Articles | Volume 20, issue 17
https://doi.org/10.5194/acp-20-10351-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-10351-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Sep 2020
Research article |
| 07 Sep 2020
| 07 Sep 2020
Treatment of non-ideality in the SPACCIM multiphase model – Part 2: Impacts on the multiphase chemical processing in deliquesced aerosol particles
Ahmad Jhony Rusumdar
Leibniz Institute for Tropospheric Research (TROPOS), 04318 Leipzig, Germany
now at: FERCHAU Engineering, Niederlassung Karlsruhe, 76185 Karlsruhe, Germany
Andreas Tilgner
Leibniz Institute for Tropospheric Research (TROPOS), 04318 Leipzig, Germany
Leibniz Institute for Tropospheric Research (TROPOS), 04318 Leipzig, Germany
Leibniz Institute for Tropospheric Research (TROPOS), 04318 Leipzig, Germany
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EGUsphere, https://doi.org/10.5194/egusphere-2025-4050, https://doi.org/10.5194/egusphere-2025-4050, 2025
This preprint is open for discussion and under review for Biogeosciences (BG).
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We conducted the first meta-analysis combining marine and freshwater studies to understand organic matter enrichment in the surface microlayer. Nitrogen-rich, particulate compounds are often enriched, with patterns varying by multiple factors. We recommend tracking both absolute concentrations and normalized enrichment patterns to better assess ecological conditions. Our study also introduces improved statistical methods for analyzing and comparing surface microlayer data.
Yaru Wang, Dominik van Pinxteren, Andreas Tilgner, Erik Hans Hoffmann, Max Hell, Susanne Bastian, and Hartmut Herrmann
Atmos. Chem. Phys., 25, 8907–8927, https://doi.org/10.5194/acp-25-8907-2025, https://doi.org/10.5194/acp-25-8907-2025, 2025
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Tropospheric ground-level ozone (O3) is a global air quality pollutant and greenhouse gas. Long-term O3 trends from 16 stations in Saxony, Germany, were compared over three periods, revealing worsened O3 pollution over the last decade. O3 formation has been volatile organic compound (VOC)-limited at traffic and urban sites for the past 20 years. To mitigate O3 pollution, moderate nitrogen oxides and additional VOC controls, particularly in solvent use, should be prioritized in the coming years.
Vikram Pratap, Christopher J. Hennigan, Bastian Stieger, Andreas Tilgner, Laurent Poulain, Dominik van Pinxteren, Gerald Spindler, and Hartmut Herrmann
Atmos. Chem. Phys., 25, 8871–8889, https://doi.org/10.5194/acp-25-8871-2025, https://doi.org/10.5194/acp-25-8871-2025, 2025
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In this work, we characterize trends in aerosol pH and its controlling factors during the period 2010–2019 at the Melpitz research station in eastern Germany. We find strong trends in aerosol pH and major inorganic species in response to changing emissions. We conduct a detailed thermodynamic analysis of the aerosol system and discuss implications for controlling particulate matter in the region.
Donger Lai, Yanxin Bai, Zijing Zhang, Pui-Kin So, Yong Jie Li, Ying-Lung Steve Tse, Ying-Yeung Yeung, Thomas Schaefer, Hartmut Herrmann, Jian Zhen Yu, Yuchen Wang, and Man Nin Chan
EGUsphere, https://doi.org/10.5194/egusphere-2025-2743, https://doi.org/10.5194/egusphere-2025-2743, 2025
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Aqueous-phase •OH oxidation can potentially act as an important atmospheric sink for α-pinene-derived organosulfates (OSs). Such oxidation can also generate a variety of new OS products, and can be as a potential source for some atmospheric OSs with previously unknown origins.
Peng Cheng, Gilles Mailhot, Mohamed Sarakha, Guillaume Voyard, Daniele Scheres Firak, Thomas Schaefer, Hartmut Herrmann, and Marcello Brigante
EGUsphere, https://doi.org/10.5194/egusphere-2025-1744, https://doi.org/10.5194/egusphere-2025-1744, 2025
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This study investigates the complexation of Fe(II) and Fe(III) with glutamic acid under cloud water conditions and the effect on Fenton and photo-Fenton reactions, hydroxyl radical formation, and their impact on amino acid oxidation.
Hanna Wiedenhaus, Roland Schrödner, Ralf Wolke, Marie L. Luttkus, Shubhi Arora, Laurent Poulain, Radek Lhotka, Petr Vodička, Jaroslav Schwarz, Petra Pokorna, Jakub Ondráček, Vladimir Ždímal, Hartmut Herrmann, and Ina Tegen
EGUsphere, https://doi.org/10.5194/egusphere-2025-1225, https://doi.org/10.5194/egusphere-2025-1225, 2025
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This study examines winter air quality in Central Europe, focusing on the impact of domestic heating. Using a chemical transport model and measurements, it was found that the model underestimated organic particle concentrations. This was due to an underestimation of gases from domestic heating that form secondary organic particles. Improving the model by increasing these emissions and the particle formation led to better results, demonstrating the important role of heating emissions in winter.
Shravan Deshmukh, Laurent Poulain, Birgit Wehner, Silvia Henning, Jean-Eudes Petit, Pauline Fombelle, Olivier Favez, Hartmut Herrmann, and Mira Pöhlker
Atmos. Chem. Phys., 25, 741–758, https://doi.org/10.5194/acp-25-741-2025, https://doi.org/10.5194/acp-25-741-2025, 2025
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Aerosol hygroscopicity has been investigated at a sub-urban site in Paris; analysis shows the sub-saturated regime's measured hygroscopicity and the chemically derived hygroscopic growth, shedding light on the large effect of external particle mixing and its influence on predicting hygroscopicity.
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Katerina Seitanidi, Pourya Shahpoury, Eduardo J. d. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech., 18, 177–195, https://doi.org/10.5194/amt-18-177-2025, https://doi.org/10.5194/amt-18-177-2025, 2025
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In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP dithiothreitol assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardisation in OP procedures.
Shengqian Zhou, Ying Chen, Shan Huang, Xianda Gong, Guipeng Yang, Honghai Zhang, Hartmut Herrmann, Alfred Wiedensohler, Laurent Poulain, Yan Zhang, Fanghui Wang, Zongjun Xu, and Ke Yan
Earth Syst. Sci. Data, 16, 4267–4290, https://doi.org/10.5194/essd-16-4267-2024, https://doi.org/10.5194/essd-16-4267-2024, 2024
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Dimethyl sulfide (DMS) is a crucial natural reactive gas in the global climate system due to its great contribution to aerosols and subsequent impact on clouds over remote oceans. Leveraging machine learning techniques, we constructed a long-term global sea surface DMS gridded dataset with daily resolution. Compared to previous datasets, our new dataset holds promise for improving atmospheric chemistry modeling and advancing our comprehension of the climate effects associated with oceanic DMS.
