Articles | Volume 22, issue 20
https://doi.org/10.5194/acp-22-13607-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-13607-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
20 Oct 2022
Research article |
| 20 Oct 2022
| 20 Oct 2022
Chemical analysis of the Asian tropopause aerosol layer (ATAL) with emphasis on secondary aerosol particles using aircraft-based in situ aerosol mass spectrometry
Oliver Appel
Max Planck Institute for Chemistry, Mainz, Germany
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Franziska Köllner
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Antonis Dragoneas
Max Planck Institute for Chemistry, Mainz, Germany
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Andreas Hünig
Max Planck Institute for Chemistry, Mainz, Germany
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Sergej Molleker
Max Planck Institute for Chemistry, Mainz, Germany
Hans Schlager
Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany
Christoph Mahnke
Max Planck Institute for Chemistry, Mainz, Germany
now at: Institute of Energy and Climate Research (IEK-8), Forschungszentrum Jülich GmbH, Jülich, Germany
Ralf Weigel
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
Max Port
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
now at: Montessori Zentrum Hofheim, Germany
Christiane Schulz
Max Planck Institute for Chemistry, Mainz, Germany
now at: Leibniz-Zentrum für Agrarlandschaftsforschung, Müncheberg, Germany
Frank Drewnick
Max Planck Institute for Chemistry, Mainz, Germany
Bärbel Vogel
Institute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich, Jülich, Germany
Fred Stroh
Institute of Energy and Climate Research (IEK-7), Forschungszentrum Jülich, Jülich, Germany
Stephan Borrmann
CORRESPONDING AUTHOR
Max Planck Institute for Chemistry, Mainz, Germany
Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany
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Preprint archived
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Bärbel Vogel, C. Michael Volk, Johannes Wintel, Valentin Lauther, Jan Clemens, Jens-Uwe Grooß, Gebhard Günther, Lars Hoffmann, Johannes C. Laube, Rolf Müller, Felix Ploeger, and Fred Stroh
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Cirrus clouds have been observed over the Himalayan region between 10 km and the tropopause at 17–18 km. Data from backscattersonde, hygrometers, and particle cloud spectrometers have been compared to assess their consistency. Empirical relationships between optical parameters accessible with remote sensing lidars and cloud microphysical parameters (such as ice water content, particle number and surface area density, and particle aspherical fraction) have been established.
Pierre Grzegorczyk, Sudha Yadav, Florian Zanger, Alexander Theis, Subir K. Mitra, Stephan Borrmann, and Miklós Szakáll
Atmos. Chem. Phys., 23, 13505–13521, https://doi.org/10.5194/acp-23-13505-2023, https://doi.org/10.5194/acp-23-13505-2023, 2023
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Secondary ice production generates high concentrations of ice crystals in clouds. These processes have been poorly understood. We conducted experiments at the wind tunnel laboratory of the Johannes Gutenberg University, Mainz, on graupel–graupel and graupel–snowflake collisions. From these experiments fragment number, size, cross-sectional area, and aspect ratio were determined.
Paul Konopka, Christian Rolf, Marc von Hobe, Sergey M. Khaykin, Benjamin Clouser, Elisabeth Moyer, Fabrizio Ravegnani, Francesco D'Amato, Silvia Viciani, Nicole Spelten, Armin Afchine, Martina Krämer, Fred Stroh, and Felix Ploeger
Atmos. Chem. Phys., 23, 12935–12947, https://doi.org/10.5194/acp-23-12935-2023, https://doi.org/10.5194/acp-23-12935-2023, 2023
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We studied water vapor in a critical region of the atmosphere, the Asian summer monsoon anticyclone, using rare in situ observations. Our study shows that extremely high water vapor values observed in the stratosphere within the Asian monsoon anticyclone still undergo significant freeze-drying and that water vapor concentrations set by the Lagrangian dry point are a better proxy for the stratospheric water vapor budget than rare observations of enhanced water mixing ratios.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
Valerian Hahn, Ralf Meerkötter, Christiane Voigt, Sonja Gisinger, Daniel Sauer, Valéry Catoire, Volker Dreiling, Hugh Coe, Cyrille Flamant, Stefan Kaufmann, Jonas Kleine, Peter Knippertz, Manuel Moser, Philip Rosenberg, Hans Schlager, Alfons Schwarzenboeck, and Jonathan Taylor
Atmos. Chem. Phys., 23, 8515–8530, https://doi.org/10.5194/acp-23-8515-2023, https://doi.org/10.5194/acp-23-8515-2023, 2023
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During the DACCIWA campaign in West Africa, we found a 35 % increase in the cloud droplet concentration that formed in a polluted compared with a less polluted environment and a decrease of 17 % in effective droplet diameter. Radiative transfer simulations, based on the measured cloud properties, reveal that these low-level polluted clouds radiate only 2.6 % more energy back to space, compared with a less polluted cloud. The corresponding additional decrease in temperature is rather small.
