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ACP | Articles | Volume 20, issue 5
Atmos. Chem. Phys., 20, 3151–3180, 2020
https://doi.org/10.5194/acp-20-3151-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-3151-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 3151–3180, 2020
https://doi.org/10.5194/acp-20-3151-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-3151-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
Research article 16 Mar 2020
Research article | 16 Mar 2020
Long-term sub-micrometer aerosol chemical composition in the boreal forest: inter- and intra-annual variability
Liine Heikkinen et al.
Related authors
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. Discuss., https://doi.org/10.5194/acp-2020-868, https://doi.org/10.5194/acp-2020-868, 2020
Preprint under review for ACP
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In many locations worldwide aerosol particles have 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 omposition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we developed 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.
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. Discuss., https://doi.org/10.5194/acp-2020-648, https://doi.org/10.5194/acp-2020-648, 2020
Preprint under review for ACP
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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 formation pathways of atmospheric organic vapors, i.e., terpenes and their oxidation products with varying oxidation degrees. This study provides a more comprehensive picture of gas-phase source identifications of organic compounds.
Mikhail Paramonov, Saskia Drossaart van Dusseldorp, Ellen Gute, Jonathan P. D. Abbatt, Paavo Heikkilä, Jorma Keskinen, Xuemeng Chen, Krista Luoma, Liine Heikkinen, Liqing Hao, Tuukka Petäjä, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 6687–6706, https://doi.org/10.5194/acp-20-6687-2020, https://doi.org/10.5194/acp-20-6687-2020, 2020
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Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland in the winter–spring of 2018. It was found that no single parameter could be used to predict the INP number concentration at the measurement location during the examined time period. It was also not possible to identify physical and chemical properties of ambient INPs despite the complexity of the instrumental set-up. Therefore, this paper addresses the necessity for future INP measurements.
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.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-248, https://doi.org/10.5194/acp-2020-248, 2020
Revised manuscript accepted for ACP
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By applying both OA-PMF and Size-PMF at the same urban measurement site in Beijing, similar particle source-types, including vehicular emissions, cooking emissions and secondary formation-related sources were resolved by both frameworks and agreed well. It is also found that in the absence of new-particle formation, vehicular and cooking emissions dominate the particle number concentration while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
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.
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.
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.
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.
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.
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
Janne Lampilahti, Hanna Elina Manninen, Katri Leino, Riikka Väänänen, Antti Manninen, Stephany Buenrostro Mazon, Tuomo Nieminen, Matti Leskinen, Joonas Enroth, Marja Bister, Sergej Zilitinkevich, Juha Kangasluoma, Heikki Järvinen, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 20, 11841–11854, https://doi.org/10.5194/acp-20-11841-2020, https://doi.org/10.5194/acp-20-11841-2020, 2020
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In this work, by using co-located airborne and ground-based measurements, we show that counter-rotating horizontal circulations in the planetary boundary layer (roll vortices) frequently enhance regional new particle formation or induce localized bursts of new particle formation. These observations can be explained by the ability of the rolls to efficiently lift low-volatile vapors emitted from the surface to the top of the boundary layer where new particle formation is more favorable.
Jose Ruiz-Jimenez, Magdalena Okuljar, Outi-Maaria Sietiö, Giorgia Demaria, Thanaporn Liangsupree, Elisa Zagatti, Juho Aalto, Kari Hartonen, Jussi Heinonsalo, Jaana Bäck, Tuukka Petäjä, and Marja-Liisa Riekkola
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1065, https://doi.org/10.5194/acp-2020-1065, 2020
Preprint under review for ACP
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Chemical compounds and microbes were determined in aerosol particles collected at Hyytiälä forestry field station in Finland. These results, and other data collected, clarified relationships between the aerosol composition and the particle size, effects of atmospheric, meteorological and environmental parameters on aerosol composition, presence of chemicals originating from microbes in aerosols, and connections between gas phase compounds in air and microbiological composition of aerosols.
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.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-973, https://doi.org/10.5194/acp-2020-973, 2020
Preprint under review for ACP
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction (RF) of •OH among detected radicals, but negatively correlated with the RF of C-centered radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Lubna Dada, Ilona Ylivinkka, Rima Baalbaki, Chang Li, Yishuo Guo, Chao Yan, Lei Yao, Nina Sarnela, Tuija Jokinen, Kaspar R. Daellenbach, Rujing Yin, Chenjuan Deng, Biwu Chu, Tuomo Nieminen, Yonghong Wang, Zhuohui Lin, Roseline C. Thakur, Jenni Kontkanen, Dominik Stolzenburg, Mikko Sipilä, Tareq Hussein, Pauli Paasonen, Federico Bianchi, Imre Salma, Tamás Weidinger, Michael Pikridas, Jean Sciare, Jingkun Jiang, Yongchun Liu, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 20, 11747–11766, https://doi.org/10.5194/acp-20-11747-2020, https://doi.org/10.5194/acp-20-11747-2020, 2020
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We rely on sulfuric acid measurements in four contrasting environments, Hyytiälä, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment, and heavily polluted megacity, respectively, in order to define the sources and sinks of sulfuric acid in these environments and to derive a new sulfuric acid proxy to be utilized in locations and during periods when it is not measured.
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. Discuss., https://doi.org/10.5194/acp-2020-923, https://doi.org/10.5194/acp-2020-923, 2020
Preprint under review for ACP
Jenni Kontkanen, Chenjuan Deng, Yueyun Fu, Lubna Dada, Ying Zhou, Jing Cai, Kaspar R. Daellenbach, Simo Hakala, Tom V. Kokkonen, Zhuohui Lin, Yongchun Liu, Yonghong Wang, Chao Yan, Tuukka Petäjä, Jingkun Jiang, Markku Kulmala, and Pauli Paasonen
Atmos. Chem. Phys., 20, 11329–11348, https://doi.org/10.5194/acp-20-11329-2020, https://doi.org/10.5194/acp-20-11329-2020, 2020
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To estimate the impacts of atmospheric aerosol particles on air quality, knowledge of size distributions of particles emitted from anthropogenic sources is needed. We introduce a new method for determining size-resolved particle number emissions from measured particle size distributions. We apply our method to data measured in Beijing, China. We find that particle number emissions at our site are dominated by emissions of particles smaller than 30 nm, originating mainly from traffic.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Tommy Chan, Runlong Cai, Lauri R. Ahonen, Yiliang Liu, Ying Zhou, Joonas Vanhanen, Lubna Dada, Yan Chao, Yongchun Liu, Lin Wang, Markku Kulmala, and Juha Kangasluoma
Atmos. Meas. Tech., 13, 4885–4898, https://doi.org/10.5194/amt-13-4885-2020, https://doi.org/10.5194/amt-13-4885-2020, 2020
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Using a particle size magnifier (PSM; Airmodus, Finland), we determined the particle size distribution using four inversion methods and compared each method to the others to establish their strengths and weaknesses. Furthermore, we provided a step-by-step procedure on how to invert measured data using the PSM. Finally, we provided recommendations, code and data related to the data inversion. This is an important paper, as no operating procedure exists regarding how to process measured PSM data.
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. Discuss., https://doi.org/10.5194/acp-2020-636, https://doi.org/10.5194/acp-2020-636, 2020
Preprint under review for ACP
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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, thus motivating the development of proxies. Using data collected in two different volcanic plumes, we show, in these specific conditions, the good performance of a proxy from the literature and highlight as well the benefit of the newly developed proxies for the prediction of the highest [H2SO4] concentrations.
Krista Luoma, Aki Virkkula, Pasi Aalto, Katrianne Lehtipalo, Tuukka Petäjä, and Markku Kulmala
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-325, https://doi.org/10.5194/amt-2020-325, 2020
Preprint under review for AMT
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The study presents a comparison of three different absorption photometers that measured ambient aerosol particles at a boreal forest site. The study aims to better understand problems related to filter-based measurements. Results show how different correction algorithms, which are used to produce the data, affect the derived optical properties of aerosol particles.
Dimitrios Bousiotis, Francis D. Pope, David C. Beddows, Manuel Dall’Osto, Andreas Massling, Jacob Klenø Nøjgaard, Claus Nørdstrom, Jarkko V. Niemi, Harri Portin, Tuukka Petäjä, Noemi Perez, Andrés Alastuey, Xavier Querol, Giorgos Kouvarakis, Stergios Vratolis, Konstantinos Eleftheriadis, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Thomas Tuch, and Roy M. Harrison
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-414, https://doi.org/10.5194/acp-2020-414, 2020
Preprint under review for ACP
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Formation of new particles is a key process in the atmosphere. New Particle Formation events arising from nucleation of gaseous precursors have been analysed in extensive datasets from thirteen sites in five European countries in terms of frequency, nucleation rate and particle growth rate, with several common features and many differences identified. Although nucleation frequencies are lower at roadside sites, nucleation rates and particle growth rates are typically higher.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-281, https://doi.org/10.5194/gmd-2020-281, 2020
Preprint under review for GMD
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. Discuss., https://doi.org/10.5194/acp-2020-868, https://doi.org/10.5194/acp-2020-868, 2020
Preprint under review for ACP
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In many locations worldwide aerosol particles have 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 omposition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we developed 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.
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-694, https://doi.org/10.5194/acp-2020-694, 2020
Preprint under review for ACP
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Cyclohexene resembles certain relatively complex compounds present in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOM) formed in cyclohexene ozonolysis, the relationship between their chemical composition and tendency to condense onto seed aerosol, and the effect of NOx pollutants on their signals. Two existing models were also tested in their ability to predict the volatility of the HOMs.
Andrea Cuesta-Mosquera, Griša Močnik, Luka Drinovec, Thomas Müller, Sascha Pfeifer, María Cruz Minguillón, Briel Björn, Paul Buckley, Vadimas Dudoitis, Javier Fernández-García, María Fernández-Amado, Joel Ferreira De Brito, Harald Flentje, Eimear Heffernan, Nikolaos Kalivitis, Athina-Cerise Kalogridis, Hannes Keernik, Luminita Marmureanu, Krista Luoma, Angela Marinoni, Michael Pikridas, Gerhard Schauer, Norbert Serfozo, Henri Servomaa, Gloria Titos, Jesús Yus-Díez, Natalia Zioła, and Alfred Wiedensohler
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-344, https://doi.org/10.5194/amt-2020-344, 2020
Preprint under review for AMT
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Twenty-three aethalometers from European monitoring networks of black carbon mass concentrations, were characterized and intercompared. Measurements of black carbon must be conducted with instruments operating in a quality checked and assured conditions to generate reliable and comparable data. The influence of different aerosol sources, maintenance activities, and the filter material, in the instrumental variabilities were investigated. Good agreements and in general low deviations were seen.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
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, Åsa Halquist, Mikael Ehn, Astrid Kiendler-Scharr, Thomas F. Mentel, Gordon McFiggans, Mattias Halquist, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-819, https://doi.org/10.5194/acp-2020-819, 2020
Preprint under review for ACP
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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 can aid identifying functionality.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-264, https://doi.org/10.5194/amt-2020-264, 2020
Preprint under review for AMT
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically-relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
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. Discuss., https://doi.org/10.5194/amt-2020-267, https://doi.org/10.5194/amt-2020-267, 2020
Preprint under review for AMT
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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.
Dimitrios Bousiotis, James Brean, Francis Pope, Manuel Dall'Osto, Xavier Querol, Andres Alastuey, Noemi Perez, Tuukka Petäjä, Andreas Massling, Jacob Klenø Nøjgaard, Claus Nørdstrom, Giorgos Kouvarakis, Stergios Vratolis, Konstantinos Eleftheriadis, Jarkko V. Niemi, Harri Portin, and Roy M. Harrison
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-555, https://doi.org/10.5194/acp-2020-555, 2020
Revised manuscript under review for ACP
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New Particle Formation events from 16 sites over Europe have been studied and the influence of meteorological and atmospheric composition variables has been investigated. Some variables like solar radiation intensity or temperature have a positive effect upon the occurrence of these events, while others have a negative effect, affecting different aspects such as the rate at which particles are formed or grow. This effect varies depending on the site type and magnitude of these variables.
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.
Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-683, https://doi.org/10.5194/acp-2020-683, 2020
Preprint under review for ACP
Martine Collaud Coen, Elisabeth Andrews, Andrés Alastuey, Todor Petkov Arsov, John Backman, Benjamin T. Brem, Nicolas Bukowiecki, Cédric Couret, Konstantinos Eleftheriadis, Harald Flentje, Markus Fiebig, Martin Gysel-Beer, Jenny L. Hand, András Hoffer, Rakesh Hooda, Christoph Hueglin, Warren Joubert, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Casper Labuschagne, Neng-Huei Lin, Yong Lin, Cathrine Lund Myhre, Krista Luoma, Hassan Lyamani, Angela Marinoni, Olga L. Mayol-Bracero, Nikos Mihalopoulos, Marco Pandolfi, Natalia Prats, Anthony J. Prenni, Jean-Philippe Putaud, Ludwig Ries, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Patrick Sheridan, James Patrick Sherman, Junying Sun, Gloria Titos, Elvis Torres, Thomas Tuch, Rolf Weller, Alfred Wiedensohler, Paul Zieger, and Paolo Laj
Atmos. Chem. Phys., 20, 8867–8908, https://doi.org/10.5194/acp-20-8867-2020, https://doi.org/10.5194/acp-20-8867-2020, 2020
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Long-term trends of aerosol radiative properties (52 stations) prove that aerosol load has significantly decreased over the last 20 years. Scattering trends are negative in Europe (EU) and North America (NA), not ss in Asia, and show a mix of positive and negative trends at polar stations. Absorption has mainly negative trends. The single scattering albedo has positive trends in Asia and eastern EU and negative in western EU and NA, leading to a global positive median trend of 0.02 % per year.
