Articles | Volume 21, issue 19
https://doi.org/10.5194/acp-21-14907-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-14907-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Photolytically induced changes in composition and volatility of biogenic secondary organic aerosol from nitrate radical oxidation during night-to-day transition
Cheng Wu
Department of Environmental Science, Stockholm University, Stockholm, Sweden
David M. Bell
CORRESPONDING AUTHOR
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
Emelie L. Graham
Department of Environmental Science, Stockholm University, Stockholm, Sweden
Sophie Haslett
Department of Environmental Science, Stockholm University, Stockholm, Sweden
Ilona Riipinen
Department of Environmental Science, Stockholm University, Stockholm, Sweden
Urs Baltensperger
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
Amelie Bertrand
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
Stamatios Giannoukos
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
now at: Department of Chemistry and Applied Biosciences, ETH Zurich, Zurich, Switzerland
Janne Schoonbaert
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
Imad El Haddad
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
Andre S. H. Prevot
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute,
Villigen, Switzerland
Wei Huang
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
Department of Environmental Science, Stockholm University, Stockholm, Sweden
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Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-15, https://doi.org/10.5194/ar-2024-15, 2024
Revised manuscript accepted for AR
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This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto-La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
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By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Arto Heitto, Cheng Wu, Diego Aliaga, Luis Blacutt, Xuemeng Chen, Yvette Gramlich, Liine Heikkinen, Wei Huang, Radovan Krejci, Paolo Laj, Isabel Moreno, Karine Sellegri, Fernando Velarde, Kay Weinhold, Alfred Wiedensohler, Qiaozhi Zha, Federico Bianchi, Marcos Andrade, Kari E. J. Lehtinen, Claudia Mohr, and Taina Yli-Juuti
Atmos. Chem. Phys., 24, 1315–1328, https://doi.org/10.5194/acp-24-1315-2024, https://doi.org/10.5194/acp-24-1315-2024, 2024
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Particle growth at the Chacaltaya station in Bolivia was simulated based on measured vapor concentrations and ambient conditions. Major contributors to the simulated growth were low-volatility organic compounds (LVOCs). Also, sulfuric acid had major role when volcanic activity was occurring in the area. This study provides insight on nanoparticle growth at this high-altitude Southern Hemispheric site and hence contributes to building knowledge of early growth of atmospheric particles.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
Atmos. Chem. Phys., 23, 7347–7362, https://doi.org/10.5194/acp-23-7347-2023, https://doi.org/10.5194/acp-23-7347-2023, 2023
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The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate-initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system, and our simulations produced variable results with different parameterizations which warrant a re-evaluation of the treatment of the nitrate functional group.
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.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
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We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
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.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
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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Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Fredrik Mattsson, Almuth Neuberger, Liine Heikkinen, Yvette Gramlich, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Paul Zieger, Ilona Riipinen, and Claudia Mohr
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Imad El Haddad, Danielle Vienneau, Kaspar R. Daellenbach, Robin Modini, Jay G. Slowik, Abhishek Upadhyay, Petros N. Vasilakos, David Bell, Kees de Hoogh, and Andre S. H. Prevot
Atmos. Chem. Phys., 24, 11981–12011, https://doi.org/10.5194/acp-24-11981-2024, https://doi.org/10.5194/acp-24-11981-2024, 2024
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This opinion paper explores how advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution. We advocate for a shift in the way we target PM pollution, focusing on the most harmful anthropogenic emissions. We highlight key observations, modelling developments, and emission measurements needed to achieve this shift.
Valeria Mardoñez-Balderrama, Griša Močnik, Marco Pandolfi, Robin L. Modini, Fernando Velarde, Laura Renzi, Angela Marinoni, Jean-Luc Jaffrezo, Isabel Moreno R., Diego Aliaga, Federico Bianchi, Claudia Mohr, Martin Gysel-Beer, Patrick Ginot, Radovan Krejci, Alfred Wiedensohler, Gaëlle Uzu, Marcos Andrade, and Paolo Laj
Atmos. Chem. Phys., 24, 12055–12077, https://doi.org/10.5194/acp-24-12055-2024, https://doi.org/10.5194/acp-24-12055-2024, 2024
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Levels of black carbon (BC) are scarcely reported in the Southern Hemisphere, especially in high-altitude conditions. This study provides insight into the concentration level, variability, and optical properties of BC in La Paz and El Alto and at the Chacaltaya Global Atmosphere Watch Station. Two methods of source apportionment of absorption were tested and compared showing traffic as the main contributor to absorption in the urban area, in addition to biomass and open waste burning.
Anderson Da Silva, Louis Marelle, Jean-Christophe Raut, Yvette Gramlich, Karolina Siegel, Sophie L. Haslett, Claudia Mohr, and Jennie L. Thomas
EGUsphere, https://doi.org/10.5194/egusphere-2024-2839, https://doi.org/10.5194/egusphere-2024-2839, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Particles sources in polar climates are unclear, affecting climate representation in models. This study introduces an evaluated method for tracking particles with backtrajectory modeling. Tests on simulated particles allowed to show that traditional detection methods often misidentify sources. An improved method that accurately traces origins of aerosol particles in the Arctic is presented. The study recommends using this enhanced method for better source identification of atmospheric species.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Hengheng Zhang, Wei Huang, Xiaoli Shen, Ramakrishna Ramisetty, Junwei Song, Olga Kiseleva, Christopher Claus Holst, Basit Khan, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 10617–10637, https://doi.org/10.5194/acp-24-10617-2024, https://doi.org/10.5194/acp-24-10617-2024, 2024
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Our study unravels how stagnant winter conditions elevate aerosol levels in Stuttgart. Cloud cover at night plays a pivotal role, impacting morning air quality. Validating a key model, our findings aid accurate air quality predictions, crucial for effective pollution mitigation in urban areas.
Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurelien Chauvigné, Sebastien Conil, Marco Pandolfi, and Oriol Jorba
EGUsphere, https://doi.org/10.5194/egusphere-2024-2086, https://doi.org/10.5194/egusphere-2024-2086, 2024
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Brown carbon (BrC) absorbs UV and visible light, affecting climate. Our study investigates BrC's imaginary refractive index (k ) using data from 12 European sites. Residential emissions are a major OA source in winter, while secondary organic aerosols (SOA) dominate in summer. We derived source-specific k values, enhancing model accuracy. This research improves understanding of BrC's climate role, emphasizing the need for source-specific constraints in atmospheric models.
Ashutosh Kumar Shukla, Sachchida Nand Tripathi, Shamitaksha Talukdar, Vishnu Murari, Sreenivas Gaddamidi, Manousos-Ioannis Manousakas, Vipul Lalchandani, Kuldeep Dixit, Vinayak M Ruge, Peeyush Khare, Mayank Kumar, Vikram Singh, Neeraj Rastogi, Suresh Tiwari, Atul K. Srivastava, Dilip Ganguly, Kaspar Rudolf Daellenbach, and Andre Stephan Henry Prevot
EGUsphere, https://doi.org/10.5194/egusphere-2024-1385, https://doi.org/10.5194/egusphere-2024-1385, 2024
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Our study delves into the elemental composition of aerosols across the Indo-Gangetic Plain (IGP), revealing distinct patterns during pollution episodes. We found significant increases in Cl-rich and SFC1 sources, indicating dynamic emissions and agricultural burning impacts. Surges in Cl-rich particles during cold periods highlight their role in particle growth under specific conditions.
Delaney B. Kilgour, Christopher M. Jernigan, Olga Garmash, Sneha Aggarwal, Claudia Mohr, Matt E. Salter, Joel A. Thornton, Jian Wang, Paul Zieger, and Timothy H. Bertram
EGUsphere, https://doi.org/10.5194/egusphere-2024-1975, https://doi.org/10.5194/egusphere-2024-1975, 2024
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We report simultaneous measurements of dimethyl sulfide (DMS) and hydroperoxymethyl thioformate (HPMTF) in the Eastern North Atlantic. We use an observationally constrained box model to show cloud loss is the dominant sink of HPMTF in this region over six weeks, resulting in large reductions in DMS-derived products that contribute to aerosol formation and growth. Our findings indicate that fast cloud processing of HPMTF must be included in global models to accurately capture the sulfur cycle.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiaa Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
EGUsphere, https://doi.org/10.5194/egusphere-2024-1912, https://doi.org/10.5194/egusphere-2024-1912, 2024
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Limited aerosol measurements in the central Arctic hinder our understanding of aerosol-climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Locally wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-15, https://doi.org/10.5194/ar-2024-15, 2024
Revised manuscript accepted for AR
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This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto-La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Tiantian Wang, Jun Zhang, Houssni Lamkaddam, Kun Li, Ka Yuen Cheung, Lisa Kattner, Erlend Gammelsæter, Michael Bauer, Zachary C. J. Decker, Deepika Bhattu, Rujin Huang, Rob L. Modini, Jay G. Slowik, Imad El Haddad, Andre S. H. Prevot, and David M. Bell
EGUsphere, https://doi.org/10.5194/egusphere-2024-1161, https://doi.org/10.5194/egusphere-2024-1161, 2024
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Our study analyzes real-time emissions of primary organic gases from solid fuel combustion, including residential and open burning. Using Vocus-PTR-TOF, we tested various fuels, finding higher emissions from wood burning. Statistical tests identified unique characteristic compounds. IVOCs are key precursors to SOA formation, particularly in open burning. Our insights benefit air quality, climate, and health, advancing atmospheric chemistry and aiding accurate emission assessments.
Liine Heikkinen, Daniel G. Partridge, Sara Blichner, Wei Huang, Rahul Ranjan, Paul Bowen, Emanuele Tovazzi, Tuukka Petäjä, Claudia Mohr, and Ilona Riipinen
Atmos. Chem. Phys., 24, 5117–5147, https://doi.org/10.5194/acp-24-5117-2024, https://doi.org/10.5194/acp-24-5117-2024, 2024
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The organic vapor condensation with water vapor (co-condensation) in rising air below clouds is modeled in this work over the boreal forest because the forest air is rich in organic vapors. We show that the number of cloud droplets can increase by 20 % if considering co-condensation. The enhancements are even larger if the air contains many small, naturally produced aerosol particles. Such conditions are most frequently met in spring in the boreal forest.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
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By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Dominic Heslin-Rees, Peter Tunved, Johan Ström, Roxana Cremer, Paul Zieger, Ilona Riipinen, Annica M. L. Ekman, Konstantinos Eleftheriadis, and Radovan Krejci
Atmos. Chem. Phys., 24, 2059–2075, https://doi.org/10.5194/acp-24-2059-2024, https://doi.org/10.5194/acp-24-2059-2024, 2024
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Light-absorbing atmospheric particles (e.g. black carbon – BC) exert a warming effect on the Arctic climate. We show that the amount of particle light absorption decreased from 2002 to 2023. We conclude that in addition to reductions in emissions of BC, wet removal plays a role in the long-term reduction of BC in the Arctic, given the increase in surface precipitation experienced by air masses arriving at the site. The potential impact of biomass burning events is shown to have increased.
