Articles | Volume 25, issue 7
https://doi.org/10.5194/acp-25-4185-2025
© Author(s) 2025. 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-25-4185-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
14 Apr 2025
Research article |
| 14 Apr 2025
| 14 Apr 2025
Age of air from ACE-FTS measurements of sulfur hexafluoride
Laura N. Saunders
Department of Physics, University of Toronto, Toronto, Canada
Department of Physics, University of Toronto, Toronto, Canada
Gabriele P. Stiller
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Thomas von Clarmann
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
deceased
Florian Haenel
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Hella Garny
Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany
Ludwig Maximilian University of Munich, Meteorological Institute, Munich, Germany
Harald Bönisch
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Chris D. Boone
Department of Chemistry, University of Waterloo, Waterloo, Canada
Ariana E. Castillo
Department of Earth and Planetary Sciences, Harvard University, Cambridge, USA
Andreas Engel
Institute for Atmospheric and Environmental Science, Goethe University Frankfurt, Frankfurt, Germany
Johannes C. Laube
Institute of Climate and Energy Systems, Stratosphere (ICE-4), Forschungszentrum Jülich, Jülich, Germany
Marianna Linz
Department of Earth and Planetary Sciences, Harvard University, Cambridge, USA
School of Engineering and Applied Sciences, Harvard University, Cambridge, USA
Felix Ploeger
Institute of Climate and Energy Systems, Stratosphere (ICE-4), Forschungszentrum Jülich, Jülich, Germany
Institute for Atmospheric and Environmental Research, University of Wuppertal, Wuppertal, Germany
David A. Plummer
Climate Research Division, Environment and Climate Change Canada, Montreal, Canada
Eric A. Ray
Chemical Sciences Division, Earth Systems Research Laboratory, NOAA, Boulder, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, USA
Patrick E. Sheese
Department of Physics, University of Toronto, Toronto, Canada
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Yunqian Zhu, Hideharu Akiyoshi, Valentina Aquila, Elizabeth Asher, Ewa M. Bednarz, Slimane Bekki, Christoph Brühl, Amy H. Butler, Parker Case, Simon Chabrillat, Gabriel Chiodo, Margot Clyne, Peter R. Colarco, Sandip Dhomse, Lola Falletti, Eric Fleming, Ben Johnson, Andrin Jörimann, Mahesh Kovilakam, Gerbrand Koren, Ales Kuchar, Nicolas Lebas, Qing Liang, Cheng-Cheng Liu, Graham Mann, Michael Manyin, Marion Marchand, Olaf Morgenstern, Paul Newman, Luke D. Oman, Freja F. Østerstrøm, Yifeng Peng, David Plummer, Ilaria Quaglia, William Randel, Samuel Rémy, Takashi Sekiya, Stephen Steenrod, Timofei Sukhodolov, Simone Tilmes, Kostas Tsigaridis, Rei Ueyama, Daniele Visioni, Xinyue Wang, Shingo Watanabe, Yousuke Yamashita, Pengfei Yu, Wandi Yu, Jun Zhang, and Zhihong Zhuo
Geosci. Model Dev., 18, 5487–5512, https://doi.org/10.5194/gmd-18-5487-2025, https://doi.org/10.5194/gmd-18-5487-2025, 2025
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To understand the climate impact of the 2022 Hunga volcanic eruption, we developed a climate model–observation comparison project. The paper describes the protocols and models that participate in the experiments. We designed several experiments to achieve our goals of this activity: (1) to evaluate the climate model performance and (2) to understand the Earth system responses to this eruption.
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.
Sarah Vervalcke, Quentin Errera, Simon Chabrillat, Marc Op de beeck, Thomas Reddmann, Gabriele Stiller, Roland Eichinger, and Emmanuel Mahieu
EGUsphere, https://doi.org/10.5194/egusphere-2025-3597, https://doi.org/10.5194/egusphere-2025-3597, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study presents three simulations of atmospheric chemistry with the BASCOE model, driven by different meteorological data sets. These simulations include newly implemented SF6 chemistry, useful for stratospheric transport studies. Results compare well with satellite observations. The lifetime of six trace gases is computed and agrees with the literature, but SF6 shows larger sensitivity to the choice of meteorology. The lifetime of SF6 ranges from 1900 to 2600 years.
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.
Jezabel Curbelo and Marianna Linz
Atmos. Chem. Phys., 25, 7941–7957, https://doi.org/10.5194/acp-25-7941-2025, https://doi.org/10.5194/acp-25-7941-2025, 2025
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Studying stratospheric mixing is crucial for understanding atmospheric dynamics and chemical transport. We propose a new Lagrangian metric based on the density of transport barriers, attracting/repelling coherent structures, to analyze mixing in the Whole Atmosphere Community Climate Model. Our metric is a promising tool for stratospheric analysis, consistent with commonly used metrics to quantify mixing while also providing the advantage of reflecting Lagrangian transport in physical latitude.
Norbert Glatthor, Thomas von Clarmann, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Alexandra Laeng, Andrea Linden, Gabriele P. Stiller, Bernd Funke, Maya Garcia-Comas, Manuel Lopez-Puertas, Oliver Kirner, and Michelle L. Santee
EGUsphere, https://doi.org/10.5194/egusphere-2025-3352, https://doi.org/10.5194/egusphere-2025-3352, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We present a global climatology of MIPAS version 8 chlorine monoxide (ClO), retrieved from spaceborne observations between 2002 and 2012. Due to an improved retrieval setup, the high bias and poor vertical resolution of upper stratospheric ClO, which had affected the previous V5 data set, has been removed. Comparisons with ClO observations of the Microwave Limb Sounder generally show good agreement. Differences can be explained by simulations with an atmospheric chemistry model.
Corinna Kloss, Gwenaël Berthet, Pasquale Sellitto, Irene Bartolome Garcia, Emmanuel Briaud, Rubel Chandra Das, Stéphane Chevrier, Nicolas Dumelié, Lilian Joly, Thomas Lecas, Pauline Marbach, Felix Ploeger, Jean-Baptiste Renard, Jean-Paul Vernier, Frank G. Wienhold, and Michaela I. Hegglin
EGUsphere, https://doi.org/10.5194/egusphere-2025-2091, https://doi.org/10.5194/egusphere-2025-2091, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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In October 2022, we detected volcanic particles in the stratosphere over France, linked to the January 2022 Hunga eruption in the South Pacific. Found between 17 and 23 km altitude, they were traced back to the tropics using trajectory simulations and satellite data. Their optical properties matched those in the Southern Hemisphere. The particles spread across the Northern Hemisphere, reflecting sunlight and slightly cooling the surface—a small but non-negligible effect.
