Articles | Volume 25, issue 22
https://doi.org/10.5194/acp-25-16533-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-25-16533-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
24 Nov 2025
Research article |
| 24 Nov 2025
Organic aerosols mixing across the tropopause and its implication for anthropogenic pollution of the UTLS
Anna Breuninger
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Frankfurt Isotope and Element Research Center (FIERCE), Goethe University Frankfurt, Frankfurt am Main, Germany
Philipp Joppe
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Aerosol Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Jonas Wilsch
Aerosol Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Cornelis Schwenk
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Heiko Bozem
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Nicolas Emig
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Laurin Merkel
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Rainer Rossberg
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Timo Keber
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Arthur Kutschka
enviscope GmbH, Messtechnik für Umweltforschung, Frankfurt am Main, Germany
Philipp Waleska
enviscope GmbH, Messtechnik für Umweltforschung, Frankfurt am Main, Germany
Stefan Hofmann
enviscope GmbH, Messtechnik für Umweltforschung, Frankfurt am Main, Germany
Sarah Richter
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Florian Ungeheuer
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Konstantin Dörholt
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Thorsten Hoffmann
Department of Chemistry, Johannes Gutenberg University Mainz, Mainz, Germany
Annette Miltenberger
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Johannes Schneider
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Aerosol Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany
Peter Hoor
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Alexander L. Vogel
CORRESPONDING AUTHOR
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany
Frankfurt Isotope and Element Research Center (FIERCE), Goethe University Frankfurt, Frankfurt am Main, Germany
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Markus Jesswein, Valentin Lauther, Nicolas Emig, Peter Hoor, Timo Keber, Hans-Christoph Lachnitt, Linda Ort, Tanja Schuck, Johannes Strobel, Ronja Van Luijt, C. Michael Volk, Franziska Weyland, and Andreas Engel
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André Ehrlich, Susanne Crewell, Andreas Herber, Marcus Klingebiel, Christof Lüpkes, Mario Mech, Sebastian Becker, Stephan Borrmann, Heiko Bozem, Matthias Buschmann, Hans-Christian Clemen, Elena De La Torre Castro, Henning Dorff, Regis Dupuy, Oliver Eppers, Florian Ewald, Geet George, Andreas Giez, Sarah Grawe, Christophe Gourbeyre, Jörg Hartmann, Evelyn Jäkel, Philipp Joppe, Olivier Jourdan, Zsófia Jurányi, Benjamin Kirbus, Johannes Lucke, Anna E. Luebke, Maximilian Maahn, Nina Maherndl, Christian Mallaun, Johanna Mayer, Stephan Mertes, Guillaume Mioche, Manuel Moser, Hanno Müller, Veronika Pörtge, Nils Risse, Greg Roberts, Sophie Rosenburg, Johannes Röttenbacher, Michael Schäfer, Jonas Schaefer, Andreas Schäfler, Imke Schirmacher, Johannes Schneider, Sabrina Schnitt, Frank Stratmann, Christian Tatzelt, Christiane Voigt, Andreas Walbröl, Anna Weber, Bruno Wetzel, Martin Wirth, and Manfred Wendisch
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Paul Konopka, Felix Ploeger, Francesco D'Amato, Teresa Campos, Marc von Hobe, Shawn B. Honomichl, Peter Hoor, Laura L. Pan, Michelle L. Santee, Silvia Viciani, Kaley A. Walker, and Michaela I. Hegglin
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We present an improved version of the Chemical Lagrangian Model of the Stratosphere (CLaMS-3.0), which better represents transport from the lower atmosphere to the upper troposphere and lower stratosphere. By refining grid resolution and improving convection representation, the model more accurately simulates carbon monoxide transport. Comparisons with satellite and in situ observations highlight its ability to capture seasonal variations and improve our understanding of atmospheric transport.
Denis Leppla, Stefanie Hildmann, Nora Zannoni, Leslie Kremper, Bruna Hollanda, Jonathan Williams, Christopher Pöhlker, Stefan Wolff, Marta Sà, Maria Cristina Solci, Ulrich Pöschl, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-141, https://doi.org/10.5194/egusphere-2025-141, 2025
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Franziska Weyland, Peter Hoor, Daniel Kunkel, Thomas Birner, Felix Plöger, and Katharina Turhal
Atmos. Chem. Phys., 25, 1227–1252, https://doi.org/10.5194/acp-25-1227-2025, https://doi.org/10.5194/acp-25-1227-2025, 2025
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The lowermost stratosphere (LMS) plays an important role in the Earth's climate, containing strong gradients of ozone and water vapor. Our results indicate that the thermodynamic structure of the LMS was changing between 1979–2019 in response to anthropogenic climate change and the recovery of stratospheric ozone, also indicating large-scale circulation changes. We find that both the upper and the lower LMS boundaries show an (upward) trend, which has implications for the LMS mass.