Arto Heitto, Cheng Wu, Diego Aliaga, Luis Blacutt, Xuemeng Chen, Yvette Gramlich, Liine Heikkinen, Wei Huang, Radovan Krejci, Paolo Laj, Isabel Moreno, Karine Sellegri, Fernando Velarde, Kay Weinhold, Alfred Wiedensohler, Qiaozhi Zha, Federico Bianchi, Marcos Andrade, Kari E. J. Lehtinen, Claudia Mohr, and Taina Yli-Juuti
Atmos. Chem. Phys., 24, 1315–1328, https://doi.org/10.5194/acp-24-1315-2024, https://doi.org/10.5194/acp-24-1315-2024, 2024
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Particle growth at the Chacaltaya station in Bolivia was simulated based on measured vapor concentrations and ambient conditions. Major contributors to the simulated growth were low-volatility organic compounds (LVOCs). Also, sulfuric acid had major role when volcanic activity was occurring in the area. This study provides insight on nanoparticle growth at this high-altitude Southern Hemispheric site and hence contributes to building knowledge of early growth of atmospheric particles.
Markku Kulmala, Anna Lintunen, Hanna Lappalainen, Annele Virtanen, Chao Yan, Ekaterina Ezhova, Tuomo Nieminen, Ilona Riipinen, Risto Makkonen, Johanna Tamminen, Anu-Maija Sundström, Antti Arola, Armin Hansel, Kari Lehtinen, Timo Vesala, Tuukka Petäjä, Jaana Bäck, Tom Kokkonen, and Veli-Matti Kerminen
Atmos. Chem. Phys., 23, 14949–14971, https://doi.org/10.5194/acp-23-14949-2023, https://doi.org/10.5194/acp-23-14949-2023, 2023
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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.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Yong Zhang, Jie Tian, Qiyuan Wang, Lu Qi, Manousos Ioannis Manousakas, Yuemei Han, Weikang Ran, Yele Sun, Huikun Liu, Renjian Zhang, Yunfei Wu, Tianqu Cui, Kaspar Rudolf Daellenbach, Jay Gates Slowik, André S. H. Prévôt, and Junji Cao
Atmos. Chem. Phys., 23, 9455–9471, https://doi.org/10.5194/acp-23-9455-2023, https://doi.org/10.5194/acp-23-9455-2023, 2023
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PM2.5 pollution still frequently occurs in northern China during winter, and it is necessary to figure out the causes of air pollution based on intensive real-time measurement. The findings elaborate the chemical characteristics and source contributions of PM2.5 in three pilot cities, reveal potential formation mechanisms of secondary aerosols, and highlight the importance of controlling biomass burning and inhibiting generation of secondary aerosol for air quality improvement.
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.
Karolina Siegel, Yvette Gramlich, Sophie L. Haslett, Gabriel Freitas, Radovan Krejci, Paul Zieger, and Claudia Mohr
Atmos. Chem. Phys., 23, 7569–7587, https://doi.org/10.5194/acp-23-7569-2023, https://doi.org/10.5194/acp-23-7569-2023, 2023
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Hydroperoxymethyl thioformate (HPMTF) is a recently discovered oxidation product of dimethyl sulfide (DMS). We present a full year of concurrent gas- and particle-phase observations of HPMTF and other DMS oxidation products from the Arctic. We did not observe significant amounts of HPMTF in the particle phase but a good agreement between gas-phase HMPTF and methanesulfonic acid in the summer. Our study provides information about the relationship between HPMTF and other DMS oxidation products.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
Atmos. Chem. Phys., 23, 7347–7362, https://doi.org/10.5194/acp-23-7347-2023, https://doi.org/10.5194/acp-23-7347-2023, 2023
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The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate-initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system, and our simulations produced variable results with different parameterizations which warrant a re-evaluation of the treatment of the nitrate functional group.
Samira Atabakhsh, Laurent Poulain, Gang Chen, Francesco Canonaco, André S. H. Prévôt, Mira Pöhlker, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6963–6988, https://doi.org/10.5194/acp-23-6963-2023, https://doi.org/10.5194/acp-23-6963-2023, 2023
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The study focuses on the aerosol chemical variations found in the rural-background station of Melpitz based on ACSM and MAAP measurements. Source apportionment on both organic aerosol (OA) and black carbon (eBC) was performed, and source seasonality was also linked to air mass trajectories. Overall, three anthropogenic sources were identified in OA and eBC plus two additional aged OA. Our results demonstrate the influence of transported coal-combustion-related OA even during summer time.
Joschka Pfeifer, Naser G. A. Mahfouz, Benjamin C. Schulze, Serge Mathot, Dominik Stolzenburg, Rima Baalbaki, Zoé Brasseur, Lucia Caudillo, Lubna Dada, Manuel Granzin, Xu-Cheng He, Houssni Lamkaddam, Brandon Lopez, Vladimir Makhmutov, Ruby Marten, Bernhard Mentler, Tatjana Müller, Antti Onnela, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Meredith Schervish, Ping Tian, Nsikanabasi S. Umo, Dongyu S. Wang, Mingyi Wang, Stefan K. Weber, André Welti, Yusheng Wu, Marcel Zauner-Wieczorek, Antonio Amorim, Imad El Haddad, Markku Kulmala, Katrianne Lehtipalo, Tuukka Petäjä, António Tomé, Sander Mirme, Hanna E. Manninen, Neil M. Donahue, Richard C. Flagan, Andreas Kürten, Joachim Curtius, and Jasper Kirkby
Atmos. Chem. Phys., 23, 6703–6718, https://doi.org/10.5194/acp-23-6703-2023, https://doi.org/10.5194/acp-23-6703-2023, 2023
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Attachment rate coefficients between ions and charged aerosol particles determine their lifetimes and may also influence cloud dynamics and aerosol processing. Here we present novel experiments that measure ion–aerosol attachment rate coefficients for multiply charged aerosol particles under atmospheric conditions in the CERN CLOUD chamber. Our results provide experimental discrimination between various theoretical models.
Yvette Gramlich, Karolina Siegel, Sophie L. Haslett, Gabriel Freitas, Radovan Krejci, Paul Zieger, and Claudia Mohr
Atmos. Chem. Phys., 23, 6813–6834, https://doi.org/10.5194/acp-23-6813-2023, https://doi.org/10.5194/acp-23-6813-2023, 2023
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In this study, we investigate the chemical composition of aerosol particles forming clouds in the Arctic. During year-long observations at a mountain site on Svalbard, we find a large contribution of naturally derived aerosol particles in the fraction forming clouds in the summer. Our observations indicate that most aerosol particles can serve as cloud seeds in this remote environment.
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.
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.
Vaishali Jain, Nidhi Tripathi, Sachchida N. Tripathi, Mansi Gupta, Lokesh K. Sahu, Vishnu Murari, Sreenivas Gaddamidi, Ashutosh K. Shukla, and Andre S. H. Prevot
Atmos. Chem. Phys., 23, 3383–3408, https://doi.org/10.5194/acp-23-3383-2023, https://doi.org/10.5194/acp-23-3383-2023, 2023
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This research chemically characterises 173 different NMVOCs (non-methane volatile organic compounds) measured in real time for three seasons in the city of the central Indo-Gangetic basin of India, Lucknow. Receptor modelling is used to analyse probable sources of NMVOCs and their crucial role in forming ozone and secondary organic aerosols. It is observed that vehicular emissions and solid fuel combustion are the highest contributors to the emission of primary and secondary NMVOCs.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
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We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
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We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
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.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech., 15, 7265–7291, https://doi.org/10.5194/amt-15-7265-2022, https://doi.org/10.5194/amt-15-7265-2022, 2022
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Jerome D. Fast, David M. Bell, Gourihar Kulkarni, Jiumeng Liu, Fan Mei, Georges Saliba, John E. Shilling, Kaitlyn Suski, Jason Tomlinson, Jian Wang, Rahul Zaveri, and Alla Zelenyuk
Atmos. Chem. Phys., 22, 11217–11238, https://doi.org/10.5194/acp-22-11217-2022, https://doi.org/10.5194/acp-22-11217-2022, 2022
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Recent aircraft measurements from the HI-SCALE campaign conducted over the Southern Great Plains (SGP) site in Oklahoma are used to quantify spatial variability of aerosol properties in terms of grid spacings typically used by weather and climate models. Surprisingly large horizontal gradients in aerosol properties were frequently observed in this rural area. This spatial variability can be used as an uncertainty range when comparing surface point measurements with model predictions.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
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We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
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.
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.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
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The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
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.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Leah R. Williams, Matteo Rinaldi, Jonathan T. Trueblood, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilkka Timonen, and Cécile Guieu
Atmos. Chem. Phys., 21, 10625–10641, https://doi.org/10.5194/acp-21-10625-2021, https://doi.org/10.5194/acp-21-10625-2021, 2021
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSAs) continuously generated along a 5-week cruise in the Mediterranean. This information is combined with seawater biogeochemical properties also measured continuously along the ship track to develop a number of parametrizations that can be used in models to determine SSA organic content in oligotrophic waters that represent 60 % of the oceans from commonly measured seawater variables.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
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.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Ines Bulatovic, Adele L. Igel, Caroline Leck, Jost Heintzenberg, Ilona Riipinen, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 3871–3897, https://doi.org/10.5194/acp-21-3871-2021, https://doi.org/10.5194/acp-21-3871-2021, 2021
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We use detailed numerical modelling to show that small aerosol particles (diameters ~25–80 nm; so-called Aitken mode particles) significantly influence low-level cloud properties in the clean summertime high Arctic. The small particles can help sustain clouds when the concentration of larger particles is low (<10–20 cm-3). Measurements from four different observational campaigns in the high Arctic support the modelling results as they indicate that Aitken mode aerosols are frequently activated.
Rosaria E. Pileci, Robin L. Modini, Michele Bertò, Jinfeng Yuan, Joel C. Corbin, Angela Marinoni, Bas Henzing, Marcel M. Moerman, Jean P. Putaud, Gerald Spindler, Birgit Wehner, Thomas Müller, Thomas Tuch, Arianna Trentini, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Meas. Tech., 14, 1379–1403, https://doi.org/10.5194/amt-14-1379-2021, https://doi.org/10.5194/amt-14-1379-2021, 2021
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Black carbon (BC), which is an important constituent of atmospheric aerosols, remains difficult to quantify due to various limitations of available methods. This study provides an extensive comparison of co-located field measurements, applying two methods based on different principles. It was shown that both methods indeed quantify the same aerosol property – BC mass concentration. The level of agreement that can be expected was quantified, and some reasons for discrepancy were identified.
