Articles | Volume 18, issue 4
https://doi.org/10.5194/acp-18-2883-2018
© Author(s) 2018. 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-18-2883-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
28 Feb 2018
Research article |
| 28 Feb 2018
| 28 Feb 2018
α-Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity
Wei Huang
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Institute of Geography and Geoecology, Karlsruhe Institute of
Technology, 76131 Karlsruhe, Germany
Harald Saathoff
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Aki Pajunoja
Department of Applied Physics, University of Eastern Finland, Kuopio,
80101, Finland
Xiaoli Shen
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Institute of Geography and Geoecology, Karlsruhe Institute of
Technology, 76131 Karlsruhe, Germany
Karl-Heinz Naumann
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Robert Wagner
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Annele Virtanen
Department of Applied Physics, University of Eastern Finland, Kuopio,
80101, Finland
Thomas Leisner
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Institute of Meteorology and Climate Research, Karlsruhe Institute of
Technology, 76344 Eggenstein-Leopoldshafen, Germany
Department of Environmental Science and Analytical Chemistry,
Stockholm University, Stockholm, 11418, Sweden
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Our study employs advanced tools, including scanning lidar, balloons, and UAVs, to explore aerosol particles in the atmosphere. The scanning lidar offers distinctive near-ground-level insights, enriching our comprehension of aerosol distribution from ground level to the free troposphere. This research provides valuable data for comparing remote sensing and in situ aerosol measurements, advancing our understanding of aerosol impacts on radiative transfer, clouds, and air quality.
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.
Johanna S. Seidel, Alexei A. Kiselev, Alice Keinert, Frank Stratmann, Thomas Leisner, and Susan Hartmann
Atmos. Chem. Phys., 24, 5247–5263, https://doi.org/10.5194/acp-24-5247-2024, https://doi.org/10.5194/acp-24-5247-2024, 2024
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Clouds often contain several thousand times more ice crystals than aerosol particles catalyzing ice formation. This phenomenon, commonly known as ice multiplication, is often explained by secondary ice formation due to the collisions between falling ice particles and droplets. In this study, we mimic this riming process. Contrary to earlier experiments, we found no efficient ice multiplication, which fundamentally questions the importance of the rime-splintering mechanism.
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.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
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.
Yiwei Gong, Feng Jiang, Yanxia Li, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 167–184, https://doi.org/10.5194/acp-24-167-2024, https://doi.org/10.5194/acp-24-167-2024, 2024
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This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
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.
Mohit Singh, Stephanie Helen Jones, Alexei Kiselev, Denis Duft, and Thomas Leisner
Atmos. Meas. Tech., 16, 5205–5215, https://doi.org/10.5194/amt-16-5205-2023, https://doi.org/10.5194/amt-16-5205-2023, 2023
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We introduce a novel method for simultaneous measurement of the viscosity and surface tension of metastable liquids. Our approach is based on the phase analysis of excited shape oscillations in levitated droplets. It is applicable to a wide range of atmospheric conditions and can monitor changes in real time. The technique holds great promise for investigating the effect of atmospheric processing on the viscosity and surface tension of solution droplets in equilibrium with water vapour.
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.
Jonas Elm, Aladár Czitrovszky, Andreas Held, Annele Virtanen, Astrid Kiendler-Scharr, Benjamin J. Murray, Daniel McCluskey, Daniele Contini, David Broday, Eirini Goudeli, Hilkka Timonen, Joan Rosell-Llompart, Jose L. Castillo, Evangelia Diapouli, Mar Viana, Maria E. Messing, Markku Kulmala, Naděžda Zíková, and Sebastian H. Schmitt
Aerosol Research, 1, 13–16, https://doi.org/10.5194/ar-1-13-2023, https://doi.org/10.5194/ar-1-13-2023, 2023
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.
Robert Wagner, Alexander D. James, Victoria L. Frankland, Ottmar Möhler, Benjamin J. Murray, John M. C. Plane, Harald Saathoff, Ralf Weigel, and Martin Schnaiter
Atmos. Chem. Phys., 23, 6789–6811, https://doi.org/10.5194/acp-23-6789-2023, https://doi.org/10.5194/acp-23-6789-2023, 2023
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Polar stratospheric clouds (PSCs) play an important role in the depletion of stratospheric ozone. They can consist of different chemical species, including crystalline nitric acid hydrates. We found that mineral dust or meteoric ablation material can efficiently catalyse the formation of a specific phase of nitric acid dihydrate crystals. We determined predominant particle shapes and infrared optical properties of these crystals, which are important inputs for remote sensing detection of PSCs.
Kara D. Lamb, Jerry Y. Harrington, Benjamin W. Clouser, Elisabeth J. Moyer, Laszlo Sarkozy, Volker Ebert, Ottmar Möhler, and Harald Saathoff
Atmos. Chem. Phys., 23, 6043–6064, https://doi.org/10.5194/acp-23-6043-2023, https://doi.org/10.5194/acp-23-6043-2023, 2023
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This study investigates how ice grows directly from vapor in cirrus clouds by comparing observations of populations of ice crystals growing in a cloud chamber against models developed in the context of single-crystal laboratory studies. We demonstrate that previous discrepancies between different experimental measurements do not necessarily point to different physical interpretations but are rather due to assumptions that were made in terms of how experiments were modeled in previous studies.
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.
Zijun Li, Angela Buchholz, Luis M. F. Barreira, Arttu Ylisirniö, Liqing Hao, Iida Pullinen, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 23, 203–220, https://doi.org/10.5194/acp-23-203-2023, https://doi.org/10.5194/acp-23-203-2023, 2023
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Interaction between NOx and biogenic emissions can be important in suburban areas. Our study showed that the addition of NOx during α-pinene SOA formation produced considerable amounts of organic nitrates and affected the composition of non-nitrated organic compounds. The compositional difference consequently altered the primary type of aqueous-phase processes during the isothermal particle evaporation.
Feng Jiang, Junwei Song, Jonas Bauer, Linyu Gao, Magdalena Vallon, Reiner Gebhardt, Thomas Leisner, Stefan Norra, and Harald Saathoff
Atmos. Chem. Phys., 22, 14971–14986, https://doi.org/10.5194/acp-22-14971-2022, https://doi.org/10.5194/acp-22-14971-2022, 2022
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We studied brown carbon aerosol during typical summer and winter periods in downtown Karlsruhe in southwestern Germany. The chromophore and chemical composition of brown carbon was determined by excitation–emission spectroscopy and mass spectrometry. The chromophore types and sources were substantially different in winter and summer. Humic-like chromophores of different degrees of oxidation dominated and were associated with molecules of different molecular weight and nitrogen content.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466, https://doi.org/10.5194/acp-22-13449-2022, https://doi.org/10.5194/acp-22-13449-2022, 2022
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Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
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.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Silvia M. Calderón, Juha Tonttila, Angela Buchholz, Jorma Joutsensaari, Mika Komppula, Ari Leskinen, Liqing Hao, Dmitri Moisseev, Iida Pullinen, Petri Tiitta, Jian Xu, Annele Virtanen, Harri Kokkola, and Sami Romakkaniemi
Atmos. Chem. Phys., 22, 12417–12441, https://doi.org/10.5194/acp-22-12417-2022, https://doi.org/10.5194/acp-22-12417-2022, 2022
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The spatial and temporal restrictions of observations and oversimplified aerosol representation in large eddy simulations (LES) limit our understanding of aerosol–stratocumulus interactions. In this closure study of in situ and remote sensing observations and outputs from UCLALES–SALSA, we have assessed the role of convective overturning and aerosol effects in two cloud events observed at the Puijo SMEAR IV station, Finland, a diurnal-high aerosol case and a nocturnal-low aerosol case.
