Articles | Volume 22, issue 22
https://doi.org/10.5194/acp-22-15135-2022
© 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-22-15135-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
28 Nov 2022
Research article |
| 28 Nov 2022
Enhanced sulfur in the upper troposphere and lower stratosphere in spring 2020
Laura Tomsche
CORRESPONDING AUTHOR
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Johannes Gutenberg University Mainz, 55099 Mainz, Germany
Andreas Marsing
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Johannes Gutenberg University Mainz, 55099 Mainz, Germany
Tina Jurkat-Witschas
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Johannes Lucke
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Faculty of Aerospace Engineering, Delft University of Technology, 2629
Delft, the Netherlands
Stefan Kaufmann
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Katharina Kaiser
Max Planck Institute for Chemistry, 55128 Mainz, Germany
Johannes Schneider
Max Planck Institute for Chemistry, 55128 Mainz, Germany
Monika Scheibe
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Hans Schlager
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Lenard Röder
Max Planck Institute for Chemistry, 55128 Mainz, Germany
Horst Fischer
Max Planck Institute for Chemistry, 55128 Mainz, Germany
Florian Obersteiner
Karlsruhe Institute of Technology (KIT), 76021 Karlsruhe, Germany
Andreas Zahn
Karlsruhe Institute of Technology (KIT), 76021 Karlsruhe, Germany
Martin Zöger
Flight Experiments, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Jos Lelieveld
Max Planck Institute for Chemistry, 55128 Mainz, Germany
Christiane Voigt
Institute of Atmospheric Physics, Deutsches Zentrum für Luft- und Raumfahrt (DLR), 82234 Oberpfaffenhofen, Germany
Johannes Gutenberg University Mainz, 55099 Mainz, Germany
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Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
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Ryan Vella, Matthew Forrest, Jos Lelieveld, and Holger Tost
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Preprint under review for ACP
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Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Andreas Marsing, Ralf Meerkötter, Romy Heller, Stefan Kaufmann, Tina Jurkat-Witschas, Martina Krämer, Christian Rolf, and Christiane Voigt
Atmos. Chem. Phys., 23, 587–609, https://doi.org/10.5194/acp-23-587-2023, https://doi.org/10.5194/acp-23-587-2023, 2023
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Mohamed Abdelkader, Georgiy Stenchikov, Andrea Pozzer, Holger Tost, and Jos Lelieveld
Atmos. Chem. Phys., 23, 471–500, https://doi.org/10.5194/acp-23-471-2023, https://doi.org/10.5194/acp-23-471-2023, 2023
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We study the effect of injected volcanic ash, water vapor, and SO2 on the development of the volcanic cloud and the stratospheric aerosol optical depth (AOD). Both are sensitive to the initial injection height and to the aging of the volcanic ash shaped by heterogeneous chemistry coupled with the ozone cycle. The paper explains the large differences in AOD for different injection scenarios, which could improve the estimate of the radiative forcing of volcanic eruptions.
Marcus Klingebiel, André Ehrlich, Elena Ruiz-Donoso, Nils Risse, Imke Schirmacher, Evelyn Jäkel, Michael Schäfer, Kevin Wolf, Mario Mech, Manuel Moser, Christiane Voigt, and Manfred Wendisch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-848, https://doi.org/10.5194/acp-2022-848, 2023
Preprint under review for ACP
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In this study we explain how we use aircraft measurements from two Arctic research campaigns to identify cloud properties (like droplet size) over sea-ice and ice-free ocean. To make sure that our measurements make sense, we compare them with other observations. Our results show e.g. larger cloud droplets in early summer than in spring. Moreover, the cloud droplets are also larger over ice-free ocean than compared to sea-ice. In the future, our data can be used to improve climate models.
Dirk Dienhart, Bettina Brendel, John N. Crowley, Philipp G. Eger, Hartwig Harder, Monica Martinez, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Sebastian Tauer, David Walter, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 23, 119–142, https://doi.org/10.5194/acp-23-119-2023, https://doi.org/10.5194/acp-23-119-2023, 2023
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Formaldehyde and hydroperoxide measurements were performed in the marine boundary layer around the Arabian Peninsula and highlight the Suez Canal and Arabian (Persian) Gulf as a hotspot of photochemical air pollution. A comparison with the EMAC model shows that the formaldehyde results match within a factor of 2, while hydrogen peroxide was overestimated by more than a factor of 5, which revealed enhanced HOx (OH+HO2) radicals in the simulation and an underestimation of dry deposition velocites.
Johannes Lucke, Tina Jurkat-Witschas, Romy Heller, Valerian Hahn, Matthew Hamman, Wolfgang Breitfuss, Venkateshwar Reddy Bora, Manuel Moser, and Christiane Voigt
Atmos. Meas. Tech., 15, 7375–7394, https://doi.org/10.5194/amt-15-7375-2022, https://doi.org/10.5194/amt-15-7375-2022, 2022
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Flight testing in icing conditions requires instruments that are able to accurately measure the liquid water content of supercooled large droplets (SLDs). This work finds that the 12 mm cone of the Nevzorov hot-wire probe has excellent collection properties for SLDs. We also derive a correction to compensate for the low collision efficiency of small droplets with the cone. The results provide a procedure to evaluate LWC measurements of the 12 mm cone during wind tunnel and airborne experiments.
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. Discuss., https://doi.org/10.5194/acp-2022-795, https://doi.org/10.5194/acp-2022-795, 2022
Revised manuscript under review for ACP
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During the DACCIWA campaign in West Africa we found a 35 % increase of cloud droplet concentration that formed in a polluted, compared to 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 to a less polluted cloud. The corresponding additional decrease in temperature turns out rather small.
Silke Groß, Tina Jurkat-Witschas, Qiang Li, Martin Wirth, Benedikt Urbanek, Martina Krämer, Ralf Weigel, and Christiane Voigt
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-721, https://doi.org/10.5194/acp-2022-721, 2022
Revised manuscript under review for ACP
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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 either 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.
Hossein Dadashazar, Andrea F. Corral, Ewan Crosbie, Sanja Dmitrovic, Simon Kirschler, Kayla McCauley, Richard Moore, Claire Robinson, Joseph S. Schlosser, Michael Shook, K. Lee Thornhill, Christiane Voigt, Edward Winstead, Luke Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 22, 13897–13913, https://doi.org/10.5194/acp-22-13897-2022, https://doi.org/10.5194/acp-22-13897-2022, 2022
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Multi-season airborne data over the northwestern Atlantic show that organic mass fraction and the relative amount of oxygenated organics within that fraction are enhanced in droplet residual particles as compared to particles below and above cloud. In-cloud aqueous processing is shown to be a potential driver of this compositional shift in cloud. This implies that aerosol–cloud interactions in the region reduce aerosol hygroscopicity due to the jump in the organic : sulfate ratio in cloud.
Oliver Appel, Franziska Köllner, Antonis Dragoneas, Andreas Hünig, Sergej Molleker, Hans Schlager, Christoph Mahnke, Ralf Weigel, Max Port, Christiane Schulz, Frank Drewnick, Bärbel Vogel, Fred Stroh, and Stephan Borrmann
Atmos. Chem. Phys., 22, 13607–13630, https://doi.org/10.5194/acp-22-13607-2022, https://doi.org/10.5194/acp-22-13607-2022, 2022
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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.
Zaneta Hamryszczak, Dirk Dienhart, Bettina Brendel, Roland Rohloff, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Birger Bohn, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-693, https://doi.org/10.5194/acp-2022-693, 2022
Revised manuscript not accepted
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Hydrogen peroxide is a key contributor to the oxidative chemistry of the atmosphere through its link to the most prominent oxidants controlling its self-cleansing capacity, HOx. During CAFE-Africa campaign, H2O2 was measured over the Atlantic Ocean and western Africa in August/September 2018. The study gives an overview of the distribution of H2O2 in the upper tropical troposphere and investigates the impact of convective processes in the Intertropical Convergence Zone on the budget of H2O2.
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.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-232, https://doi.org/10.5194/gmd-2022-232, 2022
Preprint under review for GMD
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Desert dust has significant impacts on climate, public health, infrastructure and ecosystems. The impact assessment requires numerical predictions, which are challenging because the dust emissions are not well known. We present a novel approach using satellite observations and machine learning to more accurately estimate the emissions and to improve the model simulations.
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.
Mengze Li, Andrea Pozzer, Jos Lelieveld, and Jonathan Williams
Earth Syst. Sci. Data, 14, 4351–4364, https://doi.org/10.5194/essd-14-4351-2022, https://doi.org/10.5194/essd-14-4351-2022, 2022
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We present a northern hemispheric airborne measurement dataset of atmospheric ethane, propane and methane and temporal trends for the time period 2006–2016 in the upper troposphere and lower stratosphere. The growth rates of ethane, methane, and propane in the upper troposphere are -2.24, 0.33, and -0.78 % yr-1, respectively, and in the lower stratosphere they are -3.27, 0.26, and -4.91 % yr-1, respectively, in 2006–2016.
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.
Roger Teoh, Ulrich Schumann, Edward Gryspeerdt, Marc Shapiro, Jarlath Molloy, George Koudis, Christiane Voigt, and Marc E. J. Stettler
Atmos. Chem. Phys., 22, 10919–10935, https://doi.org/10.5194/acp-22-10919-2022, https://doi.org/10.5194/acp-22-10919-2022, 2022
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Aircraft condensation trails (contrails) contribute to over half of the climate forcing attributable to aviation. This study uses historical air traffic and weather data to simulate contrails in the North Atlantic over 5 years, from 2016 to 2021. We found large intra- and inter-year variability in contrail radiative forcing and observed a 66 % reduction due to COVID-19. Most warming contrails predominantly result from night-time flights in winter.
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.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
Simon Kirschler, Christiane Voigt, Bruce Anderson, Ramon Campos Braga, Gao Chen, Andrea F. Corral, Ewan Crosbie, Hossein Dadashazar, Richard A. Ferrare, Valerian Hahn, Johannes Hendricks, Stefan Kaufmann, Richard Moore, Mira L. Pöhlker, Claire Robinson, Amy J. Scarino, Dominik Schollmayer, Michael A. Shook, K. Lee Thornhill, Edward Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 22, 8299–8319, https://doi.org/10.5194/acp-22-8299-2022, https://doi.org/10.5194/acp-22-8299-2022, 2022
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In this study we show that the vertical velocity dominantly impacts the cloud droplet number concentration (NC) of low-level clouds over the western North Atlantic in the winter and summer season, while the cloud condensation nuclei concentration, aerosol size distribution and chemical composition impact NC within a season. The observational data presented in this study can evaluate and improve the representation of aerosol–cloud interactions for a wide range of conditions.
Patrick Dewald, Clara M. Nussbaumer, Jan Schuladen, Akima Ringsdorf, Achim Edtbauer, Horst Fischer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 7051–7069, https://doi.org/10.5194/acp-22-7051-2022, https://doi.org/10.5194/acp-22-7051-2022, 2022
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We measured the gas-phase reactivity of the NO3 radical on the summit (825 m a.s.l.) of a semi-rural mountain in southwestern Germany in July 2021. The impact of VOC-induced NO3 losses (mostly monoterpenes) competing with a loss by reaction with NO and photolysis throughout the diel cycle was estimated. Besides chemistry, boundary layer dynamics and plant-physiological processes presumably have a great impact on our observations, which were compared to previous NO3 measurements at the same site.
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.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
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.
Mireia Papke Chica, Valerian Hahn, Tiziana Braeuer, Elena de la Torre Castro, Florian Ewald, Mathias Gergely, Simon Kirschler, Luca Bugliaro Goggia, Stefanie Knobloch, Martina Kraemer, Johannes Lucke, Johanna Mayer, Raphael Maerkl, Manuel Moser, Laura Tomsche, Tina Jurkat-Witschas, Martin Zoeger, Christian von Savigny, and Christiane Voigt
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-255, https://doi.org/10.5194/acp-2022-255, 2022
Preprint withdrawn
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The mixed-phase temperature regime in convective clouds challenges our understanding of microphysical and radiative cloud properties. We provide a rare and unique dataset of aircraft in situ measurements in a strong mid-latitude convective system. We find that mechanisms initiating ice nucleation and growth strongly depend on temperature, relative humidity, and vertical velocity and variate within the measured system, resulting in altitude dependent changes of the cloud liquid and ice fraction.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
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.
Adrien Deroubaix, Laurent Menut, Cyrille Flamant, Peter Knippertz, Andreas H. Fink, Anneke Batenburg, Joel Brito, Cyrielle Denjean, Cheikh Dione, Régis Dupuy, Valerian Hahn, Norbert Kalthoff, Fabienne Lohou, Alfons Schwarzenboeck, Guillaume Siour, Paolo Tuccella, and Christiane Voigt
Atmos. Chem. Phys., 22, 3251–3273, https://doi.org/10.5194/acp-22-3251-2022, https://doi.org/10.5194/acp-22-3251-2022, 2022
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During the summer monsoon in West Africa, pollutants emitted in urbanized areas modify cloud cover and precipitation patterns. We analyze these patterns with the WRF-CHIMERE model, integrating the effects of aerosols on meteorology, based on the numerous observations provided by the Dynamics-Aerosol-Climate-Interactions campaign. This study adds evidence to recent findings that increased pollution levels in West Africa delay the breakup time of low-level clouds and reduce precipitation.
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. Discuss., https://doi.org/10.5194/acp-2022-119, https://doi.org/10.5194/acp-2022-119, 2022
Revised manuscript under review for ACP
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The applicability photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the airborne observations from the known radical chemistry and on-board 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 airmasses measured.
Clara M. Nussbaumer, John N. Crowley, Jan Schuladen, Jonathan Williams, Sascha Hafermann, Andreas Reiffs, Raoul Axinte, Hartwig Harder, Cheryl Ernest, Anna Novelli, Katrin Sala, Monica Martinez, Chinmay Mallik, Laura Tomsche, Christian Plass-Dülmer, Birger Bohn, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 18413–18432, https://doi.org/10.5194/acp-21-18413-2021, https://doi.org/10.5194/acp-21-18413-2021, 2021
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HCHO is an important atmospheric trace gas influencing the photochemical processes in the Earth’s atmosphere, including the budget of HOx and the abundance of tropospheric O3. This research presents the photochemical calculations of HCHO and O3 based on three field campaigns across Europe. We show that HCHO production via the oxidation of only four volatile organic compound precursors, i.e., CH4, CH3CHO, C5H8 and CH3OH, can balance the observed loss at all sites well.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
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Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Dirk Dienhart, John N. Crowley, Efstratios Bourtsoukidis, Achim Edtbauer, Philipp G. Eger, Lisa Ernle, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Eva Y. Pfannerstill, Roland Rohloff, Jan Schuladen, Christof Stönner, Ivan Tadic, Sebastian Tauer, Nijing Wang, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 17373–17388, https://doi.org/10.5194/acp-21-17373-2021, https://doi.org/10.5194/acp-21-17373-2021, 2021
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We present the first ship-based in situ measurements of formaldehyde (HCHO), hydroxyl radicals (OH) and the OH reactivity around the Arabian Peninsula. Regression analysis of the HCHO production rate and the related OH chemistry revealed the regional HCHO yield αeff, which represents the different chemical regimes encountered. Highest values were found for the Arabian Gulf (also known as the Persian Gulf), which highlights this region as a hotspot of photochemical air pollution.