Matthew Wyatt, Peter F. Bernath, Chris Boone, Léo Lavy, and Ryan Johnson
EGUsphere, https://doi.org/10.5194/egusphere-2025-3116, https://doi.org/10.5194/egusphere-2025-3116, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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An improved version (v.5.3) of Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) winds is now available. The wind speeds are determined by use of the Doppler effect. Using a better set of reference molecules to determine the Doppler effect as well as a new method for determining the heading angle (look direction) of the satellite has improved our wind speeds, which has been validated by other instruments. These winds can be used to improve atmospheric models.
Luke M. Western, Stephen Bourguet, Molly Crotwell, Lei Hu, Paul B. Krummel, Hélène De Longueville, Alistair J. Mainning, 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
EGUsphere, https://doi.org/10.5194/egusphere-2025-3000, https://doi.org/10.5194/egusphere-2025-3000, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We used atmospheric measurements to estimate emissions of two gases, called HCFC-123 and HCFC-124, that harm the ozone layer. Despite international regulation to stop their production, we found that 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.
Johannes Degen, Bianca C. Baier, Patrick Jöckel, J. Moritz Menken, Tanja J. Schuck, Colm Sweeney, and Andreas Engel
EGUsphere, https://doi.org/10.5194/egusphere-2025-2648, https://doi.org/10.5194/egusphere-2025-2648, 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.
Simone Tilmes, Ewa M. Bednarz, Andrin Jörimann, Daniele Visioni, Douglas E. Kinnison, Gabriel Chiodo, and David Plummer
Atmos. Chem. Phys., 25, 6001–6023, https://doi.org/10.5194/acp-25-6001-2025, https://doi.org/10.5194/acp-25-6001-2025, 2025
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In this paper, we describe the details of a new multi-model intercomparison experiment to assess the effects of Stratospheric Aerosol Intervention (SAI) on stratospheric chemistry and dynamics and, therefore, ozone. Second, we discuss the advantages and differences of the more constrained experiment compared to fully interactive model experiments. This way, we advance the process-level understanding of the drivers of SAI-induced atmospheric responses.
Pengfei Yu, Yifeng Peng, Karen H. Rosenlof, Ru-Shan Gao, Robert W. Portmann, Martin Ross, Eric Ray, Jianchun Bian, Simone Tilmes, and Owen B. Toon
EGUsphere, https://doi.org/10.5194/egusphere-2025-2312, https://doi.org/10.5194/egusphere-2025-2312, 2025
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Stratospheric aerosol injection (SAI) at 50 km improves climate intervention by reducing global cooling by 22 % and polar cooling by 40 %, preserving Arctic sea ice 20 % more effectively than traditional 25-km SAI. It also reduces Antarctic ozone depletion, shortening recovery delay from 25–55 years to about 5 years. Additionally, SAI at 50 km halves tropical lower stratospheric warming, minimizing disruptions to stratospheric water vapor and jet streams compared to the 25-km method.
Frederik Harzer, Hella Garny, Felix Ploeger, J. Moritz Menken, and Thomas Birner
EGUsphere, https://doi.org/10.5194/egusphere-2025-2195, https://doi.org/10.5194/egusphere-2025-2195, 2025
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We study ozone transport in the extratropical lowermost stratosphere using potential temperature as vertical coordinate, thereby distinguishing adiabatic and diabatic processes. We find that on top of known dominant transport processes (quasi-horizontal mixing, slow diabatic descent) vertical mixing plays an important role near the tropopause. Our findings are relevant for understanding ozone's role in climate including its imprint on tropospheric ozone via stratosphere-troposphere air exchange.
Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, and David A. Plummer
Atmos. Chem. Phys., 25, 5199–5213, https://doi.org/10.5194/acp-25-5199-2025, https://doi.org/10.5194/acp-25-5199-2025, 2025
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Observations from Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) are used to examine global stratospheric water vapour trends for 2004–2021. The satellite measurements are used to quantify trend contributions arising from changes in tropical tropopause temperatures, general circulation patterns, and methane concentrations. While most of the observed trends can be explained by these changes, there remains an unaccounted-for and increasing source of water vapour in the lower mid-stratosphere at mid-latitudes, which is discussed.
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
EGUsphere, https://doi.org/10.5194/egusphere-2025-1838, https://doi.org/10.5194/egusphere-2025-1838, 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.
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
EGUsphere, https://doi.org/10.5194/egusphere-2025-1589, https://doi.org/10.5194/egusphere-2025-1589, 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 the strongest ozone gradients 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.
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.
Zhihong Zhuo, Xinyue Wang, Yunqian Zhu, Ewa M. Bednarz, Eric Fleming, Peter R. Colarco, Shingo Watanabe, David Plummer, Georgiy Stenchikov, William Randel, Adam Bourassa, Valentina Aquila, Takashi Sekiya, Mark R. Schoeberl, Simone Tilmes, Wandi Yu, Jun Zhang, Paul J. Kushner, and Francesco S. R. Pausata
EGUsphere, https://doi.org/10.5194/egusphere-2025-1505, https://doi.org/10.5194/egusphere-2025-1505, 2025
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The 2022 Hunga eruption caused unprecedented stratospheric water injection, triggering unique atmospheric impacts. This study combines observations and model simulations, projecting a stratospheric water vapor anomaly lasting 4–7 years, with significant temperature variations and ozone depletion in the upper atmosphere lasting 7–10 years. These findings offer critical insights into the role of stratospheric water vapor in shaping climate and atmospheric chemistry.
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.
Hazel Vernier, Demilson Quintão, Bruno Biazon, Eduardo Landulfo, Giovanni Souza, V. Amanda Santos, J. S. Fabio Lopes, C. P. Alex Mendes, A. S. José da Matta, K. Pinheiro Damaris, Benoit Grosslin, P. M. P. Maria Jorge, Maria de Fátima Andrade, Neeraj Rastogi, Akhil Raj, Hongyu Liu, Mahesh Kovilakam, Suvarna Fadnavis, Frank G. Wienhold, Mathieu Colombier, D. Chris Boone, Gwenael Berthet, Nicolas Dumelie, Lilian Joly, and Jean-Paul Vernier
EGUsphere, https://doi.org/10.5194/egusphere-2025-924, https://doi.org/10.5194/egusphere-2025-924, 2025
Preprint withdrawn
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The eruption of Hunga Tonga-Hunga Ha'apai injected large amounts of water vapor and sea salt into the stratosphere, altering traditional views of volcanic aerosols. Using balloon-borne samplers, we collected aerosol samples and found high levels of sea salt and calcium, suggesting sulfate depletion due to gypsum formation. These findings highlight the need to consider sea salt in climate models to better predict volcanic impacts on the atmosphere and climate.