Silke Groß, Tina Jurkat-Witschas, Qiang Li, Martin Wirth, Benedikt Urbanek, Martina Krämer, Ralf Weigel, and Christiane Voigt
Atmos. Chem. Phys., 23, 8369–8381, https://doi.org/10.5194/acp-23-8369-2023, https://doi.org/10.5194/acp-23-8369-2023, 2023
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Aviation-emitted aerosol can have an impact on cirrus clouds. We present optical and microphysical properties of mid-latitude cirrus clouds which were formed under the influence of aviation-emitted aerosol or which were formed under rather pristine conditions. We find that cirrus clouds affected by aviation-emitted aerosol show larger values of the particle linear depolarization ratio, larger mean effective ice particle diameters and decreased ice particle number concentrations.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Lars Hoffmann, Paul Konopka, Jan Clemens, and Bärbel Vogel
Atmos. Chem. Phys., 23, 7589–7609, https://doi.org/10.5194/acp-23-7589-2023, https://doi.org/10.5194/acp-23-7589-2023, 2023
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Atmospheric convection plays a key role in tracer transport in the troposphere. Global meteorological forecasts and reanalyses typically have a coarse spatiotemporal resolution that does not adequately resolve the dynamics, transport, and mixing of air associated with storm systems or deep convection. We discuss the application of the extreme convection parameterization in a Lagrangian transport model to improve simulations of tracer transport from the boundary layer into the free troposphere.
Manuel Moser, Christiane Voigt, Tina Jurkat-Witschas, Valerian Hahn, Guillaume Mioche, Olivier Jourdan, Régis Dupuy, Christophe Gourbeyre, Alfons Schwarzenboeck, Johannes Lucke, Yvonne Boose, Mario Mech, Stephan Borrmann, André Ehrlich, Andreas Herber, Christof Lüpkes, and Manfred Wendisch
Atmos. Chem. Phys., 23, 7257–7280, https://doi.org/10.5194/acp-23-7257-2023, https://doi.org/10.5194/acp-23-7257-2023, 2023
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This study provides a comprehensive microphysical and thermodynamic phase analysis of low-level clouds in the northern Fram Strait, above the sea ice and the open ocean, during spring and summer. Using airborne in situ cloud data, we show that the properties of Arctic low-level clouds vary significantly with seasonal meteorological situations and surface conditions. The observations presented in this study can help one to assess the role of clouds in the Arctic climate system.
Robert Wagner, Alexander D. James, Victoria L. Frankland, Ottmar Möhler, Benjamin J. Murray, John M. C. Plane, Harald Saathoff, Ralf Weigel, and Martin Schnaiter
Atmos. Chem. Phys., 23, 6789–6811, https://doi.org/10.5194/acp-23-6789-2023, https://doi.org/10.5194/acp-23-6789-2023, 2023
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Polar stratospheric clouds (PSCs) play an important role in the depletion of stratospheric ozone. They can consist of different chemical species, including crystalline nitric acid hydrates. We found that mineral dust or meteoric ablation material can efficiently catalyse the formation of a specific phase of nitric acid dihydrate crystals. We determined predominant particle shapes and infrared optical properties of these crystals, which are important inputs for remote sensing detection of PSCs.
Julia Pikmann, Lasse Moormann, Frank Drewnick, and Stephan Borrmann
Atmos. Meas. Tech., 16, 1323–1341, https://doi.org/10.5194/amt-16-1323-2023, https://doi.org/10.5194/amt-16-1323-2023, 2023
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Aerosols measured in complex environments are usually a mixture of emissions from different sources. To characterize sources individually, we developed a sampling system for particles and organic trace gases which is coupled to real-time data of physical and chemical aerosol properties, gas concentrations, and meteorological variables. Using suitable sampling conditions for individual aerosols which are compared with the real-time data the desired aerosols are sampled separately from each other.
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.
Yun Li, Christoph Mahnke, Susanne Rohs, Ulrich Bundke, Nicole Spelten, Georgios Dekoutsidis, Silke Groß, Christiane Voigt, Ulrich Schumann, Andreas Petzold, and Martina Krämer
Atmos. Chem. Phys., 23, 2251–2271, https://doi.org/10.5194/acp-23-2251-2023, https://doi.org/10.5194/acp-23-2251-2023, 2023
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The radiative effect of aviation-induced cirrus is closely related to ambient conditions and its microphysical properties. Our study investigated the occurrence of contrail and natural cirrus measured above central Europe in spring 2014. It finds that contrail cirrus appears frequently in the pressure range 200 to 245 hPa and occurs more often in slightly ice-subsaturated environments than expected. Avoiding slightly ice-subsaturated regions by aviation might help mitigate contrail cirrus.
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.
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.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
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.
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.
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.