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.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Jinfeng Yuan, Robin Lewis Modini, Marco Zanatta, Andreas B. Herber, Thomas Müller, Birgit Wehner, Laurent Poulain, Thomas Tuch, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 21, 635–655, https://doi.org/10.5194/acp-21-635-2021, https://doi.org/10.5194/acp-21-635-2021, 2021
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Black carbon (BC) aerosols contribute substantially to climate warming due to their unique light absorption capabilities. We performed field measurements at a central European background site in winter and found that variability in the absorption efficiency of BC particles is driven mainly by their internal mixing state. Our results suggest that, at this site, knowing the BC mixing state is sufficient to describe BC light absorption enhancements due to the lensing effect in good approximation.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
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.
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.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Liwei Wang, Jay G. Slowik, Nidhi Tripathi, Deepika Bhattu, Pragati Rai, Varun Kumar, Pawan Vats, Rangu Satish, Urs Baltensperger, Dilip Ganguly, Neeraj Rastogi, Lokesh K. Sahu, Sachchida N. Tripathi, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 9753–9770, https://doi.org/10.5194/acp-20-9753-2020, https://doi.org/10.5194/acp-20-9753-2020, 2020
Martin Rigler, Luka Drinovec, Gašper Lavrič, Athanasia Vlachou, André S. H. Prévôt, Jean Luc Jaffrezo, Iasonas Stavroulas, Jean Sciare, Judita Burger, Irena Kranjc, Janja Turšič, Anthony D. A. Hansen, and Griša Močnik
Atmos. Meas. Tech., 13, 4333–4351, https://doi.org/10.5194/amt-13-4333-2020, https://doi.org/10.5194/amt-13-4333-2020, 2020
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Carbonaceous aerosols are a large fraction of fine particulate matter. They are extremely diverse, and they directly impact air quality, visibility, cloud formation and public health. In this paper we present a new instrument and new method to measure carbon content in particulate matter in real time and at a high time resolution. The new method was validated in a 1-month winter field campaign in Ljubljana, Slovenia.
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
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.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
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.
Pragati Rai, Markus Furger, Jay G. Slowik, Francesco Canonaco, Roman Fröhlich, Christoph Hüglin, María Cruz Minguillón, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 1657–1674, https://doi.org/10.5194/acp-20-1657-2020, https://doi.org/10.5194/acp-20-1657-2020, 2020
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A source apportionment study of hourly resolved elements in PM10 measured at a traffic-influenced site in Härkingen, Switzerland, using positive matrix factorization (PMF) and multilinear engine-2 (ME-2) offered resolution of robust and unambiguous factor profiles and contributions. We show that the rotational control available in ME-2 provides a means for treating extreme events such as fireworks within a PMF analysis.
Marco Paglione, Stefania Gilardoni, Matteo Rinaldi, Stefano Decesari, Nicola Zanca, Silvia Sandrini, Lara Giulianelli, Dimitri Bacco, Silvia Ferrari, Vanes Poluzzi, Fabiana Scotto, Arianna Trentini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Francesco Canonaco, André S. H. Prévôt, Paola Massoli, Claudio Carbone, Maria Cristina Facchini, and Sandro Fuzzi
Atmos. Chem. Phys., 20, 1233–1254, https://doi.org/10.5194/acp-20-1233-2020, https://doi.org/10.5194/acp-20-1233-2020, 2020
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Our multi-year observational study regarding organic aerosol (OA) in the Po Valley indicates that more than half of OA is of secondary origin (SOA) through all the year and at both urban and rural sites. Within the SOA, the measurements show the importance of biomass burning (BB) aging products during cold seasons and indicate aqueous-phase processing of BB emissions as a fundamental driver of SOA formation in wintertime, with important consequences for air quality policy at the global level.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Jianhui Jiang, Sebnem Aksoyoglu, Imad El-Haddad, Giancarlo Ciarelli, Hugo A. C. Denier van der Gon, Francesco Canonaco, Stefania Gilardoni, Marco Paglione, María Cruz Minguillón, Olivier Favez, Yunjiang Zhang, Nicolas Marchand, Liqing Hao, Annele Virtanen, Kalliopi Florou, Colin O'Dowd, Jurgita Ovadnevaite, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, https://doi.org/10.5194/acp-19-15247-2019, 2019
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We use an air quality model with a modified organic aerosol (OA) module based on chamber experiments to identify the OA sources and their contributions in Europe. Comparisons with long-term measurements at nine sites in 2011 show an improvement in OA simulation. Our results suggest that the biomass burning and biogenic emissions are the dominant sources in winter and summer, respectively. Contributions of diesel and gasoline vehicles are relatively small compared to a previous study in the US.
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
Yunjiang Zhang, Olivier Favez, Jean-Eudes Petit, Francesco Canonaco, Francois Truong, Nicolas Bonnaire, Vincent Crenn, Tanguy Amodeo, Andre S. H. Prévôt, Jean Sciare, Valerie Gros, and Alexandre Albinet
Atmos. Chem. Phys., 19, 14755–14776, https://doi.org/10.5194/acp-19-14755-2019, https://doi.org/10.5194/acp-19-14755-2019, 2019
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We present 6-year source apportionment of organic aerosol (OA) achieved with near-continuous online measurements and subsequent receptor model analysis in the Paris region, France. The OA factors presented distinct seasonal patterns, associated with different atmospheric formation processes and roles in air pollution. Limited year-round trends for two primary anthropogenic factors and a biogenic-like secondary factor were observed, while a more oxidized secondary OA showed a decreasing feature.
Jun Zhou, Miriam Elser, Ru-Jin Huang, Manuel Krapf, Roman Fröhlich, Deepika Bhattu, Giulia Stefenelli, Peter Zotter, Emily A. Bruns, Simone M. Pieber, Haiyan Ni, Qiyuan Wang, Yichen Wang, Yaqing Zhou, Chunying Chen, Mao Xiao, Jay G. Slowik, Samuel Brown, Laure-Estelle Cassagnes, Kaspar R. Daellenbach, Thomas Nussbaumer, Marianne Geiser, André S. H. Prévôt, Imad El-Haddad, Junji Cao, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 19, 14703–14720, https://doi.org/10.5194/acp-19-14703-2019, https://doi.org/10.5194/acp-19-14703-2019, 2019
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Reactive oxygen species (ROS) are believed to contribute to the adverse health effects of aerosols. We measured particle-bound ROS (PB-ROS) with an online instrument in two distinct environments, i.e., Beijing (China) and Bern (Switzerland). In both cities these exogenic ROS are predominantly related to secondary organic aerosol (SOA). PB-ROS content in SOA from various anthropogenic emission sources tested in the laboratory was comparable to that in the ambient measurements.
Xiaoli Shen, Heike Vogel, Bernhard Vogel, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, Thomas Leisner, André S. H. Prévôt, and Harald Saathoff
Atmos. Chem. Phys., 19, 13189–13208, https://doi.org/10.5194/acp-19-13189-2019, https://doi.org/10.5194/acp-19-13189-2019, 2019
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This study provides good insight into the chemical nature and complex origin of aerosols by combining comprehensive field observations and transport modelling. We suggest that factors related to topography, metrological conditions, local emissions, in situ formation and growth, regional transport, and the interaction of biogenic and anthropogenic compounds need to be considered for a comprehensive understanding of aerosol processes.
Wei Huang, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 19, 11687–11700, https://doi.org/10.5194/acp-19-11687-2019, https://doi.org/10.5194/acp-19-11687-2019, 2019
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We investigate the molecular composition and volatility of oxygenated organic aerosol (OOA) particles in summer and winter in Stuttgart, Germany. OOA in summer is more influenced by biogenic emissions, while in winter biomass burning emissions are an important source. OOA in winter is also less volatile. Potential reasons are discussed in our paper. Our study shows the important contributions of nonfossil OA from biogenic and biomass burning even in an urban area with high traffic emissions.
Giulia Stefenelli, Jianhui Jiang, Amelie Bertrand, Emily A. Bruns, Simone M. Pieber, Urs Baltensperger, Nicolas Marchand, Sebnem Aksoyoglu, André S. H. Prévôt, Jay G. Slowik, and Imad El Haddad
Atmos. Chem. Phys., 19, 11461–11484, https://doi.org/10.5194/acp-19-11461-2019, https://doi.org/10.5194/acp-19-11461-2019, 2019
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Box model simulations, based on the volatility basis set approach, of smog chamber wood combustion experiments conducted at different temperatures (−10 °C, 2 °C, 15 °C), emission loads, combustion conditions (flaming and smoldering) and residential stoves fabricated in the last 2 decades. Novel parameterization methods based on a genetic algorithm approach allowed estimation of precursor class contributions to SOA and evaluation of the effect of emission variability on SOA yield predictions.
Felipe D. Lopez-Hilfiker, Veronika Pospisilova, Wei Huang, Markus Kalberer, Claudia Mohr, Giulia Stefenelli, Joel A. Thornton, Urs Baltensperger, Andre S. H. Prevot, and Jay G. Slowik
Atmos. Meas. Tech., 12, 4867–4886, https://doi.org/10.5194/amt-12-4867-2019, https://doi.org/10.5194/amt-12-4867-2019, 2019
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We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
Meng Wang, Ru-Jin Huang, Junji Cao, Wenting Dai, Jiamao Zhou, Chunshui Lin, Haiyan Ni, Jing Duan, Ting Wang, Yang Chen, Yongjie Li, Qi Chen, Imad El Haddad, and Thorsten Hoffmann
Atmos. Meas. Tech., 12, 4779–4789, https://doi.org/10.5194/amt-12-4779-2019, https://doi.org/10.5194/amt-12-4779-2019, 2019
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The analytical performances of SE-GC-MS and TD-GC-MS for the determination of n-alkanes, PAHs and hopanes were evaluated and compared. The two methods show a good agreement with a high correlation efficient (R2 > 0.98) and a slope close to unity. The concentrations of n-alkanes, PAHs and hopanes are found to be much higher in Beijing than those in Chengdu, Shanghai and Guangzhou, most likely due to emissions from coal combustion for wintertime heating in Beijing.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Jonathan W. Taylor, Sophie L. Haslett, Keith Bower, Michael Flynn, Ian Crawford, James Dorsey, Tom Choularton, Paul J. Connolly, Valerian Hahn, Christiane Voigt, Daniel Sauer, Régis Dupuy, Joel Brito, Alfons Schwarzenboeck, Thierry Bourriane, Cyrielle Denjean, Phil Rosenberg, Cyrille Flamant, James D. Lee, Adam R. Vaughan, Peter G. Hill, Barbara Brooks, Valéry Catoire, Peter Knippertz, and Hugh Coe
Atmos. Chem. Phys., 19, 8503–8522, https://doi.org/10.5194/acp-19-8503-2019, https://doi.org/10.5194/acp-19-8503-2019, 2019
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Low-level clouds cover a wide area of southern West Africa (SWA) and play an important role in the region's climate, reflecting sunlight away from the surface. We performed aircraft measurements of aerosols and clouds over SWA during the 2016 summer monsoon and found pollution, and polluted clouds, across the whole region. Smoke from biomass burning in Central Africa is transported to West Africa, causing a polluted background which limits the effect of local pollution on cloud properties.