Anil Kumar Mandariya, Junteng Wu, Anne Monod, Paola Formenti, Bénédicte Picquet-Varrault, Mathieu Cazaunau, Stephan Mertes, Laurent Poulain, Antonin Berge, Edouard Pangui, Andreas Tilgner, Thomas Schaefer, Liang Wen, Hartmut Herrmann, and Jean-François Doussin
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-206, https://doi.org/10.5194/amt-2023-206, 2024
Publication in AMT not foreseen
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An optimized and controlled protocol for generating quasi-adiabatic expansion clouds under simulated dark and light conditions was presented. The irradiated clouds clearly showed a gradual activation of seed particles into droplets. In contrast, non-irradiated clouds faced a flash activation. This paper will lay the foundation for multiphase photochemical studies implying water-soluble volatile organic compounds and particulate matter formation during cloud formation-evaporation cycles.
Andrea Cuesta-Mosquera, Kristina Glojek, Griša Močnik, Luka Drinovec, Asta Gregorič, Martin Rigler, Matej Ogrin, Baseerat Romshoo, Kay Weinhold, Maik Merkel, Dominik van Pinxteren, Hartmut Herrmann, Alfred Wiedensohler, Mira Pöhlker, and Thomas Müller
Atmos. Chem. Phys., 24, 2583–2605, https://doi.org/10.5194/acp-24-2583-2024, https://doi.org/10.5194/acp-24-2583-2024, 2024
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This study evaluated the air pollution and climate impacts of residential-wood-burning particle emissions from a rural European site. The authors investigate the optical and physical properties that connect the aerosol emissions with climate by evaluating atmospheric radiative impacts via simple-forcing calculations. The study contributes to reducing the lack of information on the understanding of the optical properties of air pollution from anthropogenic sources.
Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Moritz Zeising, Astrid Bracher, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 15561–15587, https://doi.org/10.5194/acp-23-15561-2023, https://doi.org/10.5194/acp-23-15561-2023, 2023
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Marine carbohydrates are produced in the surface of the ocean, enter the atmophere as part of sea spray aerosol particles, and potentially contribute to the formation of fog and clouds. Here, we present the results of a sea–air transfer study of marine carbohydrates conducted in the high Arctic. Besides a chemo-selective transfer, we observed a quick atmospheric aging of carbohydrates, possibly as a result of both biotic and abiotic processes.
Jean-Philippe Putaud, Enrico Pisoni, Alexander Mangold, Christoph Hueglin, Jean Sciare, Michael Pikridas, Chrysanthos Savvides, Jakub Ondracek, Saliou Mbengue, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Laurent Poulain, Dominik van Pinxteren, Hartmut Herrmann, Andreas Massling, Claus Nordstroem, Andrés Alastuey, Cristina Reche, Noemí Pérez, Sonia Castillo, Mar Sorribas, Jose Antonio Adame, Tuukka Petaja, Katrianne Lehtipalo, Jarkko Niemi, Véronique Riffault, Joel F. de Brito, Augustin Colette, Olivier Favez, Jean-Eudes Petit, Valérie Gros, Maria I. Gini, Stergios Vratolis, Konstantinos Eleftheriadis, Evangelia Diapouli, Hugo Denier van der Gon, Karl Espen Yttri, and Wenche Aas
Atmos. Chem. Phys., 23, 10145–10161, https://doi.org/10.5194/acp-23-10145-2023, https://doi.org/10.5194/acp-23-10145-2023, 2023
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Many European people are still exposed to levels of air pollution that can affect their health. COVID-19 lockdowns in 2020 were used to assess the impact of the reduction in human mobility on air pollution across Europe by comparing measurement data with values that would be expected if no lockdown had occurred. We show that lockdown measures did not lead to consistent decreases in the concentrations of fine particulate matter suspended in the air, and we investigate why.
Samira Atabakhsh, Laurent Poulain, Gang Chen, Francesco Canonaco, André S. H. Prévôt, Mira Pöhlker, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6963–6988, https://doi.org/10.5194/acp-23-6963-2023, https://doi.org/10.5194/acp-23-6963-2023, 2023
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The study focuses on the aerosol chemical variations found in the rural-background station of Melpitz based on ACSM and MAAP measurements. Source apportionment on both organic aerosol (OA) and black carbon (eBC) was performed, and source seasonality was also linked to air mass trajectories. Overall, three anthropogenic sources were identified in OA and eBC plus two additional aged OA. Our results demonstrate the influence of transported coal-combustion-related OA even during summer time.
Manuela van Pinxteren, Sebastian Zeppenfeld, Khanneh Wadinga Fomba, Nadja Triesch, Sanja Frka, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6571–6590, https://doi.org/10.5194/acp-23-6571-2023, https://doi.org/10.5194/acp-23-6571-2023, 2023
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Important marine organic carbon compounds were identified in the Atlantic Ocean and marine aerosol particles. These compounds were strongly enriched in the atmosphere. Their enrichment was, however, not solely explained via sea-to-air transfer but also via atmospheric in situ formation. The identified compounds constituted about 50 % of the organic carbon on the aerosol particles, and a pronounced coupling between ocean and atmosphere for this oligotrophic region could be concluded.
Yuan Wang, Silvia Henning, Laurent Poulain, Chunsong Lu, Frank Stratmann, Yuying Wang, Shengjie Niu, Mira L. Pöhlker, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 15943–15962, https://doi.org/10.5194/acp-22-15943-2022, https://doi.org/10.5194/acp-22-15943-2022, 2022
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Aerosol particle activation affects cloud, precipitation, radiation, and thus the global climate. Its long-term measurements are important but still scarce. In this study, more than 4 years of measurements at a central European station were analyzed. The overall characteristics and seasonal changes of aerosol particle activation are summarized. The power-law fit between particle hygroscopicity factor and diameter was recommended for predicting cloud
condensation nuclei number concentration.
Lady Mateus-Fontecha, Angela Vargas-Burbano, Rodrigo Jimenez, Nestor Y. Rojas, German Rueda-Saa, Dominik van Pinxteren, Manuela van Pinxteren, Khanneh Wadinga Fomba, and Hartmut Herrmann
Atmos. Chem. Phys., 22, 8473–8495, https://doi.org/10.5194/acp-22-8473-2022, https://doi.org/10.5194/acp-22-8473-2022, 2022
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This study reports the chemical composition of regionally representative PM2.5 in an area densely populated and substantially industrialized, located in the inter-Andean valley, with the highest sugarcane yield in the world and where sugarcane is burned and harvested year round. We found that sugarcane burning is not portrayed as a distinguishable sample composition component. Instead, the composition analysis revealed multiple associations among sugarcane burning components and other sources.
