Articles | Volume 20, issue 10
https://doi.org/10.5194/acp-20-5945-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-5945-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
19 May 2020
Research article |
| 19 May 2020
| 19 May 2020
Insights into atmospheric oxidation processes by performing factor analyses on subranges of mass spectra
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Otso Peräkylä
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Liine Heikkinen
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Mikko Äijälä
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Kaspar R. Daellenbach
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Qiaozhi Zha
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Matthieu Riva
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Univ. Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON,
69626, Villeurbanne, France
Olga Garmash
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Heikki Junninen
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Institute of Physics, University of Tartu, Tartu, 50090, Estonia
Pentti Paatero
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Douglas Worsnop
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
Aerodyne Research, Inc., Billerica, MA 01821, USA
Mikael Ehn
Institute for Atmospheric and Earth System Research/Physics,
Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
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To be able to meet global grand challenges, we need comprehensive open data with proper metadata. In this opinion paper, we describe the SMEAR (Station for Measuring Earth surface – Atmosphere Relations) concept and include several examples (cases), such as new particle formation and growth, feedback loops and the effect of COVID-19, and what has been learned from these investigations. The future needs and the potential of comprehensive observations of the environment are summarized.
Xiaoxiao Li, Yijing Chen, Yuyang Li, Runlong Cai, Yiran Li, Chenjuan Deng, Jin Wu, Chao Yan, Hairong Cheng, Yongchun Liu, Markku Kulmala, Jiming Hao, James N. Smith, and Jingkun Jiang
Atmos. Chem. Phys., 23, 14801–14812, https://doi.org/10.5194/acp-23-14801-2023, https://doi.org/10.5194/acp-23-14801-2023, 2023
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Near-continuous measurements show the composition, sources, and seasonal variations of ultrafine particles (UFPs) in urban Beijing. Vehicle and cooking emissions and new particle formation are the main sources of UFPs, and aqueous/heterogeneous processes increase UFP mode diameters. UFPs are the highest in winter due to the highest primary particle emission rates and new particle formation rates, and CHO fractions are the highest in summer due to the strongest photooxidation.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
Atmos. Chem. Phys., 23, 12965–12983, https://doi.org/10.5194/acp-23-12965-2023, https://doi.org/10.5194/acp-23-12965-2023, 2023
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Highly oxygenated organic molecules (HOMs) form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOMs is largely controlled by the effect of NOx on the biogenic volatile organic compound oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
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In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
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New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Yishuo Guo, Chenjuan Deng, Aino Ovaska, Feixue Zheng, Chenjie Hua, Junlei Zhan, Yiran Li, Jin Wu, Zongcheng Wang, Jiali Xie, Ying Zhang, Tingyu Liu, Yusheng Zhang, Boying Song, Wei Ma, Yongchun Liu, Chao Yan, Jingkun Jiang, Veli-Matti Kerminen, Men Xia, Tuomo Nieminen, Wei Du, Tom Kokkonen, and Markku Kulmala
Atmos. Chem. Phys., 23, 6663–6690, https://doi.org/10.5194/acp-23-6663-2023, https://doi.org/10.5194/acp-23-6663-2023, 2023
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Using the comprehensive datasets, we investigated the long-term variations of air pollutants during winter in Beijing from 2019 to 2022 and analyzed the characteristics of atmospheric pollution cocktail during different short-term special events (e.g., Beijing Winter Olympics, COVID lockdown and Chinese New Year) associated with substantial emission reductions. Our results are useful in planning more targeted and sustainable long-term pollution control plans.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Anton Rusanen, Kristo Hõrrak, Lauri R. Ahonen, Tuomo Nieminen, Pasi P. Aalto, Pasi Kolari, Markku Kulmala, Tuukka Petäjä, and Heikki Junninen
Atmos. Meas. Tech., 16, 2781–2793, https://doi.org/10.5194/amt-16-2781-2023, https://doi.org/10.5194/amt-16-2781-2023, 2023
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We present a framework for setting up SMEAR (Station for Measuring Ecosystem–Atmosphere Relations) type measurement station data flows. This framework, called SMEARcore, consists of modular open-source software components that can be chosen to suit various station configurations. The benefits of using this framework are automation of routine operations and real-time monitoring of measurement results.
Juan Hong, Min Tang, Qiaoqiao Wang, Nan Ma, Shaowen Zhu, Shaobin Zhang, Xihao Pan, Linhong Xie, Guo Li, Uwe Kuhn, Chao Yan, Jiangchuan Tao, Ye Kuang, Yao He, Wanyun Xu, Runlong Cai, Yaqing Zhou, Zhibin Wang, Guangsheng Zhou, Bin Yuan, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 23, 5699–5713, https://doi.org/10.5194/acp-23-5699-2023, https://doi.org/10.5194/acp-23-5699-2023, 2023
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A comprehensive investigation of the characteristics of new particle formation (NPF) events was conducted at a rural site on the North China Plain (NCP), China, during the wintertime of 2018 by covering the particle number size distribution down to sub–3 nm. Potential mechanisms for NPF under the current environment were explored, followed by a further discussion on the factors governing the occurrence of NPF at this rural site compared with other regions (e.g., urban areas) in the NCP region.
Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
Atmos. Chem. Phys., 23, 5567–5585, https://doi.org/10.5194/acp-23-5567-2023, https://doi.org/10.5194/acp-23-5567-2023, 2023
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Ambient ion chemical composition measurements provide insight into trace gases that are precursors for the formation and growth of new aerosol particles. We use a new data analysis approach to increase the chemical information from these measurements. We analyze results from an agricultural region, a little studied land use type that is ~41 % of global land use, and find that the composition of gases important for aerosol formation and growth differs significantly from that in other ecosystems.
Rujing Yin, Xiaoxiao Li, Chao Yan, Runlong Cai, Ying Zhou, Juha Kangasluoma, Nina Sarnela, Janne Lampilahti, Tuukka Petäjä, Veli-Matti Kerminen, Federico Bianchi, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 5279–5296, https://doi.org/10.5194/acp-23-5279-2023, https://doi.org/10.5194/acp-23-5279-2023, 2023
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Atmospheric cluster ions are important constituents in the atmosphere. However, the quantitative research on their compositions is still limited, especially in urban environments. Here we demonstrate the feasibility of an in situ quantification method of cluster ions measured by a high-resolution mass spectrometer and reveal their governing factors, sources, and sinks in urban Beijing through quantitative analysis of cluster ions, reagent ions, neutral molecules, and condensation sink.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Ella Häkkinen, Jian Zhao, Frans Graeffe, Nicolas Fauré, Jordan E. Krechmer, Douglas Worsnop, Hilkka Timonen, Mikael Ehn, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 1705–1721, https://doi.org/10.5194/amt-16-1705-2023, https://doi.org/10.5194/amt-16-1705-2023, 2023
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Highly oxygenated compounds contribute to the formation and growth of atmospheric organic aerosol and thus impact the global climate. Knowledge of their transformations and fate after condensing into the particle phase has been limited by the lack of suitable detection techniques. Here, we present an online method for measuring highly oxygenated compounds from organic aerosol. We evaluate the performance of the method and demonstrate that the method is applicable to different organic species.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Yiqun Lu, Yingge Ma, Dan Dan Huang, Shengrong Lou, Sheng'ao Jing, Yaqin Gao, Hongli Wang, Yanjun Zhang, Hui Chen, Yunhua Chang, Naiqiang Yan, Jianmin Chen, Christian George, Matthieu Riva, and Cheng Huang
Atmos. Chem. Phys., 23, 3233–3245, https://doi.org/10.5194/acp-23-3233-2023, https://doi.org/10.5194/acp-23-3233-2023, 2023
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N-containing oxygenated organic molecules have been identified as important precursors of aerosol particles. We used an ultra-high-resolution mass spectrometer coupled with an online sample inlet to accurately measure their molecular composition, concentration level and variation patterns. We show their formation process and influencing factors in a Chinese megacity involving various volatile organic compound precursors and atmospheric oxidants, and we highlight the influence of PM2.5 episodes.
