Articles | Volume 21, issue 20
https://doi.org/10.5194/acp-21-15375-2021
© Author(s) 2021. 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-21-15375-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
15 Oct 2021
Research article |
| 15 Oct 2021
| 15 Oct 2021
Organic and inorganic bromine measurements around the extratropical tropopause and lowermost stratosphere: insights into the transport pathways and total bromine
Meike K. Rotermund
CORRESPONDING AUTHOR
Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
Vera Bense
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Martyn P. Chipperfield
School of Earth and Environment, University of Leeds, Leeds, UK
National Centre for Earth Observation, University of Leeds, Leeds, UK
Andreas Engel
Institute for Atmospheric and Environmental Science, Goethe University Frankfurt, Frankfurt, Germany
Jens-Uwe Grooß
Institute of Energy and Climate Research – Stratosphere (IEK-7), Forschungszentrum Jülich, Jülich, Germany
Peter Hoor
Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
Tilman Hüneke
Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
now at: Encavis AG, Hamburg, Germany
Timo Keber
Institute for Atmospheric and Environmental Science, Goethe University Frankfurt, Frankfurt, Germany
Flora Kluge
Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
Benjamin Schreiner
Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
Tanja Schuck
Institute for Atmospheric and Environmental Science, Goethe University Frankfurt, Frankfurt, Germany
Bärbel Vogel
Institute of Energy and Climate Research – Stratosphere (IEK-7), Forschungszentrum Jülich, Jülich, Germany
Andreas Zahn
Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology (KIT), Karlsruhe, Germany
Klaus Pfeilsticker
Institute of Environmental Physics, University of Heidelberg, Heidelberg, Germany
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EGUsphere, https://doi.org/10.5194/egusphere-2025-5142, https://doi.org/10.5194/egusphere-2025-5142, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We present an extratropical cyclone case study over the North Atlantic, focusing on the role of atmospheric gravity waves (GWs) in the generation of enhanced vertical wind shear and (clear-air) turbulence, as well as their impact on tracers distribution in the lowermost stratosphere. Our research suggests the GW related processes should be considered as a key for UTLS transport and mixing and as an important candidate for the interpretation of CAT, that appear to emanate from GW-induced shear.
Benjamin Püschel, Martin Vojta, Luise Kandler, Molly Crotwell, Andreas Engel, Paul B. Krummel, Chris R. Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Thomas Wagenhäuser, Ray F. Weiss, Dickon Young, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2025-5656, https://doi.org/10.5194/egusphere-2025-5656, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We present global and regionally resolved emissions of the two highly potent greenhouse gases CF4 and C2F6 from 2006 to 2023, based on atmospheric measurements and transport modeling. In nearly all regions studied, our results show that national reports and industry-based data underestimate emissions. While emissions in Europe and the U.S. declined, we find rising emissions in South, Southeast, and East Asia. China and India are the major contributors to global emissions in recent years.
Rolf Müller, Bärbel Vogel, Martina Krämer, Christian Rolf, Nicole Spelten, and Fabrizio Ravegnani
EGUsphere, https://doi.org/10.5194/egusphere-2025-5761, https://doi.org/10.5194/egusphere-2025-5761, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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In the Asian summer monsoon anticyclone the lapse rate tropopause, and not the cold point, constitutes a good estimate of the upper boundary of the well mixed tropospheric air mass. For strong convection there is substantial dehydration at the cold point tropopause (in summer 2017). Above the cold point tropopause, under such conditions, neither ice particle occurrence, nor enhanced molar mixing ratios of water vapour (above ≲ 6 ppm) are observed.
Linda Smoydzin, Vera Bense, Heiko Bozem, Philipp Joppe, Daniel Kunkel, Hans-Christoph Lachnitt, Holger Tost, Andreas Zahn, Helmut Ziereis, Martin Riese, and Peter Hoor
EGUsphere, https://doi.org/10.5194/egusphere-2025-5372, https://doi.org/10.5194/egusphere-2025-5372, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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During a research flight in early October elevated upper tropospheric mixing ratios of CO, NO, NOy and O3 were observed over a distance of more than 1000 km east of the Brasilian coast. Ozone mixing ratios are 20–40 ppbv higher than during a flight in early September. By combining aircraft observations with model simulations we find that ozone production from biomass burning over Amazonia caused predominantly the ozone enhancements which have a local effect on the radiative forcing of 50 mWm−2.
Paul Konopka, Felix Ploeger, Francesco D'Amato, Teresa Campos, Marc von Hobe, Shawn B. Honomichl, Peter Hoor, Laura L. Pan, Michelle L. Santee, Silvia Viciani, Kaley A. Walker, and Michaela I. Hegglin
Atmos. Chem. Phys., 25, 17973–17996, https://doi.org/10.5194/acp-25-17973-2025, https://doi.org/10.5194/acp-25-17973-2025, 2025
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We present an improved version of the Chemical Lagrangian Model of the Stratosphere (CLaMS-3.0), which better represents transport from the lower atmosphere to the upper troposphere and lower stratosphere. By refining grid resolution and improving convection representation, the model more accurately simulates carbon monoxide transport. Comparisons with satellite and in situ observations highlight its ability to capture seasonal variations and improve our understanding of atmospheric transport.
Patrick Konjari, Christian Rolf, Martina Krämer, Armin Afchine, Nicole Spelten, Irene Bartolome Garcia, Annette Miltenberger, Nicolas Emig, Philipp Joppe, Johannes Schneider, Yun Li, Andreas Petzold, Heiko Bozem, and Peter Hoor
Atmos. Chem. Phys., 25, 18031–18050, https://doi.org/10.5194/acp-25-18031-2025, https://doi.org/10.5194/acp-25-18031-2025, 2025
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We investigated how a powerful storm over southern Sweden in June 2024 transported ice particles and moist air into the normally dry stratosphere. We observed unusually high water vapor and ice levels up to 1.5 kilometers above the tropopause. Although the extra water vapor lasted only a few days to weeks, it shows how such storms can temporarily alter the upper atmosphere’s composition.
Luke M. Western, Stephen Bourguet, Molly Crotwell, Lei Hu, Paul B. Krummel, Hélène De Longueville, Alistair J. Manning, Jens Mühle, Dominique Rust, Isaac Vimont, Martin K. Vollmer, Minde An, Jgor Arduini, Andreas Engel, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Chris Lunder, Michela Maione, Stephen A. Montzka, David Nance, Simon O'Doherty, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Roland Schmidt, Kieran M. Stanley, Thomas Wagenhäuser, Dickon Young, Matt Rigby, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 25, 17761–17778, https://doi.org/10.5194/acp-25-17761-2025, https://doi.org/10.5194/acp-25-17761-2025, 2025
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We used atmospheric measurements to estimate emissions of two hydrochlorofluorocarbon (HCFC) gases, called HCFC-123 and HCFC-124, that harm the ozone layer. Despite international regulation to stop their production, their emissions have not fallen. This may be linked to how they are used to make other chemicals. Our findings show that some banned substances are still reaching the atmosphere, likely through leaks during chemical production, which could slow the recovery of the ozone layer.
Bärbel Vogel, Valentin Lauther, Franziska Köllner, Fatih Ekinci, Christian Rolf, Johannes Strobel, Ronja van Luijt, Michael C. Volk, Stephan Borrmann, Antonis Dragoneas, Oliver Eppers, Sergej Molleker, Peter Hoor, Linda Ort, Franziska Weyland, Andreas Zahn, Jan Clemens, Gebhard Günther, Oleh Kachula, Rolf Müller, Felix Ploeger, and Martin Riese
EGUsphere, https://doi.org/10.5194/egusphere-2025-5609, https://doi.org/10.5194/egusphere-2025-5609, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This work highlights the impact of the Asian summer monsoon on the chemical composition of the upper troposphere and lower stratosphere. Measurements of trace gases and aerosol particles uplifted by the Asian summer monsoon to higher altitudes are sparse. Here, we had the opportunity to use a whole suite of different measured trace gases and the chemical composition of aerosols, in combination with simulations, to better understand the complex transport and mixing processes in this region.
Matthew J. Rowlinson, Lucy J. Carpenter, Mat J. Evans, James D. Lee, Simone T. Andersen, Tomas Sherwen, Anna B. Callaghan, Roberto Sommariva, William Bloss, Siqi Hou, Leigh R. Crilley, Klaus Pfeilsticker, Benjamin Weyland, Thomas B. Ryerson, Patrick R. Veres, Pedro Campuzano-Jost, Hongyu Guo, Benjamin A. Nault, Jose L. Jimenez, and Khanneh Wadinga Fomba
Atmos. Chem. Phys., 25, 16945–16968, https://doi.org/10.5194/acp-25-16945-2025, https://doi.org/10.5194/acp-25-16945-2025, 2025
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HONO is key to tropospheric chemistry. Observations show high HONO concentrations in remote air, possibly explained by nitrate aerosol photolysis. We use observations to parameterize nitrate photolysis, evaluating simulated HONO against observations from multiple sources. We show improved agreement with observed HONO, but overestimates in NOx and O3, beyond observational constraints. This implies uncertainties in the NOx budget and our understanding of atmospheric chemistry.