Silke Trömel, Clemens Simmer, Ulrich Blahak, Armin Blanke, Sabine Doktorowski, Florian Ewald, Michael Frech, Mathias Gergely, Martin Hagen, Tijana Janjic, Heike Kalesse-Los, Stefan Kneifel, Christoph Knote, Jana Mendrok, Manuel Moser, Gregor Köcher, Kai Mühlbauer, Alexander Myagkov, Velibor Pejcic, Patric Seifert, Prabhakar Shrestha, Audrey Teisseire, Leonie von Terzi, Eleni Tetoni, Teresa Vogl, Christiane Voigt, Yuefei Zeng, Tobias Zinner, and Johannes Quaas
Atmos. Chem. Phys., 21, 17291–17314, https://doi.org/10.5194/acp-21-17291-2021, https://doi.org/10.5194/acp-21-17291-2021, 2021
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The article introduces the ACP readership to ongoing research in Germany on cloud- and precipitation-related process information inherent in polarimetric radar measurements, outlines pathways to inform atmospheric models with radar-based information, and points to remaining challenges towards an improved fusion of radar polarimetry and atmospheric modelling.
Heike Konow, Florian Ewald, Geet George, Marek Jacob, Marcus Klingebiel, Tobias Kölling, Anna E. Luebke, Theresa Mieslinger, Veronika Pörtge, Jule Radtke, Michael Schäfer, Hauke Schulz, Raphaela Vogel, Martin Wirth, Sandrine Bony, Susanne Crewell, André Ehrlich, Linda Forster, Andreas Giez, Felix Gödde, Silke Groß, Manuel Gutleben, Martin Hagen, Lutz Hirsch, Friedhelm Jansen, Theresa Lang, Bernhard Mayer, Mario Mech, Marc Prange, Sabrina Schnitt, Jessica Vial, Andreas Walbröl, Manfred Wendisch, Kevin Wolf, Tobias Zinner, Martin Zöger, Felix Ament, and Bjorn Stevens
Earth Syst. Sci. Data, 13, 5545–5563, https://doi.org/10.5194/essd-13-5545-2021, https://doi.org/10.5194/essd-13-5545-2021, 2021
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The German research aircraft HALO took part in the research campaign EUREC4A in January and February 2020. The focus area was the tropical Atlantic east of the island of Barbados. We describe the characteristics of the 15 research flights, provide auxiliary information, derive combined cloud mask products from all instruments that observe clouds on board the aircraft, and provide code examples that help new users of the data to get started.
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.
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 %.
Hossein Dadashazar, Majid Alipanah, Miguel Ricardo A. Hilario, Ewan Crosbie, Simon Kirschler, Hongyu Liu, Richard H. Moore, Andrew J. Peters, Amy Jo Scarino, Michael Shook, K. Lee Thornhill, Christiane Voigt, Hailong Wang, Edward Winstead, Bo Zhang, Luke Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 21, 16121–16141, https://doi.org/10.5194/acp-21-16121-2021, https://doi.org/10.5194/acp-21-16121-2021, 2021
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This study investigates precipitation impacts on long-range transport of North American outflow over the western North Atlantic Ocean (WNAO). Results demonstrate that precipitation scavenging plays a significant role in modifying surface aerosol concentrations over the WNAO, especially in winter and spring due to large-scale scavenging processes. This study highlights how precipitation impacts surface aerosol properties with relevance for other marine regions vulnerable to continental outflow.
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.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 21, 14983–15001, https://doi.org/10.5194/acp-21-14983-2021, https://doi.org/10.5194/acp-21-14983-2021, 2021
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Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity).
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.
Philipp G. Eger, Luc Vereecken, Rolf Sander, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Ville Vakkari, Tuukka Petäjä, Jos Lelieveld, Andrea Pozzer, and John N. Crowley
Atmos. Chem. Phys., 21, 14333–14349, https://doi.org/10.5194/acp-21-14333-2021, https://doi.org/10.5194/acp-21-14333-2021, 2021
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We determine the impact of pyruvic acid photolysis on the formation of acetaldehyde and peroxy radicals during summer and autumn in the Finnish boreal forest using a data-constrained box model. Our results are dependent on the chosen scenario in which the overall quantum yield and the photolysis products are varied. We highlight that pyruvic acid photolysis can be an important contributor to acetaldehyde and peroxy radical formation in remote, forested regions.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
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Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
Bjorn Stevens, Sandrine Bony, David Farrell, Felix Ament, Alan Blyth, Christopher Fairall, Johannes Karstensen, Patricia K. Quinn, Sabrina Speich, Claudia Acquistapace, Franziska Aemisegger, Anna Lea Albright, Hugo Bellenger, Eberhard Bodenschatz, Kathy-Ann Caesar, Rebecca Chewitt-Lucas, Gijs de Boer, Julien Delanoë, Leif Denby, Florian Ewald, Benjamin Fildier, Marvin Forde, Geet George, Silke Gross, Martin Hagen, Andrea Hausold, Karen J. Heywood, Lutz Hirsch, Marek Jacob, Friedhelm Jansen, Stefan Kinne, Daniel Klocke, Tobias Kölling, Heike Konow, Marie Lothon, Wiebke Mohr, Ann Kristin Naumann, Louise Nuijens, Léa Olivier, Robert Pincus, Mira Pöhlker, Gilles Reverdin, Gregory Roberts, Sabrina Schnitt, Hauke Schulz, A. Pier Siebesma, Claudia Christine Stephan, Peter Sullivan, Ludovic Touzé-Peiffer, Jessica Vial, Raphaela Vogel, Paquita Zuidema, Nicola Alexander, Lyndon Alves, Sophian Arixi, Hamish Asmath, Gholamhossein Bagheri, Katharina Baier, Adriana Bailey, Dariusz Baranowski, Alexandre Baron, Sébastien Barrau, Paul A. Barrett, Frédéric Batier, Andreas Behrendt, Arne Bendinger, Florent Beucher, Sebastien Bigorre, Edmund Blades, Peter Blossey, Olivier Bock, Steven Böing, Pierre Bosser, Denis Bourras, Pascale Bouruet-Aubertot, Keith Bower, Pierre Branellec, Hubert Branger, Michal Brennek, Alan Brewer, Pierre-Etienne Brilouet, Björn Brügmann, Stefan A. Buehler, Elmo Burke, Ralph Burton, Radiance Calmer, Jean-Christophe Canonici, Xavier Carton, Gregory Cato Jr., Jude Andre Charles, Patrick Chazette, Yanxu Chen, Michal T. Chilinski, Thomas Choularton, Patrick Chuang, Shamal Clarke, Hugh Coe, Céline Cornet, Pierre Coutris, Fleur Couvreux, Susanne Crewell, Timothy Cronin, Zhiqiang Cui, Yannis Cuypers, Alton Daley, Gillian M. Damerell, Thibaut Dauhut, Hartwig Deneke, Jean-Philippe Desbios, Steffen Dörner, Sebastian Donner, Vincent Douet, Kyla Drushka, Marina Dütsch, André Ehrlich, Kerry Emanuel, Alexandros Emmanouilidis, Jean-Claude Etienne, Sheryl Etienne-Leblanc, Ghislain Faure, Graham Feingold, Luca Ferrero, Andreas Fix, Cyrille Flamant, Piotr Jacek Flatau, Gregory R. Foltz, Linda Forster, Iulian Furtuna, Alan Gadian, Joseph Galewsky, Martin Gallagher, Peter Gallimore, Cassandra Gaston, Chelle Gentemann, Nicolas Geyskens, Andreas Giez, John Gollop, Isabelle Gouirand, Christophe Gourbeyre, Dörte de Graaf, Geiske E. de Groot, Robert Grosz, Johannes Güttler, Manuel Gutleben, Kashawn Hall, George Harris, Kevin C. Helfer, Dean Henze, Calvert Herbert, Bruna Holanda, Antonio Ibanez-Landeta, Janet Intrieri, Suneil Iyer, Fabrice Julien, Heike Kalesse, Jan Kazil, Alexander Kellman, Abiel T. Kidane, Ulrike Kirchner, Marcus Klingebiel, Mareike Körner, Leslie Ann Kremper, Jan Kretzschmar, Ovid Krüger, Wojciech Kumala, Armin Kurz, Pierre L'Hégaret, Matthieu Labaste, Tom Lachlan-Cope, Arlene Laing, Peter Landschützer, Theresa Lang, Diego Lange, Ingo Lange, Clément Laplace, Gauke Lavik, Rémi Laxenaire, Caroline Le Bihan, Mason Leandro, Nathalie Lefevre, Marius Lena, Donald Lenschow, Qiang Li, Gary Lloyd, Sebastian Los, Niccolò Losi, Oscar Lovell, Christopher Luneau, Przemyslaw Makuch, Szymon Malinowski, Gaston Manta, Eleni Marinou, Nicholas Marsden, Sebastien Masson, Nicolas Maury, Bernhard Mayer, Margarette Mayers-Als, Christophe Mazel, Wayne McGeary, James C. McWilliams, Mario Mech, Melina Mehlmann, Agostino Niyonkuru Meroni, Theresa Mieslinger, Andreas Minikin, Peter Minnett, Gregor Möller, Yanmichel Morfa Avalos, Caroline Muller, Ionela Musat, Anna Napoli, Almuth Neuberger, Christophe Noisel, David Noone, Freja Nordsiek, Jakub L. Nowak, Lothar Oswald, Douglas J. Parker, Carolyn Peck, Renaud Person, Miriam Philippi, Albert Plueddemann, Christopher Pöhlker, Veronika Pörtge, Ulrich Pöschl, Lawrence Pologne, Michał Posyniak, Marc Prange, Estefanía Quiñones Meléndez, Jule Radtke, Karim Ramage, Jens Reimann, Lionel Renault, Klaus Reus, Ashford Reyes, Joachim Ribbe, Maximilian Ringel, Markus Ritschel, Cesar B. Rocha, Nicolas Rochetin, Johannes Röttenbacher, Callum Rollo, Haley Royer, Pauline Sadoulet, Leo Saffin, Sanola Sandiford, Irina Sandu, Michael Schäfer, Vera Schemann, Imke Schirmacher, Oliver Schlenczek, Jerome Schmidt, Marcel Schröder, Alfons Schwarzenboeck, Andrea Sealy, Christoph J. Senff, Ilya Serikov, Samkeyat Shohan, Elizabeth Siddle, Alexander Smirnov, Florian Späth, Branden Spooner, M. Katharina Stolla, Wojciech Szkółka, Simon P. de Szoeke, Stéphane Tarot, Eleni Tetoni, Elizabeth Thompson, Jim Thomson, Lorenzo Tomassini, Julien Totems, Alma Anna Ubele, Leonie Villiger, Jan von Arx, Thomas Wagner, Andi Walther, Ben Webber, Manfred Wendisch, Shanice Whitehall, Anton Wiltshire, Allison A. Wing, Martin Wirth, Jonathan Wiskandt, Kevin Wolf, Ludwig Worbes, Ethan Wright, Volker Wulfmeyer, Shanea Young, Chidong Zhang, Dongxiao Zhang, Florian Ziemen, Tobias Zinner, and Martin Zöger
Earth Syst. Sci. Data, 13, 4067–4119, https://doi.org/10.5194/essd-13-4067-2021, https://doi.org/10.5194/essd-13-4067-2021, 2021
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The EUREC4A field campaign, designed to test hypothesized mechanisms by which clouds respond to warming and benchmark next-generation Earth-system models, is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. It was the first campaign that attempted to characterize the full range of processes and scales influencing trade wind clouds.
Jean-Daniel Paris, Aurélie Riandet, Efstratios Bourtsoukidis, Marc Delmotte, Antoine Berchet, Jonathan Williams, Lisa Ernle, Ivan Tadic, Hartwig Harder, and Jos Lelieveld
Atmos. Chem. Phys., 21, 12443–12462, https://doi.org/10.5194/acp-21-12443-2021, https://doi.org/10.5194/acp-21-12443-2021, 2021
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We measured atmospheric methane and CO2 by ship in the Middle East. We probe the origin of methane with a combination of light alkane measurements and modeling. We find strong influence from nearby oil and gas production over the Arabian Gulf. Comparing our data to inventories indicates that inventories overestimate sources from the upstream gas industry but underestimate emissions from oil extraction and processing. The Red Sea was under a complex mixture of sources due to human activity.
Patrick Dewald, Raphael Dörich, Jan Schuladen, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5501–5519, https://doi.org/10.5194/amt-14-5501-2021, https://doi.org/10.5194/amt-14-5501-2021, 2021
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Organic nitrates generated from the reaction between isoprene and the nitrate radical (ISOP-NITs) were detected via their thermal dissociation in heated quartz inlets to nitrogen dioxide monitored by cavity ring-down spectroscopy. The temperature-dependent dissociation profiles of ISOP-NITs in the presence of ozone (O3) are broad in contrast to narrow profiles of common reference compounds. We demonstrate that this broadening is caused by O3-assisted reactions of ISOP-NITs on quartz surfaces.
Raphael Dörich, Philipp Eger, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 14, 5319–5332, https://doi.org/10.5194/amt-14-5319-2021, https://doi.org/10.5194/amt-14-5319-2021, 2021
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We demonstrate in laboratory experiments that the formation of IOx anions (formed in reactions of I− with O3) or acetate anions (formed e.g. by the reaction of I− with peracetic acid) results in unexpected sensitivity of an iodide chemical ionisation mass spectrometer (I-CIMS) to HNO3 at a mass-to-charge ratio of 62. This helps explain observations of apparent high daytime levels of N2O5. Airborne measurements using I-CIMS confirm these conclusions.
Vinod Kumar, Julia Remmers, Steffen Beirle, Joachim Fallmann, Astrid Kerkweg, Jos Lelieveld, Mariano Mertens, Andrea Pozzer, Benedikt Steil, Marc Barra, Holger Tost, and Thomas Wagner
Atmos. Meas. Tech., 14, 5241–5269, https://doi.org/10.5194/amt-14-5241-2021, https://doi.org/10.5194/amt-14-5241-2021, 2021
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We present high-resolution regional atmospheric chemistry model simulations focused around Germany. We highlight the importance of spatial resolution of the model itself as well as the input emissions inventory and short-scale temporal variability of emissions for simulations. We propose a consistent approach for evaluating the simulated vertical distribution of NO2 using MAX-DOAS measurements while also considering its spatial sensitivity volume and change in sensitivity within this volume.
Klaus Klingmüller and Jos Lelieveld
Geosci. Model Dev., 14, 4429–4441, https://doi.org/10.5194/gmd-14-4429-2021, https://doi.org/10.5194/gmd-14-4429-2021, 2021
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Soil moisture is of great importance for weather and climate. We present a machine learning model that produces accurate predictions of satellite-observed surface soil moisture, based on meteorological data from a climate model. It can be used as soil moisture parametrisation in climate models and to produce comprehensive global soil moisture datasets. Moreover, it may motivate similar applications of machine learning in climate science.