Arttu Ylisirniö, Luis Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-254, https://doi.org/10.5194/amt-2020-254, 2020
Preprint under review for AMT
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Juha Sulo, Nina Sarnela, Jenni Kontkanen, Lauri Ahonen, Pauli Paasonen, Tiia Laurila, Tuija Jokinen, Juha Kangasluoma, Tuukka Petäjä, Markku Kulmala, and Katrianne Lehtipalo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-719, https://doi.org/10.5194/acp-2020-719, 2020
Preprint under review for ACP
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In this study, we analyzed over five years of sub-3nm particle concentrations and their precursor vapors, identifying atmoshperic vapors important to the formation of these particles in the boreal forest. We also observed seasonal differences in both particle and precursor vapor concentrations and the formation pathways of these particles. Our results confirm the importance of organic vapors in atmospheric aerosol formation and highlight key seasonal differences that require further study.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-271, https://doi.org/10.5194/amt-2020-271, 2020
Preprint under review for AMT
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton-transfer and electron ionization to offer fast-time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad ElHaddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stefan Henri Prévôt
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-204, https://doi.org/10.5194/amt-2020-204, 2020
Preprint under review for AMT
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Long-term ambient aerosol mass spectrometric data was analyzed with a statistical model (PMF) to obtain source contributions & fingerprints. The new aspects of this manuscript involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run, by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
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. Discuss., https://doi.org/10.5194/acp-2020-648, https://doi.org/10.5194/acp-2020-648, 2020
Preprint under review for ACP
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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 formation pathways of atmospheric organic vapors, i.e., terpenes and their oxidation products with varying oxidation degrees. This study provides a more comprehensive picture of gas-phase source identifications of organic compounds.
Yuan Yang, Yonghong Wang, Putian Zhou, Dan Yao, Dongsheng Ji, Jie Sun, Yinghong Wang, Shuman Zhao, Wei Huang, Shuanghong Yang, Dean Chen, Wenkang Gao, Zirui Liu, Bo Hu, Renjian Zhang, Limin Zeng, Maofa Ge, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Yuesi Wang
Atmos. Chem. Phys., 20, 8181–8200, https://doi.org/10.5194/acp-20-8181-2020, https://doi.org/10.5194/acp-20-8181-2020, 2020
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
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.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominic V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-426, https://doi.org/10.5194/acp-2020-426, 2020
Preprint under review for ACP
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in Western Siberia for late-spring and summer in 2011. We find 2 commonly used emission inventories underestimate human emissions, when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June, and are only significant south of 60° N.
Weiqi Xu, Yao He, Yanmei Qiu, Chun Chen, Conghui Xie, Lu Lei, Zhijie Li, Jiaxing Sun, Junyao Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Meas. Tech., 13, 3205–3219, https://doi.org/10.5194/amt-13-3205-2020, https://doi.org/10.5194/amt-13-3205-2020, 2020
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We characterized mass spectral features of organic aerosol (OA) and water-soluble OA (WSOA) from 21 cooking, crop straw, wood, and coal burning experiments using aerosol mass spectrometers with standard and capture vaporizers, and we demonstrated the applications of source spectral profiles in improving source apportionment of ambient OA at a highly polluted rural site in the North China Plain in winter.
Oleg Sizov, Ekaterina Ezhova, Petr Tsymbarovich, Andrey Soromotin, Nikolay Prihod'ko, Tuukka Petäjä, Sergej Zilitinkevich, Markku Kulmala, Jaana Bäck, and Kajar Köster
Biogeosciences Discuss., https://doi.org/10.5194/bg-2020-174, https://doi.org/10.5194/bg-2020-174, 2020
Revised manuscript under review for BG
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Fires in Siberia become increasingly widespread. In changing climate, tundra fires might trigger transition to woodlands and forests, decreasing areas for reindeer pasture and increasing risk of tick-borne diseases. We studied wildfire dynamics and tundra-forest transition within 60 years in North-West Siberia near the Arctic Circle. We analyzed satellite data and ground-based observations, and found that wildfires trigger transition in 40–80 % of dry tundra, compared to 5–15 % without fires.
Mikhail Paramonov, Saskia Drossaart van Dusseldorp, Ellen Gute, Jonathan P. D. Abbatt, Paavo Heikkilä, Jorma Keskinen, Xuemeng Chen, Krista Luoma, Liine Heikkinen, Liqing Hao, Tuukka Petäjä, and Zamin A. Kanji
Atmos. Chem. Phys., 20, 6687–6706, https://doi.org/10.5194/acp-20-6687-2020, https://doi.org/10.5194/acp-20-6687-2020, 2020
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Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland in the winter–spring of 2018. It was found that no single parameter could be used to predict the INP number concentration at the measurement location during the examined time period. It was also not possible to identify physical and chemical properties of ambient INPs despite the complexity of the instrumental set-up. Therefore, this paper addresses the necessity for future INP measurements.
Ilona Ylivinkka, Santeri Kaupinmäki, Meri Virman, Maija Peltola, Ditte Taipale, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Ekaterina Ezhova
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-130, https://doi.org/10.5194/amt-2020-130, 2020
Revised manuscript accepted for AMT
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In this study, we developed a new algorithm for cloud classification using solar radiation and cloud base height measurements. Our objective was to develop a simple and inexpensive but effective algorithm for the needs of studies related ecosystem and atmosphere interactions. In the present study, we used the algorithm for obtaining cloud statistics at a measurement station in southern Finland and we discuss on the advantages and shortcomings of the algorithm.
Juan Andrés Casquero-Vera, Hassan Lyamani, Lubna Dada, Simo Hakala, Pauli Paasonen, Roberto Román, Roberto Fraile, Tuukka Petäjä, Francisco José Olmo-Reyes, and Lucas Alados-Arboledas
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-394, https://doi.org/10.5194/acp-2020-394, 2020
Revised manuscript accepted for ACP
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New particle formation was investigated at two stations located close to each other, but at different altitudes: urban and high-altitude site. Results show that sulfuric acid is able to explain a minimal fraction contribution to the observed growth rates and point to the availability of volatile organic compounds as the main factor controlling NPF events at both sites. A closer analysis of the NPF events that were observed at high-altitude site during a Saharan dust episode was carried out.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-223, https://doi.org/10.5194/acp-2020-223, 2020
Preprint under review for ACP
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.
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
Joel Kuula, Timo Mäkelä, Minna Aurela, Kimmo Teinilä, Samu Varjonen, Óscar González, and Hilkka Timonen
Atmos. Meas. Tech., 13, 2413–2423, https://doi.org/10.5194/amt-13-2413-2020, https://doi.org/10.5194/amt-13-2413-2020, 2020
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Particle-size-dependent detection ranges of low-cost particulate matter sensors were evaluated in a laboratory experiment. Six different sensor models were evaluated altogether. The results showed that none of the sensor models adhered to the technical specifications provided by the manufacturers, and thus a high risk of sensor misuse is posed. It is paramount that the limitations regarding the particle size discrimination of low-cost sensors are acknowledged properly.
Runlong Cai, Chenxi Li, Xu-Cheng He, Chenjuan Deng, Yiqun Lu, Rujing Yin, Chao Yan, Lin Wang, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-398, https://doi.org/10.5194/acp-2020-398, 2020
Revised manuscript under review for ACP
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Growth rate determines the survival probability of atmospheric new particles and hence their impacts. We clarify the impact of coagulation on the values retrieved by appearance time method, which is widely used for growth rate evaluation. A new formulae with coagulation correction is proposed based on derivation and tested using both models and atmospheric data. We show that the sub-3 nm particle growth rate in polluted environments may be overestimated without the coagulation correction.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-457, https://doi.org/10.5194/acp-2020-457, 2020
Revised manuscript accepted for ACP
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Our work presents secondary organic aerosol (SOA) formation results in the presence of gaseous ammonia. The particle phase ammonium was continuously produced even after SOA formation has ceased. The gas phase organic acids were experimentally observed to contribute to the formed particle phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-248, https://doi.org/10.5194/acp-2020-248, 2020
Revised manuscript accepted for ACP
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By applying both OA-PMF and Size-PMF at the same urban measurement site in Beijing, similar particle source-types, including vehicular emissions, cooking emissions and secondary formation-related sources were resolved by both frameworks and agreed well. It is also found that in the absence of new-particle formation, vehicular and cooking emissions dominate the particle number concentration while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-156, https://doi.org/10.5194/amt-2020-156, 2020
Revised manuscript accepted for AMT
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An inter-laboratory comparison exercise was conducted for the first time to examine the difference of water-soluble inorganic ions (WSII) measured by 10 labs using Ion Chromatography and by 2 online Aerosol Chemical Speciation Monitor method. Major ions including SO42−, NO3−, NH4+ agreed well in 10 IC labs, and correlated well with ACSM. WSII inter-lab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA-II were very similar.
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.
Krista Luoma, Jarkko V. Niemi, Aku Helin, Minna Aurela, Hilkka Timonen, Aki Virkkula, Topi Rönkkö, Anu Kousa, Pak Lun Fung, Tareq Hussein, and Tuukka Petäjä
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-201, https://doi.org/10.5194/acp-2020-201, 2020
Revised manuscript under review for ACP
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This study collated black carbon measurements from 15 different sites located in southern Finland. Sites were classified as traffic, detached housing area, urban background, and regional background sites. The seasonal, weekly and diurnal variations of the black carbon concentration were associated with local emissions from traffic and residential wood burning.
Decreasing trends for the black carbon concentration were observed and the trends were connected to decreases in traffic emissions.
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
Revised manuscript under review for ACP
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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.
Jing Duan, Ru-Jin Huang, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Chunshui Lin, Haiyan Ni, Meng Wang, Jurgita Ovadnevaite, Darius Ceburnis, Chunying Chen, Douglas R. Worsnop, Thorsten Hoffmann, Colin O'Dowd, and Junji Cao
Atmos. Chem. Phys., 20, 3793–3807, https://doi.org/10.5194/acp-20-3793-2020, https://doi.org/10.5194/acp-20-3793-2020, 2020
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We characterized secondary aerosol formation in Beijing. Our results showed that relative humidity (RH) and Ox have opposite effects on sulfate and nitrate formation in summer and winter. The wintertime more-oxidized OOA (MO-OOA) showed a good correlation with aerosol liquid water content (ALWC). Meanwhile, the dependence of less-oxidized OOA (LO-OOA) and the mass ratio of LO-OOA to MO-OOA in Ox both degraded when RH > 60 %, suggesting that RH or ALWC may also affect LO-OOA formation.
Yishuo Guo, Chao Yan, Chang Li, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1111, https://doi.org/10.5194/acp-2019-1111, 2020
Preprint under review for ACP
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Fog, cloud, haze are very common natural phenomena and all of them have a great impact on global climate. Sulfuric acid (SA) is one of the key compounds forming these suspended particles (aerosols), and therefore the concentration, source and sink of SA is very important. Daytime SA production is driven by OH radical oxiation, and here this article shows that ozonolysis of alkenes played a major role in nighttime SA formation in urabn Beijing under clean conditions.
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.
Lu Lei, Conghui Xie, Dawei Wang, Yao He, Qingqing Wang, Wei Zhou, Wei Hu, Pingqing Fu, Yong Chen, Xiaole Pan, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 20, 2877–2890, https://doi.org/10.5194/acp-20-2877-2020, https://doi.org/10.5194/acp-20-2877-2020, 2020
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We characterized aerosol composition and sources near two steel plants in a coastal region in fall and spring seasons. Our results showed substantially different aerosol composition and sources between the two seasons. We observed significant impacts of steel plant emissions on aerosol chemistry nearby, and we found that aerosol particles emitted from the steel plants were dominated by ammonium sulfate/bisulfate; NOx/CO and NOx/SO2 were distinct from those in the absence of industrial plumes.
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. Discuss., https://doi.org/10.5194/acp-2020-100, https://doi.org/10.5194/acp-2020-100, 2020
Preprint under review for ACP
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This work targets the chemical composition of alpha-pinene derived secondary organic aerosol formed in the temperature range −15 to 20 °C. Positive Matrix Factorization analysis of data obtained by a High-Resolution Time-of-Flight Aerosol Mass Spectrometer shows that the elemental SOA composition is controlled by initial alpha-pinene concentration and temperature during SOA formation. A significant new finding is that a change in temperature of up to 35 °C after SOA formation has little impact on
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.
Yongchun Liu, Yusheng Zhang, Chaofan Lian, Chao Yan, Zeming Feng, Feixue Zheng, Xiaolong Fan, Yan Chen, Weigang Wang, Biwu Chu, Yonghong Wang, Jin Cai, Wei Du, Kaspar R. Daellenbach, Juha Kangasluoma, Federico Bianchi, Joni Kujansuu, Tuukka Petäjä, Xuefei Wang, Bo Hu, Yuesi Wang, Maofa Ge, Hong He, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-150, https://doi.org/10.5194/acp-2020-150, 2020
Revised manuscript accepted for ACP
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Understanding of the chemical/physical processes leading to atmospheric aerosol particle formation is crucial to devising effective mitigation strategies to protect the public and reduce uncertainties in climate predictions. We found that the photolysis of nitrous acid could promote the formation of organic and nitrate aerosol and traffic-related emission is the major contributor to ambient nitrous acid in haze days of wintertime in Beijing.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-99, https://doi.org/10.5194/acp-2020-99, 2020
Revised manuscript accepted for ACP
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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 formed from the reactions of natural 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.
Ditte Taipale, Juho Aalto, Pauliina Schiestl-Aalto, Markku Kulmala, and Jaana Bäck
Biogeosciences Discuss., https://doi.org/10.5194/bg-2019-502, https://doi.org/10.5194/bg-2019-502, 2020
Revised manuscript not accepted
Ying Zhou, Lubna Dada, Yiliang Liu, Yueyun Fu, Juha Kangasluoma, Tommy Chan, Chao Yan, Biwu Chu, Kaspar R. Daellenbach, Federico Bianchi, Tom V. Kokkonen, Yongchun Liu, Joni Kujansuu, Veli-Matti Kerminen, Tuukka Petäjä, Lin Wang, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 20, 1201–1216, https://doi.org/10.5194/acp-20-1201-2020, https://doi.org/10.5194/acp-20-1201-2020, 2020
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In this study, we focus on explaining the concentration variations in the observed particle modes, by relating them to the potential aerosol sources and sinks, and on understanding the connections between these modes. Interestingly, even in the atmospheric cocktail in urban Beijing, secondary new particle formation (NPF) drives the particle number concentration, especially in the sub-3 nm range. We found that the total number concentration is ~ 4 times higher on NPF days than on haze days.