Johanna Schäfer, Anja Beschnitt, François Burgay, Thomas Singer, Margit Schwikowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 18, 421–430, https://doi.org/10.5194/amt-18-421-2025, https://doi.org/10.5194/amt-18-421-2025, 2025
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Glaciers preserve organic compounds from atmospheric aerosols, which can serve as markers for emission sources. Most studies overlook the enantiomers of chiral compounds. We developed a two-dimensional liquid chromatography method to determine the chiral ratios of the monoterpene oxidation products cis-pinic acid and cis-pinonic acid in ice-core samples. Applied to samples from the Belukha Glacier (1870–1970 CE), the method revealed fluctuating chiral ratios for the analytes.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Christine Borchers, Lasse Moormann, Bastien Geil, Niklas Karbach, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-4015, https://doi.org/10.5194/egusphere-2024-4015, 2025
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A three-dimensionally printed filter holder is connected to a lightweight, high-performance pump. This sampling system allows for easy and cost-effective measurements of organic aerosols at different heights and locations. By elucidating the chemical composition of organic aerosol, sources and processing of the compounds can be identified. Measurements at different altitudes and times of the day provide insight into the chemical aging and daytime trends of the aerosol particles.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
Atmos. Chem. Phys., 25, 425–439, https://doi.org/10.5194/acp-25-425-2025, https://doi.org/10.5194/acp-25-425-2025, 2025
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This study provides laboratory evidence that the photosensitizers in biomass burning extracts can enhance sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air conditions, with a lower contribution of direct photosensitization via triplets.
Cornelis Schwenk and Annette Miltenberger
Atmos. Chem. Phys., 24, 14073–14099, https://doi.org/10.5194/acp-24-14073-2024, https://doi.org/10.5194/acp-24-14073-2024, 2024
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Warm conveyor belts (WCBs) transport moisture into the upper atmosphere, where it acts as a greenhouse gas. This transport is not well understood, and the role of rapidly rising air is unclear. We simulate a WCB and look at fast- and slow-rising air to see how moisture is (differently) transported. We find that for fast-ascending air more ice particles reach higher into the atmosphere and that frozen cloud particles are removed differently than during slow ascent, which has more water vapour.
Christine Borchers, Jackson Seymore, Martanda Gautam, Konstantin Dörholt, Yannik Müller, Andreas Arndt, Laura Gömmer, Florian Ungeheuer, Miklós Szakáll, Stephan Borrmann, Alexander Theis, Alexander L. Vogel, and Thorsten Hoffmann
Atmos. Chem. Phys., 24, 13961–13974, https://doi.org/10.5194/acp-24-13961-2024, https://doi.org/10.5194/acp-24-13961-2024, 2024
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Riming, a crucial process in cloud dynamics, influences the vertical distribution of compounds in the atmosphere. Experiments in Mainz's wind tunnel investigated retention coefficients of organic compounds under varying conditions. Findings suggest a correlation between the Henry's law constant and retention, applicable even to complex organic molecules.
Katharina Turhal, Felix Plöger, Jan Clemens, Thomas Birner, Franziska Weyland, Paul Konopka, and Peter Hoor
Atmos. Chem. Phys., 24, 13653–13679, https://doi.org/10.5194/acp-24-13653-2024, https://doi.org/10.5194/acp-24-13653-2024, 2024
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The tropopause separates the troposphere, where many greenhouse gases originate, from the stratosphere. This study examines a tropopause defined by potential vorticity – an analogue for angular momentum that changes sharply in the subtropics, creating a transport barrier. Between 1980 and 2017, this tropopause shifted poleward at lower altitudes and equatorward above, suggesting height-dependent changes in atmospheric circulation that may affect greenhouse gas distribution and global warming.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Manfred Wendisch, Susanne Crewell, André Ehrlich, Andreas Herber, Benjamin Kirbus, Christof Lüpkes, Mario Mech, Steven J. Abel, Elisa F. Akansu, Felix Ament, Clémantyne Aubry, Sebastian Becker, Stephan Borrmann, Heiko Bozem, Marlen Brückner, Hans-Christian Clemen, Sandro Dahlke, Georgios Dekoutsidis, Julien Delanoë, Elena De La Torre Castro, Henning Dorff, Regis Dupuy, Oliver Eppers, Florian Ewald, Geet George, Irina V. Gorodetskaya, Sarah Grawe, Silke Groß, Jörg Hartmann, Silvia Henning, Lutz Hirsch, Evelyn Jäkel, Philipp Joppe, Olivier Jourdan, Zsofia Jurányi, Michail Karalis, Mona Kellermann, Marcus Klingebiel, Michael Lonardi, Johannes Lucke, Anna E. Luebke, Maximilian Maahn, Nina Maherndl, Marion