Hossein Dadashazar, David Painemal, Majid Alipanah, Michael Brunke, Seethala Chellappan, Andrea F. Corral, Ewan Crosbie, Simon Kirschler, Hongyu Liu, Richard H. Moore, Claire Robinson, Amy Jo Scarino, Michael Shook, Kenneth Sinclair, K. Lee Thornhill, Christiane Voigt, Hailong Wang, Edward Winstead, Xubin Zeng, Luke Ziemba, Paquita Zuidema, and Armin Sorooshian
Atmos. Chem. Phys., 21, 10499–10526, https://doi.org/10.5194/acp-21-10499-2021, https://doi.org/10.5194/acp-21-10499-2021, 2021
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This study investigates the seasonal cycle of cloud drop number concentration (Nd) over the western North Atlantic Ocean (WNAO) using multiple datasets. Reasons for the puzzling discrepancy between the seasonal cycles of Nd and aerosol concentration were identified. Results indicate that Nd is highest in winter (when aerosol proxy values are often lowest) due to conditions both linked to cold-air outbreaks and that promote greater droplet activation.
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.
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.
Romain Blot, Philippe Nedelec, Damien Boulanger, Pawel Wolff, Bastien Sauvage, Jean-Marc Cousin, Gilles Athier, Andreas Zahn, Florian Obersteiner, Dieter Scharffe, Hervé Petetin, Yasmine Bennouna, Hannah Clark, and Valérie Thouret
Atmos. Meas. Tech., 14, 3935–3951, https://doi.org/10.5194/amt-14-3935-2021, https://doi.org/10.5194/amt-14-3935-2021, 2021
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A lack of information about temporal changes in measurement uncertainties is an area of concern for long-term trend studies of the key compounds which have a direct or indirect impact on climate change. The IAGOS program has measured O3 and CO within the troposphere and lower stratosphere for more than 25 years. In this study, we demonstrated that the IAGOS database can be treated as one continuous program and is therefore appropriate for studies of long-term trends.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
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.
Ulrich Schumann, Ian Poll, Roger Teoh, Rainer Koelle, Enrico Spinielli, Jarlath Molloy, George S. Koudis, Robert Baumann, Luca Bugliaro, Marc Stettler, and Christiane Voigt
Atmos. Chem. Phys., 21, 7429–7450, https://doi.org/10.5194/acp-21-7429-2021, https://doi.org/10.5194/acp-21-7429-2021, 2021
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The roughly 70 % reduction of air traffic during the COVID-19 pandemic from March–August 2020 compared to 2019 provides a test case for the relationship between air traffic density, contrails, and their radiative forcing of climate change. This paper investigates the induced traffic and contrail changes in a model study. Besides strong weather changes, the model results indicate aviation-induced cirrus and top-of-the-atmosphere irradiance changes, which can be tested with observations.
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.
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.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Inken Knop, Stephan E. Bansmer, Valerian Hahn, and Christiane Voigt
Atmos. Meas. Tech., 14, 1761–1781, https://doi.org/10.5194/amt-14-1761-2021, https://doi.org/10.5194/amt-14-1761-2021, 2021
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Knowledge on droplet size and concentration is essential for several applications of atomizers. After having developed a new spray system for our icing wind tunnel, we did intercomparison tests of different droplet measurement techniques including two commercial probes. The probes proved the good repeatability of the spray conditions and showed good overall agreement in measuring size and concentration. Furthermore, we could identify limitations and error sources of the measuring techniques.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Domenico Taraborrelli, David Cabrera-Perez, Sara Bacer, Sergey Gromov, Jos Lelieveld, Rolf Sander, and Andrea Pozzer
Atmos. Chem. Phys., 21, 2615–2636, https://doi.org/10.5194/acp-21-2615-2021, https://doi.org/10.5194/acp-21-2615-2021, 2021
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Atmospheric pollutants from anthropogenic activities and biomass burning are usually regarded as ozone precursors. Monocyclic aromatics are no exception. Calculations with a comprehensive atmospheric model are consistent with this view but only for air masses close to pollution source regions. However, the same model predicts that aromatics, when transported to remote areas, may effectively destroy ozone. This loss of tropospheric ozone rivals the one attributed to bromine.
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.
Sara Bacer, Sylvia C. Sullivan, Odran Sourdeval, Holger Tost, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 21, 1485–1505, https://doi.org/10.5194/acp-21-1485-2021, https://doi.org/10.5194/acp-21-1485-2021, 2021
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We investigate the relative importance of the rates of both microphysical processes and unphysical correction terms that act as sources or sinks of ice crystals in cold clouds. By means of numerical simulations performed with a global chemistry–climate model, we assess the relevance of these rates at global and regional scales. This estimation is of fundamental importance to assign priority to the development of microphysics parameterizations and compare model output with observations.
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.
Klaus Klingmüller, Vlassis A. Karydis, Sara Bacer, Georgiy L. Stenchikov, and Jos Lelieveld
Atmos. Chem. Phys., 20, 15285–15295, https://doi.org/10.5194/acp-20-15285-2020, https://doi.org/10.5194/acp-20-15285-2020, 2020
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Particulate air pollution cools the climate and partially masks the greenhouse warming by reflecting sunlight and enhancing the reflection by clouds. The intensity of this cooling depends on interactions between pollution and desert dust within the atmosphere. Our simulations with a global atmospheric chemistry-climate model indicate that these interactions significantly weaken the cooling.
Matias Berasategui, Damien Amedro, Luc Vereecken, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 13541–13555, https://doi.org/10.5194/acp-20-13541-2020, https://doi.org/10.5194/acp-20-13541-2020, 2020
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Peracetic acid is one of the most abundant organic peroxides in the atmosphere. We combine experiments and theory to show that peracetic acid reacts orders of magnitude more slowly with OH than presently accepted, which results in a significant extension of its atmospheric lifetime.
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.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
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.
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.
Nijing Wang, Achim Edtbauer, Christof Stönner, Andrea Pozzer, Efstratios Bourtsoukidis, Lisa Ernle, Dirk Dienhart, Bettina Hottmann, Horst Fischer, Jan Schuladen, John N. Crowley, Jean-Daniel Paris, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 10807–10829, https://doi.org/10.5194/acp-20-10807-2020, https://doi.org/10.5194/acp-20-10807-2020, 2020
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Carbonyl compounds were measured on a ship travelling around the Arabian Peninsula in summer 2017, crossing both highly polluted and extremely clean regions of the marine boundary layer. We investigated the sources and sinks of carbonyls. The results from a global model showed a significant model underestimation for acetaldehyde, a molecule that can influence regional air chemistry. By adding a diurnal oceanic source, the model estimation was highly improved.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Sergej Molleker, Frank Helleis, Thomas Klimach, Oliver Appel, Hans-Christian Clemen, Antonis Dragoneas, Christian Gurk, Andreas Hünig, Franziska Köllner, Florian Rubach, Christiane Schulz, Johannes Schneider, and Stephan Borrmann
Atmos. Meas. Tech., 13, 3651–3660, https://doi.org/10.5194/amt-13-3651-2020, https://doi.org/10.5194/amt-13-3651-2020, 2020
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A novel constant-pressure-inlet design for use in airborne aerosol particle mass spectrometry – an aerodynamic lens focuses aerosol particles into a vacuum chamber – is presented. The pressure of a few hectopascals at the lens is precisely controlled over a large flight altitude range up to 21 km. The constant pressure is achieved by changing the inner diameter of a properly scaled flexible O-ring acting as a critical orifice. Particle transmission at various inlet pressures is characterized.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ivan Tadic, John N. Crowley, Dirk Dienhart, Philipp Eger, Hartwig Harder, Bettina Hottmann, Monica Martinez, Uwe Parchatka, Jean-Daniel Paris, Andrea Pozzer, Roland Rohloff, Jan Schuladen, Justin Shenolikar, Sebastian Tauer, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 6769–6787, https://doi.org/10.5194/acp-20-6769-2020, https://doi.org/10.5194/acp-20-6769-2020, 2020
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We present shipborne observations of NO, NO2, O3, HCHO, OH, HO2, H2O and the actinic flux obtained in the marine boundary layer (MBL) around the Arabian Peninsula during the summer 2017 AQABA ship campaign. NOx (NO+NO2) and O3 observations clearly showed anthropogenic influence in the MBL around the Arabian Peninsula. The observations were also used to calculate net O3 production in the MBL around the Arabian Peninsula, which was greatest over the northern Red Sea, Oman Gulf and Arabian Gulf.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Achim Edtbauer, Christof Stönner, Eva Y. Pfannerstill, Matias Berasategui, David Walter, John N. Crowley, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 20, 6081–6094, https://doi.org/10.5194/acp-20-6081-2020, https://doi.org/10.5194/acp-20-6081-2020, 2020
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Marine regions where deep nutrient-rich water is pushed towards the surface are called upwelling regions. In these nutrient-rich waters large algal blooms form which are the basis of the marine food web. We measured methane sulfonamide, a molecule containing sulfur and nitrogen, for the first time in ambient air and could show that the origin of this emission is an algal bloom near the Somalia upwelling. Sulfur-containing compounds from algae can promote particle formation over the oceans.
Peter H. Zimmermann, Carl A. M. Brenninkmeijer, Andrea Pozzer, Patrick Jöckel, Franziska Winterstein, Andreas Zahn, Sander Houweling, and Jos Lelieveld
Atmos. Chem. Phys., 20, 5787–5809, https://doi.org/10.5194/acp-20-5787-2020, https://doi.org/10.5194/acp-20-5787-2020, 2020
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The atmospheric abundance of the greenhouse gas methane is determined by interacting emission sources and sinks in a dynamic global environment. In this study, its global budget from 1997 to 2016 is simulated with a general circulation model using emission estimates of 11 source categories. The model results are evaluated against 17 ground station and 320 intercontinental flight observation series. Deviations are used to re-scale the emission quantities with the aim of matching observations.
Bruna A. Holanda, Mira L. Pöhlker, David Walter, Jorge Saturno, Matthias Sörgel, Jeannine Ditas, Florian Ditas, Christiane Schulz, Marco Aurélio Franco, Qiaoqiao Wang, Tobias Donth, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Ramon Braga, Joel Brito, Yafang Cheng, Maximilian Dollner, Johannes W. Kaiser, Thomas Klimach, Christoph Knote, Ovid O. Krüger, Daniel Fütterer, Jošt V. Lavrič, Nan Ma, Luiz A. T. Machado, Jing Ming, Fernando G. Morais, Hauke Paulsen, Daniel Sauer, Hans Schlager, Johannes Schneider, Hang Su, Bernadett Weinzierl, Adrian Walser, Manfred Wendisch, Helmut Ziereis, Martin Zöger, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 20, 4757–4785, https://doi.org/10.5194/acp-20-4757-2020, https://doi.org/10.5194/acp-20-4757-2020, 2020
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Biomass burning smoke from African savanna and grassland is transported across the South Atlantic Ocean in defined layers within the free troposphere. The combination of in situ aircraft and ground-based measurements aided by satellite observations showed that these layers are transported into the Amazon Basin during the early dry season. The influx of aged smoke, enriched in black carbon and cloud condensation nuclei, has important implications for the Amazonian aerosol and cloud cycling.
Siddika Celik, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Hugh Coe, Jean-Daniel Paris, Philipp G. Eger, Jan Schuladen, Ivan Tadic, Nils Friedrich, Dirk Dienhart, Bettina Hottmann, Horst Fischer, John N. Crowley, Hartwig Harder, and Stephan Borrmann
Atmos. Chem. Phys., 20, 4713–4734, https://doi.org/10.5194/acp-20-4713-2020, https://doi.org/10.5194/acp-20-4713-2020, 2020
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Analysis of 252 ship emission plumes in the Mediterranean Sea and around the Arabian Peninsula examined particulate- and gas-phase characteristics. By identifying the corresponding ships, source features and plume age were determined. Emission factors (amount of pollutant per kilogram of fuel burned) were calculated and investigated for dependencies on source characteristics, atmospheric conditions, and transport time, providing insight into the most relevant influences on ship emissions.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
Mattia Righi, Johannes Hendricks, Ulrike Lohmann, Christof Gerhard Beer, Valerian Hahn, Bernd Heinold, Romy Heller, Martina Krämer, Michael Ponater, Christian Rolf, Ina Tegen, and Christiane Voigt
Geosci. Model Dev., 13, 1635–1661, https://doi.org/10.5194/gmd-13-1635-2020, https://doi.org/10.5194/gmd-13-1635-2020, 2020
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A new cloud microphysical scheme is implemented in the global EMAC-MADE3 aerosol model and evaluated. The new scheme features a detailed parameterization for aerosol-driven ice formation in cirrus clouds, accounting for the competition between homogeneous and heterogeneous ice formation processes. The comparison against satellite data and in situ measurements shows that the model performance is in line with similar global coupled models featuring ice cloud parameterizations.
Philipp G. Eger, Jan Schuladen, Nicolas Sobanski, Horst Fischer, Einar Karu, Jonathan Williams, Matthieu Riva, Qiaozhi Zha, Mikael Ehn, Lauriane L. J. Quéléver, Simon Schallhart, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 3697–3711, https://doi.org/10.5194/acp-20-3697-2020, https://doi.org/10.5194/acp-20-3697-2020, 2020
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Pyruvic acid, CH3C(O)C(O)OH, is an organic acid of biogenic origin that plays a crucial role in plant metabolism, is present in tropospheric air in both gas-phase and aerosol-phase, and is implicated in the formation of secondary organic aerosols. From the first gas-phase measurements of pyruvic acid in the Finnish boreal forest in September 2016 we derive its source strength and discuss potential sources and sinks, with a focus on the relevance of gas-phase pyruvic acid for radical chemistry.
Matthew Forrest, Holger Tost, Jos Lelieveld, and Thomas Hickler
Geosci. Model Dev., 13, 1285–1309, https://doi.org/10.5194/gmd-13-1285-2020, https://doi.org/10.5194/gmd-13-1285-2020, 2020
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We have integrated the LPJ-GUESS dynamic global vegetation model into the EMAC atmospheric chemistry-enabled GCM (general circulation model). This combined framework will enable the investigation of many land–atmosphere interactions and feedbacks with state-of-the-art simulation models. Initial results show that using the climate produced by EMAC together with LPJ-GUESS produces an acceptable representation of the global vegetation.