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.
Marja Hemmilä, Ulla Makkonen, Aki Virkkula, Georgia Panagiotopoulou, Juho Aalto, Markku Kulmala, Tuukka Petäjä, Hannele Hakola, and Heidi Hellén
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-1157, https://doi.org/10.5194/acp-2019-1157, 2020
Publication in ACP not foreseen
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Amines are atmospheric bases, which can affect to nucleation of aerosols. Lately, a computational study showed that guanidine could be even more effective to stabilize sulphuric acid clusters. In this paper we used a a dynamic flow-through chamber with an online ion chromatograph MARGA coupled with a mass spectrometer (MARGA-MS). We studied amine and guanidine emission from a boreal forest floor in Finland, and find out, that the boreal forest floor is a source of amines and guanidine.
Matti Räsänen, Mika Aurela, Ville Vakkari, Johan P. Beukes, Juha-Pekka Tuovinen, Pieter G. Van Zyl, Miroslav Josipovic, Stefan J. Siebert, Tuomas Laurila, Markku Kulmala, Lauri Laakso, Janne Rinne, Ram Oren, and Gabriel Katul
Hydrol. Earth Syst. Sci. Discuss., https://doi.org/10.5194/hess-2019-651, https://doi.org/10.5194/hess-2019-651, 2020
Revised manuscript under review for HESS
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The annual ET is approximately equal to precipitation during six measured years for grazed savanna grassland. The computed annual transpiration was highly constrained when rainfall was near or above the long-term mean but was reduced during severe drought year. The developed methodologies can be used in a wide range of arid and semi-arid ecosystems.
Yonghong Wang, Miao Yu, Yuesi Wang, Guiqian Tang, Tao Song, Putian Zhou, Zirui Liu, Bo Hu, Dongsheng Ji, Lili Wang, Xiaowan Zhu, Chao Yan, Mikael Ehn, Wenkang Gao, Yuepeng Pan, Jinyuan Xin, Yang Sun, Veli-Matti Kerminen, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 20, 45–53, https://doi.org/10.5194/acp-20-45-2020, https://doi.org/10.5194/acp-20-45-2020, 2020
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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.
Miska Olin, Heino Kuuluvainen, Minna Aurela, Joni Kalliokoski, Niina Kuittinen, Mia Isotalo, Hilkka J. Timonen, Jarkko V. Niemi, Topi Rönkkö, and Miikka Dal Maso
Atmos. Chem. Phys., 20, 1–13, https://doi.org/10.5194/acp-20-1-2020, https://doi.org/10.5194/acp-20-1-2020, 2020
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Photochemically formed sulfuric acid is generally considered the main source for new particle formation in the atmosphere. Contrary to current understanding, our measurements of nanoclusters and gaseous sulfuric acid performed in an urban area imply that traffic contributes to sulfuric acid concentration and that even for the smallest particles, the traffic-emitted fraction mostly exceeds the photochemistry-driven regional new particle formation.
Yicheng Shen, Aki Virkkula, Aijun Ding, Krista Luoma, Helmi Keskinen, Pasi P. Aalto, Xuguang Chi, Ximeng Qi, Wei Nie, Xin Huang, Tuukka Petäjä, Markku Kulmala, and Veli-Matti Kerminen
Atmos. Chem. Phys., 19, 15483–15502, https://doi.org/10.5194/acp-19-15483-2019, https://doi.org/10.5194/acp-19-15483-2019, 2019
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Long-term cloud condensation nuclei (CCN) number concentration (NCCN) data are scarce; there are a lot more data on aerosol optical properties (AOPs). It is therefore valuable to derive parameterizations for estimating NCCN from AOP measurements. With the new parameterization NCCN can be estimated from backscatter fraction, scattering Ångström exponent, and total light-scattering coefficient. The NCCN–AOP relationships depend on the geometric mean diameter and the width of the size distribution.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Giulia Stefenelli, Veronika Pospisilova, Felipe D. Lopez-Hilfiker, Kaspar R. Daellenbach, Christoph Hüglin, Yandong Tong, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 14825–14848, https://doi.org/10.5194/acp-19-14825-2019, https://doi.org/10.5194/acp-19-14825-2019, 2019
Arnaud P. Praplan, Toni Tykkä, Dean Chen, Michael Boy, Ditte Taipale, Ville Vakkari, Putian Zhou, Tuukka Petäjä, and Heidi Hellén
Atmos. Chem. Phys., 19, 14431–14453, https://doi.org/10.5194/acp-19-14431-2019, https://doi.org/10.5194/acp-19-14431-2019, 2019
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Our study shows that, despite our best efforts and recent progress, our knowledge of the chemical composition of the air under the canopy of a boreal forest still cannot be fully characterized. The discrepancy between the measured total reactivity of the air and the reactivity derived from the known chemical composition highlights the need to better understand the emissions from vegetation, but also other sources, such as the forest soil.
Jingda Liu, Lili Wang, Mingge Li, Zhiheng Liao, Yang Sun, Tao Song, Wenkang Gao, Yonghong Wang, Yan Li, Dongsheng Ji, Bo Hu, Veli-Matti Kerminen, Yuesi Wang, and Markku Kulmala
Atmos. Chem. Phys., 19, 14477–14492, https://doi.org/10.5194/acp-19-14477-2019, https://doi.org/10.5194/acp-19-14477-2019, 2019
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We analyzed the surface ozone variation characteristics and quantified the impact of synoptic and local meteorological factors on northern China during the warm season based on multi-city, in situ ozone and meteorological data, as well as meteorological reanalysis. The results of quantitative exploration on synoptic and local meteorological factors influencing both interannual and day-to-day ozone variations will provide the scientific basis for evaluating emission reduction measures.
Simonas Kecorius, Teresa Vogl, Pauli Paasonen, Janne Lampilahti, Daniel Rothenberg, Heike Wex, Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Silvia Henning, Xianda Gong, Andre Welti, Markku Kulmala, Frank Stratmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 19, 14339–14364, https://doi.org/10.5194/acp-19-14339-2019, https://doi.org/10.5194/acp-19-14339-2019, 2019
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Arctic sea-ice retreat, atmospheric new particle formation (NPF), and aerosol–cloud interaction may all be linked via a positive feedback mechanism. Understanding the sources of cloud condensation nuclei (CCN) is an important piece in the Arctic amplification puzzle. We show that Arctic newly formed particles do not have to grow beyond the Aitken mode to act as CCN. This is important, because NPF occurrence in the Arctic is expected to increase, making it a significant contributor to CCN budget.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545, https://doi.org/10.5194/amt-12-5535-2019, https://doi.org/10.5194/amt-12-5535-2019, 2019
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We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Xiaoxiao Li, Shaojie Song, Wei Zhou, Jiming Hao, Douglas R. Worsnop, and Jingkun Jiang
Atmos. Chem. Phys., 19, 12163–12174, https://doi.org/10.5194/acp-19-12163-2019, https://doi.org/10.5194/acp-19-12163-2019, 2019
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Aerosol liquid water is ubiquitous in ambient aerosol. Using long-term aerosol chemical composition to model the aerosol water in Beijing, we found that water absorbed by organics contributes a significant fraction to the total aerosol water. We emphasize the hygroscopicity of organics is highly variable and should be taken into consideration in modelling. A positive feedback loop between organic hygroscopicity and aerosol water was found as one of the driving factors of severe haze in Beijing.
Krista Luoma, Aki Virkkula, Pasi Aalto, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 19, 11363–11382, https://doi.org/10.5194/acp-19-11363-2019, https://doi.org/10.5194/acp-19-11363-2019, 2019
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We present an over 10-year-long time series of aerosol optical properties (AOPs) measured at a rural boreal forest site. Knowledge of AOPs is needed in determining the direct effect of aerosol particles on climate. We observed decreasing trends in scattering and absorption and increasing trends in backscattering fraction and single-scattering albedo. Trends of single-scattering albedo and backscattering fraction increased the efficiency of aerosol particles to scatter radiation back into space.
Simo Hakala, Mansour A. Alghamdi, Pauli Paasonen, Ville Vakkari, Mamdouh I. Khoder, Kimmo Neitola, Lubna Dada, Ahmad S. Abdelmaksoud, Hisham Al-Jeelani, Ibrahim I. Shabbaj, Fahd M. Almehmadi, Anu-Maija Sundström, Heikki Lihavainen, Veli-Matti Kerminen, Jenni Kontkanen, Markku Kulmala, Tareq Hussein, and Antti-Pekka Hyvärinen
Atmos. Chem. Phys., 19, 10537–10555, https://doi.org/10.5194/acp-19-10537-2019, https://doi.org/10.5194/acp-19-10537-2019, 2019
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Atmospheric aerosols have significant effects on human health and the climate. A large fraction of these aerosols originate from new particle formation, where atmospheric vapors form small nanosized particles that grow into larger sizes, thus becoming climatically relevant. We show that large amounts of fast-growing particles are formed frequently at a site located in western Saudi Arabia and that these particles are likely connected to strong nearby emissions from human activities.
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.
Jing Duan, Ru-Jin Huang, Chunshui Lin, Wenting Dai, Meng Wang, Yifang Gu, Ying Wang, Haobin Zhong, Yan Zheng, Haiyan Ni, Uli Dusek, Yang Chen, Yongjie Li, Qi Chen, Douglas R. Worsnop, Colin D. O'Dowd, and Junji Cao
Atmos. Chem. Phys., 19, 10319–10334, https://doi.org/10.5194/acp-19-10319-2019, https://doi.org/10.5194/acp-19-10319-2019, 2019
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We present the seasonal distinction of secondary aerosol formation in urban Beijing. Both photochemical oxidation and aqueous-phase processing played important roles in SOA (secondary organic aerosol) formation during all three seasons; while for sulfate formation, gas-phase photochemical oxidation was the major pathway in late summer, aqueous-phase reactions were more responsible during early winter, and both processes had contributions during autumn.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920, https://doi.org/10.5194/amt-12-3907-2019, https://doi.org/10.5194/amt-12-3907-2019, 2019
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An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
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.
Athanasia Vlachou, Anna Tobler, Houssni Lamkaddam, Francesco Canonaco, Kaspar R. Daellenbach, Jean-Luc Jaffrezo, María Cruz Minguillón, Marek Maasikmets, Erik Teinemaa, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 7279–7295, https://doi.org/10.5194/acp-19-7279-2019, https://doi.org/10.5194/acp-19-7279-2019, 2019
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The resolution of rotational ambiguity in positive matrix factorization (PMF) models is a major challenge. Here, we developed a method based on bootstrapping and correlations to extract environmentally meaningful solutions from PMF analysis based on offline aerosol mass spectrometry data. The method has been tested on a dataset that covers 1 full year of filter samples collected at three different sites in Estonia.
Kaspar R. Daellenbach, Ivan Kourtchev, Alexander L. Vogel, Emily A. Bruns, Jianhui Jiang, Tuukka Petäjä, Jean-Luc Jaffrezo, Sebnem Aksoyoglu, Markus Kalberer, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, https://doi.org/10.5194/acp-19-5973-2019, 2019
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Here we present the molecular composition of the organic aerosol (OA) at an urban site in Central Europe (Zurich, Switzerland) and compare it to smog chamber wood smoke and ambient biogenic secondary OA (SOA) (Orbitrap analyses). Accordingly, we are able to explain the strong seasonality of the molecular composition by aged wood smoke and biogenic SOA during winter and summer. Our results could also explain the predominance of non-fossil organic carbon at European locations throughout the year.
Yonghong Wang, Yuesi Wang, Lili Wang, Tuukka Petäjä, Qiaozhi Zha, Chongshui Gong, Sixuan Li, Yuepeng Pan, Bo Hu, Jinyuan Xin, and Markku Kulmala
Atmos. Chem. Phys., 19, 5881–5888, https://doi.org/10.5194/acp-19-5881-2019, https://doi.org/10.5194/acp-19-5881-2019, 2019
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Satellite observations combined with in situ measurements demonstrate that increased inorganic aerosol fractions of NO2 and SO2 contribute to air pollution and frequently occurring haze in China from 1980 to 2010. Currently, the reduction of nitrate, sulfate and their precursor gases would contribute towards better visibility in China.
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.