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Jingkun Jiang, Chao Yan, Markku Kulmala, and Jenni Kontkanen
Atmos. Chem. Phys., 22, 15071–15091, https://doi.org/10.5194/acp-22-15071-2022, https://doi.org/10.5194/acp-22-15071-2022, 2022
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We compare observed survival probabilities of atmospheric particles from Beijing, China, with survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower than or similar to theoretical survival probabilities. Uncertainties in condensation sink and growth rate are unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
Chenjuan Deng, Yiran Li, Chao Yan, Jin Wu, Runlong Cai, Dongbin Wang, Yongchun Liu, Juha Kangasluoma, Veli-Matti Kerminen, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 22, 13569–13580, https://doi.org/10.5194/acp-22-13569-2022, https://doi.org/10.5194/acp-22-13569-2022, 2022
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The size distributions of urban atmospheric particles convey important information on their origins and impacts. This study investigates the characteristics of typical particle size distributions and key gaseous precursors in the long term in urban Beijing. A fitting function is proposed to represent and help interpret size distribution including particles and gaseous precursors. In addition to NPF (new particle formation) as the major source, vehicles can emit sub-3 nm particles as well
Chao Yan, Yicheng Shen, Dominik Stolzenburg, Lubna Dada, Ximeng Qi, Simo Hakala, Anu-Maija Sundström, Yishuo Guo, Antti Lipponen, Tom V. Kokkonen, Jenni Kontkanen, Runlong Cai, Jing Cai, Tommy Chan, Liangduo Chen, Biwu Chu, Chenjuan Deng, Wei Du, Xiaolong Fan, Xu-Cheng He, Juha Kangasluoma, Joni Kujansuu, Mona Kurppa, Chang Li, Yiran Li, Zhuohui Lin, Yiliang Liu, Yuliang Liu, Yiqun Lu, Wei Nie, Jouni Pulliainen, Xiaohui Qiao, Yonghong Wang, Yifan Wen, Ye Wu, Gan Yang, Lei Yao, Rujing Yin, Gen Zhang, Shaojun Zhang, Feixue Zheng, Ying Zhou, Antti Arola, Johanna Tamminen, Pauli Paasonen, Yele Sun, Lin Wang, Neil M. Donahue, Yongchun Liu, Federico Bianchi, Kaspar R. Daellenbach, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Aijun Ding, Jingkun Jiang, and Markku Kulmala
Atmos. Chem. Phys., 22, 12207–12220, https://doi.org/10.5194/acp-22-12207-2022, https://doi.org/10.5194/acp-22-12207-2022, 2022
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Atmospheric new particle formation (NPF) is a dominant source of atmospheric ultrafine particles. In urban environments, traffic emissions are a major source of primary pollutants, but their contribution to NPF remains under debate. During the COVID-19 lockdown, traffic emissions were significantly reduced, providing a unique chance to examine their relevance to NPF. Based on our comprehensive measurements, we demonstrate that traffic emissions alone are not able to explain the NPF in Beijing.
Sini Isokääntä, Paul Kim, Santtu Mikkonen, Thomas Kühn, Harri Kokkola, Taina Yli-Juuti, Liine Heikkinen, Krista Luoma, Tuukka Petäjä, Zak Kipling, Daniel Partridge, and Annele Virtanen
Atmos. Chem. Phys., 22, 11823–11843, https://doi.org/10.5194/acp-22-11823-2022, https://doi.org/10.5194/acp-22-11823-2022, 2022
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This research employs air mass history analysis and observations to study how clouds and precipitation affect atmospheric aerosols during transport to a boreal forest site. The mass concentrations of studied chemical species showed exponential decrease as a function of accumulated rain along the air mass route. Our analysis revealed in-cloud sulfate formation, while no major changes in organic mass were seen. Most of the in-cloud-formed sulfate could be assigned to particle sizes above 200 nm.
Runlong Cai, Ella Häkkinen, Chao Yan, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 11529–11541, https://doi.org/10.5194/acp-22-11529-2022, https://doi.org/10.5194/acp-22-11529-2022, 2022
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The influences of new particle formation on the climate and air quality are governed by particle survival, which has been under debate due to uncertainties in the coagulation sink. Here we measure the coagulation coefficient of sub-10 nm particles and demonstrate that collisions between the freshly nucleated and background particles can effectively lead to coagulation. We further show that the effective coagulation sink is consistent with the new particle formation measured in urban Beijing.
Benjamin Foreback, Lubna Dada, Kaspar R. Daellenbach, Chao Yan, Lili Wang, Biwu Chu, Ying Zhou, Tom V. Kokkonen, Mona Kurppa, Rosaria E. Pileci, Yonghong Wang, Tommy Chan, Juha Kangasluoma, Lin Zhuohui, Yishou Guo, Chang Li, Rima Baalbaki, Joni Kujansuu, Xiaolong Fan, Zemin Feng, Pekka Rantala, Shahzad Gani, Federico Bianchi, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, Yongchun Liu, and Pauli Paasonen
Atmos. Chem. Phys., 22, 11089–11104, https://doi.org/10.5194/acp-22-11089-2022, https://doi.org/10.5194/acp-22-11089-2022, 2022
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This study analyzed air quality in Beijing during the Chinese New Year over 7 years, including data from a new in-depth measurement station. This is one of few studies to look at long-term impacts, including the outcome of firework restrictions starting in 2018. Results show that firework pollution has gone down since 2016, indicating a positive result from the restrictions. Results of this study may be useful in making future decisions about the use of fireworks to improve air quality.
Yishuo Guo, Chao Yan, Yuliang Liu, Xiaohui Qiao, Feixue Zheng, Ying Zhang, Ying Zhou, Chang Li, Xiaolong Fan, Zhuohui Lin, Zemin Feng, Yusheng Zhang, Penggang Zheng, Linhui Tian, Wei Nie, Zhe Wang, Dandan Huang, Kaspar R. Daellenbach, Lei Yao, Lubna Dada, Federico Bianchi, Jingkun Jiang, Yongchun Liu, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 10077–10097, https://doi.org/10.5194/acp-22-10077-2022, https://doi.org/10.5194/acp-22-10077-2022, 2022
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Gaseous oxygenated organic molecules (OOMs) are able to form atmospheric aerosols, which will impact on human health and climate change. Here, we find that OOMs in urban Beijing are dominated by anthropogenic sources, i.e. aromatic (29 %–41 %) and aliphatic (26 %–41 %) OOMs. They are also the main contributors to the condensational growth of secondary organic aerosols (SOAs). Therefore, the restriction on anthropogenic VOCs is crucial for the reduction of SOAs and haze formation.
Lisa J. Beck, Siegfried Schobesberger, Heikki Junninen, Janne Lampilahti, Antti Manninen, Lubna Dada, Katri Leino, Xu-Cheng He, Iida Pullinen, Lauriane L. J. Quéléver, Anna Franck, Pyry Poutanen, Daniela Wimmer, Frans Korhonen, Mikko Sipilä, Mikael Ehn, Douglas R. Worsnop, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 8547–8577, https://doi.org/10.5194/acp-22-8547-2022, https://doi.org/10.5194/acp-22-8547-2022, 2022
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The presented article introduces an overview of atmospheric ions and their composition above the boreal forest. We provide the results of an extensive airborne measurement campaign with an air ion mass spectrometer and particle measurements, showing their diurnal evolution within the boundary layer and free troposphere. In addition, we compare the airborne dataset with the co-located data from the ground at SMEAR II station, Finland.