Lars Hoffmann, Paul F. Baumeister, Zhongyin Cai, Jan Clemens, Sabine Griessbach, Gebhard Günther, Yi Heng, Mingzhao Liu, Kaveh Haghighi Mood, Olaf Stein, Nicole Thomas, Bärbel Vogel, Xue Wu, and Ling Zou
Geosci. Model Dev., 15, 2731–2762, https://doi.org/10.5194/gmd-15-2731-2022, https://doi.org/10.5194/gmd-15-2731-2022, 2022
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We describe the new version (2.2) of the Lagrangian transport model MPTRAC, which has been ported for application on GPUs. The model was verified by comparing kinematic trajectories and synthetic tracer simulations for the free troposphere and stratosphere from GPUs and CPUs. Benchmarking showed a speed-up of a factor of 16 of GPU-enabled simulations compared to CPU-only runs, indicating the great potential of applying GPUs for Lagrangian transport simulations on upcoming HPC systems.
Sergey M. Khaykin, Elizabeth Moyer, Martina Krämer, Benjamin Clouser, Silvia Bucci, Bernard Legras, Alexey Lykov, Armin Afchine, Francesco Cairo, Ivan Formanyuk, Valentin Mitev, Renaud Matthey, Christian Rolf, Clare E. Singer, Nicole Spelten, Vasiliy Volkov, Vladimir Yushkov, and Fred Stroh
Atmos. Chem. Phys., 22, 3169–3189, https://doi.org/10.5194/acp-22-3169-2022, https://doi.org/10.5194/acp-22-3169-2022, 2022
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The Asian monsoon anticyclone is the key contributor to the global annual maximum in lower stratospheric water vapour. We investigate the impact of deep convection on the lower stratospheric water using a unique set of observations aboard the high-altitude M55-Geophysica aircraft deployed in Nepal in summer 2017 within the EU StratoClim project. We find that convective plumes of wet air can persist within the Asian anticyclone for weeks, thereby enhancing the occurrence of high-level clouds.
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.
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.
Tiziana Bräuer, Christiane Voigt, Daniel Sauer, Stefan Kaufmann, Valerian Hahn, Monika Scheibe, Hans Schlager, Felix Huber, Patrick Le Clercq, Richard H. Moore, and Bruce E. Anderson
Atmos. Chem. Phys., 21, 16817–16826, https://doi.org/10.5194/acp-21-16817-2021, https://doi.org/10.5194/acp-21-16817-2021, 2021
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Over half of aviation climate impact is caused by contrails. Biofuels can reduce the ice crystal numbers in contrails and mitigate the climate impact. The experiment ECLIF II/NDMAX in 2018 assessed the effects of biofuels on contrails and aviation emissions. The NASA DC-8 aircraft performed measurements inside the contrail of the DLR A320. One reference fuel and two blends of the biofuel HEFA and kerosene are analysed. We find a max reduction of contrail ice numbers through biofuel use of 40 %.
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
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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.
Christoph Mahnke, Ralf Weigel, Francesco Cairo, Jean-Paul Vernier, Armin Afchine, Martina Krämer, Valentin Mitev, Renaud Matthey, Silvia Viciani, Francesco D'Amato, Felix Ploeger, Terry Deshler, and Stephan Borrmann
Atmos. Chem. Phys., 21, 15259–15282, https://doi.org/10.5194/acp-21-15259-2021, https://doi.org/10.5194/acp-21-15259-2021, 2021
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In 2017, in situ aerosol measurements were conducted aboard the M55 Geophysica in the Asian monsoon region. The vertical particle mixing ratio profiles show a distinct layer (15–18.5 km), the Asian tropopause aerosol layer (ATAL). The backscatter ratio (BR) was calculated based on the aerosol size distributions and compared with the BRs detected by a backscatter probe and a lidar aboard M55, and by the CALIOP lidar. All four methods show enhanced BRs in the ATAL altitude range (max. at 17.5 km).
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Martina Krämer, Peter Spichtinger, Nicole Spelten, Armin Afchine, Christian Rolf, Silvia Viciani, Francesco D'Amato, Holger Tost, and Stephan Borrmann
Atmos. Chem. Phys., 21, 13455–13481, https://doi.org/10.5194/acp-21-13455-2021, https://doi.org/10.5194/acp-21-13455-2021, 2021
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In July and August 2017, the StratoClim mission took place in Nepal with eight flights of the M-55 Geophysica at up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) next to cloud ice was detected in situ by abundant nucleation-mode aerosols (> 6 nm) along with ice particles (> 3 µm). NPF was observed mainly below the tropopause, down to 15 % being non-volatile residues. Observed intra-cloud NPF indicates its importance for the composition in the tropical tropopause layer.
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Antonis Dragoneas, Bärbel Vogel, Felix Ploeger, Silvia Viciani, Francesco D'Amato, Silvia Bucci, Bernard Legras, Beiping Luo, and Stephan Borrmann
Atmos. Chem. Phys., 21, 11689–11722, https://doi.org/10.5194/acp-21-11689-2021, https://doi.org/10.5194/acp-21-11689-2021, 2021
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In July and August 2017, eight StratoClim mission flights of the Geophysica reached up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) was identified in situ by abundant nucleation-mode aerosols (6–15 nm in diameter) with mixing ratios of up to 50 000 mg−1. NPF occurred most frequently at 12–16 km with fractions of non-volatile residues of down to 15 %. Abundance and productivity of observed NPF indicate its ability to promote the Asian tropopause aerosol layer.