Sini Isokääntä, Paul Kim, Santtu Mikkonen, Thomas Kühn, Harri Kokkola, Taina Yli-Juuti, Liine Heikkinen, Krista Luoma, Tuukka Petäjä, Zak Kipling, Daniel Partridge, and Annele Virtanen
Atmos. Chem. Phys., 22, 11823–11843, https://doi.org/10.5194/acp-22-11823-2022, https://doi.org/10.5194/acp-22-11823-2022, 2022
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This research employs air mass history analysis and observations to study how clouds and precipitation affect atmospheric aerosols during transport to a boreal forest site. The mass concentrations of studied chemical species showed exponential decrease as a function of accumulated rain along the air mass route. Our analysis revealed in-cloud sulfate formation, while no major changes in organic mass were seen. Most of the in-cloud-formed sulfate could be assigned to particle sizes above 200 nm.
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.
Fritz Waitz, Martin Schnaiter, Thomas Leisner, and Emma Järvinen
Atmos. Chem. Phys., 22, 7087–7103, https://doi.org/10.5194/acp-22-7087-2022, https://doi.org/10.5194/acp-22-7087-2022, 2022
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Riming, i.e., the accretion of small droplets on the surface of ice particles via collision, is one of the major uncertainties in model prediction of mixed-phase clouds. We discuss the occurrence (up to 50% of particles) and aging of rimed ice particles and show correlations of the occurrence and the degree of riming with ambient meteorological parameters using data gathered by the Particle Habit Imaging and Polar Scattering (PHIPS) probe during three airborne in situ field campaigns.
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.
Zoé Brasseur, Dimitri Castarède, Erik S. Thomson, Michael P. Adams, Saskia Drossaart van Dusseldorp, Paavo Heikkilä, Kimmo Korhonen, Janne Lampilahti, Mikhail Paramonov, Julia Schneider, Franziska Vogel, Yusheng Wu, Jonathan P. D. Abbatt, Nina S. Atanasova, Dennis H. Bamford, Barbara Bertozzi, Matthew Boyer, David Brus, Martin I. Daily, Romy Fösig, Ellen Gute, Alexander D. Harrison, Paula Hietala, Kristina Höhler, Zamin A. Kanji, Jorma Keskinen, Larissa Lacher, Markus Lampimäki, Janne Levula, Antti Manninen, Jens Nadolny, Maija Peltola, Grace C. E. Porter, Pyry Poutanen, Ulrike Proske, Tobias Schorr, Nsikanabasi Silas Umo, János Stenszky, Annele Virtanen, Dmitri Moisseev, Markku Kulmala, Benjamin J. Murray, Tuukka Petäjä, Ottmar Möhler, and Jonathan Duplissy
Atmos. Chem. Phys., 22, 5117–5145, https://doi.org/10.5194/acp-22-5117-2022, https://doi.org/10.5194/acp-22-5117-2022, 2022
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The present measurement report introduces the ice nucleation campaign organized in Hyytiälä, Finland, in 2018 (HyICE-2018). We provide an overview of the campaign settings, and we describe the measurement infrastructure and operating procedures used. In addition, we use results from ice nucleation instrument inter-comparison to show that the suite of these instruments deployed during the campaign reports consistent results.
Magdalena Vallon, Linyu Gao, Feng Jiang, Bianca Krumm, Jens Nadolny, Junwei Song, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 15, 1795–1810, https://doi.org/10.5194/amt-15-1795-2022, https://doi.org/10.5194/amt-15-1795-2022, 2022
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A LED-based light source has been constructed for the AIDA simulation chamber at the Karlsruhe Institute of Technology. It allows aerosol formation and ageing studies under atmospherically relevant illumination intensities and spectral characteristics at temperatures from –90 °C to 30 °C with the possibility of changing the photon flux and irradiation spectrum at any point. The first results of photolysis experiments with 2,3-pentanedione, iron oxalate and a brown carbon component are shown.
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.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631, https://doi.org/10.5194/acp-22-1615-2022, https://doi.org/10.5194/acp-22-1615-2022, 2022
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We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
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.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208, https://doi.org/10.5194/acp-22-1195-2022, https://doi.org/10.5194/acp-22-1195-2022, 2022
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Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Zijun Li, Angela Buchholz, Arttu Ylisirniö, Luis Barreira, Liqing Hao, Siegfried Schobesberger, Taina Yli-Juuti, and Annele Virtanen
Atmos. Chem. Phys., 21, 18283–18302, https://doi.org/10.5194/acp-21-18283-2021, https://doi.org/10.5194/acp-21-18283-2021, 2021
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We compared the evolution of two types of secondary organic aerosol (SOA) particles during isothermal evaporation. The sesquiterpene SOA particles demonstrated higher resilience to evaporation than α-pinene SOA particles generated under comparable conditions. In-depth analysis showed that under high-relative-humidity conditions, particulate water drove the evolution of particulate constituents by reducing the particle viscosity and initiating chemical aqueous-phase processes.
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.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Ulrich Platt, Thomas Wagner, Jonas Kuhn, and Thomas Leisner
Atmos. Meas. Tech., 14, 6867–6883, https://doi.org/10.5194/amt-14-6867-2021, https://doi.org/10.5194/amt-14-6867-2021, 2021
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Absorption spectroscopy of scattered sunlight is extremely useful for the analysis of atmospheric trace gas distributions. A central parameter for the achievable sensitivity of spectroscopic instruments is the light throughput, which can be enhanced in a number of ways. We present new ideas and considerations of how instruments could be optimized. Particular emphasis is on arrays of massively parallel instruments. Such arrays can reduce the size and weight of instruments by orders of magnitude.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Julia Schneider, Kristina Höhler, Robert Wagner, Harald Saathoff, Martin Schnaiter, Tobias Schorr, Isabelle Steinke, Stefan Benz, Manuel Baumgartner, Christian Rolf, Martina Krämer, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14403–14425, https://doi.org/10.5194/acp-21-14403-2021, https://doi.org/10.5194/acp-21-14403-2021, 2021
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Homogeneous freezing is a relevant mechanism for the formation of cirrus clouds in the upper troposphere. Based on an extensive set of homogeneous freezing experiments at the AIDA chamber with aqueous sulfuric acid aerosol, we provide a new fit line for homogeneous freezing onset conditions of sulfuric acid aerosol focusing on cirrus temperatures. In the atmosphere, homogeneous freezing thresholds have important implications on the cirrus cloud occurrence and related cloud radiative effects.