Lauriane L. J. Quéléver, Lubna Dada, Eija Asmi, Janne Lampilahti, Tommy Chan, Jonathan E. Ferrara, Gustavo E. Copes, German Pérez-Fogwill, Luis Barreira, Minna Aurela, Douglas R. Worsnop, Tuija Jokinen, and Mikko Sipilä
Atmos. Chem. Phys., 22, 8417–8437, https://doi.org/10.5194/acp-22-8417-2022, https://doi.org/10.5194/acp-22-8417-2022, 2022
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Understanding how aerosols form is crucial for correctly modeling the climate and improving future predictions. This work provides extensive analysis of aerosol particles and their precursors at Marambio Station, Antarctic Peninsula. We show that sulfuric acid, ammonia, and dimethylamine are key contributors to the frequent new particle formation events observed at the site. We discuss nucleation mechanisms and highlight the need for targeted measurement to fully understand these processes.
Yuanyuan Luo, Olga Garmash, Haiyan Li, Frans Graeffe, Arnaud P. Praplan, Anssi Liikanen, Yanjun Zhang, Melissa Meder, Otso Peräkylä, Josep Peñuelas, Ana María Yáñez-Serrano, and Mikael Ehn
Atmos. Chem. Phys., 22, 5619–5637, https://doi.org/10.5194/acp-22-5619-2022, https://doi.org/10.5194/acp-22-5619-2022, 2022
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Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and we characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Ying Zhou, Simo Hakala, Chao Yan, Yang Gao, Xiaohong Yao, Biwu Chu, Tommy Chan, Juha Kangasluoma, Shahzad Gani, Jenni Kontkanen, Pauli Paasonen, Yongchun Liu, Tuukka Petäjä, Markku Kulmala, and Lubna Dada
Atmos. Chem. Phys., 21, 17885–17906, https://doi.org/10.5194/acp-21-17885-2021, https://doi.org/10.5194/acp-21-17885-2021, 2021
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We characterized the connection between new particle formation (NPF) events in terms of frequency, intensity and growth at a near-highway location in central Beijing and at a background mountain site 80 km away. Due to the substantial contribution of NPF to the global aerosol budget, identifying the conditions that promote the occurrence of regional NPF events could help understand their contribution on a large scale and would improve their implementation in global models.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
Ditte Taipale, Veli-Matti Kerminen, Mikael Ehn, Markku Kulmala, and Ülo Niinemets
Atmos. Chem. Phys., 21, 17389–17431, https://doi.org/10.5194/acp-21-17389-2021, https://doi.org/10.5194/acp-21-17389-2021, 2021
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Larval feeding and fungal infections of leaves can greatly change the emission of volatile compounds from plants and thereby influence aerosol processes in the air. We developed a model that considers the dynamics of larvae and fungi and the dependency of the emission on the severity of stress. We show that the infections can be highly atmospherically relevant during long periods of time and at times more important to consider than the parameters that are currently used in emission models.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Yuliang Liu, Wei Nie, Yuanyuan Li, Dafeng Ge, Chong Liu, Zhengning Xu, Liangduo Chen, Tianyi Wang, Lei Wang, Peng Sun, Ximeng Qi, Jiaping Wang, Zheng Xu, Jian Yuan, Chao Yan, Yanjun Zhang, Dandan Huang, Zhe Wang, Neil M. Donahue, Douglas Worsnop, Xuguang Chi, Mikael Ehn, and Aijun Ding
Atmos. Chem. Phys., 21, 14789–14814, https://doi.org/10.5194/acp-21-14789-2021, https://doi.org/10.5194/acp-21-14789-2021, 2021
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Oxygenated organic molecules (OOMs) are crucial intermediates linking volatile organic compounds to secondary organic aerosols. Using nitrate time-of-flight chemical ionization mass spectrometry in eastern China, we performed positive matrix factorization (PMF) on binned OOM mass spectra. We reconstructed over 1000 molecules from 14 derived PMF factors and identified about 72 % of the observed OOMs as organic nitrates, highlighting the decisive role of NOx in OOM formation in populated areas.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Yongchun Liu, Zemin Feng, Feixue Zheng, Xiaolei Bao, Pengfei Liu, Yanli Ge, Yan Zhao, Tao Jiang, Yunwen Liao, Yusheng Zhang, Xiaolong Fan, Chao Yan, Biwu Chu, Yonghong Wang, Wei Du, Jing Cai, Federico Bianchi, Tuukka Petäjä, Yujing Mu, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 21, 13269–13286, https://doi.org/10.5194/acp-21-13269-2021, https://doi.org/10.5194/acp-21-13269-2021, 2021
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The mechanisms and kinetics of particulate sulfate formation in the atmosphere are still open questions although they have been extensively discussed. We found that uptake of SO2 is the rate-determining step for the conversion of SO2 to particulate sulfate. NH4NO3 plays an important role in AWC, the phase state of aerosol particles, and subsequently the uptake kinetics of SO2 under high-RH conditions. This work is a good example of the feedback between aerosol physics and aerosol chemistry.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
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We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
Luis M. F. Barreira, Arttu Ylisirniö, Iida Pullinen, Angela Buchholz, Zijun Li, Helina Lipp, Heikki Junninen, Urmas Hõrrak, Steffen M. Noe, Alisa Krasnova, Dmitrii Krasnov, Kaia Kask, Eero Talts, Ülo Niinemets, Jose Ruiz-Jimenez, and Siegfried Schobesberger
Atmos. Chem. Phys., 21, 11781–11800, https://doi.org/10.5194/acp-21-11781-2021, https://doi.org/10.5194/acp-21-11781-2021, 2021
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We present results from PM1 atmospheric composition and concentration measurements performed in a springtime hemiboreal forest. Sesquiterpene mixing ratios and particle-phase concentrations of corresponding oxidation products were rapidly increasing on some early mornings. The particle volatility suggested that condensable sesquiterpene oxidation products are rapidly formed in the atmosphere. The results revealed the importance of sesquiterpenes for secondary organic aerosol particulate mass.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
Xiaolong Fan, Jing Cai, Chao Yan, Jian Zhao, Yishuo Guo, Chang Li, Kaspar R. Dällenbach, Feixue Zheng, Zhuohui Lin, Biwu Chu, Yonghong Wang, Lubna Dada, Qiaozhi Zha, Wei Du, Jenni Kontkanen, Theo Kurtén, Siddhart Iyer, Joni T. Kujansuu, Tuukka Petäjä, Douglas R. Worsnop, Veli-Matti Kerminen, Yongchun Liu, Federico Bianchi, Yee Jun Tham, Lei Yao, and Markku Kulmala
Atmos. Chem. Phys., 21, 11437–11452, https://doi.org/10.5194/acp-21-11437-2021, https://doi.org/10.5194/acp-21-11437-2021, 2021
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We observed significant concentrations of gaseous HBr and HCl throughout the winter and springtime in urban Beijing, China. Our results indicate that gaseous HCl and HBr are most likely originated from anthropogenic emissions such as burning activities, and the gas–aerosol partitioning may play a crucial role in contributing to the gaseous HCl and HBr. These observations suggest that there is an important recycling pathway of halogen species in inland megacities.