Lukas Krasauskas, Jörn Ungermann, Peter Preusse, Felix Friedl-Vallon, Andreas Zahn, Helmut Ziereis, Christian Rolf, Felix Plöger, Paul Konopka, Bärbel Vogel, and Martin Riese
Atmos. Chem. Phys., 21, 10249–10272, https://doi.org/10.5194/acp-21-10249-2021, https://doi.org/10.5194/acp-21-10249-2021, 2021
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A Rossby wave (RW) breaking event was observed over the North Atlantic during the WISE measurement campaign in October 2017. Infrared limb sounding measurements of trace gases in the lower stratosphere, including high-resolution 3-D tomographic reconstruction, revealed complex spatial structures in stratospheric tracers near the polar jet related to previous RW breaking events. Backward-trajectory analysis and tracer correlations were used to study mixing and stratosphere–troposphere exchange.
Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Jens-Uwe Grooß, Thomas Gulde, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Erik Kretschmer, Guido Maucher, Hans Nordmeyer, Hermann Oelhaf, Johannes Orphal, Christof Piesch, Björn-Martin Sinnhuber, Jörn Ungermann, and Bärbel Vogel
Atmos. Chem. Phys., 21, 8213–8232, https://doi.org/10.5194/acp-21-8213-2021, https://doi.org/10.5194/acp-21-8213-2021, 2021
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Measurements of the pollutants C2H6, C2H2, HCOOH, and PAN were performed in the North Atlantic UTLS region with the airborne limb imager GLORIA in 2017. Enhanced amounts of these species were detected in the upper troposphere and even in the lowermost stratosphere (PAN). Main sources of these gases are forest fires in North America and anthropogenic pollution in South Asia. Simulations of EMAC and CAMS are qualitatively able to reproduce the measured data but underestimate the absolute amounts.
Nils Friedrich, Philipp Eger, Justin Shenolikar, Nicolas Sobanski, Jan Schuladen, Dirk Dienhart, Bettina Hottmann, Ivan Tadic, Horst Fischer, Monica Martinez, Roland Rohloff, Sebastian Tauer, Hartwig Harder, Eva Y. Pfannerstill, Nijing Wang, Jonathan Williams, James Brooks, Frank Drewnick, Hang Su, Guo Li, Yafang Cheng, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 21, 7473–7498, https://doi.org/10.5194/acp-21-7473-2021, https://doi.org/10.5194/acp-21-7473-2021, 2021
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This paper uses NOx and NOz measurements from the 2017 AQABA ship campaign in the Mediterranean Sea and around the Arabian Peninsula to examine the influence e.g. of emissions from shipping and oil and gas production. Night-time losses of NOx dominated in the Arabian Gulf and in the Red Sea, whereas daytime losses were more important in the Mediterranean Sea. Nitric acid and organic nitrates were the most prevalent components of NOz.
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.
Maxi Boettcher, Andreas Schäfler, Michael Sprenger, Harald Sodemann, Stefan Kaufmann, Christiane Voigt, Hans Schlager, Donato Summa, Paolo Di Girolamo, Daniele Nerini, Urs Germann, and Heini Wernli
Atmos. Chem. Phys., 21, 5477–5498, https://doi.org/10.5194/acp-21-5477-2021, https://doi.org/10.5194/acp-21-5477-2021, 2021
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Warm conveyor belts (WCBs) are important airstreams in extratropical cyclones, often leading to the formation of intense precipitation. We present a case study that involves aircraft, lidar and radar observations of water and clouds in a WCB ascending from western Europe across the Alps towards the Baltic Sea during the field campaigns HyMeX and T-NAWDEX-Falcon in October 2012. A probabilistic trajectory measure and an airborne tracer experiment were used to confirm the long pathway of the WCB.
Sebastian O'Shea, Jonathan Crosier, James Dorsey, Louis Gallagher, Waldemar Schledewitz, Keith Bower, Oliver Schlenczek, Stephan Borrmann, Richard Cotton, Christopher Westbrook, and Zbigniew Ulanowski
Atmos. Meas. Tech., 14, 1917–1939, https://doi.org/10.5194/amt-14-1917-2021, https://doi.org/10.5194/amt-14-1917-2021, 2021
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The number, shape, and size of ice crystals in clouds are important properties that influence the Earth's radiation budget, cloud evolution, and precipitation formation. This work suggests that one of the most widely used methods for in situ measurements of these properties has significant uncertainties and biases. We suggest methods that dramatically improve these measurements, which can be applied to past and future datasets from these instruments.
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.