Anna Breuninger, Philipp Joppe, Jonas Wilsch, Cornelis Schwenk, Heiko Bozem, Nicolas Emig, Laurin Merkel, Rainer Rossberg, Timo Keber, Arthur Kutschka, Philipp Waleska, Stefan Hofmann, Sarah Richter, Florian Ungeheuer, Konstantin Dörholt, Thorsten Hoffmann, Annette Miltenberger, Johannes Schneider, Peter Hoor, and Alexander L. Vogel
Atmos. Chem. Phys., 25, 16533–16551, https://doi.org/10.5194/acp-25-16533-2025, https://doi.org/10.5194/acp-25-16533-2025, 2025
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This study investigates molecular organic aerosol composition in the upper troposphere and lower stratosphere from an airborne campaign over Central Europe in summer 2024. Via ultra-high-performance liquid chromatography and high-resolution mass spectrometry of tropospheric and stratospheric filter samples, we identified various organic compounds. Our findings underscore the significant cross-tropopause transport of biogenic secondary organic aerosol and anthropogenic pollutants.
Yuwen Li, Wuhu Feng, John M. C. Plane, Tijian Wang, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2025-5346, https://doi.org/10.5194/egusphere-2025-5346, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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The space industry is growing rapidly, but its environmental effects remain uncertain. We used a global chemistry-climate model to study how chlorine released by rocket launches could affect the ozone layer and its recovery from past depletion. Even with large growth in launches, global ozone loss remains small but could locally slow the healing of the ozone layer. These findings highlight the need to consider rocket emissions in future environmental policies.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 15991–16007, https://doi.org/10.5194/acp-25-15991-2025, https://doi.org/10.5194/acp-25-15991-2025, 2025
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Tropospheric ozone (O3) is a harmful secondary atmospheric pollutant and an important greenhouse gas. Here, we present an in-depth analysis of lower-tropospheric sub-column O3 (LTCO3, surface – 6 km) records from three satellite products produced by the Rutherford Appleton Laboratory (RAL) over Europe between 1996 and 2017. Overall, we detect moderate negative trends in the satellite records, but corresponding model simulations and ozonesonde measurements show negligible trends.
Michael P. Cartwright, Jeremy J. Harrison, David P. Moore, Richard J. Pope, Martyn P. Chipperfield, Chris Wilson, and Wuhu Feng
Atmos. Chem. Phys., 25, 15913–15934, https://doi.org/10.5194/acp-25-15913-2025, https://doi.org/10.5194/acp-25-15913-2025, 2025
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We use satellite measurements to estimate quantities of a gas called carbonyl sulfide (OCS) in the atmosphere. OCS is consumed during photosynthesis, much like carbon dioxide (CO2). Our data is focused mostly over the global oceans for the year 2018, and we find it compares well with past satellite observations, ground-based measurements and modelled OCS. We hope to extend this measurement record and use it in data-driven tools in the future to better understand the carbon cycle globally.
Johannes Degen, Bianca C. Baier, Patrick Jöckel, J. Moritz Menken, Tanja J. Schuck, Colm Sweeney, and Andreas Engel
Atmos. Chem. Phys., 25, 15741–15763, https://doi.org/10.5194/acp-25-15741-2025, https://doi.org/10.5194/acp-25-15741-2025, 2025
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We investigate the distribution of CO2 in the upper troposphere and lower stratosphere using both, observations and an atmospheric model. Simulating an artificial tracer, we separate CO2 seasonality from long-term trend and transport variability. We found that patterns in the seasonal signal are attributable to large-scale transport features like the subtropical jet or the Brewer-Dobson circulation. Being a powerful diagnostic tool we recommend to use this tracer for model intercomparisons.
Heiko Bozem, Philipp Joppe, Yun Li, Nicolas Emig, Armin Afchine, Anna Breuninger, Joachim Curtius, Stefan Hofmann, Sadath Ismayil, Konrad Kandler, Daniel Kunkel, Arthur Kutschka, Hans-Christoph Lachnitt, Andreas Petzold, Sarah Richter, Timo Röschenthaler, Christian Rolf, Lisa Schneider, Johannes Schneider, Alexander Vogel, and Peter Hoor
Atmos. Meas. Tech., 18, 6545–6568, https://doi.org/10.5194/amt-18-6545-2025, https://doi.org/10.5194/amt-18-6545-2025, 2025
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Deployed on a Learjet as a tandem measurement platform during the TPEx I (TropoPause composition gradients and mixing Experiment) campaign in June 2024, the new TPC-TOSS (TropoPause Composition Towed Sensor Shuttle) system delivers high-resolution in situ data on ozone, aerosol, and key meteorological parameters. Laboratory and in-flight tests confirmed its precision and stability. Observed gradients near the tropopause reveal active mixing and transport processes in the tropopause region.
Antonio G. Bruno, David P. Moore, Jeremy J. Harrison, Ailish Graham, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2025-5109, https://doi.org/10.5194/egusphere-2025-5109, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Indonesian peatlands store vast carbon reserves, but can release large quantities of greenhouse gases and other species with significant environmental impacts, including HCN, when fires occur. Analyzing three major El Niño years with satellites and models, we found that emissions depend on local hydrological conditions, not just El Niño strength. Including soil moisture and burn depth can improve emission estimates and climate strategies.
Chun Hang Chau, Peter Hoor, Katharina Kaiser, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2025-5382, https://doi.org/10.5194/egusphere-2025-5382, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study examines the sensitivity of different greenhouse gases to vertical mixing by clear air turbulence in the upper troposphere and lower stratosphere. We found that ozone is most sensitive to vertical mixing and could lead to cooling at the top of the atmosphere by -0.2 W/m2. We also found that the vertical mixing by clear air turbulence could lead to changes in methane lifetime and the ozone chemistry.
Philipp Joppe, Johannes Schneider, Jonas Wilsch, Heiko Bozem, Anna Breuninger, Joachim Curtius, Martin Ebert, Nicolas Emig, Peter Hoor, Sadath Ismayil, Konrad Kandler, Daniel Kunkel, Isabel Kurth, Hans-Christoph Lachnitt, Yun Li, Annette Miltenberger, Sarah Richter, Christian Rolf, Lisa Schneider, Cornelis Schwenk, Nicole Spelten, Alexander L. Vogel, Yafang Cheng, and Stephan Borrmann
Atmos. Chem. Phys., 25, 15077–15103, https://doi.org/10.5194/acp-25-15077-2025, https://doi.org/10.5194/acp-25-15077-2025, 2025
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We show measurements of a filament with biomass burning influence transported by a warm conveyor belt (WCB) into the tropopause region over Europe. The pollution originates from Canadian forest fires and is transported in the lower troposphere towards Europe. The WCB transport is followed by mixing with air masses of stratospheric chemical signatures. We hypothesize that this mixing leads to a change in the vertical gradient of the potential temperature.
Oleh Kachula, Bärbel Vogel, Gebhard Günther, and Rolf Müller
Atmos. Chem. Phys., 25, 15171–15195, https://doi.org/10.5194/acp-25-15171-2025, https://doi.org/10.5194/acp-25-15171-2025, 2025
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We propose a novel method to define the boundary of the Asian summer monsoon anticyclone (ASMA) and provide the inter-annual and intra-seasonal analyses based on 44 years (1980–2023) and highlight individual years – 2017, 2022 and 2023 during which aircraft campaigns StratoClim, ACCLIP and PHILEAS took place respectively. Our method shows consistent results with previous studies but also provide new information about possible bimodality of the ASMA and inter-annual decrease of the ASMA area.
Linda Ort, Andrea Pozzer, Peter Hoor, Florian Obersteiner, Andreas Zahn, Thomas B. Ryerson, Chelsea R. Thompson, Jeff Peischl, Róisín Commane, Bruce Daube, Ilann Bourgeois, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 25, 14987–15007, https://doi.org/10.5194/acp-25-14987-2025, https://doi.org/10.5194/acp-25-14987-2025, 2025
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This study investigates the role of lightning emissions on the O3–CO ratio in the northern subtropics. We used in situ observations and a global circulation model to show an effect of up to 40 % onto the subtropical O3–CO ratio by tropical air masses transported via the Hadley cell. This influence of lightning emissions and its photochemistry has a global effect on trace and greenhouse gases and needs to be considered for global chemical distributions.
Sophie Bauchinger, Andreas Engel, Markus Jesswein, Timo Keber, Harald Bönisch, Florian Obersteiner, Andreas Zahn, Nicolas Emig, Peter Hoor, Hans-Christoph Lachnitt, Franziska Weyland, Linda Ort, and Tanja J. Schuck
Atmos. Chem. Phys., 25, 14167–14186, https://doi.org/10.5194/acp-25-14167-2025, https://doi.org/10.5194/acp-25-14167-2025, 2025
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We compared different ways to define the upper barrier of the troposphere in the extra-tropics, the “tropopause”. By analysing ozone distributions sorted by different definitions, we found that the traditional temperature-based tropopause works less well than dynamic or tracer-based definitions. We saw a sharper transition of ozone across the tropopause using a higher value of potential vorticity than often used and recommend this value for future studies of exchange processes in this region.
Gerald Wetzel, Anne Kleinert, Sören Johansson, Felix Friedl-Vallon, Michael Höpfner, Jörn Ungermann, Tom Neubert, Valéry Catoire, Cyril Crevoisier, Andreas Engel, Thomas Gulde, Patrick Jacquet, Oliver Kirner, Erik Kretschmer, Thomas Kulessa, Johannes C. Laube, Guido Maucher, Hans Nordmeyer, Christof Piesch, Peter Preusse, Markus Retzlaff, Georg Schardt, Johan Schillings, Herbert Schneider, Axel Schönfeld, Tanja Schuck, Wolfgang Woiwode, Martin Riese, and Peter Braesicke
Atmos. Meas. Tech., 18, 5873–5894, https://doi.org/10.5194/amt-18-5873-2025, https://doi.org/10.5194/amt-18-5873-2025, 2025
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We present vertical trace gas profiles from the first balloon flight of the newly developed GLORIA-B limb-imaging Fourier-Transform spectrometer. Longer-lived gases are compared to external measurements to assess the quality of the GLORIA-B observations. Diurnal changes of photochemically active species are compared to model simulations. GLORIA-B demonstrates the capability of balloon-borne limb imaging to provide high-resolution vertical profiles of trace gases up to the middle stratosphere.