Liine Heikkinen, Mikko Äijälä, Kaspar R. Daellenbach, Gang Chen, Olga Garmash, Diego Aliaga, Frans Graeffe, Meri Räty, Krista Luoma, Pasi Aalto, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 21, 10081–10109, https://doi.org/10.5194/acp-21-10081-2021, https://doi.org/10.5194/acp-21-10081-2021, 2021
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In many locations worldwide aerosol particles have been shown to be made up of organic aerosol (OA). The boreal forest is a region where aerosol particles possess a high OA mass fraction. Here, we studied OA composition using the longest time series of OA composition ever obtained from a boreal environment. For this purpose, we tested a new analysis framework and discovered that most of the OA was highly oxidized, with strong seasonal behaviour reflecting different sources in summer and winter.
Magdalena Okuljar, Heino Kuuluvainen, Jenni Kontkanen, Olga Garmash, Miska Olin, Jarkko V. Niemi, Hilkka Timonen, Juha Kangasluoma, Yee Jun Tham, Rima Baalbaki, Mikko Sipilä, Laura Salo, Henna Lintusaari, Harri Portin, Kimmo Teinilä, Minna Aurela, Miikka Dal Maso, Topi Rönkkö, Tuukka Petäjä, and Pauli Paasonen
Atmos. Chem. Phys., 21, 9931–9953, https://doi.org/10.5194/acp-21-9931-2021, https://doi.org/10.5194/acp-21-9931-2021, 2021
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To estimate the relative contribution of different sources to the particle population in an urban environment, we conducted simultaneous measurements at a street canyon and an urban background station in Helsinki. We investigated the contribution of traffic and new particle formation to particles with a diameter between 1 and 800 nm. We found that during spring traffic does not dominate the particles smaller than 3 nm at either of the stations.
Wei Huang, Haiyan Li, Nina Sarnela, Liine Heikkinen, Yee Jun Tham, Jyri Mikkilä, Steven J. Thomas, Neil M. Donahue, Markku Kulmala, and Federico Bianchi
Atmos. Chem. Phys., 21, 8961–8977, https://doi.org/10.5194/acp-21-8961-2021, https://doi.org/10.5194/acp-21-8961-2021, 2021
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We show full characterization of gaseous organic compounds in a boreal forest. Molecular composition and volatility of gaseous organic compounds with different oxidation extents (from volatile organic compounds to highly oxygenated organic molecules) were investigated and discussed. We provide a more comprehensive understanding of atmospheric organic compounds in this boreal forest and new insights into interpreting ambient measurements or testing and improving parameterizations in models.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys., 21, 7357–7372, https://doi.org/10.5194/acp-21-7357-2021, https://doi.org/10.5194/acp-21-7357-2021, 2021
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Cyclohexene resembles certain relatively complex compounds in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOMs) formed in cyclohexene ozonolysis, the relationship between their chemical composition and their tendency to condense onto seed aerosol, as well as the effect of NOx pollutants on their signals. Two existing models were also tested for their ability to predict the volatility of the HOMs.
Yishuo Guo, Chao Yan, Chang Li, Wei Ma, Zemin Feng, Ying Zhou, Zhuohui Lin, Lubna Dada, Dominik Stolzenburg, Rujing Yin, Jenni Kontkanen, Kaspar R. Daellenbach, Juha Kangasluoma, Lei Yao, Biwu Chu, Yonghong Wang, Runlong Cai, Federico Bianchi, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 5499–5511, https://doi.org/10.5194/acp-21-5499-2021, https://doi.org/10.5194/acp-21-5499-2021, 2021
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Fog, cloud and haze are very common natural phenomena. Sulfuric acid (SA) is one of the key compounds forming those suspended particles, technically called aerosols, through gas-to-particle conversion. Therefore, the concentration level, source and sink of SA is very important. Our results show that ozonolysis of alkenes plays a major role in nighttime SA formation under unpolluted conditions in urban Beijing, and nighttime cluster mode particles are probably driven by SA in urban environments.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Runlong Cai, Yihao Li, Yohann Clément, Dandan Li, Clément Dubois, Marlène Fabre, Laurence Besson, Sebastien Perrier, Christian George, Mikael Ehn, Cheng Huang, Ping Yi, Yingge Ma, and Matthieu Riva
Atmos. Meas. Tech., 14, 2377–2387, https://doi.org/10.5194/amt-14-2377-2021, https://doi.org/10.5194/amt-14-2377-2021, 2021
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Orbitool is an open-source software tool, mainly coded in Python, with a graphical user interface (GUI), specifically developed to facilitate the analysis of online Orbitrap mass spectrometric data. It is notably optimized for long-term atmospheric measurements and laboratory studies.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Runlong Cai, Chao Yan, Dongsen Yang, Rujing Yin, Yiqun Lu, Chenjuan Deng, Yueyun Fu, Jiaxin Ruan, Xiaoxiao Li, Jenni Kontkanen, Qiang Zhang, Juha Kangasluoma, Yan Ma, Jiming Hao, Douglas R. Worsnop, Federico Bianchi, Pauli Paasonen, Veli-Matti Kerminen, Yongchun Liu, Lin Wang, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 21, 2457–2468, https://doi.org/10.5194/acp-21-2457-2021, https://doi.org/10.5194/acp-21-2457-2021, 2021
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Based on long-term measurements, we discovered that the collision of H2SO4–amine clusters is the governing mechanism that initializes fast new particle formation in the polluted atmospheric environment of urban Beijing. The mechanism and the governing factors for H2SO4–amine nucleation in the polluted atmosphere are quantitatively investigated in this study.
Runlong Cai, Chenxi Li, Xu-Cheng He, Chenjuan Deng, Yiqun Lu, Rujing Yin, Chao Yan, Lin Wang, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 21, 2287–2304, https://doi.org/10.5194/acp-21-2287-2021, https://doi.org/10.5194/acp-21-2287-2021, 2021
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Growth rate determines the survival probability of atmospheric new particles and hence their impacts. We clarify the impacts of coagulation on the values retrieved by the appearance time method, which is widely used for growth rate evaluation. A new formula with coagulation correction is proposed based on derivation and tested using both models and atmospheric data. We show that the sub-3 nm particle growth rate in polluted environments may be overestimated without the coagulation correction.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943, https://doi.org/10.5194/amt-14-923-2021, https://doi.org/10.5194/amt-14-923-2021, 2021
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Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Juha Sulo, Nina Sarnela, Jenni Kontkanen, Lauri Ahonen, Pauli Paasonen, Tiia Laurila, Tuija Jokinen, Juha Kangasluoma, Heikki Junninen, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Katrianne Lehtipalo
Atmos. Chem. Phys., 21, 695–715, https://doi.org/10.5194/acp-21-695-2021, https://doi.org/10.5194/acp-21-695-2021, 2021
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In this study, we analyzed over 5 years of sub-3 nm particle concentrations and their precursor vapors, identifying atmoshperic vapors important to the formation of these particles in the boreal forest. We also observed seasonal differences in both particle and precursor vapor concentrations and the formation pathways of these particles. Our results confirm the importance of organic vapors in atmospheric aerosol formation and highlight key seasonal differences that require further study.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Helmi-Marja Keskinen, Ilona Ylivinkka, Liine Heikkinen, Pasi P. Aalto, Tuomo Nieminen, Katrianne Lehtipalo, Juho Aalto, Janne Levula, Jutta Kesti, Lauri R. Ahonen, Ekaterina Ezhova, Markku Kulmala, and Tuukka Petäjä
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-447, https://doi.org/10.5194/amt-2020-447, 2020
Publication in AMT not foreseen
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Long-term (2005–2017) aerosol particulate matter (PM) concentration measurements at Finland at Station for Measuring Ecosystem-Atmosphere Relations (SMEAR II, Hyytiälä) have been measured with three different measurement equipment. The comparison revealed an equivalence among the three methods. Mass concentrations were generally highest in summer. The descending trend was visible here in spring, summer and winter. This might have resulted at least partly from air quality legislation.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Jingsha Xu, Shaojie Song, Roy M. Harrison, Congbo Song, Lianfang Wei, Qiang Zhang, Yele Sun, Lu Lei, Chao Zhang, Xiaohong Yao, Dihui Chen, Weijun Li, Miaomiao Wu, Hezhong Tian, Lining Luo, Shengrui Tong, Weiran Li, Junling Wang, Guoliang Shi, Yanqi Huangfu, Yingze Tian, Baozhu Ge, Shaoli Su, Chao Peng, Yang Chen, Fumo Yang, Aleksandra Mihajlidi-Zelić, Dragana Đorđević, Stefan J. Swift, Imogen Andrews, Jacqueline F. Hamilton, Ye Sun, Agung Kramawijaya, Jinxiu Han, Supattarachai Saksakulkrai, Clarissa Baldo, Siqi Hou, Feixue Zheng, Kaspar R. Daellenbach, Chao Yan, Yongchun Liu, Markku Kulmala, Pingqing Fu, and Zongbo Shi
Atmos. Meas. Tech., 13, 6325–6341, https://doi.org/10.5194/amt-13-6325-2020, https://doi.org/10.5194/amt-13-6325-2020, 2020
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An interlaboratory comparison was conducted for the first time to examine differences in water-soluble inorganic ions (WSIIs) measured by 10 labs using ion chromatography (IC) and by two online aerosol chemical speciation monitor (ACSM) methods. Major ions including SO42−, NO3− and NH4+ agreed well in 10 IC labs and correlated well with ACSM data. WSII interlab variability strongly affected aerosol acidity results based on ion balance, but aerosol pH computed by ISORROPIA II was very similar.