Lu Qi, Mindong Chen, Giulia Stefenelli, Veronika Pospisilova, Yandong Tong, Amelie Bertrand, Christoph Hueglin, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 8037–8062, https://doi.org/10.5194/acp-19-8037-2019, https://doi.org/10.5194/acp-19-8037-2019, 2019
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Current understanding of OA sources is limited by the chemical resolution of existing real-time measurement technology. We describe the first wintertime deployment of a novel extractive electrospray ionization time-of-flight mass spectrometer, which provides near-molecular OA measurements with high time resolution. We show that biomass combustion strongly influences winter OA. Via factor analysis, aging-dependent signatures and time contributions of biomass-combustion-derived OA are resolved.
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.
Naruki Hiranuma, Kouji Adachi, David M. Bell, Franco Belosi, Hassan Beydoun, Bhaskar Bhaduri, Heinz Bingemer, Carsten Budke, Hans-Christian Clemen, Franz Conen, Kimberly M. Cory, Joachim Curtius, Paul J. DeMott, Oliver Eppers, Sarah Grawe, Susan Hartmann, Nadine Hoffmann, Kristina Höhler, Evelyn Jantsch, Alexei Kiselev, Thomas Koop, Gourihar Kulkarni, Amelie Mayer, Masataka Murakami, Benjamin J. Murray, Alessia Nicosia, Markus D. Petters, Matteo Piazza, Michael Polen, Naama Reicher, Yinon Rudich, Atsushi Saito, Gianni Santachiara, Thea Schiebel, Gregg P. Schill, Johannes Schneider, Lior Segev, Emiliano Stopelli, Ryan C. Sullivan, Kaitlyn Suski, Miklós Szakáll, Takuya Tajiri, Hans Taylor, Yutaka Tobo, Romy Ullrich, Daniel Weber, Heike Wex, Thomas F. Whale, Craig L. Whiteside, Katsuya Yamashita, Alla Zelenyuk, and Ottmar Möhler
Atmos. Chem. Phys., 19, 4823–4849, https://doi.org/10.5194/acp-19-4823-2019, https://doi.org/10.5194/acp-19-4823-2019, 2019
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A total of 20 ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of cellulose particles – natural polymers. Our data showed several types of cellulose are able to nucleate ice as efficiently as some mineral dust samples and cellulose has the potential to be an important atmospheric ice-nucleating particle. Continued investigation/collaboration is necessary to obtain further insight into consistency or diversity of ice nucleation measurements.
Xiaoli Shen, Harald Saathoff, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, and Thomas Leisner
Atmos. Meas. Tech., 12, 2219–2240, https://doi.org/10.5194/amt-12-2219-2019, https://doi.org/10.5194/amt-12-2219-2019, 2019
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Based on single-particle mass spectra from field measurements in the upper Rhine valley, we identified characteristic particle classes and estimated their mass contributions without the need of a reference instrument in the field. Our study provides a good example for quantitative interpretation of single-particle data. Together with the complimentary results from bulk measurements, we have shown how a better understanding of the mixing state of ambient aerosol particles can be achieved.
Karl Espen Yttri, David Simpson, Robert Bergström, Gyula Kiss, Sönke Szidat, Darius Ceburnis, Sabine Eckhardt, Christoph Hueglin, Jacob Klenø Nøjgaard, Cinzia Perrino, Ignazio Pisso, Andre Stephan Henry Prevot, Jean-Philippe Putaud, Gerald Spindler, Milan Vana, Yan-Lin Zhang, and Wenche Aas
Atmos. Chem. Phys., 19, 4211–4233, https://doi.org/10.5194/acp-19-4211-2019, https://doi.org/10.5194/acp-19-4211-2019, 2019
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Carbonaceous aerosols from natural sources were abundant regardless of season. Residential wood burning (RWB) emissions were occasionally equally as large as or larger than of fossil-fuel sources, depending on season and region. RWB emissions are poorly constrained; thus emissions inventories need improvement. Harmonizing emission factors between countries is likely the most important step to improve model calculations for biomass burning emissions and European PM2.5 concentrations in general.
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.
Ghislain Motos, Julia Schmale, Joel C. Corbin, Rob. L. Modini, Nadine Karlen, Michele Bertò, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 3833–3855, https://doi.org/10.5194/acp-19-3833-2019, https://doi.org/10.5194/acp-19-3833-2019, 2019
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Atmospheric black carbon (BC) particles are strong light absorbers that contribute to global warming. In situ cloud measurements performed at a high-altitude site showed that cloud supersaturation mainly drives the activation of BC to cloud droplets. It was further shown how BC particle size and mixing state modulate this nucleation scavenging in agreement with simplified theoretical predictions. These findings can inform model simulations towards a better representation of the BC life cycle.
Jianhui Jiang, Sebnem Aksoyoglu, Giancarlo Ciarelli, Emmanouil Oikonomakis, Imad El-Haddad, Francesco Canonaco, Colin O'Dowd, Jurgita Ovadnevaite, María Cruz Minguillón, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 3747–3768, https://doi.org/10.5194/acp-19-3747-2019, https://doi.org/10.5194/acp-19-3747-2019, 2019
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Biogenic volatile organic compound (BVOC) emissions from vegetation are essential inputs for air quality models but their uncertainties are very high. In this study we show the importance of BVOC emissions for modelled ozone and aerosol concentrations in Europe. Using different biogenic emissions from MEGAN and PSI models significantly affected organic aerosols (smaller effect on ozone), indicating the importance of harmonising the BVOC emissions in the model inter-comparison studies.
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.
Li Xing, Jiarui Wu, Miriam Elser, Shengrui Tong, Suixin Liu, Xia Li, Lang Liu, Junji Cao, Jiamao Zhou, Imad El-Haddad, Rujin Huang, Maofa Ge, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 19, 2343–2359, https://doi.org/10.5194/acp-19-2343-2019, https://doi.org/10.5194/acp-19-2343-2019, 2019
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We used the WRF-CHEM model to simulate wintertime secondary organic aerosol (SOA) concentrations over Beijing–Tianjin–Hebei (BTH), China. Heterogeneous HONO sources increased the near-surface SOA by 46.3 % in BTH. Direct emissions of glyoxal and methylglyoxal from residential sources contributed 25.5 % to the total SOA mass. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation in winter over BTH.
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.
Ghislain Motos, Julia Schmale, Joel C. Corbin, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 2183–2207, https://doi.org/10.5194/acp-19-2183-2019, https://doi.org/10.5194/acp-19-2183-2019, 2019
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Clouds form by condensation of water vapour on aerosol particles. We showed that black carbon, a subset of particles responsible for a climate warming due to their strong light absorption and known to be insoluble in water, were able to form droplets when the humidity of the air is very slightly over 100 %. This is made possible by their acquisition of a
coatingmade of hydrophilic material during atmospheric aging. The predictability of this process using theory was successfully tested.
Michael Boy, Erik S. Thomson, Juan-C. Acosta Navarro, Olafur Arnalds, Ekaterina Batchvarova, Jaana Bäck, Frank Berninger, Merete Bilde, Zoé Brasseur, Pavla Dagsson-Waldhauserova, Dimitri Castarède, Maryam Dalirian, Gerrit de Leeuw, Monika Dragosics, Ella-Maria Duplissy, Jonathan Duplissy, Annica M. L. Ekman, Keyan Fang, Jean-Charles Gallet, Marianne Glasius, Sven-Erik Gryning, Henrik Grythe, Hans-Christen Hansson, Margareta Hansson, Elisabeth Isaksson, Trond Iversen, Ingibjorg Jonsdottir, Ville Kasurinen, Alf Kirkevåg, Atte Korhola, Radovan Krejci, Jon Egill Kristjansson, Hanna K. Lappalainen, Antti Lauri, Matti Leppäranta, Heikki Lihavainen, Risto Makkonen, Andreas Massling, Outi Meinander, E. Douglas Nilsson, Haraldur Olafsson, Jan B. C. Pettersson, Nønne L. Prisle, Ilona Riipinen, Pontus Roldin, Meri Ruppel, Matthew Salter, Maria Sand, Øyvind Seland, Heikki Seppä, Henrik Skov, Joana Soares, Andreas Stohl, Johan Ström, Jonas Svensson, Erik Swietlicki, Ksenia Tabakova, Throstur Thorsteinsson, Aki Virkkula, Gesa A. Weyhenmeyer, Yusheng Wu, Paul Zieger, and Markku Kulmala
Atmos. Chem. Phys., 19, 2015–2061, https://doi.org/10.5194/acp-19-2015-2019, https://doi.org/10.5194/acp-19-2015-2019, 2019
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The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date and aimed to strengthen research and innovation regarding climate change issues in the Nordic region. The paper presents an overview of the main scientific topics investigated and provides a state-of-the-art comprehensive summary of what has been achieved in CRAICC.
Sophie L. Haslett, Jonathan W. Taylor, Konrad Deetz, Bernhard Vogel, Karmen Babić, Norbert Kalthoff, Andreas Wieser, Cheikh Dione, Fabienne Lohou, Joel Brito, Régis Dupuy, Alfons Schwarzenboeck, Paul Zieger, and Hugh Coe
Atmos. Chem. Phys., 19, 1505–1520, https://doi.org/10.5194/acp-19-1505-2019, https://doi.org/10.5194/acp-19-1505-2019, 2019
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As the population in West Africa grows and air pollution increases, it is becoming ever more important to understand the effects of this pollution on the climate and on health. Aerosol particles can grow by absorbing water from the air around them. This paper shows that during the monsoon season, aerosol particles in the region are likely to grow significantly because of the high moisture in the air. This means that climate effects from increasing pollution will be enhanced.
Jian Wang, John E. Shilling, Jiumeng Liu, Alla Zelenyuk, David M. Bell, Markus D. Petters, Ryan Thalman, Fan Mei, Rahul A. Zaveri, and Guangjie Zheng
Atmos. Chem. Phys., 19, 941–954, https://doi.org/10.5194/acp-19-941-2019, https://doi.org/10.5194/acp-19-941-2019, 2019
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Earlier studies showed organic hygroscopicity increases with oxidation level. Such increases have been attributed to higher water solubility for more oxidized organics. By systematically varying the water content of activating droplets, we show that for secondary organic aerosols, essentially all organics are dissolved at the point of droplet activation. Therefore, the organic hygroscopicity is not limited by solubility but is dictated mainly by the molecular weight of organic species.