Katri Leino, Janne Lampilahti, Pyry Poutanen, Riikka Väänänen, Antti Manninen, Stephany Buenrostro Mazon, Lubna Dada, Anna Franck, Daniela Wimmer, Pasi P. Aalto, Lauri R. Ahonen, Joonas Enroth, Juha Kangasluoma, Petri Keronen, Frans Korhonen, Heikki Laakso, Teemu Matilainen, Erkki Siivola, Hanna E. Manninen, Katrianne Lehtipalo, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 19, 4127–4138, https://doi.org/10.5194/acp-19-4127-2019, https://doi.org/10.5194/acp-19-4127-2019, 2019
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This study presents airborne observations of particles, starting from 1.5 nm in diameter, above the boreal forest from 100 m up to 2700 m. The aim was to study the extent of NPF and likely places for nucleation. We found that the highest concentrations of 1.5–3 nm particles were above the forest canopy top on NPF event mornings, and the concentration decreased with increasing altitude. This would indicate the importance of gaseous precursors from vegetation for NPF processes in this area.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
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.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Nikos Kalivitis, Veli-Matti Kerminen, Giorgos Kouvarakis, Iasonas Stavroulas, Evaggelia Tzitzikalaki, Panayiotis Kalkavouras, Nikos Daskalakis, Stelios Myriokefalitakis, Aikaterini Bougiatioti, Hanna E. Manninen, Pontus Roldin, Tuukka Petäjä, Michael Boy, Markku Kulmala, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 2671–2686, https://doi.org/10.5194/acp-19-2671-2019, https://doi.org/10.5194/acp-19-2671-2019, 2019
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New particle formation (NPF) is an important source of atmospheric aerosols. For the Mediterranean atmosphere, only few studies exist. In this study we present one of the longest series of NPF by analyzing 10 years of data from Crete, Greece. NPF took place on 27 % of the available days; it was more frequent in spring and less so in late summer. Model simulations showed that NPF in the subtropical environment may differ greatly from that in the boreal environment.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Michael Boy, Erik S. Thomson, Juan-C. Acosta Navarro, Olafur Arnalds, Ekaterina Batchvarova, Jaana Bäck, Frank Berninger, Merete Bilde, Zoé Brasseur, Pavla Dagsson-Waldhauserova, Dimitri Castarède, Maryam Dalirian, Gerrit de Leeuw, Monika Dragosics, Ella-Maria Duplissy, Jonathan Duplissy, Annica M. L. Ekman, Keyan Fang, Jean-Charles Gallet, Marianne Glasius, Sven-Erik Gryning, Henrik Grythe, Hans-Christen Hansson, Margareta Hansson, Elisabeth Isaksson, Trond Iversen, Ingibjorg Jonsdottir, Ville Kasurinen, Alf Kirkevåg, Atte Korhola, Radovan Krejci, Jon Egill Kristjansson, Hanna K. Lappalainen, Antti Lauri, Matti Leppäranta, Heikki Lihavainen, Risto Makkonen, Andreas Massling, Outi Meinander, E. Douglas Nilsson, Haraldur Olafsson, Jan B. C. Pettersson, Nønne L. Prisle, Ilona Riipinen, Pontus Roldin, Meri Ruppel, Matthew Salter, Maria Sand, Øyvind Seland, Heikki Seppä, Henrik Skov, Joana Soares, Andreas Stohl, Johan Ström, Jonas Svensson, Erik Swietlicki, Ksenia Tabakova, Throstur Thorsteinsson, Aki Virkkula, Gesa A. Weyhenmeyer, Yusheng Wu, Paul Zieger, and Markku Kulmala
Atmos. Chem. Phys., 19, 2015–2061, https://doi.org/10.5194/acp-19-2015-2019, https://doi.org/10.5194/acp-19-2015-2019, 2019
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The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date and aimed to strengthen research and innovation regarding climate change issues in the Nordic region. The paper presents an overview of the main scientific topics investigated and provides a state-of-the-art comprehensive summary of what has been achieved in CRAICC.
Timo Vihma, Petteri Uotila, Stein Sandven, Dmitry Pozdnyakov, Alexander Makshtas, Alexander Pelyasov, Roberta Pirazzini, Finn Danielsen, Sergey Chalov, Hanna K. Lappalainen, Vladimir Ivanov, Ivan Frolov, Anna Albin, Bin Cheng, Sergey Dobrolyubov, Viktor Arkhipkin, Stanislav Myslenkov, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 19, 1941–1970, https://doi.org/10.5194/acp-19-1941-2019, https://doi.org/10.5194/acp-19-1941-2019, 2019
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The Arctic marine climate system, ecosystems, and socio-economic systems are changing rapidly. This calls for the establishment of a marine Arctic component of the Pan-Eurasian Experiment (MA-PEEX), for which we present a plan. The program will promote international collaboration; sustainable marine meteorological, sea ice, and oceanographic observations; advanced data management; and multidisciplinary research on the marine Arctic and its interaction with the Eurasian continent.
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.
Shaojie Song, Meng Gao, Weiqi Xu, Yele Sun, Douglas R. Worsnop, John T. Jayne, Yuzhong Zhang, Lei Zhu, Mei Li, Zhen Zhou, Chunlei Cheng, Yibing Lv, Ying Wang, Wei Peng, Xiaobin Xu, Nan Lin, Yuxuan Wang, Shuxiao Wang, J. William Munger, Daniel J. Jacob, and Michael B. McElroy
Atmos. Chem. Phys., 19, 1357–1371, https://doi.org/10.5194/acp-19-1357-2019, https://doi.org/10.5194/acp-19-1357-2019, 2019
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Chemistry responsible for sulfate production in northern China winter haze remains mysterious. We propose a potentially key pathway through the reaction of formaldehyde and sulfur dioxide that has not been accounted for in previous studies. The special atmospheric conditions favor the formation and existence of their complex, hydroxymethanesulfonate (HMS).
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
Biwu Chu, Veli-Matti Kerminen, Federico Bianchi, Chao Yan, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 19, 115–138, https://doi.org/10.5194/acp-19-115-2019, https://doi.org/10.5194/acp-19-115-2019, 2019
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The characteristics of new particle formation (NPF) in China, including frequency, formation rate, and particle growth rate, were summarized comprehensively and were compared among observations in different environments. The interactions between air pollution and NPF are discussed, as well as the possible reasons for more frequent NPF under heavy pollution conditions than in our current understanding. Significant and future research directions for NPF studies in China are also summarized.
Fidel Pankratov, Alexander Mahura, Tuukka Petäjä, Valentin Popov, and Vladimir Masloboev
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1228, https://doi.org/10.5194/acp-2018-1228, 2018
Revised manuscript not accepted
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Analysis of long-term observations for atmospheric mercury in the Russian Arctic, considering inter-annual, seasonal and monthly variabilities is in focus. Linkage of elevated concentrations with volcanic eruptions in Iceland is explored. Results showed that active volcanoes can play a role of sources for increased mercury levels in the Northern Hemisphere due to long-range atmospheric transport of volcanic clouds towards the Arctic.
Ekaterina Ezhova, Ilona Ylivinkka, Joel Kuusk, Kaupo Komsaare, Marko Vana, Alisa Krasnova, Steffen Noe, Mikhail Arshinov, Boris Belan, Sung-Bin Park, Jošt Valentin Lavrič, Martin Heimann, Tuukka Petäjä, Timo Vesala, Ivan Mammarella, Pasi Kolari, Jaana Bäck, Üllar Rannik, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 17863–17881, https://doi.org/10.5194/acp-18-17863-2018, https://doi.org/10.5194/acp-18-17863-2018, 2018
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Understanding the connections between aerosols, solar radiation and photosynthesis in terrestrial ecosystems is important for estimates of the CO2 balance in the atmosphere. Atmospheric aerosols and clouds influence solar radiation. In this study, we quantify the aerosol effect on solar radiation in boreal forests and study forest ecosystems response to this change in the radiation conditions. The analysis is based on atmospheric observations from several remote stations in Eurasian forests.
Lubna Dada, Robert Chellapermal, Stephany Buenrostro Mazon, Pauli Paasonen, Janne Lampilahti, Hanna E. Manninen, Heikki Junninen, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 17883–17893, https://doi.org/10.5194/acp-18-17883-2018, https://doi.org/10.5194/acp-18-17883-2018, 2018
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Our paper provides an automatic method to classify new particle formation events into four classes based on the accompanying air ion concentrations. The method is applied to 10 years of data measured within the SMEAR II station and was capable of eliminating the undefined class as well as defining the start, peak and end times of a regional event by monitoring the initial steps of cluster formation. Our method can be modified and applied to different locations where particle formation occurs.
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.
Cristina Carnerero, Noemí Pérez, Cristina Reche, Marina Ealo, Gloria Titos, Hong-Ku Lee, Hee-Ram Eun, Yong-Hee Park, Lubna Dada, Pauli Paasonen, Veli-Matti Kerminen, Enrique Mantilla, Miguel Escudero, Francisco J. Gómez-Moreno, Elisabeth Alonso-Blanco, Esther Coz, Alfonso Saiz-Lopez, Brice Temime-Roussel, Nicolas Marchand, David C. S. Beddows, Roy M. Harrison, Tuukka Petäjä, Markku Kulmala, Kang-Ho Ahn, Andrés Alastuey, and Xavier Querol
Atmos. Chem. Phys., 18, 16601–16618, https://doi.org/10.5194/acp-18-16601-2018, https://doi.org/10.5194/acp-18-16601-2018, 2018
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The vertical distribution of new particle formation events was studied using tethered balloons carrying miniaturized instrumentation. Results show that new particle formation and growth occurs only in the lower layer of the atmosphere, where aerosols are mixed due to convection, especially when the atmosphere is clean. A comparison of urban and suburban surface stations was also made, suggesting that such events may have a significant impact on ultrafine particle concentrations in a wide area.
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.
Tracey Leah Laban, Pieter Gideon van Zyl, Johan Paul Beukes, Ville Vakkari, Kerneels Jaars, Nadine Borduas-Dedekind, Miroslav Josipovic, Anne Mee Thompson, Markku Kulmala, and Lauri Laakso
Atmos. Chem. Phys., 18, 15491–15514, https://doi.org/10.5194/acp-18-15491-2018, https://doi.org/10.5194/acp-18-15491-2018, 2018
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Surface O3 was measured at four sites in the north-eastern interior of South Africa, which revealed that O3 is a regional problem in continental South Africa, with elevated O3 levels found at rural background and industrial sites. Increased O3 concentrations were associated with high CO levels predominantly related to regional biomass burning, while the O3 production regime was established to be predominantly VOC limited. Increased O3 is associated with strong seasonality of precursor sources.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
Juan Hong, Hanbing Xu, Haobo Tan, Changqing Yin, Liqing Hao, Fei Li, Mingfu Cai, Xuejiao Deng, Nan Wang, Hang Su, Yafang Cheng, Lin Wang, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 18, 14079–14094, https://doi.org/10.5194/acp-18-14079-2018, https://doi.org/10.5194/acp-18-14079-2018, 2018
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In this manuscript, we provide the results of the hygroscopicity of a more anthropogenically influenced aerosol in a suburban site in China. Organic material in the current type of aerosols showed moderate hygroscopicity, and it appeared to be less sensitive towards the variation of its oxidation level, which suggests different characteristics of the oxidation products in secondary organic aerosols (SOA) under the suburban/urban atmosphere in China when compared to other background environments.
Leena Järvi, Üllar Rannik, Tom V. Kokkonen, Mona Kurppa, Ari Karppinen, Rostislav D. Kouznetsov, Pekka Rantala, Timo Vesala, and Curtis R. Wood
Atmos. Meas. Tech., 11, 5421–5438, https://doi.org/10.5194/amt-11-5421-2018, https://doi.org/10.5194/amt-11-5421-2018, 2018
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Identical EC systems on two sides of a building in central Helsinki were used to assess the uncertainty of the vertical fluxes on the single measurement point from July 2013 to September 2015. Sampling at only one point yielded up to 12% underestimation in the cumulative carbon fluxes; for sensible and latent heat the respective values were up to 5 and 8%. The commonly used statistics, kurtosis and skewness, are not necessarily suitable for filtering out data in a densely built urban area.
Heidi Hellén, Arnaud P. Praplan, Toni Tykkä, Ilona Ylivinkka, Ville Vakkari, Jaana Bäck, Tuukka Petäjä, Markku Kulmala, and Hannele Hakola
Atmos. Chem. Phys., 18, 13839–13863, https://doi.org/10.5194/acp-18-13839-2018, https://doi.org/10.5194/acp-18-13839-2018, 2018
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Exceptionally large ambient air concentration datasets of VOCs were measured in a boreal forest. For the first time concentration of the main sesquiterpene (β-caryophyllene) emitted by the local trees was also measured. Sesquiterpenes were found to have a major impact on local atmospheric chemistry, even though their concentrations were 30 times lower than the monoterpene concentrations. In addition, sesquiterpenes are expected to have a high impact on local secondary organic aerosol production.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
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PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
Jenni Kontkanen, Tinja Olenius, Markku Kulmala, and Ilona Riipinen
Atmos. Chem. Phys., 18, 13733–13754, https://doi.org/10.5194/acp-18-13733-2018, https://doi.org/10.5194/acp-18-13733-2018, 2018
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New particle formation involving sulfuric acid, bases and organic compounds is an important source of atmospheric aerosol particles. We investigate the capability of nano-Köhler theory to describe this process by simulating the dynamics of atmospheric molecular clusters. We find that nano-Köhler-type behavior occurs in our simulations when the saturation ratio of the organic vapor and the ratio between organic and inorganic vapor concentrations are in a suitable range.
John N. Crowley, Nicolas Pouvesle, Gavin J. Phillips, Raoul Axinte, Horst Fischer, Tuukka Petäjä, Anke Nölscher, Jonathan Williams, Korbinian Hens, Hartwig Harder, Monica Martinez-Harder, Anna Novelli, Dagmar Kubistin, Birger Bohn, and Jos Lelieveld
Atmos. Chem. Phys., 18, 13457–13479, https://doi.org/10.5194/acp-18-13457-2018, https://doi.org/10.5194/acp-18-13457-2018, 2018
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Simultaneous observations of PAA, PAN and H2O2 are used to provide insight into processes influencing the HOx chemistry of the boreal forest, including two biomass-burning-impacted periods. A significant contribution from photolytic HOx sources was included in a box model analysis to align model predictions with measurements. The model predicts high levels of organic peroxy radicals, also at night-time.
Pertti Hari, Steffen Noe, Sigrid Dengel, Jan Elbers, Bert Gielen, Veli-Matti Kerminen, Bart Kruijt, Liisa Kulmala, Anders Lindroth, Ivan Mammarella, Tuukka Petäjä, Guy Schurgers, Anni Vanhatalo, Markku Kulmala, and Jaana Bäck
Atmos. Chem. Phys., 18, 13321–13328, https://doi.org/10.5194/acp-18-13321-2018, https://doi.org/10.5194/acp-18-13321-2018, 2018
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The development of eddy-covariance measurements of ecosystem CO2 fluxes began a new era in the field studies of photosynthesis. The interpretation of the very variable CO2 fluxes in evergreen forests has been problematic especially in seasonal transition times. We apply two theoretical needle-level equations and show they can predict photosynthetic CO2 flux between the atmosphere and Scots pine forests. This has strong implications for the interpretation of the global change and boreal forests.