Manuela van Pinxteren, Tiera-Brandy Robinson, Sebastian Zeppenfeld, Xianda Gong, Enno Bahlmann, Khanneh Wadinga Fomba, Nadja Triesch, Frank Stratmann, Oliver Wurl, Anja Engel, Heike Wex, and Hartmut Herrmann
Atmos. Chem. Phys., 22, 5725–5742, https://doi.org/10.5194/acp-22-5725-2022, https://doi.org/10.5194/acp-22-5725-2022, 2022
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A class of marine particles (transparent exopolymer particles, TEPs) that is ubiquitously found in the world oceans was measured for the first time in ambient marine aerosol particles and marine cloud waters in the tropical Atlantic Ocean. TEPs are likely to have good properties for influencing clouds. We show that TEPs are transferred from the ocean to the marine atmosphere via sea-spray formation and our results suggest that they can also form directly in aerosol particles and in cloud water.
Kristina Glojek, Griša Močnik, Honey Dawn C. Alas, Andrea Cuesta-Mosquera, Luka Drinovec, Asta Gregorič, Matej Ogrin, Kay Weinhold, Irena Ježek, Thomas Müller, Martin Rigler, Maja Remškar, Dominik van Pinxteren, Hartmut Herrmann, Martina Ristorini, Maik Merkel, Miha Markelj, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 5577–5601, https://doi.org/10.5194/acp-22-5577-2022, https://doi.org/10.5194/acp-22-5577-2022, 2022
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A pilot study to determine the emissions of wood burning under
real-world laboratoryconditions was conducted. We found that measured black carbon (eBC) and particulate matter (PM) in rural shallow terrain depressions with residential wood burning could be much greater than predicted by models. The exceeding levels are a cause for concern since similar conditions can be expected in numerous hilly and mountainous regions across Europe, where approximately 20 % of the total population lives.
Nabil Deabji, Khanneh Wadinga Fomba, Souad El Hajjaji, Abdelwahid Mellouki, Laurent Poulain, Sebastian Zeppenfeld, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 18147–18174, https://doi.org/10.5194/acp-21-18147-2021, https://doi.org/10.5194/acp-21-18147-2021, 2021
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Mountain and high-altitude sites provide representative data for the lower free troposphere, various pathways for aerosol interactions, and changing boundary layer heights useful in understanding atmospheric composition. However, only few studies exist in African regions despite diversity in both natural and anthropogenic emissions. This study provides detailed atmospheric studies in the northern African high-altitude region.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
Markus Hartmann, Xianda Gong, Simonas Kecorius, Manuela van Pinxteren, Teresa Vogl, André Welti, Heike Wex, Sebastian Zeppenfeld, Hartmut Herrmann, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 21, 11613–11636, https://doi.org/10.5194/acp-21-11613-2021, https://doi.org/10.5194/acp-21-11613-2021, 2021
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Ice-nucleating particles (INPs) are not well characterized in the Arctic despite their importance for the Arctic energy budget. Little is known about their nature (mineral or biological) and sources (terrestrial or marine, long-range transport or local). We find indications that, at the beginning of the melt season, a local, biogenic, probably marine source is likely, but significant enrichment of INPs has to take place from the ocean to the aerosol phase.
Anke Mutzel, Yanli Zhang, Olaf Böge, Maria Rodigast, Agata Kolodziejczyk, Xinming Wang, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 8479–8498, https://doi.org/10.5194/acp-21-8479-2021, https://doi.org/10.5194/acp-21-8479-2021, 2021
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This study investigates secondary organic aerosol (SOA) formation and particle growth from α-pinene, limonene, and m-cresol oxidation through NO3 and OH radicals and the effect of relative humidity. The formed SOA is comprehensively characterized with respect to the content of OC / EC, WSOC, SOA-bound peroxides, and SOA marker compounds. The findings present new insights and implications of nighttime chemistry, which can form SOA more efficiently than OH radical reaction during daytime.
Matthias Faust, Ralf Wolke, Steffen Münch, Roger Funk, and Kerstin Schepanski
Geosci. Model Dev., 14, 2205–2220, https://doi.org/10.5194/gmd-14-2205-2021, https://doi.org/10.5194/gmd-14-2205-2021, 2021
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Trajectory dispersion models are powerful and intuitive tools for tracing air pollution through the atmosphere. But the turbulent nature of the atmospheric boundary layer makes it challenging to provide accurate predictions near the surface. To overcome this, we propose an approach using wind and turbulence information at high temporal resolution. Finally, we demonstrate the strength of our approach in a case study on dust emissions from agriculture.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
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Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
Nadja Triesch, Manuela van Pinxteren, Sanja Frka, Christian Stolle, Tobias Spranger, Erik Hans Hoffmann, Xianda Gong, Heike Wex, Detlef Schulz-Bull, Blaženka Gašparović, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 4267–4283, https://doi.org/10.5194/acp-21-4267-2021, https://doi.org/10.5194/acp-21-4267-2021, 2021
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To investigate the source of lipids and their representatives in the marine atmosphere, concerted measurements of seawater and submicrometer aerosol particle sampling were carried out on the Cabo Verde islands. This field study describes the biogenic sources of lipids, their selective transfer from the ocean into the atmosphere and their enrichment as part of organic matter. A strong enrichment of the studied representatives of the lipid classes on submicrometer aerosol particles was observed.
Laurent Poulain, Benjamin Fahlbusch, Gerald Spindler, Konrad Müller, Dominik van Pinxteren, Zhijun Wu, Yoshiteru Iinuma, Wolfram Birmili, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 3667–3684, https://doi.org/10.5194/acp-21-3667-2021, https://doi.org/10.5194/acp-21-3667-2021, 2021
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We present results from source apportionment analysis on the carbonaceous aerosol particles, including organic aerosol (OA) and equivalent black carbon (eBC), allowing us to distinguish local emissions from long-range transport for OA and eBC sources. By merging online chemical measurements and considering particle number size distribution, the different air masses reaching the sampling place were described and discussed, based on their respective chemical composition and size distribution.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
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Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Nadja Triesch, Manuela van Pinxteren, Anja Engel, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 163–181, https://doi.org/10.5194/acp-21-163-2021, https://doi.org/10.5194/acp-21-163-2021, 2021
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To investigate the sources of free amino acids (FAAs) in the marine atmosphere, concerted measurements (the simultaneous investigation of seawater, size-segregated aerosol particles and cloud water) were performed at the Cabo Verde islands. This study describes the transfer of FAAs as part of organic matter from the ocean into the atmosphere on a molecular level. In the investigated marine environment, a high enrichment of FAAs in submicron aerosol particles and in cloud droplets was observed.