Nivedita K. Kumar, Joel C. Corbin, Emily A. Bruns, Dario Massabó, Jay G. Slowik, Luka Drinovec, Griša Močnik, Paolo Prati, Athanasia Vlachou, Urs Baltensperger, Martin Gysel, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 17843–17861, https://doi.org/10.5194/acp-18-17843-2018, https://doi.org/10.5194/acp-18-17843-2018, 2018
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It is clear that considerable uncertainties still exist in understanding the magnitude of aerosol absorption on a global scale and its contribution to global warming. This manuscript provides a comprehensive assessment of the optical absorption by organic aerosols (brown carbon) from residential wood combustion as a function of atmospheric aging.
Kaitlyn J. Suski, David M. Bell, Naruki Hiranuma, Ottmar Möhler, Dan Imre, and Alla Zelenyuk
Atmos. Chem. Phys., 18, 17497–17513, https://doi.org/10.5194/acp-18-17497-2018, https://doi.org/10.5194/acp-18-17497-2018, 2018
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This work investigates the cloud condensation nuclei and ice nucleation activity of bacteria using cloud chamber data and a single particle mass spectrometer. The size and chemical composition of the cloud residuals show that bacterial fragments mixed with agar growth media activate preferentially over intact bacteria cells as cloud condensation nuclei. Intact bacteria cells do not make it into cloud droplets; they thus cannot serve as immersion-mode ice nucleating particles.
Siegfried Schobesberger, Emma L. D'Ambro, Felipe D. Lopez-Hilfiker, Claudia Mohr, and Joel A. Thornton
Atmos. Chem. Phys., 18, 14757–14785, https://doi.org/10.5194/acp-18-14757-2018, https://doi.org/10.5194/acp-18-14757-2018, 2018
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Current mass spectrometers allow us to measure the composition of individual organic molecules in aerosol particles, as well as how they evaporate from the particles when those are slowly heated up to 200 °C. We have developed a detailed computer model to simulate the physical and chemical processes that underlie that evaporation and thus help us understand important aerosol properties. Among other factors, we discuss the roles of vapor pressures, and accretion and decomposition reactions.
Yingjie Zhang, Wei Du, Yuying Wang, Qingqing Wang, Haofei Wang, Haitao Zheng, Fang Zhang, Hongrong Shi, Yuxuan Bian, Yongxiang Han, Pingqing Fu, Francesco Canonaco, André S. H. Prévôt, Tong Zhu, Pucai Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 18, 14637–14651, https://doi.org/10.5194/acp-18-14637-2018, https://doi.org/10.5194/acp-18-14637-2018, 2018
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We have a comprehensive characterization of aerosol chemistry and particle growth events at a downwind site of a highly polluted city in the North China Plain. Aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. New particle growth events were also frequently observed on both clean and polluted days. While both sulfate and SOA played important roles in particle growth during clean periods, SOA was more important than sulfate during polluted events.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
Konrad Deetz, Heike Vogel, Sophie Haslett, Peter Knippertz, Hugh Coe, and Bernhard Vogel
Atmos. Chem. Phys., 18, 14271–14295, https://doi.org/10.5194/acp-18-14271-2018, https://doi.org/10.5194/acp-18-14271-2018, 2018
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Water uptake can significantly increase the size and therefore alters the optical properties of aerosols. Our model study reveals that the high moisture and aerosol burden in the southern West African monsoon
layer makes it favorable to quantify properties that determine the aerosol liquid water content and its impact on the aerosol optical depth and radiative transfer. Especially in moist tropical environments the relative humidity impact on AOD has to be considered in atmospheric models.
Marco Zanatta, Paolo Laj, Martin Gysel, Urs Baltensperger, Stergios Vratolis, Konstantinos Eleftheriadis, Yutaka Kondo, Philippe Dubuisson, Victor Winiarek, Stelios Kazadzis, Peter Tunved, and Hans-Werner Jacobi
Atmos. Chem. Phys., 18, 14037–14057, https://doi.org/10.5194/acp-18-14037-2018, https://doi.org/10.5194/acp-18-14037-2018, 2018
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The research community aims to quantify the actual contribution of soot particles to the recent Arctic warming. We discovered that mixing of soot with other components might enhance its light absorption power by 50 %. The neglection of such amplification might lead to the underestimation of radiative forcing by 0.12 W m−2. Thus a better understanding of the optical properties of soot is a crucial step for an accurate quantification of the radiative impact of soot in the Arctic atmosphere.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
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PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
Jenni Kontkanen, Tinja Olenius, Markku Kulmala, and Ilona Riipinen
Atmos. Chem. Phys., 18, 13733–13754, https://doi.org/10.5194/acp-18-13733-2018, https://doi.org/10.5194/acp-18-13733-2018, 2018
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New particle formation involving sulfuric acid, bases and organic compounds is an important source of atmospheric aerosol particles. We investigate the capability of nano-Köhler theory to describe this process by simulating the dynamics of atmospheric molecular clusters. We find that nano-Köhler-type behavior occurs in our simulations when the saturation ratio of the organic vapor and the ratio between organic and inorganic vapor concentrations are in a suitable range.
Maryam Dalirian, Arttu Ylisirniö, Angela Buchholz, Daniel Schlesinger, Johan Ström, Annele Virtanen, and Ilona Riipinen
Atmos. Chem. Phys., 18, 12477–12489, https://doi.org/10.5194/acp-18-12477-2018, https://doi.org/10.5194/acp-18-12477-2018, 2018
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Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect is, however, still uncertain. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC particles, in pure state or coated by various organic species. Our results show that existing theories have potential in describing the CCN activation of atmospheric BC mixed with soluble pollutants.
Xiao-Feng Huang, Bei-Bing Zou, Ling-Yan He, Min Hu, André S. H. Prévôt, and Yuan-Hang Zhang
Atmos. Chem. Phys., 18, 11563–11580, https://doi.org/10.5194/acp-18-11563-2018, https://doi.org/10.5194/acp-18-11563-2018, 2018
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A novel multilinear engine (ME-2) model was applied to the PM2.5 dataset observed in the Pearl River Delta (PRD) of China in 2015 and identified the sources of secondary sulfate (21 %), vehicle emissions (14 %), industrial emissions (13 %), secondary nitrate (11 %), biomass burning (11 %), secondary organic aerosol (7 %), coal burning (6 %), fugitive dust (5 %), ship emissions (3 %) and aged sea salt (2 %). The central PRD area was clearly identified as the key emission area in the PRD.
Amelie Bertrand, Giulia Stefenelli, Simone M. Pieber, Emily A. Bruns, Brice Temime-Roussel, Jay G. Slowik, Henri Wortham, André S. H. Prévôt, Imad El Haddad, and Nicolas Marchand
Atmos. Chem. Phys., 18, 10915–10930, https://doi.org/10.5194/acp-18-10915-2018, https://doi.org/10.5194/acp-18-10915-2018, 2018
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We model the evolution of several BBOA markers including levoglucosan during aging experiments conducted in an atmospheric Teflon chamber, in order to evaluate the influence of vapor wall loss on the determination of the rate constants of the compounds with hydroxyl radicals (OH).
Xia Li, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Rujin Huang, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 18, 10675–10691, https://doi.org/10.5194/acp-18-10675-2018, https://doi.org/10.5194/acp-18-10675-2018, 2018
Ramakrishna Ramisetty, Ahmed Abdelmonem, Xiaoli Shen, Harald Saathoff, Thomas Leisner, and Claudia Mohr
Atmos. Meas. Tech., 11, 4345–4360, https://doi.org/10.5194/amt-11-4345-2018, https://doi.org/10.5194/amt-11-4345-2018, 2018
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In this study we coupled a laser ablation aerosol time-of-flight (LAAPTOF) single-particle mass spectrometer, originally equipped with an excimer laser, to a femtosecond laser. The objective was to assess the influence of the higher laser power density of the femtosecond laser on ablation–ionization of atmospheric particles, ion signal, and ultimately quantitative abilities of the single-particle mass spectrometer.
Simone M. Pieber, Nivedita K. Kumar, Felix Klein, Pierre Comte, Deepika Bhattu, Josef Dommen, Emily A. Bruns, Doǧuşhan Kılıç, Imad El Haddad, Alejandro Keller, Jan Czerwinski, Norbert Heeb, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 9929–9954, https://doi.org/10.5194/acp-18-9929-2018, https://doi.org/10.5194/acp-18-9929-2018, 2018
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We studied primary emissions and secondary organic aerosol (SOA) from gasoline direct injection (GDI) vehicles including GDIs retrofitted with gasoline particle filters (GPF). GPF retrofitting significantly decreased the primary particulate matter, particularly through removal of refractory black carbon and, to a lesser extent, of non-refractory organic particulates. SOA experiments were conducted in a batch and flow reactor. GPF retrofitting did not significantly affect precursors or yields.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Martin Wild, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 9741–9765, https://doi.org/10.5194/acp-18-9741-2018, https://doi.org/10.5194/acp-18-9741-2018, 2018
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We report a model sensitivity study on the impact of aerosol–radiation interaction (ARI) changes in Europe between 1990 and 2010 on summer surface ozone via effects on photolysis rates and biogenic emissions. The overall impact of ARI changes on ozone was relatively small when compared to the total ozone concentrations, but it was more important when compared to the order of magnitude of ozone trends, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.
Konrad Deetz, Heike Vogel, Peter Knippertz, Bianca Adler, Jonathan Taylor, Hugh Coe, Keith Bower, Sophie Haslett, Michael Flynn, James Dorsey, Ian Crawford, Christoph Kottmeier, and Bernhard Vogel
Atmos. Chem. Phys., 18, 9767–9788, https://doi.org/10.5194/acp-18-9767-2018, https://doi.org/10.5194/acp-18-9767-2018, 2018
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Highly resolved process study simulations for 2–3 July are conducted with COSMO-ART to assess the aerosol direct and indirect effect on meteorological conditions over southern West Africa. The meteorological phenomena of Atlantic inflow and stratus-to-cumulus transition are identified as highly susceptible to the aerosol direct effect, leading to a spatial shift of the Atlantic inflow front and a temporal shift of the stratus-to-cumulus transition with changes in the aerosol amount.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
Marco Pandolfi, Lucas Alados-Arboledas, Andrés Alastuey, Marcos Andrade, Christo Angelov, Begoña Artiñano, John Backman, Urs Baltensperger, Paolo Bonasoni, Nicolas Bukowiecki, Martine Collaud Coen, Sébastien Conil, Esther Coz, Vincent Crenn, Vadimas Dudoitis, Marina Ealo, Kostas Eleftheriadis, Olivier Favez, Prodromos Fetfatzis, Markus Fiebig, Harald Flentje, Patrick Ginot, Martin Gysel, Bas Henzing, Andras Hoffer, Adela Holubova Smejkalova, Ivo Kalapov, Nikos Kalivitis, Giorgos Kouvarakis, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Chris Lunder, Krista Luoma, Hassan Lyamani, Angela Marinoni, Nikos Mihalopoulos, Marcel Moerman, José Nicolas, Colin O'Dowd, Tuukka Petäjä, Jean-Eudes Petit, Jean Marc Pichon, Nina Prokopciuk, Jean-Philippe Putaud, Sergio Rodríguez, Jean Sciare, Karine Sellegri, Erik Swietlicki, Gloria Titos, Thomas Tuch, Peter Tunved, Vidmantas Ulevicius, Aditya Vaishya, Milan Vana, Aki Virkkula, Stergios Vratolis, Ernest Weingartner, Alfred Wiedensohler, and Paolo Laj
Atmos. Chem. Phys., 18, 7877–7911, https://doi.org/10.5194/acp-18-7877-2018, https://doi.org/10.5194/acp-18-7877-2018, 2018
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This investigation presents the variability in near-surface in situ aerosol particle light-scattering measurements obtained over the past decade at 28 measuring atmospheric observatories which are part of the ACTRIS Research Infrastructure, and most of them belong to the GAW network. This paper provides a comprehensive picture of the spatial and temporal variability of aerosol particles optical properties in Europe.