Naruki Hiranuma, Brent W. Auvermann, Franco Belosi, Jack Bush, Kimberly M. Cory, Dimitrios G. Georgakopoulos, Kristina Höhler, Yidi Hou, Larissa Lacher, Harald Saathoff, Gianni Santachiara, Xiaoli Shen, Isabelle Steinke, Romy Ullrich, Nsikanabasi S. Umo, Hemanth S. K. Vepuri, Franziska Vogel, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14215–14234, https://doi.org/10.5194/acp-21-14215-2021, https://doi.org/10.5194/acp-21-14215-2021, 2021
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We present laboratory and field studies showing that an open-lot livestock facility is a substantial source of atmospheric ice-nucleating particles (INPs). The ambient concentration of INPs from livestock facilities in Texas is very high. It is up to several thousand INPs per liter below –20 °C and may impact regional aerosol–cloud interactions. About 50% of feedlot INPs were supermicron in diameter. No notable amount of known ice-nucleating microorganisms was found in our feedlot samples.
Robert Wagner, Luisa Ickes, Allan K. Bertram, Nora Els, Elena Gorokhova, Ottmar Möhler, Benjamin J. Murray, Nsikanabasi Silas Umo, and Matthew E. Salter
Atmos. Chem. Phys., 21, 13903–13930, https://doi.org/10.5194/acp-21-13903-2021, https://doi.org/10.5194/acp-21-13903-2021, 2021
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Sea spray aerosol particles are a mixture of inorganic salts and organic matter from phytoplankton organisms. At low temperatures in the upper troposphere, both inorganic and organic constituents can induce the formation of ice crystals and thereby impact cloud properties and climate. In this study, we performed experiments in a cloud simulation chamber with particles produced from Arctic seawater samples to quantify the relative contribution of inorganic and organic species in ice formation.
Alexei A. Kiselev, Alice Keinert, Tilia Gaedeke, Thomas Leisner, Christoph Sutter, Elena Petrishcheva, and Rainer Abart
Atmos. Chem. Phys., 21, 11801–11814, https://doi.org/10.5194/acp-21-11801-2021, https://doi.org/10.5194/acp-21-11801-2021, 2021
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Alkali feldspar is the most abundant mineral in the Earth's crust and is often present in mineral dust aerosols that are responsible for the formation of rain and snow in clouds. However, the cloud droplets containing pure potassium-rich feldspar would not freeze unless cooled down to a very low temperature. Here we show that partly replacing potassium with sodium would induce fracturing of feldspar, exposing a crystalline surface that could initiate freezing at higher temperature.
Hengheng Zhang, Frank Wagner, Harald Saathoff, Heike Vogel, Gholam Ali Hoshyaripour, Vanessa Bachmann, Jochen Förstner, and Thomas Leisner
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-193, https://doi.org/10.5194/amt-2021-193, 2021
Revised manuscript not accepted
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The evolution and the properties of Saharan dust plume were characterized by LIDARs, a sun photometer, and a regional transport model. Comparison between LIDAR measurements, sun photometer and ICON-ART predictions shows a good agreement for dust arrival time, dust layer height, and dust structure but also that the model overestimates the backscatter coefficients by a factor of (2.2 ± 0.16) and underestimate aerosol optical depth by a factor of (1.5 ± 0.11).
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
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Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
Barbara Bertozzi, Robert Wagner, Junwei Song, Kristina Höhler, Joschka Pfeifer, Harald Saathoff, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 10779–10798, https://doi.org/10.5194/acp-21-10779-2021, https://doi.org/10.5194/acp-21-10779-2021, 2021
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Internally mixed particles composed of sulfate and organics are among the most abundant aerosol types. Their ice nucleation (IN) ability influences the formation of cirrus and, thus, the climate. We show that the presence of a thin organic coating suppresses the heterogeneous IN ability of crystalline ammonium sulfate particles. However, the IN ability of the same particle can substantially change if subjected to atmospheric processing, mainly due to differences in the resulting morphology.
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.
Fritz Waitz, Martin Schnaiter, Thomas Leisner, and Emma Järvinen
Atmos. Meas. Tech., 14, 3049–3070, https://doi.org/10.5194/amt-14-3049-2021, https://doi.org/10.5194/amt-14-3049-2021, 2021
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A major challenge in the observations of mixed-phase clouds remains the phase discrimination and sizing of cloud droplets and ice crystals, especially for particles with diameters smaller than 0.1 mm. Here, we present a new method to derive the phase and size of single cloud particles using their angular-light-scattering information. Comparisons with other in situ instruments in three case studies show good agreement.
Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys., 21, 3899–3918, https://doi.org/10.5194/acp-21-3899-2021, https://doi.org/10.5194/acp-21-3899-2021, 2021
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By triggering the formation of ice crystals, ice-nucleating particles (INP) strongly influence cloud formation. Continuous, long-term measurements are needed to characterize the atmospheric INP variability. Here, a first long-term time series of INP spectra measured in the boreal forest for more than 1 year is presented, showing a clear seasonal cycle. It is shown that the seasonal dependency of INP concentrations and prevalent INP types is driven by the abundance of biogenic aerosol.
Robert Wagner, Baptiste Testa, Michael Höpfner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, Jörn Ungermann, and Thomas Leisner
Atmos. Meas. Tech., 14, 1977–1991, https://doi.org/10.5194/amt-14-1977-2021, https://doi.org/10.5194/amt-14-1977-2021, 2021
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During the Asian summer monsoon period, air pollutants are transported from layers near the ground to high altitudes of 13 to 18 km in the atmosphere. Infrared measurements have shown that particles composed of solid ammonium nitrate are a major part of these pollutants. To enable the quantitative analysis of the infrared spectra, we have determined for the first time accurate optical constants of ammonium nitrate for the low-temperature conditions of the upper atmosphere.
Antti Ruuskanen, Sami Romakkaniemi, Harri Kokkola, Antti Arola, Santtu Mikkonen, Harri Portin, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, and Ari Leskinen
Atmos. Chem. Phys., 21, 1683–1695, https://doi.org/10.5194/acp-21-1683-2021, https://doi.org/10.5194/acp-21-1683-2021, 2021
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The study focuses mainly on cloud-scavenging efficiency of absorbing particulate matter (mainly black carbon) but additionally covers cloud-scavenging efficiency of scattering particles and statistics of cloud condensation nuclei. The main findings give insight into how black carbon is distributed in different particle sizes and the sensitivity to cloud scavenged. The main findings are useful for large-scale modelling for evaluating cloud scavenging.