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.
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
EGUsphere, https://doi.org/10.5194/egusphere-2025-1155, https://doi.org/10.5194/egusphere-2025-1155, 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.
Louis Rivoire, Marianna Linz, Jessica L. Neu, Pu Lin, and Michelle L. Santee
Atmos. Chem. Phys., 25, 2269–2289, https://doi.org/10.5194/acp-25-2269-2025, https://doi.org/10.5194/acp-25-2269-2025, 2025
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The recovery of the ozone hole since the 1987 Montreal Protocol has been observed in some regions but has yet to be seen globally. We ask how long it will take to witness a global recovery. Using a technique akin to flying a virtual satellite in a climate model, we find that the degree of confidence we place in the answer to this question is dramatically affected by errors in satellite observations.
Paul S. Jeffery, James R. Drummond, C. Thomas McElroy, Kaley A. Walker, and Jiansheng Zou
Atmos. Meas. Tech., 18, 569–602, https://doi.org/10.5194/amt-18-569-2025, https://doi.org/10.5194/amt-18-569-2025, 2025
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The MAESTRO instrument has been monitoring ozone and NO2 since February 2004. A new version of these data products has recently been released; however, these new products must be validated against other datasets to ensure their validity. This study presents such an assessment, using measurements from 11 satellite instruments to characterize the new MAESTRO products. In the stratosphere, good agreement is found for ozone and acceptable agreement is found for NO2 with these other datasets.
Kimberlee Dubé, Susann Tegtmeier, Felix Ploeger, and Kaley A. Walker
Atmos. Chem. Phys., 25, 1433–1447, https://doi.org/10.5194/acp-25-1433-2025, https://doi.org/10.5194/acp-25-1433-2025, 2025
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The transport rate of air in the stratosphere has changed in response to human emissions of greenhouse gases and ozone-depleting substances. This transport rate can be approximated using measurements of long-lived trace gases. We use observations and model results to derive anomalies and trends in the mean rate of stratospheric air transport. We find that air in the Northern Hemisphere aged by up to 0.3 years per decade relative to air in the Southern Hemisphere over 2004–2017.
Xiaolu Yan, Paul Konopka, Felix Ploeger, and Aurélien Podglajen
Atmos. Chem. Phys., 25, 1289–1305, https://doi.org/10.5194/acp-25-1289-2025, https://doi.org/10.5194/acp-25-1289-2025, 2025
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Our study finds that the air mass fractions (AMFs) from the Asian boundary layer (ABL) to the polar regions are about 1.5 times larger than those from the same latitude band in the Southern Hemisphere. The transport of AMFs from the ABL to the polar vortex primarily occurs above 20 km and over timescales exceeding 2 years. Our analysis reveals a strong correlation between the polar pollutants and the AMFs from the ABL. About 20 % of SF6 in the polar stratosphere originates from the ABL.
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.
Norbert Glatthor, Gabriele P. Stiller, Thomas von Clarmann, Bernd Funke, Sylvia Kellmann, and Andrea Linden
Atmos. Chem. Phys., 25, 1175–1208, https://doi.org/10.5194/acp-25-1175-2025, https://doi.org/10.5194/acp-25-1175-2025, 2025
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We present global upper-tropospheric distributions of the pollutants HCN, CO, C2H2, C2H6, PAN, and HCOOH, observed between 2002 and 2012 by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the Environmental Satellite (Envisat). By comparing the spatial distributions of their volume mixing ratios and by global correlation and regression analyses, we draw conclusions on their sources, such as biomass burning, anthropogenic sources, and biogenic release.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-3969, https://doi.org/10.5194/egusphere-2024-3969, 2025
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IAGOS-CARIBIC operates an instrumented container laboratory on commercial regular passenger flights to obtain a long-term representative data set on the composition of the upper troposphere and lowermost stratosphere. Here we report on the development on 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 first in-flight data.
Rasul Baikhadzhaev, Felix Ploeger, Peter Preusse, Manfred Ern, and Thomas Birner
EGUsphere, https://doi.org/10.5194/egusphere-2024-4088, https://doi.org/10.5194/egusphere-2024-4088, 2025
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Across four reanalyses, shallow branch of the stratospheric overturning circulation was found to be driven by the largest waves with wavenumbers 1 to 3, and deep branch of the circulation was found to be driven by smaller-scale waves. Yet, the height of the level separating the branches is depended on the reanalysis considered. Thus using the appropriate separation levels in model inter-comparisons could reduce the spread between models regarding climatology and trends in the circulation.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Jiansheng Zou, Kaley A. Walker, Patrick E. Sheese, Chris D. Boone, Ryan M. Stauffer, Anne M. Thompson, and David W. Tarasick
Atmos. Meas. Tech., 17, 6983–7005, https://doi.org/10.5194/amt-17-6983-2024, https://doi.org/10.5194/amt-17-6983-2024, 2024
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Ozone measurements from the ACE-FTS satellite instrument have been compared to worldwide balloon-borne ozonesonde profiles using pairs of closely spaced profiles and monthly averaged profiles. ACE-FTS typically measures more ozone in the stratosphere by up to 10 %. The long-term stability of the ACE-FTS ozone data is good, exhibiting small (but non-significant) drifts of less than 3 % per decade in the stratosphere. Lower in the profiles, the calculated drifts are larger (up to 10 % per decade).
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.
Hongyue Wang, Mijeong Park, Mengchu Tao, Cristina Peña-Ortiz, Nuria Pilar Plaza, Felix Ploeger, and Paul Konopka
EGUsphere, https://doi.org/10.5194/egusphere-2024-3260, https://doi.org/10.5194/egusphere-2024-3260, 2024
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We investigated how stratospheric water vapor behaves over the Asian and North American monsoons. Using a method that tracks air movement, we recreated the moisture patterns. Our results show that the moisture in monsoon regions is primarily controlled by largescale air temperatures, while the North American monsoon is influenced by distant transport. These findings enhance our understanding of summertime stratospheric water vapor changes and offer insights into climate feedback mechanisms.
Eric A. Ray, Fred L. Moore, Hella Garny, Eric J. Hintsa, Bradley D. Hall, Geoff S. Dutton, David Nance, James W. Elkins, Steven C. Wofsy, Jasna Pittman, Bruce Daube, Bianca C. Baier, Jianghanyang Li, and Colm Sweeney
Atmos. Chem. Phys., 24, 12425–12445, https://doi.org/10.5194/acp-24-12425-2024, https://doi.org/10.5194/acp-24-12425-2024, 2024
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In this study we describe new techniques to derive age of air from multiple simultaneous measurements of long-lived trace gases in order to improve the fidelity of the age-of-air estimates and to be able to compare age of air from measurements taken from different instruments, platforms and decades. This technique also allows new transport information to be obtained from the measurements such as the primary source latitude that can also be compared to models.
