Articles | Volume 15, issue 10
https://doi.org/10.5194/acp-15-5585-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-5585-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Compilation and evaluation of gas phase diffusion coefficients of reactive trace gases in the atmosphere: Volume 2. Diffusivities of organic compounds, pressure-normalised mean free paths, and average Knudsen numbers for gas uptake calculations
Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
M. Shiraiwa
Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128, Mainz, Germany
U. Pöschl
Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128, Mainz, Germany
R. A. Cox
Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
M. Kalberer
CORRESPONDING AUTHOR
Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
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EGUsphere, https://doi.org/10.5194/egusphere-2026-3780, https://doi.org/10.5194/egusphere-2026-3780, 2026
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Matthias Kohl, Christoph Brühl, Holger Tost, Christos Xenofontos, Theodoros Christoudias, Sergey Gromov, Oliver Appel, Stephan Borrmann, Adam Bourassa, Pedro Campunzano-Jost, Yafang Cheng, Oliver Eppers, Karl D. Froyd, Bruna A. Holanda, Jose L. Jimenez, Patrick Jöckel, Philipp Joppe, Katharina Kaiser, Joseph M. Katich, Klaus Klingmüller, Franziska Köllner, Agnieszka Kupc, Anna Martin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Landon Rieger, Samuel Ruhl, Gregory P. Schill, Johannes Schneider, Christiane Schulz, Joshua P. Schwarz, Alexandra P. Tsimpidi, Ryan Vella, Christina J. Williamson, Yifan Yang, Daniel Zawada, Jos Lelieveld, and Andrea Pozzer
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Rui Li, Haley E. Plaas, Yifan Zhang, Yizhu Chen, Tianyu Zhang, Yi Yang, Sagar Rathod, Guohua Zhang, Xinming Wang, Douglas S. Hamilton, and Mingjin Tang
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Denis Leppla, Stefanie Hildmann, Nora Zannoni, Leslie A. Kremper, Bruna A. Holanda, Jonathan Williams, Christopher Pöhlker, Stefan Wolff, Marta Sà, Maria Christina Solci, Ulrich Pöschl, and Thorsten Hoffmann
Atmos. Chem. Phys., 26, 365–390, https://doi.org/10.5194/acp-26-365-2026, https://doi.org/10.5194/acp-26-365-2026, 2026
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Sebastian Brill, Björn Nillius, Jan-David Förster, Paulo Artaxo, Florian Ditas, Dennis Geis, Christian Gurk, Thomas Kenntner, Thomas Klimach, Mark Lamneck, Rafael Valiati, Bettina Weber, Stefan Wolff, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Meas. Tech., 19, 101–118, https://doi.org/10.5194/amt-19-101-2026, https://doi.org/10.5194/amt-19-101-2026, 2026
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Jianqiang Zhu, Guo Li, Uwe Kuhn, Bruno Backes Meller, Christopher Pöhlker, Paulo Artaxo, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 25, 17667–17684, https://doi.org/10.5194/acp-25-17667-2025, https://doi.org/10.5194/acp-25-17667-2025, 2025
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Tianyu Zhang, Yizhu Chen, Huanhuan Zhang, Lei Liu, Chengpeng Huang, Zhengyang Fang, Yifan Zhang, Fu Wang, Lan Luo, Guohua Zhang, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 25, 17091–17106, https://doi.org/10.5194/acp-25-17091-2025, https://doi.org/10.5194/acp-25-17091-2025, 2025
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Rafael Valiati, Bruno B. Meller, Marco A. Franco, Luciana V. Rizzo, Luiz A. T. Machado, Sebastian Brill, Bruna A. Holanda, Leslie A. Kremper, Subha S. Raj, Samara Carbone, Cléo Q. Dias-Júnior, Fernando G. Morais, Meinrat O. Andreae, Ulrich Pöschl, Christopher Pöhlker, and Paulo Artaxo
Atmos. Chem. Phys., 25, 14923–14944, https://doi.org/10.5194/acp-25-14923-2025, https://doi.org/10.5194/acp-25-14923-2025, 2025
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This study highlights the different aerosol populations that are commonly observed in the central Amazon. Vertical gradients of aerosol optical and chemical properties were evaluated on different atmospheric conditions, and showed distinct characteristics of these particles. Intercontinental transport events bring to the region particles with a contrasting chemical composition, while vertical transport processes influence the aerosol properties by promoting the development of coating and aging.