Matias Berasategui, Damien Amedro, Achim Edtbauer, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 2695–2707, https://doi.org/10.5194/acp-20-2695-2020, https://doi.org/10.5194/acp-20-2695-2020, 2020
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We have determined the rate coefficient and mechanism for the reaction of the OH radical with methane sulphonamide, a trace gas which has recently been found in the atmosphere. The rate coefficient is 1.4 × 10−13 cm3 molec.−1 s−1, which indicates a tropospheric lifetime of > 2 months. The observation of CO, CO2, SO2, HNO3, HCOOH, and N2O products enabled us to derive a detailed reaction mechanism for the reaction, which proceeds predominantly by H abstraction from the CH3 group.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
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In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
Pascal Polonik, Christoph Knote, Tobias Zinner, Florian Ewald, Tobias Kölling, Bernhard Mayer, Meinrat O. Andreae, Tina Jurkat-Witschas, Thomas Klimach, Christoph Mahnke, Sergej Molleker, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Ralf Weigel, and Manfred Wendisch
Atmos. Chem. Phys., 20, 1591–1605, https://doi.org/10.5194/acp-20-1591-2020, https://doi.org/10.5194/acp-20-1591-2020, 2020
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A realistic representation of cloud–aerosol interactions is central to accurate climate projections. Here we combine observations collected during the ACRIDICON-CHUVA campaign with chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysics. We find an upper limit for the model sensitivity on cloud condensation nuclei concentrations well below the levels reached during the burning season in the Amazon Basin.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Heiko Bozem, Peter Hoor, Daniel Kunkel, Franziska Köllner, Johannes Schneider, Andreas Herber, Hannes Schulz, W. Richard Leaitch, Amir A. Aliabadi, Megan D. Willis, Julia Burkart, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 19, 15049–15071, https://doi.org/10.5194/acp-19-15049-2019, https://doi.org/10.5194/acp-19-15049-2019, 2019
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We present airborne trace gas measurements in the European and Canadian Arctic for July 2014 and April 2015. Based on CO and CO2 in situ data as well as 10 d kinematic back trajectories, we characterize the prevailing transport regimes and derive a tracer-based diagnostic for the determination of the polar dome boundary. Using the tracer-derived boundary, an analysis of the recent transport history of air masses within the polar dome reveals significant differences between spring and summer.
André Ehrlich, Manfred Wendisch, Christof Lüpkes, Matthias Buschmann, Heiko Bozem, Dmitri Chechin, Hans-Christian Clemen, Régis Dupuy, Olliver Eppers, Jörg Hartmann, Andreas Herber, Evelyn Jäkel, Emma Järvinen, Olivier Jourdan, Udo Kästner, Leif-Leonard Kliesch, Franziska Köllner, Mario Mech, Stephan Mertes, Roland Neuber, Elena Ruiz-Donoso, Martin Schnaiter, Johannes Schneider, Johannes Stapf, and Marco Zanatta
Earth Syst. Sci. Data, 11, 1853–1881, https://doi.org/10.5194/essd-11-1853-2019, https://doi.org/10.5194/essd-11-1853-2019, 2019
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During the Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign, two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. The data set combines remote sensing and in situ measurement of cloud, aerosol, and trace gas properties, as well as turbulent and radiative fluxes, which will be used to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification.
Philipp G. Eger, Nils Friedrich, Jan Schuladen, Justin Shenolikar, Horst Fischer, Ivan Tadic, Hartwig Harder, Monica Martinez, Roland Rohloff, Sebastian Tauer, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Jean Sciare, Michael Pikridas, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, https://doi.org/10.5194/acp-19-12121-2019, 2019
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Shipborne measurements of nitryl chloride (ClNO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea and around the Arabian Peninsula with observed mixing ratios ranging from the limit of detection to 600 pptv. We examined the regional variability in the generation of ClNO2 and its importance for Cl atom generation in a marine boundary layer influenced by ships and industry.
Horst Fischer, Raoul Axinte, Heiko Bozem, John N. Crowley, Cheryl Ernest, Stefan Gilge, Sascha Hafermann, Hartwig Harder, Korbinian Hens, Ruud H. H. Janssen, Rainer Königstedt, Dagmar Kubistin, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Christian Plass-Dülmer, Andrea Pozzer, Eric Regelin, Andreas Reiffs, Torsten Schmidt, Jan Schuladen, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11953–11968, https://doi.org/10.5194/acp-19-11953-2019, https://doi.org/10.5194/acp-19-11953-2019, 2019
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We use in situ observations of H2O2 to study the interplay between photochemistry, transport and deposition processes. The data were obtained during five ground-based field campaigns across Europe. A budget calculation indicates that the photochemical production rate was much larger than photochemical loss and that dry deposition is the dominant loss process. To reproduce the change in H2O2 mixing ratios after sunrise, a variable contribution of entrainment from the residual layer is required.
Matthias Kippenberger, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 11939–11951, https://doi.org/10.5194/acp-19-11939-2019, https://doi.org/10.5194/acp-19-11939-2019, 2019
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We investigated the uptake of several trace gases to growing ice surfaces at temperatures relevant to cirrus clouds. HCl, a strong inorganic acid that ionises at the surface, was efficiently trapped in the growing ice, whereas oxidised organic trace gases, which attach to ice by hydrogen bonding, were not. HCl can be efficiently and rapidly removed from the gas phase in supersaturated ice clouds.
Jianzhong Ma, Christoph Brühl, Qianshan He, Benedikt Steil, Vlassis A. Karydis, Klaus Klingmüller, Holger Tost, Bin Chen, Yufang Jin, Ningwei Liu, Xiangde Xu, Peng Yan, Xiuji Zhou, Kamal Abdelrahman, Andrea Pozzer, and Jos Lelieveld
Atmos. Chem. Phys., 19, 11587–11612, https://doi.org/10.5194/acp-19-11587-2019, https://doi.org/10.5194/acp-19-11587-2019, 2019
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We find a pronounced maximum in aerosol extinction in the upper troposphere and lower stratosphere over the Tibetan Plateau during the Asian summer monsoon, caused mainly by mineral dust emitted from the northern Tibetan Plateau and slope area, lofted to and accumulating within the anticyclonic circulation. Mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction around the tropopause within the Asian summer monsoon anticyclone.
Eva Y. Pfannerstill, Nijing Wang, Achim Edtbauer, Efstratios Bourtsoukidis, John N. Crowley, Dirk Dienhart, Philipp G. Eger, Lisa Ernle, Horst Fischer, Bettina Hottmann, Jean-Daniel Paris, Christof Stönner, Ivan Tadic, David Walter, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 19, 11501–11523, https://doi.org/10.5194/acp-19-11501-2019, https://doi.org/10.5194/acp-19-11501-2019, 2019
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The Arabian Peninsula is a global hot spot of ozone pollution. Our measurements, made on a ship in summer 2017, indicate underlying reasons. Despite being at sea, we observed ozone-forming reactive trace gases (measured as so-called total OH reactivity) comparable to highly populated urban regions in amount and composition. This is due to strong emissions from oil extraction and ship traffic. These emissions were quickly converted to ozone due to intense solar irradiation and high temperatures.
Vanessa Brocchi, Gisèle Krysztofiak, Adrien Deroubaix, Greta Stratmann, Daniel Sauer, Hans Schlager, Konrad Deetz, Guillaume Dayma, Claude Robert, Stéphane Chevrier, and Valéry Catoire
Atmos. Chem. Phys., 19, 11401–11411, https://doi.org/10.5194/acp-19-11401-2019, https://doi.org/10.5194/acp-19-11401-2019, 2019
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This study reports the first flaring in situ measurements in southern West Africa. According to the measurements, oil rig flaring plumes in Ghana lead to increases in NO2 and aerosols but not always in CO and not in SO2. Flaring measurements can be reproduced using FLEXPART model, adjusting both the emission flux and the injection height. The DACCIWA satellite flaring inventory provides a reasonable estimate of flaring emission.
Andreas Marsing, Tina Jurkat-Witschas, Jens-Uwe Grooß, Stefan Kaufmann, Romy Heller, Andreas Engel, Peter Hoor, Jens Krause, and Christiane Voigt
Atmos. Chem. Phys., 19, 10757–10772, https://doi.org/10.5194/acp-19-10757-2019, https://doi.org/10.5194/acp-19-10757-2019, 2019
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We study the partitioning of inorganic chlorine into active (ozone-depleting) and reservoir species in the lowermost stratosphere of the Arctic polar vortex, using novel in situ aircraft measurements in winter 2015/2016. We observe a change in recovery pathways of the reservoirs HCl and ClONO2 with increasing potential temperature. A comparison with the CLaMS model relates the observations to the vortex-wide evolution and confirms unresolved discrepancies in the mid-winter HCl distribution.
Jonathan Liebmann, Nicolas Sobanski, Jan Schuladen, Einar Karu, Heidi Hellén, Hannele Hakola, Qiaozhi Zha, Mikael Ehn, Matthieu Riva, Liine Heikkinen, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 10391–10403, https://doi.org/10.5194/acp-19-10391-2019, https://doi.org/10.5194/acp-19-10391-2019, 2019
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The formation of alkyl nitrates in the boreal forest was dominated by reactions of the NO3 radical with terpenes, both during the day and the night, with fewer contributions from OH and ozone. The alkyl nitrates formed had lifetimes on the order of 2 h, reflecting efficient loss via uptake to aerosol and deposition.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Jonathan W. Taylor, Sophie L. Haslett, Keith Bower, Michael Flynn, Ian Crawford, James Dorsey, Tom Choularton, Paul J. Connolly, Valerian Hahn, Christiane Voigt, Daniel Sauer, Régis Dupuy, Joel Brito, Alfons Schwarzenboeck, Thierry Bourriane, Cyrielle Denjean, Phil Rosenberg, Cyrille Flamant, James D. Lee, Adam R. Vaughan, Peter G. Hill, Barbara Brooks, Valéry Catoire, Peter Knippertz, and Hugh Coe
Atmos. Chem. Phys., 19, 8503–8522, https://doi.org/10.5194/acp-19-8503-2019, https://doi.org/10.5194/acp-19-8503-2019, 2019
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Low-level clouds cover a wide area of southern West Africa (SWA) and play an important role in the region's climate, reflecting sunlight away from the surface. We performed aircraft measurements of aerosols and clouds over SWA during the 2016 summer monsoon and found pollution, and polluted clouds, across the whole region. Smoke from biomass burning in Central Africa is transported to West Africa, causing a polluted background which limits the effect of local pollution on cloud properties.
Klaus Klingmüller, Jos Lelieveld, Vlassis A. Karydis, and Georgiy L. Stenchikov
Atmos. Chem. Phys., 19, 7397–7408, https://doi.org/10.5194/acp-19-7397-2019, https://doi.org/10.5194/acp-19-7397-2019, 2019
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Within the atmosphere, desert dust and anthropogenic pollution are mixed and interact, which affects the abundance and optical properties of the particulate matter. This results in an anthropogenic climate forcing associated with mineral dust notwithstanding the natural origin of most aeolian dust. With a global chemistry–climate model, we estimate this forcing to represent a considerable fraction of the total dust forcing.
Efstratios Bourtsoukidis, Lisa Ernle, John N. Crowley, Jos Lelieveld, Jean-Daniel Paris, Andrea Pozzer, David Walter, and Jonathan Williams
Atmos. Chem. Phys., 19, 7209–7232, https://doi.org/10.5194/acp-19-7209-2019, https://doi.org/10.5194/acp-19-7209-2019, 2019
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We report on results that demonstrate the utility of non-methane hydrocarbons as source/sink identification tracers while providing their mixing ratios around the Arabian Peninsula. By introducing novel data-analysis approaches, we establish a new method for separating associated and non-associated (with liquids) gases. We formulate a relationship between hydrocarbon oxidative pairs that can be used to evaluate the relative abundance of the hydroxyl and chlorine radicals in the troposphere.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-251, https://doi.org/10.5194/acp-2019-251, 2019
Publication in ACP not foreseen
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Bioaerosols have been an important topic in atmospheric science in the last two decades. This paper compares different emission parametrizations used in fungal spores modeling and compare their results to two sets of new observational datasets. It emphasises their uncertainties in order to improve their modeling in the future. This comparison is addressed primarily to the scientific community (publishing in ACP) interested in this type of modeling and the related experimental work in this field.
Naruki Hiranuma, Kouji Adachi, David M. Bell, Franco Belosi, Hassan Beydoun, Bhaskar Bhaduri, Heinz Bingemer, Carsten Budke, Hans-Christian Clemen, Franz Conen, Kimberly M. Cory, Joachim Curtius, Paul J. DeMott, Oliver Eppers, Sarah Grawe, Susan Hartmann, Nadine Hoffmann, Kristina Höhler, Evelyn Jantsch, Alexei Kiselev, Thomas Koop, Gourihar Kulkarni, Amelie Mayer, Masataka Murakami, Benjamin J. Murray, Alessia Nicosia, Markus D. Petters, Matteo Piazza, Michael Polen, Naama Reicher, Yinon Rudich, Atsushi Saito, Gianni Santachiara, Thea Schiebel, Gregg P. Schill, Johannes Schneider, Lior Segev, Emiliano Stopelli, Ryan C. Sullivan, Kaitlyn Suski, Miklós Szakáll, Takuya Tajiri, Hans Taylor, Yutaka Tobo, Romy Ullrich, Daniel Weber, Heike Wex, Thomas F. Whale, Craig L. Whiteside, Katsuya Yamashita, Alla Zelenyuk, and Ottmar Möhler
Atmos. Chem. Phys., 19, 4823–4849, https://doi.org/10.5194/acp-19-4823-2019, https://doi.org/10.5194/acp-19-4823-2019, 2019
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A total of 20 ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of cellulose particles – natural polymers. Our data showed several types of cellulose are able to nucleate ice as efficiently as some mineral dust samples and cellulose has the potential to be an important atmospheric ice-nucleating particle. Continued investigation/collaboration is necessary to obtain further insight into consistency or diversity of ice nucleation measurements.
Philipp G. Eger, Frank Helleis, Gerhard Schuster, Gavin J. Phillips, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 12, 1935–1954, https://doi.org/10.5194/amt-12-1935-2019, https://doi.org/10.5194/amt-12-1935-2019, 2019
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We present a chemical ionization quadrupole mass spectrometer (CI-QMS) with a novel discharge ion source. In addition to the expected detection of PAN, peracetic acid and ClNO2, the instrument is also sensitive to SO2, HCl and acetic acid through ion chemistry unique for our ion source. We present ionization schemes along with illustrative datasets from field campaigns underlining the potential of the CI-QMS as an alternative to polonium, especially for application in the marine boundary layer.
Umar Javed, Dagmar Kubistin, Monica Martinez, Jan Pollmann, Markus Rudolf, Uwe Parchatka, Andreas Reiffs, Jim Thieser, Gerhard Schuster, Martin Horbanski, Denis Pöhler, John N. Crowley, Horst Fischer, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 12, 1461–1481, https://doi.org/10.5194/amt-12-1461-2019, https://doi.org/10.5194/amt-12-1461-2019, 2019
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Nitrogen dioxide (NO2) affects the concentration of key species like ozone, hydroxyl radical, and nitrate radical in the atmosphere. In situ, direct, and interference-free NO2 measurements are important for validating our understanding of NOx chemistry related to ozone formation and the radical loss process. This article describes the important features and performance of a newly developed NO2 instrument during a field intercomparison.