Maturilli, Bernhard Mayer, Johanna Mayer, Stephan Mertes, Janosch Michaelis, Michel Michalkov, Guillaume Mioche, Manuel Moser, Hanno Müller, Roel Neggers, Davide Ori, Daria Paul, Fiona M. Paulus, Christian Pilz, Felix Pithan, Mira Pöhlker, Veronika Pörtge, Maximilian Ringel, Nils Risse, Gregory C. Roberts, Sophie Rosenburg, Johannes Röttenbacher, Janna Rückert, Michael Schäfer, Jonas Schaefer, Vera Schemann, Imke Schirmacher, Jörg Schmidt, Sebastian Schmidt, Johannes Schneider, Sabrina Schnitt, Anja Schwarz, Holger Siebert, Harald Sodemann, Tim Sperzel, Gunnar Spreen, Bjorn Stevens, Frank Stratmann, Gunilla Svensson, Christian Tatzelt, Thomas Tuch, Timo Vihma, Christiane Voigt, Lea Volkmer, Andreas Walbröl, Anna Weber, Birgit Wehner, Bruno Wetzel, Martin Wirth, and Tobias Zinner
Atmos. Chem. Phys., 24, 8865–8892, https://doi.org/10.5194/acp-24-8865-2024, https://doi.org/10.5194/acp-24-8865-2024, 2024
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The Arctic is warming faster than the rest of the globe. Warm-air intrusions (WAIs) into the Arctic may play an important role in explaining this phenomenon. Cold-air outbreaks (CAOs) out of the Arctic may link the Arctic climate changes to mid-latitude weather. In our article, we describe how to observe air mass transformations during CAOs and WAIs using three research aircraft instrumented with state-of-the-art remote-sensing and in situ measurement devices.
Luis F. Millán, Peter Hoor, Michaela I. Hegglin, Gloria L. Manney, Harald Boenisch, Paul Jeffery, Daniel Kunkel, Irina Petropavlovskikh, Hao Ye, Thierry Leblanc, and Kaley Walker
Atmos. Chem. Phys., 24, 7927–7959, https://doi.org/10.5194/acp-24-7927-2024, https://doi.org/10.5194/acp-24-7927-2024, 2024
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In the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we have mapped multiplatform ozone datasets into coordinate systems to systematically evaluate the influence of these coordinates on binned climatological variability. This effort unifies the work of studies that focused on individual coordinate system variability. Our goal was to create the most comprehensive assessment of this topic.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
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The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, and Stephan Borrmann
Atmos. Chem. Phys., 24, 7499–7522, https://doi.org/10.5194/acp-24-7499-2024, https://doi.org/10.5194/acp-24-7499-2024, 2024
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From aircraft measurements in the upper troposphere/lower stratosphere, we find a correlation between the ozone and particulate sulfate in the lower stratosphere. The correlation exhibits some variability over the measurement period exceeding the background sulfate-to-ozone correlation. From our analysis, we conclude that gas-to-particle conversion of volcanic sulfur dioxide leads to observed enhanced sulfate aerosol mixing ratios.
Edward Groot, Patrick Kuntze, Annette Miltenberger, and Holger Tost
Weather Clim. Dynam., 5, 779–803, https://doi.org/10.5194/wcd-5-779-2024, https://doi.org/10.5194/wcd-5-779-2024, 2024
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Deep convective clouds (thunderstorms), which may cause severe weather, tend to coherently organise into structured cloud systems. Accurate representation of these systems in models is difficult due to their complex dynamics and, in numerical simulations, the dependence of their dynamics on resolution. Here, the effect of convective organisation and geometry on their outflow winds (altitudes of 7–14 km) is investigated. Representation of their dynamics and outflows improves at higher resolution.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-516, https://doi.org/10.5194/egusphere-2024-516, 2024
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This study assesses atmospheric composition using air quality models during aircraft campaigns in Europe and Asia, focusing on carbonaceous aerosols and trace gases. While carbon monoxide is well modeled, other pollutants have moderate to weak agreement with observations. Wind speed modeling is reliable for identifying pollution plumes, where models tend to overestimate concentrations. This highlights challenges in accurately modeling aerosol and trace gas composition, particularly in cities.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-521, https://doi.org/10.5194/egusphere-2024-521, 2024
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This study explores the proportional relationships between carbonaceous aerosols (black and organic carbon) and trace gases using airborne measurements from two campaigns in Europe and East Asia. Differences between regions were found, but air quality models struggled to reproduce them accurately. We show that these proportional relationships can help to constrain models and can be used to infer aerosol concentrations from satellite observations of trace gases, especially in urban areas.