Miklós Szakáll, Michael Debertshäuser, Christian Philipp Lackner, Amelie Mayer, Oliver Eppers, Karoline Diehl, Alexander Theis, Subir Kumar Mitra, and Stephan Borrmann
Atmos. Chem. Phys., 21, 3289–3316, https://doi.org/10.5194/acp-21-3289-2021, https://doi.org/10.5194/acp-21-3289-2021, 2021
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The freezing of cloud drops is promoted by ice-nucleating particles immersed in the drops. This process is essential to understand ice and subsequent precipitation formation in clouds. We investigated the efficiency of several particle types to trigger immersion freezing with two single-drop levitation techniques: a wind tunnel and an acoustic levitator. The evaluation accounted for different conditions during our two series of experiments, which is also applicable to future comparison studies.
Sabine Robrecht, Bärbel Vogel, Simone Tilmes, and Rolf Müller
Atmos. Chem. Phys., 21, 2427–2455, https://doi.org/10.5194/acp-21-2427-2021, https://doi.org/10.5194/acp-21-2427-2021, 2021
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Column ozone protects life on Earth from radiation damage. Stratospheric chlorine compounds cause immense ozone loss in polar winter. Whether similar loss processes can occur in the lower stratosphere above North America today or in future is a matter of debate. We show that these ozone loss processes are very unlikely today or in future independently of whether sulfate geoengineering is applied and that less than 0.1 % of column ozone would be destroyed by this process in any future scenario.
Joan Stude, Heinfried Aufmhoff, Hans Schlager, Markus Rapp, Frank Arnold, and Boris Strelnikov
Atmos. Meas. Tech., 14, 983–993, https://doi.org/10.5194/amt-14-983-2021, https://doi.org/10.5194/amt-14-983-2021, 2021
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In this paper we describe the instrument ROMARA and show data from the first flight on a research rocket.
On the way through the atmosphere, the instrument detects positive and negative, natural occurring ions before returning back to ground.
ROMARA was successfully launched together with other instruments into a special radar echo.
We detected typical, light ions of positive and negative charge and heavy negative ions, but no heavy positive ions.
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.
Manuel Baumgartner, Ralf Weigel, Allan H. Harvey, Felix Plöger, Ulrich Achatz, and Peter Spichtinger
Atmos. Chem. Phys., 20, 15585–15616, https://doi.org/10.5194/acp-20-15585-2020, https://doi.org/10.5194/acp-20-15585-2020, 2020
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The potential temperature is routinely used in atmospheric science. We review its derivation and suggest a new potential temperature, based on a temperature-dependent parameterization of the dry air's specific heat capacity. Moreover, we compare the new potential temperature to the common one and discuss the differences which become more important at higher altitudes. Finally, we indicate some consequences of using the new potential temperature in typical applications.
Maximilian Weitzel, Subir K. Mitra, Miklós Szakáll, Jacob P. Fugal, and Stephan Borrmann
Atmos. Chem. Phys., 20, 14889–14901, https://doi.org/10.5194/acp-20-14889-2020, https://doi.org/10.5194/acp-20-14889-2020, 2020
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The properties of ice crystals smaller than 150 µm in diameter were investigated in a cold-room laboratory using digital holography and microscopy. Automated image processing has been used to determine the track of falling ice crystals, and collected crystals were melted and scanned under a microscope to infer particle mass. A parameterization relating particle size and mass was determined which describes ice crystals in this size range more accurately than existing relationships.
Sreeharsha Hanumanthu, Bärbel Vogel, Rolf Müller, Simone Brunamonti, Suvarna Fadnavis, Dan Li, Peter Ölsner, Manish Naja, Bhupendra Bahadur Singh, Kunchala Ravi Kumar, Sunil Sonbawne, Hannu Jauhiainen, Holger Vömel, Beiping Luo, Teresa Jorge, Frank G. Wienhold, Ruud Dirkson, and Thomas Peter
Atmos. Chem. Phys., 20, 14273–14302, https://doi.org/10.5194/acp-20-14273-2020, https://doi.org/10.5194/acp-20-14273-2020, 2020
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During boreal summer, anthropogenic sources yield the Asian Tropopause Aerosol Layer (ATAL), found in Asia between about 13 and 18 km altitude. Balloon-borne measurements of the ATAL conducted in northern India in 2016 show the strong variability of the ATAL. To explain its observed variability, model simulations are performed to deduce the origin of air masses on the Earth's surface, which is important to develop recommendations for regulations of anthropogenic surface emissions of the ATAL.
Hans-Christian Clemen, Johannes Schneider, Thomas Klimach, Frank Helleis, Franziska Köllner, Andreas Hünig, Florian Rubach, Stephan Mertes, Heike Wex, Frank Stratmann, André Welti, Rebecca Kohl, Fabian Frank, and Stephan Borrmann
Atmos. Meas. Tech., 13, 5923–5953, https://doi.org/10.5194/amt-13-5923-2020, https://doi.org/10.5194/amt-13-5923-2020, 2020
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We improved the efficiency of a single-particle mass spectrometer with a newly developed aerodynamic lens system, delayed ion extraction, and better electric shielding. The new components result in significantly improved particle analysis and sample statistics. This is particularly important for measurements of low-number-density particles, such as ice-nucleating particles, and for aircraft-based measurements at high altitudes or where high temporal and spatial resolution is required.