Sujan Khanal, Matthew Toohey, Adam Bourassa, C. Thomas McElroy, Christopher Sioris, and Kaley A. Walker
EGUsphere, https://doi.org/10.5194/egusphere-2024-3286, https://doi.org/10.5194/egusphere-2024-3286, 2024
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Measurements of stratospheric aerosol from the MAESTRO instrument are compared to other measurements to assess their scientific value. We find that medians of MAESTRO measurements binned by month and latitude show reasonable correlation with other data sets, with notable increases after volcanic eruptions, and that biases in the data can be alleviated through a simple correction technique. Used with care, MAESTRO aerosol measurements provide information that can complement other data sets.
Selena Zhang, Susan Solomon, Chris D. Boone, and Ghassan Taha
Atmos. Chem. Phys., 24, 11727–11736, https://doi.org/10.5194/acp-24-11727-2024, https://doi.org/10.5194/acp-24-11727-2024, 2024
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This paper investigates the vertical impacts of the anomalous 2023 Canadian wildfire season using multiple satellite instruments. Our results highlight that despite a record-breaking area burned, only a small amount of smoke managed to enter the stratosphere. This shows that the conditions for deep convection were rarely met in the 2023 wildfire season, suggesting that even a massive area burned is not necessarily an indicator of stratospheric perturbations.
Cynthia Whaley, Montana Etten-Bohm, Courtney Schumacher, Ayodeji Akingunola, Vivek Arora, Jason Cole, Michael Lazare, David Plummer, Knut von Salzen, and Barbara Winter
Geosci. Model Dev., 17, 7141–7155, https://doi.org/10.5194/gmd-17-7141-2024, https://doi.org/10.5194/gmd-17-7141-2024, 2024
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This paper describes how lightning was added as a process in the Canadian Earth System Model in order to interactively respond to climate changes. As lightning is an important cause of global wildfires, this new model development allows for more realistic projections of how wildfires may change in the future, responding to a changing climate.
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.
Karen De Los Ríos, Paulina Ordoñez, Gabriele P. Stiller, Piera Raspollini, Marco Gai, Kaley A. Walker, Cristina Peña-Ortiz, and Luis Acosta
Atmos. Meas. Tech., 17, 3401–3418, https://doi.org/10.5194/amt-17-3401-2024, https://doi.org/10.5194/amt-17-3401-2024, 2024
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This study examines newer versions of H2O and HDO retrievals from Envisat/MIPAS and SCISAT/ACE-FTS. Results reveal a better agreement in stratospheric H2O profiles than in HDO profiles. The H2O tape recorder signal is consistent across databases, but δD tape recorder composites show differences that impact the interpretation of water vapour transport. These findings enhance the need for intercomparisons to refine our insights.
Xin Yang, Kimberly Strong, Alison S. Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley A. Walker, Sara M. Morris, and Peter Effertz
Atmos. Chem. Phys., 24, 5863–5886, https://doi.org/10.5194/acp-24-5863-2024, https://doi.org/10.5194/acp-24-5863-2024, 2024
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This study uses snow samples collected from a Canadian high Arctic site, Eureka, to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. Surface snow bromide and nitrate are significantly correlated, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. In addition, we show evidence that snow photochemical release of reactive bromine is very weak, and its emission flux is much smaller than the deposition flux of bromide.
Norbert Glatthor, Thomas von Clarmann, Bernd Funke, Maya García-Comas, Udo Grabowski, Michael Höpfner, Sylvia Kellmann, Michael Kiefer, Alexandra Laeng, Andrea Linden, Manuel López-Puertas, and Gabriele P. Stiller
Atmos. Meas. Tech., 17, 2849–2871, https://doi.org/10.5194/amt-17-2849-2024, https://doi.org/10.5194/amt-17-2849-2024, 2024
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We present global atmospheric methane (CH4) and nitrous oxide (N2O) distributions retrieved from measurements of the MIPAS instrument on board the Environmental Satellite (Envisat) during 2002 to 2012. Monitoring of these gases is of scientific interest because both of them are strong greenhouse gases. We analyze the latest, improved version of calibrated MIPAS measurements. Further, we apply a new retrieval scheme leading to an improved CH4 and N2O data product .
Cristina Peña-Ortiz, Nuria Pilar Plaza, David Gallego, and Felix Ploeger
Atmos. Chem. Phys., 24, 5457–5478, https://doi.org/10.5194/acp-24-5457-2024, https://doi.org/10.5194/acp-24-5457-2024, 2024
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Although water vapour (H2O) in the lower stratosphere is only a few molecules among 1 million air molecules, atmospheric radiative forcing and surface temperature are sensitive to changes in its concentration. Monsoon regions play a key role in H2O transport and its concentration in the lower stratosphere. We show how the quasi-biennial oscillation (QBO) has a major impact on H2O over the Asian monsoon during August through changes in temperature caused by QBO modulation of tropical clouds.
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.
Hella Garny, Roland Eichinger, Johannes C. Laube, Eric A. Ray, Gabriele P. Stiller, Harald Bönisch, Laura Saunders, and Marianna Linz
Atmos. Chem. Phys., 24, 4193–4215, https://doi.org/10.5194/acp-24-4193-2024, https://doi.org/10.5194/acp-24-4193-2024, 2024
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Transport circulation in the stratosphere is important for the distribution of tracers, but its strength is hard to measure. Mean transport times can be inferred from observations of trace gases with certain properties, such as sulfur hexafluoride (SF6). However, this gas has a chemical sink in the high atmosphere, which can lead to substantial biases in inferred transport times. In this paper we present a method to correct mean transport times derived from SF6 for the effects of chemical sinks.
Paul S. Jeffery, James R. Drummond, Jiansheng Zou, and Kaley A. Walker
Atmos. Chem. Phys., 24, 4253–4263, https://doi.org/10.5194/acp-24-4253-2024, https://doi.org/10.5194/acp-24-4253-2024, 2024
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The MOPITT instrument has been monitoring carbon monoxide (CO) since March 2000. This dataset has been used for many applications; however, episodic emission events, which release large amounts of CO into the atmosphere, are a major source of uncertainty. This study presents a method for identifying these events by determining measurements that are unlikely to have typically arisen. The distribution and frequency of these flagged measurements in the MOPITT dataset are presented and discussed.