Jiarong Li, Chao Zhu, Hui Chen, Defeng Zhao, Likun Xue, Xinfeng Wang, Hongyong Li, Pengfei Liu, Junfeng Liu, Chenglong Zhang, Yujing Mu, Wenjin Zhang, Luming Zhang, Hartmut Herrmann, Kai Li, Min Liu, and Jianmin Chen
Atmos. Chem. Phys., 20, 13735–13751, https://doi.org/10.5194/acp-20-13735-2020, https://doi.org/10.5194/acp-20-13735-2020, 2020
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Based on a field study at Mt. Tai, China, the simultaneous variations of cloud microphysics, aerosol microphysics and their potential interactions during cloud life cycles were discussed. Results demonstrated that clouds on clean days were more susceptible to the concentrations of particle number, while clouds formed on polluted days might be more sensitive to meteorological parameters. Particles larger than 150 nm played important roles in forming cloud droplets with sizes of 5–10 μm.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, https://doi.org/10.5194/acp-20-13497-2020, 2020
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Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
Yangang Ren, Bastian Stieger, Gerald Spindler, Benoit Grosselin, Abdelwahid Mellouki, Thomas Tuch, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 20, 13069–13089, https://doi.org/10.5194/acp-20-13069-2020, https://doi.org/10.5194/acp-20-13069-2020, 2020
Short summary
Short summary
We present HONO measurements from the TROPOS research site in Melpitz, Germany. Investigations of HONO sources and sinks revealed the nighttime formation by heterogeneous conversion of NO2 to HONO followed by a significant surface deposition at night. The evaporation of dew was identified as the main HONO source in the morning. In the following, dew measurements with a self-made dew collector were performed to estimate the amount of evaporated HONO from dew in the atmospheric HONO distribution.
Laurent Poulain, Gerald Spindler, Achim Grüner, Thomas Tuch, Bastian Stieger, Dominik van Pinxteren, Jean-Eudes Petit, Olivier Favez, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Meas. Tech., 13, 4973–4994, https://doi.org/10.5194/amt-13-4973-2020, https://doi.org/10.5194/amt-13-4973-2020, 2020
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The stability and the comparability between ACSM and collocated filter sampling and MPSS measurements was investigated in order to examine the instruments robustness for year-long measurements. Specific attention was paid to the influence of the upper size cutoff diameter to better understand how it might affect the data validation. Recommendations are provided for better on-site quality assurance and quality control of the ACSM, which would be useful for either long-term or intensive campaigns.
Khanneh Wadinga Fomba, Nabil Deabji, Sayf El Islam Barcha, Ibrahim Ouchen, El Mehdi Elbaramoussi, Rajaa Cherkaoui El Moursli, Mimoun Harnafi, Souad El Hajjaji, Abdelwahid Mellouki, and Hartmut Herrmann
Atmos. Meas. Tech., 13, 4773–4790, https://doi.org/10.5194/amt-13-4773-2020, https://doi.org/10.5194/amt-13-4773-2020, 2020
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Short summary
As air quality monitoring networks often sample aerosol particles on quartz filters, the development and applicability of analytical methods with quartz filters are becoming important. In this study different filter preparation methods (e.g., baking, acid digestion) were investigated for quantifying trace metals on quartz and polycarbonate filters, and cloud water using the total reflection X-Ray fluorescence (TXRF) technique, with low detection limits of about 0.3 ng cm−3 for some elements.
Cited articles
Adriano, D. C. and Johnson, A. H.: Acidic Precipitation: Biological and
Ecological Effects, Springer New York, 85–136, 1989.
Akimoto, H.: Global Air Quality and Pollution, Science, 302, 1716–1719, https://doi.org/10.1126/science.1092666, 2003.
Amundson, N. R., Caboussat, A., He, J. W., Martynenko, A. V., Savarin, V.
B., Seinfeld, J. H., and Yoo, K. Y.: A new inorganic atmospheric aerosol
phase equilibrium model (UHAERO), Atmos. Chem. Phys., 6, 975–992, https://doi.org/10.5194/acp-6-975-2006, 2006.
Amundson, N. R., Caboussat, A., He, J. W., Martynenko, A. V., Landry, C.,
Tong, C., and Seinfeld, J. H.: A new atmospheric aerosol phase equilibrium
model (UHAERO): organic systems, Atmos. Chem. Phys., 7, 4675–4698,
https://doi.org/10.5194/acp-7-4675-2007, 2007.
Andreae, M. O. and Crutzen, P. J.: Atmospheric Aerosols: Biogeochemical
Sources and Role in Atmospheric Chemistry, Science, 276, 1052, https://doi.org/10.1126/science.276.5315.1052, 1997.
Ansari, A. S. and Pandis, S. N.: Prediction of multicomponent inorganic
atmospheric aerosol behavior, Atmos. Environ., 33, 745–757, https://doi.org/10.1016/S1352-2310(98)00221-0, 1999.
Barth, M. C.: The importance of cloud drop representation on cloud
photochemistry, Atmos. Res., 82, 294–309, https://doi.org/10.1016/j.atmosres.2005.10.008, 2006.
Boucher, O., Randall, D., Artaxo, P., Bretherton, C., Feingold, G., Forster,
P., Kerminen, V.-M., Kondo, Y., Liao, H., Lohmann, U., Rasch, P., Satheesh,
S. K., Sherwood, S., Stevens, B., and Zhang, X. Y.: Clouds and Aerosols, in:
Climate Change 2013: The Physical Science Basis, Contribution of Working
Group I to the Fifth Assessment Report of the Intergovernmental Panel on
Climate Change, edited by: Stocker, T. F., Qin, D., Plattner, G.-K., Tignor,
M., Allen, S. K., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley,
P. M., Cambridge, Großbritannien und New York, USA, 2013.
Bräuer, P., Tilgner, A., Wolke, R., and Herrmann, H.: Mechanism
development and modelling of tropospheric multiphase halogen chemistry: The
CAPRAM Halogen Module 2.0 (HM2), J. Atmos. Chem., 70, 19–52, https://doi.org/10.1007/S10874-013-9249-6, 2013.