Benjamin Weyland, Simon Rosanka, Domenico Taraborrelli, Birger Bohn, Andreas Zahn, Florian Obersteiner, Eric Förster, Mariano Mertens, Patrick Jöckel, Helmut Ziereis, Katharina Kaiser, Horst Fischer, John N. Crowley, Nijing Wang, Achim Edtbauer, Jonathan Williams, Maria Dolores Andrés Hernández, John P. Burrows, Flora Kluge, Meike Rotermund, Andre Butz, and Klaus Pfeilsticker
EGUsphere, https://doi.org/10.5194/egusphere-2025-5085, https://doi.org/10.5194/egusphere-2025-5085, 2025
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The destruction by sunlight of nitrous acid (HONO) produces the so-called detergent of the atmosphere. HONO has been measured in concentrations which exceed predictions based on known chemistry for decades. Several reactions have been proposed which may explain this excess HONO. This study reports on airborne measurements of HONO; the observations exceed predictions and form a C-shaped profile in the troposphere. Together with a host of other measurements, various reactions are investigated.
Chun Hang Chau, Peter Hoor, and Holger Tost
Atmos. Chem. Phys., 25, 13123–13140, https://doi.org/10.5194/acp-25-13123-2025, https://doi.org/10.5194/acp-25-13123-2025, 2025
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This study examines how the turbulence in the upper troposphere/lower stratosphere (UTLS) could modify the tracer distribution under different situations. Using a multi-scale chemistry model with a novel diagnostic, we found that both the pre-existing tracer gradient and the dynamical and thermodynamical forcing play a role in modifying the tracer distribution. These results allow further research on the UTLS turbulent mixing and its implications for the climate system.
Nicolas Emig, Annette K. Miltenberger, Peter M. Hoor, and Andreas Petzold
Atmos. Chem. Phys., 25, 13077–13101, https://doi.org/10.5194/acp-25-13077-2025, https://doi.org/10.5194/acp-25-13077-2025, 2025
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This study presents in situ observations of cirrus occurrence from aircraft measurements in the extratropical transition layer (ExTL) using simultaneous measurements from two platforms. Lagrangian diagnostics based on high-resolution ICON simulations show long residence times of the cirrus in stratospheric air, allowing us to separate different diabatic processes during transit. The findings suggest that radiative diabatic cloud processes significantly impact the tropopause thermodynamic structure.
Zhen Yang, Bärbel Vogel, Felix Plöger, Zhixuan Bai, Dan Li, Sabine Griessbach, Lars Hoffmann, Frank G. Wienhold, Elizabeth Asher, Alexandre A. Baron, Katie R. Smith, Troy Thornberry, Jianchun Bian, and Michaela I. Hegglin
EGUsphere, https://doi.org/10.5194/egusphere-2025-4842, https://doi.org/10.5194/egusphere-2025-4842, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Night-time balloon profiles over Lhasa, combined with satellite-constrained modeling, tracked the 2019 Raikoke volcano’s aerosol plumes through the Asian summer monsoon. We find two altitude-separated routes into the anticyclone. The monsoon partly blocks transport but permits entrainment and internal mixing, explaining gradual dilution. Matching the observations required stronger subgrid mixing, and the plume likely rose ~4–5 km from radiative heating.
Johannes Schneider, Christiane Schulz, Florian Rubach, Anna Ludwig, Jonas Wilsch, Philipp Joppe, Christian Gurk, Sergej Molleker, Laurent Poulain, Florian Obersteiner, Torsten Gehrlein, Harald Bönisch, Andreas Zahn, Peter Hoor, Nicolas Emig, Heiko Bozem, Stephan Borrmann, and Markus Hermann
Atmos. Meas. Tech., 18, 5103–5128, https://doi.org/10.5194/amt-18-5103-2025, https://doi.org/10.5194/amt-18-5103-2025, 2025
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An instrumented container laboratory is operated on regular commercial passenger flights to obtain a long-term representative dataset on the composition of the upper troposphere and lower stratosphere. Here we report on the development of a fully automated aerosol mass spectrometer for this project. We present technical specifications, necessary modifications for the automation, instrument calibration and comparisons, detection limits, and the first in-flight data.
Martin K. Vollmer, Joseph R. Pitt, Dickon Young, Stephan Henne, Blagoj Mitrevski, Jens Mühle, Anita Ganesan, Jgor Arduini, Alistair J. Manning, Thomas Wagenhäuser, Alison L. Redington, Brendan Murphy, Ray Gluckmann, Kieran M. Stanley, Paul B. Krummel, Chris R. Lunder, Jaegeun Yun, Dominique Rust, Angelina Wenger, Myriam Guillevic, Jooil Kim, Ray H. J. Wang, Tae Siek Rhee, Lionel Constantin, Arnoud Frumau, Christina M. Harth, Peter K. Salameh, Ove Hermansen, Andreas Engel, Simon O'Doherty, Sunyoung Park, Michela Maione, Paul J. Fraser, Ronald G. Prinn, Ray F. Weiss, and Stefan Reimann
EGUsphere, https://doi.org/10.5194/egusphere-2025-4824, https://doi.org/10.5194/egusphere-2025-4824, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We provide atmospheric measurements of halogenated olefins from the Advanced Global Atmospheric Gases Experiments and we calculate NorthWest European Emissions.
Evgenia Galytska, Birgit Hassler, Carlo Arosio, Martyn P. Chipperfield, Sandip S. Dhomse, Kimberlee Dubé, Wuhu Feng, Fernando Iglesias-Suarez, and Jakob Runge
EGUsphere, https://doi.org/10.21203/rs.3.rs-6426983/v2, https://doi.org/10.21203/rs.3.rs-6426983/v2, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We explored how chemical and dynamical processes shape ozone in the tropical middle stratosphere. Using a method that identifies cause and effect with satellite data and a chemistry-transport model, we found that from 2004–2011 nitrous oxide quickly affected nitrogen dioxide and ozone, while from 2012–2018 this effect was delayed, weakening ozone loss. Large-scale winds also influenced this link, clarifying how different mechanisms control ozone.
Herman G. J. Smit, Torben Galle, Romain Blot, Florian Obersteiner, Philippe Nédélec, Andreas Zahn, Jean-Marc Cousin, Ulrich Bundke, Andreas Petzold, Valerie Thouret, and Hannah Clark
Atmos. Meas. Tech., 18, 4985–5001, https://doi.org/10.5194/amt-18-4985-2025, https://doi.org/10.5194/amt-18-4985-2025, 2025
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The two ozone instruments of IAGOS (In-service Aircraft for a Global Observation System) have been compared with the Ozone PhotoMeter (OPM) of the World Calibration Center of Ozone Sondes (WCCOS) in an atmospheric simulation chamber under realistic flight conditions of pressure, temperature, and ozone concentrations. The two IAGOS-instruments showed good agreement with the OPM within 5–6 %. The observed differences are small but systematic and reproducible during the intercomparison.
Sarah Richter, Timo Keber, Martin Heinritzi, Lisa Beck, Laurin Merkel, Sarah Kirchhoff, Jann Schrod, Patrick Weber, and Joachim Curtius
EGUsphere, https://doi.org/10.5194/egusphere-2025-4349, https://doi.org/10.5194/egusphere-2025-4349, 2025
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We constructed and characterized a Fluorinert multi-channel Condensation Particle Counter for aircraft applications that comprises three channels and a pressure regulation system to measure nucleation mode particles in the upper troposphere. The cutoffs were determined at several ambient and internal pressures and sample flows. During the first aircraft campaign TPEx we were able to identify possible new particle formation events.
Johannes C. Laube, Tanja J. Schuck, Sophie Baartman, Huilin Chen, Markus Geldenhuys, Steven van Heuven, Timo Keber, Maria Elena Popa, Elinor Tuffnell, Florian Voet, Bärbel Vogel, Thomas Wagenhäuser, Alessandro Zanchetta, and Andreas Engel
Atmos. Meas. Tech., 18, 4087–4102, https://doi.org/10.5194/amt-18-4087-2025, https://doi.org/10.5194/amt-18-4087-2025, 2025
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A large balloon was launched in summer 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km, above the reach of aircraft. The main aims were to evaluate different techniques and atmospheric processes. We focus on halogenated greenhouse gases and ozone-depleting substances. For this, air was collected with the AirCore technique and a cryogenic air sampler and measured after the flight. A companion paper reports observations of major greenhouse gases.
Maria P. Veláquez-García, Richard J. Pope, Steven T. Turnock, Chetan Deva, David P. Moore, Guilherme Mataveli, Steve R. Arnold, Ruth M. Doherty, and Martyn P. Chiperffield
EGUsphere, https://doi.org/10.5194/egusphere-2025-3579, https://doi.org/10.5194/egusphere-2025-3579, 2025
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Incorporating fire simulation into climate models is crucial for accurately representing the interactions between fires, ecosystems, and climate, thereby enhancing climate projections. In South America, the INFERNO fire model captures active fire zones, e.g. the Amazon Arc of Deforestation, but it overestimates emissions in other areas (mainly in tree-rich ecosystems). The model errors capturing seasonal emission cycles relate to the effects of soil moisture on plant flammability and growth.