Sekou Keita, Cathy Liousse, Véronique Yoboué, Pamela Dominutti, Benjamin Guinot, Eric-Michel Assamoi, Agnès Borbon, Sophie L. Haslett, Laetitia Bouvier, Aurélie Colomb, Hugh Coe, Aristide Akpo, Jacques Adon, Julien Bahino, Madina Doumbia, Julien Djossou, Corinne Galy-Lacaux, Eric Gardrat, Sylvain Gnamien, Jean F. Léon, Money Ossohou, E. Touré N'Datchoh, and Laurent Roblou
Atmos. Chem. Phys., 18, 7691–7708, https://doi.org/10.5194/acp-18-7691-2018, https://doi.org/10.5194/acp-18-7691-2018, 2018
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This study provides emission factor (EF) data for elemental and organic carbon, total particulate matter and 58 volatile organic compound species for combustion sources specific to Africa to establish emission inventories with less uncertainty. EFs obtained in this study are generally higher than those in the literature whose values are used in emissions inventories for Africa. This shows that particles and VOC emissions were sometimes underestimated and underlines this study's importance.
Quentin Bourgeois, Annica M. L. Ekman, Jean-Baptiste Renard, Radovan Krejci, Abhay Devasthale, Frida A.-M. Bender, Ilona Riipinen, Gwenaël Berthet, and Jason L. Tackett
Atmos. Chem. Phys., 18, 7709–7720, https://doi.org/10.5194/acp-18-7709-2018, https://doi.org/10.5194/acp-18-7709-2018, 2018
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The altitude of aerosols is crucial as they can impact cloud formation and radiation. In this study, satellite observations have been used to characterize the global aerosol optical depth (AOD) in the boundary layer and the free troposphere. The free troposphere contributes 39 % to the global AOD during daytime. Overall, the results have implications for the description of budgets, sources, sinks and transport of aerosol particles as presently described in the atmospheric model.
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Doğuşhan Kılıç, Imad El Haddad, Benjamin T. Brem, Emily Bruns, Carlo Bozetti, Joel Corbin, Lukas Durdina, Ru-Jin Huang, Jianhui Jiang, Felix Klein, Avi Lavi, Simone M. Pieber, Theo Rindlisbacher, Yinon Rudich, Jay G. Slowik, Jing Wang, Urs Baltensperger, and Andre S. H. Prévôt
Atmos. Chem. Phys., 18, 7379–7391, https://doi.org/10.5194/acp-18-7379-2018, https://doi.org/10.5194/acp-18-7379-2018, 2018
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We study primary emissions and secondary aerosol (SA) from an aircraft turbofan. By monitoring the chemical composition of both gaseous and particulate emissions at different engine loads, we explained SA formed in an oxidation flow reactor (PAM) by the oxidation of gaseous species. At idle, more than 90 % of the secondary particle mass was organic and could be explained by the oxidation of gaseous aromatic species, while at an approximated cruise load sulfates comprised 85 % of the total SA.
Arineh Cholakian, Matthias Beekmann, Augustin Colette, Isabelle Coll, Guillaume Siour, Jean Sciare, Nicolas Marchand, Florian Couvidat, Jorge Pey, Valerie Gros, Stéphane Sauvage, Vincent Michoud, Karine Sellegri, Aurélie Colomb, Karine Sartelet, Helen Langley DeWitt, Miriam Elser, André S. H. Prévot, Sonke Szidat, and François Dulac
Atmos. Chem. Phys., 18, 7287–7312, https://doi.org/10.5194/acp-18-7287-2018, https://doi.org/10.5194/acp-18-7287-2018, 2018
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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
Jun Zhou, Peter Zotter, Emily A. Bruns, Giulia Stefenelli, Deepika Bhattu, Samuel Brown, Amelie Bertrand, Nicolas Marchand, Houssni Lamkaddam, Jay G. Slowik, André S. H. Prévôt, Urs Baltensperger, Thomas Nussbaumer, Imad El-Haddad, and Josef Dommen
Atmos. Chem. Phys., 18, 6985–7000, https://doi.org/10.5194/acp-18-6985-2018, https://doi.org/10.5194/acp-18-6985-2018, 2018
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We thoroughly studied the reactive oxygen species (ROS) generation potential of particulate wood combustion emissions, from different combustion technologies, fuel types, operation methods, combustion regimes and phases. ROS from automatically operated combustion devices under optimal conditions were much lower than those from manually operated appliances. We examined the impact of atmospheric aging on ROS content in SOA and determined the controlling parameters, by using an online ROS analyzer.
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.
Xiaoli Shen, Ramakrishna Ramisetty, Claudia Mohr, Wei Huang, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 11, 2325–2343, https://doi.org/10.5194/amt-11-2325-2018, https://doi.org/10.5194/amt-11-2325-2018, 2018
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This paper presents performance data and reference spectra from the commercially available single-particle mass spectrometer LAAPTOF. The main characteristics of the instrument, like its detection efficiency, are given for a wide particle size range. Furthermore, reference mass spectra for 32 well-defined different particle types relevant for atmospheric aerosol compounds are presented. It is shown that these reference mass spectra are very useful in analysis of atmospheric aerosol particles.
Ernesto Reyes-Villegas, Michael Priestley, Yu-Chieh Ting, Sophie Haslett, Thomas Bannan, Michael Le Breton, Paul I. Williams, Asan Bacak, Michael J. Flynn, Hugh Coe, Carl Percival, and James D. Allan
Atmos. Chem. Phys., 18, 4093–4111, https://doi.org/10.5194/acp-18-4093-2018, https://doi.org/10.5194/acp-18-4093-2018, 2018
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This work presents the analysis of a special event with high biomass burning emissions, named Bonfire Night. Nitrogen chemistry was observed and it was possible to study the night time chemistry. It was possible to quantify particulate organic oxides of nitrogen (PON) concentrations of 2.8 µg m−3 using 46 : 30 ratios from aerosol mass spectrometry measurements. The use of the receptor model positive matrix factorization (PMF) allowed to separate organic aerosols into different sources.
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.
Wei Huang, Harald Saathoff, Aki Pajunoja, Xiaoli Shen, Karl-Heinz Naumann, Robert Wagner, Annele Virtanen, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, https://doi.org/10.5194/acp-18-2883-2018, 2018
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.
Qiao Zhu, Xiao-Feng Huang, Li-Ming Cao, Lin-Tong Wei, Bin Zhang, Ling-Yan He, Miriam Elser, Francesco Canonaco, Jay G. Slowik, Carlo Bozzetti, Imad El-Haddad, and André S. H. Prévôt
Atmos. Meas. Tech., 11, 1049–1060, https://doi.org/10.5194/amt-11-1049-2018, https://doi.org/10.5194/amt-11-1049-2018, 2018
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Organic aerosol constitutes one of the major components of atmospheric particulate matter globally and is emitted from various sources. Therefore, identifying and quantifying the sources of organic aerosol accurately is a key task in the field. In this study, we applied a rather novel procedure for an improved source apportionment method (ME-2) to resolve the
less meaningful or mixed factorsproblems for organic aerosol using the traditional method (PMF).
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.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 2175–2198, https://doi.org/10.5194/acp-18-2175-2018, https://doi.org/10.5194/acp-18-2175-2018, 2018
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We report a modeling study investigating the uncertainties in ozone production in Europe. Using various methods for different emission and meteorological scenarios, we searched for the possible reasons for underestimation of high ozone levels in Europe by models. Our results suggest that emissions, especially NOx, might be too low in the European inventories. Improvement of the modeled ozone production will contribute to more consistent and effective ozone mitigation strategies for the future.
Ugo Molteni, Federico Bianchi, Felix Klein, Imad El Haddad, Carla Frege, Michel J. Rossi, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 1909–1921, https://doi.org/10.5194/acp-18-1909-2018, https://doi.org/10.5194/acp-18-1909-2018, 2018
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Anthropogenic volatile organic compounds often dominate the urban atmosphere and consist to a large degree of aromatics. These compounds are already known as important precursors for the formation of secondary organic aerosol. This study shows how the oxidation of aromatics with an OH radical leads to subsequent autoxidation chain reactions forming highly oxygenated molecules. We hypothesize that these may contribute substantially to new particle formation events detected in urban areas.
Joel Brito, Evelyn Freney, Pamela Dominutti, Agnes Borbon, Sophie L. Haslett, Anneke M. Batenburg, Aurelie Colomb, Regis Dupuy, Cyrielle Denjean, Frederic Burnet, Thierry Bourriane, Adrien Deroubaix, Karine Sellegri, Stephan Borrmann, Hugh Coe, Cyrille Flamant, Peter Knippertz, and Alfons Schwarzenboeck
Atmos. Chem. Phys., 18, 757–772, https://doi.org/10.5194/acp-18-757-2018, https://doi.org/10.5194/acp-18-757-2018, 2018
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This work focuses on sources of submicron aerosol particles over southern West Africa (SWA). Results have shown that isoprene, a gas-phase compound of biogenic origin, is responsible for roughly 25 % of the organic aerosol (OA) loading, under most background or urban plumes alike. This fraction represents a lower estimate from the biogenic contribution in this fairly polluted region. This work sheds light upon the role of anthropogenic and biogenic emissions on the pollution burden over SWA.
Sophie L. Haslett, J. Chris Thomas, William T. Morgan, Rory Hadden, Dantong Liu, James D. Allan, Paul I. Williams, Sekou Keita, Cathy Liousse, and Hugh Coe
Atmos. Chem. Phys., 18, 385–403, https://doi.org/10.5194/acp-18-385-2018, https://doi.org/10.5194/acp-18-385-2018, 2018
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Wood burning is chaotic, so the particles emitted can be difficult to study in a repeatable way. Here, we addressed this problem by carefully controlling small wood fires in the lab. We saw three burning phases, which could be told apart chemically; we also saw evidence of these in measurements of wood burning in London in 2012. Controlled experiments like this help us to understand why emissions are so variable and to recognise burning conditions just from the particles seen in the atmosphere.