Bräuer, P., Mouchel-Vallon, C., Tilgner, A., Mutzel, A., Böge, O.,
Rodigast, M., Poulain, L., van Pinxteren, D., Wolke, R., Aumont, B., and
Herrmann, H.: Development of a protocol for the auto-generation of explicit
aqueous-phase oxidation schemes of organic compounds, Atmos. Chem. Phys.,
19, 9209–9239, https://doi.org/10.5194/acp-19-9209-2019, 2019.
Brunekreef, B. and Holgate, S. T.: Air pollution and health, Lancet, 360,
1233–1242, https://doi.org/10.1016/S0140-6736(02)11274-8, 2002.
Cappa, C. D., Lovejoy, E. R., and Ravishankara, A. R.: Evidence for
liquid-like and nonideal behavior of a mixture of organic aerosol
components, P. Natl. Acad. Sci. USA, 105, 18687–18691, https://doi.org/10.1073/pnas.0802144105, 2008.
Chameides, W. L. and Stelson, A. W.: Aqueous-phase chemical processes in
deliquescent sea-salt aerosols: A mechanism that couples the atmospheric
cycles of S and sea salt, J. Geophys. Res.-Atmos., 97, 20565–20580,
https://doi.org/10.1029/92JD01923, 1992.
Charlson, R. J., Schwartz, S. E., Hales, J. M., Cess, R. D., Coakley, J. A.,
Hansen, J. E., and Hofmann, D. J.: Climate Forcing by Anthropogenic
Aerosols, Science, 255, 423–430, https://doi.org/10.1126/science.255.5043.423, 1992.
Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: Thermodynamic Model of
the System H+-
Clegg, S. L., Brimblecombe, P., and Wexler, A. S.: A thermodynamic model of
the system H+-
Clegg, S. L., Kleeman, M. J., Griffin, R. J., and Seinfeld, J. H.: Effects
of uncertainties in the thermodynamic properties of aerosol components in an
air quality model–Part 1: Treatment of inorganic electrolytes and organic
compounds in the condensed phase, Atmos. Chem. Phys., 8, 1057–1085,
https://doi.org/10.5194/acp-8-1057-2008, 2008.
Craig, R. L., Peterson, P. K., Nandy, L., Lei, Z., Hossain, M. A., Camarena,
S., Dodson, R. A., Cook, R. D., Dutcher, C. S., and Ault, A. P.: Direct
Determination of Aerosol pH: Size-Resolved Measurements of Submicrometer and
Supermicrometer Aqueous Particles, Anal. Chem., 90, 11232–11239, https://doi.org/10.1021/acs.analchem.8b00586, 2018.
Deguillaume, L., Leriche, M., Monod, A., and Chaumerliac, N.: The role of
transition metal ions on HOx radicals in clouds: a numerical evaluation of
its impact on multiphase chemistry, Atmos. Chem. Phys., 4, 95–110,
https://doi.org/10.5194/acp-4-95-2004, 2004.
Deguillaume, L., Leriche, M., Desboeufs, K., Mailhot, G., George, C., and
Chaumerliac, N.: Transition metals in atmospheric liquid phases: Sources,
reactivity, and sensitive parameters, Chem. Rev., 105, 3388–3431, https://doi.org/10.1021/cr040649c, 2005.
Deguillaume, L., Tilgner, A., Schrödner, R., Wolke, R., Chaumerliac, N.,
and Herrmann, H.: Towards an operational aqueous phase chemistry mechanism
for regional chemistry-transport models: CAPRAM-RED and its application to
the COSMO-MUSCAT model, J. Atmos. Chem., 64, 1–35, https://doi.org/10.1007/s10874-010-9168-8, 2009.
Erdakos, G. B., Asher, W. E., Seinfeld, J. H., and Pankow, J. F.: Prediction
of activity coefficients in liquid aerosol particles containing organic
compounds, dissolved inorganic salts, and water – Part 1: Organic compounds
and water by consideration of short-and long-range effects using X-UNIFAC,
1, Atmos. Environ., 40, 6410–6421, https://doi.org/10.1016/j.atmosenv.2006.04.030, 2006a.
Erdakos, G. B., Chang, E. I., Pankow, J. F., and Seinfeld, J. H.: Prediction
of activity coefficients in liquid aerosol particles containing organic
compounds, dissolved inorganic salts, and water – Part 3: Organic compounds,
water, and ionic constituents by consideration of short-, mid-, and
long-range effects using X-UNIFAC, 3, Atmos. Environ., 40, 6437–6452,
https://doi.org/10.1016/j.atmosenv.2006.04.001, 2006b.
Ervens, B.: Modeling the processing of aerosol and trace gases in clouds and
fogs, Chem. Rev., 115, 4157–4198, https://doi.org/10.1021/cr5005887, 2015.
Ervens, B., George, C., Williams, J. E., Buxton, G. V., Salmon, G. A.,
Bydder, M., Wilkinson, F., Dentener, F., Mirabel, P., Wolke, R., and
Herrmann, H.: CAPRAM 2.4 (MODAC mechanism): An extended and condensed
tropospheric aqueous phase mechanism and its application, J. Geophys.
Res.-Atmos., 108, 4426, https://doi.org/10.1029/2002JD002202,
2003.
Ervens, B., Feingold, G., Frost, G. J., and Kreidenweis, S. M.: A modeling
study of aqueous production of dicarboxylic acids: 1. Chemical pathways and
speciated organic mass production, J. Geophys. Res.-Atmos., 109, D15205,
https://doi.org/10.1029/2004JD004575, 2004.
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol
formation in cloud droplets and aqueous particles (aqSOA): a review of
laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102,
https://doi.org/10.5194/acp-11-11069-2011, 2011.
Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient
thermodynamic equilibrium model for K+-Ca2+-Mg2+-
Fredenslund, A., Jones, R. L., and Prausnitz, J. M.: Group-contribution
estimation of activity coefficients in non-ideal liquid mixtures, AIChE J.,
21, 1086–1098, https://doi.org/10.1002/aic.690210607, 1975.
Fridlind, A. M. and Jacobson, M. Z.: A study of gas-aerosol equilibrium and
aerosol pH in the remote marine boundary layer during the First Aerosol
Characterization Experiment (ACE 1), J. Geophys. Res.-Atmos., 105,
17325–17340, https://doi.org/10.1029/2000JD900209, 2000.
Ganbavale, G., Zuend, A., Marcolli, C., and Peter, T.: Improved AIOMFAC
model parameterisation of the temperature dependence of activity
coefficients for aqueous organic mixtures, Atmos. Chem. Phys., 15, 447–493,
https://doi.org/10.5194/acp-15-447-2015, 2015.