Rodrigo J. Seguel, Charlie Opazo, Yann Cohen, Owen R. Cooper, Laura Gallardo, Björn-Martin Sinnhuber, Florian Obersteiner, Andreas Zahn, Peter Hoor, Susanne Rohs, and Andreas Marsing
Atmos. Chem. Phys., 25, 8553–8573, https://doi.org/10.5194/acp-25-8553-2025, https://doi.org/10.5194/acp-25-8553-2025, 2025
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We explored ozone differences between the Northern Hemisphere and Southern Hemispheres in the upper troposphere–lower stratosphere. We found lower ozone (with stratospheric origin) in the Southern Hemisphere, especially during years of severe ozone depletion. Sudden stratospheric warming events increased the ozone in each hemisphere, highlighting the relationship between stratospheric processes and ozone in the upper troposphere, where ozone is an important greenhouse gas.
Markus Jesswein, Valentin Lauther, Nicolas Emig, Peter Hoor, Timo Keber, Hans-Christoph Lachnitt, Linda Ort, Tanja Schuck, Johannes Strobel, Ronja Van Luijt, C. Michael Volk, Franziska Weyland, and Andreas Engel
Atmos. Chem. Phys., 25, 8107–8126, https://doi.org/10.5194/acp-25-8107-2025, https://doi.org/10.5194/acp-25-8107-2025, 2025
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The study investigates transport within the Asian Summer Monsoon, focusing on how CH2Cl2 reaches the subarctic tropopause region. Using data from the PHILEAS campaign in 2023, events with increased mixing ratios were detected. Their origin, the transport paths to the tropopause region, and the potential entry into the stratosphere were analyzed. The East Asian Summer Monsoon was identified as the main transport pathway, with only a small contribution to the stratosphere in the following days.
Yann Cohen, Didier Hauglustaine, Nicolas Bellouin, Marianne Tronstad Lund, Sigrun Matthes, Agnieszka Skowron, Robin Thor, Ulrich Bundke, Andreas Petzold, Susanne Rohs, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 25, 5793–5836, https://doi.org/10.5194/acp-25-5793-2025, https://doi.org/10.5194/acp-25-5793-2025, 2025
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The chemical composition of the atmosphere near the tropopause is a key parameter for evaluating the climate impact of subsonic aviation pollutants. This study uses in situ data collected aboard passenger aircraft to assess the ability of four chemistry–climate models to reproduce (bi-)decadal climatologies of ozone, carbon monoxide, water vapour, and reactive nitrogen in this region. The models reproduce the very distinct ozone seasonality in the upper troposphere and in the lower stratosphere well.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
Atmos. Chem. Phys., 25, 4403–4418, https://doi.org/10.5194/acp-25-4403-2025, https://doi.org/10.5194/acp-25-4403-2025, 2025
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4391–4401, https://doi.org/10.5194/acp-25-4391-2025, https://doi.org/10.5194/acp-25-4391-2025, 2025
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Globally, lockdowns were implemented to limit the spread of COVID-19, leading to a decrease in emissions of key air pollutants. Here, we use novel satellite data and a chemistry model to investigate the impact of the pandemic on tropospheric ozone (O3), a key pollutant, in 2020. Overall, we found substantial decreases of up to 20 %, two-thirds of which came from emission reductions, while one-third was due to a decrease in the stratospheric O3 flux into the troposphere.
Tanja J. Schuck, Johannes Degen, Timo Keber, Katharina Meixner, Thomas Wagenhäuser, Mélanie Ghysels, Georges Durry, Nadir Amarouche, Alessandro Zanchetta, Steven van Heuven, Huilin Chen, Johannes C. Laube, Sophie L. Baartman, Carina van der Veen, Maria Elena Popa, and Andreas Engel
Atmos. Chem. Phys., 25, 4333–4348, https://doi.org/10.5194/acp-25-4333-2025, https://doi.org/10.5194/acp-25-4333-2025, 2025
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A balloon was launched in 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km. One purpose was to compare measurement techniques. We focus on the major greenhouse gases. To measure these, air was sampled with the AirCore technique and with flask sampling, and samples were analysed after the flight. In flight, observations were done with an optical method. In a companion paper, we report on observations of chlorine and bromine containing trace gases.
Patrick Konjari, Christian Rolf, Michaela I. Hegglin, Susanne Rohs, Yun Li, Andreas Zahn, Harald Bönisch, Philippe Nedelec, Martina Krämer, and Andreas Petzold
Atmos. Chem. Phys., 25, 4269–4289, https://doi.org/10.5194/acp-25-4269-2025, https://doi.org/10.5194/acp-25-4269-2025, 2025
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This study introduces a new method to derive adjusted water vapor (H2O) climatologies for the upper tropopshere and lower statosphere (UT/LS) using data from 60 000 flights under the IAGOS program. Biases in the IAGOS water vapour dataset are adjusted, based on the more accurate IAGOS-CARIBIC data. The resulting highly resolved H2O climatologies will contribute to a better understanding of the H2O variability in the UT/LS and its connection to various transport and mixing processes.
Laura N. Saunders, Kaley A. Walker, Gabriele P. Stiller, Thomas von Clarmann, Florian Haenel, Hella Garny, Harald Bönisch, Chris D. Boone, Ariana E. Castillo, Andreas Engel, Johannes C. Laube, Marianna Linz, Felix Ploeger, David A. Plummer, Eric A. Ray, and Patrick E. Sheese
Atmos. Chem. Phys., 25, 4185–4209, https://doi.org/10.5194/acp-25-4185-2025, https://doi.org/10.5194/acp-25-4185-2025, 2025
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We present a 17-year stratospheric age-of-air dataset derived from ACE-FTS satellite measurements of sulfur hexafluoride. This is the longest continuous, global, and vertically resolved age of air time series available to date. In this paper, we show that this dataset agrees well with age-of-air datasets based on measurements from other instruments. We also present trends in the midlatitude lower stratosphere that indicate changes in the global circulation that are predicted by climate models.
Florian Voet, Felix Ploeger, Johannes Laube, Peter Preusse, Paul Konopka, Jens-Uwe Grooß, Jörn Ungermann, Björn-Martin Sinnhuber, Michael Höpfner, Bernd Funke, Gerald Wetzel, Sören Johansson, Gabriele Stiller, Eric Ray, and Michaela I. Hegglin
Atmos. Chem. Phys., 25, 3541–3565, https://doi.org/10.5194/acp-25-3541-2025, https://doi.org/10.5194/acp-25-3541-2025, 2025
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This study refines estimates of the stratospheric “age of air”, a measure of how long air circulates in the stratosphere. By analyzing correlations between trace gases measurable by satellites, the research introduces a method that reduces uncertainties and detects small-scale atmospheric features. This improved understanding of stratospheric circulation is crucial for better climate models and predictions, enhancing our ability to assess the impacts of climate change on the atmosphere.
Douwang Li, Zhe Wang, Siyi Zhao, Jiankai Zhang, Wuhu Feng, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2025-955, https://doi.org/10.5194/egusphere-2025-955, 2025
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We find that wind variations at the equator (QBO) modulate the occurrence of Arctic polar stratospheric clouds (PSCs), which are key contributors to ozone depletion. During westerly QBO, the PSC occurrence is significantly greater than during easterly QBO. The QBO affects PSC mainly through temperature, while H2O and HNO3 have less effect. This suggests that future climate change may affect ozone recovery if it alters the QBO pattern. This study provides a new perspective on ozone prediction.
Jamal Makkor, Mathias Palm, Matthias Buschmann, Emmanuel Mahieu, Martyn P. Chipperfield, and Justus Notholt
Atmos. Meas. Tech., 18, 1105–1114, https://doi.org/10.5194/amt-18-1105-2025, https://doi.org/10.5194/amt-18-1105-2025, 2025
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During the years 1950 and 1951, Marcel Migeotte took regular solar measurements in the form of paper rolls at the Jungfraujoch site. These historical spectra proved to be valuable for atmospheric research and needed to be saved for posterity. Therefore, a digitization method which used image-processing techniques was developed to extract them from the historical paper rolls. This allowed them to be saved in a machine-readable format that is easily accessible to the scientific community.
Franziska Weyland, Peter Hoor, Daniel Kunkel, Thomas Birner, Felix Plöger, and Katharina Turhal
Atmos. Chem. Phys., 25, 1227–1252, https://doi.org/10.5194/acp-25-1227-2025, https://doi.org/10.5194/acp-25-1227-2025, 2025
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The lowermost stratosphere (LMS) plays an important role in the Earth's climate, containing strong gradients of ozone and water vapor. Our results indicate that the thermodynamic structure of the LMS was changing between 1979–2019 in response to anthropogenic climate change and the recovery of stratospheric ozone, also indicating large-scale circulation changes. We find that both the upper and the lower LMS boundaries show an (upward) trend, which has implications for the LMS mass.
Katharina Turhal, Felix Plöger, Jan Clemens, Thomas Birner, Franziska Weyland, Paul Konopka, and Peter Hoor
Atmos. Chem. Phys., 24, 13653–13679, https://doi.org/10.5194/acp-24-13653-2024, https://doi.org/10.5194/acp-24-13653-2024, 2024
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The tropopause separates the troposphere, where many greenhouse gases originate, from the stratosphere. This study examines a tropopause defined by potential vorticity – an analogue for angular momentum that changes sharply in the subtropics, creating a transport barrier. Between 1980 and 2017, this tropopause shifted poleward at lower altitudes and equatorward above, suggesting height-dependent changes in atmospheric circulation that may affect greenhouse gas distribution and global warming.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn P. Chipperfield, Wuhu Feng, David E. Oram, Karina E. Adcock, Stephen A. Montzka, Isobel J. Simpson, Andrea Mazzeo, Amber A. Leeson, Elliot Atlas, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 13457–13475, https://doi.org/10.5194/acp-24-13457-2024, https://doi.org/10.5194/acp-24-13457-2024, 2024
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DCE (1,2-dichloroethane) is an industrial chemical used to produce PVC (polyvinyl chloride). We analysed DCE production data to estimate global DCE emissions (2002–2020). The emissions were included in an atmospheric model and evaluated by comparing simulated DCE to DCE measurements in the troposphere. We show that DCE contributes ozone-depleting Cl to the stratosphere and that this has increased with increasing DCE emissions. DCE’s impact on stratospheric O3 is currently small but non-zero.