Yongchun Liu, Yusheng Zhang, Chaofan Lian, Chao Yan, Zeming Feng, Feixue Zheng, Xiaolong Fan, Yan Chen, Weigang Wang, Biwu Chu, Yonghong Wang, Jing Cai, Wei Du, Kaspar R. Daellenbach, Juha Kangasluoma, Federico Bianchi, Joni Kujansuu, Tuukka Petäjä, Xuefei Wang, Bo Hu, Yuesi Wang, Maofa Ge, Hong He, and Markku Kulmala
Atmos. Chem. Phys., 20, 13023–13040, https://doi.org/10.5194/acp-20-13023-2020, https://doi.org/10.5194/acp-20-13023-2020, 2020
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Understanding of the chemical and physical processes leading to atmospheric aerosol particle formation is crucial to devising effective mitigation strategies to protect the public and reduce uncertainties in climate predictions. We found that the photolysis of nitrous acid could promote the formation of organic and nitrate aerosol and that traffic-related emission is a major contributor to ambient nitrous acid on haze days in wintertime in Beijing.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Lubna Dada, Ilona Ylivinkka, Rima Baalbaki, Chang Li, Yishuo Guo, Chao Yan, Lei Yao, Nina Sarnela, Tuija Jokinen, Kaspar R. Daellenbach, Rujing Yin, Chenjuan Deng, Biwu Chu, Tuomo Nieminen, Yonghong Wang, Zhuohui Lin, Roseline C. Thakur, Jenni Kontkanen, Dominik Stolzenburg, Mikko Sipilä, Tareq Hussein, Pauli Paasonen, Federico Bianchi, Imre Salma, Tamás Weidinger, Michael Pikridas, Jean Sciare, Jingkun Jiang, Yongchun Liu, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 20, 11747–11766, https://doi.org/10.5194/acp-20-11747-2020, https://doi.org/10.5194/acp-20-11747-2020, 2020
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We rely on sulfuric acid measurements in four contrasting environments, Hyytiälä, Finland; Agia Marina, Cyprus; Budapest, Hungary; and Beijing, China, representing semi-pristine boreal forest, rural environment in the Mediterranean area, urban environment, and heavily polluted megacity, respectively, in order to define the sources and sinks of sulfuric acid in these environments and to derive a new sulfuric acid proxy to be utilized in locations and during periods when it is not measured.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Liine Heikkinen, Mikko Äijälä, Matthieu Riva, Krista Luoma, Kaspar Dällenbach, Juho Aalto, Pasi Aalto, Diego Aliaga, Minna Aurela, Helmi Keskinen, Ulla Makkonen, Pekka Rantala, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 3151–3180, https://doi.org/10.5194/acp-20-3151-2020, https://doi.org/10.5194/acp-20-3151-2020, 2020
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Atmospheric aerosols are solid or liquid particles suspended in the air. They are known as a health risk, but they also influence the Earth's climate. The composition of aerosols becomes important when predicting their effect on climate. We show both seasonal and year-to-year variability of aerosol chemical composition in the boreal forest of Finland. We observed a consistent bimodal seasonal trend: a biogenic summertime maximum and an anthropogenic wintertime maximum in the mass concentration.
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.
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.
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.
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.
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
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.
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.
Ingeborg E. Nielsen, Henrik Skov, Andreas Massling, Axel C. Eriksson, Manuel Dall'Osto, Heikki Junninen, Nina Sarnela, Robert Lange, Sonya Collier, Qi Zhang, Christopher D. Cappa, and Jacob K. Nøjgaard
Atmos. Chem. Phys., 19, 10239–10256, https://doi.org/10.5194/acp-19-10239-2019, https://doi.org/10.5194/acp-19-10239-2019, 2019
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Measurements of the chemical composition of sub-micrometer aerosols were carried out in northern Greenland during the Arctic haze (February–May) where concentrations are high due to favorable conditions for long-range transport. Sulfate was the dominant aerosol (66 %), followed by organic matter (24 %). The highest black carbon concentrations where observed in February. Source apportionment yielded three factors: a primary factor (12 %), an Arctic haze factor (64 %) and a marine factor (22 %).
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.
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.
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.
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.
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.
Sri Hapsari Budisulistiorini, Matthieu Riva, Michael Williams, Takuma Miyakawa, Jing Chen, Masayuki Itoh, Jason D. Surratt, and Mikinori Kuwata
Atmos. Chem. Phys., 18, 16481–16498, https://doi.org/10.5194/acp-18-16481-2018, https://doi.org/10.5194/acp-18-16481-2018, 2018
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Wildfire emits a large number of haze particles. During transport in the atmosphere, the organic aerosol in the haze particles can undergo atmospheric processes and become highly oxidized. We show that the haze particles transported from wildfires in Indonesia are dominated by oxygenated organic aerosols. This study highlights the impact of atmospheric processes on the transboundary haze particles.
Chao Yan, Lubna Dada, Clémence Rose, Tuija Jokinen, Wei Nie, Siegfried Schobesberger, Heikki Junninen, Katrianne Lehtipalo, Nina Sarnela, Ulla Makkonen, Olga Garmash, Yonghong Wang, Qiaozhi Zha, Pauli Paasonen, Federico Bianchi, Mikko Sipilä, Mikael Ehn, Tuukka Petäjä, Veli-Matti Kerminen, Douglas R. Worsnop, and Markku Kulmala
Atmos. Chem. Phys., 18, 13231–13243, https://doi.org/10.5194/acp-18-13231-2018, https://doi.org/10.5194/acp-18-13231-2018, 2018
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Ions can play an important role in atmospheric new particle formation by stabilizing the embryonic clusters. Such a process is called ion-induced nucleation (IIN). We found two distinct IIN mechanisms – driven by H2SO4-NH3 clusters and by organic vapors, respectively. The concentration ratio of organic vapors to H2SO4 regulates via which pathway the IIN occur. As the organic vapor concentration is influenced by temperature, a seasonal variation in the main IIN mechanism can be expected.