George, C., Ammann, M., D'Anna, B., Donaldson, D. J., and Nizkorodov, S. A.:
Heterogeneous Photochemistry in the Atmosphere, Chem. Rev., 115, 4218–4258,
https://doi.org/10.1021/cr500648z, 2015.
Gervasi, N. R., Topping, D. O., and Zuend, A.: A predictive group-contribution model for the viscosity of aqueous organic aerosol, Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, 2020.
Guo, J., Tilgner, A., Yeung, C., Wang, Z., Louie, P. K. K., Luk, C. W. Y.,
Xu, Z., Yuan, C., Gao, Y., Poon, S., Herrmann, H., Lee, S., Lam, K. S., and
Wang, T.: Atmospheric peroxides in a polluted subtropical environment:
Seasonal variation, sources and sinks, and importance of heterogeneous
processes, Environ. Sci. Technol., 48, 1443–1450, https://doi.org/10.1021/es403229x, 2014.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Hansen, H. K., Rasmussen, P., Fredenslung, A., Schiller, M., and Gmehling,
J.: Vapor-liquid equilibria by UNIFAC group contribution, 5. Revision and
extention, Ind. Eng. Chem. Res., 30, 2352–2355, https://doi.org/10.1021/ie00058a017, 1991.
Herrmann, H., Tilgner, A., Barzaghi, P., Majdik, Z.-T., Gligorovski, S.,
Poulain, L., and Monod, A.: Towards a more detailed description of
tropospheric aqueous phase organic chemistry: CAPRAM 3.0, Atmos. Environ.,
39, 4351–4363, https://doi.org/10.1016/j.atmosenv.2005.02.016,
2005.
Herrmann, H., Schaefer, T., Tilgner, A., Styler, S. A., Weller, C., Teich,
M., and Otto, T.: Tropospheric aqueous-phase chemistry: kinetics,
mechanisms, and its coupling to a changing gas phase, Chem. Rev., 115,
4259–4334, https://doi.org/10.1021/cr500447k, 2015.
Hoffmann, E. H., Tilgner, A., Schrodner, R., Brauer, P., Wolke, R., and
Herrmann, H.: An advanced modeling study on the impacts and atmospheric
implications of multiphase dimethyl sulfide chemistry, P. Natl. Acad.
Sci. USA, 113, 11776–11781, https://doi.org/10.1073/pnas.1606320113, 2016.
Hoffmann, E. H., Tilgner, A., Wolke, R., Boge, O., Walter, A., and Herrmann,
H.: Oxidation of substituted aromatic hydrocarbons in the tropospheric
aqueous phase: kinetic mechanism development and modelling, Phys. Chem.
Chem. Phys., 20, 10960–10977, https://doi.org/10.1039/C7CP08576A, 2018.
Holgate, S. T.: The epidemic of allergy and asthma, Nature, 402, 2–4,
https://doi.org/10.1038/35037000, 1999.
Jacobson, M. Z.: Development and application of a new air pollution modeling
system, Part II. Aerosol module structure and design, Atmos. Environ., 31,
131–144, https://doi.org/10.1016/1352-2310(96)00202-6, 1997.
Jacobson, M. Z., Tabazadeh, A., and Turco, R. P.: Simulating equilibrium
within aerosols and nonequilibrium between gases and aerosols, J. Geophys.
Res.-Atmos., 101, 9071–9091, https://doi.org/10.1029/96JD00348, 1996.
Jang, M., Kamens, R., Leach, K., and Strommen, M.: A thermodynamic approach
using group contribution methods to model the partitioning of semivolatile
organic compounds on atmospheric particulate matter, Environ. Sci. Technol.,
31, 2805–2811, https://doi.org/10.1021/es970014d, 1997.
Johnson, M. T.: A numerical scheme to calculate temperature and salinity
dependent air-water transfer velocities for any gas, Ocean Sci., 6, 913–932,
https://doi.org/10.5194/os-6-913-2010, 2010.
Kawamura, K. and Bikkina, S.: A review of dicarboxylic acids and related
compounds in atmospheric aerosols: Molecular distributions, sources and
transformation, Atmos. Res., 170, 140–160, https://doi.org/10.1016/j.atmosres.2015.11.018, 2016.
Kiepe, J., Noll, O., and Gmehling, J.: Modified LIQUAC and Modified LIFACA
Further Development of Electrolyte Models for the Reliable Prediction of
Phase Equilibria with Strong Electrolytes, Ind. Eng. Chem. Res., 45,
2361–2373, https://doi.org/10.1021/ie0510122, 2006.
Köhler, H.: The nucleus in and the growth of hygroscopic droplets,
Trans. Faraday Soc., 32, 1152–1161, https://doi.org/10.1039/TF9363201152, 1936.
Lelieveld, J., Evans, J. S., Fnais, M., Giannadaki, D., and Pozzer, A.: The
contribution of outdoor air pollution sources to premature mortality on a
global scale, Nature, 525, 367–371, https://doi.org/10.1038/nature15371, 2015.
Li, J., Polka, H.-M., and Gmehling, J.: A gE model for single and mixed
solvent electrolyte systems: 1. Model and results for strong electrolytes,
Fluid Phase Equilib., 94, 89–114, https://doi.org/10.1016/0378-3812(94)87052-7, 1994.
Lim, H. J., Carlton, A. G., and Turpin, B. J.: Isoprene forms secondary
organic aerosol through cloud processing: Model simulations, Environ. Sci.
Technol., 39, 4441–4446, https://doi.org/10.1021/es048039h,
2005.
Lohmann, U. and Feichter, J.: Global indirect aerosol effects: a review,
Atmos. Chem. Phys., 5, 715–737, https://doi.org/10.5194/acp-5-715-2005, 2005.
Mao, J., Fan, S., Jacob, D. J., and Travis, K. R.: Radical loss in the
atmosphere from Cu-Fe redox coupling in aerosols, Atmos. Chem. Phys., 13,
509–519, https://doi.org/10.5194/acp-13-509-2013, 2013.
Marini, L.: The Aqueous Electrolyte Solution, chap. 4, in: Developments
in Geochemistry, edited by: Marini, L., Elsevier, 53–77,https://doi.org/10.1016/S0921-3198(06)80024-4, 2007.
McNeill, V. F., Woo, J. L., Kim, D. D., Schwier, A. N., Wannell, N. J.,
Sumner, A. J., and Barakat, J. M.: Aqueous-Phase Secondary Organic Aerosol
and Organosulfate Formation in Atmospheric Aerosols: A Modeling Study,
Environ. Sci. Technol., 46, 8075–8081, https://doi.org/10.1021/es3002986, 2012a.