Mingjin Tang, Morgane M. G. Perron, Alex R. Baker, Rui Li, Andrew R. Bowie, Clifton S. Buck, Ashwini Kumar, Rachel Shelley, Simon J. Ussher, Robert Clough, Scott Meyerink, Prema P. Panda, Ashley T. Townsend, and Neil Wyatt
Atmos. Meas. Tech., 18, 6125–6141, https://doi.org/10.5194/amt-18-6125-2025, https://doi.org/10.5194/amt-18-6125-2025, 2025
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This work, initiated by the SCOR (Scientific Committee on Oceanic Research) Working Group 167, has examined eight leaching protocols commonly used in the literature, is the first large-scale international laboratory comparison for aerosol trace element leaching protocols.
Barbara Ervens, Ken S. Carslaw, Thomas Koop, and Ulrich Pöschl
Atmos. Chem. Phys., 25, 13903–13952, https://doi.org/10.5194/acp-25-13903-2025, https://doi.org/10.5194/acp-25-13903-2025, 2025
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Over 25 years, the European Geosciences Union (EGU) has demonstrated the success, viability and benefits of interactive open-access (OA) publishing with public peer review in its journals, its publishing platform EGUsphere and virtual compilations. The article summarizes the evolution of the EGU/Copernicus publications and of OA publishing with interactive public peer review at large by placing the EGU/Copernicus publications in the context of current and future global open science.
Matteo Krüger, Tommaso Galeazzo, Ivan Eremets, Bertil Schmidt, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Geosci. Model Dev., 18, 7357–7371, https://doi.org/10.5194/gmd-18-7357-2025, https://doi.org/10.5194/gmd-18-7357-2025, 2025
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This work uses machine learning to predict saturation vapor pressures of atmospherically-relevant organic compounds, crucial for partitioning of secondary organic aerosol (SOA). We introduce a new method using graph convolutional neural networks, in which molecular graphs enable the model to capture molecular connectivity better than with non-structural embeddings. The method shows strong agreement with experimentally determined vapor pressures, and outperforms existing estimation methods.
Yifan Zhang, Rui Li, Zachary B. Bunnell, Yizhu Chen, Guanhong Zhu, Jinlong Ma, Guohua Zhang, Tim M. Conway, and Mingjin Tang
Atmos. Chem. Phys., 25, 11067–11086, https://doi.org/10.5194/acp-25-11067-2025, https://doi.org/10.5194/acp-25-11067-2025, 2025
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The sources of aerosol Fe, especially soluble aerosol Fe, remain to be constrained. The stable isotope ratio of Fe has emerged as a potential tracer for discriminating and quantifying sources of aerosol Fe. In this review, we examine the state of the field for using Fe isotopes as an aerosol source tracer, and constraints on endmember signatures.
Laura M. D. Heinlein, Junwei He, Michael Oluwatoyin Sunday, Fangzhou Guo, James Campbell, Allison Moon, Sukriti Kapur, Ting Fang, Kasey Edwards, Meeta Cesler-Maloney, Alyssa J. Burns, Jack Dibb, William Simpson, Manabu Shiraiwa, Becky Alexander, Jingqiu Mao, James H. Flynn III, Jochen Stutz, and Cort Anastasio
Atmos. Chem. Phys., 25, 9561–9581, https://doi.org/10.5194/acp-25-9561-2025, https://doi.org/10.5194/acp-25-9561-2025, 2025
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Anni Hartikainen, Mika Ihalainen, Deeksha Shukla, Marius Rohkamp, Arya Mukherjee, Quanfu He, Sandra Piel, Aki Virkkula, Delun Li, Tuukka Kokkola, Seongho Jeong, Hanna Koponen, Uwe Etzien, Anusmita Das, Krista Luoma, Lukas Schwalb, Thomas Gröger, Alexandre Barth, Martin Sklorz, Thorsten Streibel, Hendryk Czech, Benedikt Gündling, Markus Kalberer, Bert Buchholz, Andreas Hupfer, Thomas Adam, Thorsten Hohaus, Johan Øvrevik, Ralf Zimmermann, and Olli Sippula
Atmos. Chem. Phys., 25, 9275–9294, https://doi.org/10.5194/acp-25-9275-2025, https://doi.org/10.5194/acp-25-9275-2025, 2025
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Photochemical reactions altered the properties of kerosene-operated jet engine burner exhaust emissions, which were studied in a laboratory using an oxidation flow reactor. Particle mass increased 300-fold as particles and gases became more oxidized. Light absorption increased, but the total direct radiative forcing efficiency was estimated to have shifted from positive to negative. The results highlight the importance of considering secondary aerosol formation when assessing the impacts of aviation.