Larissa Lacher, Michael P. Adams, Kevin Barry, Barbara Bertozzi, Heinz Bingemer, Cristian Boffo, Yannick Bras, Nicole Büttner, Dimitri Castarede, Daniel J. Cziczo, Paul J. DeMott, Romy Fösig, Megan Goodell, Kristina Höhler, Thomas C. J. Hill, Conrad Jentzsch, Luis A. Ladino, Ezra J. T. Levin, Stephan Mertes, Ottmar Möhler, Kathryn A. Moore, Benjamin J. Murray, Jens Nadolny, Tatjana Pfeuffer, David Picard, Carolina Ramírez-Romero, Mickael Ribeiro, Sarah Richter, Jann Schrod, Karine Sellegri, Frank Stratmann, Benjamin E. Swanson, Erik S. Thomson, Heike Wex, Martin J. Wolf, and Evelyn Freney
Atmos. Chem. Phys., 24, 2651–2678, https://doi.org/10.5194/acp-24-2651-2024, https://doi.org/10.5194/acp-24-2651-2024, 2024
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Aerosol particles that trigger ice formation in clouds are important for the climate system but are very rare in the atmosphere, challenging measurement techniques. Here we compare three cloud chambers and seven methods for collecting aerosol particles on filters for offline analysis at a mountaintop station. A general good agreement of the methods was found when sampling aerosol particles behind a whole air inlet, supporting their use for obtaining data that can be implemented in models.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Frederik Harzer, Hella Garny, Felix Ploeger, Harald Bönisch, Peter Hoor, and Thomas Birner
Atmos. Chem. Phys., 23, 10661–10675, https://doi.org/10.5194/acp-23-10661-2023, https://doi.org/10.5194/acp-23-10661-2023, 2023
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We study the statistical relation between year-by-year fluctuations in winter-mean ozone and the strength of the stratospheric polar vortex. In the latitude–pressure plane, regression analysis shows that anomalously weak polar vortex years are associated with three pronounced local ozone maxima over the polar cap relative to the winter climatology. These response maxima primarily reflect the non-trivial combination of different ozone transport processes with varying relative contributions.
Julia Homann, Niklas Karbach, Stacy A. Carolin, Daniel H. James, David Hodell, Sebastian F. M. Breitenbach, Ola Kwiecien, Mark Brenner, Carlos Peraza Lope, and Thorsten Hoffmann
Biogeosciences, 20, 3249–3260, https://doi.org/10.5194/bg-20-3249-2023, https://doi.org/10.5194/bg-20-3249-2023, 2023
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Cave stalagmites contain substances that can be used to reconstruct past changes in local and regional environmental conditions. We used two classes of biomarkers (polycyclic aromatic hydrocarbons and monosaccharide anhydrides) to detect the presence of fire and to also explore changes in fire regime (e.g. fire frequency, intensity, and fuel source). We tested our new method on a stalagmite from Mayapan, a large Maya city on the Yucatán Peninsula.
Annika Oertel, Annette K. Miltenberger, Christian M. Grams, and Corinna Hoose
Atmos. Chem. Phys., 23, 8553–8581, https://doi.org/10.5194/acp-23-8553-2023, https://doi.org/10.5194/acp-23-8553-2023, 2023
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Warm conveyor belts (WCBs) are cloud- and precipitation-producing airstreams in extratropical cyclones that are important for the large-scale flow and cloud radiative forcing. We analyze cloud formation processes during WCB ascent in a two-moment microphysics scheme. Quantification of individual diabatic heating rates shows the importance of condensation, vapor deposition, rain evaporation, melting, and cloud-top radiative cooling for total heating and WCB-related potential vorticity structure.