Jun Zhou, Emily A. Bruns, Peter Zotter, Giulia Stefenelli, André S. H. Prévôt, Urs Baltensperger, Imad El-Haddad, and Josef Dommen
Atmos. Meas. Tech., 11, 65–80, https://doi.org/10.5194/amt-11-65-2018, https://doi.org/10.5194/amt-11-65-2018, 2018
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Reactive oxygen species (ROS) in the particle phase may induce oxidative stress in the human lungs upon inhalation. Here we present and thoroughly characterize a modified online and offline ROS analyzer. Selected model organic compounds were tested and potential interferences from gas-phase and matrix effects of particulate constituents were evaluated. ROS measurements of filter samples revealed the rapid decay of a substantial ROS fraction, supporting the application of online measurements.
Ulrich K. Krieger, Franziska Siegrist, Claudia Marcolli, Eva U. Emanuelsson, Freya M. Gøbel, Merete Bilde, Aleksandra Marsh, Jonathan P. Reid, Andrew J. Huisman, Ilona Riipinen, Noora Hyttinen, Nanna Myllys, Theo Kurtén, Thomas Bannan, Carl J. Percival, and David Topping
Atmos. Meas. Tech., 11, 49–63, https://doi.org/10.5194/amt-11-49-2018, https://doi.org/10.5194/amt-11-49-2018, 2018
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Vapor pressures of low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique, which is generally reported to be smaller than a factor of 2. We determined saturation vapor pressures for the homologous series of polyethylene glycols ranging in vapor pressure at 298 K from 1E−7 Pa to 5E−2 Pa as a reference set.
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
Naifang Bei, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Xia Li, Rujin Huang, Zhengqiang Li, Xin Long, Li Xing, Shuyu Zhao, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 17, 14579–14591, https://doi.org/10.5194/acp-17-14579-2017, https://doi.org/10.5194/acp-17-14579-2017, 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.
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.
Laura-Hélèna Rivellini, Isabelle Chiapello, Emmanuel Tison, Marc Fourmentin, Anaïs Féron, Aboubacry Diallo, Thierno N'Diaye, Philippe Goloub, Francesco Canonaco, André Stephan Henry Prévôt, and Véronique Riffault
Atmos. Chem. Phys., 17, 10291–10314, https://doi.org/10.5194/acp-17-10291-2017, https://doi.org/10.5194/acp-17-10291-2017, 2017
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A 3-month field campaign was conducted in March–June 2015 in Senegal, as part of the SHADOW (SaHAran Dust Over West Africa) project. This article presents the time variability of the chemical composition of submicron particles. Organics (sulfates) were predominant for days under continental (marine) influence. Half the organic sources were identified as local, including one due to open waste-burning, and half were linked to regional air masses and enhanced photochemical processes.
Yi Ming Qin, Hao Bo Tan, Yong Jie Li, Misha I. Schurman, Fei Li, Francesco Canonaco, André S. H. Prévôt, and Chak K. Chan
Atmos. Chem. Phys., 17, 10245–10258, https://doi.org/10.5194/acp-17-10245-2017, https://doi.org/10.5194/acp-17-10245-2017, 2017
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Freshly emitted HOA contributed significantly to the high concentrations of organics at night as heavy-duty vehicles enter downtown Guangzhou, while SOA contributed to the daytime high concentration. The large input of NOx, from automobile emissions, resulted in the significant formation of nitrate in both daytime and nighttime. Mitigating the PM pollution in urbanized areas such as Guangzhou can potentially benefit their peripheral cities, by reductions in traffic-related pollutants.
Prettiny K. Ma, Yunliang Zhao, Allen L. Robinson, David R. Worton, Allen H. Goldstein, Amber M. Ortega, Jose L. Jimenez, Peter Zotter, André S. H. Prévôt, Sönke Szidat, and Patrick L. Hayes
Atmos. Chem. Phys., 17, 9237–9259, https://doi.org/10.5194/acp-17-9237-2017, https://doi.org/10.5194/acp-17-9237-2017, 2017
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Airborne particulate matter (PM) negatively impacts air quality in cities throughout the world. An important fraction of PM is organic aerosol. We have evaluated and developed several new models for secondary organic aerosol (SOA), which is formed from the chemical processing of gaseous precursors. Using our model results, we have quantified important SOA sources and precursors and also identified possible model parameterizations that could be used for air quality predictions.
Georgios Tsagkogeorgas, Pontus Roldin, Jonathan Duplissy, Linda Rondo, Jasmin Tröstl, Jay G. Slowik, Sebastian Ehrhart, Alessandro Franchin, Andreas Kürten, Antonio Amorim, Federico Bianchi, Jasper Kirkby, Tuukka Petäjä, Urs Baltensperger, Michael Boy, Joachim Curtius, Richard C. Flagan, Markku Kulmala, Neil M. Donahue, and Frank Stratmann
Atmos. Chem. Phys., 17, 8923–8938, https://doi.org/10.5194/acp-17-8923-2017, https://doi.org/10.5194/acp-17-8923-2017, 2017
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The H2SO4 vapour pressure plays key role in Earth's and Venus' atmospheres. In regions where RH is low and stabilising bases are scarce, H2SO4 can evaporate from particles; however the H2SO4 vapour pressure at low RH is uncertain. To address this, we measured H2SO4 evaporation versus T and RH in the CLOUD chamber and constrained the equilibrium constants for dissociation and dehydration of H2SO4. This study is important for nucleation, particle growth and H2SO4 formation occurring in atmosphere.
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.
Sebnem Aksoyoglu, Giancarlo Ciarelli, Imad El-Haddad, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 7757–7773, https://doi.org/10.5194/acp-17-7757-2017, https://doi.org/10.5194/acp-17-7757-2017, 2017
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Sources of inorganic aerosols in Europe were investigated using a regional air quality model. Results of this study suggested that biogenic volatile organic coumpounds emitted from vegetation had a significant effect on inorganic aerosols, especially on ammonium nitrate concentrations. Sensitivity analyses showed that it is mainly terpene reactions with nitrate radical at night that lead to a decrease in ammonium nitrate.
Giancarlo Ciarelli, Imad El Haddad, Emily Bruns, Sebnem Aksoyoglu, Ottmar Möhler, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 10, 2303–2320, https://doi.org/10.5194/gmd-10-2303-2017, https://doi.org/10.5194/gmd-10-2303-2017, 2017
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In Europe, residential wood-burning emissions constitute one of the main anthropogenic sources of air pollution. Novel wood-burning experiments performed in a state-of-the-art smog chamber provide valuable information on the chemical properties of wood-burning emissions and the transformation in the atmosphere. In this study, these new data were used in a box model to constrain a parameterization suitable for predicting the contribution of wood burning to air pollution with large-scale models.
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).
Markus Furger, María Cruz Minguillón, Varun Yadav, Jay G. Slowik, Christoph Hüglin, Roman Fröhlich, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Meas. Tech., 10, 2061–2076, https://doi.org/10.5194/amt-10-2061-2017, https://doi.org/10.5194/amt-10-2061-2017, 2017
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An Xact 625 Ambient Metals Monitor was tested during a 3-week summer field campaign at a rural, traffic-influenced site in Switzerland. The objective was to characterize the operation of the instrument, evaluate the data quality by intercomparison with other independent measurements, and test its applicability for aerosol source quantification. The results demonstrate significant advantages compared to traditional elemental analysis methods, with some desirable improvements.
Lisa Stirnweis, Claudia Marcolli, Josef Dommen, Peter Barmet, Carla Frege, Stephen M. Platt, Emily A. Bruns, Manuel Krapf, Jay G. Slowik, Robert Wolf, Andre S. H. Prévôt, Urs Baltensperger, and Imad El-Haddad
Atmos. Chem. Phys., 17, 5035–5061, https://doi.org/10.5194/acp-17-5035-2017, https://doi.org/10.5194/acp-17-5035-2017, 2017
Haiyan Li, Qi Zhang, Qiang Zhang, Chunrong Chen, Litao Wang, Zhe Wei, Shan Zhou, Caroline Parworth, Bo Zheng, Francesco Canonaco, André S. H. Prévôt, Ping Chen, Hongliang Zhang, Timothy J. Wallington, and Kebin He
Atmos. Chem. Phys., 17, 4751–4768, https://doi.org/10.5194/acp-17-4751-2017, https://doi.org/10.5194/acp-17-4751-2017, 2017
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The sources and aerosol evolution processes of severe pollution episodes were investigated in Handan during wintertime using real-time measurements. An in-depth analysis of the data uncovered that primary emissions from coal combustion and biomass burning together with secondary formation of sulfate (mainly from SO2 emitted by coal combustion) are important driving factors for haze evolution. Our findings provide useful insights into air pollution control in heavily polluted regions.
Peter Zotter, Hanna Herich, Martin Gysel, Imad El-Haddad, Yanlin Zhang, Griša Močnik, Christoph Hüglin, Urs Baltensperger, Sönke Szidat, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 4229–4249, https://doi.org/10.5194/acp-17-4229-2017, https://doi.org/10.5194/acp-17-4229-2017, 2017
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Most studies use a single Ångström exponent for wood burning (αWB) and traffic (αTR) emissions in the Aethalometer model, used for source apportionment of black carbon, derived from previous work. However, accurate determination of the α values is currently lacking. Comparing radiocarbon measurements (14C) with the Aehtalometer model, good agreement was found, indicating that the Aethalometer model reproduces reasonably well the 14C results using our best estimate of a single αWB and αTR.
Luka Drinovec, Asta Gregorič, Peter Zotter, Robert Wolf, Emily Anne Bruns, André S. H. Prévôt, Jean-Eudes Petit, Olivier Favez, Jean Sciare, Ian J. Arnold, Rajan K. Chakrabarty, Hans Moosmüller, Agnes Filep, and Griša Močnik
Atmos. Meas. Tech., 10, 1043–1059, https://doi.org/10.5194/amt-10-1043-2017, https://doi.org/10.5194/amt-10-1043-2017, 2017
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Black carbon measurements are usually conducted with absorption filter photometers, which are prone to the filter-loading effect – a saturation of the instrumental response due to the accumulation of the sample in the filter matrix. In this paper, we conducted several field campaigns to investigate the hypothesis that this filter-loading effect depends on the optical properties of particles present in the filter matrix, especially on the coating of black carbon particles.
Mikko Äijälä, Liine Heikkinen, Roman Fröhlich, Francesco Canonaco, André S. H. Prévôt, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 17, 3165–3197, https://doi.org/10.5194/acp-17-3165-2017, https://doi.org/10.5194/acp-17-3165-2017, 2017
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Mass spectrometric measurements commonly yield data on hundreds of variables over thousands of points in time. Refining and synthesising this “raw” data into chemical information necessitates the use of advanced, statistics-based data analysis techniques. Here we present an example of combining data dimensionality reduction (factorisation) with exploratory classification (clustering) and show that the results complement and broaden our current perspectives on aerosol chemical classification.