Michael Krayer, Agathe Chouippe, Markus Uhlmann, Jan Dušek, and Thomas Leisner
Atmos. Chem. Phys., 21, 561–575, https://doi.org/10.5194/acp-21-561-2021, https://doi.org/10.5194/acp-21-561-2021, 2021
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We address the phenomenon of ice enhancement in the vicinity of warm hydrometeors using highly accurate flow simulation techniques. It is found that the transiently supersaturated zones induced by the hydrometeor's wake are by far larger than what has been previously estimated. The ice enhancement is quantified on the micro- and macroscale, and its relevance is discussed. The results provided may contribute to a (currently unavailable) parametrization of the phenomenon.
Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367, https://doi.org/10.5194/amt-14-355-2021, https://doi.org/10.5194/amt-14-355-2021, 2021
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FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
André Welti, Kimmo Korhonen, Pasi Miettinen, Ana A. Piedehierro, Yrjö Viisanen, Annele Virtanen, and Ari Laaksonen
Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, https://doi.org/10.5194/amt-13-7059-2020, 2020
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We describe a modification of the SPectrometer for Ice Nuclei (SPIN) chamber to study ice nucleation at low temperatures, relevant for ice formation in cirrus clouds. Validation experiments of homogeneous freezing of aqueous ammonium sulfate droplets and heterogeneous ice nucleation on silver iodide particles are included to demonstrate the advantages of the modified SPIN chamber for the investigation of ice nucleation in the extended temperature range.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
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.
Alexei Korolev and Thomas Leisner
Atmos. Chem. Phys., 20, 11767–11797, https://doi.org/10.5194/acp-20-11767-2020, https://doi.org/10.5194/acp-20-11767-2020, 2020
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Secondary ice production (SIP) plays a key role in the formation of ice particles in tropospheric clouds. This work presents a critical review of the laboratory studies related to secondary ice production. It aims to identify gaps in our knowledge of SIP as well as to stimulate further laboratory studies focused on obtaining a quantitative description of efficiencies for each SIP mechanism.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
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In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
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.
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.
Sini Isokääntä, Eetu Kari, Angela Buchholz, Liqing Hao, Siegfried Schobesberger, Annele Virtanen, and Santtu Mikkonen
Atmos. Meas. Tech., 13, 2995–3022, https://doi.org/10.5194/amt-13-2995-2020, https://doi.org/10.5194/amt-13-2995-2020, 2020
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Online mass spectrometry produces large amounts of data. These data can be interpreted with statistical methods, enabling scientists to more easily understand the underlying processes. We compared these techniques on car exhaust measurements. We show differences and similarities between the methods and give recommendations on applicability of the methods on certain types of data. We show that applying multiple methods leads to more robust results, thus increasing reliability of the findings.
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.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Ricardo Luis Carvalho, Vilhelm Malmborg, Axel Eriksson, Christoffer Boman, Joakim Pagels, Birgitta Svenningsson, Mika Komppula, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 20, 4951–4968, https://doi.org/10.5194/acp-20-4951-2020, https://doi.org/10.5194/acp-20-4951-2020, 2020
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Ice-nucleating abilities of particulate emissions from solid-fuel-burning cookstoves were studied using a portable ice nuclei counter in an extensive laboratory experiment campaign. We found that even small changes in combustion conditions may affect the ice-nucleating ability of the emissions significantly. Also six different physico-chemical properties of the emissions were studied, but no clear correlation to their ice-nucleating ability was found.
Benjamin W. Clouser, Kara D. Lamb, Laszlo C. Sarkozy, Jan Habig, Volker Ebert, Harald Saathoff, Ottmar Möhler, and Elisabeth J. Moyer
Atmos. Chem. Phys., 20, 1089–1103, https://doi.org/10.5194/acp-20-1089-2020, https://doi.org/10.5194/acp-20-1089-2020, 2020
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Previous measurements of water vapor in the upper troposphere and lower stratosphere (UT/LS) have shown unexpectedly high concentrations of water vapor in ice clouds, which may be due to an incomplete understanding of the structure of ice and the behavior of ice growth in this part of the atmosphere. Water vapor measurements during the 2013 IsoCloud campaign at the AIDA cloud chamber show no evidence of this
anomalous supersaturationin conditions similar to the real atmosphere.
Eetu Kari, Liqing Hao, Arttu Ylisirniö, Angela Buchholz, Ari Leskinen, Pasi Yli-Pirilä, Ilpo Nuutinen, Kari Kuuspalo, Jorma Jokiniemi, Celia L. Faiola, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 15651–15671, https://doi.org/10.5194/acp-19-15651-2019, https://doi.org/10.5194/acp-19-15651-2019, 2019
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We present, for the first time, the dual effect of GDI-vehicle exhaust on α-pinene SOA mass yield suppression. The first effect is a well-known NOx effect, but the second effect is more complex. Our results imply that this second effect is related to change of reaction pathways of α-pinene in the presence of GDI exhaust. The presence of vehicle exhaust caused more than 50 % suppression in α-pinene SOA mass yield compared to the α-pinene SOA mass yield measured in the absence of GDI emissions.
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.
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.
Tasha Aylett, James S. A. Brooke, Alexander D. James, Mario Nachbar, Denis Duft, Thomas Leisner, and John M. C. Plane
Atmos. Chem. Phys., 19, 12767–12777, https://doi.org/10.5194/acp-19-12767-2019, https://doi.org/10.5194/acp-19-12767-2019, 2019
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Interplanetary dust particles entering the Earth's atmosphere often melt and evaporate, injecting metals such as iron and magnesium into the atmosphere between 80 and 105 km. These metals become oxidized and then coagulate into small particles a few nanometres is size, known as meteoric smoke. In this study, iron oxide smoke particles were created in the laboratory, and their composition and optical properties were determined in order to understand satellite measurements.
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.
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.
Martin Schnaiter, Claudia Linke, Inas Ibrahim, Alexei Kiselev, Fritz Waitz, Thomas Leisner, Stefan Norra, and Till Rehm
Atmos. Chem. Phys., 19, 10829–10844, https://doi.org/10.5194/acp-19-10829-2019, https://doi.org/10.5194/acp-19-10829-2019, 2019
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When combustion particles are deposited to the ground, they darken Earth's snow and ice surfaces by even tiny quantities. This darkening reduces the back reflection of sunlight and induces an additional climate warming. Particles from fresh snow samples were investigated according to their light absorption strength. Enhanced absorption was found in the snow that cannot fully be attributed to combustion particles. Dust and biogenic matter are likely the cause of this additional snow darkening.
Nsikanabasi Silas Umo, Robert Wagner, Romy Ullrich, Alexei Kiselev, Harald Saathoff, Peter G. Weidler, Daniel J. Cziczo, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 19, 8783–8800, https://doi.org/10.5194/acp-19-8783-2019, https://doi.org/10.5194/acp-19-8783-2019, 2019
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Annually, over 600 Tg of coal fly ash (CFA) is produced; a significant proportion of this amount is injected into the atmosphere, which could significantly contribute to heterogeneous ice formation in clouds. This study presents an improved understanding of CFA particles' behaviour in forming ice in clouds, especially when exposed to lower temperatures before being re-circulated in the upper troposphere or entrained into the lower troposphere.