Martina Krämer, Christian Rolf, Nicole Spelten, Armin Afchine, David Fahey, Eric Jensen, Sergey Khaykin, Thomas Kuhn, Paul Lawson, Alexey Lykov, Laura L. Pan, Martin Riese, Andrew Rollins, Fred Stroh, Troy Thornberry, Veronika Wolf, Sarah Woods, Peter Spichtinger, Johannes Quaas, and Odran Sourdeval
Atmos. Chem. Phys., 20, 12569–12608, https://doi.org/10.5194/acp-20-12569-2020, https://doi.org/10.5194/acp-20-12569-2020, 2020
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To improve the representations of cirrus clouds in climate predictions, extended knowledge of their properties and geographical distribution is required. This study presents extensive airborne in situ and satellite remote sensing climatologies of cirrus and humidity, which serve as a guide to cirrus clouds. Further, exemplary radiative characteristics of cirrus types and also in situ observations of tropical tropopause layer cirrus and humidity in the Asian monsoon anticyclone are shown.
Flora Kluge, Tilman Hüneke, Matthias Knecht, Michael Lichtenstern, Meike Rotermund, Hans Schlager, Benjamin Schreiner, and Klaus Pfeilsticker
Atmos. Chem. Phys., 20, 12363–12389, https://doi.org/10.5194/acp-20-12363-2020, https://doi.org/10.5194/acp-20-12363-2020, 2020
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The presented study reports on airborne measurements of formaldehyde, glyoxal, methylglyoxal, and CO over the Amazon basin and lays a special focus on the influence of biomass burning emissions on the atmospheric profiles of these carbonyl compounds within the planetary boundary layer as well as in the free and upper troposphere.
Nils Friedrich, Ivan Tadic, Jan Schuladen, James Brooks, Eoghan Darbyshire, Frank Drewnick, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 13, 5739–5761, https://doi.org/10.5194/amt-13-5739-2020, https://doi.org/10.5194/amt-13-5739-2020, 2020
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We present a new instrument for the measurement of NOx and NOy based on a combination of the thermal dissociation of NOy to NOx and cavity ring-down spectroscopic detection of NO2. It features a denuder to separate the contributions of gas-phase and particulate nitrates to NOy. We provide a detailed characterization of the instrument and briefly outline results from first deployments.
Silvia Bucci, Bernard Legras, Pasquale Sellitto, Francesco D'Amato, Silvia Viciani, Alessio Montori, Antonio Chiarugi, Fabrizio Ravegnani, Alexey Ulanovsky, Francesco Cairo, and Fred Stroh
Atmos. Chem. Phys., 20, 12193–12210, https://doi.org/10.5194/acp-20-12193-2020, https://doi.org/10.5194/acp-20-12193-2020, 2020
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The paper presents and evaluates a transport analysis method to study the convective injection of air in the upper troposphere–lower stratosphere of the Asian monsoon anticyclone region. The approach is thereby used to analyse the trace gas data collected during the StratoClim aircraft campaign. The results showed that fresh convective air can be injected fast at a high level of the atmosphere (above 17 km), with potential impacts on the stratospheric chemistry of the Northern Hemisphere.
Hirofumi Ohyama, Isamu Morino, Voltaire A. Velazco, Theresa Klausner, Gerry Bagtasa, Matthäus Kiel, Matthias Frey, Akihiro Hori, Osamu Uchino, Tsuneo Matsunaga, Nicholas M. Deutscher, Joshua P. DiGangi, Yonghoon Choi, Glenn S. Diskin, Sally E. Pusede, Alina Fiehn, Anke Roiger, Michael Lichtenstern, Hans Schlager, Pao K. Wang, Charles C.-K. Chou, Maria Dolores Andrés-Hernández, and John P. Burrows
Atmos. Meas. Tech., 13, 5149–5163, https://doi.org/10.5194/amt-13-5149-2020, https://doi.org/10.5194/amt-13-5149-2020, 2020
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Column-averaged dry-air mole fractions of CO2 and CH4 measured by a solar viewing portable Fourier transform spectrometer (EM27/SUN) were validated with in situ profile data obtained during the transfer flights of two aircraft campaigns. Atmospheric dynamical properties based on ERA5 and WRF-Chem were used as criteria for selecting the best aircraft profiles for the validation. The resulting air-mass-independent correction factors for the EM27/SUN data were 0.9878 for CO2 and 0.9829 for CH4.