Jonathan P. D. Abbatt, W. Richard Leaitch, Amir A. Aliabadi, Allan K. Bertram, Jean-Pierre Blanchet, Aude Boivin-Rioux, Heiko Bozem, Julia Burkart, Rachel Y. W. Chang, Joannie Charette, Jai P. Chaubey, Robert J. Christensen, Ana Cirisan, Douglas B. Collins, Betty Croft, Joelle Dionne, Greg J. Evans, Christopher G. Fletcher, Martí Galí, Roya Ghahreman, Eric Girard, Wanmin Gong, Michel Gosselin, Margaux Gourdal, Sarah J. Hanna, Hakase Hayashida, Andreas B. Herber, Sareh Hesaraki, Peter Hoor, Lin Huang, Rachel Hussherr, Victoria E. Irish, Setigui A. Keita, John K. Kodros, Franziska Köllner, Felicia Kolonjari, Daniel Kunkel, Luis A. Ladino, Kathy Law, Maurice Levasseur, Quentin Libois, John Liggio, Martine Lizotte, Katrina M. Macdonald, Rashed Mahmood, Randall V. Martin, Ryan H. Mason, Lisa A. Miller, Alexander Moravek, Eric Mortenson, Emma L. Mungall, Jennifer G. Murphy, Maryam Namazi, Ann-Lise Norman, Norman T. O'Neill, Jeffrey R. Pierce, Lynn M. Russell, Johannes Schneider, Hannes Schulz, Sangeeta Sharma, Meng Si, Ralf M. Staebler, Nadja S. Steiner, Jennie L. Thomas, Knut von Salzen, Jeremy J. B. Wentzell, Megan D. Willis, Gregory R. Wentworth, Jun-Wei Xu, and Jacqueline D. Yakobi-Hancock
Atmos. Chem. Phys., 19, 2527–2560, https://doi.org/10.5194/acp-19-2527-2019, https://doi.org/10.5194/acp-19-2527-2019, 2019
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The Arctic is experiencing considerable environmental change with climate warming, illustrated by the dramatic decrease in sea-ice extent. It is important to understand both the natural and perturbed Arctic systems to gain a better understanding of how they will change in the future. This paper summarizes new insights into the relationships between Arctic aerosol particles and climate, as learned over the past five or so years by a large Canadian research consortium, NETCARE.
Laura Tomsche, Andrea Pozzer, Narendra Ojha, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 19, 1915–1939, https://doi.org/10.5194/acp-19-1915-2019, https://doi.org/10.5194/acp-19-1915-2019, 2019
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The Asian monsoon anticyclone (AMA) is an annual phenomenon in the northern hemispheric upper troposphere (UT) and lower stratosphere. We performed in situ measurements of carbon monoxide (CO) and methane (CH4) in the monsoon outflow region and in background air in the UT (Mediterranean, Arabian Peninsula, Arabian Sea) using airborne optical absorption spectroscopy during the Oxidation Mechanism Observations mission (summer 2015). The trace gases increased within the AMA, particularly CH4.
Yingying Yan, David Cabrera-Perez, Jintai Lin, Andrea Pozzer, Lu Hu, Dylan B. Millet, William C. Porter, and Jos Lelieveld
Geosci. Model Dev., 12, 111–130, https://doi.org/10.5194/gmd-12-111-2019, https://doi.org/10.5194/gmd-12-111-2019, 2019
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The GEOS-Chem model has been updated with the SAPRC-11 aromatics chemical mechanism to evaluate global and regional effects of aromatics on tropospheric oxidation capacity. Our results reveal relatively slight changes in ozone, hydroxyl radical, and nitrogen oxides on a global mean basis (1–4 %), although remarkable regional differences (5–20 %) exist near the source regions. Improved representation of aromatics is important to simulate the tropospheric oxidation.
Johannes Eckstein, Roland Ruhnke, Stephan Pfahl, Emanuel Christner, Christopher Diekmann, Christoph Dyroff, Daniel Reinert, Daniel Rieger, Matthias Schneider, Jennifer Schröter, Andreas Zahn, and Peter Braesicke
Geosci. Model Dev., 11, 5113–5133, https://doi.org/10.5194/gmd-11-5113-2018, https://doi.org/10.5194/gmd-11-5113-2018, 2018
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We present ICON-ART-Iso, an extension to the global circulation model ICON, which allows for the simulation of the stable isotopologues of water. The main advantage over other isotope-enabled models is its flexible design with respect to the number of tracers simulated. We compare the results of several simulations to measurements of different scale. ICON-ART-Iso is able to reasonably reproduce the measurements. It is a promising tool to aid in the investigation of the atmospheric water cycle.
Michael Weger, Bernd Heinold, Christa Engler, Ulrich Schumann, Axel Seifert, Romy Fößig, Christiane Voigt, Holger Baars, Ulrich Blahak, Stephan Borrmann, Corinna Hoose, Stefan Kaufmann, Martina Krämer, Patric Seifert, Fabian Senf, Johannes Schneider, and Ina Tegen
Atmos. Chem. Phys., 18, 17545–17572, https://doi.org/10.5194/acp-18-17545-2018, https://doi.org/10.5194/acp-18-17545-2018, 2018
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The impact of desert dust on cloud formation is investigated for a major Saharan dust event over Europe by interactive regional dust modeling. Dust particles are very efficient ice-nucleating particles promoting the formation of ice crystals in clouds. The simulations show that the observed extensive cirrus development was likely related to the above-average dust load. The interactive dust–cloud feedback in the model significantly improves the agreement with aircraft and satellite observations.
Sebastian Ehrhart, Eimear M. Dunne, Hanna E. Manninen, Tuomo Nieminen, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4987–5001, https://doi.org/10.5194/gmd-11-4987-2018, https://doi.org/10.5194/gmd-11-4987-2018, 2018
Stefan Kaufmann, Christiane Voigt, Romy Heller, Tina Jurkat-Witschas, Martina Krämer, Christian Rolf, Martin Zöger, Andreas Giez, Bernhard Buchholz, Volker Ebert, Troy Thornberry, and Ulrich Schumann
Atmos. Chem. Phys., 18, 16729–16745, https://doi.org/10.5194/acp-18-16729-2018, https://doi.org/10.5194/acp-18-16729-2018, 2018
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We present an intercomparison of the airborne water vapor measurements during the ML-CIRRUS mission. Although the agreement of the hygrometers significantly improved compared to studies from recent decades, systematic differences remain under specific meteorological conditions. We compare the measurements to model data, where we observe a model wet bias in the lower stratosphere close to the tropopause, likely caused by a blurred humidity gradient in the model tropopause.
Christiane Voigt, Andreas Dörnbrack, Martin Wirth, Silke M. Groß, Michael C. Pitts, Lamont R. Poole, Robert Baumann, Benedikt Ehard, Björn-Martin Sinnhuber, Wolfgang Woiwode, and Hermann Oelhaf
Atmos. Chem. Phys., 18, 15623–15641, https://doi.org/10.5194/acp-18-15623-2018, https://doi.org/10.5194/acp-18-15623-2018, 2018
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The 2015–2016 stratospheric winter was the coldest in the 36-year climatological data record. The extreme conditions promoted the formation of persistent Arctic polar stratospheric ice clouds. An extended ice PSC detected by airborne lidar in January 2016 shows a second mode with higher particle depolarization ratios. Back-trajectories from the high-depol ice matched to CALIOP PSC curtains provide evidence for ice nucleation on NAT. The novel data consolidate our understanding of PSC formation.
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
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Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Stine Eriksen Hammer, Stephan Mertes, Johannes Schneider, Martin Ebert, Konrad Kandler, and Stephan Weinbruch
Atmos. Chem. Phys., 18, 13987–14003, https://doi.org/10.5194/acp-18-13987-2018, https://doi.org/10.5194/acp-18-13987-2018, 2018
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It is important to study ice-nucleating particles in the environment to learn more about cloud formation. We studied the composition of ice particle residuals and total aerosol particles sampled in parallel during mixed-phase cloud events at Jungfraujoch and discovered that soot and complex secondary particles were not present. In contrast, silica, aluminosilicates, and other aluminosilicates were the most important ice particle residual groups at site temperatures between −11 and −18 °C.
Sarah Grawe, Stefanie Augustin-Bauditz, Hans-Christian Clemen, Martin Ebert, Stine Eriksen Hammer, Jasmin Lubitz, Naama Reicher, Yinon Rudich, Johannes Schneider, Robert Staacke, Frank Stratmann, André Welti, and Heike Wex
Atmos. Chem. Phys., 18, 13903–13923, https://doi.org/10.5194/acp-18-13903-2018, https://doi.org/10.5194/acp-18-13903-2018, 2018
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In this study, coal fly ash particles immersed in supercooled cloud droplets were analyzed concerning their freezing behavior. Additionally, physico-chemical particle properties (morphology, chemical composition, crystallography) were investigated. In combining both aspects, components that potentially contribute to the observed freezing behavior of the ash could be identified. Interactions at the particle-water interface, that depend on suspension time and influence freezing, are discussed.
John N. Crowley, Nicolas Pouvesle, Gavin J. Phillips, Raoul Axinte, Horst Fischer, Tuukka Petäjä, Anke Nölscher, Jonathan Williams, Korbinian Hens, Hartwig Harder, Monica Martinez-Harder, Anna Novelli, Dagmar Kubistin, Birger Bohn, and Jos Lelieveld
Atmos. Chem. Phys., 18, 13457–13479, https://doi.org/10.5194/acp-18-13457-2018, https://doi.org/10.5194/acp-18-13457-2018, 2018
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Simultaneous observations of PAA, PAN and H2O2 are used to provide insight into processes influencing the HOx chemistry of the boreal forest, including two biomass-burning-impacted periods. A significant contribution from photolytic HOx sources was included in a box model analysis to align model predictions with measurements. The model predicts high levels of organic peroxy radicals, also at night-time.
Franz Slemr, Andreas Weigelt, Ralf Ebinghaus, Johannes Bieser, Carl A. M. Brenninkmeijer, Armin Rauthe-Schöch, Markus Hermann, Bengt G. Martinsson, Peter van Velthoven, Harald Bönisch, Marco Neumaier, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 12329–12343, https://doi.org/10.5194/acp-18-12329-2018, https://doi.org/10.5194/acp-18-12329-2018, 2018
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Total and elemental mercury were measured in the upper troposphere and lower stratosphere onboard a passenger aircraft. Their concentrations in the upper troposphere were comparable implying low concentrations of oxidized mercury in this region. Large scale seasonally dependent influence of emissions from biomass burning was also observed. Their distributions in the lower stratosphere implies a long stratospheric lifetime, which precludes significant mercury oxidation by ozone.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Jonathan M. Liebmann, Jennifer B. A. Muller, Dagmar Kubistin, Anja Claude, Robert Holla, Christian Plass-Dülmer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 12045–12059, https://doi.org/10.5194/acp-18-12045-2018, https://doi.org/10.5194/acp-18-12045-2018, 2018
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We present direct measurements of the summertime total reactivity (inverse lifetime) of NO3 towards organic trace gases at a rural mountain site. High daytime and low night-time values were found. The reactivity was dominated by reaction with monoterpenes and sufficiently high to compete with photolysis and reaction with NO during daytime. NO3 radical measurements from one night are presented. For the first time, direct measurements of OH and NO3 reactivity are compared.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Zacharias Marinou Nikolaou, Jyh-Yuan Chen, Yiannis Proestos, Jos Lelieveld, and Rolf Sander
Geosci. Model Dev., 11, 3391–3407, https://doi.org/10.5194/gmd-11-3391-2018, https://doi.org/10.5194/gmd-11-3391-2018, 2018
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Chemistry is an important component of the atmosphere that describes many important physical processes. However, atmospheric chemical mechanisms include hundreds of species and reactions, posing a significant computational load. In this work, we use a powerful reduction method in order to develop a computationally faster chemical mechanism from a detailed mechanism. This enables accelerated simulations, which can be used to examine a wider range of processes in increased detail.
Sören Johansson, Wolfgang Woiwode, Michael Höpfner, Felix Friedl-Vallon, Anne Kleinert, Erik Kretschmer, Thomas Latzko, Johannes Orphal, Peter Preusse, Jörn Ungermann, Michelle L. Santee, Tina Jurkat-Witschas, Andreas Marsing, Christiane Voigt, Andreas Giez, Martina Krämer, Christian Rolf, Andreas Zahn, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Meas. Tech., 11, 4737–4756, https://doi.org/10.5194/amt-11-4737-2018, https://doi.org/10.5194/amt-11-4737-2018, 2018
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We present two-dimensional cross sections of temperature, HNO3, O3, ClONO2, H2O and CFC-12 from measurements of the GLORIA infrared limb imager during the POLSTRACC/GW-LCYCLE/SALSA aircraft campaigns in the Arctic winter 2015/2016. GLORIA sounded the atmosphere between 5 and 14 km with vertical resolutions of 0.4–1 km. Estimated errors are in the range of 1–2 K (temperature) and 10 %–20 % (trace gases). Comparisons to in situ instruments onboard the aircraft and to Aura/MLS are shown.
Chinmay Mallik, Laura Tomsche, Efstratios Bourtsoukidis, John N. Crowley, Bettina Derstroff, Horst Fischer, Sascha Hafermann, Imke Hüser, Umar Javed, Stephan Keßel, Jos Lelieveld, Monica Martinez, Hannah Meusel, Anna Novelli, Gavin J. Phillips, Andrea Pozzer, Andreas Reiffs, Rolf Sander, Domenico Taraborrelli, Carina Sauvage, Jan Schuladen, Hang Su, Jonathan Williams, and Hartwig Harder
Atmos. Chem. Phys., 18, 10825–10847, https://doi.org/10.5194/acp-18-10825-2018, https://doi.org/10.5194/acp-18-10825-2018, 2018
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OH and HO2 control the transformation of air pollutants and O3 formation. Their implication for air quality over the climatically sensitive Mediterranean region was studied during a field campaign in Cyprus. Production of OH, HO2, and recycled OH was lower in aged marine air masses. Box model simulations of OH and HO2 agreed with measurements except at high terpene concentrations when model RO2 due to terpenes caused large HO2 loss. Autoxidation schemes for RO2 improved the agreement.
Jorge Saturno, Florian Ditas, Marloes Penning de Vries, Bruna A. Holanda, Mira L. Pöhlker, Samara Carbone, David Walter, Nicole Bobrowski, Joel Brito, Xuguang Chi, Alexandra Gutmann, Isabella Hrabe de Angelis, Luiz A. T. Machado, Daniel Moran-Zuloaga, Julian Rüdiger, Johannes Schneider, Christiane Schulz, Qiaoqiao Wang, Manfred Wendisch, Paulo Artaxo, Thomas Wagner, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 18, 10391–10405, https://doi.org/10.5194/acp-18-10391-2018, https://doi.org/10.5194/acp-18-10391-2018, 2018
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This study uses satellite observations to track volcanic emissions in eastern Congo and their subsequent transport across the Atlantic Ocean into the Amazon Basin. Aircraft and ground-based observations are used to characterize the influence of volcanogenic aerosol on the chemical and microphysical properties of Amazonian aerosols. Further, this work is an illustrative example of the conditions and dynamics driving the transatlantic transport of African emissions to South America.
Aurélien Chauvigné, Olivier Jourdan, Alfons Schwarzenboeck, Christophe Gourbeyre, Jean François Gayet, Christiane Voigt, Hans Schlager, Stefan Kaufmann, Stephan Borrmann, Sergej Molleker, Andreas Minikin, Tina Jurkat, and Ulrich Schumann
Atmos. Chem. Phys., 18, 9803–9822, https://doi.org/10.5194/acp-18-9803-2018, https://doi.org/10.5194/acp-18-9803-2018, 2018
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This paper demonstrates a new form of statistical analysis of contrail to cirrus evolution. The authors show well-separated analyses of the different stages of the contrail's evolution, which allows us to study their optical, microphysical, and chemical properties. These results could be used to develop representative parameterizations of the scattering and geometrical properties of the ice crystals’ shapes and sizes, observed in the visible wavelength range.
