study presents a simple and novel method, which succeeds in analyzing both synthetic and ambient datasets. We believe it will become a powerful approach in the data analysis of mass spectra.
Lauriane L. J. Quéléver, Kasper Kristensen, Louise Normann Jensen, Bernadette Rosati, Ricky Teiwes, Kaspar R. Daellenbach, Otso Peräkylä, Pontus Roldin, Rossana Bossi, Henrik B. Pedersen, Marianne Glasius, Merete Bilde, and Mikael Ehn
Atmos. Chem. Phys., 19, 7609–7625, https://doi.org/10.5194/acp-19-7609-2019, https://doi.org/10.5194/acp-19-7609-2019, 2019
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Highly oxygenated organic molecules (HOMs) form rapidly in oxidation of monoterpenes and have been shown to be crucial for secondary organic aerosol formation. We studied the formation of HOMs under different temperatures, finding a strong dependence on their yields. As temperatures decrease, the isomerization reactions that allow rapid oxidation by molecular oxygen slow down, and competing reaction pathways can suppress the HOM formation almost completely, especially at high VOC loadings.
Matthieu Riva, Pekka Rantala, Jordan E. Krechmer, Otso Peräkylä, Yanjun Zhang, Liine Heikkinen, Olga Garmash, Chao Yan, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 2403–2421, https://doi.org/10.5194/amt-12-2403-2019, https://doi.org/10.5194/amt-12-2403-2019, 2019
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The impact of aerosol particles on climate and air quality remains poorly understood due to multiple factors. One of the current limitations is the incomplete understanding of the contribution of oxygenated species, formed from the oxidation of volatile organic compounds (VOCs) to aerosol formation. Taking advantage of recent mass spectrometric developments, we have evaluated and compared the capability of multiple state-of-the-art mass spectrometers to detect a wide variety of oxygenated VOCs.
Mikko Äijälä, Kaspar R. Daellenbach, Francesco Canonaco, Liine Heikkinen, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, André S. H. Prévôt, and Mikael Ehn
Atmos. Chem. Phys., 19, 3645–3672, https://doi.org/10.5194/acp-19-3645-2019, https://doi.org/10.5194/acp-19-3645-2019, 2019
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Aerosol mass spectrometry produces large amounts of complex data, the analysis of which necessitates chemometrics – the application of advanced statistical and mathematical tools to chemical data. Here, we perform a data-driven analysis of multiple aerosol mass spectrometric data sets, to show that the traditional separation of organics and inorganics is not necessary. The resulting 7-component aerosol speciation explains 83 % to 96 % of observed variability at our boreal forest experiment site.
Yiqun Lu, Chao Yan, Yueyun Fu, Yan Chen, Yiliang Liu, Gan Yang, Yuwei Wang, Federico Bianchi, Biwu Chu, Ying Zhou, Rujing Yin, Rima Baalbaki, Olga Garmash, Chenjuan Deng, Weigang Wang, Yongchun Liu, Tuukka Petäjä, Veli-Matti Kerminen, Jingkun Jiang, Markku Kulmala, and Lin Wang
Atmos. Chem. Phys., 19, 1971–1983, https://doi.org/10.5194/acp-19-1971-2019, https://doi.org/10.5194/acp-19-1971-2019, 2019
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Gaseous sulfuric acid is one of the key precursors for atmospheric new particle formation processes, but its measurement remains challenging. This work develops an estimation method for the gaseous sulfuric acid concentration in an urban environment in China using multiple atmospheric variables that are easier to measure. The consideration of the heterogeneous formation of HONO and the subsequent photo-production of OH radicals improves the performance of the estimation method.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Qiaozhi Zha, Chao Yan, Heikki Junninen, Matthieu Riva, Nina Sarnela, Juho Aalto, Lauriane Quéléver, Simon Schallhart, Lubna Dada, Liine Heikkinen, Otso Peräkylä, Jun Zou, Clémence Rose, Yonghong Wang, Ivan Mammarella, Gabriel Katul, Timo Vesala, Douglas R. Worsnop, Markku Kulmala, Tuukka Petäjä, Federico Bianchi, and Mikael Ehn
Atmos. Chem. Phys., 18, 17437–17450, https://doi.org/10.5194/acp-18-17437-2018, https://doi.org/10.5194/acp-18-17437-2018, 2018
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Vertical measurements of highly oxygenated molecules (HOMs) below and above the forest canopy were performed for the first time in a boreal forest during September 2016. Our results highlight that near-ground HOM measurements may only be representative of a small fraction of the entire nocturnal boundary layer, which may sequentially influence the growth of newly formed particles and SOA formation close to ground surface, where the majority of measurements are conducted.
Sri Hapsari Budisulistiorini, Matthieu Riva, Michael Williams, Takuma Miyakawa, Jing Chen, Masayuki Itoh, Jason D. Surratt, and Mikinori Kuwata
Atmos. Chem. Phys., 18, 16481–16498, https://doi.org/10.5194/acp-18-16481-2018, https://doi.org/10.5194/acp-18-16481-2018, 2018
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Wildfire emits a large number of haze particles. During transport in the atmosphere, the organic aerosol in the haze particles can undergo atmospheric processes and become highly oxidized. We show that the haze particles transported from wildfires in Indonesia are dominated by oxygenated organic aerosols. This study highlights the impact of atmospheric processes on the transboundary haze particles.
Chao Yan, Lubna Dada, Clémence Rose, Tuija Jokinen, Wei Nie, Siegfried Schobesberger, Heikki Junninen, Katrianne Lehtipalo, Nina Sarnela, Ulla Makkonen, Olga Garmash, Yonghong Wang, Qiaozhi Zha, Pauli Paasonen, Federico Bianchi, Mikko Sipilä, Mikael Ehn, Tuukka Petäjä, Veli-Matti Kerminen, Douglas R. Worsnop, and Markku Kulmala
Atmos. Chem. Phys., 18, 13231–13243, https://doi.org/10.5194/acp-18-13231-2018, https://doi.org/10.5194/acp-18-13231-2018, 2018
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Ions can play an important role in atmospheric new particle formation by stabilizing the embryonic clusters. Such a process is called ion-induced nucleation (IIN). We found two distinct IIN mechanisms – driven by H2SO4-NH3 clusters and by organic vapors, respectively. The concentration ratio of organic vapors to H2SO4 regulates via which pathway the IIN occur. As the organic vapor concentration is influenced by temperature, a seasonal variation in the main IIN mechanism can be expected.