Yee Jun Tham, Zhe Wang, Qinyi Li, Weihao Wang, Xinfeng Wang, Keding Lu, Nan Ma, Chao Yan, Simonas Kecorius, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
Atmos. Chem. Phys., 18, 13155–13171, https://doi.org/10.5194/acp-18-13155-2018, https://doi.org/10.5194/acp-18-13155-2018, 2018
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This study addresses the limited understanding of heterogeneous N2O5 uptake and ClNO2 production in the polluted environment of China. The results showed that N2O5 uptake and ClNO2 yield cannot be well explained by previous parameterizations and were largely influenced by factors like aerosol water content and biomass burning emission. Our findings illuminate the need to realistically parameterize these heterogeneous processes for better simulation of photochemical and haze pollution in China.
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.
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.
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.
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.
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.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
Lei Yao, Ming-Yi Wang, Xin-Ke Wang, Yi-Jun Liu, Hang-Fei Chen, Jun Zheng, Wei Nie, Ai-Jun Ding, Fu-Hai Geng, Dong-Fang Wang, Jian-Min Chen, Douglas R. Worsnop, and Lin Wang
Atmos. Chem. Phys., 16, 14527–14543, https://doi.org/10.5194/acp-16-14527-2016, https://doi.org/10.5194/acp-16-14527-2016, 2016
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We present the development of a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) method, utilizing protonated ethanol as reagent ions to simultaneously detect atmospheric gaseous amines (C1 to C6) and amides (C1 to C6). Deployment of this ethanol HR-ToF-CIMS has been demonstrated in a field campaign in urban Shanghai, China, detecting amines (from a few pptv to hundreds of pptv) and amides (from tens of pptv to a few ppbv).
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.
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.
Hilkka Timonen, Mike Cubison, Minna Aurela, David Brus, Heikki Lihavainen, Risto Hillamo, Manjula Canagaratna, Bettina Nekat, Rolf Weller, Douglas Worsnop, and Sanna Saarikoski
Atmos. Meas. Tech., 9, 3263–3281, https://doi.org/10.5194/amt-9-3263-2016, https://doi.org/10.5194/amt-9-3263-2016, 2016
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The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power (m∕Δm50 ∼ 500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements and ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results.
Jordan E. Krechmer, Michael Groessl, Xuan Zhang, Heikki Junninen, Paola Massoli, Andrew T. Lambe, Joel R. Kimmel, Michael J. Cubison, Stephan Graf, Ying-Hsuan Lin, Sri H. Budisulistiorini, Haofei Zhang, Jason D. Surratt, Richard Knochenmuss, John T. Jayne, Douglas R. Worsnop, Jose-Luis Jimenez, and Manjula R. Canagaratna
Atmos. Meas. Tech., 9, 3245–3262, https://doi.org/10.5194/amt-9-3245-2016, https://doi.org/10.5194/amt-9-3245-2016, 2016
Yele Sun, Wei Du, Pingqing Fu, Qingqing Wang, Jie Li, Xinlei Ge, Qi Zhang, Chunmao Zhu, Lujie Ren, Weiqi Xu, Jian Zhao, Tingting Han, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 16, 8309–8329, https://doi.org/10.5194/acp-16-8309-2016, https://doi.org/10.5194/acp-16-8309-2016, 2016
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We have a comprehensive characterization of the sources, variations and processes of submicron aerosols in Beijing in winter using HR-AMS and GC/MS measurements. The primary sources including traffic, cooking, biomass burning and coal combustion emissions, and secondary components were separated and quantified with PMF. Our results elucidated the important roles of primary emissions, particularly coal combustion, and aqueous-phase processing in the formation of severe air pollution in winter.
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.
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
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
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.
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.
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.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
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.
W. Q. Xu, Y. L. Sun, C. Chen, W. Du, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, X. J. Zhao, L. B. Zhou, D. S. Ji, P. C. Wang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 13681–13698, https://doi.org/10.5194/acp-15-13681-2015, https://doi.org/10.5194/acp-15-13681-2015, 2015
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We have investigated the response of aerosol composition, size distributions, and oxidation properties to emission controls during the 2014 Asia- Pacific Economic Cooperation (APEC) summit in Beijing. Our results showed substantial changes of aerosol bulk composition during APEC with the most reductions in secondary aerosols in large accumulation modes, demonstrating that that emission controls over regional scales can substantially reduce secondary particulates.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
V. Crenn, J. Sciare, P. L. Croteau, S. Verlhac, R. Fröhlich, C. A. Belis, W. Aas, M. Äijälä, A. Alastuey, B. Artiñano, D. Baisnée, N. Bonnaire, M. Bressi, M. Canagaratna, F. Canonaco, C. Carbone, F. Cavalli, E. Coz, M. J. Cubison, J. K. Esser-Gietl, D. C. Green, V. Gros, L. Heikkinen, H. Herrmann, C. Lunder, M. C. Minguillón, G. Močnik, C. D. O'Dowd, J. Ovadnevaite, J.-E. Petit, E. Petralia, L. Poulain, M. Priestman, V. Riffault, A. Ripoll, R. Sarda-Estève, J. G. Slowik, A. Setyan, A. Wiedensohler, U. Baltensperger, A. S. H. Prévôt, J. T. Jayne, and O. Favez
Atmos. Meas. Tech., 8, 5063–5087, https://doi.org/10.5194/amt-8-5063-2015, https://doi.org/10.5194/amt-8-5063-2015, 2015
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A large intercomparison study of 13 Q-ACSM was conducted for a 3-week period in the region of Paris to evaluate the performance of this instrument and to monitor the major NR-PM1 chemical components. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were found to be 9, 15, 19, 28, and 36% for NR-PM1, NO3, OM, SO4, and NH4, respectively. Some recommendations regarding best calibration practices, standardized data processing and data treatment are also provided.
C. Chen, Y. L. Sun, W. Q. Xu, W. Du, L. B. Zhou, T. T. Han, Q. Q. Wang, P. Q. Fu, Z. F. Wang, Z. Q. Gao, Q. Zhang, and D. R. Worsnop
Atmos. Chem. Phys., 15, 12879–12895, https://doi.org/10.5194/acp-15-12879-2015, https://doi.org/10.5194/acp-15-12879-2015, 2015
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A comprehensive characterization of submicron aerosol composition and sources at 260m in urban Beijing during APEC 2014 is presented. Aerosol species were shown to decrease substantially by 40–80% during APEC, whereas the bulk composition was relatively similar to the result of synergetic controls of secondary precursors. Our results elucidated that the good air quality during APEC was the combined result of emission controls and meteorological effects, with the former playing the dominant role.
S. Carbone, T. Onasch, S. Saarikoski, H. Timonen, K. Saarnio, D. Sueper, T. Rönkkö, L. Pirjola, A. Häyrinen, D. Worsnop, and R. Hillamo
Atmos. Meas. Tech., 8, 4803–4815, https://doi.org/10.5194/amt-8-4803-2015, https://doi.org/10.5194/amt-8-4803-2015, 2015
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The purpose of this study was to develop a method for the quantification of trace metal content in black carbon aerosol in real time, such as combustion-related emissions, by using the SP-AMS. The properties of 13 different trace metals (Na, Al, Ca, V, Cr, Fe, Mn, Ni, Cu, Zn, Rb, Sr and Ba) were investigated in a controlled laboratory experiment. The results from the laboratory tests were applied to study fine particles in emissions of a heavy-fuel-oil-fired heating station.