Daniela Wimmer, Stephany Buenrostro Mazon, Hanna Elina Manninen, Juha Kangasluoma, Alessandro Franchin, Tuomo Nieminen, John Backman, Jian Wang, Chongai Kuang, Radovan Krejci, Joel Brito, Fernando Goncalves Morais, Scot Turnbull Martin, Paulo Artaxo, Markku Kulmala, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 18, 13245–13264, https://doi.org/10.5194/acp-18-13245-2018, https://doi.org/10.5194/acp-18-13245-2018, 2018
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This work focuses on understanding the production of very small airborne particles in the undisturbed environment of the Amazon basin. Computer models have shown that up to 70 % of these tiny particles are responsible for cloud formation on a global scale. The processes behind the production of these very small particles have been studied intensely recently. Their appearance has been observed almost all over the world. We directly measure sub-3 nm aerosols for the first time in the Amazon basin.
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.
Martha A. Zaidan, Ville Haapasilta, Rishi Relan, Pauli Paasonen, Veli-Matti Kerminen, Heikki Junninen, Markku Kulmala, and Adam S. Foster
Atmos. Chem. Phys., 18, 12699–12714, https://doi.org/10.5194/acp-18-12699-2018, https://doi.org/10.5194/acp-18-12699-2018, 2018
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This article promotes the use of the mutual information method for finding any non-linear associations among atmospheric variables. We demonstrate that the same results from previous studies are obtained by this method, which operates without supervision and without the need of understanding the physics deeply. This suggests that the method is suitable to be implemented widely in the atmospheric field to discover other interesting phenomena and their relevant variables.
Pauli Paasonen, Maija Peltola, Jenni Kontkanen, Heikki Junninen, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 12085–12103, https://doi.org/10.5194/acp-18-12085-2018, https://doi.org/10.5194/acp-18-12085-2018, 2018
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We determine aerosol growth rates in diameter ranges from below 10 to over 300 nm from long-term data with a novel automatic method. We show that aerosol growth rate in boreal forest increases with increasing particle diameter from 10 nm to cloud condensation nuclei (CCN) sizes and that the growth rate of sub-CCN particles is not suppressed by increasing condensation sink. Our findings suggest that aerosol growth to CCN sizes is a faster and less self-regulated process than previously estimated.
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.
Wei Zhou, Jian Zhao, Bin Ouyang, Archit Mehra, Weiqi Xu, Yuying Wang, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Qi Chen, Conghui Xie, Qingqing Wang, Junfeng Wang, Wei Du, Yingjie Zhang, Xinlei Ge, Penglin Ye, James D. Lee, Pingqing Fu, Zifa Wang, Douglas Worsnop, Roderic Jones, Carl J. Percival, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 18, 11581–11597, https://doi.org/10.5194/acp-18-11581-2018, https://doi.org/10.5194/acp-18-11581-2018, 2018
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We present measurements of gas-phase N2O5 and ClNO2 by ToF-CIMS during summer in urban Beijing as part of the APHH campaign. High reactivity of N2O5 indicative of active nocturnal chemistry was observed. The lifetime of N2O5 as a function of aerosol surface area and relative humidity was characterized, and N2O5 uptake coefficients were estimated. We also found that the N2O5 loss in this study is mainly attributed to its indirect loss via reactions of NO3 with VOCs and NO.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Runlong Cai, Dongsen Yang, Lauri R. Ahonen, Linlin Shi, Frans Korhonen, Yan Ma, Jiming Hao, Tuukka Petäjä, Jun Zheng, Juha Kangasluoma, and Jingkun Jiang
Atmos. Meas. Tech., 11, 4477–4491, https://doi.org/10.5194/amt-11-4477-2018, https://doi.org/10.5194/amt-11-4477-2018, 2018
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We tested the performance of four inversion methods to recover sub-3 nm aerosol size distributions using the particle size magnifier (PSM). The PSM is widely used in new particle formation study; however, the inversion methods used in previous studies may report false particle concentrations. Due to the results, we suggest using the expectation–maximization algorithm to address the PSM inversion problem. We also gave practical suggestions on PSM operation based on the inversion analysis.
Anna Nikandrova, Ksenia Tabakova, Antti Manninen, Riikka Väänänen, Tuukka Petäjä, Markku Kulmala, Veli-Matti Kerminen, and Ewan O'Connor
Atmos. Chem. Phys., 18, 10575–10591, https://doi.org/10.5194/acp-18-10575-2018, https://doi.org/10.5194/acp-18-10575-2018, 2018
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We investigated temporal and vertical aerosol properties in a rural environment during BAECC (Biogenic Aerosols – Effects on Cloud and Climate) campaign. Differences were observed in aerosol number size distribution, variability and mixing in the layers between two case studies: clear-sky and partly cloudy case. We also conclude that care should be taken in selecting appropriate arrival heights of backward trajectories, since the modelled and observed layer heights did not always coincide.
Luciana Varanda Rizzo, Pontus Roldin, Joel Brito, John Backman, Erik Swietlicki, Radovan Krejci, Peter Tunved, Tukka Petäjä, Markku Kulmala, and Paulo Artaxo
Atmos. Chem. Phys., 18, 10255–10274, https://doi.org/10.5194/acp-18-10255-2018, https://doi.org/10.5194/acp-18-10255-2018, 2018
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Aerosols are tiny particles suspended in the air that can interact with sunlight and form clouds, which in turn affect the climate. They can also recycle nutrients in forest environments. Aerosols are naturally emitted at the surface in the Amazon forest, in addition to being brought down from above the boundary layer by intense air movements. In this work, we describe how the particle size number concentrations of aerosols change over hours, days and seasons in a multi-year study in Amazonia.
Filippo Xausa, Pauli Paasonen, Risto Makkonen, Mikhail Arshinov, Aijun Ding, Hugo Denier Van Der Gon, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 10039–10054, https://doi.org/10.5194/acp-18-10039-2018, https://doi.org/10.5194/acp-18-10039-2018, 2018
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Our project describes the feasibility of implementing particle number emissions taken from the GAINS model in global climate modeling through a simulation with the ECHAM-HAM global climate model. The results from the simulations have important implications regarding modeled particle number concentrations and future climate effects. Our findings represent an important starting point for further simulations concerning climate effects derived from anthropogenic particle emissions on a global scale.
Yue Zhang, Shachi Katira, Andrew Lee, Andrew T. Lambe, Timothy B. Onasch, Wen Xu, William A. Brooks, Manjula R. Canagaratna, Andrew Freedman, John T. Jayne, Doug R. Worsnop, Paul Davidovits, David Chandler, and Charles E. Kolb
Atmos. Meas. Tech., 11, 3479–3490, https://doi.org/10.5194/amt-11-3479-2018, https://doi.org/10.5194/amt-11-3479-2018, 2018
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We have adopted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols at submicron sizes and relatively low mass concentrations. Aerosol particles are deposited in the form of a thin film with interdigitated electrodes using electrostatic precipitation. Broadband dielectric spectroscopy is used to measure the kinetically controlled glass transition temperatures of glycerol and citric acid aerosols with three atmospheric relevant cooling rates.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
Marco Pandolfi, Lucas Alados-Arboledas, Andrés Alastuey, Marcos Andrade, Christo Angelov, Begoña Artiñano, John Backman, Urs Baltensperger, Paolo Bonasoni, Nicolas Bukowiecki, Martine Collaud Coen, Sébastien Conil, Esther Coz, Vincent Crenn, Vadimas Dudoitis, Marina Ealo, Kostas Eleftheriadis, Olivier Favez, Prodromos Fetfatzis, Markus Fiebig, Harald Flentje, Patrick Ginot, Martin Gysel, Bas Henzing, Andras Hoffer, Adela Holubova Smejkalova, Ivo Kalapov, Nikos Kalivitis, Giorgos Kouvarakis, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Chris Lunder, Krista Luoma, Hassan Lyamani, Angela Marinoni, Nikos Mihalopoulos, Marcel Moerman, José Nicolas, Colin O'Dowd, Tuukka Petäjä, Jean-Eudes Petit, Jean Marc Pichon, Nina Prokopciuk, Jean-Philippe Putaud, Sergio Rodríguez, Jean Sciare, Karine Sellegri, Erik Swietlicki, Gloria Titos, Thomas Tuch, Peter Tunved, Vidmantas Ulevicius, Aditya Vaishya, Milan Vana, Aki Virkkula, Stergios Vratolis, Ernest Weingartner, Alfred Wiedensohler, and Paolo Laj
Atmos. Chem. Phys., 18, 7877–7911, https://doi.org/10.5194/acp-18-7877-2018, https://doi.org/10.5194/acp-18-7877-2018, 2018
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This investigation presents the variability in near-surface in situ aerosol particle light-scattering measurements obtained over the past decade at 28 measuring atmospheric observatories which are part of the ACTRIS Research Infrastructure, and most of them belong to the GAW network. This paper provides a comprehensive picture of the spatial and temporal variability of aerosol particles optical properties in Europe.
Vladimir Melnikov, Viktor Gennadinik, Markku Kulmala, Hanna K. Lappalainen, Tuukka Petäjä, and Sergej Zilitinkevich
Atmos. Chem. Phys., 18, 6535–6542, https://doi.org/10.5194/acp-18-6535-2018, https://doi.org/10.5194/acp-18-6535-2018, 2018
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The cryosphere of the Earth overlaps with the atmosphere, hydrosphere and lithosphere over vast areas with temperatures below zero C and pronounced H2O phase changes. The cryosphere plays the role of a global thermostat; however, the processes related to the cryosphere attract insufficient attention from research communities. We call attention to crucial importance of cryogenic anomalies, which make the Earth atmosphere and the entire Earth system unique.
Marja Hemmilä, Heidi Hellén, Aki Virkkula, Ulla Makkonen, Arnaud P. Praplan, Jenni Kontkanen, Lauri Ahonen, Markku Kulmala, and Hannele Hakola
Atmos. Chem. Phys., 18, 6367–6380, https://doi.org/10.5194/acp-18-6367-2018, https://doi.org/10.5194/acp-18-6367-2018, 2018
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We measured gas- and particle-phase amine and ammonia concentrations in a boreal forest site in 2015 with online ion chromatography coupled with mass spectrometry. We wanted to know how much and which kinds of amines there are, and how they behave and could affect nucleation. We observed seasonal and diurnal variations for different amines. Amines turned out to be a heterogeneous group of compounds. To our best knowledge, our amine measurements are the longest time series that has been made.
Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Benjamin Chazeau, Gary A. Salazar, Soenke Szidat, Jean-Luc Jaffrezo, Christoph Hueglin, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 6187–6206, https://doi.org/10.5194/acp-18-6187-2018, https://doi.org/10.5194/acp-18-6187-2018, 2018
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Carbonaceous aerosols are related to adverse human health effects, which depend on the aerosol chemical composition and size. Here, we combine aerosol mass spectrometry and radiocarbon measurements of size-resolved samples collected over a long term to identify the origins of primary and secondary carbonaceous aerosols in the fine and coarse modes.
Yicheng Shen, Aki Virkkula, Aijun Ding, Jiaping Wang, Xuguang Chi, Wei Nie, Ximeng Qi, Xin Huang, Qiang Liu, Longfei Zheng, Zheng Xu, Tuukka Petäjä, Pasi P. Aalto, Congbin Fu, and Markku Kulmala
Atmos. Chem. Phys., 18, 5265–5292, https://doi.org/10.5194/acp-18-5265-2018, https://doi.org/10.5194/acp-18-5265-2018, 2018
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Aerosol optical properties (AOPs) were measured at SORPES, a regional background station in Nanjing, China from June 2013 to May 2015. The aerosol was highly scattering. The single-scattering albedo in Nanjing appears to be slightly higher than at several other sites. The data do not suggest any significant contribution to absorption by brown carbon. The sources of high values are mainly in eastern China. During pollution episodes, pollutant concentrations increased gradually but decreased fast.
Joonas Enroth, Jyri Mikkilä, Zoltán Németh, Markku Kulmala, and Imre Salma
Atmos. Chem. Phys., 18, 4533–4548, https://doi.org/10.5194/acp-18-4533-2018, https://doi.org/10.5194/acp-18-4533-2018, 2018
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The urban aerosol particles in central Budapest consist of two externally mixed classes – nearly hydrophobic and less volatile particles, which were assigned to vehicle emissions (large mass fractions of soot likely coated with water-insoluble organic compounds) – and of less hygroscopic and volatile particles (moderately transformed aged combustion particles composed of partly oxygenated organics and inorganic salts internally mixed).
Yan-Lin Zhang, Imad El-Haddad, Ru-Jin Huang, Kin-Fai Ho, Jun-Ji Cao, Yongming Han, Peter Zotter, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Gary Salazar, André S. H. Prévôt, and Sönke Szidat
Atmos. Chem. Phys., 18, 4005–4017, https://doi.org/10.5194/acp-18-4005-2018, https://doi.org/10.5194/acp-18-4005-2018, 2018
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Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time of flight aerosol mass spectrometer measurements. We demonstrate a dominant contribution of non-fossil emissions to WSOC aerosols in the Northern Hemisphere. However, the fossil fraction is substantially larger in aerosols from East Asia and the east Asian pollution outflow, especially during winter, due to increasing coal combustion.
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
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.
Ekaterina Ezhova, Veli-Matti Kerminen, Kari E. J. Lehtinen, and Markku Kulmala
Atmos. Chem. Phys., 18, 2431–2442, https://doi.org/10.5194/acp-18-2431-2018, https://doi.org/10.5194/acp-18-2431-2018, 2018
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A condensation sink (CS) quantifies the rate of uptake of condensing vapours by pre-existing aerosol and can be used as well to quantify losses of monomers/clusters. An analytical solution of the condensation equation valid in a wide range of particle diameters is presented. We describe the dynamics of atmospheric CS, test the formulas against field observations and further use them to develop a simplified model of the coupled dynamics of aerosol and condensing vapours in the atmosphere.