Zamin A. Kanji, Ryan C. Sullivan, Monika Niemand, Paul J. DeMott, Anthony J. Prenni, Cédric Chou, Harald Saathoff, and Ottmar Möhler
Atmos. Chem. Phys., 19, 5091–5110, https://doi.org/10.5194/acp-19-5091-2019, https://doi.org/10.5194/acp-19-5091-2019, 2019
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The ice nucleation ability of two natural desert dusts coated with a proxy of secondary organic aerosol is presented for temperatures and relative humidity conditions relevant for mixed-phase clouds. We find that at the tested conditions, there is no effect on the ice nucleation ability of the particles due to the organic coating. Furthermore, the two dust samples do not show variability within measurement uncertainty. Particle size and surface area may play a role in any difference observed.
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.
Mario Nachbar, Henrike Wilms, Denis Duft, Tasha Aylett, Kensei Kitajima, Takuya Majima, John M. C. Plane, Markus Rapp, and Thomas Leisner
Atmos. Chem. Phys., 19, 4311–4322, https://doi.org/10.5194/acp-19-4311-2019, https://doi.org/10.5194/acp-19-4311-2019, 2019
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Polar mesospheric clouds (PMC) are water ice clouds forming on nanoparticles in the polar summer mesopause. We investigate the impact of solar radiation on PMC formation in the laboratory. We show that Mie theory calculations combined with an equilibrium temperature model presented in this work predict the warming of the particles very well. Using this model we demonstrate that the impact of solar radiation on ice particle formation is significantly lower than previously assumed.
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.
Denis Duft, Mario Nachbar, and Thomas Leisner
Atmos. Chem. Phys., 19, 2871–2879, https://doi.org/10.5194/acp-19-2871-2019, https://doi.org/10.5194/acp-19-2871-2019, 2019
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How ice particles form in polar mesospheric clouds is still a challenging question. We measured the water adsorption and onset conditions for ice growth on meteoric smoke analogue particles in the laboratory. We find that the particles activate by growth of amorphous ice and at much warmer conditions than previously assumed, affirming meteoric smoke as likely seeds in mesospheric ice clouds. We propose an ice-activation model and show that the particle charge does not play a significant role.
Liqing Hao, Olga Garmash, Mikael Ehn, Pasi Miettinen, Paola Massoli, Santtu Mikkonen, Tuija Jokinen, Pontus Roldin, Pasi Aalto, Taina Yli-Juuti, Jorma Joutsensaari, Tuukka Petäjä, Markku Kulmala, Kari E. J. Lehtinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 18, 17705–17716, https://doi.org/10.5194/acp-18-17705-2018, https://doi.org/10.5194/acp-18-17705-2018, 2018
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An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the nighttime, the increase in organic aerosol mass correlated well with the increase in condensed highly oxygenated organic molecules' mass.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Emma Järvinen, Olivier Jourdan, David Neubauer, Bin Yao, Chao Liu, Meinrat O. Andreae, Ulrike Lohmann, Manfred Wendisch, Greg M. McFarquhar, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 18, 15767–15781, https://doi.org/10.5194/acp-18-15767-2018, https://doi.org/10.5194/acp-18-15767-2018, 2018
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Using light diffraction it is possible to detect microscopic features within ice particles that have not yet been fully characterized. Here, this technique was applied in airborne measurements, where it was found that majority of atmospheric ice particles have features that significantly change the way ice particles interact with solar light. The microscopic features make ice-containing clouds more reflective than previously thought, which could have consequences for predicting our climate.
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.
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.
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.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
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.
Wiebke Frey, Dawei Hu, James Dorsey, M. Rami Alfarra, Aki Pajunoja, Annele Virtanen, Paul Connolly, and Gordon McFiggans
Atmos. Chem. Phys., 18, 9393–9409, https://doi.org/10.5194/acp-18-9393-2018, https://doi.org/10.5194/acp-18-9393-2018, 2018
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The coupled system of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber was used to study the ice-forming abilities of secondary
organic aerosol particles under mixed-phase cloud conditions. Given the vast abundance of secondary organic particles in the atmosphere, they
might present an important contribution to ice-nucleating particles. However, we find that in the studied temperature range (20 to 28 °C)
the secondary organic particles do not nucleate ice particles.
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.
Mario Nachbar, Denis Duft, and Thomas Leisner
Atmos. Chem. Phys., 18, 3419–3431, https://doi.org/10.5194/acp-18-3419-2018, https://doi.org/10.5194/acp-18-3419-2018, 2018
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The crystallization process of amorphous ice below 160 K forms nano-crystalline ice. We report high-quality vapor pressure measurements over ice crystallized from amorphous ice below 160 K. We show that the vapor pressure is increased by more than 100 % compared to bulk crystalline ice and that amorphous ice always forms first, followed by the crystallization of nano-crystalline ice. Our findings are relevant for cold ice clouds in the atmospheres of planets, e.g., Earth and Mars.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Martin Schnaiter, Emma Järvinen, Ahmed Abdelmonem, and Thomas Leisner
Atmos. Meas. Tech., 11, 341–357, https://doi.org/10.5194/amt-11-341-2018, https://doi.org/10.5194/amt-11-341-2018, 2018
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PHIPS-HALO is a novel aircraft instrument for cloud research. It combines microscopic imaging of single cloud particles with the measurement of their spacial light scattering properties. The knowledge of how atmospheric ice particles in clouds scatter visible light is important for improving future climate models.
Juan Hong, Mikko Äijälä, Silja A. K. Häme, Liqing Hao, Jonathan Duplissy, Liine M. Heikkinen, Wei Nie, Jyri Mikkilä, Markku Kulmala, Nønne L. Prisle, Annele Virtanen, Mikael Ehn, Pauli Paasonen, Douglas R. Worsnop, Ilona Riipinen, Tuukka Petäjä, and Veli-Matti Kerminen
Atmos. Chem. Phys., 17, 4387–4399, https://doi.org/10.5194/acp-17-4387-2017, https://doi.org/10.5194/acp-17-4387-2017, 2017
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Estimates of volatility of secondary organic aerosols was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model and by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer data. About 16 % of the variation can be explained by the linear regression between the results from these two methods.
Wei Nie, Juan Hong, Silja A. K. Häme, Aijun Ding, Yugen Li, Chao Yan, Liqing Hao, Jyri Mikkilä, Longfei Zheng, Yuning Xie, Caijun Zhu, Zheng Xu, Xuguang Chi, Xin Huang, Yang Zhou, Peng Lin, Annele Virtanen, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, Jianzhen Yu, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 3659–3672, https://doi.org/10.5194/acp-17-3659-2017, https://doi.org/10.5194/acp-17-3659-2017, 2017
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HULIS are demonstrated to be important low-volatility, or even extremely low volatility, compounds in the organic aerosol phase. This sheds new light on the connection between atmospheric HULIS and ELVOCs. The interaction between HULIS and ammonium sulfate was found to decrease the volatility of the HULIS part in HULIS-AS mixed samples, indicating multiphase processes have the potential to lower the volatility of organic compounds in the aerosol phase.