Gabriele P. Stiller, Thomas von Clarmann, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Alexandra Laeng, Andrea Linden, Bernd Funke, Maya García-Comas, and Manuel López-Puertas
Atmos. Meas. Tech., 17, 1759–1789, https://doi.org/10.5194/amt-17-1759-2024, https://doi.org/10.5194/amt-17-1759-2024, 2024
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CFC-11, CFC-12, and HCFC-22 contribute to the depletion of ozone and are potent greenhouse gases. They have been banned by the Montreal protocol. With MIPAS on Envisat the atmospheric composition could be observed between 2002 and 2012. We present here the retrieval of their atmospheric distributions for the final data version 8. We characterise the derived data by their error budget and their spatial resolution. An additional representation for direct comparison to models is also provided.
Felix Ploeger, Thomas Birner, Edward Charlesworth, Paul Konopka, and Rolf Müller
Atmos. Chem. Phys., 24, 2033–2043, https://doi.org/10.5194/acp-24-2033-2024, https://doi.org/10.5194/acp-24-2033-2024, 2024
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We present a novel mechanism of how regional anomalies in water vapour concentrations in the upper troposphere and lower stratosphere impact regional atmospheric circulation systems. These impacts include a displaced upper-level Asian monsoon circulation and strengthened prevailing westerlies in the Pacific region. Current climate models have biases in simulating these regional water vapour anomalies and circulation impacts, but the biases can be avoided by improving the model transport.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
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During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models generally underpredict the concentrations of these gases in the Arctic troposphere.
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.
Manuel López-Puertas, Maya García-Comas, Bernd Funke, Thomas von Clarmann, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Alexandra Laeng, Andrea Linden, and Gabriele P. Stiller
Atmos. Meas. Tech., 16, 5609–5645, https://doi.org/10.5194/amt-16-5609-2023, https://doi.org/10.5194/amt-16-5609-2023, 2023
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This paper describes a new version (V8) of ozone data from MIPAS middle-atmosphere spectra. The dataset comprises high-quality ozone profiles from 20 to 100 km, with pole-to-pole latitude coverage for the day- and nighttime, spanning 2005 until 2012. An exhaustive treatment of errors has been performed. Compared to other satellite instruments, MIPAS ozone shows a positive bias of 5 %–8 % below 70 km. In the upper mesosphere, this new version agrees much better than previous ones (within 10 %).
Maya García-Comas, Bernd Funke, Manuel López-Puertas, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Belén Martínez-Mondéjar, Gabriele P. Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 16, 5357–5386, https://doi.org/10.5194/amt-16-5357-2023, https://doi.org/10.5194/amt-16-5357-2023, 2023
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We have released version 8 of MIPAS IMK–IAA temperatures and pointing information retrieved from MIPAS Middle and Upper Atmosphere mode version 8.03 calibrated spectra, covering 20–115 km altitude. We considered non-local thermodynamic equilibrium emission explicitly for each limb scan, essential to retrieve accurate temperatures above the mid-mesosphere. Comparisons of this temperature dataset with SABER measurements show excellent agreement, improving those of previous MIPAS versions.
Kimberlee Dubé, Susann Tegtmeier, Adam Bourassa, Daniel Zawada, Douglas Degenstein, Patrick E. Sheese, Kaley A. Walker, and William Randel
Atmos. Chem. Phys., 23, 13283–13300, https://doi.org/10.5194/acp-23-13283-2023, https://doi.org/10.5194/acp-23-13283-2023, 2023
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This paper presents a technique for understanding the causes of long-term changes in stratospheric composition. By using N2O as a proxy for stratospheric circulation in the model used to calculated trends, it is possible to separate the effects of dynamics and chemistry on observed trace gas trends. We find that observed HCl increases are due to changes in the stratospheric circulation, as are O3 decreases above 30 hPa in the Northern Hemisphere.
Monali Borthakur, Miriam Sinnhuber, Alexandra Laeng, Thomas Reddmann, Peter Braesicke, Gabriele Stiller, Thomas von Clarmann, Bernd Funke, Ilya Usoskin, Jan Maik Wissing, and Olesya Yakovchuk
Atmos. Chem. Phys., 23, 12985–13013, https://doi.org/10.5194/acp-23-12985-2023, https://doi.org/10.5194/acp-23-12985-2023, 2023
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Reduced ozone levels resulting from ozone depletion mean more exposure to UV radiation, which has various effects on human health. We analysed solar events to see what influence it has on the chemistry of Earth's atmosphere and how this atmospheric chemistry change can affect the ozone. To do this, we used an atmospheric model considering only chemistry and compared it with satellite data. The focus was mainly on the contribution of chlorine, and we found about 10 %–20 % ozone loss due to that.
Paul Konopka, Christian Rolf, Marc von Hobe, Sergey M. Khaykin, Benjamin Clouser, Elisabeth Moyer, Fabrizio Ravegnani, Francesco D'Amato, Silvia Viciani, Nicole Spelten, Armin Afchine, Martina Krämer, Fred Stroh, and Felix Ploeger
Atmos. Chem. Phys., 23, 12935–12947, https://doi.org/10.5194/acp-23-12935-2023, https://doi.org/10.5194/acp-23-12935-2023, 2023
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We studied water vapor in a critical region of the atmosphere, the Asian summer monsoon anticyclone, using rare in situ observations. Our study shows that extremely high water vapor values observed in the stratosphere within the Asian monsoon anticyclone still undergo significant freeze-drying and that water vapor concentrations set by the Lagrangian dry point are a better proxy for the stratospheric water vapor budget than rare observations of enhanced water mixing ratios.
Michael Kiefer, Dale F. Hurst, Gabriele P. Stiller, Stefan Lossow, Holger Vömel, John Anderson, Faiza Azam, Jean-Loup Bertaux, Laurent Blanot, Klaus Bramstedt, John P. Burrows, Robert Damadeo, Bianca Maria Dinelli, Patrick Eriksson, Maya García-Comas, John C. Gille, Mark Hervig, Yasuko Kasai, Farahnaz Khosrawi, Donal Murtagh, Gerald E. Nedoluha, Stefan Noël, Piera Raspollini, William G. Read, Karen H. Rosenlof, Alexei Rozanov, Christopher E. Sioris, Takafumi Sugita, Thomas von Clarmann, Kaley A. Walker, and Katja Weigel
Atmos. Meas. Tech., 16, 4589–4642, https://doi.org/10.5194/amt-16-4589-2023, https://doi.org/10.5194/amt-16-4589-2023, 2023
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We quantify biases and drifts (and their uncertainties) between the stratospheric water vapor measurement records of 15 satellite-based instruments (SATs, with 31 different retrievals) and balloon-borne frost point hygrometers (FPs) launched at 27 globally distributed stations. These comparisons of measurements during the period 2000–2016 are made using robust, consistent statistical methods. With some exceptions, the biases and drifts determined for most SAT–FP pairs are < 10 % and < 1 % yr−1.