Marco Zanatta, Stephan Mertes, Olivier Jourdan, Regis Dupuy, Emma Järvinen, Martin Schnaiter, Oliver Eppers, Johannes Schneider, Zsófia Jurányi, and Andreas Herber
Atmos. Chem. Phys., 23, 7955–7973, https://doi.org/10.5194/acp-23-7955-2023, https://doi.org/10.5194/acp-23-7955-2023, 2023
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Black carbon (BC) particles influence the Arctic radiative balance. Vertical measurements of black carbon were conducted during the ACLOUD campaign in the European Arctic to study the interaction of BC with clouds. This study shows that clouds influence the vertical variability of BC properties across the inversion layer and that multiple activation and transformation mechanisms of BC may occur in the presence of low-level, persistent, mixed-phase clouds.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Luis F. Millán, Gloria L. Manney, Harald Boenisch, Michaela I. Hegglin, Peter Hoor, Daniel Kunkel, Thierry Leblanc, Irina Petropavlovskikh, Kaley Walker, Krzysztof Wargan, and Andreas Zahn
Atmos. Meas. Tech., 16, 2957–2988, https://doi.org/10.5194/amt-16-2957-2023, https://doi.org/10.5194/amt-16-2957-2023, 2023
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The determination of atmospheric composition trends in the upper troposphere and lower stratosphere (UTLS) is still highly uncertain. We present the creation of dynamical diagnostics to map several ozone datasets (ozonesondes, lidars, aircraft, and satellite measurements) in geophysically based coordinate systems. The diagnostics can also be used to analyze other greenhouse gases relevant to surface climate and UTLS chemistry.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
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During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
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.
Hans-Christoph Lachnitt, Peter Hoor, Daniel Kunkel, Martina Bramberger, Andreas Dörnbrack, Stefan Müller, Philipp Reutter, Andreas Giez, Thorsten Kaluza, and Markus Rapp
Atmos. Chem. Phys., 23, 355–373, https://doi.org/10.5194/acp-23-355-2023, https://doi.org/10.5194/acp-23-355-2023, 2023
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We present an analysis of high-resolution airborne measurements during a flight of the DEEPWAVE 2014 campaign in New Zealand. The focus of this flight was to study the effects of enhanced mountain wave activity over the Southern Alps. We discuss changes in the upstream and downstream distributions of N2O and CO and show that these changes are related to turbulence-induced trace gas fluxes which have persistent effects on the trace gas composition in the lower stratosphere.
Markus Thoma, Franziska Bachmeier, Felix Leonard Gottwald, Mario Simon, and Alexander Lucas Vogel
Atmos. Meas. Tech., 15, 7137–7154, https://doi.org/10.5194/amt-15-7137-2022, https://doi.org/10.5194/amt-15-7137-2022, 2022
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We introduce the aerosolomics database and apply it to particulate matter samples. Nine VOCs were oxidized under various conditions in an oxidation flow reactor, and the formed SOA was measured using liquid chromatography mass spectrometry. With the database, an unambiguous top-down attribution of atmospheric oxidation products to their parent VOCs is now possible. Combining the database with hierarchical clustering enables a better understanding of sources, formation, and partitioning of SOA.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Antonis Dragoneas, Sergej Molleker, Oliver Appel, Andreas Hünig, Thomas Böttger, Markus Hermann, Frank Drewnick, Johannes Schneider, Ralf Weigel, and Stephan Borrmann
Atmos. Meas. Tech., 15, 5719–5742, https://doi.org/10.5194/amt-15-5719-2022, https://doi.org/10.5194/amt-15-5719-2022, 2022
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The ERICA is a specially designed aerosol particle mass spectrometer for in situ, real-time chemical composition analysis of aerosols. It can operate completely autonomously, in the absence of an instrument operator. Its design has enabled its operation under harsh conditions, like those experienced in the upper troposphere and lower stratosphere, aboard unpressurized high-altitude research aircraft. The instrument has successfully participated in several aircraft operations around the world.
Paul Konopka, Mengchu Tao, Marc von Hobe, Lars Hoffmann, Corinna Kloss, Fabrizio Ravegnani, C. Michael Volk, Valentin Lauther, Andreas Zahn, Peter Hoor, and Felix Ploeger
Geosci. Model Dev., 15, 7471–7487, https://doi.org/10.5194/gmd-15-7471-2022, https://doi.org/10.5194/gmd-15-7471-2022, 2022
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Pure trajectory-based transport models driven by meteorology derived from reanalysis products (ERA5) take into account only the resolved, advective part of transport. That means neither mixing processes nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS) includes these processes. We show that isentropic mixing dominates unresolved transport. The second most important transport process is unresolved convection.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.9 to 7.8 × 105 cm-3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
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.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
Preprint withdrawn
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The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Jing Duan, Ru-Jin Huang, Yifang Gu, Chunshui Lin, Haobin Zhong, Wei Xu, Quan Liu, Yan You, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 22, 10139–10153, https://doi.org/10.5194/acp-22-10139-2022, https://doi.org/10.5194/acp-22-10139-2022, 2022
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Biomass-burning-influenced oxygenated organic aerosol (OOA-BB), formed from the photochemical oxidation and aging of biomass burning OA (BBOA), was resolved in urban Xi’an. The aqueous-phase processed oxygenated OA (aq-OOA) concentration was more dependent on secondary inorganic aerosol (SIA) content and aerosol liquid water content (ALWC). The increased aq-OOA contribution during SIA-enhanced periods likely reflects OA evolution due to the addition of alcohol or peroxide groups
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Andreas Hünig, Oliver Appel, Antonis Dragoneas, Sergej Molleker, Hans-Christian Clemen, Frank Helleis, Thomas Klimach, Franziska Köllner, Thomas Böttger, Frank Drewnick, Johannes Schneider, and Stephan Borrmann
Atmos. Meas. Tech., 15, 2889–2921, https://doi.org/10.5194/amt-15-2889-2022, https://doi.org/10.5194/amt-15-2889-2022, 2022
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We have serially combined the two well-established methods for in situ real-time measurement of fine particle chemical composition, the single-particle laser ablation method and the flash evaporation with electron impact ionization method, into a novel instrument. Here we present the design; instrument characteristics, as derived from laboratory and field measurements; and results from the first field deployment during the 2017 StratoClim aircraft campaign.