Cited articles
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Bela, M. M., Barth, M. C., Toon, O. B., Fried, A., Homeyer, C. R., Morrison, H., Cummings, K. A., Li, Y., Pickering, K. E., Allen, D. J., Yang, Q., Wennberg, P. O., Crounse, J. D., St. Clair, J. M., Teng, A. P., O'Sullivan, D., Huey, L. G., Chen, D., Liu, X., Blake, D. R., Blake, N. J., Apel, E. C., Hornbrook, R. S., Flocke, F., Campos, T., and Diskin, G.: Wet scavenging of soluble gases in DC3 deep convective storms using WRF-Chem simulations and aircraft observations, J. Geophys. Res.-Atmos., 121, 4233–4257, https://doi.org/10.1002/2015JD024623, 2016. a
Borrmann, S., Kunkel, D., Weigel, R., Minikin, A., Deshler, T., Wilson, J. C., Curtius, J., Volk, C. M., Homan, C. D., Ulanovsky, A., Ravegnani, F., Viciani, S., Shur, G. N., Belyaev, G. V., Law, K. S., and Cairo, F.: Aerosols in the tropical and subtropical UT/LS: in-situ measurements of submicron particle abundance and volatility, Atmos. Chem. Phys., 10, 5573–5592, https://doi.org/10.5194/acp-10-5573-2010, 2010. a
Bossolasco, A., Jegou, F., Sellitto, P., Berthet, G., Kloss, C., and Legras, B.: Global modeling studies of composition and decadal trends of the Asian Tropopause Aerosol Layer, Atmos. Chem. Phys., 21, 2745–2764, https://doi.org/10.5194/acp-21-2745-2021, 2021. a
Brands, M., Kamphus, M., Böttger, T., Schneider, J., Drewnick, F., Roth, A., Curtius, J., Voigt, C., Borbon, A., Beekmann, M., Bourdon, A., Perrin, T., and Borrmann, S.: Characterization of a Newly Developed Aircraft-Based Laser Ablation Aerosol Mass Spectrometer (ALABAMA) and First Field Deployment in Urban Pollution Plumes over Paris During MEGAPOLI 2009, Aerosol Sci. Tech., 45, 46–64, https://doi.org/10.1080/02786826.2010.517813, 2011. a, b
Brenninkmeijer, C. A. M., Crutzen, P., Boumard, F., Dauer, T., Dix, B., Ebinghaus, R., Filippi, D., Fischer, H., Franke, H., Frieß, U., Heintzenberg, J., Helleis, F., Hermann, M., Kock, H. H., Koeppel, C., Lelieveld, J., Leuenberger, M., Martinsson, B. G., Miemczyk, S., Moret, H. P., Nguyen, H. N., Nyfeler, P., Oram, D., O'Sullivan, D., Penkett, S., Platt, U., Pupek, M., Ramonet, M., Randa, B., Reichelt, M., Rhee, T. S., Rohwer, J., Rosenfeld, K., Scharffe, D., Schlager, H., Schumann, U., Slemr, F., Sprung, D., Stock, P., Thaler, R., Valentino, F., van Velthoven, P., Waibel, A., Wandel, A., Waschitschek, K., Wiedensohler, A., Xueref-Remy, I., Zahn, A., Zech, U., and Ziereis, H.: Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system, Atmos. Chem. Phys., 7, 4953–4976, https://doi.org/10.5194/acp-7-4953-2007, 2007. a
Brüggemann, M., Xu, R., Tilgner, A., Kwong, K. C., Mutzel, A., Poon, H. Y., Otto, T., Schaefer, T., Poulain, L., Chan, M. N., and Herrmann, H.: Organosulfates in Ambient Aerosol: State of Knowledge and Future Research Directions on Formation, Abundance, Fate, and Importance, Environ. Sci. Technol., 54, 3767–3782, https://doi.org/10.1021/acs.est.9b06751, 2020. a
Brühl, C., Schallock, J., Klingmüller, K., Robert, C., Bingen, C., Clarisse, L., Heckel, A., North, P., and Rieger, L.: Stratospheric aerosol radiative forcing simulated by the chemistry climate model EMAC using Aerosol CCI satellite data, Atmos. Chem. Phys., 18, 12845–12857, https://doi.org/10.5194/acp-18-12845-2018, 2018. a
Brunamonti, S., Jorge, T., Oelsner, P., Hanumanthu, S., Singh, B. B., Kumar, K. R., Sonbawne, S., Meier, S., Singh, D., Wienhold, F. G., Luo, B. P., Boettcher, M., Poltera, Y., Jauhiainen, H., Kayastha, R., Karmacharya, J., Dirksen, R., Naja, M., Rex, M., Fadnavis, S., and Peter, T.: Balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter on the southern slopes of the Himalayas during StratoClim 2016–2017, Atmos. Chem. Phys., 18, 15937–15957, https://doi.org/10.5194/acp-18-15937-2018, 2018. a
Bucci, S., Legras, B., Sellitto, P., D'Amato, F., Viciani, S., Montori, A., Chiarugi, A., Ravegnani, F., Ulanovsky, A., Cairo, F., and Stroh, F.: Deep-convective influence on the upper troposphere–lower stratosphere composition in the Asian monsoon anticyclone region: 2017 StratoClim campaign results, Atmos. Chem. Phys., 20, 12193–12210, https://doi.org/10.5194/acp-20-12193-2020, 2020. a, b, c