Carla Frege, Federico Bianchi, Ugo Molteni, Jasmin Tröstl, Heikki Junninen, Stephan Henne, Mikko Sipilä, Erik Herrmann, Michel J. Rossi, Markku Kulmala, Christopher R. Hoyle, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 17, 2613–2629, https://doi.org/10.5194/acp-17-2613-2017, https://doi.org/10.5194/acp-17-2613-2017, 2017
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We present measurements of the chemical composition of atmospheric ions at high altitude (3450 m a.s.l.) during a 9-month campaign. We detected remarkably high correlation between methanesulfonic acid (MSA) and SO5−. Halogenated species were also detected frequently at this continental location. New-particle formation events occurred via the condensation of highly oxygenated molecules (HOMs) at very low sulfuric acid concentration or, less frequently, due to ammonia–sulfuric acid clusters.
Emily A. Bruns, Jay G. Slowik, Imad El Haddad, Dogushan Kilic, Felix Klein, Josef Dommen, Brice Temime-Roussel, Nicolas Marchand, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 705–720, https://doi.org/10.5194/acp-17-705-2017, https://doi.org/10.5194/acp-17-705-2017, 2017
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We characterize primary and aged gaseous emissions from residential wood combustion using proton transfer reaction time-of-flight mass spectrometry. This approach allows for improved characterization, particularly of oxygenated gases, which are a considerable fraction of the total gaseous mass emitted during residential wood combustion. This study is the first thorough characterization of organic gases from this source and provides a benchmark for future studies.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
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.
Ernesto Reyes-Villegas, David C. Green, Max Priestman, Francesco Canonaco, Hugh Coe, André S. H. Prévôt, and James D. Allan
Atmos. Chem. Phys., 16, 15545–15559, https://doi.org/10.5194/acp-16-15545-2016, https://doi.org/10.5194/acp-16-15545-2016, 2016
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For the first time in the UK, an Aerosol Chemical Speciation Monitor was used to measure aerosol concentrations in London in March–December 2013, with further organic aerosol (OA) source apportionment using the ME-2 factorization tool. Five OA sources were identified: biomass burning OA, hydrocarbon-like OA, cooking OA, semivolatile oxygenated OA and low-volatility oxygenated OA. This information can be used to take future action on the respective legislation in order to improve the air quality.
Jianzhong Xu, Jinsen Shi, Qi Zhang, Xinlei Ge, Francesco Canonaco, André S. H. Prévôt, Matthias Vonwiller, Sönke Szidat, Jinming Ge, Jianmin Ma, Yanqing An, Shichang Kang, and Dahe Qin
Atmos. Chem. Phys., 16, 14937–14957, https://doi.org/10.5194/acp-16-14937-2016, https://doi.org/10.5194/acp-16-14937-2016, 2016
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This study deployed an AMS field study in Lanzhou, a city in northwestern China, evaluating the chemical composition, sources, and processes of urban aerosols during wintertime. In comparison with the results during summer in Lanzhou, the air pollution during winter was more severe and the sources were more complex. In addition, this paper estimates the contributions of fossil and non-fossil sources of organic carbon to primary and secondary organic carbon using the carbon isotopic method.
Neha Sareen, Annmarie G. Carlton, Jason D. Surratt, Avram Gold, Ben Lee, Felipe D. Lopez-Hilfiker, Claudia Mohr, Joel A. Thornton, Zhenfa Zhang, Yong B. Lim, and Barbara J. Turpin
Atmos. Chem. Phys., 16, 14409–14420, https://doi.org/10.5194/acp-16-14409-2016, https://doi.org/10.5194/acp-16-14409-2016, 2016
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Michael Bressi, Fabrizia Cavalli, Claudio A. Belis, Jean-Philippe Putaud, Roman Fröhlich, Sebastiao Martins dos Santos, Ettore Petralia, André S. H. Prévôt, Massimo Berico, Antonella Malaguti, and Francesco Canonaco
Atmos. Chem. Phys., 16, 12875–12896, https://doi.org/10.5194/acp-16-12875-2016, https://doi.org/10.5194/acp-16-12875-2016, 2016
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Atmospheric particulate matter (PM) levels and resulting impacts on human health are in the Po Valley (Italy) among the highest in Europe. This study discusses submicron PM chemical composition, sources and atmospheric processes in this region, using state-of-the-art measurement techniques and receptor models. Based on these results, effective PM abatement strategies are suggested in the upper Po Valley.
Bertrand Bessagnet, Guido Pirovano, Mihaela Mircea, Cornelius Cuvelier, Armin Aulinger, Giuseppe Calori, Giancarlo Ciarelli, Astrid Manders, Rainer Stern, Svetlana Tsyro, Marta García Vivanco, Philippe Thunis, Maria-Teresa Pay, Augustin Colette, Florian Couvidat, Frédérik Meleux, Laurence Rouïl, Anthony Ung, Sebnem Aksoyoglu, José María Baldasano, Johannes Bieser, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Sandro Finardi, Richard Kranenburg, Camillo Silibello, Claudio Carnevale, Wenche Aas, Jean-Charles Dupont, Hilde Fagerli, Lucia Gonzalez, Laurent Menut, André S. H. Prévôt, Pete Roberts, and Les White
Atmos. Chem. Phys., 16, 12667–12701, https://doi.org/10.5194/acp-16-12667-2016, https://doi.org/10.5194/acp-16-12667-2016, 2016
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The EURODELTA III exercise allows a very comprehensive intercomparison and evaluation of air quality models' performance. On average, the models provide a rather good picture of the particulate matter (PM) concentrations over Europe even if the highest concentrations are underestimated. The meteorology is responsible for model discrepancies, while the lack of emissions, particularly in winter, is mentioned as the main reason for the underestimations of PM.
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.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
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.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
Bernadette Rosati, Martin Gysel, Florian Rubach, Thomas F. Mentel, Brigitta Goger, Laurent Poulain, Patrick Schlag, Pasi Miettinen, Aki Pajunoja, Annele Virtanen, Henk Klein Baltink, J. S. Bas Henzing, Johannes Größ, Gian Paolo Gobbi, Alfred Wiedensohler, Astrid Kiendler-Scharr, Stefano Decesari, Maria Cristina Facchini, Ernest Weingartner, and Urs Baltensperger
Atmos. Chem. Phys., 16, 7295–7315, https://doi.org/10.5194/acp-16-7295-2016, https://doi.org/10.5194/acp-16-7295-2016, 2016
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This study presents PEGASOS project data from field campaigns in the Po Valley, Italy and the Netherlands. Vertical profiles of aerosol hygroscopicity and chemical composition were investigated with airborne measurements on board a Zeppelin NT airship. A special focus was on the evolution of different mixing layers within the PBL as a function of daytime. A closure study showed that variations in aerosol hygroscopicity can well be explained by the variations in chemical composition.
Miriam Elser, Carlo Bozzetti, Imad El-Haddad, Marek Maasikmets, Erik Teinemaa, Rene Richter, Robert Wolf, Jay G. Slowik, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 7117–7134, https://doi.org/10.5194/acp-16-7117-2016, https://doi.org/10.5194/acp-16-7117-2016, 2016
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This work presents the first detailed in-situ measurements of major air pollutants (including NR-PM2.5, eBC, and trace gases) in the two biggest cities in Estonia. The sources of organic aerosols were investigated by means of positive matrix factorization. Highly time-resolved mobile measurements allowed for the identification of source areas and the determination of regional background concentrations as well as urban increments of the individual components.
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.
Bernadette Rosati, Erik Herrmann, Silvia Bucci, Federico Fierli, Francesco Cairo, Martin Gysel, Ralf Tillmann, Johannes Größ, Gian Paolo Gobbi, Luca Di Liberto, Guido Di Donfrancesco, Alfred Wiedensohler, Ernest Weingartner, Annele Virtanen, Thomas F. Mentel, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4539–4554, https://doi.org/10.5194/acp-16-4539-2016, https://doi.org/10.5194/acp-16-4539-2016, 2016
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We present vertical profiles of aerosol optical properties, which were explored within the planetary boundary layer in a case study in 2012 in the Po Valley region. A comparison of in situ measurements recorded aboard a Zeppelin NT and ground-based remote-sensing data was performed yielding good agreement. Additionally, the role of ambient relative humidity for the aerosol particles' optical properties was investigated.
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
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
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We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061, https://doi.org/10.5194/acp-16-4043-2016, https://doi.org/10.5194/acp-16-4043-2016, 2016
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A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Christos Fountoukis, Athanasios G. Megaritis, Ksakousti Skyllakou, Panagiotis E. Charalampidis, Hugo A. C. Denier van der Gon, Monica Crippa, André S. H. Prévôt, Friederike Fachinger, Alfred Wiedensohler, Christodoulos Pilinis, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 3727–3741, https://doi.org/10.5194/acp-16-3727-2016, https://doi.org/10.5194/acp-16-3727-2016, 2016
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We use PMCAMx with high grid resolution over Paris to simulate carbonaceous aerosol during the summer and winter MEGAPOLI campaigns. PMCAMx reproduces BC observations well. Addition of cooking organic aerosol emissions of 80 mg per day per capita is needed to reproduce the corresponding observations. While the oxygenated organic aerosol predictions during the summer are encouraging a major wintertime source appears to be missing.
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.
Andrea Paciga, Eleni Karnezi, Evangelia Kostenidou, Lea Hildebrandt, Magda Psichoudaki, Gabriella J. Engelhart, Byong-Hyoek Lee, Monica Crippa, André S. H. Prévôt, Urs Baltensperger, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 2013–2023, https://doi.org/10.5194/acp-16-2013-2016, https://doi.org/10.5194/acp-16-2013-2016, 2016
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We estimate the volatility distribution for the organic aerosol (OA) components during summer and winter field campaigns in Paris, France as part of the collaborative project MEGAPOLI. The OA factors (hydrocarbon like OA, cooking OA, marine OA, oxygenated OA) had a broad spectrum of volatilities with no direct link between the average volatility and average oxygen to carbon of the OA components.
Sebnem Aksoyoglu, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 1895–1906, https://doi.org/10.5194/acp-16-1895-2016, https://doi.org/10.5194/acp-16-1895-2016, 2016
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As a least-regulated source, ship emissions contribute significantly to air pollution. We used an air quality model to determine the effects of international shipping on the annual and seasonal concentrations of ozone, primary and secondary components of PM2.5, and dry and wet deposition of N and S compounds in Europe. The results presented in this paper suggest evolution of NOx emissions from ships and land-based NH3 emissions will play a significant role in the future European air quality.
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.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
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.
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.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
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