Yiran Zhang-Liu, Rolf Müller, Jens-Uwe Grooß, Sabine Robrecht, Bärbel Vogel, Abdul Mannan Zafar, and Ralph Lehmann
Atmos. Chem. Phys., 24, 12557–12574, https://doi.org/10.5194/acp-24-12557-2024, https://doi.org/10.5194/acp-24-12557-2024, 2024
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HCl null cycles in Antarctica are important for maintaining high values of ozone-destroying chlorine in Antarctic spring. These HCl null cycles are not affected by (1) using the most recent recommendations of chemical kinetics (compared to older recommendations), (2) accounting for dehydration in the Antarctic winter vortex, and (3) considering the observed (but unexplained) depletion of HCl in mid-winter in the Antarctic vortex throughout Antarctic winter.
Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5731–5746, https://doi.org/10.5194/amt-17-5731-2024, https://doi.org/10.5194/amt-17-5731-2024, 2024
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The ozone sink into oceans and marine clouds is seldom studied and highly uncertain. Calculations suggest O3 destruction at aqueous surfaces (ocean, droplets) may be strongly accelerated, but field evidence is missing. Here we compare three fast airborne O3 instruments to measure eddy covariance fluxes of O3 over the remote ocean, in clear and cloudy air. We find O3 fluxes below clouds are consistently directed into clouds, while O3 fluxes into oceans are much smaller and spatially variable.
Chris Wilson, Brian J. Kerridge, Richard Siddans, David P. Moore, Lucy J. Ventress, Emily Dowd, Wuhu Feng, Martyn P. Chipperfield, and John J. Remedios
Atmos. Chem. Phys., 24, 10639–10653, https://doi.org/10.5194/acp-24-10639-2024, https://doi.org/10.5194/acp-24-10639-2024, 2024
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The leaks from the Nord Stream gas pipelines in September 2022 released a large amount of methane (CH4) into the atmosphere. We provide observational data from a satellite instrument that shows a large CH4 plume over the North Sea off the coast of Scandinavia. We use this together with atmospheric models to quantify the CH4 leaked into the atmosphere from the pipelines. We find that 219–427 Gg CH4 was emitted, making this the largest individual fossil-fuel-related CH4 leak on record.
Richard J. Pope, Fiona M. O'Connor, Mohit Dalvi, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Brice Barret, Eric Le Flochmoen, Anne Boynard, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, Catherine Wespes, and Richard Rigby
Atmos. Chem. Phys., 24, 9177–9195, https://doi.org/10.5194/acp-24-9177-2024, https://doi.org/10.5194/acp-24-9177-2024, 2024
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Ozone is a potent air pollutant in the lower troposphere, with adverse impacts on human health. Satellite records of tropospheric ozone currently show large-scale inconsistencies in long-term trends. Our detailed study of the potential factors (e.g. satellite errors, where the satellite can observe ozone) potentially driving these inconsistencies found that, in North America, Europe, and East Asia, the underlying trends are typically small with large uncertainties.
Karolin Voss, Philip Holzbeck, Klaus Pfeilsticker, Ralph Kleinschek, Gerald Wetzel, Blanca Fuentes Andrade, Michael Höpfner, Jörn Ungermann, Björn-Martin Sinnhuber, and André Butz
Atmos. Meas. Tech., 17, 4507–4528, https://doi.org/10.5194/amt-17-4507-2024, https://doi.org/10.5194/amt-17-4507-2024, 2024
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A novel balloon-borne instrument for direct sun and solar occultation measurements of several UV–Vis absorbing gases (e.g. O3, NO2, BrO, IO, and HONO) is described. Its major design features and performance during two stratospheric deployments are discussed. From the measured overhead BrO concentration and a suitable photochemical correction, total stratospheric bromine is inferred to (17.5 ± 2.2) ppt in air masses which entered the stratosphere around early 2017 ± 1 year.
Yang Li, Wuhu Feng, Xin Zhou, Yajuan Li, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 8277–8293, https://doi.org/10.5194/acp-24-8277-2024, https://doi.org/10.5194/acp-24-8277-2024, 2024
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The Tibetan Plateau (TP), the highest and largest plateau, experiences strong surface solar UV radiation, whose excess can cause harmful influences on local biota. Hence, it is critical to study TP ozone. We find ENSO, the strongest interannual phenomenon, tends to induce tropospheric temperature change and thus modulate tropopause variability, which in turn favours ozone change over the TP. Our results have implications for a better understanding of the interannual variability of TP ozone.
Luis F. Millán, Peter Hoor, Michaela I. Hegglin, Gloria L. Manney, Harald Boenisch, Paul Jeffery, Daniel Kunkel, Irina Petropavlovskikh, Hao Ye, Thierry Leblanc, and Kaley Walker
Atmos. Chem. Phys., 24, 7927–7959, https://doi.org/10.5194/acp-24-7927-2024, https://doi.org/10.5194/acp-24-7927-2024, 2024
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In the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we have mapped multiplatform ozone datasets into coordinate systems to systematically evaluate the influence of these coordinates on binned climatological variability. This effort unifies the work of studies that focused on individual coordinate system variability. Our goal was to create the most comprehensive assessment of this topic.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
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The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, and Stephan Borrmann
Atmos. Chem. Phys., 24, 7499–7522, https://doi.org/10.5194/acp-24-7499-2024, https://doi.org/10.5194/acp-24-7499-2024, 2024
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From aircraft measurements in the upper troposphere/lower stratosphere, we find a correlation between the ozone and particulate sulfate in the lower stratosphere. The correlation exhibits some variability over the measurement period exceeding the background sulfate-to-ozone correlation. From our analysis, we conclude that gas-to-particle conversion of volcanic sulfur dioxide leads to observed enhanced sulfate aerosol mixing ratios.
Sandra Graßl, Christoph Ritter, Ines Tritscher, and Bärbel Vogel
Atmos. Chem. Phys., 24, 7535–7557, https://doi.org/10.5194/acp-24-7535-2024, https://doi.org/10.5194/acp-24-7535-2024, 2024
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Arctic lidar data for 1 year are compared with global modeling of aerosol tracers in the stratosphere. A trend in the aerosol backscatter can be found. These observations are further compared with a model study to investigate the aerosol origin of the observed arctic aerosol. We found a correlation with increased backscatter signal during summer and early autumn and pathways from the Southeast Asian monsoon region and remains of the Asian tropopause aerosol layer in the Arctic.
Jan Clemens, Lars Hoffmann, Bärbel Vogel, Sabine Grießbach, and Nicole Thomas
Geosci. Model Dev., 17, 4467–4493, https://doi.org/10.5194/gmd-17-4467-2024, https://doi.org/10.5194/gmd-17-4467-2024, 2024
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Lagrangian transport models simulate the transport of air masses in the atmosphere. For example, one model (CLaMS) is well suited to calculating transport as it uses a special coordinate system and special vertical wind. However, it only runs inefficiently on modern supercomputers. Hence, we have implemented the benefits of CLaMS into a new model (MPTRAC), which is already highly efficient on modern supercomputers. Finally, in extensive tests, we showed that CLaMS and MPTRAC agree very well.
Felicia Kolonjari, Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, David A. Plummer, Andreas Engel, Stephen A. Montzka, David E. Oram, Tanja Schuck, Gabriele P. Stiller, and Geoffrey C. Toon
Atmos. Meas. Tech., 17, 2429–2449, https://doi.org/10.5194/amt-17-2429-2024, https://doi.org/10.5194/amt-17-2429-2024, 2024
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The Canadian Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) satellite instrument is currently providing the only vertically resolved chlorodifluoromethane (HCFC-22) measurements from space. This study assesses the most current ACE-FTS HCFC-22 data product in the upper troposphere and lower stratosphere, as well as modelled HCFC-22 from a 39-year run of the Canadian Middle Atmosphere Model (CMAM39) in the same region.
Martin Ebert, Ralf Weigel, Stephan Weinbruch, Lisa Schneider, Konrad Kandler, Stefan Lauterbach, Franziska Köllner, Felix Plöger, Gebhard Günther, Bärbel Vogel, and Stephan Borrmann
Atmos. Chem. Phys., 24, 4771–4788, https://doi.org/10.5194/acp-24-4771-2024, https://doi.org/10.5194/acp-24-4771-2024, 2024
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Particles were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL). Refractory particles from seven different flights were characterized by scanning and transmission electron microscopy (SEM, TEM). The most abundant refractory particles are silicates and non-volatile organics. The most important sources are combustion processes at the ground and the agitation of soil material. During one flight, small cinnabar particles (HgS) were also detected.