Ximeng Qi, Aijun Ding, Pontus Roldin, Zhengning Xu, Putian Zhou, Nina Sarnela, Wei Nie, Xin Huang, Anton Rusanen, Mikael Ehn, Matti P. Rissanen, Tuukka Petäjä, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 18, 11779–11791, https://doi.org/10.5194/acp-18-11779-2018, https://doi.org/10.5194/acp-18-11779-2018, 2018
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In this study we simulate the HOM concentrations and discuss their roles in NPF at a remote boreal forest site in Finland and a suburban site in eastern China. We found that sulfuric acid and HOM organonitrate concentrations in the gas phase are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower in eastern China. This study highlights the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
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.
Xuemeng Chen, Lauriane L. J. Quéléver, Pak L. Fung, Jutta Kesti, Matti P. Rissanen, Jaana Bäck, Petri Keronen, Heikki Junninen, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 49–63, https://doi.org/10.5194/acp-18-49-2018, https://doi.org/10.5194/acp-18-49-2018, 2018
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We analysed a 20-year-long dataset collected in a Finnish boreal forest at SMEAR II station to investigate the frequency and strength of ozone depletion events. We could identify a number of ozone depletion events that lasted for more than 3 h, mainly in the autumn and winter months. Their occurrence was likely related to the formation of a low mixing layer under the conditions of low temperatures, low wind speeds, high relative humidities and limited intensity of solar radiation.
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
Putian Zhou, Laurens Ganzeveld, Ditte Taipale, Üllar Rannik, Pekka Rantala, Matti Petteri Rissanen, Dean Chen, and Michael Boy
Atmos. Chem. Phys., 17, 14309–14332, https://doi.org/10.5194/acp-17-14309-2017, https://doi.org/10.5194/acp-17-14309-2017, 2017
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In boreal forest, there is a large number of gaseous organic compounds called biogenic volatile organic compounds (BVOCs). Within the canopy, they can be emitted from vegetation and soil, react with each other and other gases, be transported in the air, and be removed from vegetation and soil surfaces. We applied a numerical model to simulate these processes and found that these BVOCs can be divided into five categories according to the significance of their sources and sinks.
Federico Bianchi, Olga Garmash, Xucheng He, Chao Yan, Siddharth Iyer, Ida Rosendahl, Zhengning Xu, Matti P. Rissanen, Matthieu Riva, Risto Taipale, Nina Sarnela, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, and Heikki Junninen
Atmos. Chem. Phys., 17, 13819–13831, https://doi.org/10.5194/acp-17-13819-2017, https://doi.org/10.5194/acp-17-13819-2017, 2017
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Naturally charged highly oxidised molecules (HOMs) were characterized using advanced mass spectrometers. Two different classes of compounds, clustered with the nitrate and bisulfate ions, were identified: HOMs containing only carbon, hydrogen and oxygen and nitrogen-containing HOMs or organonitrates (ONs). They exhibit strong diurnal variations where HOMs peak during night and ONs during day. Finally, large clusters containing up to 40 carbon atoms (four oxidized
α-pinene units) were observed.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Lubna Dada, Pauli Paasonen, Tuomo Nieminen, Stephany Buenrostro Mazon, Jenni Kontkanen, Otso Peräkylä, Katrianne Lehtipalo, Tareq Hussein, Tuukka Petäjä, Veli-Matti Kerminen, Jaana Bäck, and Markku Kulmala
Atmos. Chem. Phys., 17, 6227–6241, https://doi.org/10.5194/acp-17-6227-2017, https://doi.org/10.5194/acp-17-6227-2017, 2017
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We studied new particle formation under clear-sky conditions in the boreal forest in southern Finland. We compared varying conditions between new particle events and nonevents. We then formulated a threshold value that separates new particle events from nonevents and reached a probability distribution for the frequency of new particle formation. This study serves as the basis for scientists aiming to improve their understanding of new particle formation.
Juan Hong, Mikko Äijälä, Silja A. K. Häme, Liqing Hao, Jonathan Duplissy, Liine M. Heikkinen, Wei Nie, Jyri Mikkilä, Markku Kulmala, Nønne L. Prisle, Annele Virtanen, Mikael Ehn, Pauli Paasonen, Douglas R. Worsnop, Ilona Riipinen, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 17, 4387–4399, https://doi.org/10.5194/acp-17-4387-2017, https://doi.org/10.5194/acp-17-4387-2017, 2017
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Estimates of volatility of secondary organic aerosols was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model and by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer data. About 16 % of the variation can be explained by the linear regression between the results from these two methods.
Wei Nie, Juan Hong, Silja A. K. Häme, Aijun Ding, Yugen Li, Chao Yan, Liqing Hao, Jyri Mikkilä, Longfei Zheng, Yuning Xie, Caijun Zhu, Zheng Xu, Xuguang Chi, Xin Huang, Yang Zhou, Peng Lin, Annele Virtanen, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, Jianzhen Yu, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 3659–3672, https://doi.org/10.5194/acp-17-3659-2017, https://doi.org/10.5194/acp-17-3659-2017, 2017
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HULIS are demonstrated to be important low-volatility, or even extremely low volatility, compounds in the organic aerosol phase. This sheds new light on the connection between atmospheric HULIS and ELVOCs. The interaction between HULIS and ammonium sulfate was found to decrease the volatility of the HULIS part in HULIS-AS mixed samples, indicating multiphase processes have the potential to lower the volatility of organic compounds in the aerosol phase.
Mikko Äijälä, Liine Heikkinen, Roman Fröhlich, Francesco Canonaco, André S. H. Prévôt, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 17, 3165–3197, https://doi.org/10.5194/acp-17-3165-2017, https://doi.org/10.5194/acp-17-3165-2017, 2017
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Mass spectrometric measurements commonly yield data on hundreds of variables over thousands of points in time. Refining and synthesising this “raw” data into chemical information necessitates the use of advanced, statistics-based data analysis techniques. Here we present an example of combining data dimensionality reduction (factorisation) with exploratory classification (clustering) and show that the results complement and broaden our current perspectives on aerosol chemical classification.