Armin Afchine, Christian Rolf, Anja Costa, Nicole Spelten, Martin Riese, Bernhard Buchholz, Volker Ebert, Romy Heller, Stefan Kaufmann, Andreas Minikin, Christiane Voigt, Martin Zöger, Jessica Smith, Paul Lawson, Alexey Lykov, Sergey Khaykin, and Martina Krämer
Atmos. Meas. Tech., 11, 4015–4031, https://doi.org/10.5194/amt-11-4015-2018, https://doi.org/10.5194/amt-11-4015-2018, 2018
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The ice water content (IWC) of cirrus clouds is an essential parameter that determines their radiative properties and is thus important for climate simulations. Experimental investigations of IWCs measured on board research aircraft reveal that their accuracy is influenced by the sampling position. IWCs detected at the aircraft roof deviate significantly from wing, side or bottom IWCs. The reasons are deflections of the gas streamlines and ice particle trajectories behind the aircraft cockpit.
Aristeidis K. Georgoulias, Athanasios Tsikerdekis, Vassilis Amiridis, Eleni Marinou, Angela Benedetti, Prodromos Zanis, Georgia Alexandri, Lucia Mona, Konstantinos A. Kourtidis, and Jos Lelieveld
Atmos. Chem. Phys., 18, 8601–8620, https://doi.org/10.5194/acp-18-8601-2018, https://doi.org/10.5194/acp-18-8601-2018, 2018
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In this work, the MACC reanalysis dust product is evaluated over Europe, Northern Africa and the Middle East using the EARLINET-optimized CALIOP/CALIPSO pure dust satellite-based product LIVAS (2007–2012). As dust plays a determinant role in processes related to weather and climate, human healt, and the economy, it is obvious that adequately simulating the amount of dust and its optical properties is essential. Our results could be used as a reference in future climate model evaluations.
Stephan E. Bansmer, Arne Baumert, Stephan Sattler, Inken Knop, Delphine Leroy, Alfons Schwarzenboeck, Tina Jurkat-Witschas, Christiane Voigt, Hugo Pervier, and Biagio Esposito
Atmos. Meas. Tech., 11, 3221–3249, https://doi.org/10.5194/amt-11-3221-2018, https://doi.org/10.5194/amt-11-3221-2018, 2018
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Snow, frost formation and ice cubes in our drinks are part of our daily life. But what about our technical innovations like aviation, electrical power transmission and wind-energy production, can they cope with icing? Icing Wind Tunnels are an ideal laboratory environment to answer that question. In this paper, we show how the icing wind tunnel in Braunschweig (Germany) was built and how we can use it for engineering and climate research.
Meryem Tanarhte, Sara Bacer, Susannah M. Burrows, J. Alex Huffman, Kyle M. Pierce, Andrea Pozzer, Roland Sarda-Estève, Nicole J. Savage, and Jos Lelieveld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-361, https://doi.org/10.5194/acp-2018-361, 2018
Revised manuscript not accepted
Klaus-Dirk Gottschaldt, Hans Schlager, Robert Baumann, Duy Sinh Cai, Veronika Eyring, Phoebe Graf, Volker Grewe, Patrick Jöckel, Tina Jurkat-Witschas, Christiane Voigt, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 5655–5675, https://doi.org/10.5194/acp-18-5655-2018, https://doi.org/10.5194/acp-18-5655-2018, 2018
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This study places aircraft trace gas measurements from within the Asian summer monsoon anticyclone into the context of regional, intra- and interannual variability. We find that the processes reflected in the measurements are present throughout multiple simulated monsoon seasons. Dynamical instabilities, photochemical ozone production, lightning and entrainments from the lower troposphere and from the tropopause region determine the distinct composition of the anticyclone and its outflow.
Yingying Yan, Andrea Pozzer, Narendra Ojha, Jintai Lin, and Jos Lelieveld
Atmos. Chem. Phys., 18, 5589–5605, https://doi.org/10.5194/acp-18-5589-2018, https://doi.org/10.5194/acp-18-5589-2018, 2018
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Surface-based measurements from the EMEP network and EMAC model simulations are used to estimate the European surface ozone changes over 1995–2014. It shows a significantly decreasing trend in the 95th percentile ozone concentrations, while increasing in the 5th percentile ozone. Sensitivity simulations and statistical analysis show that a decrease in European anthropogenic emissions had contrasting effects on surface ozone trends between the 95th and 5th percentile levels.
Trismono C. Krisna, Manfred Wendisch, André Ehrlich, Evelyn Jäkel, Frank Werner, Ralf Weigel, Stephan Borrmann, Christoph Mahnke, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Luiz A. T. Machado
Atmos. Chem. Phys., 18, 4439–4462, https://doi.org/10.5194/acp-18-4439-2018, https://doi.org/10.5194/acp-18-4439-2018, 2018
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The optical thickness and particle effective radius of a cirrus above liquid water clouds and a DCC topped by an anvil cirrus are retrieved based on SMART and MODIS radiance measurements. For the cirrus, retrieved particle effective radius are validated with corresponding in situ data using a vertical weighting method. This approach allows to assess the measurements, retrieval algorithms, and derived cloud products.
Klaus Klingmüller, Swen Metzger, Mohamed Abdelkader, Vlassis A. Karydis, Georgiy L. Stenchikov, Andrea Pozzer, and Jos Lelieveld
Geosci. Model Dev., 11, 989–1008, https://doi.org/10.5194/gmd-11-989-2018, https://doi.org/10.5194/gmd-11-989-2018, 2018
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More than 1 billion tons of mineral dust particles are raised into the atmosphere every year, which has a significant impact on climate, society and ecosystems. The location, time and amount of dust emissions depend on surface and wind conditions. In the atmospheric chemistry–climate model EMAC, we have updated the relevant surface data and equations. Our validation shows that the updates substantially improve the agreement of model results and observations.
Jonathan Liebmann, Einar Karu, Nicolas Sobanski, Jan Schuladen, Mikael Ehn, Simon Schallhart, Lauriane Quéléver, Heidi Hellen, Hannele Hakola, Thorsten Hoffmann, Jonathan Williams, Horst Fischer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 18, 3799–3815, https://doi.org/10.5194/acp-18-3799-2018, https://doi.org/10.5194/acp-18-3799-2018, 2018
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Using a newly developed experimental setup, we have made the first direct measurements (during autumn 2016) of NO3 reactivity in the Finnish boreal forest. The NO3 reactivity was generally very high (maximum value of 0.94/s) so that daytime reaction with organics was a substantial fraction of the NO3 loss. Observations of biogenic hydrocarbons (BVOCs) suggested a dominant role for monoterpenes in determining the NO3 reactivity, which displayed a strong vertical gradient between 8.5 and 25 m.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
Atmos. Chem. Phys., 18, 921–961, https://doi.org/10.5194/acp-18-921-2018, https://doi.org/10.5194/acp-18-921-2018, 2018
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We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
Hannah Meusel, Alexandra Tamm, Uwe Kuhn, Dianming Wu, Anna Lena Leifke, Sabine Fiedler, Nina Ruckteschler, Petya Yordanova, Naama Lang-Yona, Mira Pöhlker, Jos Lelieveld, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Bettina Weber, and Yafang Cheng
Atmos. Chem. Phys., 18, 799–813, https://doi.org/10.5194/acp-18-799-2018, https://doi.org/10.5194/acp-18-799-2018, 2018
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The photolysis of nitrous acid (HONO) forms the OH radical. However, not all sources are known. Recent studies showed that HONO can be emitted from soil but they did not evaluate the importance to the HONO budget. In this work HONO emissions from 43 soil and biological soil crust samples from Cyprus were measured in a dynamic chamber and extrapolated to the real atmosphere. A large fraction of the local missing source (published earlier; Meusel et al., 2016) could be assigned to soil emissions.
Efstratios Bourtsoukidis, Frank Helleis, Laura Tomsche, Horst Fischer, Rolf Hofmann, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, https://doi.org/10.5194/amt-10-5089-2017, 2017
Romy Heller, Christiane Voigt, Stuart Beaton, Andreas Dörnbrack, Andreas Giez, Stefan Kaufmann, Christian Mallaun, Hans Schlager, Johannes Wagner, Kate Young, and Markus Rapp
Atmos. Chem. Phys., 17, 14853–14869, https://doi.org/10.5194/acp-17-14853-2017, https://doi.org/10.5194/acp-17-14853-2017, 2017
Amit Sharma, Narendra Ojha, Andrea Pozzer, Kathleen A. Mar, Gufran Beig, Jos Lelieveld, and Sachin S. Gunthe
Atmos. Chem. Phys., 17, 14393–14413, https://doi.org/10.5194/acp-17-14393-2017, https://doi.org/10.5194/acp-17-14393-2017, 2017
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We evaluate the numerical simulations of surface ozone during pre-monsoon season against a network of stations including clean, rural and polluted urban environments in the south Asian region. Significant effects of the employed emission inventory and chemical mechanism on the simulated ozone are found during the noon hours of intense photochemistry. The presented evaluation on the diurnal timescale would have implications for assessing ozone buildup and impacts on human health and crop yields.
Ramon Campos Braga, Daniel Rosenfeld, Ralf Weigel, Tina Jurkat, Meinrat O. Andreae, Manfred Wendisch, Ulrich Pöschl, Christiane Voigt, Christoph Mahnke, Stephan Borrmann, Rachel I. Albrecht, Sergej Molleker, Daniel A. Vila, Luiz A. T. Machado, and Lucas Grulich
Atmos. Chem. Phys., 17, 14433–14456, https://doi.org/10.5194/acp-17-14433-2017, https://doi.org/10.5194/acp-17-14433-2017, 2017
Franziska Köllner, Johannes Schneider, Megan D. Willis, Thomas Klimach, Frank Helleis, Heiko Bozem, Daniel Kunkel, Peter Hoor, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 17, 13747–13766, https://doi.org/10.5194/acp-17-13747-2017, https://doi.org/10.5194/acp-17-13747-2017, 2017
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We conducted aircraft-based single particle chemical composition measurements in the Canadian high Arctic during summer. Our results provide evidence for a marine-biogenic influence on secondary formation of particulate trimethylamine in the Arctic boundary layer. Understanding emission sources and further processes controlling aerosol number concentration and chemical composition in the pristine Arctic summer is crucial for modeling future climate in the area.
Tilman Hüneke, Oliver-Alex Aderhold, Jannik Bounin, Marcel Dorf, Eric Gentry, Katja Grossmann, Jens-Uwe Grooß, Peter Hoor, Patrick Jöckel, Mareike Kenntner, Marvin Knapp, Matthias Knecht, Dominique Lörks, Sabrina Ludmann, Sigrun Matthes, Rasmus Raecke, Marcel Reichert, Jannis Weimar, Bodo Werner, Andreas Zahn, Helmut Ziereis, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 4209–4234, https://doi.org/10.5194/amt-10-4209-2017, https://doi.org/10.5194/amt-10-4209-2017, 2017
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This paper describes a novel instrument for the aircraft-borne remote sensing of trace gases and liquid and solid water. Until recently, such measurements could only be evaluated under clear-sky conditions. We present a characterization and error assessment of the novel "scaling method", which allows for the retrieval of absolute trace gas concentrations under all sky conditions, significantly expanding the applicability of such measurements to study atmospheric photochemistry.
Andrea Pozzer, Alexandra P. Tsimpidi, Vlassis A. Karydis, Alexander de Meij, and Jos Lelieveld
Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, https://doi.org/10.5194/acp-17-12813-2017, 2017
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This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
David Cabrera-Perez, Domenico Taraborrelli, Jos Lelieveld, Thorsten Hoffmann, and Andrea Pozzer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-928, https://doi.org/10.5194/acp-2017-928, 2017
Revised manuscript not accepted
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Aromatic compounds are present in rural and urban atmospheres. The aim of this work is to disentangle the impacts of these compounds in different important atmospheric chemical species with the help of a numerical model. Aromatics have low impact OH, NOx and Ozone concentrations in the global scale (below 4 %). The impact however is larger in the regional scale (up to 10 %). The largest impact is in glyoxal and NO3 concentrations, with changes up to 10 % globally and 40 % regionally.
Heiko Bozem, Andrea Pozzer, Hartwig Harder, Monica Martinez, Jonathan Williams, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 11835–11848, https://doi.org/10.5194/acp-17-11835-2017, https://doi.org/10.5194/acp-17-11835-2017, 2017
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We present a case study of deep convection over Germany in July 2007 within the framework of the HOOVER II project. Airborne in situ measurements within the in- and outflow regions of an isolated thunderstorm provide a unique data set to study the influence of deep convection on the transport efficiency of soluble and insoluble trace gases. Despite their high solubility HCHO and H2O2 show enhanced concentrations in the outflow presumably due to degassing from cloud droplets during freezing.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Jean-Christophe Raut, Louis Marelle, Jerome D. Fast, Jennie L. Thomas, Bernadett Weinzierl, Katharine S. Law, Larry K. Berg, Anke Roiger, Richard C. Easter, Katharina Heimerl, Tatsuo Onishi, Julien Delanoë, and Hans Schlager
Atmos. Chem. Phys., 17, 10969–10995, https://doi.org/10.5194/acp-17-10969-2017, https://doi.org/10.5194/acp-17-10969-2017, 2017
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We study the cross-polar transport of plumes from Siberian fires to the Arctic in summer, both in terms of transport pathways and efficiency of deposition processes. Those plumes containing soot may originate from anthropogenic and biomass burning sources in mid-latitude regions and may impact the Arctic climate by depositing on snow and ice surfaces. We evaluate the role of the respective source contributions, investigate the transport of plumes and treat pathway-dependent removal of particles.
Bengt G. Martinsson, Johan Friberg, Oscar S. Sandvik, Markus Hermann, Peter F. J. van Velthoven, and Andreas Zahn
Atmos. Chem. Phys., 17, 10937–10953, https://doi.org/10.5194/acp-17-10937-2017, https://doi.org/10.5194/acp-17-10937-2017, 2017
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We find that the aerosol of the lowermost stratosphere has a considerable climate forcing. The upper tropospheric (UT) particulate sulfur is strongly influenced by stratospheric sources the first half of the year, whereas tropospheric sources dominate in fall; 50 % of the UT particulate sulfur (S) was found to be stratospheric at background condition, and 70 % under moderate influence from volcanism. The Asian monsoon is found to be an important tropospheric source of S in the NH extratropical UT.
Heiko Bozem, Tim M. Butler, Mark G. Lawrence, Hartwig Harder, Monica Martinez, Dagmar Kubistin, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, https://doi.org/10.5194/acp-17-10565-2017, 2017
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We present airborne measurements and model simulations in the tropics and mid-latitudes during GABRIEL and HOOVER, respectively. Based only on in situ data net ozone formation/destruction tendencies (NOPR) are calculated and compared to a 3-D chemistry transport model. The NOPR is positive in the continental boundary layer and the upper troposphere above 6 km. In the marine boundary layer and the middle troposphere ozone destruction prevails. Fresh convection shows strong net ozone formation.