Santo Fedele Colosimo, Nathaniel Brockway, Vijay Natraj, Robert Spurr, Klaus Pfeilsticker, Lisa Scalone, Max Spolaor, Sarah Woods, and Jochen Stutz
Atmos. Meas. Tech., 17, 2367–2385, https://doi.org/10.5194/amt-17-2367-2024, https://doi.org/10.5194/amt-17-2367-2024, 2024
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Cirrus clouds are poorly understood components of the climate system, in part due to the challenge of observing thin, sub-visible ice clouds. We address this issue with a new observational approach that uses the remote sensing of near-infrared ice water absorption features from a high-altitude aircraft. We describe the underlying principle of this approach and present a new procedure to retrieve ice concentration in cirrus clouds. Our retrievals compare well with in situ observations.
Richard J. Pope, Alexandru Rap, Matilda A. Pimlott, Brice Barret, Eric Le Flochmoen, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Anne Boynard, Christian Retscher, Wuhu Feng, Richard Rigby, Sandip S. Dhomse, Catherine Wespes, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 3613–3626, https://doi.org/10.5194/acp-24-3613-2024, https://doi.org/10.5194/acp-24-3613-2024, 2024
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Tropospheric ozone is an important short-lived climate forcer which influences the incoming solar short-wave radiation and the outgoing long-wave radiation in the atmosphere (8–15 km) where the balance between the two yields a net positive (i.e. warming) effect at the surface. Overall, we find that the tropospheric ozone radiative effect ranges between 1.21 and 1.26 W m−2 with a negligible trend (2008–2017), suggesting that tropospheric ozone influences on climate have remained stable with time.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-516, https://doi.org/10.5194/egusphere-2024-516, 2024
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This study assesses atmospheric composition using air quality models during aircraft campaigns in Europe and Asia, focusing on carbonaceous aerosols and trace gases. While carbon monoxide is well modeled, other pollutants have moderate to weak agreement with observations. Wind speed modeling is reliable for identifying pollution plumes, where models tend to overestimate concentrations. This highlights challenges in accurately modeling aerosol and trace gas composition, particularly in cities.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-521, https://doi.org/10.5194/egusphere-2024-521, 2024
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This study explores the proportional relationships between carbonaceous aerosols (black and organic carbon) and trace gases using airborne measurements from two campaigns in Europe and East Asia. Differences between regions were found, but air quality models struggled to reproduce them accurately. We show that these proportional relationships can help to constrain models and can be used to infer aerosol concentrations from satellite observations of trace gases, especially in urban areas.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Ailish M. Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matilda Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
Atmos. Chem. Phys., 24, 789–806, https://doi.org/10.5194/acp-24-789-2024, https://doi.org/10.5194/acp-24-789-2024, 2024
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Our paper uses novel satellite datasets and high-resolution emissions datasets alongside a back-trajectory model to investigate the balance of local and external sources influencing NOx air pollution changes in Delhi. We find in the post-monsoon season that NOx from local and non-local transport emissions contributes most to poor air quality in Delhi. Therefore, air quality mitigation strategies in Delhi and surrounding regions are used to control this issue.
Jan Clemens, Bärbel Vogel, Lars Hoffmann, Sabine Griessbach, Nicole Thomas, Suvarna Fadnavis, Rolf Müller, Thomas Peter, and Felix Ploeger
Atmos. Chem. Phys., 24, 763–787, https://doi.org/10.5194/acp-24-763-2024, https://doi.org/10.5194/acp-24-763-2024, 2024
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The source regions of the Asian tropopause aerosol layer (ATAL) are debated. We use balloon-borne measurements of the layer above Nainital (India) in August 2016 and atmospheric transport models to find ATAL source regions. Most air originated from the Tibetan plateau. However, the measured ATAL was stronger when more air originated from the Indo-Gangetic Plain and weaker when more air originated from the Pacific. Hence, the results indicate important anthropogenic contributions to the ATAL.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Bärbel Vogel, C. Michael Volk, Johannes Wintel, Valentin Lauther, Jan Clemens, Jens-Uwe Grooß, Gebhard Günther, Lars Hoffmann, Johannes C. Laube, Rolf Müller, Felix Ploeger, and Fred Stroh
Atmos. Chem. Phys., 24, 317–343, https://doi.org/10.5194/acp-24-317-2024, https://doi.org/10.5194/acp-24-317-2024, 2024
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Over the Indian subcontinent, polluted air is rapidly uplifted to higher altitudes during the Asian monsoon season. We present an assessment of vertical transport in this region using different wind data provided by the European Centre for Medium-Range Weather Forecasts (ECMWF), as well as high-resolution aircraft measurements. In general, our findings confirm that the newest ECMWF reanalysis product, ERA5, yields a better representation of transport compared to the predecessor, ERA-Interim.
Andrea Pazmiño, Florence Goutail, Sophie Godin-Beekmann, Alain Hauchecorne, Jean-Pierre Pommereau, Martyn P. Chipperfield, Wuhu Feng, Franck Lefèvre, Audrey Lecouffe, Michel Van Roozendael, Nis Jepsen, Georg Hansen, Rigel Kivi, Kimberly Strong, and Kaley A. Walker
Atmos. Chem. Phys., 23, 15655–15670, https://doi.org/10.5194/acp-23-15655-2023, https://doi.org/10.5194/acp-23-15655-2023, 2023
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The vortex-averaged ozone loss over the last 3 decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from the SAOZ network and MSR2 reanalysis. Three metrics were developed to compute ozone trends since 2000. The study confirms the ozone recovery in the Antarctic and shows a potential sign of quantitative detection of ozone recovery in the Arctic that needs to be robustly confirmed in the future.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, and Richard Rigby
Atmos. Chem. Phys., 23, 14933–14947, https://doi.org/10.5194/acp-23-14933-2023, https://doi.org/10.5194/acp-23-14933-2023, 2023
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Ozone is a potent air pollutant, and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTCO3) from space. We have constructed a merged LTCO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTCO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small-scale differences.
Sandip S. Dhomse and Martyn P. Chipperfield
Earth Syst. Sci. Data, 15, 5105–5120, https://doi.org/10.5194/essd-15-5105-2023, https://doi.org/10.5194/essd-15-5105-2023, 2023
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There are no long-term stratospheric profile data sets for two very important greenhouse gases: methane (CH4) and nitrous oxide (N2O). Along with radiative feedback, these species play an important role in controlling ozone loss in the stratosphere. Here, we use machine learning to fuse satellite measurements with a chemical model to construct long-term gap-free profile data sets for CH4 and N2O. We aim to construct similar data sets for other important trace gases (e.g. O3, Cly, NOy species).
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
James Barry, Stefanie Meilinger, Klaus Pfeilsticker, Anna Herman-Czezuch, Nicola Kimiaie, Christopher Schirrmeister, Rone Yousif, Tina Buchmann, Johannes Grabenstein, Hartwig Deneke, Jonas Witthuhn, Claudia Emde, Felix Gödde, Bernhard Mayer, Leonhard Scheck, Marion Schroedter-Homscheidt, Philipp Hofbauer, and Matthias Struck
Atmos. Meas. Tech., 16, 4975–5007, https://doi.org/10.5194/amt-16-4975-2023, https://doi.org/10.5194/amt-16-4975-2023, 2023
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Measured power data from solar photovoltaic (PV) systems contain information about the state of the atmosphere. In this work, power data from PV systems in the Allgäu region in Germany were used to determine the solar irradiance at each location, using state-of-the-art simulation and modelling. The results were validated using concurrent measurements of the incoming solar radiation in each case. If applied on a wider scale, this algorithm could help improve weather and climate models.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys., 23, 13235–13253, https://doi.org/10.5194/acp-23-13235-2023, https://doi.org/10.5194/acp-23-13235-2023, 2023
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
Frederik Harzer, Hella Garny, Felix Ploeger, Harald Bönisch, Peter Hoor, and Thomas Birner
Atmos. Chem. Phys., 23, 10661–10675, https://doi.org/10.5194/acp-23-10661-2023, https://doi.org/10.5194/acp-23-10661-2023, 2023
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We study the statistical relation between year-by-year fluctuations in winter-mean ozone and the strength of the stratospheric polar vortex. In the latitude–pressure plane, regression analysis shows that anomalously weak polar vortex years are associated with three pronounced local ozone maxima over the polar cap relative to the winter climatology. These response maxima primarily reflect the non-trivial combination of different ozone transport processes with varying relative contributions.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Lars Hoffmann, Paul Konopka, Jan Clemens, and Bärbel Vogel
Atmos. Chem. Phys., 23, 7589–7609, https://doi.org/10.5194/acp-23-7589-2023, https://doi.org/10.5194/acp-23-7589-2023, 2023
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Atmospheric convection plays a key role in tracer transport in the troposphere. Global meteorological forecasts and reanalyses typically have a coarse spatiotemporal resolution that does not adequately resolve the dynamics, transport, and mixing of air associated with storm systems or deep convection. We discuss the application of the extreme convection parameterization in a Lagrangian transport model to improve simulations of tracer transport from the boundary layer into the free troposphere.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Luis F. Millán, Gloria L. Manney, Harald Boenisch, Michaela I. Hegglin, Peter Hoor, Daniel Kunkel, Thierry Leblanc, Irina Petropavlovskikh, Kaley Walker, Krzysztof Wargan, and Andreas Zahn
Atmos. Meas. Tech., 16, 2957–2988, https://doi.org/10.5194/amt-16-2957-2023, https://doi.org/10.5194/amt-16-2957-2023, 2023
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The determination of atmospheric composition trends in the upper troposphere and lower stratosphere (UTLS) is still highly uncertain. We present the creation of dynamical diagnostics to map several ozone datasets (ozonesondes, lidars, aircraft, and satellite measurements) in geophysically based coordinate systems. The diagnostics can also be used to analyze other greenhouse gases relevant to surface climate and UTLS chemistry.