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.
Helmut Ziereis, Peter Hoor, Jens-Uwe Grooß, Andreas Zahn, Greta Stratmann, Paul Stock, Michael Lichtenstern, Jens Krause, Vera Bense, Armin Afchine, Christian Rolf, Wolfgang Woiwode, Marleen Braun, Jörn Ungermann, Andreas Marsing, Christiane Voigt, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Chem. Phys., 22, 3631–3654, https://doi.org/10.5194/acp-22-3631-2022, https://doi.org/10.5194/acp-22-3631-2022, 2022
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Airborne observations were conducted in the lowermost Arctic stratosphere during the winter of 2015/2016. The observed distribution of reactive nitrogen shows clear indications of nitrification in mid-winter and denitrification in late winter. This was caused by the formation of polar stratospheric cloud particles, which were observed during several flights. The sedimentation and evaporation of these particles and the descent of air masses cause a redistribution of reactive nitrogen.
Rupert Holzinger, Oliver Eppers, Kouji Adachi, Heiko Bozem, Markus Hartmann, Andreas Herber, Makoto Koike, Dylan B. Millet, Nobuhiro Moteki, Sho Ohata, Frank Stratmann, and Atsushi Yoshida
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-95, https://doi.org/10.5194/acp-2022-95, 2022
Revised manuscript not accepted
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In spring 2018 the research aircraft Polar 5 conducted flights in the Arctic atmosphere. The flight operation was from Station Nord in Greenland, 1700 km north of the Arctic Circle (81°43'N, 17°47'W). Using a mass spectrometer we measured more than 100 organic compounds in the air. We found a clear signature of natural organic compounds that are transported from forests to the high Arctic. These compounds have the potential to change the cloud cover and energy budget of the Arctic region.
Valentin Lauther, Bärbel Vogel, Johannes Wintel, Andrea Rau, Peter Hoor, Vera Bense, Rolf Müller, and C. Michael Volk
Atmos. Chem. Phys., 22, 2049–2077, https://doi.org/10.5194/acp-22-2049-2022, https://doi.org/10.5194/acp-22-2049-2022, 2022
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We show airborne in situ measurements of the very short-lived ozone-depleting substances CH2Cl2 and CHCl3, revealing particularly high concentrations of both species in the lower stratosphere. Back-trajectory calculations and 3D model simulations show that the air masses with high concentrations originated in the Asian boundary layer and were transported via the Asian summer monsoon. We also identify a fast transport pathway into the stratosphere via the North American monsoon and by hurricanes.
Stefan Niebler, Annette Miltenberger, Bertil Schmidt, and Peter Spichtinger
Weather Clim. Dynam., 3, 113–137, https://doi.org/10.5194/wcd-3-113-2022, https://doi.org/10.5194/wcd-3-113-2022, 2022
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We use machine learning to create a network that detects and classifies four types of synoptic-scale weather fronts from ERA5 atmospheric reanalysis data. We present an application of our method, showing its use case in a scientific context. Additionally, our results show that multiple sources of training data are necessary to perform well on different regions, implying differences within those regions. Qualitative evaluation shows that the results are physically plausible.