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
M. Dal Maso, L. Liao, J. Wildt, A. Kiendler-Scharr, E. Kleist, R. Tillmann, M. Sipilä, J. Hakala, K. Lehtipalo, M. Ehn, V.-M. Kerminen, M. Kulmala, D. Worsnop, and T. Mentel
Atmos. Chem. Phys., 16, 1955–1970, https://doi.org/10.5194/acp-16-1955-2016, https://doi.org/10.5194/acp-16-1955-2016, 2016
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In this paper, we present the first direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We found that the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength, and that the formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
R. L. Mauldin III, M. P. Rissanen, T. Petäjä, and M. Kulmala
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2015-398, https://doi.org/10.5194/amt-2015-398, 2016
Revised manuscript under review for AMT
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The manuscript describes a novel instrument for the measurement of OH, HO2+RO2, and other atmospheric species. The instrument described combines the chemical ionization techniques of nitrate CIMS, OH conversion to H2SO4, HO2+RO2 conversion to H2SO4, and high resolution time of flight mass spectroscopy into one system. By using one instrument to obtain spectra it is possible to compare spectra from the different modes and gain further chemical information towards peak identification.
J. Hong, J. Kim, T. Nieminen, J. Duplissy, M. Ehn, M. Äijälä, L. Q. Hao, W. Nie, N. Sarnela, N. L. Prisle, M. Kulmala, A. Virtanen, T. Petäjä, and V.-M. Kerminen
Atmos. Chem. Phys., 15, 11999–12009, https://doi.org/10.5194/acp-15-11999-2015, https://doi.org/10.5194/acp-15-11999-2015, 2015
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
P. Roldin, L. Liao, D. Mogensen, M. Dal Maso, A. Rusanen, V.-M. Kerminen, T. F. Mentel, J. Wildt, E. Kleist, A. Kiendler-Scharr, R. Tillmann, M. Ehn, M. Kulmala, and M. Boy
Atmos. Chem. Phys., 15, 10777–10798, https://doi.org/10.5194/acp-15-10777-2015, https://doi.org/10.5194/acp-15-10777-2015, 2015
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We used the ADCHAM model to study new particle formation events in the JPAC chamber. The model results show that the new particles may be formed by a kinetic type of nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of volatile organic compounds (VOCs). The observed particle growth may either be controlled by the condensation of semi- and low-volatililty organic compounds or by the formation of low-volatility compounds (oligomers) at the particle surface.
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
S. Schobesberger, A. Franchin, F. Bianchi, L. Rondo, J. Duplissy, A. Kürten, I. K. Ortega, A. Metzger, R. Schnitzhofer, J. Almeida, A. Amorim, J. Dommen, E. M. Dunne, M. Ehn, S. Gagné, L. Ickes, H. Junninen, A. Hansel, V.-M. Kerminen, J. Kirkby, A. Kupc, A. Laaksonen, K. Lehtipalo, S. Mathot, A. Onnela, T. Petäjä, F. Riccobono, F. D. Santos, M. Sipilä, A. Tomé, G. Tsagkogeorgas, Y. Viisanen, P. E. Wagner, D. Wimmer, J. Curtius, N. M. Donahue, U. Baltensperger, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 55–78, https://doi.org/10.5194/acp-15-55-2015, https://doi.org/10.5194/acp-15-55-2015, 2015
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We used an ion mass spectrometer at CERN's CLOUD chamber to investigate the detailed composition of ammonia--sulfuric acid ion clusters (of both polarities) as they initially form and then grow into aerosol particles, at atmospherically relevant conditions. We found that these clusters’ composition is mainly determined by the ratio of the precursor vapors and ranges from ammonia-free clusters to clusters containing > 1 ammonia per sulfuric acid. Acid--base bindings are a key formation mechanism.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
J. Wildt, T. F. Mentel, A. Kiendler-Scharr, T. Hoffmann, S. Andres, M. Ehn, E. Kleist, P. Müsgen, F. Rohrer, Y. Rudich, M. Springer, R. Tillmann, and A. Wahner
Atmos. Chem. Phys., 14, 2789–2804, https://doi.org/10.5194/acp-14-2789-2014, https://doi.org/10.5194/acp-14-2789-2014, 2014
J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä
Atmos. Meas. Tech., 7, 689–700, https://doi.org/10.5194/amt-7-689-2014, https://doi.org/10.5194/amt-7-689-2014, 2014
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
A. L. Vogel, M. Äijälä, A. L. Corrigan, H. Junninen, M. Ehn, T. Petäjä, D. R. Worsnop, M. Kulmala, L. M. Russell, J. Williams, and T. Hoffmann
Atmos. Chem. Phys., 13, 10933–10950, https://doi.org/10.5194/acp-13-10933-2013, https://doi.org/10.5194/acp-13-10933-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Viscosity of aqueous ammonium nitrate–organic particles: Equilibrium partitioning may be a reasonable assumption for most tropospheric conditions
Role of sea spray aerosol at the air–sea interface in transporting aromatic acids to the atmosphere
Modeling the influence of carbon branching structure on secondary organic aerosol formation via multiphase reactions of alkanes
Technical note: Characterization of a single-beam gradient force aerosol optical tweezer for droplet trapping, phase transition monitoring, and morphology studies
Soot aerosols from commercial aviation engines are poor ice-nucleating particles at cirrus cloud temperatures
Contribution of brown carbon to light absorption in emissions of European residential biomass combustion appliances
Measurement report: Water diffusion in single suspended phase-separated aerosols
Water activity and surface tension of aqueous ammonium sulfate and D-glucose aerosol nanoparticles
Jet aircraft lubrication oil droplets as contrail ice-forming particles
A study on the influence of inorganic ions, organic carbon and microstructure on the hygroscopic property of soot
Measurement report: The ice-nucleating activity of lichen sampled in a northern European boreal forest
Is transport of microplastics different from mineral particles? Idealized wind tunnel studies on polyethylene microspheres
Insights into secondary organic aerosol formation from the day- and nighttime oxidation of polycyclic aromatic hydrocarbons and furans in an oxidation flow reactor
Analysis of insoluble particles in hailstones in China
Influence of acidity on liquid–liquid phase transitions of mixed secondary organic aerosol (SOA) proxy–inorganic aerosol droplets
Deposition freezing, pore condensation freezing and adsorption: three processes, one description?