J. C. Corbin, A. Othman, J. D. Allan, D. R. Worsnop, J. D. Haskins, B. Sierau, U. Lohmann, and A. A. Mensah
Atmos. Meas. Tech., 8, 4615–4636, https://doi.org/10.5194/amt-8-4615-2015, https://doi.org/10.5194/amt-8-4615-2015, 2015
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Peak-integration uncertainties in the Aerodyne high-resolution aerosol mass spectrometer (AMS) are analyzed in detail using a combination of empirical data analysis and Monte Carlo approaches. The most general conclusion, applicable to any mass spectrometer, is that non-zero mass accuracy leads to a percentage error in constrained peak fits, even for well-resolved peaks. For overlapping peaks, this mass-accuracy effect may be viewed as a reduction in the effective m/z-calibration precision.
J. Hong, J. Kim, T. Nieminen, J. Duplissy, M. Ehn, M. Äijälä, L. Q. Hao, W. Nie, N. Sarnela, N. L. Prisle, M. Kulmala, A. Virtanen, T. Petäjä, and V.-M. Kerminen
Atmos. Chem. Phys., 15, 11999–12009, https://doi.org/10.5194/acp-15-11999-2015, https://doi.org/10.5194/acp-15-11999-2015, 2015
R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, F. Canonaco, P. L. Croteau, M. Gysel, S. Henne, E. Herrmann, J. T. Jayne, M. Steinbacher, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11373–11398, https://doi.org/10.5194/acp-15-11373-2015, https://doi.org/10.5194/acp-15-11373-2015, 2015
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This manuscript presents the first long-term (14-month) and highly time-resolved (10 min) measurements of NR-PM1 aerosol chemical composition at a high-altitude site (JFJ, Switzerland, 3580m a.s.l.). The elevated location allowed the investigation of free tropospheric aerosol year round. Total and relative mass loadings, diurnal variations as well as seasonal variations are discussed together with geographical origin, organic aerosol sources and the influence of the planetary boundary layer.
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
P. Roldin, L. Liao, D. Mogensen, M. Dal Maso, A. Rusanen, V.-M. Kerminen, T. F. Mentel, J. Wildt, E. Kleist, A. Kiendler-Scharr, R. Tillmann, M. Ehn, M. Kulmala, and M. Boy
Atmos. Chem. Phys., 15, 10777–10798, https://doi.org/10.5194/acp-15-10777-2015, https://doi.org/10.5194/acp-15-10777-2015, 2015
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We used the ADCHAM model to study new particle formation events in the JPAC chamber. The model results show that the new particles may be formed by a kinetic type of nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of volatile organic compounds (VOCs). The observed particle growth may either be controlled by the condensation of semi- and low-volatililty organic compounds or by the formation of low-volatility compounds (oligomers) at the particle surface.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
Y. L. Sun, Z. F. Wang, W. Du, Q. Zhang, Q. Q. Wang, P. Q. Fu, X. L. Pan, J. Li, J. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 10149–10165, https://doi.org/10.5194/acp-15-10149-2015, https://doi.org/10.5194/acp-15-10149-2015, 2015
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We conducted the first long-term real-time measurement of submicron aerosol composition in Beijing using an ACSM for 1 year. The seasonal variations of mass concentrations and chemical composition of submicron aerosol were investigated in detail, and the meteorological effects on aerosol chemistry, particularly temperature and relative humidity, were elucidated. Finally, the potential source areas of aerosol species during four seasons were identified.
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
P. Zieger, P. P. Aalto, V. Aaltonen, M. Äijälä, J. Backman, J. Hong, M. Komppula, R. Krejci, M. Laborde, J. Lampilahti, G. de Leeuw, A. Pfüller, B. Rosati, M. Tesche, P. Tunved, R. Väänänen, and T. Petäjä
Atmos. Chem. Phys., 15, 7247–7267, https://doi.org/10.5194/acp-15-7247-2015, https://doi.org/10.5194/acp-15-7247-2015, 2015
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The effect of water uptake (hygroscopicity) on aerosol light scattering properties is generally lower for boreal aerosol due to the dominance of organic substances. A columnar optical closure study using ground-based and airborne measurements of aerosol optical, chemical and microphysical properties was conducted and the implications and limitations are discussed.
R. Fröhlich, V. Crenn, A. Setyan, C. A. Belis, F. Canonaco, O. Favez, V. Riffault, J. G. Slowik, W. Aas, M. Aijälä, A. Alastuey, B. Artiñano, N. Bonnaire, C. Bozzetti, M. Bressi, C. Carbone, E. Coz, P. L. Croteau, M. J. Cubison, J. K. Esser-Gietl, D. C. Green, V. Gros, L. Heikkinen, H. Herrmann, J. T. Jayne, C. R. Lunder, M. C. Minguillón, G. Močnik, C. D. O'Dowd, J. Ovadnevaite, E. Petralia, L. Poulain, M. Priestman, A. Ripoll, R. Sarda-Estève, A. Wiedensohler, U. Baltensperger, J. Sciare, and A. S. H. Prévôt
Atmos. Meas. Tech., 8, 2555–2576, https://doi.org/10.5194/amt-8-2555-2015, https://doi.org/10.5194/amt-8-2555-2015, 2015
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Source apportionment (SA) of organic aerosol mass spectrometric data measured with the Aerodyne ACSM using PMF/ME2 is a frequently used technique in the AMS/ACSM community. ME2 uncertainties due to instrument-to-instrument variations are elucidated by performing SA on ambient data from 14 individual, co-located ACSMs, recorded during the first ACTRIS ACSM intercomparison study at SIRTA near Paris (France). The mean uncertainty was 17.2%. Recommendations for future studies using ME2 are provided.
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
A. T. Lambe, P. S. Chhabra, T. B. Onasch, W. H. Brune, J. F. Hunter, J. H. Kroll, M. J. Cummings, J. F. Brogan, Y. Parmar, D. R. Worsnop, C. E. Kolb, and P. Davidovits
Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, https://doi.org/10.5194/acp-15-3063-2015, 2015
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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
S. Xiao, M. Y. Wang, L. Yao, M. Kulmala, B. Zhou, X. Yang, J. M. Chen, D. F. Wang, Q. Y. Fu, D. R. Worsnop, and L. Wang
Atmos. Chem. Phys., 15, 1769–1781, https://doi.org/10.5194/acp-15-1769-2015, https://doi.org/10.5194/acp-15-1769-2015, 2015
Y.-L. Zhang, R.-J. Huang, I. El Haddad, K.-F. Ho, J.-J. Cao, Y. Han, P. Zotter, C. Bozzetti, K. R. Daellenbach, F. Canonaco, J. G. Slowik, G. Salazar, M. Schwikowski, J. Schnelle-Kreis, G. Abbaszade, R. Zimmermann, U. Baltensperger, A. S. H. Prévôt, and S. Szidat
Atmos. Chem. Phys., 15, 1299–1312, https://doi.org/10.5194/acp-15-1299-2015, https://doi.org/10.5194/acp-15-1299-2015, 2015
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Source apportionment of fine carbonaceous aerosols using radiocarbon and other organic markers measurements during 2013 winter haze episodes was conducted at four megacities in China. Our results demonstrate that fossil emissions predominate EC with a mean contribution of 75±8%, whereas non-fossil sources account for 55±10% of OC; and the increment of TC on heavily polluted days was mainly driven by the increase of secondary OC from both fossil-fuel and non-fossil emissions.