Rachel E. Hawker, Annette K. Miltenberger, Jill S. Johnson, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Paul R. Field, Benjamin J. Murray, and Ken S. Carslaw
Atmos. Chem. Phys., 21, 17315–17343, https://doi.org/10.5194/acp-21-17315-2021, https://doi.org/10.5194/acp-21-17315-2021, 2021
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We find that ice-nucleating particles (INPs), aerosols that can initiate the freezing of cloud droplets, cause substantial changes to the properties of radiatively important convectively generated anvil cirrus. The number concentration of INPs had a large effect on ice crystal number concentration while the INP temperature dependence controlled ice crystal size and cloud fraction. The results indicate information on INP number and source is necessary for the representation of cloud glaciation.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Sho Ohata, Makoto Koike, Atsushi Yoshida, Nobuhiro Moteki, Kouji Adachi, Naga Oshima, Hitoshi Matsui, Oliver Eppers, Heiko Bozem, Marco Zanatta, and Andreas B. Herber
Atmos. Chem. Phys., 21, 15861–15881, https://doi.org/10.5194/acp-21-15861-2021, https://doi.org/10.5194/acp-21-15861-2021, 2021
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Vertical profiles of black carbon (BC) in the Arctic were measured during the PAMARCMiP aircraft-based experiment in spring 2018 and compared with those observed during previous aircraft campaigns in 2008, 2010, and 2015. Their differences were explained primarily by the year-to-year variation of biomass burning activities in northern midlatitudes over Eurasia. Our observations provide a bases to evaluate numerical model simulations that assess the BC radiative effects in the Arctic spring.
Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-788, https://doi.org/10.5194/acp-2021-788, 2021
Preprint withdrawn
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By presenting an approach using EMeRGe-Asia airborne field measurements and surface observations, this study shows that the fraction of OH reactivity due to SO2-OH reaction has a significant correlation with the sulfate concentration. Approximately 30 % of sulfate is produced by SO2-OH reaction. Our results underline the importance of SO2-OH gas-phase oxidation in sulfate formation, and demonstrate that the method can be applied to other regions and under different meteorological conditions.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, and Thorsten Hoffmann
Atmos. Meas. Tech., 14, 6395–6406, https://doi.org/10.5194/amt-14-6395-2021, https://doi.org/10.5194/amt-14-6395-2021, 2021
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Motivated by a special interest in bromine chemistry in volcanic plumes, the study presented here describes a new method for the quantitative collection of gaseous hydrogen bromide in gas diffusion denuders. The hydrogen bromide reacted during sampling with appropriate epoxides applied to the denuder walls. The denuder sampling assembly was successfully deployed in the volcanic plume of Masaya volcano, Nicaragua.
Thorsten Kaluza, Daniel Kunkel, and Peter Hoor
Weather Clim. Dynam., 2, 631–651, https://doi.org/10.5194/wcd-2-631-2021, https://doi.org/10.5194/wcd-2-631-2021, 2021
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We present a 10-year analysis on the occurrence of strong wind shear in the Northern Hemisphere, focusing on the region around the transport barrier that separates the first two layers of the atmosphere. The major result of our analysis is that strong wind shear above a certain threshold occurs frequently and nearly exclusively in this region, which, as an indicator for turbulent mixing, might have major implications concerning the separation efficiency of the transport barrier.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Marco Zanatta, Andreas Herber, Zsófia Jurányi, Oliver Eppers, Johannes Schneider, and Joshua P. Schwarz
Atmos. Chem. Phys., 21, 9329–9342, https://doi.org/10.5194/acp-21-9329-2021, https://doi.org/10.5194/acp-21-9329-2021, 2021
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Saline snow samples were collected from the sea ice in the Fram Strait. Laboratory experiments revealed that sea salt can bias the quantification of black carbon with a laser-induced incandescence technique. The maximum underestimation was quantified to reach values of 80 %–90 %. This salt-induced interference is reported here for the first time and should be considered in future studies aiming to quantify black carbon in snow in marine environments.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
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Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Bo Galle, Santiago Arellano, Nicole Bobrowski, Vladimir Conde, Tobias P. Fischer, Gustav Gerdes, Alexandra Gutmann, Thorsten Hoffmann, Ima Itikarai, Tomas Krejci, Emma J. Liu, Kila Mulina, Scott Nowicki, Tom Richardson, Julian Rüdiger, Kieran Wood, and Jiazhi Xu
Atmos. Meas. Tech., 14, 4255–4277, https://doi.org/10.5194/amt-14-4255-2021, https://doi.org/10.5194/amt-14-4255-2021, 2021
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Measurements of volcanic gases are important for geophysical research, risk assessment and environmental impact studies. Some gases, like SO2 and BrO, may be studied from the ground at a safe distance using remote sensing techniques. Many other gases require in situ access to the gas plume. Here, a drone may be an attractive alternative. This paper describes a drone specially adapted for volcanic gas studies and demonstrates its use in a field campaign at Manam volcano in Papua New Guinea.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Hannes Schulz, Daniel Kunkel, Heiko Bozem, Peter Hoor, Thomas Klimach, Frank Helleis, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 21, 6509–6539, https://doi.org/10.5194/acp-21-6509-2021, https://doi.org/10.5194/acp-21-6509-2021, 2021
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We present in situ observations of vertically resolved particle chemical composition in the summertime Arctic lower troposphere. Our analysis demonstrates the strong vertical contrast between particle properties within the boundary layer and aloft. Emissions from vegetation fires and anthropogenic sources in northern Canada, Europe, and East Asia influenced particle composition in the free troposphere. Organics detected in Arctic aerosol particles can partly be identified as dicarboxylic acids.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
Inken Heidke, Adam Hartland, Denis Scholz, Andrew Pearson, John Hellstrom, Sebastian F. M. Breitenbach, and Thorsten Hoffmann
Biogeosciences, 18, 2289–2300, https://doi.org/10.5194/bg-18-2289-2021, https://doi.org/10.5194/bg-18-2289-2021, 2021
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We analyzed lignin oxidation products (LOPs) in leaf litter and different soil horizons as well as dripwater and flowstone samples from four different cave sites from different vegetation zones in New Zealand using liquid chromatography coupled to mass spectrometry. We test whether the original source-dependent LOP signal of the overlying vegetation is preserved and can be recovered from flowstone samples and investigate how the signal is altered by the transport from the soil to the cave.