Measurements and calculations of enhanced side- and back-scattering of visible radiation by black carbon aggregates
Direct observation for relative-humidity-dependent mixing states of submicron particles containing organic surfactants and inorganic salts
Complex refractive index and single scattering albedo of Icelandic dust in the shortwave part of the spectrum
Volatility of aerosol particles from NO3 oxidation of various biogenic organic precursors
Saturation vapor pressure characterization of selected low-volatility organic compounds using a residence time chamber
Influence of the previous North Atlantic Oscillation (NAO) on the spring dust aerosols over North China
HUB: a method to model and extract the distribution of ice nucleation temperatures from drop-freezing experiments
Size-dependent hygroscopicity of levoglucosan and D-glucose aerosol nanoparticles
Technical note: Sublimation of frozen CsCl solutions in an environmental scanning electron microscope (ESEM) – determining the number and size of salt particles relevant to sea salt aerosols
Microphysics of liquid water in sub-10 nm ultrafine aerosol particles
Comparing the ice nucleation properties of the kaolin minerals kaolinite and halloysite
Physicochemical properties of charcoal aerosols derived from biomass pyrolysis affect their ice-nucleating abilities at cirrus and mixed-phase cloud conditions
Reconsideration of surface tension and phase state effects on cloud condensation nuclei activity based on the atomic force microscopy measurement
Hygroscopicity and CCN potential of DMS-derived aerosol particles
Hybrid water adsorption and solubility partitioning for aerosol hygroscopicity and droplet growth
Experimental development of a lake spray source function and its model implementation for Great Lakes surface emissions
The effectiveness of the coagulation sink of 3–10 nm atmospheric particles
What caused the interdecadal shift in the El Niño–Southern Oscillation (ENSO) impact on dust mass concentration over northwestern South Asia?
Measurement report: An exploratory study of fluorescence and cloud condensation nuclei activity of urban aerosols in San Juan, Puerto Rico
Viscosity and physical state of sucrose mixed with ammonium sulfate droplets
Distribution and stable carbon isotopic composition of dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in fresh and aged biomass burning aerosols
Time dependence of heterogeneous ice nucleation by ambient aerosols: laboratory observations and a formulation for models
Laboratory studies of ice nucleation onto bare and internally mixed soot–sulfuric acid particles
Enhanced soot particle ice nucleation ability induced by aggregate compaction and densification
Opinion: Insights into updating Ambient Air Quality Directive 2008/50/EC
On the evolution of sub- and super-saturated water uptake of secondary organic aerosol in chamber experiments from mixed precursors
Hygroscopicity of organic compounds as a function of organic functionality, water solubility, molecular weight, and oxidation level
Particle emissions from a modern heavy-duty diesel engine as ice nuclei in immersion freezing mode: a laboratory study on fossil and renewable fuels
Comparison of saturation vapor pressures of α-pinene + O3 oxidation products derived from COSMO-RS computations and thermal desorption experiments
Physical and chemical properties of black carbon and organic matter from different combustion and photochemical sources using aerodynamic aerosol classification
Technical note: Pyrolysis principles explain time-resolved organic aerosol release from biomass burning
The effect of (NH4)2SO4 on the freezing properties of non-mineral dust ice-nucleating substances of atmospheric relevance
Heterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperatures
Aerosol formation and growth rates from chamber experiments using Kalman smoothing
Liviana K. Klein, Allan K. Bertram, Andreas Zuend, Florence Gregson, and Ulrich K. Krieger
EGUsphere, https://doi.org/10.5194/egusphere-2024-1459, https://doi.org/10.5194/egusphere-2024-1459, 2024
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The viscosity of ammonium nitrate–sucrose–H2O was quantified with three methods ranging from liquid to solid state depending on the relative humidity. Moreover, the corresponding estimated internal aerosol mixing times remain below an hour for most tropospheric conditions, making equilibrium partitioning a reasonable assumption.
Yaru Song, Jianlong Li, Narcisse Tsona Tchinda, Kun Li, and Lin Du
Atmos. Chem. Phys., 24, 5847–5862, https://doi.org/10.5194/acp-24-5847-2024, https://doi.org/10.5194/acp-24-5847-2024, 2024
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Aromatic acids can be transferred from seawater to the atmosphere through bubble bursting. The air–sea transfer efficiency of aromatic acids was evaluated by simulating SSA generation with a plunging jet. As a whole, the transfer capacity of aromatic acids may depend on their functional groups and on the bridging effect of cations, as well as their concentration in seawater, as these factors influence the global emission flux of aromatic acids via SSA.
Azad Madhu, Myoseon Jang, and Yujin Jo
Atmos. Chem. Phys., 24, 5585–5602, https://doi.org/10.5194/acp-24-5585-2024, https://doi.org/10.5194/acp-24-5585-2024, 2024
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Secondary organic aerosol (SOA) formation from branched alkanes (BAs) was simulated using the UNIPAR model, which predicted SOA growth via multiphase reactions of hydrocarbons, and compared with chamber data. Product distributions (PDs) of BAs were created by extrapolating PDs of linear alkanes (LAs). To account for methyl branching, an autoxidation reduction factor was applied to PDs. BAs in diesel fuel were shown to produce a higher proportion of SOA compared with LAs.
Xiangyu Pei, Yikan Meng, Yueling Chen, Huichao Liu, Yao Song, Zhengning Xu, Fei Zhang, Thomas C. Preston, and Zhibin Wang
Atmos. Chem. Phys., 24, 5235–5246, https://doi.org/10.5194/acp-24-5235-2024, https://doi.org/10.5194/acp-24-5235-2024, 2024
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An aerosol optical tweezer (AOT) Raman spectroscopy system is developed to capture a single aerosol droplet for phase transition monitoring and morphology studies. Rapid droplet capture is achieved and accurate droplet size and refractive index are retrieved. Results indicate that mixed inorganic/organic droplets are more inclined to form core–shell morphology when RH decreases. The phase transitions of secondary mixed organic aerosol/inorganic droplets vary with their precursors.
Baptiste Testa, Lukas Durdina, Peter A. Alpert, Fabian Mahrt, Christopher H. Dreimol, Jacinta Edebeli, Curdin Spirig, Zachary C. J. Decker, Julien Anet, and Zamin A. Kanji
Atmos. Chem. Phys., 24, 4537–4567, https://doi.org/10.5194/acp-24-4537-2024, https://doi.org/10.5194/acp-24-4537-2024, 2024
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Laboratory experiments on the ice nucleation of real commercial aviation soot particles are investigated for their cirrus cloud formation potential. Our results show that aircraft-emitted soot in the upper troposphere will be poor ice-nucleating particles. Measuring the soot particle morphology and modifying their mixing state allow us to elucidate why these particles are ineffective at forming ice, in contrast to previously used soot surrogates.