I. Nuaaman, S.-M. Li, K. L. Hayden, T. B. Onasch, P. Massoli, D. Sueper, D. R. Worsnop, T. S. Bates, P. K. Quinn, and R. McLaren
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-2085-2015, https://doi.org/10.5194/acpd-15-2085-2015, 2015
Revised manuscript has not been submitted
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In this paper, we focus on the measurement and reporting of mass concentrations of particulate chloride and sea salt in a marine area off the coast of California using a High Resolution Aerosol Mass Spectrometer. We outline a method of deconvolving the total aerosol chloride mass into refractory and non-refractory components, previously not reported in the literature. This can be important in regions where refractory sea salt aerosols can contribute to the aerosol chloride signal measured with t
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
S. Schobesberger, A. Franchin, F. Bianchi, L. Rondo, J. Duplissy, A. Kürten, I. K. Ortega, A. Metzger, R. Schnitzhofer, J. Almeida, A. Amorim, J. Dommen, E. M. Dunne, M. Ehn, S. Gagné, L. Ickes, H. Junninen, A. Hansel, V.-M. Kerminen, J. Kirkby, A. Kupc, A. Laaksonen, K. Lehtipalo, S. Mathot, A. Onnela, T. Petäjä, F. Riccobono, F. D. Santos, M. Sipilä, A. Tomé, G. Tsagkogeorgas, Y. Viisanen, P. E. Wagner, D. Wimmer, J. Curtius, N. M. Donahue, U. Baltensperger, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 55–78, https://doi.org/10.5194/acp-15-55-2015, https://doi.org/10.5194/acp-15-55-2015, 2015
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We used an ion mass spectrometer at CERN's CLOUD chamber to investigate the detailed composition of ammonia--sulfuric acid ion clusters (of both polarities) as they initially form and then grow into aerosol particles, at atmospherically relevant conditions. We found that these clusters’ composition is mainly determined by the ratio of the precursor vapors and ranges from ammonia-free clusters to clusters containing > 1 ammonia per sulfuric acid. Acid--base bindings are a key formation mechanism.
P. S. Chhabra, A. T. Lambe, M. R. Canagaratna, H. Stark, J. T. Jayne, T. B. Onasch, P. Davidovits, J. R. Kimmel, and D. R. Worsnop
Atmos. Meas. Tech., 8, 1–18, https://doi.org/10.5194/amt-8-1-2015, https://doi.org/10.5194/amt-8-1-2015, 2015
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Authors of this publication used acetate chemical ionization mass spectrometry (acetate-CIMS) to measure experimental products of alpha-pinene and naphthalene oxidation formed in a flow reactor. Acetate-CIMS instrumentation is selective toward carboxylic acid compounds which are readily formed in atmospheric photooxidation processes. Spectral information was used to identify previously measured products of both systems and to estimate their volatilities.
J.-E. Petit, O. Favez, J. Sciare, F. Canonaco, P. Croteau, G. Močnik, J. Jayne, D. Worsnop, and E. Leoz-Garziandia
Atmos. Chem. Phys., 14, 13773–13787, https://doi.org/10.5194/acp-14-13773-2014, https://doi.org/10.5194/acp-14-13773-2014, 2014
P. Zotter, V. G. Ciobanu, Y. L. Zhang, I. El-Haddad, M. Macchia, K. R. Daellenbach, G. A. Salazar, R.-J. Huang, L. Wacker, C. Hueglin, A. Piazzalunga, P. Fermo, M. Schwikowski, U. Baltensperger, S. Szidat, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 13551–13570, https://doi.org/10.5194/acp-14-13551-2014, https://doi.org/10.5194/acp-14-13551-2014, 2014
L. Q. Hao, A. Kortelainen, S. Romakkaniemi, H. Portin, A. Jaatinen, A. Leskinen, M. Komppula, P. Miettinen, D. Sueper, A. Pajunoja, J. N. Smith, K. E. J. Lehtinen, D. R. Worsnop, A. Laaksonen, and A. Virtanen
Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, https://doi.org/10.5194/acp-14-13483-2014, 2014
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Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions from the measurement in a mixed region between the boreal forestland and the urban area. The PMF analysis succeeded in separating the mixed spectra into three distinct organic factors and one inorganic factor. The particulate organic nitrate was distinguished by PMF for the first time, with a contribution of one-third of the total nitrate mass.
M. D. Willis, A. K. Y. Lee, T. B. Onasch, E. C. Fortner, L. R. Williams, A. T. Lambe, D. R. Worsnop, and J. P. D. Abbatt
Atmos. Meas. Tech., 7, 4507–4516, https://doi.org/10.5194/amt-7-4507-2014, https://doi.org/10.5194/amt-7-4507-2014, 2014
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
L. Rondo, A. Kürten, S. Ehrhart, S. Schobesberger, A. Franchin, H. Junninen, T. Petäjä, M. Sipilä, D. R. Worsnop, and J. Curtius
Atmos. Meas. Tech., 7, 3849–3859, https://doi.org/10.5194/amt-7-3849-2014, https://doi.org/10.5194/amt-7-3849-2014, 2014
S. Decesari, J. Allan, C. Plass-Duelmer, B. J. Williams, M. Paglione, M. C. Facchini, C. O'Dowd, R. M. Harrison, J. K. Gietl, H. Coe, L. Giulianelli, G. P. Gobbi, C. Lanconelli, C. Carbone, D. Worsnop, A. T. Lambe, A. T. Ahern, F. Moretti, E. Tagliavini, T. Elste, S. Gilge, Y. Zhang, and M. Dall'Osto
Atmos. Chem. Phys., 14, 12109–12132, https://doi.org/10.5194/acp-14-12109-2014, https://doi.org/10.5194/acp-14-12109-2014, 2014
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We made use of multiple spectrometric techniques for characterizing the aerosol chemical composition and mixing in the Po Valley in the summer.
The oxygenated organic aerosol (OOA) concentrations were correlated with simple tracers for recirculated planetary boundary layer air.
A full internal mixing between black carbon (BC) and the non-refractory aerosol components was never observed. Local sources in the Po Valley were responsible for the production of organic particles unmixed with BC.
T. R. Dallmann, T. B. Onasch, T. W. Kirchstetter, D. R. Worton, E. C. Fortner, S. C. Herndon, E. C. Wood, J. P. Franklin, D. R. Worsnop, A. H. Goldstein, and R. A. Harley
Atmos. Chem. Phys., 14, 7585–7599, https://doi.org/10.5194/acp-14-7585-2014, https://doi.org/10.5194/acp-14-7585-2014, 2014
S. Saarikoski, S. Carbone, M. J. Cubison, R. Hillamo, P. Keronen, C. Sioutas, D. R. Worsnop, and J. L. Jimenez
Atmos. Meas. Tech., 7, 2121–2135, https://doi.org/10.5194/amt-7-2121-2014, https://doi.org/10.5194/amt-7-2121-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, and Q. Zhang
Atmos. Chem. Phys., 14, 6477–6494, https://doi.org/10.5194/acp-14-6477-2014, https://doi.org/10.5194/acp-14-6477-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
M. Paglione, S. Saarikoski, S. Carbone, R. Hillamo, M. C. Facchini, E. Finessi, L. Giulianelli, C. Carbone, S. Fuzzi, F. Moretti, E. Tagliavini, E. Swietlicki, K. Eriksson Stenström, A. S. H. Prévôt, P. Massoli, M. Canaragatna, D. Worsnop, and S. Decesari
Atmos. Chem. Phys., 14, 5089–5110, https://doi.org/10.5194/acp-14-5089-2014, https://doi.org/10.5194/acp-14-5089-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
P. Paatero, S. Eberly, S. G. Brown, and G. A. Norris
Atmos. Meas. Tech., 7, 781–797, https://doi.org/10.5194/amt-7-781-2014,<