Kaspar R. Daellenbach, Imad El-Haddad, Lassi Karvonen, Athanasia Vlachou, Joel C. Corbin, Jay G. Slowik, Maarten F. Heringa, Emily A. Bruns, Samuel M. Luedin, Jean-Luc Jaffrezo, Sönke Szidat, Andrea Piazzalunga, Raquel Gonzalez, Paola Fermo, Valentin Pflueger, Guido Vogel, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 2155–2174, https://doi.org/10.5194/acp-18-2155-2018, https://doi.org/10.5194/acp-18-2155-2018, 2018
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A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at multiple sites in central Europe during the entire year of 2013. PM sources were identified by positive matrix factorization. Wood burning emissions were separated according to the burning conditions; inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. Moreover, primary tailpipe exhaust was distinguished from aged/secondary traffic emissions.
Luís Miguel Feijó Barreira, Geoffroy Duporté, Tuukka Rönkkö, Jevgeni Parshintsev, Kari Hartonen, Lydia Hyrsky, Enna Heikkinen, Matti Jussila, Markku Kulmala, and Marja-Liisa Riekkola
Atmos. Meas. Tech., 11, 881–893, https://doi.org/10.5194/amt-11-881-2018, https://doi.org/10.5194/amt-11-881-2018, 2018
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Our results demonstrated the benefits and challenges of using new SPME Arrow over SPME fiber for the sampling of BVOCs emitted by terrestrial vegetation in the atmosphere. The new SPME Arrow system showed significant improvement on sampling capacity, with collected amounts being approximately 2 times higher for monoterpenes and 7–8 times higher for aldehydes than with SPME fiber. Higher extraction efficiencies were obtained with dynamic collection prior to equilibrium regime.
Johannes Größ, Amar Hamed, André Sonntag, Gerald Spindler, Hanna Elina Manninen, Tuomo Nieminen, Markku Kulmala, Urmas Hõrrak, Christian Plass-Dülmer, Alfred Wiedensohler, and Wolfram Birmili
Atmos. Chem. Phys., 18, 1835–1861, https://doi.org/10.5194/acp-18-1835-2018, https://doi.org/10.5194/acp-18-1835-2018, 2018
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This paper revisits the atmospheric new particle formation (NPF) process in the polluted troposphere. Novel aspects include a new NPF classification, which aims at more objectivity, and a long-term analysis of neutral cluster and air ion spectrometer data. Intense NPF events were associated with enhanced sulfur dioxide concentrations and solar radiation, while no significant relationships were observed with the condensation sink, surface-measured turbulence parameters, or ammonia.
Wu Sun, Linda M. J. Kooijmans, Kadmiel Maseyk, Huilin Chen, Ivan Mammarella, Timo Vesala, Janne Levula, Helmi Keskinen, and Ulli Seibt
Atmos. Chem. Phys., 18, 1363–1378, https://doi.org/10.5194/acp-18-1363-2018, https://doi.org/10.5194/acp-18-1363-2018, 2018
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Most soils consume carbonyl sulfide (COS) and CO due to microbial uptake, but whether boreal forest soils act like this is uncertain. We measured growing season soil COS and CO fluxes in a Finnish pine forest. The soil behaved as a consistent and relatively invariant sink of COS and CO. Uptake rates of COS and CO decrease with soil moisture due to diffusion limitation and increase with respiration because of microbial control. Using COS to infer photosynthesis is not affected by soil COS flux.
Simon Schallhart, Pekka Rantala, Maija K. Kajos, Juho Aalto, Ivan Mammarella, Taina M. Ruuskanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 815–832, https://doi.org/10.5194/acp-18-815-2018, https://doi.org/10.5194/acp-18-815-2018, 2018
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Emissions of volatile organic compounds (VOCs) have impact to air quality, human health and climate. We investigated the development of VOC exchange in a boreal forest between April and June 2013. VOC exchange and diversity increased towards summer, but over 75 % of the biogenic net exchange was driven by methanol, monoterpenes and acetone only. The boreal forest emitted less than 0.2 % carbon in form of VOCs in relation to the carbon uptake.
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
Pertti Hari, Veli-Matti Kerminen, Liisa Kulmala, Markku Kulmala, Steffen Noe, Tuukka Petäjä, Anni Vanhatalo, and Jaana Bäck
Atmos. Chem. Phys., 17, 15045–15053, https://doi.org/10.5194/acp-17-15045-2017, https://doi.org/10.5194/acp-17-15045-2017, 2017
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We developed a theory on the seasonal behaviour of photosynthesis in natural conditions and tested the theory with intensive measurements. Light, temperature, water vapor and CO2 concentration explained the daily variation in photosynthesis, and the physiological state of the photosynthetic machinery explained the annual pattern of photosynthesis. The theory explained about 95 % of the variance of photosynthesis measured with chambers in the field in northern Finland.
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
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.
Xuemeng Chen, Aki Virkkula, Veli-Matti Kerminen, Hanna E. Manninen, Maurizio Busetto, Christian Lanconelli, Angelo Lupi, Vito Vitale, Massimo Del Guasta, Paolo Grigioni, Riikka Väänänen, Ella-Maria Duplissy, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 13783–13800, https://doi.org/10.5194/acp-17-13783-2017, https://doi.org/10.5194/acp-17-13783-2017, 2017
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An air ion spectrometer was deployed for characterizing air ions for the first time at the Concordia station at Dome C on the Antarctic Plateau. We observed different ion processes: new particle formation (NPF), wind-induced ion production, and ion formation related to cloud and/or fog formation. Insights into these phenomena are presented. Additionally, the analysis on the growth of NPF events showed a size dependency of growth rates (GRs), i.e. GRs increase with particle sizes.
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.
Elham Baranizadeh, Tuomo Nieminen, Taina Yli-Juuti, Markku Kulmala, Tuukka Petäjä, Ari Leskinen, Mika Komppula, Ari Laaksonen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 17, 13361–13371, https://doi.org/10.5194/acp-17-13361-2017, https://doi.org/10.5194/acp-17-13361-2017, 2017
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Extrapolation of the particle formation rates from one measured larger size (e.g., 7 nm) to smaller sizes (e.g., 3 nm) based on simplified growth-scavenging dynamics works fairly well to estimate mean daily formation rates, but it fails to predict the time evolution of the particle population. This points to the challenges in predicting atmospheric nucleation rates for locations where the particle growth and loss rates are size- and time-dependent.
Kaspar R. Daellenbach, Giulia Stefenelli, Carlo Bozzetti, Athanasia Vlachou, Paola Fermo, Raquel Gonzalez, Andrea Piazzalunga, Cristina Colombi, Francesco Canonaco, Christoph Hueglin, Anne Kasper-Giebl, Jean-Luc Jaffrezo, Federico Bianchi, Jay G. Slowik, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 13265–13282, https://doi.org/10.5194/acp-17-13265-2017, https://doi.org/10.5194/acp-17-13265-2017, 2017
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We present offline AMS analyses for the organic aerosol (OA) in PM10 at nine sites in central Europe for 2013. Primary OA is separated into traffic, cooking, and wood-burning components. A factor explaining sulfur-containing ions, with an event-driven time series, is also separated. We observe enhanced production of secondary OA (SOA) in summer, following biogenic emissions with temperature. In winter a SOA component is dominant, which correlates with anthropogenic inorganic species.
Eben S. Cross, Leah R. Williams, David K. Lewis, Gregory R. Magoon, Timothy B. Onasch, Michael L. Kaminsky, Douglas R. Worsnop, and John T. Jayne
Atmos. Meas. Tech., 10, 3575–3588, https://doi.org/10.5194/amt-10-3575-2017, https://doi.org/10.5194/amt-10-3575-2017, 2017
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Low-cost air quality sensor technologies offer new opportunities for fast and distributed measurements of air pollution, but a persistent characterization gap remains when it comes to evaluating sensor performance under realistic environmental sampling conditions. We present results from a newly developed integrated AQ-sensor system (ARISense) and demonstrate the utility of using high-dimensional model representation to improve the conversion of raw sensor signal to ambient concentration.
Linda M. J. Kooijmans, Kadmiel Maseyk, Ulli Seibt, Wu Sun, Timo Vesala, Ivan Mammarella, Pasi Kolari, Juho Aalto, Alessandro Franchin, Roberta Vecchi, Gianluigi Valli, and Huilin Chen
Atmos. Chem. Phys., 17, 11453–11465, https://doi.org/10.5194/acp-17-11453-2017, https://doi.org/10.5194/acp-17-11453-2017, 2017
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Carbon cycle studies rely on the accuracy of models to estimate the amount of CO2 being taken up by vegetation. The gas carbonyl sulfide (COS) can serve as a tool to estimate the vegetative CO2 uptake by scaling the ecosystem uptake of COS to that of CO2. Here we investigate the nighttime fluxes of COS. The relationships found in this study will aid in implementing nighttime COS uptake in models, which is key to obtain accurate estimates of vegetative CO2 uptake with the use of COS.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
Georgios Tsagkogeorgas, Pontus Roldin, Jonathan Duplissy, Linda Rondo, Jasmin Tröstl, Jay G. Slowik, Sebastian Ehrhart, Alessandro Franchin, Andreas Kürten, Antonio Amorim, Federico Bianchi, Jasper Kirkby, Tuukka Petäjä, Urs Baltensperger, Michael Boy, Joachim Curtius, Richard C. Flagan, Markku Kulmala, Neil M. Donahue, and Frank Stratmann
Atmos. Chem. Phys., 17, 8923–8938, https://doi.org/10.5194/acp-17-8923-2017, https://doi.org/10.5194/acp-17-8923-2017, 2017
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The H2SO4 vapour pressure plays key role in Earth's and Venus' atmospheres. In regions where RH is low and stabilising bases are scarce, H2SO4 can evaporate from particles; however the H2SO4 vapour pressure at low RH is uncertain. To address this, we measured H2SO4 evaporation versus T and RH in the CLOUD chamber and constrained the equilibrium constants for dissociation and dehydration of H2SO4. This study is important for nucleation, particle growth and H2SO4 formation occurring in atmosphere.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Carlo Bozzetti, Imad El Haddad, Dalia Salameh, Kaspar Rudolf Daellenbach, Paola Fermo, Raquel Gonzalez, María Cruz Minguillón, Yoshiteru Iinuma, Laurent Poulain, Miriam Elser, Emanuel Müller, Jay Gates Slowik, Jean-Luc Jaffrezo, Urs Baltensperger, Nicolas Marchand, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 17, 8247–8268, https://doi.org/10.5194/acp-17-8247-2017, https://doi.org/10.5194/acp-17-8247-2017, 2017
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We present the first long-term organic aerosol source apportionment in an environment influenced by anthropogenic emissions including biomass burning and industrial processes and an active photochemistry. Online and offline aerosol mass spectrometry were used to characterize these emissions and their transformation. Measurements of organic markers provided insights into the origin of biomass smoke in this area, with different seasonal contributions from domestic heating and agricultural burning.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Imad El Haddad, Emily A. Bruns, Monica Crippa, Laurent Poulain, Mikko Äijälä, Samara Carbone, Evelyn Freney, Colin O'Dowd, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 7653–7669, https://doi.org/10.5194/acp-17-7653-2017, https://doi.org/10.5194/acp-17-7653-2017, 2017
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Organic aerosol (OA) comprises the main fraction of fine particulate matter (PM1). Using a new VBS parameterization, we performed model-based source apportionment studies to assess the importance of different emission sources to the total OA loads in Europe during winter periods. Our results indicate that residential wood burning emissions represent the major source of OA, followed by non-residential emission sources (i.e. traffic and industries).
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
Juha Kangasluoma, Susanne Hering, David Picard, Gregory Lewis, Joonas Enroth, Frans Korhonen, Markku Kulmala, Karine Sellegri, Michel Attoui, and Tuukka Petäjä
Atmos. Meas. Tech., 10, 2271–2281, https://doi.org/10.5194/amt-10-2271-2017, https://doi.org/10.5194/amt-10-2271-2017, 2017
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The manuscript presents a characterization of three new particle counters able to detect airborne nanoparticles smaller than 3 nm in diameter. We explored some of the parameters affecting the smallest detectable particle size, such as sample flow relative humidity, the particle chemical composition and the electrical charging state. The characterization results help one to select a suitable particle counter for a given application.
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.
Kgaugelo Euphinia Chiloane, Johan Paul Beukes, Pieter Gideon van Zyl, Petra Maritz, Ville Vakkari, Miroslav Josipovic, Andrew Derick Venter, Kerneels Jaars, Petri Tiitta, Markku Kulmala, Alfred Wiedensohler, Catherine Liousse, Gabisile Vuyisile Mkhatshwa, Avishkar Ramandh, and Lauri Laakso
Atmos. Chem. Phys., 17, 6177–6196, https://doi.org/10.5194/acp-17-6177-2017, https://doi.org/10.5194/acp-17-6177-2017, 2017
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This paper presents atmospheric black carbon (BC) data collected in South Africa (SA). In general, BC level were higher than in the developed world. At one site, five sources were identified, with household combustion as well as savannah and grassland fires the most significant sources during winter and spring, while coal-fired power stations, pyrometallurgical smelters and traffic contributed year round.