Satish Basnet, Anni Hartikainen, Aki Virkkula, Pasi Yli-Pirilä, Miika Kortelainen, Heikki Suhonen, Laura Kilpeläinen, Mika Ihalainen, Sampsa Väätäinen, Juho Louhisalmi, Markus Somero, Jarkko Tissari, Gert Jakobi, Ralf Zimmermann, Antti Kilpeläinen, and Olli Sippula
Atmos. Chem. Phys., 24, 3197–3215, https://doi.org/10.5194/acp-24-3197-2024, https://doi.org/10.5194/acp-24-3197-2024, 2024
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Brown carbon (BrC) emissions were estimated, for residential wood combustion (RWC) from various northern European appliances, utilizing an extensive seven-wavelength aethalometer dataset and thermal–optical carbon analysis. The contribution of BrC370–950 to the absorption of visible light varied between 1 % and 21 %, and was linked with fuel moisture content and combustion efficiency. This study provides important information required for assessing the climate effects of RWC emissions.
Yu-Kai Tong, Zhijun Wu, Min Hu, and Anpei Ye
Atmos. Chem. Phys., 24, 2937–2950, https://doi.org/10.5194/acp-24-2937-2024, https://doi.org/10.5194/acp-24-2937-2024, 2024
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The interplay between aerosols and moisture is one of the most crucial atmospheric processes. However, to date, literature results on the influence of phase separation on water diffusion in aerosols are divergent. This work directly unveiled the water diffusion process in single suspended phase-separated microdroplets and quantitatively analyzed the diffusion rate and extent. The results show that diffusion limitations and certain molecule clusters existed in the phase-separated aerosols.
Eugene F. Mikhailov, Sergey S. Vlasenko, and Alexei A. Kiselev
Atmos. Chem. Phys., 24, 2971–2984, https://doi.org/10.5194/acp-24-2971-2024, https://doi.org/10.5194/acp-24-2971-2024, 2024
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Surface tension and water activity are key thermodynamic parameters determining the impact of atmospheric aerosols on human health and climate. However, these parameters are not well constrained for nanoparticles composed of organic and inorganic compounds. In this study, we determined for the first time the water activity and surface tension of mixed organic/inorganic nanodroplets by applying a differential Köhler analysis (DKA) to hygroscopic growth measurements.
Joel Ponsonby, Leon King, Benjamin J. Murray, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 2045–2058, https://doi.org/10.5194/acp-24-2045-2024, https://doi.org/10.5194/acp-24-2045-2024, 2024
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Aerosol emissions from aircraft engines contribute to the formation of contrails, which have a climate impact as important as that of aviation’s CO2 emissions. For the first time, we experimentally investigate the freezing behaviour of water droplets formed on jet lubrication oil aerosol. We show that they can activate to form water droplets and discuss their potential impact on contrail formation. Our study has implications for contrails produced by future aircraft engine and fuel technologies.
Zhanyu Su, Lanxiadi Chen, Yuan Liu, Peng Zhang, Tianzeng Chen, Biwu Chu, Mingjin Tang, Qingxin Ma, and Hong He
Atmos. Chem. Phys., 24, 993–1003, https://doi.org/10.5194/acp-24-993-2024, https://doi.org/10.5194/acp-24-993-2024, 2024
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In this study, different soot particles were analyzed to better understand their behavior. It was discovered that water-soluble substances in soot facilitate water adsorption at low humidity while increasing the number of water layers at high humidity. Soot from organic fuels exhibits hygroscopicity influenced by organic carbon and microstructure. Additionally, the presence of sulfate ions due to the oxidation of SO2 enhances soot's hygroscopicity.
Ulrike Proske, Michael P. Adams, Grace C. E. Porter, Mark Holden, Jaana Bäck, and Benjamin J. Murray
EGUsphere, https://doi.org/10.5194/egusphere-2023-2780, https://doi.org/10.5194/egusphere-2023-2780, 2024
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Ice nucleating particles aid freezing of water droplets in clouds and thus modify clouds' properties. During a campaign in the boreal forest in Finland, substantial concentrations of biological ice nucleating particles were observed, despite many of their potential biological sources being snow covered. We sampled lichen in this location and tested its ice nculeation ability in the laboratory. We find that indeed the lichen harbours INPs, which may be important in such snow covered environments.
Eike Maximilian Esders, Sebastian Sittl, Inka Krammel, Wolfgang Babel, Georg Papastavrou, and Christoph Karl Thomas
Atmos. Chem. Phys., 23, 15835–15851, https://doi.org/10.5194/acp-23-15835-2023, https://doi.org/10.5194/acp-23-15835-2023, 2023
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Do microplastics behave differently from mineral particles when they are exposed to wind? We observed plastic and mineral particles in a wind tunnel and measured at what wind speeds the particles start to move. The results indicate that microplastics start to move at smaller wind speeds as they weigh less and are less sticky. Hence, we think that microplastics also move more easily in the environment.
Abd El Rahman El Mais, Barbara D'Anna, Luka Drinovec, Andrew T. Lambe, Zhe Peng, Jean-Eudes Petit, Olivier Favez, Selim Aït-Aïssa, and Alexandre Albinet
Atmos. Chem. Phys., 23, 15077–15096, https://doi.org/10.5194/acp-23-15077-2023, https://doi.org/10.5194/acp-23-15077-2023, 2023
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Polycyclic aromatic hydrocarbons (PAHS) and furans are key precursors of secondary organic aerosols (SOAs) related to biomass burning emissions. We evaluated and compared the formation yields, and the physical and light absorption properties, of laboratory-generated SOAs from the oxidation of such compounds for both, day- and nighttime reactivities. The results illustrate that PAHs are large SOA precursors and may contribute significantly to the biomass burning brown carbon in the atmosphere.
Haifan Zhang, Xiangyu Lin, Qinghong Zhang, Kai Bi, Chan-Pang Ng, Yangze Ren, Huiwen Xue, Li Chen, and Zhuolin Chang
Atmos. Chem. Phys., 23, 13957–13971, https://doi.org/10.5194/acp-23-13957-2023, https://doi.org/10.5194/acp-23-13957-2023, 2023
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This work is the first study to simultaneously analyze the number concentrations and species of insoluble particles in hailstones. The size distribution of insoluble particles for each species vary greatly in different hailstorms but little in shells. Two classic size distribution modes of organics and dust were fitted for the description of insoluble particles in deep convection. Combining this study with future experiments will lead to refinement of weather and climate models.