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.
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
Claudia Linke, Inas Ibrahim, Nina Schleicher, Regina Hitzenberger, Meinrat O. Andreae, Thomas Leisner, and Martin Schnaiter
Atmos. Meas. Tech., 9, 5331–5346, https://doi.org/10.5194/amt-9-5331-2016, https://doi.org/10.5194/amt-9-5331-2016, 2016
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Various carbonaceous materials are present in the atmosphere. Besides gaseous organic compounds, carbonaceous particles like soot are emitted into the air from traffic sources, residential wood combustion, or wildfires. Variable chemical compositions of such materials, which often result from incomplete combustion processes, show differences in the absorption behavior at visible wavelengths. Our instrument is able to measure the absorption at three visible wavelengths.
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.
Andreas Peckhaus, Alexei Kiselev, Thibault Hiron, Martin Ebert, and Thomas Leisner
Atmos. Chem. Phys., 16, 11477–11496, https://doi.org/10.5194/acp-16-11477-2016, https://doi.org/10.5194/acp-16-11477-2016, 2016
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The precipitation in midlatitude clouds proceeds predominantly via nucleation of ice in the supercooled droplets containing foreign inclusions, like feldspar mineral dust, that have been recently identified as one of the most active ice nucleating agents in the atmosphere. We have built an apparatus to observe the freezing of feldspar immersed in up to 1500 identical droplets simultaneously. With this setup we investigated four feldspar samples and show that it can induce freezing at −5 °C.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Naruki Hiranuma, Ottmar Möhler, Gourihar Kulkarni, Martin Schnaiter, Steffen Vogt, Paul Vochezer, Emma Järvinen, Robert Wagner, David M. Bell, Jacqueline Wilson, Alla Zelenyuk, and Daniel J. Cziczo
Atmos. Meas. Tech., 9, 3817–3836, https://doi.org/10.5194/amt-9-3817-2016, https://doi.org/10.5194/amt-9-3817-2016, 2016
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A new pumped counterflow virtual impactor (PCVI) called the ice-selecting PCVI (IS-PCVI) has been developed to collect ice crystal residuals for investigating physico-chemical properties of ice-nucleating particles. The results show that the ice crystals of volume-equivalent diameter ~ 10 to 30 µm can be efficiently separated from the supercooled droplets and interstitial particles. The IS-PCVI is efficient when the counterflow-to-input flow ratio is within 0.09 to 0.18.
Olli Väisänen, Antti Ruuskanen, Arttu Ylisirniö, Pasi Miettinen, Harri Portin, Liqing Hao, Ari Leskinen, Mika Komppula, Sami Romakkaniemi, Kari E. J. Lehtinen, and Annele Virtanen
Atmos. Chem. Phys., 16, 10385–10398, https://doi.org/10.5194/acp-16-10385-2016, https://doi.org/10.5194/acp-16-10385-2016, 2016
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In-cloud measurements of aerosol hygroscopicity and cloud droplet activation were conducted in Kuopio, Finland. According to the observations, the less hygroscopic accumulation mode particles were present in the non-activated aerosol, whereas the more hygroscopic particles were scavenged into cloud droplets. The results illustrate the sensitivity of cloud droplet formation to varying chemical composition and highlight the need for proper treatment of anthropogenic aerosols in CCN predictions.
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.
Ahmed Abdelmonem, Emma Järvinen, Denis Duft, Edwin Hirst, Steffen Vogt, Thomas Leisner, and Martin Schnaiter
Atmos. Meas. Tech., 9, 3131–3144, https://doi.org/10.5194/amt-9-3131-2016, https://doi.org/10.5194/amt-9-3131-2016, 2016
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The properties of ice crystals present in mixed-phase and ice clouds influence the radiation properties, precipitation occurrence and lifetime of these clouds. It is necessary to investigate the optical and microphysical properties of cloud particles particularly in situ, and to get correlation between these properties. To this end we have developed PHIPS-HALO to measure the optical properties and the corresponding microphysical parameters of individual cloud particles simultaneously.
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.
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.
Martin Schnaiter, Emma Järvinen, Paul Vochezer, Ahmed Abdelmonem, Robert Wagner, Olivier Jourdan, Guillaume Mioche, Valery N. Shcherbakov, Carl G. Schmitt, Ugo Tricoli, Zbigniew Ulanowski, and Andrew J. Heymsfield
Atmos. Chem. Phys., 16, 5091–5110, https://doi.org/10.5194/acp-16-5091-2016, https://doi.org/10.5194/acp-16-5091-2016, 2016
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.
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
Robert Wagner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, and Isabelle Steinke
Atmos. Chem. Phys., 16, 2025–2042, https://doi.org/10.5194/acp-16-2025-2016, https://doi.org/10.5194/acp-16-2025-2016, 2016
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We have investigated the enhancement of the ice nucleation ability of well-known and abundant ice nucleating particles like dust grains due to pre-activation. Temporary exposure to a low temperature (228 K) provokes that pores and surface cracks of the particles are filled with ice, which makes them better nuclei for the growth of macroscopic ice crystals at high temperatures (245–260 K).
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.
P. Vochezer, E. Järvinen, R. Wagner, P. Kupiszewski, T. Leisner, and M. Schnaiter
Atmos. Meas. Tech., 9, 159–177, https://doi.org/10.5194/amt-9-159-2016, https://doi.org/10.5194/amt-9-159-2016, 2016
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To study clouds constituting of liquid droplets as well as ice particles we used the latest versions of the Small Ice Detector which record high resolution scattering patterns of individual small cloud particles. In the case of a droplet its precise size is obtained and for ice particles its shape is deduced from the scattering pattern.We present results from artificial clouds at the AIDA cloud chamber and natural clouds probed at a mountain top station as well as from an aircraft in the arctic.
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.
A. M. K. Hansen, J. Hong, T. Raatikainen, K. Kristensen, A. Ylisirniö, A. Virtanen, T. Petäjä, M. Glasius, and N. L. Prisle
Atmos. Chem. Phys., 15, 14071–14089, https://doi.org/10.5194/acp-15-14071-2015, https://doi.org/10.5194/acp-15-14071-2015, 2015
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This paper presents the first study of the hygroscopic properties of limonene derived organosulfates (L-OS 250). The results showed that L-OS 250 particles are weakly hygroscopic and able to activate into cloud droplets. Particles of L-OS 250 mixed with ammonium sulfate were much more hygroscopic than expected from model parametrizations and the ZSR mixing rule, indicating that solubility and non-ideal droplet interactions could be important for the hygroscopic properties of the mixed particles.