Eero Nikinmaa, Tuomo Kalliokoski, Kari Minkkinen, Jaana Bäck, Michael Boy, Yao Gao, Nina Janasik-Honkela, Janne I. Hukkinen, Maarit Kallio, Markku Kulmala, Nea Kuusinen, Annikki Mäkelä, Brent D. Matthies, Mikko Peltoniemi, Risto Sievänen, Ditte Taipale, Lauri Valsta, Anni Vanhatalo, Martin Welp, Luxi Zhou, Putian Zhou, and Frank Berninger
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-141, https://doi.org/10.5194/bg-2017-141, 2017
Manuscript not accepted for further review
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We estimated the impact of boreal forest management on climate, considering the effects of carbon, albedo, aerosols, and effects of industrial wood use. We made analyses both in current and warmer climate of 2050. The aerosol effect was comparable to that of carbon sequestration. Deciduous trees may have a large potential for mitigation due to their high albedo and aerosol effects. If the forests will be used more intensively and mainly for pulp and energy, the warming influence is clear.
Yuqin Liu, Gerrit de Leeuw, Veli-Matti Kerminen, Jiahua Zhang, Putian Zhou, Wei Nie, Ximeng Qi, Juan Hong, Yonghong Wang, Aijun Ding, Huadong Guo, Olaf Krüger, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 5623–5641, https://doi.org/10.5194/acp-17-5623-2017, https://doi.org/10.5194/acp-17-5623-2017, 2017
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The aerosol effects on warm cloud parameters over the Yangtze River Delta are systematically examined using multi-sensor retrievals. This study shows that the COT–CDR and CWP–CDR relationships are not unique, but are affected by atmospheric aerosol loading. CDR and cloud fraction show different behaviours for low and high AOD. Aerosol–cloud interaction (ACI) is stronger for clouds mixed with smoke aerosol than for clouds mixed with dust. Meteorological conditions play an important role in ACI.
Hilkka Timonen, Panu Karjalainen, Erkka Saukko, Sanna Saarikoski, Päivi Aakko-Saksa, Pauli Simonen, Timo Murtonen, Miikka Dal Maso, Heino Kuuluvainen, Matthew Bloss, Erik Ahlberg, Birgitta Svenningsson, Joakim Pagels, William H. Brune, Jorma Keskinen, Douglas R. Worsnop, Risto Hillamo, and Topi Rönkkö
Atmos. Chem. Phys., 17, 5311–5329, https://doi.org/10.5194/acp-17-5311-2017, https://doi.org/10.5194/acp-17-5311-2017, 2017
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The effect of fuel ethanol content (10–100 %) on primary emissions and the subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. The emissions were characterized during the New European Driving Cycle (NEDC) using high time-resolution instruments. The chemical composition of the exhaust particulate matter was studied using a soot particle aerosol mass spectrometer (SP-AMS), and the secondary aerosol formation was studied with an oxidation chamber.
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.
Ellis Shipley Robinson, Timothy B. Onasch, Douglas Worsnop, and Neil M. Donahue
Atmos. Meas. Tech., 10, 1139–1154, https://doi.org/10.5194/amt-10-1139-2017, https://doi.org/10.5194/amt-10-1139-2017, 2017
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.
Antti-Jussi Kieloaho, Mari Pihlatie, Samuli Launiainen, Markku Kulmala, Marja-Liisa Riekkola, Jevgeni Parshintsev, Ivan Mammarella, Timo Vesala, and Jussi Heinonsalo
Biogeosciences, 14, 1075–1091, https://doi.org/10.5194/bg-14-1075-2017, https://doi.org/10.5194/bg-14-1075-2017, 2017
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The alkylamines are important precursors in secondary aerosol formation in boreal forests. We quantified alkylamine concentrations in fungal species present in boreal forests in order to estimate soil as a source of atmospheric alkylamines. Based on our knowledge we estimated possible soil–atmosphere exchange of these compounds. The results shows that the boreal forest soil could act as a source of alkylamines depending on environmental conditions and studied compound.
Hannele Hakola, Virpi Tarvainen, Arnaud P. Praplan, Kerneels Jaars, Marja Hemmilä, Markku Kulmala, Jaana Bäck, and Heidi Hellén
Atmos. Chem. Phys., 17, 3357–3370, https://doi.org/10.5194/acp-17-3357-2017, https://doi.org/10.5194/acp-17-3357-2017, 2017
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We present spring and summer VOC emission rate measurements from Norway spruce using an in situ gas chromatograph. Monoterpene and C4–C10 aldehyde emission rates reached maxima in July. SQT emissions increased at the end of July and in August SQT were the most abundant group. The MT emission pattern varied a lot from tree to tree and therefore emission fluxes on canopy level should be conducted for more representative measurements. However, leaf level measurements produce more reliable SQT data.
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.
Carla Frege, Federico Bianchi, Ugo Molteni, Jasmin Tröstl, Heikki Junninen, Stephan Henne, Mikko Sipilä, Erik Herrmann, Michel J. Rossi, Markku Kulmala, Christopher R. Hoyle, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 17, 2613–2629, https://doi.org/10.5194/acp-17-2613-2017, https://doi.org/10.5194/acp-17-2613-2017, 2017
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We present measurements of the chemical composition of atmospheric ions at high altitude (3450 m a.s.l.) during a 9-month campaign. We detected remarkably high correlation between methanesulfonic acid (MSA) and SO5−. Halogenated species were also detected frequently at this continental location. New-particle formation events occurred via the condensation of highly oxygenated molecules (HOMs) at very low sulfuric acid concentration or, less frequently, due to ammonia–sulfuric acid clusters.
Jenni Kontkanen, Katrianne Lehtipalo, Lauri Ahonen, Juha Kangasluoma, Hanna E. Manninen, Jani Hakala, Clémence Rose, Karine Sellegri, Shan Xiao, Lin Wang, Ximeng Qi, Wei Nie, Aijun Ding, Huan Yu, Shanhu Lee, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 2163–2187, https://doi.org/10.5194/acp-17-2163-2017, https://doi.org/10.5194/acp-17-2163-2017, 2017
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The concentrations of ~1–3 nm particles were investigated at nine sites around the world. Sub-3 nm particle concentrations were highest at the sites with strong anthropogenic influence. Electrically neutral particles dominated sub-3 nm particle concentrations in polluted environments and in boreal forest during spring and summer. Sub-3 nm particle concentrations were observed to be determined by the availability of precursor vapors rather than the sink caused by preexisting aerosol particles.
Heidi Hellén, Simon Schallhart, Arnaud P. Praplan, Tuukka Petäjä, and Hannele Hakola
Atmos. Meas. Tech., 10, 281–289, https://doi.org/10.5194/amt-10-281-2017, https://doi.org/10.5194/amt-10-281-2017, 2017
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There is a lack of knowledge of volatile organic acids (VOAs), other than formic and acetic acids in gas phase, and this is at least partly due to the lack of sensitive enough measurement methods. In the present study we developed an in situ GC–MS measurement method for measuring C2–C7 monocarboxylic VOAs at ambient air concentration levels, which we used to measure ambient air concentrations in a boreal forest site. In addition, found mixing ratios were compared with PTR-TOFMS data.
Carlo Bozzetti, Yuliya Sosedova, Mao Xiao, Kaspar R. Daellenbach, Vidmantas Ulevicius, Vadimas Dudoitis, Genrik Mordas, Steigvilė Byčenkienė, Kristina Plauškaitė, Athanasia Vlachou, Benjamin Golly, Benjamin Chazeau, Jean-Luc Besombes, Urs Baltensperger, Jean-Luc Jaffrezo, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 117–141, https://doi.org/10.5194/acp-17-117-2017, https://doi.org/10.5194/acp-17-117-2017, 2017
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In this study we present the offline-AMS source apportionment of the submicron organic aerosol (OA) sources conducted over 1 year at three locations in the south east Baltic region, which has so far received small attention. Offline-AMS enabled broadening the AMS spatial and temporal coverage, and provided a full characterization of the OA sources. Source apportionment results revealed that biomass burning and biogenic secondary emissions were the major OA sources during winter and summer.
Kerneels Jaars, Pieter G. van Zyl, Johan P. Beukes, Heidi Hellén, Ville Vakkari, Micky Josipovic, Andrew D. Venter, Matti Räsänen, Leandra Knoetze, Dirk P. Cilliers, Stefan J. Siebert, Markku Kulmala, Janne Rinne, Alex Guenther, Lauri Laakso, and Hannele Hakola
Atmos. Chem. Phys., 16, 15665–15688, https://doi.org/10.5194/acp-16-15665-2016, https://doi.org/10.5194/acp-16-15665-2016, 2016
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Biogenic volatile organic compounds (BVOCs) – important in tropospheric ozone and secondary organic aerosol formation – were measured at a savannah grassland in South Africa. Results presented are the most extensive for this type of landscape. Compared to other parts of the world, monoterpene levels were similar, while very low isoprene levels led to significantly lower total BVOC levels. BVOC levels were an order of magnitude lower compared to anthropogenic VOC levels measured at Welgegund.
Hanna K. Lappalainen, Veli-Matti Kerminen, Tuukka Petäjä, Theo Kurten, Aleksander Baklanov, Anatoly Shvidenko, Jaana Bäck, Timo Vihma, Pavel Alekseychik, Meinrat O. Andreae, Stephen R. Arnold, Mikhail Arshinov, Eija Asmi, Boris Belan, Leonid Bobylev, Sergey Chalov, Yafang Cheng, Natalia Chubarova, Gerrit de Leeuw, Aijun Ding, Sergey Dobrolyubov, Sergei Dubtsov, Egor Dyukarev, Nikolai Elansky, Kostas Eleftheriadis, Igor Esau, Nikolay Filatov, Mikhail Flint, Congbin Fu, Olga Glezer, Aleksander Gliko, Martin Heimann, Albert A. M. Holtslag, Urmas Hõrrak, Juha Janhunen, Sirkku Juhola, Leena Järvi, Heikki Järvinen, Anna Kanukhina, Pavel Konstantinov, Vladimir Kotlyakov, Antti-Jussi Kieloaho, Alexander S. Komarov, Joni Kujansuu, Ilmo Kukkonen, Ella-Maria Duplissy, Ari Laaksonen, Tuomas Laurila, Heikki Lihavainen, Alexander Lisitzin, Alexsander Mahura, Alexander Makshtas, Evgeny Mareev, Stephany Mazon, Dmitry Matishov, Vladimir Melnikov, Eugene Mikhailov, Dmitri Moisseev, Robert Nigmatulin, Steffen M. Noe, Anne Ojala, Mari Pihlatie, Olga Popovicheva, Jukka Pumpanen, Tatjana Regerand, Irina Repina, Aleksei Shcherbinin, Vladimir Shevchenko, Mikko Sipilä, Andrey Skorokhod, Dominick V. Spracklen, Hang Su, Dmitry A. Subetto, Junying Sun, Arkady Y. Terzhevik, Yuri Timofeyev, Yuliya Troitskaya, Veli-Pekka Tynkkynen, Viacheslav I. Kharuk, Nina Zaytseva, Jiahua Zhang, Yrjö Viisanen, Timo Vesala, Pertti Hari, Hans Christen Hansson, Gennady G. Matvienko, Nikolai S. Kasimov, Huadong Guo, Valery Bondur, Sergej Zilitinkevich, and Markku Kulmala
Atmos. Chem. Phys., 16, 14421–14461, https://doi.org/10.5194/acp-16-14421-2016, https://doi.org/10.5194/acp-16-14421-2016, 2016
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After kick off in 2012, the Pan-Eurasian Experiment (PEEX) program has expanded fast and today the multi-disciplinary research community covers ca. 80 institutes and a network of ca. 500 scientists from Europe, Russia, and China. Here we introduce scientific topics relevant in this context. This is one of the first multi-disciplinary overviews crossing scientific boundaries, from atmospheric sciences to socio-economics and social sciences.
Laura Riuttanen, Marja Bister, Veli-Matti Kerminen, Viju O. John, Anu-Maija Sundström, Miikka Dal Maso, Jouni Räisänen, Victoria A. Sinclair, Risto Makkonen, Filippo Xausa, Gerrit de Leeuw, and Markku Kulmala
Atmos. Chem. Phys., 16, 14331–14342, https://doi.org/10.5194/acp-16-14331-2016, https://doi.org/10.5194/acp-16-14331-2016, 2016
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Here we show observational evidence that aerosols increase upper tropospheric humidity (UTH) via changes in the microphysics of deep convection. Using remote sensing data over the ocean east of China in summer, we show that increased aerosol loads are associated with an UTH increase of 2.2 ± 1.5 in units of relative humidity. We show that humidification of aerosols or other meteorological covariation is very unlikely to be the cause for this result indicating relevance for the global climate.
Xuemeng Chen, Veli-Matti Kerminen, Jussi Paatero, Pauli Paasonen, Hanna E. Manninen, Tuomo Nieminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 16, 14297–14315, https://doi.org/10.5194/acp-16-14297-2016, https://doi.org/10.5194/acp-16-14297-2016, 2016
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Ionising radiation is responsible for air ion production. However, minor efforts have been invested in understanding the connection of observed air ions to ionising radiation in the lower atmosphere and underlying processes therein. In this work, we analysed 4 years of ambient data collected in a Finnish boreal forest and found that gamma radiation dominates air ion production in the lower atmosphere and demonstrated clear promotion effects of the ionising radiation on air ion production.
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.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Jenni Kontkanen, Pauli Paasonen, Juho Aalto, Jaana Bäck, Pekka Rantala, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 16, 13291–13307, https://doi.org/10.5194/acp-16-13291-2016, https://doi.org/10.5194/acp-16-13291-2016, 2016
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We developed proxies for estimating the concentrations of monoterpenes and their oxidation products at a boreal forest site in Hyytiälä, Finland. The proxies for the monoterpene concentration include temperature-controlled emissions, dilution and different oxidation processes. The proxies were observed to capture the seasonal and diurnal variation of the monoterpene concentration reasonably well. Our proxies can be used in the analysis of new particle formation and growth in boreal environments.
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
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.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Monica Crippa, Jose-Luis Jimenez, Eriko Nemitz, Karine Sellegri, Mikko Äijälä, Samara Carbone, Claudia Mohr, Colin O'Dowd, Laurent Poulain, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 10313–10332, https://doi.org/10.5194/acp-16-10313-2016, https://doi.org/10.5194/acp-16-10313-2016, 2016
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Recent studies based on aerosol mass spectrometer measurements revealed that the organic fraction dominates the non-refractory PM1 composition. However its representation in chemical transport models is still very challenging due to uncertainties in emission sources and formation pathways. In this study, a novel organic aerosol scheme was tested in the regional air quality model CAMx and results were compared with ambient measurements at 11 different sites in Europe.