Yueling Chen, Xiangyu Pei, Huichao Liu, Yikan Meng, Zhengning Xu, Fei Zhang, Chun Xiong, Thomas C. Preston, and Zhibin Wang
Atmos. Chem. Phys., 23, 10255–10265, https://doi.org/10.5194/acp-23-10255-2023, https://doi.org/10.5194/acp-23-10255-2023, 2023
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The impact of acidity on the phase transition behavior of levitated aerosol particles was examined. Our results revealed that lower acidity decreases the separation relative humidity of aerosol droplets mixed with ammonium sulfate and secondary organic aerosol proxy. Our research suggests that in real atmospheric conditions, with the high acidity found in many ambient aerosol particles, droplets encounter heightened impediments to phase separation and tend to display a homogeneous structure.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, https://doi.org/10.5194/acp-23-10057-2023, 2023
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Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
Carynelisa Haspel, Cuiqi Zhang, Martin J. Wolf, Daniel J. Cziczo, and Maor Sela
Atmos. Chem. Phys., 23, 10091–10115, https://doi.org/10.5194/acp-23-10091-2023, https://doi.org/10.5194/acp-23-10091-2023, 2023
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Small particles, commonly termed aerosols, can be found throughout the atmosphere and come from both natural and anthropogenic sources. One important type of aerosol is black carbon (BC). In this study, we conducted laboratory measurements of light scattering by particles meant to mimic atmospheric BC and compared them to calculations of scattering. We find that it is likely that calculations underpredict the scattering by BC particles of certain polarizations of light in certain directions.
Chun Xiong, Binyu Kuang, Fei Zhang, Xiangyu Pei, Zhengning Xu, and Zhibin Wang
Atmos. Chem. Phys., 23, 8979–8991, https://doi.org/10.5194/acp-23-8979-2023, https://doi.org/10.5194/acp-23-8979-2023, 2023
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In hydration, an apparent water diffusion hindrance by an organic surfactant shell was confirmed, raising the inorganic deliquescence relative humidity (RH) to a nearly saturated condition. In dehydration, phase separations were observed for inorganic surfactant systems, showing a strong dependence on the organic molecular
oxygen-to-carbon ratio. Our results could improve fundamental knowledge about aerosol mixing states and decrease uncertainty in model estimations of global radiative effects.
Clarissa Baldo, Paola Formenti, Claudia Di Biagio, Gongda Lu, Congbo Song, Mathieu Cazaunau, Edouard Pangui, Jean-Francois Doussin, Pavla Dagsson-Waldhauserova, Olafur Arnalds, David Beddows, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys., 23, 7975–8000, https://doi.org/10.5194/acp-23-7975-2023, https://doi.org/10.5194/acp-23-7975-2023, 2023
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This paper presents new shortwave spectral complex refractive index and single scattering albedo data for Icelandic dust. Our results show that the imaginary part of the complex refractive index of Icelandic dust is at the upper end of the range of low-latitude dust. Furthermore, we observed that Icelandic dust is more absorbing towards the near-infrared, which we attribute to its high magnetite content. These findings are important for modeling dust aerosol radiative effects in the Arctic.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
Atmos. Chem. Phys., 23, 7347–7362, https://doi.org/10.5194/acp-23-7347-2023, https://doi.org/10.5194/acp-23-7347-2023, 2023
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The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate-initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system, and our simulations produced variable results with different parameterizations which warrant a re-evaluation of the treatment of the nitrate functional group.
Zijun Li, Noora Hyttinen, Miika Vainikka, Olli-Pekka Tikkasalo, Siegfried Schobesberger, and Taina Yli-Juuti
Atmos. Chem. Phys., 23, 6863–6877, https://doi.org/10.5194/acp-23-6863-2023, https://doi.org/10.5194/acp-23-6863-2023, 2023
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The saturation vapor pressure (psat) of low-volatility organic compounds (LVOCs) governs their partitioning between the gas and particle phases. To estimate the psat of selected LVOCs, we performed particle evaporation measurements in a residence time chamber at a temperature setting relevant to atmospheric aerosol formation and conducted state-of-the-art computational calculations. We found good agreement between the experimentally measured and model-estimated psat values for most LVOCs.
Yan Li, Falei Xu, Juan Feng, Mengying Du, Wenjun Song, Chao Li, and Wenjing Zhao
Atmos. Chem. Phys., 23, 6021–6042, https://doi.org/10.5194/acp-23-6021-2023, https://doi.org/10.5194/acp-23-6021-2023, 2023
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There is a significantly negative relationship between boreal winter North Atlantic Oscillation (NAO) and dust aerosols (DAs) in the eastern part of China (30–40°N, 105–120°E), which is not a DA source area but is severely affected by the dust events (DEs). Under the effect of the NAO negative phase, main atmospheric circulation during the DEs is characterized by variation of the transient eddy flux. The work is of reference value to the prediction of DEs and the understanding of their causes.
Ingrid de Almeida Ribeiro, Konrad Meister, and Valeria Molinero
Atmos. Chem. Phys., 23, 5623–5639, https://doi.org/10.5194/acp-23-5623-2023, https://doi.org/10.5194/acp-23-5623-2023, 2023
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Ice formation is a key atmospheric process facilitated by a wide range of aerosols. We present a method to model and interpret ice nucleation experiments and extract the distribution of the potency of nucleation sites. We use the method to optimize the conditions of laboratory sampling and extract distributions of ice nucleation temperatures from bacteria, fungi, and pollen. These reveal unforeseen subpopulations of nuclei in these systems and how they respond to changes in their environment.
Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774, https://doi.org/10.5194/acp-23-4763-2023, https://doi.org/10.5194/acp-23-4763-2023, 2023
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We investigate the hygroscopic behavior of levoglucosan and D-glucose nanoparticles using a nano-HTDMA. There is a weak size dependence of the hygroscopic growth factor of levoglucosan and D-glucose with diameters down to 20 nm, while a strong size dependence of the hygroscopic growth factor of D-glucose has been clearly observed in the size range 6 to 20 nm. The use of the DKA method leads to good agreement with the hygroscopic growth factor of glucose nanoparticles with diameters down to 6 nm.
Lubica Vetráková, Vilém Neděla, Kamila Závacká, Xin Yang, and Dominik Heger
Atmos. Chem. Phys., 23, 4463–4488, https://doi.org/10.5194/acp-23-4463-2023, https://doi.org/10.5194/acp-23-4463-2023, 2023
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Salt aerosols are important to polar atmospheric chemistry and global climate. Therefore, we utilized a unique electron microscope to identify the most suitable conditions for formation of the small salt (CsCl) particles, proxies of the aerosols, from sublimating salty snow. Very low sublimation temperature and low salt concentration are needed for formation of such particles. These observations may help us to better understand polar spring ozone depletion and bromine explosion events.