Sara L. Farrell, Quazi Z. Rasool, Havala O. T. Pye, Yue Zhang, Ying Li, Yuzhi Chen, Chi-Tsan Wang, Haofei Zhang, Ryan Schmedding, Manabu Shiraiwa, Jaime Greene, Sri H. Budisulistiorini, Jose L. Jimenez, Weiwei Hu, Jason D. Surratt, and William Vizuete
EGUsphere, https://doi.org/10.5194/egusphere-2025-2253, https://doi.org/10.5194/egusphere-2025-2253, 2025
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Fine particulate matter (PM2.5) has become increasingly important to regulate and model. In this study, we parameterize non-ideal aerosol mixing and phase state into the Community Multiscale Air Quality (CMAQ) model and analyze its impact on the formation of a globally important source of PM2.5, isoprene epoxydiol (IEPOX)-derived PM2.5. Incorporating these features furthers model bias in IEPOX-derived PM2.5, however, this work provides potential phase state bounds for future PM2.5 modeling work.
Yue Sun, Yujiao Zhu, Hengde Liu, Lanxiadi Chen, Hongyong Li, Yujian Bi, Di Wu, Xiangkun Yin, Can Cui, Ping Liu, Yu Yang, Jisheng Zhang, Yanqiu Nie, Lanxin Zhang, Jiangshan Mu, Yuhong Liu, Zhaoxin Guo, Qinyi Li, Yuqiang Zhang, Xinfeng Wang, Mingjin Tang, Wenxing Wang, and Likun Xue
EGUsphere, https://doi.org/10.5194/egusphere-2025-2855, https://doi.org/10.5194/egusphere-2025-2855, 2025
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Rainwater samples collected at the summit of Mount Tai were analyzed for ice-nucleating particles (INPs). Our findings revealed that INP concentrations peaked in spring, driven predominantly by long-range transport of dust aerosols. Mineral dust contributed 43.6 % of annual INPs, with its contribution rising sharply to 71.7 % in spring. Satellite observations further revealed that the long-range transport of dust in spring promotes large-scale cloud formation over the NCP region.
Benjamin Gfeller, Mariia Becker, Adrian D. Aebi, Nicolas Bukowiecki, Marcus Wyss, and Markus Kalberer
Aerosol Research, 3, 351–369, https://doi.org/10.5194/ar-3-351-2025, https://doi.org/10.5194/ar-3-351-2025, 2025
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Metal nanoparticles (Au, Pt, Cu and Ni) were generated in the aerosol phase using spark ablation and analysed for size, shape and number concentration. Particles as small as 1 nm and up to > 60 nm show shapes from fully spherical to fractal-like as characterized by electron microscopy. Furthermore, the metal particles were mixed with TiO2 nanoparticles, and the number and size of metal particles coating the TiO2 were determined.
Kevin Kilchhofer, Alexandre Barth, Battist Utinger, Markus Kalberer, and Markus Ammann
Aerosol Research, 3, 337–349, https://doi.org/10.5194/ar-3-337-2025, https://doi.org/10.5194/ar-3-337-2025, 2025
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We report a substantial buildup of reactive molecules (due to sunlight) in organic particulate matter, causing adverse health effects. Metals, which occur naturally or are emitted by traffic, can complex with organic materials and initiate photochemical processes. At low humidity, organic particles may become highly viscous, which allows for the accumulation of reactive species. We found that copper acts as an reducing species to remove some of these harmful species from particles.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
Atmos. Chem. Phys., 25, 5087–5100, https://doi.org/10.5194/acp-25-5087-2025, https://doi.org/10.5194/acp-25-5087-2025, 2025
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that the illumination of brown carbon can rapidly form HOOH within particles, even under the low-sunlight conditions of Fairbanks, Alaska, during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Battist Utinger, Alexandre Barth, Andreas Paul, Arya Mukherjee, Steven John Campbell, Christa-Maria Müller, Mika Ihalainen, Pasi Yli-Pirilä, Miika Kortelainen, Zheng Fang, Patrick Martens, Markus Somero, Juho Louhisalmi, Thorsten Hohaus, Hendryk Czech, Olli Sippula, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Aerosol Research, 3, 205–218, https://doi.org/10.5194/ar-3-205-2025, https://doi.org/10.5194/ar-3-205-2025, 2025
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The oxidative potential (OP) of air pollution particles might be a metric explaining particle toxicity. This study quantifies the OP of fresh and aged car and wood burning emission particles and explores how the OP changes over time, using novel high-temporal-resolution instruments. We show that emissions from wood burning are more toxic than car exhaust per unit particle mass, especially as they age in the atmosphere. We also calculate emission factors for the OP, which could help to improve air pollution policies.