Peter Joyce, Cristina Ruiz Villena, Yahui Huang, Alex Webb, Manuel Gloor, Fabien H. Wagner, Martyn P. Chipperfield, Rocío Barrio Guilló, Chris Wilson, and Hartmut Boesch
Atmos. Meas. Tech., 16, 2627–2640, https://doi.org/10.5194/amt-16-2627-2023, https://doi.org/10.5194/amt-16-2627-2023, 2023
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Methane emissions are responsible for a lot of the warming caused by the greenhouse effect, much of which comes from a small number of point sources. We can identify methane point sources by analysing satellite data, but it requires a lot of time invested by experts and is prone to very high errors. Here, we produce a neural network that can automatically identify methane point sources and estimate the mass of methane that is being released per hour and are able to do so with far smaller errors.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
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During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
Phuc Thi Minh Ha, Yugo Kanaya, Fumikazu Taketani, Maria Dolores Andrés Hernández, Benjamin Schreiner, Klaus Pfeilsticker, and Kengo Sudo
Geosci. Model Dev., 16, 927–960, https://doi.org/10.5194/gmd-16-927-2023, https://doi.org/10.5194/gmd-16-927-2023, 2023
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HONO affects tropospheric oxidizing capacity; thus, it is implemented into the chemistry–climate model CHASER. The model substantially underpredicts daytime HONO, while nitrate photolysis on surfaces can supplement the daytime HONO budget. Current HONO chemistry predicts reductions of 20.4 % for global tropospheric NOx, 40–67 % for OH, and 30–45 % for O3 in the summer North Pacific. In contrast, OH and O3 winter levels in China are greatly enhanced.
Eric Förster, Harald Bönisch, Marco Neumaier, Florian Obersteiner, Andreas Zahn, Andreas Hilboll, Anna B. Kalisz Hedegaard, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Mihalis Vrekoussis, Michael Lichtenstern, and Peter Braesicke
Atmos. Chem. Phys., 23, 1893–1918, https://doi.org/10.5194/acp-23-1893-2023, https://doi.org/10.5194/acp-23-1893-2023, 2023
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The airborne megacity campaign EMeRGe provided an unprecedented amount of trace gas measurements. We combine measured volatile organic compounds (VOCs) with trajectory-modelled emission uptakes to identify potential source regions of pollution. We also characterise the chemical fingerprints (e.g. biomass burning and anthropogenic signatures) of the probed air masses to corroborate the contributing source regions. Our approach is the first large-scale study of VOCs originating from megacities.
Flora Kluge, Tilman Hüneke, Christophe Lerot, Simon Rosanka, Meike K. Rotermund, Domenico Taraborrelli, Benjamin Weyland, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 1369–1401, https://doi.org/10.5194/acp-23-1369-2023, https://doi.org/10.5194/acp-23-1369-2023, 2023
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Using airborne glyoxal concentration and vertical column density measurements, vertical profiles are inferred for eight global regions in aged biomass burning plumes and the tropical marine boundary layer. Using TROPOMI observations, an analysis of space- and airborne measurements is performed. A comparison to EMAC simulations shows a general glyoxal underprediction, which points to various missing sources and precursors from anthropogenic activities, biomass burning, and the sea surface.
Hans-Christoph Lachnitt, Peter Hoor, Daniel Kunkel, Martina Bramberger, Andreas Dörnbrack, Stefan Müller, Philipp Reutter, Andreas Giez, Thorsten Kaluza, and Markus Rapp
Atmos. Chem. Phys., 23, 355–373, https://doi.org/10.5194/acp-23-355-2023, https://doi.org/10.5194/acp-23-355-2023, 2023
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We present an analysis of high-resolution airborne measurements during a flight of the DEEPWAVE 2014 campaign in New Zealand. The focus of this flight was to study the effects of enhanced mountain wave activity over the Southern Alps. We discuss changes in the upstream and downstream distributions of N2O and CO and show that these changes are related to turbulence-induced trace gas fluxes which have persistent effects on the trace gas composition in the lower stratosphere.
Robert J. Parker, Chris Wilson, Edward Comyn-Platt, Garry Hayman, Toby R. Marthews, A. Anthony Bloom, Mark F. Lunt, Nicola Gedney, Simon J. Dadson, Joe McNorton, Neil Humpage, Hartmut Boesch, Martyn P. Chipperfield, Paul I. Palmer, and Dai Yamazaki
Biogeosciences, 19, 5779–5805, https://doi.org/10.5194/bg-19-5779-2022, https://doi.org/10.5194/bg-19-5779-2022, 2022
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Wetlands are the largest natural source of methane, one of the most important climate gases. The JULES land surface model simulates these emissions. We use satellite data to evaluate how well JULES reproduces the methane seasonal cycle over different tropical wetlands. It performs well for most regions; however, it struggles for some African wetlands influenced heavily by river flooding. We explain the reasons for these deficiencies and highlight how future development will improve these areas.
Reimar Bauer, Jens-Uwe Grooß, Jörn Ungermann, May Bär, Markus Geldenhuys, and Lars Hoffmann
Geosci. Model Dev., 15, 8983–8997, https://doi.org/10.5194/gmd-15-8983-2022, https://doi.org/10.5194/gmd-15-8983-2022, 2022
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The Mission Support System (MSS) is an open source software package that has been used for planning flight tracks of scientific aircraft in multiple measurement campaigns during the last decade. Here, we describe the MSS software and its use during the SouthTRAC measurement campaign in 2019. As an example for how the MSS software is used in conjunction with many datasets, we describe the planning of a single flight probing orographic gravity waves propagating up into the lower mesosphere.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Bernard Legras, Clair Duchamp, Pasquale Sellitto, Aurélien Podglajen, Elisa Carboni, Richard Siddans, Jens-Uwe Grooß, Sergey Khaykin, and Felix Ploeger
Atmos. Chem. Phys., 22, 14957–14970, https://doi.org/10.5194/acp-22-14957-2022, https://doi.org/10.5194/acp-22-14957-2022, 2022
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The long-duration atmospheric impact of the Tonga eruption in January 2022 is a plume of water and sulfate aerosols in the stratosphere that persisted for more than 6 months. We study this evolution using several satellite instruments and analyse the unusual behaviour of this plume as sulfates and water first moved down rapidly and then separated into two layers. We also report the self-organization in compact and long-lived patches.
Mohamadou A. Diallo, Felix Ploeger, Michaela I. Hegglin, Manfred Ern, Jens-Uwe Grooß, Sergey Khaykin, and Martin Riese
Atmos. Chem. Phys., 22, 14303–14321, https://doi.org/10.5194/acp-22-14303-2022, https://doi.org/10.5194/acp-22-14303-2022, 2022
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The quasi-biennial oacillation disruption events in both 2016 and 2020 decreased lower-stratospheric water vapour and ozone. Differences in the strength and depth of the anomalous lower-stratospheric circulation and ozone are due to differences in tropical upwelling and cold-point temperature induced by lower-stratospheric planetary and gravity wave breaking. The differences in water vapour are due to higher cold-point temperature in 2020 induced by Australian wildfire.
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.
Paul Konopka, Mengchu Tao, Marc von Hobe, Lars Hoffmann, Corinna Kloss, Fabrizio Ravegnani, C. Michael Volk, Valentin Lauther, Andreas Zahn, Peter Hoor, and Felix Ploeger
Geosci. Model Dev., 15, 7471–7487, https://doi.org/10.5194/gmd-15-7471-2022, https://doi.org/10.5194/gmd-15-7471-2022, 2022
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Pure trajectory-based transport models driven by meteorology derived from reanalysis products (ERA5) take into account only the resolved, advective part of transport. That means neither mixing processes nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS) includes these processes. We show that isentropic mixing dominates unresolved transport. The second most important transport process is unresolved convection.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.9 to 7.8 × 105 cm-3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
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The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Lars Hoffmann, Paul F. Baumeister, Zhongyin Cai, Jan Clemens, Sabine Griessbach, Gebhard Günther, Yi Heng, Mingzhao Liu, Kaveh Haghighi Mood, Olaf Stein, Nicole Thomas, Bärbel Vogel, Xue Wu, and Ling Zou
Geosci. Model Dev., 15, 2731–2762, https://doi.org/10.5194/gmd-15-2731-2022, https://doi.org/10.5194/gmd-15-2731-2022, 2022
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We describe the new version (2.2) of the Lagrangian transport model MPTRAC, which has been ported for application on GPUs. The model was verified by comparing kinematic trajectories and synthetic tracer simulations for the free troposphere and stratosphere from GPUs and CPUs. Benchmarking showed a speed-up of a factor of 16 of GPU-enabled simulations compared to CPU-only runs, indicating the great potential of applying GPUs for Lagrangian transport simulations on upcoming HPC systems.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Piera Raspollini, Enrico Arnone, Flavio Barbara, Massimo Bianchini, Bruno Carli, Simone Ceccherini, Martyn P. Chipperfield, Angelika Dehn, Stefano Della Fera, Bianca Maria Dinelli, Anu Dudhia, Jean-Marie Flaud, Marco Gai, Michael Kiefer, Manuel López-Puertas, David P. Moore, Alessandro Piro, John J. Remedios, Marco Ridolfi, Harjinder Sembhi, Luca Sgheri, and Nicola Zoppetti
Atmos. Meas. Tech., 15, 1871–1901, https://doi.org/10.5194/amt-15-1871-2022, https://doi.org/10.5194/amt-15-1871-2022, 2022
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The MIPAS instrument onboard the ENVISAT satellite provided 10 years of measurements of the atmospheric emission al limb that allow for the retrieval of latitude- and altitude-resolved atmospheric composition. We describe the improvements implemented in the retrieval algorithm used for the full mission reanalysis, which allows for the generation of the global distributions of 21 atmospheric constituents plus temperature with increased accuracy with respect to previously generated data.