Xiaohan Li and Ian C. Bourg
Atmos. Chem. Phys., 23, 2525–2556, https://doi.org/10.5194/acp-23-2525-2023, https://doi.org/10.5194/acp-23-2525-2023, 2023
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Aerosol particles with sizes smaller than 50 nm impact cloud formation and precipitation. Representation of this effect is hindered by limited understanding of the properties of liquid water in these particles. Our simulations of aerosol particles containing salt or organic compounds reveal that water enters a less cohesive phase at droplet sizes below 4 nm. This effect causes important deviations from theoretical predictions of aerosol properties, including phase state and hygroscopic growth.
Kristian Klumpp, Claudia Marcolli, Ana Alonso-Hellweg, Christopher H. Dreimol, and Thomas Peter
Atmos. Chem. Phys., 23, 1579–1598, https://doi.org/10.5194/acp-23-1579-2023, https://doi.org/10.5194/acp-23-1579-2023, 2023
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The prerequisites of a particle surface for efficient ice nucleation are still poorly understood. This study compares the ice nucleation activity of two chemically identical but morphologically different minerals (kaolinite and halloysite). We observe, on average, not only higher ice nucleation activities for halloysite than kaolinite but also higher diversity between individual samples. We identify the particle edges as being the most likely site for ice nucleation.
Fabian Mahrt, Carolin Rösch, Kunfeng Gao, Christopher H. Dreimol, Maria A. Zawadowicz, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 1285–1308, https://doi.org/10.5194/acp-23-1285-2023, https://doi.org/10.5194/acp-23-1285-2023, 2023
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Major aerosol types emitted by biomass burning include soot, ash, and charcoal particles. Here, we investigated the ice nucleation activity of 400 nm size-selected particles of two different pyrolyis-derived charcoal types in the mixed phase and cirrus cloud regime. We find that ice nucleation is constrained to cirrus cloud conditions, takes place via pore condensation and freezing, and is largely governed by the particle porosity and mineral content.
Chun Xiong, Xueyan Chen, Xiaolei Ding, Binyu Kuang, Xiangyu Pei, Zhengning Xu, Shikuan Yang, Huan Hu, and Zhibin Wang
Atmos. Chem. Phys., 22, 16123–16135, https://doi.org/10.5194/acp-22-16123-2022, https://doi.org/10.5194/acp-22-16123-2022, 2022
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Water surface tension is applied widely in current aerosol–cloud models but could be inappropriate in the presence of atmospheric surfactants. With cloud condensation nuclei (CCN) activity and atomic force microscopy (AFM) measurement results of mixed inorganic salt and dicarboxylic acid particles, we concluded that surface tension reduction and phase state should be carefully considered in aerosol–cloud interactions. Our results could help to decease uncertainties in climate models.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Kanishk Gohil, Chun-Ning Mao, Dewansh Rastogi, Chao Peng, Mingjin Tang, and Akua Asa-Awuku
Atmos. Chem. Phys., 22, 12769–12787, https://doi.org/10.5194/acp-22-12769-2022, https://doi.org/10.5194/acp-22-12769-2022, 2022
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The Hybrid Activity Model (HAM) is a promising new droplet growth model that can be potentially used for the analysis of any type of atmospheric compound. HAM may potentially improve the representation of hygroscopicity of organic aerosols in large-scale global climate models (GCMs), hence reducing the uncertainties in the climate forcing due to the aerosol indirect effect.
Charbel Harb and Hosein Foroutan
Atmos. Chem. Phys., 22, 11759–11779, https://doi.org/10.5194/acp-22-11759-2022, https://doi.org/10.5194/acp-22-11759-2022, 2022
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A model representation of lake spray aerosol (LSA) ejection from freshwater breaking waves is crucial for understanding their climatic and public health impacts. We develop an LSA emission parameterization and implement it in an atmospheric model to investigate Great Lakes surface emissions. We find that the same breaking wave is likely to produce fewer aerosols in freshwater than in saltwater and that Great Lakes emissions influence the regional aerosol burden and can reach the cloud layer.
Runlong Cai, Ella Häkkinen, Chao Yan, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 11529–11541, https://doi.org/10.5194/acp-22-11529-2022, https://doi.org/10.5194/acp-22-11529-2022, 2022
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The influences of new particle formation on the climate and air quality are governed by particle survival, which has been under debate due to uncertainties in the coagulation sink. Here we measure the coagulation coefficient of sub-10 nm particles and demonstrate that collisions between the freshly nucleated and background particles can effectively lead to coagulation. We further show that the effective coagulation sink is consistent with the new particle formation measured in urban Beijing.
Lamei Shi, Jiahua Zhang, Da Zhang, Jingwen Wang, Xianglei Meng, Yuqin Liu, and Fengmei Yao
Atmos. Chem. Phys., 22, 11255–11274, https://doi.org/10.5194/acp-22-11255-2022, https://doi.org/10.5194/acp-22-11255-2022, 2022
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Dust impacts climate and human life. Analyzing the interdecadal change in dust activity and its influence factors is crucial for disaster mitigation. Based on a linear regression method, this study revealed the interdecadal variability of relationships between ENSO and dust over northwestern South Asia from 1982 to 2014 and analyzed the effects of atmospheric factors on this interdecadal variability. The result sheds new light on numerical simulation involving the interdecadal variation of dust.
Bighnaraj Sarangi, Darrel Baumgardner, Benjamin Bolaños-Rosero, and Olga L. Mayol-Bracero
Atmos. Chem. Phys., 22, 9647–9661, https://doi.org/10.5194/acp-22-9647-2022, https://doi.org/10.5194/acp-22-9647-2022, 2022
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Here, the fluorescent characteristics and cloud-forming efficiency of aerosols at an urban site in Puerto Rico are discussed. The results from this pilot study highlight the capabilities of ultraviolet-induced fluorescence (UV-IF) measurements for characterizing the properties of fluorescing aerosol particles, as they relate to the daily evolution of primary biological aerosol particles. This work has established a database of measurements on which future, longer-term studies will be initiated.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817, https://doi.org/10.5194/acp-22-8805-2022, https://doi.org/10.5194/acp-22-8805-2022, 2022
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In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Minxia Shen, Kin Fai Ho, Wenting Dai, Suixin Liu, Ting Zhang, Qiyuan Wang, Jingjing Meng, Judith C. Chow, John G. Watson, Junji Cao, and Jianjun Li
Atmos. Chem. Phys., 22, 7489–7504, https://doi.org/10.5194/acp-22-7489-2022, https://doi.org/10.5194/acp-22-7489-2022, 2022
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Looking at characteristics and δ13C compositions of dicarboxylic acids and related compounds in BB aerosols, we used a combined combustion and aging system to generate fresh and aged aerosols from burning straw. The results showed the emission factors (EFaged) of total diacids of aging experiments were around an order of magnitude higher than EFfresh. This meant that dicarboxylic acids are involved with secondary photochemical processes in the atmosphere rather than primary emissions from BB.