Mega Octaviani, Benjamin A. Musa Bandowe, Qing Mu, Jake Wilson, Holger Tost, Hang Su, Yafang Cheng, Manabu Shiraiwa, Ulrich Pöschl, Thomas Berkemeier, and Gerhard Lammel
EGUsphere, https://doi.org/10.5194/egusphere-2025-186, https://doi.org/10.5194/egusphere-2025-186, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This research explores the atmospheric concentration of benzo(a)pyrene (BaP), a harmful air pollutant linked to lung cancer. Using advanced Earth system modeling, the study examines how BaP's degradation varies with temperature and humidity, affecting its global distribution and associated lung cancer risks. The findings reveal that BaP persists longer in colder, less humid regions, leading to higher lung cancer risks in parts of Europe and Asia.
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.
Florian Wieland, Nadine Bothen, Ralph Schwidetzky, Teresa M. Seifried, Paul Bieber, Ulrich Pöschl, Konrad Meister, Mischa Bonn, Janine Fröhlich-Nowoisky, and Hinrich Grothe
Biogeosciences, 22, 103–115, https://doi.org/10.5194/bg-22-103-2025, https://doi.org/10.5194/bg-22-103-2025, 2025
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Betula pendula is a widespread birch tree species containing ice nucleation agents that can trigger the freezing of cloud droplets and thereby alter the evolution of clouds. Our study identifies three distinct ice-nucleating macromolecule (INM) aggregates of varying size that can nucleate ice at temperatures up to –5.4°C. Our findings suggest that these vegetation-derived particles may influence atmospheric processes, weather, and climate more strongly than previously thought.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 8893–8910, https://doi.org/10.5194/acp-24-8893-2024, https://doi.org/10.5194/acp-24-8893-2024, 2024
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Composite analysis of gas concentration before and after rainfall, during the day and night, gives insight into the complex relationship between trace gas variability and precipitation. The analysis helps us to understand the sources and sinks of trace gases within a forest ecosystem. It elucidates processes that are not discernible under undisturbed conditions and contributes to a deeper understanding of the trace gas life cycle and its intricate interactions with cloud dynamics in the Amazon.
Marco A. Franco, Rafael Valiati, Bruna A. Holanda, Bruno B. Meller, Leslie A. Kremper, Luciana V. Rizzo, Samara Carbone, Fernando G. Morais, Janaína P. Nascimento, Meinrat O. Andreae, Micael A. Cecchini, Luiz A. T. Machado, Milena Ponczek, Ulrich Pöschl, David Walter, Christopher Pöhlker, and Paulo Artaxo
Atmos. Chem. Phys., 24, 8751–8770, https://doi.org/10.5194/acp-24-8751-2024, https://doi.org/10.5194/acp-24-8751-2024, 2024
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The Amazon wet-season atmosphere was studied at the Amazon Tall Tower Observatory site, revealing vertical variations (between 60 and 325 m) in natural aerosols. Daytime mixing contrasted with nighttime stratification, with distinct rain-induced changes in aerosol populations. Notably, optical property recovery at higher levels was faster, while near-canopy aerosols showed higher scattering efficiency. These findings enhance our understanding of aerosol impacts on climate dynamics.