Micael A. Cecchini, Luiz A. T. Machado, Meinrat O. Andreae, Scot T. Martin, Rachel I. Albrecht, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Daniel Fütterer, Tina Jurkat, Christoph Mahnke, Andreas Minikin, Sergej Molleker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Bernadett Weinzierl, and Manfred Wendisch
Atmos. Chem. Phys., 17, 10037–10050, https://doi.org/10.5194/acp-17-10037-2017, https://doi.org/10.5194/acp-17-10037-2017, 2017
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We study the effects of aerosol particles and updraft speed on the warm phase of Amazonian clouds. We expand the sensitivity analysis usually found in the literature by concomitantly considering cloud evolution and the effects on droplet size distribution (DSD) shape. The quantitative results show that particle concentration is the primary driver for the vertical profiles of effective diameter and droplet concentration in the warm phase of Amazonian convective clouds.
Bettina Derstroff, Imke Hüser, Efstratios Bourtsoukidis, John N. Crowley, Horst Fischer, Sergey Gromov, Hartwig Harder, Ruud H. H. Janssen, Jürgen Kesselmeier, Jos Lelieveld, Chinmay Mallik, Monica Martinez, Anna Novelli, Uwe Parchatka, Gavin J. Phillips, Rolf Sander, Carina Sauvage, Jan Schuladen, Christof Stönner, Laura Tomsche, and Jonathan Williams
Atmos. Chem. Phys., 17, 9547–9566, https://doi.org/10.5194/acp-17-9547-2017, https://doi.org/10.5194/acp-17-9547-2017, 2017
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The aim of the study was to examine aged air masses being transported from the European continent towards Cyprus. Longer-lived oxygenated volatile organic compounds (OVOCs) such as methanol were mainly impacted by long-distance transport and showed higher values in air masses from eastern Europe than in a flow regime from the west. The impact of the transport through the marine boundary layer as well as the influence of the residual layer/free troposphere on OVOCs were studied.
Evelyn Jäkel, Manfred Wendisch, Trismono C. Krisna, Florian Ewald, Tobias Kölling, Tina Jurkat, Christiane Voigt, Micael A. Cecchini, Luiz A. T. Machado, Armin Afchine, Anja Costa, Martina Krämer, Meinrat O. Andreae, Ulrich Pöschl, Daniel Rosenfeld, and Tianle Yuan
Atmos. Chem. Phys., 17, 9049–9066, https://doi.org/10.5194/acp-17-9049-2017, https://doi.org/10.5194/acp-17-9049-2017, 2017
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Vertical profiles of the cloud particle phase state in tropical deep convective clouds (DCCs) were investigated using airborne imaging spectrometer measurements during the ACRIDICON-CHUVA campaign, which was conducted over the Brazilian rainforest in September 2014. A phase discrimination retrieval was applied to observations of clouds formed in different aerosol conditions. The profiles were compared to in situ and satellite measurements.
Stephan Keßel, David Cabrera-Perez, Abraham Horowitz, Patrick R. Veres, Rolf Sander, Domenico Taraborrelli, Maria Tucceri, John N. Crowley, Andrea Pozzer, Christof Stönner, Luc Vereecken, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 17, 8789–8804, https://doi.org/10.5194/acp-17-8789-2017, https://doi.org/10.5194/acp-17-8789-2017, 2017
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In this study we identify an often overlooked stable oxide of carbon, namely carbon suboxide (C3O2), in ambient air. We have made C3O2 and in the laboratory determined its absorption cross section data and the rate of reaction with two important atmospheric oxidants, OH and O3. By incorporating known sources and sinks in a global model we have generated a first global picture of the distribution of this species in the atmosphere.
Anna Novelli, Korbinian Hens, Cheryl Tatum Ernest, Monica Martinez, Anke C. Nölscher, Vinayak Sinha, Pauli Paasonen, Tuukka Petäjä, Mikko Sipilä, Thomas Elste, Christian Plass-Dülmer, Gavin J. Phillips, Dagmar Kubistin, Jonathan Williams, Luc Vereecken, Jos Lelieveld, and Hartwig Harder
Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, https://doi.org/10.5194/acp-17-7807-2017, 2017
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The ambient concentration of stabilised Criegee intermediates (SCIs) was estimated for two
environments using field data. The low concentrations predicted indicate that SCIs are
unlikely to have a large impact on atmospheric chemistry. Concurrent measurements of an OH background signal using the Mainz IPI-LIF-FAGE instrument were found to be consistent with the chemistry of SCIs during the measurement campaigns.
Ramon Campos Braga, Daniel Rosenfeld, Ralf Weigel, Tina Jurkat, Meinrat O. Andreae, Manfred Wendisch, Mira L. Pöhlker, Thomas Klimach, Ulrich Pöschl, Christopher Pöhlker, Christiane Voigt, Christoph Mahnke, Stephan Borrmann, Rachel I. Albrecht, Sergej Molleker, Daniel A. Vila, Luiz A. T. Machado, and Paulo Artaxo
Atmos. Chem. Phys., 17, 7365–7386, https://doi.org/10.5194/acp-17-7365-2017, https://doi.org/10.5194/acp-17-7365-2017, 2017
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Johannes Bieser, Franz Slemr, Jesse Ambrose, Carl Brenninkmeijer, Steve Brooks, Ashu Dastoor, Francesco DeSimone, Ralf Ebinghaus, Christian N. Gencarelli, Beate Geyer, Lynne E. Gratz, Ian M. Hedgecock, Daniel Jaffe, Paul Kelley, Che-Jen Lin, Lyatt Jaegle, Volker Matthias, Andrei Ryjkov, Noelle E. Selin, Shaojie Song, Oleg Travnikov, Andreas Weigelt, Winston Luke, Xinrong Ren, Andreas Zahn, Xin Yang, Yun Zhu, and Nicola Pirrone
Atmos. Chem. Phys., 17, 6925–6955, https://doi.org/10.5194/acp-17-6925-2017, https://doi.org/10.5194/acp-17-6925-2017, 2017
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We conducted a multi model study to investigate our ability to reproduce the vertical distribution of mercury in the atmosphere. For this, we used observational data from over 40 aircraft flights in EU and US. We compared observations to the results of seven chemistry transport models and found that the models are able to reproduce vertical gradients of total and elemental Hg. Finally, we found that different chemical reactions seem responsible for the oxidation of Hg depending on altitude.
Narendra Ojha, Andrea Pozzer, Dimitris Akritidis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 6743–6757, https://doi.org/10.5194/acp-17-6743-2017, https://doi.org/10.5194/acp-17-6743-2017, 2017
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We investigate the processes, frequency of occurrence and seasonality, and effects of strongly enhanced ozone layers in the middle–upper troposphere (SOPs) over the Himalayas using a global model (EMAC). Rapid transport of stratospheric air masses is found as a key underlying process. Model predicts more frequent SOP events during the pre-monsoon. SOPs are found to significantly enhance the tropospheric ozone column over the Himalayas.
Klaus-D. Gottschaldt, Hans Schlager, Robert Baumann, Heiko Bozem, Veronika Eyring, Peter Hoor, Patrick Jöckel, Tina Jurkat, Christiane Voigt, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 17, 6091–6111, https://doi.org/10.5194/acp-17-6091-2017, https://doi.org/10.5194/acp-17-6091-2017, 2017
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We present upper-tropospheric trace gas measurements in the Asian summer monsoon anticyclone, obtained with the HALO research aircraft in September 2012. The anticyclone is one of the largest atmospheric features on Earth, but many aspects of it are not well understood. With the help of model simulations we find that entrainments from the tropopause region and the lower troposphere, combined with photochemistry and dynamical instabilities, can explain the observations.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Julia Burkart, Megan D. Willis, Heiko Bozem, Jennie L. Thomas, Kathy Law, Peter Hoor, Amir A. Aliabadi, Franziska Köllner, Johannes Schneider, Andreas Herber, Jonathan P. D. Abbatt, and W. Richard Leaitch
Atmos. Chem. Phys., 17, 5515–5535, https://doi.org/10.5194/acp-17-5515-2017, https://doi.org/10.5194/acp-17-5515-2017, 2017
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Our aircraft study for the first time systematically investigates aerosol size distributions, including ultrafine particles (5–20 nm in diameter), in the Arctic summertime atmosphere. We find that ultrafine particles occur very frequently in the boundary layer and not aloft, suggesting a surface source of these particles. Understanding aerosol properties and sources is crucial to predict climate and especially important in the Arctic as this region responds extremely fast to climate change.
Liang Feng, Paul I. Palmer, Hartmut Bösch, Robert J. Parker, Alex J. Webb, Caio S. C. Correia, Nicholas M. Deutscher, Lucas G. Domingues, Dietrich G. Feist, Luciana V. Gatti, Emanuel Gloor, Frank Hase, Rigel Kivi, Yi Liu, John B. Miller, Isamu Morino, Ralf Sussmann, Kimberly Strong, Osamu Uchino, Jing Wang, and Andreas Zahn
Atmos. Chem. Phys., 17, 4781–4797, https://doi.org/10.5194/acp-17-4781-2017, https://doi.org/10.5194/acp-17-4781-2017, 2017
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We use the GEOS-Chem global 3-D model of atmospheric chemistry and transport and an ensemble Kalman filter to simultaneously infer regional fluxes of methane (CH4) and carbon dioxide (CO2) directly from GOSAT retrievals of XCH4:XCO2, using sparse ground-based CH4 and CO2 mole fraction data to anchor the ratio. Our results show that assimilation of GOSAT data significantly reduced the posterior uncertainty and changed the a priori spatial distribution of CH4 emissions.
Jonathan M. Liebmann, Gerhard Schuster, Jan B. Schuladen, Nicolas Sobanski, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 10, 1241–1258, https://doi.org/10.5194/amt-10-1241-2017, https://doi.org/10.5194/amt-10-1241-2017, 2017
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We describe the first instrument for measurement of the rate constant for reactive loss (i.e. the total reactivity) of NO3 in ambient air. This is essentially a measureement of the lifetime of NO3 and will help assess the role of NO3 and N2O5 in conversion of reactive nitrogen oxides to reservoir species in the troposphere.
Nicolas Sobanski, Jim Thieser, Jan Schuladen, Carina Sauvage, Wei Song, Jonathan Williams, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 17, 4115–4130, https://doi.org/10.5194/acp-17-4115-2017, https://doi.org/10.5194/acp-17-4115-2017, 2017
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We investigated the formation of gas-phase organic nitrates at a forested semi-urban site. This work constitutes the first detailed analysis of the sum of organic nitrate mixing ratios measured by thermal dissociation cavity ring-down spectroscopy in continental Europe. Day (OH-initiated) and night-time (NO3-initiated) production of alkyl nitrates proceed at similar rates.
Mohamed Abdelkader, Swen Metzger, Benedikt Steil, Klaus Klingmüller, Holger Tost, Andrea Pozzer, Georgiy Stenchikov, Leonard Barrie, and Jos Lelieveld
Atmos. Chem. Phys., 17, 3799–3821, https://doi.org/10.5194/acp-17-3799-2017, https://doi.org/10.5194/acp-17-3799-2017, 2017
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We present a modeling study on the impacts of the key processes (dust emission flux, convection and dust aging parameterizations) that control the transatlantic dust transport using an advanced version of the EMAC atmospheric chemistry general circulation model. We define the
direct effect of dust agingas an increase in the AOD as a result of hygroscopic growth. We define the
indirect effectas a reduction in the dust AOD due to the higher removal of the aged dust particles.
Johannes Eckstein, Roland Ruhnke, Andreas Zahn, Marco Neumaier, Ole Kirner, and Peter Braesicke
Atmos. Chem. Phys., 17, 2775–2794, https://doi.org/10.5194/acp-17-2775-2017, https://doi.org/10.5194/acp-17-2775-2017, 2017
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Data on atmospheric trace gases have been collected with instruments on-board a commercial airliner for more than 10 years in the CARIBIC project. We investigate which species in the dataset can be used for a representative climatology, by comparing data from the chemistry–climate model EMAC along the flight paths to a larger set of model data. We find that long-lived species are captured quite well by the CARIBIC sample while this is not the case for more variable, shorter-lived species.
Ulrich Schumann, Christoph Kiemle, Hans Schlager, Ralf Weigel, Stephan Borrmann, Francesco D'Amato, Martina Krämer, Renaud Matthey, Alain Protat, Christiane Voigt, and C. Michael Volk
Atmos. Chem. Phys., 17, 2311–2346, https://doi.org/10.5194/acp-17-2311-2017, https://doi.org/10.5194/acp-17-2311-2017, 2017
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A long-lived (1 h) contrail and overshooting convection were observed in the tropics, near Darwin, Australia. The data are used to study the contrail life cycle at low temperatures and cirrus from deep overturning convection in the lower tropical stratosphere. Airborne in situ, lidar, profiler, radar, and satellite data, as well as a photo, are used to distinguish contrail cirrus from convective cirrus and to study the origin of the observed ice and aerosol, up to 2.3 km above the tropopause.
Garlich Fischbeck, Harald Bönisch, Marco Neumaier, Carl A. M. Brenninkmeijer, Johannes Orphal, Joel Brito, Julia Becker, Detlev Sprung, Peter F. J. van Velthoven, and Andreas Zahn
Atmos. Chem. Phys., 17, 1985–2008, https://doi.org/10.5194/acp-17-1985-2017, https://doi.org/10.5194/acp-17-1985-2017, 2017
Johannes Schneider, Stephan Mertes, Dominik van Pinxteren, Hartmut Herrmann, and Stephan Borrmann
Atmos. Chem. Phys., 17, 1571–1593, https://doi.org/10.5194/acp-17-1571-2017, https://doi.org/10.5194/acp-17-1571-2017, 2017
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We analyzed the composition of cloud droplet residuals and of aerosol particles sampled on a mountaintop site. The data show that about 85 % of the submicron aerosol mass partitions into the cloud phase, and that the uptake of soluble compounds (nitric acid, ammonia, and organic gases) from the gas phase into the cloud droplets is very effective. This will lead to a redistribution of these compounds among the aerosol particles and thereby to a more uniform aerosol after cloud evaporation.
Susan Schmidt, Johannes Schneider, Thomas Klimach, Stephan Mertes, Ludwig Paul Schenk, Piotr Kupiszewski, Joachim Curtius, and Stephan Borrmann
Atmos. Chem. Phys., 17, 575–594, https://doi.org/10.5194/acp-17-575-2017, https://doi.org/10.5194/acp-17-575-2017, 2017
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Ice formation in clouds is an important process in the formation of precipitation, especially at midlatitudes, but the exact properties of the aerosol particles that initiate freezing is not fully understood. We analysed residual particles from ice crystals sampled from mixed phase clouds. The results show that the residues contain a larger relative amount of soil dust and minerals, but also particles from industrial emissions and lead-containing particles, than the out-of-cloud aerosol.