McNeill, V. F., Woo, J. L., Kim, D. D., Schwier, A. N., Wannell, N. J.,
Sumner, A. J., and Barakat, J. M.: Aqueous-phase secondary organic aerosol
and organosulfate formation in atmospheric aerosols: a modeling study,
Environ. Sci. Technol., 46, 8075–8081, https://doi.org/10.1021/es3002986, 2012b.
Millero, F. J. and Woosley, R.: The Hydrolysis of Al(III) in NaCl
solutions – A Model for Fe(III), Environ. Sci. Technol., 43, 1818–1823,
https://doi.org/10.1021/es802504u, 2009.
Ming, Y. and Russell, L. M.: Thermodynamic equilibrium of
organic-electrolyte mixtures in aerosol particles, Environmental and Energy Engineering, 48, 1331–1348, https://doi.org/10.1002/aic.690480619, 2002.
Mouchel-Vallon, C., Deguillaume, L., Monod, A., Perroux, H., Rose, C.,
Ghigo, G., Long, Y., Leriche, M., Aumont, B., Patryl, L., Armand, P., and
Chaumerliac, N.: CLEPS 1.0: A new protocol for cloud aqueous phase oxidation
of VOC mechanisms, Geosci. Model Dev., 10, 1339–1362, https://doi.org/10.5194/gmd-10-1339-2017, 2017.
Mukherji, S., Peters, C., and Weber, W.: Mass transfer of polynuclear
aromatic hydrocarbons from complex DNAPL mixtures, Environ. Sci. Technol.,
31, 416–423, https://doi.org/10.1021/es960227n, 1997.
Myhre, G., Shindell, D., Bréon, F.-M., Collins, W., Fuglestvedt, J.,
Huang, J., Koch, D., Lamarque, J.-F., Lee, D., Mendoza, B., Nakajima, T.,
Robock, A., Stephens, G., Takemura, T., and Zhang, H.: Anthropogenic and
natural radiative forcing, in: Climate Change 2013: The Physical Science
Basis, Contribution of Working Group I to the Fifth Assessment Report of the
Intergovernmental Panel on Climate Change, edited by: Stocker, T. F., Qin,
D., Plattner, G.-K., Tignor, M., Allen, S. K., Boschung, J., Nauels, A.,
Xia, Y., Bex, V., and Midgley, P. M., Cambridge, UK and New York, USA, 2013.
Nenes, A., Pandis, S. N., and Pilinis, C.: ISORROPIA: A New Thermodynamic
Equilibrium Model for Multiphase Multicomponent Inorganic Aerosols, Aquat.
Geochem., 4, 123–152, https://doi.org/10.1023/A:100960400,
1998.
Oelkers, E. H. and Helgeson, H. C.: Calculation of activity coefficients
and degrees of formation of neutral ion pairs in supercritical electrolyte
solutions, Geochim. Cosmochim. Ac., 55, 1235–1251, https://doi.org/10.1016/0016-7037(91)90303-M, 1991.
Pechtl, S., Schmitz, G., and von Glasow, R.: Modelling iodide-iodate
speciation in atmospheric aerosol: Contributions of inorganic and organic
iodine chemistry, Atmos. Chem. Phys., 7, 1381–1393, https://doi.org/10.5194/acp-7-1381-2007, 2007.
Pitzer, K. S.: Activity Coefficients in Electrolyte Solutions, CRC Press,
Boca Raton, 542 pp., 1991.
Pöschl, U.: Atmospheric aerosols: Composition, transformation, climate
and health effects, Angew. Chem. Int. Edit., 44, 7520–7540, https://doi.org/10.1002/anie.200501122, 2005.
Prausnitz, J. M., Lichtenthaler, R. N., and de Azevedo, E. G.: Molecular
Thermodynamics of Fluid-Phase Equilibria, Prentice Hall, Upper Saddle River,
New Jersey, 896 pp., 1998.
Raatikainen, T. and Laaksonen, A.: Application of several activity
coefficient models to water-organic-electrolyte aerosols of atmospheric
interest, Atmos. Chem. Phys., 5, 2475–2495, https://doi.org/10.5194/acp-5-2475-2005, 2005.
Ravishankara, A. R.: Heterogeneous and multiphase chemistry in the
troposphere, Science, 276, 1058–1065, https://doi.org/10.1126/science.276.5315.1058, 1997.
Rose, C., Chaumerliac, N., Deguillaume, L., Perroux, H., Mouchel-Vallon, C.,
Leriche, M., Patryl, L., and Armand, P.: Modeling the partitioning of
organic chemical species in cloud phases with CLEPS (1.1), Atmos. Chem.
Phys., 18, 2225–2242, https://doi.org/10.5194/acp-18-2225-2018,
2018.
Rusumdar, A. J., Wolke, R., Tilgner, A., and Herrmann, H.: Treatment of
non-ideality in the SPACCIM multiphase model – Part 1: Model development,
Geosci. Model Dev., 9, 247–281, https://doi.org/10.5194/gmd-9-247-2016, 2016.
Sander, R. and Crutzen, P. J.: Model study indicating halogen activation
and ozone destruction in polluted air masses transported to the sea, J.
Geophys. Res.-Atmos., 101, 9121–9138, https://doi.org/10.1029/95JD03793, 1996.
Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric
particles: A critical review of the literature and application of
thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57–109,
https://doi.org/10.1007/BF00053823, 1996.
Schwartz, S.: Mass-transport considerations pertinent to aqueous-phase reactions of gases in liquid-water clouds, in: Chemistry of Multiphase Atmospheric Systems, Springer, New York, 415–471, 1986.
Sehili, A. M., Wolke, R., Knoth, O., Simmel, M., Tilgner, A., and Herrmann, H.: Comparison of different model approaches for the simulation of multiphase processes, Atmos. Environ., 39, 4403–4417, https://doi.org/10.1016/j.atmosenv.2005.02.039, 2005.
Setchenow, M.: Action de l'acide carbonique sur les solutions des sels a
acides forts, Ann. Chim. Phys., 25, 226–270, 1892.
Shrivastava, M., Fast, J., Easter, R., Gustafson Jr, W., Zaveri, R. A.,
Jimenez, J. L., Saide, P., and Hodzic, A.: Modeling organic aerosols in a
megacity: comparison of simple and complex representations of the volatility
basis set approach, Atmos. Chem. Phys., 11, 6639–6662, https://doi.org/10.5194/acp-11-6639-2011, 2011.