Rui Li, Prema Piyusha Panda, Yizhu Chen, Zhenming Zhu, Fu Wang, Yujiao Zhu, He Meng, Yan Ren, Ashwini Kumar, and Mingjin Tang
Atmos. Meas. Tech., 17, 3147–3156, https://doi.org/10.5194/amt-17-3147-2024, https://doi.org/10.5194/amt-17-3147-2024, 2024
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We found that for ultrapure water batch leaching, the difference in specific experimental parameters, including agitation methods, filter pore size, and contact time, only led to a small and sometimes insignificant difference in determined aerosol trace element solubility. Furthermore, aerosol trace element solubility determined using four common ultrapure water leaching protocols showed good agreement.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Gabriela R. Unfer, Luiz A. T. Machado, Paulo Artaxo, Marco A. Franco, Leslie A. Kremper, Mira L. Pöhlker, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 3869–3882, https://doi.org/10.5194/acp-24-3869-2024, https://doi.org/10.5194/acp-24-3869-2024, 2024
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Amazonian aerosols and their interactions with precipitation were studied by understanding them in a 3D space based on three parameters that characterize the concentration and size distribution of aerosols. The results showed characteristic arrangements regarding seasonal and diurnal cycles, as well as when interacting with precipitation. The use of this 3D space appears to be a promising tool for aerosol population analysis and for model validation and parameterization.
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.
Yue Sun, Yujiao Zhu, Yanbin Qi, Lanxiadi Chen, Jiangshan Mu, Ye Shan, Yu Yang, Yanqiu Nie, Ping Liu, Can Cui, Ji Zhang, Mingxuan Liu, Lingli Zhang, Yufei Wang, Xinfeng Wang, Mingjin Tang, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 24, 3241–3256, https://doi.org/10.5194/acp-24-3241-2024, https://doi.org/10.5194/acp-24-3241-2024, 2024
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Field observations were conducted at the summit of Changbai Mountain in northeast Asia. The cumulative number concentration of ice-nucleating particles (INPs) varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 ℃. Biological INPs (bio-INPs) accounted for the majority of INPs, and the proportion exceeded 90% above −13.0 ℃. Planetary boundary layer height, valley breezes, and long-distance transport of air mass influence the abundance of bio-INPs.
Zhanyu Su, Lanxiadi Chen, Yuan Liu, Peng Zhang, Tianzeng Chen, Biwu Chu, Mingjin Tang, Qingxin Ma, and Hong He
Atmos. Chem. Phys., 24, 993–1003, https://doi.org/10.5194/acp-24-993-2024, https://doi.org/10.5194/acp-24-993-2024, 2024
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In this study, different soot particles were analyzed to better understand their behavior. It was discovered that water-soluble substances in soot facilitate water adsorption at low humidity while increasing the number of water layers at high humidity. Soot from organic fuels exhibits hygroscopicity influenced by organic carbon and microstructure. Additionally, the presence of sulfate ions due to the oxidation of SO2 enhances soot's hygroscopicity.
Morgane M. G. Perron, Susanne Fietz, Douglas S. Hamilton, Akinori Ito, Rachel U. Shelley, and Mingjin Tang
Atmos. Meas. Tech., 17, 165–166, https://doi.org/10.5194/amt-17-165-2024, https://doi.org/10.5194/amt-17-165-2024, 2024
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The solubility of vital and toxic trace elements delivered by the atmosphere determines their potential to fertilise or limit ocean productivity. A poor understanding of aeolian trace element solubility and the absence of a standard method to define this parameter hinder accurate model representation of the impact of atmospheric deposition on ocean productivity in a changing climate. The inter-journal special issue aims at “Reducing Uncertainty in Soluble aerosol Trace Element Deposition”.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
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.
Najin Kim, Hang Su, Nan Ma, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 16, 2771–2780, https://doi.org/10.5194/amt-16-2771-2023, https://doi.org/10.5194/amt-16-2771-2023, 2023
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We propose a multiple-charging correction algorithm for a broad-supersaturation scanning cloud condensation nuclei (BS2-CCN) system which can obtain high time-resolution aerosol hygroscopicity and CCN activity. The correction algorithm aims at deriving the activation fraction's true value for each particle size. The meaningful differences between corrected and original κ values (single hygroscopicity parameter) emphasize the correction algorithm's importance for ambient aerosol measurement.
Battist Utinger, Steven John Campbell, Nicolas Bukowiecki, Alexandre Barth, Benjamin Gfeller, Ray Freshwater, Hans-Rudolf Rüegg, and Markus Kalberer
Atmos. Meas. Tech., 16, 2641–2654, https://doi.org/10.5194/amt-16-2641-2023, https://doi.org/10.5194/amt-16-2641-2023, 2023
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Exposure to atmospheric aerosols can lead to adverse health effect, but particle components responsible for this are unknown. Redox-active compounds, some with very short lifetimes, are considered to be a toxic class of compounds in particles. We developed the first online field instrument to quantify short-lived and stable redox-active compounds with a physiological assay based on ascorbic acid and a high time resolution and detection limits to allow measurements at unpolluted locations.
Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774, https://doi.org/10.5194/acp-23-4763-2023, https://doi.org/10.5194/acp-23-4763-2023, 2023
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We investigate the hygroscopic behavior of levoglucosan and D-glucose nanoparticles using a nano-HTDMA. There is a weak size dependence of the hygroscopic growth factor of levoglucosan and D-glucose with diameters down to 20 nm, while a strong size dependence of the hygroscopic growth factor of D-glucose has been clearly observed in the size range 6 to 20 nm. The use of the DKA method leads to good agreement with the hygroscopic growth factor of glucose nanoparticles with diameters down to 6 nm.
Thomas Berkemeier, Matteo Krüger, Aryeh Feinberg, Marcel Müller, Ulrich Pöschl, and Ulrich K. Krieger
Geosci. Model Dev., 16, 2037–2054, https://doi.org/10.5194/gmd-16-2037-2023, https://doi.org/10.5194/gmd-16-2037-2023, 2023
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Kinetic multi-layer models (KMs) successfully describe heterogeneous and multiphase atmospheric chemistry. In applications requiring repeated execution, however, these models can be too expensive. We trained machine learning surrogate models on output of the model KM-SUB and achieved high correlations. The surrogate models run orders of magnitude faster, which suggests potential applicability in global optimization tasks and as sub-modules in large-scale atmospheric models.
Huanhuan Zhang, Rui Li, Chengpeng Huang, Xiaofei Li, Shuwei Dong, Fu Wang, Tingting Li, Yizhu Chen, Guohua Zhang, Yan Ren, Qingcai Chen, Ru-jin Huang, Siyu Chen, Tao Xue, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 23, 3543–3559, https://doi.org/10.5194/acp-23-3543-2023, https://doi.org/10.5194/acp-23-3543-2023, 2023
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This work investigated the seasonal variation of aerosol Fe solubility for coarse and fine particles in Xi’an, a megacity in northwestern China severely affected by anthropogenic emission and desert dust aerosol. In addition, we discussed in depth what controlled aerosol Fe solubility at different seasons for coarse and fine particles.
Haley M. Royer, Mira L. Pöhlker, Ovid Krüger, Edmund Blades, Peter Sealy, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Andrew P. Ault, Patricia K. Quinn, Paquita Zuidema, Christopher Pöhlker, Ulrich Pöschl, Meinrat Andreae, and Cassandra J. Gaston
Atmos. Chem. Phys., 23, 981–998, https://doi.org/10.5194/acp-23-981-2023, https://doi.org/10.5194/acp-23-981-2023, 2023
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This paper presents atmospheric particle chemical composition and measurements of aerosol water uptake properties collected at Ragged Point, Barbados, during the winter of 2020. The result of this study indicates the importance of small African smoke particles for cloud droplet formation in the tropical North Atlantic and highlights the large spatial and temporal pervasiveness of smoke over the Atlantic Ocean.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
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Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Guo Li, Hang Su, Meng Li, Uwe Kuhn, Guangjie Zheng, Lei Han, Fengxia Bao, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 15, 6433–6446, https://doi.org/10.5194/amt-15-6433-2022, https://doi.org/10.5194/amt-15-6433-2022, 2022
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A large fraction of previous work using dynamic flow chambers was to quantify gas exchange in terms of flux or deposition/emission rate. Here, we extended the usage of this technique to examine uptake kinetics on sample surfaces. The good performance of the chamber system was validated. This technique can be further used for liquid samples and real atmospheric aerosol samples without complicated coating procedures, which complements the existing techniques in atmospheric kinetic studies.