J. Hong, J. Kim, T. Nieminen, J. Duplissy, M. Ehn, M. Äijälä, L. Q. Hao, W. Nie, N. Sarnela, N. L. Prisle, M. Kulmala, A. Virtanen, T. Petäjä, and V.-M. Kerminen
Atmos. Chem. Phys., 15, 11999–12009, https://doi.org/10.5194/acp-15-11999-2015, https://doi.org/10.5194/acp-15-11999-2015, 2015
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, F. Canonaco, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, H. Coe, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, E. Nemitz, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11291–11309, https://doi.org/10.5194/acp-15-11291-2015, https://doi.org/10.5194/acp-15-11291-2015, 2015
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Trace element measurements in three particle size ranges (PM10-2.5, PM2.5-1.0 and PM1.0-0.3) were performed with 2h time resolution at kerbside, urban background and rural sites during the ClearfLo winter 2012 campaign in London. The environment-dependent variability of emissions was characterized using the Multilinear Engine implementation of the positive matrix factorization model. A total of nine different factors were resolved from local, regional and natural origin.
A. Abdelmonem, J. Lützenkirchen, and T. Leisner
Atmos. Meas. Tech., 8, 3519–3526, https://doi.org/10.5194/amt-8-3519-2015, https://doi.org/10.5194/amt-8-3519-2015, 2015
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This manuscript belongs and is important to the environmental and atmospheric science, particularly cloud formation and cloud seeding, and presents a setup to apply Second Harmonic Generation spectroscopy to heterogeneous freezing research. We describe the setup and provide first results on temperature-dependent structural changes of water on the surfaces of two relevant atmospheric aerosol substances (sapphire and mica as poor and good ice nucleators, respectively).
J. Diab, T. Streibel, F. Cavalli, S. C. Lee, H. Saathoff, A. Mamakos, J. C. Chow, L.-W. A. Chen, J. G. Watson, O. Sippula, and R. Zimmermann
Atmos. Meas. Tech., 8, 3337–3353, https://doi.org/10.5194/amt-8-3337-2015, https://doi.org/10.5194/amt-8-3337-2015, 2015
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This paper depicts several fields of application of a new analytical method, which expands the well-established EC/OC method, which enables one to measure the carbon content (organic and elemental) of particulate aerosols. It was coupled to photo-ionization mass spectrometry to get structural information of the evolving carbonaceous species. Application fields such as smoke chamber-, ambient - and wood combustion particles were addressed, covering exemplary primary and secondary aerosol sources.
J. Meyer, C. Rolf, C. Schiller, S. Rohs, N. Spelten, A. Afchine, M. Zöger, N. Sitnikov, T. D. Thornberry, A. W. Rollins, Z. Bozóki, D. Tátrai, V. Ebert, B. Kühnreich, P. Mackrodt, O. Möhler, H. Saathoff, K. H. Rosenlof, and M. Krämer
Atmos. Chem. Phys., 15, 8521–8538, https://doi.org/10.5194/acp-15-8521-2015, https://doi.org/10.5194/acp-15-8521-2015, 2015
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
A. Leskinen, P. Yli-Pirilä, K. Kuuspalo, O. Sippula, P. Jalava, M.-R. Hirvonen, J. Jokiniemi, A. Virtanen, M. Komppula, and K. E. J. Lehtinen
Atmos. Meas. Tech., 8, 2267–2278, https://doi.org/10.5194/amt-8-2267-2015, https://doi.org/10.5194/amt-8-2267-2015, 2015
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A 29 m3 Teflon chamber was characterized and tested with oxidation experiments of toluene. Secondary organic aerosol yields of 12-42 % were obtained. These yields are comparable to those obtained in other laboratories.
M. Dalirian, H. Keskinen, L. Ahlm, A. Ylisirniö, S. Romakkaniemi, A. Laaksonen, A. Virtanen, and I. Riipinen
Atmos. Chem. Phys., 15, 3815–3829, https://doi.org/10.5194/acp-15-3815-2015, https://doi.org/10.5194/acp-15-3815-2015, 2015
I. Steinke, C. Hoose, O. Möhler, P. Connolly, and T. Leisner
Atmos. Chem. Phys., 15, 3703–3717, https://doi.org/10.5194/acp-15-3703-2015, https://doi.org/10.5194/acp-15-3703-2015, 2015
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Ice nucleation in clouds has a significant influence on the global radiative budget and the hydrological cycle. Several studies have investigated the ice formation in droplets and parameterizations have been developed in order to include immersion freezing in climate models. In contrast, there are fewer studies regarding the conversion of water vapor into ice (so-called deposition nucleation) which is the topic of this paper which investigates deposition nucleation by Arizona Test dust in detail
L. R. Crilley, W. J. Bloss, J. Yin, D. C. S. Beddows, R. M. Harrison, J. D. Allan, D. E. Young, M. Flynn, P. Williams, P. Zotter, A. S. H. Prevot, M. R. Heal, J. F. Barlow, C. H. Halios, J. D. Lee, S. Szidat, and C. Mohr
Atmos. Chem. Phys., 15, 3149–3171, https://doi.org/10.5194/acp-15-3149-2015, https://doi.org/10.5194/acp-15-3149-2015, 2015
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Wood is a renewable fuel but its combustion for residential heating releases a number of locally acting air pollutants, most notably particulate matter known to have adverse effects on human health. This paper used chemical tracers for wood smoke to estimate the contribution that burning wood makes to concentrations of airborne particles in the atmosphere of southern England and most particularly in London.
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, R. Dressler, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, S. C. Herndon, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, A. Detournay, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 2367–2386, https://doi.org/10.5194/acp-15-2367-2015, https://doi.org/10.5194/acp-15-2367-2015, 2015
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Ambient concentrations of trace elements with 2h time resolution were measured in three size ranges (PM10–2.5, PM2.5–1.0, PM1.0–0.3) at kerbside, urban background and rural sites in London during the ClearfLo (Clean Air for London) field campaign. Quantification of kerb and urban increments, and assessment of diurnal and weekly variability provided insight into sources governing urban air quality and the effects of urban micro-environments on human exposure.
L. Q. Hao, A. Kortelainen, S. Romakkaniemi, H. Portin, A. Jaatinen, A. Leskinen, M. Komppula, P. Miettinen, D. Sueper, A. Pajunoja, J. N. Smith, K. E. J. Lehtinen, D. R. Worsnop, A. Laaksonen, and A. Virtanen
Atmos. Chem. Phys., 14, 13483–13495, https://doi.org/10.5194/acp-14-13483-2014, https://doi.org/10.5194/acp-14-13483-2014, 2014
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Positive matrix factorization (PMF) was applied to the unified high-resolution mass spectra organic species with NO+ and NO2+ ions from the measurement in a mixed region between the boreal forestland and the urban area. The PMF analysis succeeded in separating the mixed spectra into three distinct organic factors and one inorganic factor. The particulate organic nitrate was distinguished by PMF for the first time, with a contribution of one-third of the total nitrate mass.
N. Hiranuma, M. Paukert, I. Steinke, K. Zhang, G. Kulkarni, C. Hoose, M. Schnaiter, H. Saathoff, and O. Möhler
Atmos. Chem. Phys., 14, 13145–13158, https://doi.org/10.5194/acp-14-13145-2014, https://doi.org/10.5194/acp-14-13145-2014, 2014
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A new heterogeneous ice nucleation parameterization is developed and implemented in cloud models. The results of our simulations suggest stronger influence of dust particles lifted to the upper troposphere on heterogeneous nucleation and more ice nucleation at temperature and humidity conditions relevant to both mixed-phase and cirrus clouds when compared to the existing parametrical frameworks.