Roland Eichinger, Sebastian Rhode, Hella Garny, Peter Preusse, Petr Pisoft, Aleš Kuchař, Patrick Jöckel, Astrid Kerkweg, and Bastian Kern
Geosci. Model Dev., 16, 5561–5583, https://doi.org/10.5194/gmd-16-5561-2023, https://doi.org/10.5194/gmd-16-5561-2023, 2023
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The columnar approach of gravity wave (GW) schemes results in dynamical model biases, but parallel decomposition makes horizontal GW propagation computationally unfeasible. In the global model EMAC, we approximate it by GW redistribution at one altitude using tailor-made redistribution maps generated with a ray tracer. More spread-out GW drag helps reconcile the model with observations and close the 60°S GW gap. Polar vortex dynamics are improved, enhancing climate model credibility.
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.
Jason Neil Steven Cole, Knut von Salzen, Jiangnan Li, John Scinocca, David Plummer, Vivek Arora, Norman McFarlane, Michael Lazare, Murray MacKay, and Diana Verseghy
Geosci. Model Dev., 16, 5427–5448, https://doi.org/10.5194/gmd-16-5427-2023, https://doi.org/10.5194/gmd-16-5427-2023, 2023
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The Canadian Atmospheric Model version 5 (CanAM5) is used to simulate on a global scale the climate of Earth's atmosphere, land, and lakes. We document changes to the physics in CanAM5 since the last major version of the model (CanAM4) and evaluate the climate simulated relative to observations and CanAM4. The climate simulated by CanAM5 is similar to CanAM4, but there are improvements, including better simulation of temperature and precipitation over the Amazon and better simulation of cloud.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Stephen Bourguet and Marianna Linz
Atmos. Chem. Phys., 23, 7447–7460, https://doi.org/10.5194/acp-23-7447-2023, https://doi.org/10.5194/acp-23-7447-2023, 2023
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Here, we show how projected changes to tropical circulation will impact the water vapor concentration in the lower stratosphere, which has implications for surface climate and stratospheric chemistry. In our transport scenarios with slower east–west winds, air parcels ascending into the stratosphere do not experience the same cold temperatures that they would today. This effect could act in concert with previously modeled changes to stratospheric water vapor to amplify surface warming.
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.
Bernd Funke, Maya García-Comas, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Manuel López-Puertas, Gabriele P. Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 16, 2167–2196, https://doi.org/10.5194/amt-16-2167-2023, https://doi.org/10.5194/amt-16-2167-2023, 2023
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New global nitric oxide (NO) volume-mixing-ratio and lower-thermospheric temperature data products, retrieved from Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) spectra with the IMK-IAA MIPAS data processor, have been released. The dataset covers the entire Envisat mission lifetime and includes retrieval results from all MIPAS observation modes. The data are based on ESA version 8 calibration and were processed using an improved retrieval approach.
Viktoria F. Sofieva, Monika Szelag, Johanna Tamminen, Carlo Arosio, Alexei Rozanov, Mark Weber, Doug Degenstein, Adam Bourassa, Daniel Zawada, Michael Kiefer, Alexandra Laeng, Kaley A. Walker, Patrick Sheese, Daan Hubert, Michel van Roozendael, Christian Retscher, Robert Damadeo, and Jerry D. Lumpe
Atmos. Meas. Tech., 16, 1881–1899, https://doi.org/10.5194/amt-16-1881-2023, https://doi.org/10.5194/amt-16-1881-2023, 2023
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The paper presents the updated SAGE-CCI-OMPS+ climate data record of monthly zonal mean ozone profiles. This dataset covers the stratosphere and combines measurements by nine limb and occultation satellite instruments (SAGE II, OSIRIS, MIPAS, SCIAMACHY, GOMOS, ACE-FTS, OMPS-LP, POAM III, and SAGE III/ISS). The update includes new versions of MIPAS, ACE-FTS, and OSIRIS datasets and introduces data from additional sensors (POAM III and SAGE III/ISS) and retrieval processors (OMPS-LP).
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.
Michael Kiefer, Thomas von Clarmann, Bernd Funke, Maya García-Comas, Norbert Glatthor, Udo Grabowski, Michael Höpfner, Sylvia Kellmann, Alexandra Laeng, Andrea Linden, Manuel López-Puertas, and Gabriele P. Stiller
Atmos. Meas. Tech., 16, 1443–1460, https://doi.org/10.5194/amt-16-1443-2023, https://doi.org/10.5194/amt-16-1443-2023, 2023
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A new ozone data set, derived from radiation measurements of the space-borne instrument MIPAS, is presented. It consists of more than 2 million single ozone profiles from 2002–2012, covering virtually all latitudes and altitudes between 5 and 70 km. Progress in data calibration and processing methods allowed for significant improvement of the data quality, compared to previous data versions. Hence, the data set will help to better understand e.g. the time evolution of ozone in the stratosphere.
Sean M. Davis, Nicholas Davis, Robert W. Portmann, Eric Ray, and Karen Rosenlof
Atmos. Chem. Phys., 23, 3347–3361, https://doi.org/10.5194/acp-23-3347-2023, https://doi.org/10.5194/acp-23-3347-2023, 2023
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Ozone in the lower part of the stratosphere has not increased and has perhaps even continued to decline in recent decades. This study demonstrates that the amount of ozone in this region is highly sensitive to the amount of air upwelling into the stratosphere in the tropics and that simulations from a climate model nudged to historical meteorological fields often fail to accurately capture the variations in tropical upwelling that control short-term trends in lower-stratospheric ozone.
Nasrin Mostafavi Pak, Jacob K. Hedelius, Sébastien Roche, Liz Cunningham, Bianca Baier, Colm Sweeney, Coleen Roehl, Joshua Laughner, Geoffrey Toon, Paul Wennberg, Harrison Parker, Colin Arrowsmith, Joseph Mendonca, Pierre Fogal, Tyler Wizenberg, Beatriz Herrera, Kimberly Strong, Kaley A. Walker, Felix Vogel, and Debra Wunch
Atmos. Meas. Tech., 16, 1239–1261, https://doi.org/10.5194/amt-16-1239-2023, https://doi.org/10.5194/amt-16-1239-2023, 2023
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Ground-based remote sensing instruments in the Total Carbon Column Observing Network (TCCON) measure greenhouse gases in the atmosphere. Consistency between TCCON measurements is crucial to accurately infer changes in atmospheric composition. We use portable remote sensing instruments (EM27/SUN) to evaluate biases between TCCON stations in North America. We also improve the retrievals of EM27/SUN instruments and evaluate the previous (GGG2014) and newest (GGG2020) retrieval algorithms.