Kanishk Gohil, Chun-Ning Mao, Dewansh Rastogi, Chao Peng, Mingjin Tang, and Akua Asa-Awuku
Atmos. Chem. Phys., 22, 12769–12787, https://doi.org/10.5194/acp-22-12769-2022, https://doi.org/10.5194/acp-22-12769-2022, 2022
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The Hybrid Activity Model (HAM) is a promising new droplet growth model that can be potentially used for the analysis of any type of atmospheric compound. HAM may potentially improve the representation of hygroscopicity of organic aerosols in large-scale global climate models (GCMs), hence reducing the uncertainties in the climate forcing due to the aerosol indirect effect.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
Guohua Zhang, Xiaodong Hu, Wei Sun, Yuxiang Yang, Ziyong Guo, Yuzhen Fu, Haichao Wang, Shengzhen Zhou, Lei Li, Mingjin Tang, Zongbo Shi, Duohong Chen, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 22, 9571–9582, https://doi.org/10.5194/acp-22-9571-2022, https://doi.org/10.5194/acp-22-9571-2022, 2022
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We show a significant enhancement of nitrate mass fraction in cloud water and relative intensity of nitrate in the cloud residual particles and highlight that hydrolysis of N2O5 serves as the critical route for the in-cloud formation of nitrate, even during the daytime. Given that N2O5 hydrolysis acts as a major sink of NOx in the atmosphere, further model updates may improve our understanding about the processes contributing to nitrate production in cloud and the cycling of odd nitrogen.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Marco A. Franco, Florian Ditas, Leslie A. Kremper, Luiz A. T. Machado, Meinrat O. Andreae, Alessandro Araújo, Henrique M. J. Barbosa, Joel F. de Brito, Samara Carbone, Bruna A. Holanda, Fernando G. Morais, Janaína P. Nascimento, Mira L. Pöhlker, Luciana V. Rizzo, Marta Sá, Jorge Saturno, David Walter, Stefan Wolff, Ulrich Pöschl, Paulo Artaxo, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 3469–3492, https://doi.org/10.5194/acp-22-3469-2022, https://doi.org/10.5194/acp-22-3469-2022, 2022
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In Central Amazonia, new particle formation in the planetary boundary layer is rare. Instead, there is the appearance of sub-50 nm aerosols with diameters larger than about 20 nm that eventually grow to cloud condensation nuclei size range. Here, 254 growth events were characterized which have higher predominance in the wet season. About 70 % of them showed direct relation to convective downdrafts, while 30 % occurred partly under clear-sky conditions, evidencing still unknown particle sources.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Kai Tang, Beatriz Sánchez-Parra, Petya Yordanova, Jörn Wehking, Anna T. Backes, Daniel A. Pickersgill, Stefanie Maier, Jean Sciare, Ulrich Pöschl, Bettina Weber, and Janine Fröhlich-Nowoisky
Biogeosciences, 19, 71–91, https://doi.org/10.5194/bg-19-71-2022, https://doi.org/10.5194/bg-19-71-2022, 2022
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Metagenomic sequencing and freezing experiments of aerosol samples collected on Cyprus revealed rain-related short-term changes of bioaerosol and ice nuclei composition. Filtration experiments showed a rain-related enhancement of biological ice nuclei > 5 µm and < 0.1 µm. The observed effects of rainfall on the composition of atmospheric bioaerosols and ice nuclei may influence the hydrological cycle as well as the health effects of air particulate matter (pathogens, allergens).
Luiz A. T. Machado, Marco A. Franco, Leslie A. Kremper, Florian Ditas, Meinrat O. Andreae, Paulo Artaxo, Micael A. Cecchini, Bruna A. Holanda, Mira L. Pöhlker, Ivan Saraiva, Stefan Wolff, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 21, 18065–18086, https://doi.org/10.5194/acp-21-18065-2021, https://doi.org/10.5194/acp-21-18065-2021, 2021
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Several studies evaluate aerosol–cloud interactions, but only a few attempted to describe how clouds modify aerosol properties. This study evaluates the effect of weather events on the particle size distribution at the ATTO, combining remote sensing and in situ data. Ultrafine, Aitken and accumulation particles modes have different behaviors for the diurnal cycle and for rainfall events. This study opens up new scientific questions that need to be pursued in detail in new field campaigns.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
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Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Najin Kim, Yafang Cheng, Nan Ma, Mira L. Pöhlker, Thomas Klimach, Thomas F. Mentel, Ovid O. Krüger, Ulrich Pöschl, and Hang Su
Atmos. Meas. Tech., 14, 6991–7005, https://doi.org/10.5194/amt-14-6991-2021, https://doi.org/10.5194/amt-14-6991-2021, 2021
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A broad supersaturation scanning CCN (BS2-CCN) system, in which particles are exposed to a range of supersaturation simultaneously, can measure a broad range of CCN activity distribution with a high time resolution. We describe how the BS2-CCN system can be effectively calibrated and which factors can affect the calibration curve. Intercomparison experiments between typical DMA-CCN and BS2-CCN measurements to evaluate the BS2-CCN system showed high correlation and good agreement.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
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Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
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