Luís Miguel Feijó Barreira, Yu Xue, Geoffroy Duporté, Jevgeni Parshintsev, Kari Hartonen, Matti Jussila, Markku Kulmala, and Marja-Liisa Riekkola
Atmos. Meas. Tech., 9, 3661–3671, https://doi.org/10.5194/amt-9-3661-2016, https://doi.org/10.5194/amt-9-3661-2016, 2016
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Volatile organic compounds play a key role in atmospheric chemistry and physics by influencing the climate. Trace concentrations need to be determined, even at remote locations, like forests. In this research, an easy and fast method using a portable device was developed for determination of relevant atmospheric compounds. Links between these compounds and meteorological factors were observed. Also, accumulation of volatiles in the snow was measured.
Hanna E. Manninen, Sander Mirme, Aadu Mirme, Tuukka Petäjä, and Markku Kulmala
Atmos. Meas. Tech., 9, 3577–3605, https://doi.org/10.5194/amt-9-3577-2016, https://doi.org/10.5194/amt-9-3577-2016, 2016
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This paper reports a standard operation procedure (SOP) for a Neutral cluster and Air Ion Spectrometer (NAIS) to detect small clusters and nucleation mode particles. The NAIS measures number size distributions of charged and neutral aerosol particles. The SOP is needed to provide comparable results measured by NAIS users around the world. The work is based on discussions between the NAIS users (lead by University of Helsinki, Finland) and the NAIS manufacturer (Airel Ltd., Estonia).
Moa K. Sporre, Ewan J. O'Connor, Nina Håkansson, Anke Thoss, Erik Swietlicki, and Tuukka Petäjä
Atmos. Meas. Tech., 9, 3193–3203, https://doi.org/10.5194/amt-9-3193-2016, https://doi.org/10.5194/amt-9-3193-2016, 2016
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Satellite measurements of cloud top height and liquid water path are compared to ground-based remote sensing to evaluate the satellite retrievals. The overall performance of the satellite retrievals of cloud top height are good, but they become more problematic when several layers of clouds are present. The liquid water path retrievals also agree well, and the average differences are within the estimated measurement uncertainties.
Imre Salma, Zoltán Németh, Veli-Matti Kerminen, Pasi Aalto, Tuomo Nieminen, Tamás Weidinger, Ágnes Molnár, Kornélia Imre, and Markku Kulmala
Atmos. Chem. Phys., 16, 8715–8728, https://doi.org/10.5194/acp-16-8715-2016, https://doi.org/10.5194/acp-16-8715-2016, 2016
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We revealed that NPF seen in a central large city of the Carpathian Basin, Budapest, and its regional background occur in a consistent and spatially coherent way as a result of a joint atmospheric phenomenon taking place on large horizontal scales.
Riikka Väänänen, Radovan Krejci, Hanna E. Manninen, Antti Manninen, Janne Lampilahti, Stephany Buenrostro Mazon, Tuomo Nieminen, Taina Yli-Juuti, Jenni Kontkanen, Ari Asmi, Pasi P. Aalto, Petri Keronen, Toivo Pohja, Ewan O'Connor, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-556, https://doi.org/10.5194/acp-2016-556, 2016
Revised manuscript has not been submitted
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A light aircraft was used as a platform to explore the horizontal and vertical variability of the aerosol particles over a boreal forest in Central Finland. This information is needed when data measured at ground level station is extrapolated and parameterized to represent the
conditions of the larger scale. The measurements showed that despite local fluctuations there was a good agreement between the on-ground and airborne measurements inside the planetary boundary layer.
Juha Kangasluoma, Alessandro Franchin, Jonahtan Duplissy, Lauri Ahonen, Frans Korhonen, Michel Attoui, Jyri Mikkilä, Katrianne Lehtipalo, Joonas Vanhanen, Markku Kulmala, and Tuukka Petäjä
Atmos. Meas. Tech., 9, 2977–2988, https://doi.org/10.5194/amt-9-2977-2016, https://doi.org/10.5194/amt-9-2977-2016, 2016
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The paper describes technical aspects of using the Airmodus A11 nCNC at various inlet pressures and how temperature selection affects the performance of the instrument. We also present a sampling box to minimize the inlet losses and make use of the instrument more convenient.
Pekka Rantala, Leena Järvi, Risto Taipale, Terhi K. Laurila, Johanna Patokoski, Maija K. Kajos, Mona Kurppa, Sami Haapanala, Erkki Siivola, Tuukka Petäjä, Taina M. Ruuskanen, and Janne Rinne
Atmos. Chem. Phys., 16, 7981–8007, https://doi.org/10.5194/acp-16-7981-2016, https://doi.org/10.5194/acp-16-7981-2016, 2016
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Fluxes of volatile organic compounds (VOCs) were measured above an urban landscape in Helsinki, northern Europe. We found that traffic was a major source for many oxygenated and aromatic VOCs, whereas isoprene originated mostly from the urban vegetation. Overall, the VOC fluxes were quite small in comparison with the earlier urban VOC flux measurements.
Alessandro Franchin, Andy Downard, Juha Kangasluoma, Tuomo Nieminen, Katrianne Lehtipalo, Gerhard Steiner, Hanna E. Manninen, Tuukka Petäjä, Richard C. Flagan, and Markku Kulmala
Atmos. Meas. Tech., 9, 2709–2720, https://doi.org/10.5194/amt-9-2709-2016, https://doi.org/10.5194/amt-9-2709-2016, 2016
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High transmission efficiency is key for classifying and counting atmospheric aerosol below 10 nm. We developed a new high-transmission inlet for the Caltech nano-radial DMA (nRDMA) and successfully deployed the nRDMA, equipped with the new inlet, in chamber measurements, using a particle size magnifier (PSM) and a booster CPC as a counter. With this setup, we were able to measure size distributions of ions between 1.3 and 6 nm in mobility diameter.
Simon Schallhart, Pekka Rantala, Eiko Nemitz, Ditte Taipale, Ralf Tillmann, Thomas F. Mentel, Benjamin Loubet, Giacomo Gerosa, Angelo Finco, Janne Rinne, and Taina M. Ruuskanen
Atmos. Chem. Phys., 16, 7171–7194, https://doi.org/10.5194/acp-16-7171-2016, https://doi.org/10.5194/acp-16-7171-2016, 2016
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We present ecosystem exchange fluxes from a mixed oak–hornbeam forest in the Po Valley, Italy. Detectable fluxes were observed for 29 compounds, dominated by isoprene, which comprised over 60 % of the upward flux. Methanol seemed to be deposited to dew, as the deposition happened in the early morning. We estimated that up to 30 % of the upward flux of methyl vinyl ketone and methacrolein originated from atmospheric oxidation of isoprene.
W. Joe F. Acton, Simon Schallhart, Ben Langford, Amy Valach, Pekka Rantala, Silvano Fares, Giulia Carriero, Ralf Tillmann, Sam J. Tomlinson, Ulrike Dragosits, Damiano Gianelle, C. Nicholas Hewitt, and Eiko Nemitz
Atmos. Chem. Phys., 16, 7149–7170, https://doi.org/10.5194/acp-16-7149-2016, https://doi.org/10.5194/acp-16-7149-2016, 2016
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Volatile organic compounds (VOCs) represent a large source of reactive carbon in the atmosphere and hence have a significant impact on air quality. It is therefore important that we can accurately quantify their emission. In this paper we use three methods to determine the fluxes of reactive VOCs from a woodland canopy. We show that two different canopy-scale measurement methods give good agreement, whereas estimates based on leaf-level-based emission underestimate isoprene fluxes.
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
Vidmantas Ulevicius, Steigvilė Byčenkienė, Carlo Bozzetti, Athanasia Vlachou, Kristina Plauškaitė, Genrik Mordas, Vadimas Dudoitis, Gülcin Abbaszade, Vidmantas Remeikis, Andrius Garbaras, Agne Masalaite, Jan Blees, Roman Fröhlich, Kaspar R. Dällenbach, Francesco Canonaco, Jay G. Slowik, Josef Dommen, Ralf Zimmermann, Jürgen Schnelle-Kreis, Gary A. Salazar, Konstantinos Agrios, Sönke Szidat, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 5513–5529, https://doi.org/10.5194/acp-16-5513-2016, https://doi.org/10.5194/acp-16-5513-2016, 2016
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In early spring the Baltic region is frequently affected by high pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires.
Jenni Kontkanen, Tinja Olenius, Katrianne Lehtipalo, Hanna Vehkamäki, Markku Kulmala, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 16, 5545–5560, https://doi.org/10.5194/acp-16-5545-2016, https://doi.org/10.5194/acp-16-5545-2016, 2016
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Miriam Elser, Ru-Jin Huang, Robert Wolf, Jay G. Slowik, Qiyuan Wang, Francesco Canonaco, Guohui Li, Carlo Bozzetti, Kaspar R. Daellenbach, Yu Huang, Renjian Zhang, Zhengqiang Li, Junji Cao, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 3207–3225, https://doi.org/10.5194/acp-16-3207-2016, https://doi.org/10.5194/acp-16-3207-2016, 2016
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This work represents the first online chemical characterization of the PM2.5 using a high-resolution time-of flight aerosol mass spectrometer during extreme haze events China. The application of novel source apportionment techniques allowed for an improved identification and quantification of the sources of organic aerosols. The main sources and processes driving the extreme haze events are assessed.
Antti J. Manninen, Ewan J. O'Connor, Ville Vakkari, and Tuukka Petäjä
Atmos. Meas. Tech., 9, 817–827, https://doi.org/10.5194/amt-9-817-2016, https://doi.org/10.5194/amt-9-817-2016, 2016
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Current commercially available Doppler lidars provide a cost-effective solution for measuring vertical and horizontal wind velocities, and the co- and cross-polarised backscatter profiles. However, the background noise behaviour becomes a limiting factor for the instrument sensitivity in low aerosol load regions. In this paper we present a correction method which can improve the data availability up to 50 % and greatly improves the calculation of turbulent properties in weak signal regimes.
Xin Huang, Luxi Zhou, Aijun Ding, Ximeng Qi, Wei Nie, Minghuai Wang, Xuguang Chi, Tuukka Petäjä, Veli-Matti Kerminen, Pontus Roldin, Anton Rusanen, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 16, 2477–2492, https://doi.org/10.5194/acp-16-2477-2016, https://doi.org/10.5194/acp-16-2477-2016, 2016
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By combining a regional model and a box model, this study simulates new particle formation in Nanjing, China, when the air masses were affected by anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. The simulations reveal that biogenic organic compounds play a vital role in growth of newly formed clusters. This novel combination of two models makes it possible to accomplish new particle formation simulation without direct measurements of all chemical species.
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.
Jenni Kontkanen, Emma Järvinen, Hanna E. Manninen, Katrianne Lehtipalo, Juha Kangasluoma, Stefano Decesari, Gian Paolo Gobbi, Ari Laaksonen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 16, 1919–1935, https://doi.org/10.5194/acp-16-1919-2016, https://doi.org/10.5194/acp-16-1919-2016, 2016
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
J. Kukkonen, M. Karl, M. P. Keuken, H. A. C. Denier van der Gon, B. R. Denby, V. Singh, J. Douros, A. Manders, Z. Samaras, N. Moussiopoulos, S. Jonkers, M. Aarnio, A. Karppinen, L. Kangas, S. Lützenkirchen, T. Petäjä, I. Vouitsis, and R. S. Sokhi
Geosci. Model Dev., 9, 451–478, https://doi.org/10.5194/gmd-9-451-2016, https://doi.org/10.5194/gmd-9-451-2016, 2016
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For analyzing the health effects of particulate matter, it is necessary to consider not only the mass of particles, but also their sizes and composition. A simple measure for the former is the number concentration of particles. We present particle number concentrations in five major European cities, namely Helsinki, Oslo, London, Rotterdam, and Athens, in 2008, based mainly on modelling. The concentrations of PN were mostly influenced by the emissions from local vehicular traffic.
P. Hari, T. Petäjä, J. Bäck, V.-M. Kerminen, H. K. Lappalainen, T. Vihma, T. Laurila, Y. Viisanen, T. Vesala, and M. Kulmala
Atmos. Chem. Phys., 16, 1017–1028, https://doi.org/10.5194/acp-16-1017-2016, https://doi.org/10.5194/acp-16-1017-2016, 2016
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This manuscript introduces a conceptual design of a global, hierarchical observation network which provides tools and increased understanding to tackle the inter-connected environmental and societal challenges that we will face in the coming decades. Each ecosystem type on the globe has its own characteristic features that need to be taken into consideration. The hierarchical network is able to tackle problems related to large spatial scales, heterogeneity of ecosystems and their complexity.
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 not accepted
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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.
K. R. Daellenbach, C. Bozzetti, A. Křepelová, F. Canonaco, R. Wolf, P. Zotter, P. Fermo, M. Crippa, J. G. Slowik, Y. Sosedova, Y. Zhang, R.-J. Huang, L. Poulain, S. Szidat, U. Baltensperger, I. El Haddad, and A. S. H. Prévôt
Atmos. Meas. Tech., 9, 23–39, https://doi.org/10.5194/amt-9-23-2016, https://doi.org/10.5194/amt-9-23-2016, 2016
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In this study, we developed an offline technique using the AMS for the characterization of the chemical fingerprints of aerosols collected on quartz filters, and evaluated the suitability of the organic mass spectral data for source apportionment. This technique may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.
A. M. K. Hansen, J. Hong, T. Raatikainen, K. Kristensen, A. Ylisirniö, A. Virtanen, T. Petäjä, M. Glasius, and N. L. Prisle
Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/ac