Joshua L. Laughner, Sébastien Roche, Matthäus Kiel, Geoffrey C. Toon, Debra Wunch, Bianca C. Baier, Sébastien Biraud, Huilin Chen, Rigel Kivi, Thomas Laemmel, Kathryn McKain, Pierre-Yves Quéhé, Constantina Rousogenous, Britton B. Stephens, Kaley Walker, and Paul O. Wennberg
Atmos. Meas. Tech., 16, 1121–1146, https://doi.org/10.5194/amt-16-1121-2023, https://doi.org/10.5194/amt-16-1121-2023, 2023
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Observations using sunlight to measure surface-to-space total column of greenhouse gases in the atmosphere need an initial guess of the vertical distribution of those gases to start from. We have developed an approach to provide those initial guess profiles that uses readily available meteorological data as input. This lets us make these guesses without simulating them with a global model. The profiles generated this way match independent observations well.
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.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Matthias Nützel, Sabine Brinkop, Martin Dameris, Hella Garny, Patrick Jöckel, Laura L. Pan, and Mijeong Park
Atmos. Chem. Phys., 22, 15659–15683, https://doi.org/10.5194/acp-22-15659-2022, https://doi.org/10.5194/acp-22-15659-2022, 2022
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During the Asian summer monsoon season, a large high-pressure system is present at levels close to the tropopause above Asia. We analyse how air masses are transported from surface levels to this high-pressure system, which shows distinct features from the surrounding air masses. To this end, we employ multiannual data from two complementary models that allow us to analyse the climatology as well as the interannual and intraseasonal variability of these transport pathways.
Thomas von Clarmann, Norbert Glatthor, Udo Grabowski, Bernd Funke, Michael Kiefer, Anne Kleinert, Gabriele P. Stiller, Andrea Linden, and Sylvia Kellmann
Atmos. Meas. Tech., 15, 6991–7018, https://doi.org/10.5194/amt-15-6991-2022, https://doi.org/10.5194/amt-15-6991-2022, 2022
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Errors of profiles of temperature and mixing ratios retrieved from spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding are estimated. All known and quantified sources of uncertainty are considered. Some ongoing uncertaities contribute to both the random and to the systematic errors. In some cases, one source of uncertainty propagates onto the error budget via multiple pathways. Problems arise when the correlations of errors to be propagated are unknown.
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.
Ali Jalali, Kaley A. Walker, Kimberly Strong, Rebecca R. Buchholz, Merritt N. Deeter, Debra Wunch, Sébastien Roche, Tyler Wizenberg, Erik Lutsch, Erin McGee, Helen M. Worden, Pierre Fogal, and James R. Drummond
Atmos. Meas. Tech., 15, 6837–6863, https://doi.org/10.5194/amt-15-6837-2022, https://doi.org/10.5194/amt-15-6837-2022, 2022
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This study validates MOPITT version 8 carbon monoxide measurements over the Canadian high Arctic for the period 2006 to 2019. The MOPITT products from different detector pixels and channels are compared with ground-based measurements from the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut, Canada. These results show good consistency between the satellite and ground-based measurements and provide guidance on the usage of these MOPITT data at high latitudes.
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.
Paul S. Jeffery, Kaley A. Walker, Chris E. Sioris, Chris D. Boone, Doug Degenstein, Gloria L. Manney, C. Thomas McElroy, Luis Millán, David A. Plummer, Niall J. Ryan, Patrick E. Sheese, and Jiansheng Zou
Atmos. Chem. Phys., 22, 14709–14734, https://doi.org/10.5194/acp-22-14709-2022, https://doi.org/10.5194/acp-22-14709-2022, 2022
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The upper troposphere–lower stratosphere is one of the most variable regions in the atmosphere. To improve our understanding of water vapour and ozone concentrations in this region, climatologies have been developed from 14 years of measurements from three Canadian satellite instruments. Horizontal and vertical coordinates have been chosen to minimize the effects of variability. To aid in analysis, model simulations have been used to characterize differences between instrument climatologies.
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.
Kimberlee Dubé, Daniel Zawada, Adam Bourassa, Doug Degenstein, William Randel, David Flittner, Patrick Sheese, and Kaley Walker
Atmos. Meas. Tech., 15, 6163–6180, https://doi.org/10.5194/amt-15-6163-2022, https://doi.org/10.5194/amt-15-6163-2022, 2022
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Satellite observations are important for monitoring changes in atmospheric composition. Here we describe an improved version of the NO2 retrieval for the Optical Spectrograph and InfraRed Imager System. The resulting NO2 profiles are compared to those from the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer and the Stratospheric Aerosol and Gas Experiment III on the International Space Station. All datasets agree within 20 % throughout the stratosphere.
Stephen Bourguet and Marianna Linz
Atmos. Chem. Phys., 22, 13325–13339, https://doi.org/10.5194/acp-22-13325-2022, https://doi.org/10.5194/acp-22-13325-2022, 2022
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Here, we tested the impact of spatial and temporal resolution on Lagrangian trajectory studies in a key region of interest for climate feedbacks and stratospheric chemistry. Our analysis shows that new higher-resolution input data provide an opportunity for a better understanding of physical processes that control how air moves from the troposphere to the stratosphere. Future studies of how these processes will change in a warming climate will benefit from these results.
Xin Yang, Kimberly Strong, Alison S. Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley A. Walker, Sara M. Morris, and Peter Effertz
EGUsphere, https://doi.org/10.5194/egusphere-2022-696, https://doi.org/10.5194/egusphere-2022-696, 2022
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Snow pack in high Arctic plays a key role in polar atmospheric chemistry, especially in spring when photochemistry becomes active. By sampling surface snow from a Canadian high Arctic location at Eureka, Nunavut (80° N, 86° W), we demonstrate that surface snow is a net sink rather than a source of atmospheric reactive bromine and nitrate. This finding is new and opposite to previous conclusions that snowpack is a large and direct source of reactive bromine in polar spring.
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.