Jonas K. F. Jakobsson, Deepak B. Waman, Vaughan T. J. Phillips, and Thomas Bjerring Kristensen
Atmos. Chem. Phys., 22, 6717–6748, https://doi.org/10.5194/acp-22-6717-2022, https://doi.org/10.5194/acp-22-6717-2022, 2022
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Long-lived cold-layer clouds at subzero temperatures are observed to be remarkably persistent in their generation of ice particles and snow precipitation. There is uncertainty about why this is so. This motivates the present lab study to observe the long-term ice-nucleating ability of aerosol samples from the real troposphere. Time dependence of their ice nucleation is observed to be weak in lab experiments exposing the samples to isothermal conditions for up to about 10 h.
Kunfeng Gao, Chong-Wen Zhou, Eszter J. Barthazy Meier, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 5331–5364, https://doi.org/10.5194/acp-22-5331-2022, https://doi.org/10.5194/acp-22-5331-2022, 2022
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Incomplete combustion of fossil fuel produces carbonaceous particles called soot. These particles can affect cloud formation by acting as centres for droplet or ice formation. The atmospheric residence time of soot particles is of the order of days to weeks, which can result in them becoming coated by various trace species in the atmosphere such as acids. In this study, we quantify the cirrus cloud-forming ability of soot particles coated with the atmospherically ubiquitous sulfuric acid.
Kunfeng Gao, Franz Friebel, Chong-Wen Zhou, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 4985–5016, https://doi.org/10.5194/acp-22-4985-2022, https://doi.org/10.5194/acp-22-4985-2022, 2022
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Soot particles impact cloud formation and radiative properties in the upper atmosphere where aircraft emit carbonaceous particles. We use cloud chambers to mimic the upper atmosphere temperature and humidity to test the influence of the morphology of the soot particles on ice cloud formation. For particles larger than 200 nm, the compacted (densified) samples have a higher affinity for ice crystal formation in the cirrus regime than the fluffy (un-compacted) soot particles of the same sample.
Joel Kuula, Hilkka Timonen, Jarkko V. Niemi, Hanna E. Manninen, Topi Rönkkö, Tareq Hussein, Pak Lun Fung, Sasu Tarkoma, Mikko Laakso, Erkka Saukko, Aino Ovaska, Markku Kulmala, Ari Karppinen, Lasse Johansson, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 4801–4808, https://doi.org/10.5194/acp-22-4801-2022, https://doi.org/10.5194/acp-22-4801-2022, 2022
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Modern and up-to-date policies and air quality management strategies are instrumental in tackling global air pollution. As the European Union is preparing to revise Ambient Air Quality Directive 2008/50/EC, this paper initiates discussion on selected features of the directive that we believe would benefit from a reassessment. The scientific community has the most recent and deepest understanding of air pollution; thus, its contribution is essential.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166, https://doi.org/10.5194/acp-22-4149-2022, https://doi.org/10.5194/acp-22-4149-2022, 2022
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Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Shuang Han, Juan Hong, Qingwei Luo, Hanbing Xu, Haobo Tan, Qiaoqiao Wang, Jiangchuan Tao, Yaqing Zhou, Long Peng, Yao He, Jingnan Shi, Nan Ma, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3985–4004, https://doi.org/10.5194/acp-22-3985-2022, https://doi.org/10.5194/acp-22-3985-2022, 2022
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We present the hygroscopicity of 23 organic species with different physicochemical properties using a hygroscopicity tandem differential mobility analyzer (HTDMA) and compare the results with previous studies. Based on the hygroscopicity parameter κ, the influence of different physicochemical properties that potentially drive hygroscopicity, such as the functionality, water solubility, molar volume, and O : C ratio of organics, are examined separately.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
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We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182, https://doi.org/10.5194/acp-21-16161-2021, https://doi.org/10.5194/acp-21-16161-2021, 2021
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Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
Mariam Fawaz, Anita Avery, Timothy B. Onasch, Leah R. Williams, and Tami C. Bond
Atmos. Chem. Phys., 21, 15605–15618, https://doi.org/10.5194/acp-21-15605-2021, https://doi.org/10.5194/acp-21-15605-2021, 2021
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Biomass burning is responsible for 90 % of the emissions of primary organic aerosols to the atmosphere. Emissions from biomass burning sources are considered chaotic. In this work, we developed a controlled experimental approach to understand the controlling factors in emission. Our results showed that emissions are repeatable and deterministic and that emissions from wood can be constrained.
Soleil E. Worthy, Anand Kumar, Yu Xi, Jingwei Yun, Jessie Chen, Cuishan Xu, Victoria E. Irish, Pierre Amato, and Allan K. Bertram
Atmos. Chem. Phys., 21, 14631–14648, https://doi.org/10.5194/acp-21-14631-2021, https://doi.org/10.5194/acp-21-14631-2021, 2021
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We studied the effect of (NH4)2SO4 on the immersion freezing of non-mineral dust ice-nucleating substances (INSs) and mineral dusts. (NH4)2SO4 had no effect on the median freezing temperature of 9 of the 10 tested non-mineral dust INSs, slightly decreased that of the other, and increased that of all the mineral dusts. The difference in the response of mineral dust and non-mineral dust INSs to (NH4)2SO4 suggests that they nucleate ice and/or interact with (NH4)2SO4 via different mechanisms.
Robert Wagner, Luisa Ickes, Allan K. Bertram, Nora Els, Elena Gorokhova, Ottmar Möhler, Benjamin J. Murray, Nsikanabasi Silas Umo, and Matthew E. Salter
Atmos. Chem. Phys., 21, 13903–13930, https://doi.org/10.5194/acp-21-13903-2021, https://doi.org/10.5194/acp-21-13903-2021, 2021
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Sea spray aerosol particles are a mixture of inorganic salts and organic matter from phytoplankton organisms. At low temperatures in the upper troposphere, both inorganic and organic constituents can induce the formation of ice crystals and thereby impact cloud properties and climate. In this study, we performed experiments in a cloud simulation chamber with particles produced from Arctic seawater samples to quantify the relative contribution of inorganic and organic species in ice formation.
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.
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Short summary
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.
Cyclohexene resembles certain relatively complex compounds in the atmosphere that through...
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