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.
Valentin Lauther, Bärbel Vogel, Johannes Wintel, Andrea Rau, Peter Hoor, Vera Bense, Rolf Müller, and C. Michael Volk
Atmos. Chem. Phys., 22, 2049–2077, https://doi.org/10.5194/acp-22-2049-2022, https://doi.org/10.5194/acp-22-2049-2022, 2022
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We show airborne in situ measurements of the very short-lived ozone-depleting substances CH2Cl2 and CHCl3, revealing particularly high concentrations of both species in the lower stratosphere. Back-trajectory calculations and 3D model simulations show that the air masses with high concentrations originated in the Asian boundary layer and were transported via the Asian summer monsoon. We also identify a fast transport pathway into the stratosphere via the North American monsoon and by hurricanes.
Dina Khordakova, Christian Rolf, Jens-Uwe Grooß, Rolf Müller, Paul Konopka, Andreas Wieser, Martina Krämer, and Martin Riese
Atmos. Chem. Phys., 22, 1059–1079, https://doi.org/10.5194/acp-22-1059-2022, https://doi.org/10.5194/acp-22-1059-2022, 2022
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Extreme storms transport humidity from the troposphere to the stratosphere. Here it has a strong impact on the climate. With ongoing global warming, we expect more storms and, hence, an enhancement of this effect. A case study was performed in order to measure the impact of the direct injection of water vapor into the lower stratosphere. The measurements displayed a significant transport of water vapor into the lower stratosphere, and this was supported by satellite and reanalysis data.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Manuel Baumgartner, Christian Rolf, Jens-Uwe Grooß, Julia Schneider, Tobias Schorr, Ottmar Möhler, Peter Spichtinger, and Martina Krämer
Atmos. Chem. Phys., 22, 65–91, https://doi.org/10.5194/acp-22-65-2022, https://doi.org/10.5194/acp-22-65-2022, 2022
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An important mechanism for the appearance of ice particles in the upper troposphere at low temperatures is homogeneous nucleation. This process is commonly described by the
Koop line, predicting the humidity at freezing. However, laboratory measurements suggest that the freezing humidities are above the Koop line, motivating the present study to investigate the influence of different physical parameterizations on the homogeneous freezing with the help of a detailed numerical model.
Sandip S. Dhomse, Carlo Arosio, Wuhu Feng, Alexei Rozanov, Mark Weber, and Martyn P. Chipperfield
Earth Syst. Sci. Data, 13, 5711–5729, https://doi.org/10.5194/essd-13-5711-2021, https://doi.org/10.5194/essd-13-5711-2021, 2021
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High-quality long-term ozone profile data sets are key to estimating short- and long-term ozone variability. Almost all the satellite (and chemical model) data sets show some kind of bias with respect to each other. This is because of differences in measurement methodologies as well as simplified processes in the models. We use satellite data sets and chemical model output to generate 42 years of ozone profile data sets using a random-forest machine-learning algorithm that is named ML-TOMCAT.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
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.
Alistair J. Manning, Alison L. Redington, Daniel Say, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Martin K. Vollmer, Jens Mühle, Jgor Arduini, Gerard Spain, Adam Wisher, Michela Maione, Tanja J. Schuck, Kieran Stanley, Stefan Reimann, Andreas Engel, Paul B. Krummel, Paul J. Fraser, Christina M. Harth, Peter K. Salameh, Ray F. Weiss, Ray Gluckman, Peter N. Brown, John D. Watterson, and Tim Arnold
Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, https://doi.org/10.5194/acp-21-12739-2021, 2021
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This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs)) using high-quality atmospheric observations and atmospheric modelling. We compare these estimates with those submitted by the UK to the United Nations. We conclude that global concentrations of these gases are still increasing. Our estimates for the UK are 73 % of those reported and that the UK emissions are now falling, demonstrating an impact of UK government policy.
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Antonis Dragoneas, Bärbel Vogel, Felix Ploeger, Silvia Viciani, Francesco D'Amato, Silvia Bucci, Bernard Legras, Beiping Luo, and Stephan Borrmann
Atmos. Chem. Phys., 21, 11689–11722, https://doi.org/10.5194/acp-21-11689-2021, https://doi.org/10.5194/acp-21-11689-2021, 2021
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In July and August 2017, eight StratoClim mission flights of the Geophysica reached up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) was identified in situ by abundant nucleation-mode aerosols (6–15 nm in diameter) with mixing ratios of up to 50 000 mg−1. NPF occurred most frequently at 12–16 km with fractions of non-volatile residues of down to 15 %. Abundance and productivity of observed NPF indicate its ability to promote the Asian tropopause aerosol layer.
Thorsten Kaluza, Daniel Kunkel, and Peter Hoor
Weather Clim. Dynam., 2, 631–651, https://doi.org/10.5194/wcd-2-631-2021, https://doi.org/10.5194/wcd-2-631-2021, 2021
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We present a 10-year analysis on the occurrence of strong wind shear in the Northern Hemisphere, focusing on the region around the transport barrier that separates the first two layers of the atmosphere. The major result of our analysis is that strong wind shear above a certain threshold occurs frequently and nearly exclusively in this region, which, as an indicator for turbulent mixing, might have major implications concerning the separation efficiency of the transport barrier.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
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.
Fides Lefrancois, Markus Jesswein, Markus Thoma, Andreas Engel, Kieran Stanley, and Tanja Schuck
Atmos. Meas. Tech., 14, 4669–4687, https://doi.org/10.5194/amt-14-4669-2021, https://doi.org/10.5194/amt-14-4669-2021, 2021
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Synthetic halocarbons can contribute to stratospheric ozone depletion or to climate change. In many applications they have been replaced over the last years. The presented non-target analysis shows an application approach to quantify those replacements retrospectively, using recorded data of air measurements with gas chromatography coupled to time-of-flight mass spectrometry. We focus on the retrospective analysis of the fourth-generation halocarbons, detected at Taunus Observatory in Germany.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412, https://doi.org/10.5194/acp-21-8393-2021, https://doi.org/10.5194/acp-21-8393-2021, 2021
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We investigate the global stratospheric circulation (Brewer–Dobson circulation) in the new ECMWF ERA5 reanalysis based on age of air simulations, and we compare it to results from the preceding ERA-Interim reanalysis. Our results show a slower stratospheric circulation and higher age for ERA5. The age of air trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, related to multi-annual variability and a potential contribution from changes in the reanalysis system.
Thomas Wagenhäuser, Andreas Engel, and Robert Sitals
Atmos. Meas. Tech., 14, 3923–3934, https://doi.org/10.5194/amt-14-3923-2021, https://doi.org/10.5194/amt-14-3923-2021, 2021
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AirCore samplers are increasingly deployed to weather balloons to collect continuous atmospheric samples. We introduce a technique that can be used in situ to evaluate different data processing methods that are required to derive vertical trace gas profiles from AirCore measurements after sample recovery. Results from two test flights with a specific AirCore configuration provide evidence for systematic deviations in altitude attribution for the upper levels, which can be empirically corrected.
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.
Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Jens-Uwe Grooß, Thomas Gulde, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Erik Kretschmer, Guido Maucher, Hans Nordmeyer, Hermann Oelhaf, Johannes Orphal, Christof Piesch, Björn-Martin Sinnhuber, Jörn Ungermann, and Bärbel Vogel
Atmos. Chem. Phys., 21, 8213–8232, https://doi.org/10.5194/acp-21-8213-2021, https://doi.org/10.5194/acp-21-8213-2021, 2021
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Measurements of the pollutants C2H6, C2H2, HCOOH, and PAN were performed in the North Atlantic UTLS region with the airborne limb imager GLORIA in 2017. Enhanced amounts of these species were detected in the upper troposphere and even in the lowermost stratosphere (PAN). Main sources of these gases are forest fires in North America and anthropogenic pollution in South Asia. Simulations of EMAC and CAMS are qualitatively able to reproduce the measured data but underestimate the absolute amounts.
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.
Akash Biswal, Vikas Singh, Shweta Singh, Amit P. Kesarkar, Khaiwal Ravindra, Ranjeet S. Sokhi, Martyn P. Chipperfield, Sandip S. Dhomse, Richard J. Pope, Tanbir Singh, and Suman Mor
Atmos. Chem. Phys., 21, 5235–5251, https://doi.org/10.5194/acp-21-5235-2021, https://doi.org/10.5194/acp-21-5235-2021, 2021
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Satellite and surface observations show a reduction in NO2 levels over India during the lockdown compared to business-as-usual years. A substantial reduction, proportional to the population, was observed over the urban areas. The changes in NO2 levels at the surface during the lockdown appear to be present in the satellite observations. However, TROPOMI showed a better correlation with surface NO2 and was more sensitive to the changes than OMI because of the finer resolution.
Sabine Robrecht, Bärbel Vogel, Simone Tilmes, and Rolf Müller
Atmos. Chem. Phys., 21, 2427–2455, https://doi.org/10.5194/acp-21-2427-2021, https://doi.org/10.5194/acp-21-2427-2021, 2021
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Column ozone protects life on Earth from radiation damage. Stratospheric chlorine compounds cause immense ozone loss in polar winter. Whether similar loss processes can occur in the lower stratosphere above North America today or in future is a matter of debate. We show that these ozone loss processes are very unlikely today or in future independently of whether sulfate geoengineering is applied and that less than 0.1 % of column ozone would be destroyed by this process in any future scenario.
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.
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Short summary
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.
Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses...
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