Florian Ungeheuer, Dominik van Pinxteren, and Alexander L. Vogel
Atmos. Chem. Phys., 21, 3763–3775, https://doi.org/10.5194/acp-21-3763-2021, https://doi.org/10.5194/acp-21-3763-2021, 2021
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We analysed the chemical composition of ultrafine particles from 10–56 nm near Frankfurt Airport based on cascade impactor samples. We used an offline non-target screening to determine size-resolved molecular fingerprints. Unambiguous attribution of two homologous ester series to jet engine oils enables a new strategy of source attribution and explains the majority of the detected compounds. In addition, we identified additives of jet oils and a detrimental thermal transformation product.
Annette K. Miltenberger and Paul R. Field
Atmos. Chem. Phys., 21, 3627–3642, https://doi.org/10.5194/acp-21-3627-2021, https://doi.org/10.5194/acp-21-3627-2021, 2021
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The formation of ice in clouds is an important processes in mixed-phase and ice-phase clouds. However, the representation of ice formation in numerical models is highly uncertain. In the last decade, several new parameterizations for heterogeneous freezing have been proposed. Here, we investigate the impact of the parameterization choice on the representation of the convective cloud field and compare the impact to that of initial condition uncertainty.
Wei Yuan, Ru-Jin Huang, Lu Yang, Ting Wang, Jing Duan, Jie Guo, Haiyan Ni, Yang Chen, Qi Chen, Yongjie Li, Ulrike Dusek, Colin O'Dowd, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3685–3697, https://doi.org/10.5194/acp-21-3685-2021, https://doi.org/10.5194/acp-21-3685-2021, 2021
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We characterized the seasonal variations in nitrated aromatic compounds (NACs) in composition, sources, and their light absorption contribution to brown carbon (BrC) aerosol in Xi'an, Northwest China. Our results show that secondary formation and vehicular emission were dominant sources in summer (~80 %), and biomass burning and coal combustion were major sources in winter (~75 %), and they indicate that the composition and sources of NACs have a profound impact on the light absorption of BrC
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Julian Rüdiger, Alexandra Gutmann, Nicole Bobrowski, Marcello Liotta, J. Maarten de Moor, Rolf Sander, Florian Dinger, Jan-Lukas Tirpitz, Martha Ibarra, Armando Saballos, María Martínez, Elvis Mendoza, Arnoldo Ferrufino, John Stix, Juan Valdés, Jonathan M. Castro, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 3371–3393, https://doi.org/10.5194/acp-21-3371-2021, https://doi.org/10.5194/acp-21-3371-2021, 2021
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We present an innovative approach to study halogen chemistry in the plume of Masaya volcano in Nicaragua. An unique data set was collected using multiple techniques, including drones. These data enabled us to determine the fraction of activation of the respective halogens at various plume ages, where in-mixing of ambient air causes chemical reactions. An atmospheric chemistry box model was employed to further examine the field results and help our understanding of volcanic plume chemistry.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Cited articles
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Short summary
This study investigates molecular organic aerosol composition in the upper troposphere and lower stratosphere from an airborne campaign over Central Europe in summer 2024. Via ultra-high-performance liquid chromatography and high-resolution mass spectrometry of tropospheric and stratospheric filter samples, we identified various organic compounds. Our findings underscore the significant cross-tropopause transport of biogenic secondary organic aerosol and anthropogenic pollutants.
This study investigates molecular organic aerosol composition in the upper troposphere and lower...
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