Canagaratna, M., Jayne, J., Jimenez, J., Allan, J., Alfarra, M., Zhang, Q., Onasch, T., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L., Trimborn, A., Northway, M., DeCarlo, P., Kolb, C., Davidovits, P., and Worsnop, D.: Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer, Mass Spectrom. Rev., 26, 185–222, https://doi.org/10.1002/mas.20115, 2007. a
Dragoneas, A., Molleker, S., Appel, O., Hünig, A., Böttger, T., Hermann, M., Drewnick, F., Schneider, J., Weigel, R., and Borrmann, S.: The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere, Atmos. Meas. Tech., 15, 5719–5742, https://doi.org/10.5194/amt-15-5719-2022, 2022. a, b, c, d
Drewnick, F., Hings, S. S., DeCarlo, P., Jayne, J. T., Gonin, M., Fuhrer, K., Weimer, S., Jimenez, J. L., Demerjian, K. L., Borrmann, S., and Worsnop, D. R.: A New Time-of-Flight Aerosol Mass Spectrometer (TOF-AMS)–Instrument Description and First Field Deployment, Aerosol Sci. Tech., 39, 637–658, https://doi.org/10.1080/02786820500182040, 2005. a
Drewnick, F., Hings, S. S., Alfarra, M. R., Prevot, A. S. H., and Borrmann, S.: Aerosol quantification with the Aerodyne Aerosol Mass Spectrometer: detection limits and ionizer background effects, Atmos. Meas. Tech., 2, 33–46, https://doi.org/10.5194/amt-2-33-2009, 2009. a
Fadnavis, S., Semeniuk, K., Pozzoli, L., Schultz, M. G., Ghude, S. D., Das, S., and Kakatkar, R.: Transport of aerosols into the UTLS and their impact on the Asian monsoon region as seen in a global model simulation, Atmos. Chem. Phys., 13, 8771–8786, https://doi.org/10.5194/acp-13-8771-2013, 2013. a, b, c, d, e
Fadnavis, S., Roy, C., Chattopadhyay, R., Sioris, C. E., Rap, A., Müller, R., Kumar, K. R., and Krishnan, R.: Transport of trace gases via eddy shedding from the Asian summer monsoon anticyclone and associated impacts on ozone heating rates, Atmos. Chem. Phys., 18, 11493–11506, https://doi.org/10.5194/acp-18-11493-2018, 2018. a
Fadnavis, S., Sabin, T. P., Roy, C., Rowlinson, M., Rap, A., Vernier, J.-P., and Sioris, C. E.: Elevated aerosol layer over South Asia worsens the Indian droughts, Sci- Rep.-UK, 9, 10268, https://doi.org/10.1038/s41598-019-46704-9, 2019. a
Fairlie, T. D., Liu, H., Vernier, J.-P., Campuzano-Jost, P., Jimenez, J. L., Jo, D. S., Zhang, B., Natarajan, M., Avery, M. A., and Huey, G.: Estimates of Regional Source Contributions to the Asian Tropopause Aerosol Layer Using a Chemical Transport Model, J. Geophys. Res.-Atmos., 125, e2019JD031506, https://doi.org/10.1029/2019JD031506, 2020. a, b, c
Froyd, K. D., Murphy, S. M., Murphy, D. M., de Gouw, J. A., Eddingsaas, N. C., and Wennberg, P. O.: Contribution of isoprene-derived organosulfates to free tropospheric aerosol mass, P. Natl. Acad. Sci. USA, 107, 21360–21365, https://doi.org/10.1073/pnas.1012561107, 2010. a, b, c, d
Fujiwara, M., Sakai, T., Nagai, T., Shiraishi, K., Inai, Y., Khaykin, S., Xi, H., Shibata, T., Shiotani, M., and Pan, L. L.: Lower-stratospheric aerosol measurements in eastward-shedding vortices over Japan from the Asian summer monsoon anticyclone during the summer of 2018, Atmos. Chem. Phys., 21, 3073–3090, https://doi.org/10.5194/acp-21-3073-2021, 2021. a
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Short summary
This paper clarifies the chemical composition of the Asian tropopause aerosol layer (ATAL) by means of airborne in situ aerosol mass spectrometry (AMS). Ammonium nitrate and organics are found to significantly contribute to the particle layer, while sulfate does not show a layered structure. An analysis of the single-particle mass spectra suggests that secondary particle formation and subsequent growth dominate the particle composition, rather than condensation on pre-existing primary particles.
This paper clarifies the chemical composition of the Asian tropopause aerosol layer (ATAL) by...
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