Ulrich Schumann, Robert Baumann, Darrel Baumgardner, Sarah T. Bedka, David P. Duda, Volker Freudenthaler, Jean-Francois Gayet, Andrew J. Heymsfield, Patrick Minnis, Markus Quante, Ehrhard Raschke, Hans Schlager, Margarita Vázquez-Navarro, Christiane Voigt, and Zhien Wang
Atmos. Chem. Phys., 17, 403–438, https://doi.org/10.5194/acp-17-403-2017, https://doi.org/10.5194/acp-17-403-2017, 2017
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The initially linear clouds often seen behind aircraft are known as contrails. Contrails are prototype cirrus clouds forming under well-known conditions, but with less certain life cycle and climate effects. This paper collects contrail data from a large set of measurements and compares them among each other and with models. The observations show consistent contrail properties over a wide range of aircraft and atmosphere conditions. The dataset is available for further research.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Andrea Pozzer, Yogesh K. Tiwari, K. Ravi Kumar, and Jos Lelieveld
Atmos. Chem. Phys., 17, 257–275, https://doi.org/10.5194/acp-17-257-2017, https://doi.org/10.5194/acp-17-257-2017, 2017
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This study presents first ship-borne measurements of trace gases over the Bay of Bengal during summer monsoon. The observed variations in trace gases are shown to be due to dynamics/transport and en route photochemistry. Analysis of meteorological and chemical fields shows that significantly lower ozone during rainfall is associated with the downdrafts. A regional model reproduces the observed variations and revealed the rapid transport of ozone across the Bay of Bengal during an event.
Christiane Voigt, Andreas Dörnbrack, Martin Wirth, Silke M. Groß, Robert Baumann, Benedikt Ehard, Michael C. Pitts, Lamont R. Poole, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-1082, https://doi.org/10.5194/acp-2016-1082, 2016
Revised manuscript not accepted
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The letter describes unprecedented observations of widespread and persistent polar stratospheric ice clouds (ice PSCs) in the exceptionally cold Arctic stratospheric winter 2015/16. The unique observations are of global relevance because trends in Arctic ozone loss and in polar temperatures are highly uncertain. The new observations at cold conditions serve to enhance our knowledge on ice PSC formation, Arctic ozone loss and polar stratrospheric temperatures in a changing climate.
Bärbel Vogel, Gebhard Günther, Rolf Müller, Jens-Uwe Grooß, Armin Afchine, Heiko Bozem, Peter Hoor, Martina Krämer, Stefan Müller, Martin Riese, Christian Rolf, Nicole Spelten, Gabriele P. Stiller, Jörn Ungermann, and Andreas Zahn
Atmos. Chem. Phys., 16, 15301–15325, https://doi.org/10.5194/acp-16-15301-2016, https://doi.org/10.5194/acp-16-15301-2016, 2016
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The identification of transport pathways from the Asian monsoon anticyclone into the lower stratosphere is unclear. Global simulations with the CLaMS model demonstrate that source regions in Asia and in the Pacific Ocean have a significant impact on the chemical composition of the lower stratosphere of the Northern Hemisphere by flooding the extratropical lower stratosphere with young moist air masses. Two main horizontal transport pathways from the Asian monsoon anticyclone are identified.
Hannah Meusel, Uwe Kuhn, Andreas Reiffs, Chinmay Mallik, Hartwig Harder, Monica Martinez, Jan Schuladen, Birger Bohn, Uwe Parchatka, John N. Crowley, Horst Fischer, Laura Tomsche, Anna Novelli, Thorsten Hoffmann, Ruud H. H. Janssen, Oscar Hartogensis, Michael Pikridas, Mihalis Vrekoussis, Efstratios Bourtsoukidis, Bettina Weber, Jos Lelieveld, Jonathan Williams, Ulrich Pöschl, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 16, 14475–14493, https://doi.org/10.5194/acp-16-14475-2016, https://doi.org/10.5194/acp-16-14475-2016, 2016
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There are many studies which show discrepancies between modeled and measured nitrous acid (HONO, precursor of OH radical) in the troposphere but with no satisfactory explanation. Ideal conditions to study the unknown sources of HONO were found on Cyprus, a remote Mediterranean island. Budget analysis of trace gas measurements indicates a common source of NO and HONO, which is not related to anthropogenic activity and is most likely derived from biologic activity in soils and subsequent emission.
Dimitris Akritidis, Andrea Pozzer, Prodromos Zanis, Evangelos Tyrlis, Bojan Škerlak, Michael Sprenger, and Jos Lelieveld
Atmos. Chem. Phys., 16, 14025–14039, https://doi.org/10.5194/acp-16-14025-2016, https://doi.org/10.5194/acp-16-14025-2016, 2016
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We investigate the contribution of tropopause folds in the summertime tropospheric ozone pool over the eastern Mediterranean and the Middle East. For this purpose we use the EMAC atmospheric chemistry–climate model and a fold identification algorithm. A clear increase of ozone is found in the middle troposphere due to fold activity. The interannual variability of near-surface ozone over the eastern Mediterranean is related to that of both tropopause folds and ozone in the free troposphere.
Aristeidis K. Georgoulias, Georgia Alexandri, Konstantinos A. Kourtidis, Jos Lelieveld, Prodromos Zanis, Ulrich Pöschl, Robert Levy, Vassilis Amiridis, Eleni Marinou, and Athanasios Tsikerdekis
Atmos. Chem. Phys., 16, 13853–13884, https://doi.org/10.5194/acp-16-13853-2016, https://doi.org/10.5194/acp-16-13853-2016, 2016
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In this work, single pixel observations from MODIS Terra and Aqua are analyzed together with data from other satellite sensors, reanalysis projects and a chemistry–aerosol-transport model to study the spatiotemporal variability of different aerosol types. The results are in accordance with previous works and are a good reference for future studies in the area focusing on aerosols, clouds, radiation and the effects of particle pollution on human health.
Florian Obersteiner, Harald Bönisch, Timo Keber, Simon O'Doherty, and Andreas Engel
Atmos. Meas. Tech., 9, 5265–5279, https://doi.org/10.5194/amt-9-5265-2016, https://doi.org/10.5194/amt-9-5265-2016, 2016
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The analysis of trace gases in ambient air requires a preconcentration technique, in many cases to make the species of interest detectable and quantifiable. In this paper, such a preconcentration set-up is presented. Target species are trapped on adsorptive material cooled by a Stirling cooler which allows for a very low adsorption temperature but only requires electrical power. A simple and lightweight mechanical design guarantees very good suitability for remote-site field operation.
Gerard Ancellet, Nikos Daskalakis, Jean Christophe Raut, David Tarasick, Jonathan Hair, Boris Quennehen, François Ravetta, Hans Schlager, Andrew J. Weinheimer, Anne M. Thompson, Bryan Johnson, Jennie L. Thomas, and Katharine S. Law
Atmos. Chem. Phys., 16, 13341–13358, https://doi.org/10.5194/acp-16-13341-2016, https://doi.org/10.5194/acp-16-13341-2016, 2016
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An integrated analysis of all the ozone observations (lidar, sondes, and airborne in situ measurements) conducted during the 2008 IPY campaigns is performed and the processes that determine summer ozone concentrations over Greenland and Canada are discussed. Combined with a regional model simulation (WRFChem), the analysis of ozone, CO, and PV latitudinal and vertical variability allows the determination of the influence of stratospheric sources and biomass burning and anthropogenic emissions.
Gavin J. Phillips, Jim Thieser, Mingjin Tang, Nicolas Sobanski, Gerhard Schuster, Johannes Fachinger, Frank Drewnick, Stephan Borrmann, Heinz Bingemer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 16, 13231–13249, https://doi.org/10.5194/acp-16-13231-2016, https://doi.org/10.5194/acp-16-13231-2016, 2016
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We use trace gas measurements (N2O5, ClNO2, NO3) and particle properties (surface area, nitrate content etc.) to derive uptake coefficients (the probability of removal from the gas-phase on a per-collision basis) for the interaction of N2O5 with ambient aerosol and also the efficiency of formation of ClNO2. The uptake coefficients show high variability but are reasonably well captured by parameterisations based on laboratory measurements.
Ralf Weigel, Peter Spichtinger, Christoph Mahnke, Marcus Klingebiel, Armin Afchine, Andreas Petzold, Martina Krämer, Anja Costa, Sergej Molleker, Philipp Reutter, Miklós Szakáll, Max Port, Lucas Grulich, Tina Jurkat, Andreas Minikin, and Stephan Borrmann
Atmos. Meas. Tech., 9, 5135–5162, https://doi.org/10.5194/amt-9-5135-2016, https://doi.org/10.5194/amt-9-5135-2016, 2016
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The subject of our study concerns measurements with optical array probes (OAPs) on fast-flying aircraft such as the G550 (HALO or HIAPER). At up to Mach 0.7 the effect of air compression upstream of underwing-mounted instruments and particles' inertia need consideration for determining ambient particle concentrations. Compared to conventional practices the introduced correction procedure eliminates ambiguities and exhibits consistency over flight speeds between 50 and 250 m s−.
Nicolas Sobanski, Jan Schuladen, Gerhard Schuster, Jos Lelieveld, and John N. Crowley
Atmos. Meas. Tech., 9, 5103–5118, https://doi.org/10.5194/amt-9-5103-2016, https://doi.org/10.5194/amt-9-5103-2016, 2016
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We report the characteristics and performances of a cavity ring-down spectrometer (CRDS) designed for field measurements that uses light absorption at 662 and 405 nm to detect different reactive nitrogen species or group of species in the gas phase, either directly or after thermal decomposition. We report improvements compared to currently existing instruments, and describe the corrections applied to the raw data to account for chemical and optical interferences.
Jos Lelieveld, Sergey Gromov, Andrea Pozzer, and Domenico Taraborrelli
Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, https://doi.org/10.5194/acp-16-12477-2016, 2016
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The self-cleaning capacity of the atmosphere is controlled by hydroxyl (OH) radicals in the troposphere. There are primary and secondary OH sources, the former through the photodissociation of ozone, the latter through OH recycling. We used a global model, showing that secondary sources are larger than assumed previously, which buffers OH. Complementary OH formation mechanisms in pristine and polluted environments, connected through transport of ozone, can maintain stable global OH levels.
Valery Shcherbakov, Olivier Jourdan, Christiane Voigt, Jean-Francois Gayet, Aurélien Chauvigne, Alfons Schwarzenboeck, Andreas Minikin, Marcus Klingebiel, Ralf Weigel, Stephan Borrmann, Tina Jurkat, Stefan Kaufmann, Romy Schlage, Christophe Gourbeyre, Guy Febvre, Tatyana Lapyonok, Wiebke Frey, Sergej Molleker, and Bernadett Weinzierl
Atmos. Chem. Phys., 16, 11883–11897, https://doi.org/10.5194/acp-16-11883-2016, https://doi.org/10.5194/acp-16-11883-2016, 2016
W. Richard Leaitch, Alexei Korolev, Amir A. Aliabadi, Julia Burkart, Megan D. Willis, Jonathan P. D. Abbatt, Heiko Bozem, Peter Hoor, Franziska Köllner, Johannes Schneider, Andreas Herber, Christian Konrad, and Ralf Brauner
Atmos. Chem. Phys., 16, 11107–11124, https://doi.org/10.5194/acp-16-11107-2016, https://doi.org/10.5194/acp-16-11107-2016, 2016
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Thought to be mostly unimportant for summertime Arctic liquid-water clouds, airborne observations show that atmospheric aerosol particles 50 nm in diameter or smaller and most likely from natural sources are often involved in cloud formation in the pristine Arctic summer. The result expands the reference for aerosol forcing of climate. Further, for extremely low droplet concentrations, no evidence is found for a connection between cloud liquid water and aerosol particle concentrations.
Stefan Müller, Peter Hoor, Heiko Bozem, Ellen Gute, Bärbel Vogel, Andreas Zahn, Harald Bönisch, Timo Keber, Martina Krämer, Christian Rolf, Martin Riese, Hans Schlager, and Andreas Engel
Atmos. Chem. Phys., 16, 10573–10589, https://doi.org/10.5194/acp-16-10573-2016, https://doi.org/10.5194/acp-16-10573-2016, 2016
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In situ airborne measurements performed during TACTS/ESMVal 2012 were analysed to investigate the chemical compostion of the upper troposphere and lower stratosphere. N2O, CO and O3 data show an increase in tropospherically affected air masses within the extratropical stratosphere from August to September 2012, which originate from the Asian monsoon region. Thus, the Asian monsoon anticyclone significantly affected the chemical composition of the extratropical stratosphere during summer 2012.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Amir A. Aliabadi, Jennie L. Thomas, Andreas B. Herber, Ralf M. Staebler, W. Richard Leaitch, Hannes Schulz, Kathy S. Law, Louis Marelle, Julia Burkart, Megan D. Willis, Heiko Bozem, Peter M. Hoor, Franziska Köllner, Johannes Schneider, Maurice Levasseur, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 7899–7916, https://doi.org/10.5194/acp-16-7899-2016, https://doi.org/10.5194/acp-16-7899-2016, 2016
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For the first time, ship emissions of an ice-breaker, the Amundsen, is characterized while breaking ice in the Canadian Arctic using the plume intercepts by the Polar 6 aircraft. The study is novel, estimating lower plume expansion rates over the stable Arctic marine boundary layer and different emissions factors for oxides of nitrogen, black carbon, and carbon monoxide, compared to plume intercept studies in mid latitudes. These results can inform policy making and emission inventory datasets.
Megan D. Willis, Julia Burkart, Jennie L. Thomas, Franziska Köllner, Johannes Schneider, Heiko Bozem, Peter M. Hoor, Amir A. Aliabadi, Hannes Schulz, Andreas B. Herber, W. Richard Leaitch, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 7663–7679, https://doi.org/10.5194/acp-16-7663-2016, https://doi.org/10.5194/acp-16-7663-2016, 2016
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We present a case study focused on an aerosol growth event observed in the Canadian High Arctic during summer. Using measurements of aerosol chemical and physical properties we find evidence for aerosol growth into cloud condensation nuclei-active sizes, through marine-influenced secondary organic aerosol formation. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties, and therefore radiative balance and climate.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Franz Slemr, Andreas Weigelt, Ralf Ebinghaus, Hans H. Kock, Jan Bödewadt, Carl A. M. Brenninkmeijer, Armin Rauthe-Schöch, Stefan Weber, Markus Hermann, Julia Becker, Andreas Zahn, and Bengt Martinsson
Atmos. Meas. Tech., 9, 2291–2302, https://doi.org/10.5194/amt-9-2291-2016, https://doi.org/10.5194/amt-9-2291-2016, 2016
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The goal of CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrumented Container) is to carry out regular and detailed observations of atmospheric chemistry at 9–12 km altitude. Mercury has been measured since May 2005 during intercontinental flights between Europe and South and North America, Africa, and Asia. Here we describe the instrument modifications, the post-flight processing of the raw instrument signal, and the fractionation experiments.
Markus Hermann, Andreas Weigelt, Denise Assmann, Sascha Pfeifer, Thomas Müller, Thomas Conrath, Jens Voigtländer, Jost Heintzenberg, Alfred Wiedensohler, Bengt G. Martinsson, Terry Deshler, Carl A. M. Brenninkmeijer, and Andreas Zahn
Atmos. Meas. Tech., 9, 2179–2194, https://doi.org/10.5194/amt-9-2179-2016, https://doi.org/10.5194/amt-9-2179-2016, 2016
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Aerosol particles are an important component of the Earth's atmosphere. Here we describe the composition and characterization of a new optical particle size spectrometer (OPSS) for aircraft-borne measurements of the aerosol particle size distribution (how many particles there are with a certain size) in the 140–1050 nm size range. The OPSS was characterized throughout concerning its measurement capabilities (response, pressure dependence, coincidence) and validated versus balloon measurement.