D. W. Fahey, R.-S. Gao, O. Möhler, H. Saathoff, C. Schiller, V. Ebert, M. Krämer, T. Peter, N. Amarouche, L. M. Avallone, R. Bauer, Z. Bozóki, L. E. Christensen, S. M. Davis, G. Durry, C. Dyroff, R. L. Herman, S. Hunsmann, S. M. Khaykin, P. Mackrodt, J. Meyer, J. B. Smith, N. Spelten, R. F. Troy, H. Vömel, S. Wagner, and F. G. Wienhold
Atmos. Meas. Tech., 7, 3177–3213, https://doi.org/10.5194/amt-7-3177-2014, https://doi.org/10.5194/amt-7-3177-2014, 2014
C. Fountoukis, A. G. Megaritis, K. Skyllakou, P. E. Charalampidis, C. Pilinis, H. A. C. Denier van der Gon, M. Crippa, F. Canonaco, C. Mohr, A. S. H. Prévôt, J. D. Allan, L. Poulain, T. Petäjä, P. Tiitta, S. Carbone, A. Kiendler-Scharr, E. Nemitz, C. O'Dowd, E. Swietlicki, and S. N. Pandis
Atmos. Chem. Phys., 14, 9061–9076, https://doi.org/10.5194/acp-14-9061-2014, https://doi.org/10.5194/acp-14-9061-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
H. Kokkola, P. Yli-Pirilä, M. Vesterinen, H. Korhonen, H. Keskinen, S. Romakkaniemi, L. Hao, A. Kortelainen, J. Joutsensaari, D. R. Worsnop, A. Virtanen, and K. E. J. Lehtinen
Atmos. Chem. Phys., 14, 1689–1700, https://doi.org/10.5194/acp-14-1689-2014, https://doi.org/10.5194/acp-14-1689-2014, 2014
N. Hoffmann, A. Kiselev, D. Rzesanke, D. Duft, and T. Leisner
Atmos. Meas. Tech., 6, 2373–2382, https://doi.org/10.5194/amt-6-2373-2013, https://doi.org/10.5194/amt-6-2373-2013, 2013
M. Crippa, F. Canonaco, J. G. Slowik, I. El Haddad, P. F. DeCarlo, C. Mohr, M. F. Heringa, R. Chirico, N. Marchand, B. Temime-Roussel, E. Abidi, L. Poulain, A. Wiedensohler, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 13, 8411–8426, https://doi.org/10.5194/acp-13-8411-2013, https://doi.org/10.5194/acp-13-8411-2013, 2013
H. Saathoff, S. Henin, K. Stelmaszczyk, M. Petrarca, R. Delagrange, Z. Hao, J. Lüder, O. Möhler, Y. Petit, P. Rohwetter, M. Schnaiter, J. Kasparian, T. Leisner, J.-P. Wolf, and L. Wöste
Atmos. Chem. Phys., 13, 4593–4604, https://doi.org/10.5194/acp-13-4593-2013, https://doi.org/10.5194/acp-13-4593-2013, 2013
J. Skrotzki, P. Connolly, M. Schnaiter, H. Saathoff, O. Möhler, R. Wagner, M. Niemand, V. Ebert, and T. Leisner
Atmos. Chem. Phys., 13, 4451–4466, https://doi.org/10.5194/acp-13-4451-2013, https://doi.org/10.5194/acp-13-4451-2013, 2013
M. Crippa, P. F. DeCarlo, J. G. Slowik, C. Mohr, M. F. Heringa, R. Chirico, L. Poulain, F. Freutel, J. Sciare, J. Cozic, C. F. Di Marco, M. Elsasser, J. B. Nicolas, N. Marchand, E. Abidi, A. Wiedensohler, F. Drewnick, J. Schneider, S. Borrmann, E. Nemitz, R. Zimmermann, J.-L. Jaffrezo, A. S. H. Prévôt, and U. Baltensperger
Atmos. Chem. Phys., 13, 961–981, https://doi.org/10.5194/acp-13-961-2013, https://doi.org/10.5194/acp-13-961-2013, 2013
M. Laborde, M. Schnaiter, C. Linke, H. Saathoff, K.-H. Naumann, O. Möhler, S. Berlenz, U. Wagner, J. W. Taylor, D. Liu, M. Flynn, J. D. Allan, H. Coe, K. Heimerl, F. Dahlkötter, B. Weinzierl, A. G. Wollny, M. Zanatta, J. Cozic, P. Laj, R. Hitzenberger, J. P. Schwarz, and M. Gysel
Atmos. Meas. Tech., 5, 3077–3097, https://doi.org/10.5194/amt-5-3077-2012, https://doi.org/10.5194/amt-5-3077-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photochemical reactions: remarkably enhancing effects of seeds and ammonia
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
The lifetimes and potential change in planetary albedo owing to the oxidation of organic films extracted from atmospheric aerosol by hydroyxl (OH) radical oxidation at the air-water interface of aerosol particles
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement Report: Changes of ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice core record
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Si Zhang, Yining Gao, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 14177–14190, https://doi.org/10.5194/acp-24-14177-2024, https://doi.org/10.5194/acp-24-14177-2024, 2024
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Secondary organic aerosols (SOAs) from acetone photooxidation in the presence of various seeds were studied to illustrate SOA formation kinetics under ammonia-rich conditions. The oxidation mechanism of acetone was investigated using an observation-based model incorporating a Master Chemical Mechanism model. A higher SOA yield of acetone was observed compared to methylglyoxal due to an enhanced uptake of the small photooxidation products of acetone.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
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We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
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.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
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This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Rosalie Shepherd, Martin King, Andrew Ward, Edward Stuckey, Rebecca Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2367, https://doi.org/10.5194/egusphere-2024-2367, 2024
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Thin film formation at the air-water interface from material extracted from atmospheric aerosol was demonstrated, supporting core-shell morphology. The film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 hour. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top of the atmosphere albedo for urban films.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
EGUsphere, https://doi.org/10.5194/egusphere-2024-1381, https://doi.org/10.5194/egusphere-2024-1381, 2024
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A record of ammonium covering the years 1750 to 2008 was extracted from a 182-meter-long ice core drilled in 2009 at Mt. Elbrus in the Caucasus, Russia. Changes in ammonia emissions in southeastern Europe during the pre-industrial and industrial periods were investigated. The level of ammonium in 1750 indicates a significant contribution of natural sources to the ammonia budget, contrasting with present-day conditions, where agricultural emissions outweigh those from biogenic sources in Europe.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
EGUsphere, https://doi.org/10.5194/egusphere-2024-1880, https://doi.org/10.5194/egusphere-2024-1880, 2024
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The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolite and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
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.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
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Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Cited articles
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