Simmel, M., and Wurzler, S.: Condensation and activation in sectional cloud microphysical models, Atmos. Res., 80, 218–236, https://doi.org/10.1016/j.atmosres.2005.08.002, 2006.
Simmel, M., Diehl, K., and Wurzler, S.: Numerical simulation of the microphysics of an orographic cloud: Comparison with measurements and sensitivity studies, Atmos. Environ., 39, 4365–4373, https://doi.org/10.1016/j.atmosenv.2005.02.017, 2005.
Tilgner, A. and Herrmann, H.: Radical-driven carbonyl-to-acid conversion
and acid degradation in tropospheric aqueous systems studied by CAPRAM,
Atmos. Environ., 44, 5415–5422, https://doi.org/10.1016/j.atmosenv.2010.07.050, 2010.
Tilgner, A., Bräuer, P., Wolke, R., and Herrmann, H.: Modelling
multiphase chemistry in deliquescent aerosols and clouds using CAPRAM3.0i,
J. Atmos. Chem., 70, 221–256, https://doi.org/10.1007/s10874-013-9267-4, 2013.
van Pinxteren, D., Neusüß, C., and Herrmann, H.: On the abundance
and source contributions of dicarboxylic acids in size-resolved aerosol
particles at continental sites in central Europe, Atmos. Chem. Phys., 14,
3913–3928, https://doi.org/10.5194/acp-14-3913-2014, 2014.
Vogt, R., Crutzen, P. J., and Sander, R.: A mechanism for halogen release from sea-salt aerosol in the remote marine boundary layer, Nature, 383, 327–330, https://doi.org/10.1038/383327a0, 1996.
Vogt, R., Sander, R., Von Glasow, R., and Crutzen, P. J.: Iodine chemistry and its role in halogen activation and ozone loss in the marine boundary layer: A model study, J. Atmos Chem., 32, 375–395, https://doi.org/10.1023/A:1006179901037, 1999.
von Glasow, R. and Sander, R.: Variation of sea salt aerosol pH with
relative humidity, Geophys. Res. Lett., 28, 247–250, https://doi.org/10.1029/2000GL012387, 2001.
von Glasow, R., Sander, R., Bott, A., and Crutzen, P. J.: Modeling halogen
chemistry in the marine boundary layer – 2. Interactions with sulfur and the
cloud-covered MBL, J. Geophys. Res.-Atmos., 107, 4323, https://doi.org/10.1029/2001jd000943, 2002a.
von Glasow, R., Sander, R., Bott, A., and Crutzen, P. J.: Modeling halogen
chemistry in the marine boundary layer – 1. Cloud-free MBL, J. Geophys.
Res.-Atmos., 107, 4341, https://doi.org/10.1029/2001jd000942,
2002b.
von Glasow, R., von Kuhlmann, R., Lawrence, M. G., Platt, U., and Crutzen,
P. J.: Impact of reactive bromine chemistry in the troposphere, Atmos. Chem.
Phys., 4, 2481–2497, https://doi.org/10.5194/acp-4-2481-2004,
2004.
von Schneidemesser, E., Monks, P. S., Allan, J. D., Bruhwiler, L., Forster,
P., Fowler, D., Lauer, A., Morgan, W. T., Paasonen, P., Righi, M.,
Sindelarova, K., and Sutton, M. A.: Chemistry and the Linkages between Air
Quality and Climate Change, Chem. Rev., 115, 3856–3897, https://doi.org/10.1021/acs.chemrev.5b00089, 2015.
Walther, J. V.: Determination of activity coefficients of neutral species in
supercritical H2O solutions, Geochim. Cosmochim. Ac., 61, 3311–3318,
https://doi.org/10.1016/S0016-7037(97)00170-1, 1997.
Wolke, R. and Knoth, O.: Time-integration of multiphase chemistry in size-resolved cloud models, Appl. Numer. Math., 42, 473–487, https://doi.org/10.1016/S0168-9274(01)00169-6, 2002.
Wolke, R., Sehili, A. M., Simmel, M., Knoth, O., Tilgner, A., and Herrmann, H.: SPACCIM: A parcel model with detailed microphysics and complex multiphase chemistry, Atmos. Environ., 39, 4375–4388, https://doi.org/10.1016/j.atmosenv.2005.02.038, 2005.
Yan, W. D., Topphoff, M., Rose, C., and Gemhling, J.: Prediction of
vapor-liquid equilibria in mixed-solvent electrolyte systems using the group
contribution concept, Fluid Phase Equilibr., 162, 97–113,
https://doi.org/10.1016/S0378-3812(99)00201-0, 1999.
Yu, X. and Yu, R.: Setschenow Constant Prediction Based on the IEF-PCM
Calculations, Ind. Eng. Chem. Res., 52, 11182–11188, https://doi.org/10.1021/ie400001u, 2013.
Zaveri, R. A., Easter, R. C., and Peters, L. K.: A computationally efficient
Multicomponent Equilibrium Solver for Aerosols (MESA), J. Geophys.
Res.-Atmos., 110, D24203, https://doi.org/10.1029/2004JD005618,
2005a.
Zaveri, R. A., Easter, R. C., and Wexler, A. S.: A new method for
multicomponent activity coefficients of electrolytes in aqueous atmospheric
aerosols, J. Geophys. Res.-Atmos., 110, D02201, https://doi.org/10.1029/2004JD004681, 2005b.
Zhu, Y., Yang, L., Chen, J., Kawamura, K., Sato, M., Tilgner, A., van
Pinxteren, D., Chen, Y., Xue, L., Wang, X., Simpson, I. J., Herrmann, H.,
Blake, D. R., and Wang, W.: Molecular distributions of dicarboxylic acids,
oxocarboxylic acids and α-dicarbonyls in PM2.5 collected at the top
of Mt. Tai, North China, during the wheat burning season of 2014, Atmos.
Chem. Phys., 18, 10741–10758, https://doi.org/10.5194/acp-18-10741-2018, 2018.
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of
mixed organic-inorganic aerosols to predict activity coefficients, 8,
4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V.,
Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J.
H.: New and extended parameterization of the thermodynamic model AIOMFAC:
calculation of activity coefficients for organic-inorganic mixtures
containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and
aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
Short summary
In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are performed. The investigations aim at assessing the impact of a detailed treatment of non-ideality in multiphase models dealing with aqueous aerosol chemistry. The model studies demonstrate that the inclusion of non-ideality considerably affects the multiphase chemical processing of transition metal ions, oxidants, and related chemical subsystems such as organic chemistry in aqueous aerosols.
In the present study, simulations with the SPACCIM-SpactMod multiphase chemistry model are...
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