Liubov Poshyvailo-Strube, Rolf Müller, Stephan Fueglistaler, Michaela I. Hegglin, Johannes C. Laube, C. Michael Volk, and Felix Ploeger
Atmos. Chem. Phys., 22, 9895–9914, https://doi.org/10.5194/acp-22-9895-2022, https://doi.org/10.5194/acp-22-9895-2022, 2022
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Brewer–Dobson circulation (BDC) controls the composition of the stratosphere, which in turn affects radiation and climate. As the BDC cannot be measured directly, it is necessary to infer its strength and trends indirectly. In this study, we test in the
model worlddifferent methods for estimating the mean age of air trends based on a combination of stratospheric water vapour and methane data. We also provide simple practical advice of a more reliable estimation of the mean age of air trends.
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.
William G. Read, Gabriele Stiller, Stefan Lossow, Michael Kiefer, Farahnaz Khosrawi, Dale Hurst, Holger Vömel, Karen Rosenlof, Bianca M. Dinelli, Piera Raspollini, Gerald E. Nedoluha, John C. Gille, Yasuko Kasai, Patrick Eriksson, Christopher E. Sioris, Kaley A. Walker, Katja Weigel, John P. Burrows, and Alexei Rozanov
Atmos. Meas. Tech., 15, 3377–3400, https://doi.org/10.5194/amt-15-3377-2022, https://doi.org/10.5194/amt-15-3377-2022, 2022
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This paper attempts to provide an assessment of the accuracy of 21 satellite-based instruments that remotely measure atmospheric humidity in the upper troposphere of the Earth's atmosphere. The instruments made their measurements from 1984 to the present time; however, most of these instruments began operations after 2000, and only a few are still operational. The objective of this study is to quantify the accuracy of each satellite humidity data set.
Suvarna Fadnavis, Prashant Chavan, Akash Joshi, Sunil M. Sonbawne, Asutosh Acharya, Panuganti C. S. Devara, Alexandru Rap, Felix Ploeger, and Rolf Müller
Atmos. Chem. Phys., 22, 7179–7191, https://doi.org/10.5194/acp-22-7179-2022, https://doi.org/10.5194/acp-22-7179-2022, 2022
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We show that large amounts of anthropogenic aerosols are transported from South Asia to the northern Indian Ocean. These aerosols are then lifted into the UTLS by the ascending branch of the Hadley circulation. They are further transported to the Southern Hemisphere and downward via westerly ducts over the tropical Atlantic and Pacific. These aerosols increase tropospheric heating, resulting in an increase in water vapor, which is then transported to the UTLS.
Eric A. Ray, Elliot L. Atlas, Sue Schauffler, Sofia Chelpon, Laura Pan, Harald Bönisch, and Karen H. Rosenlof
Atmos. Chem. Phys., 22, 6539–6558, https://doi.org/10.5194/acp-22-6539-2022, https://doi.org/10.5194/acp-22-6539-2022, 2022
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The movement of air masses and the trace gases they contain from the Earth’s surface into the upper troposphere and lower stratosphere (UTLS) can have important implications for the radiative and chemical balance of the atmosphere. In this study we build on recent techniques and use new ones to estimate a range of transport diagnostics based on simultaneously measured trace gases in the UTLS during the monsoon season in North America.
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.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Felix Ploeger and Hella Garny
Atmos. Chem. Phys., 22, 5559–5576, https://doi.org/10.5194/acp-22-5559-2022, https://doi.org/10.5194/acp-22-5559-2022, 2022
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We investigate hemispheric asymmetries in stratospheric circulation changes in the last 2 decades in model simulations and atmospheric observations. We find that observed trace gas changes can be explained by a structural circulation change related to a deepening circulation in the Northern Hemisphere relative to the Southern Hemisphere. As this asymmetric signal is small compared to internal variability observed circulation trends over the recent past are not in contradiction to climate models.
Jan Clemens, Felix Ploeger, Paul Konopka, Raphael Portmann, Michael Sprenger, and Heini Wernli
Atmos. Chem. Phys., 22, 3841–3860, https://doi.org/10.5194/acp-22-3841-2022, https://doi.org/10.5194/acp-22-3841-2022, 2022
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Highly polluted air flows from the surface to higher levels of the atmosphere during the Asian summer monsoon. At high levels, the air is trapped within eddies. Here, we study how air masses can leave the eddy within its cutoff, how they distribute, and how their chemical composition changes. We found evidence for transport from the eddy to higher latitudes over the North Pacific and even Alaska. During transport, trace gas concentrations within cutoffs changed gradually, showing steady mixing.
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.
Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, Adam E. Bourassa, Doug A. Degenstein, Lucien Froidevaux, C. Thomas McElroy, Donal Murtagh, James M. Russell III, and Jiansheng Zou
Atmos. Meas. Tech., 15, 1233–1249, https://doi.org/10.5194/amt-15-1233-2022, https://doi.org/10.5194/amt-15-1233-2022, 2022
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This study analyzes the quality of two versions (v3.6 and v4.1) of ozone concentration measurements from the ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer), by comparing with data from five satellite instruments between 2004 and 2020. It was found that although the v3.6 data exhibit a better agreement than v4.1 with respect to the other instruments, v4.1 exhibits much better stability over time than v3.6. The stability of v4.1 makes it suitable for ozone trend studies.
Florian Haenel, Wolfgang Woiwode, Jennifer Buchmüller, Felix Friedl-Vallon, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Hermann Oelhaf, Johannes Orphal, Roland Ruhnke, Björn-Martin Sinnhuber, Jörn Ungermann, Michael Weimer, and Peter Braesicke
Atmos. Chem. Phys., 22, 2843–2870, https://doi.org/10.5194/acp-22-2843-2022, https://doi.org/10.5194/acp-22-2843-2022, 2022
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We compare remote sensing observations of H2O, O3, HNO3 and clouds in the upper troposphere–lowermost stratosphere during an Arctic winter long-range research flight with simulations by two different state-of-the-art model systems. We find good agreement for dynamical structures, trace gas distributions and clouds. We investigate model biases and sensitivities, with the goal of aiding model development and improving our understanding of processes in the upper troposphere–lowermost stratosphere.
Sheena Loeffel, Roland Eichinger, Hella Garny, Thomas Reddmann, Frauke Fritsch, Stefan Versick, Gabriele Stiller, and Florian Haenel
Atmos. Chem. Phys., 22, 1175–1193, https://doi.org/10.5194/acp-22-1175-2022, https://doi.org/10.5194/acp-22-1175-2022, 2022
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SF6-derived trends of stratospheric AoA from observations and model simulations disagree in sign. SF6 experiences chemical degradation, which we explicitly integrate in a global climate model. In our simulations, the AoA trend changes sign when SF6 sinks are considered; thus, the process has the potential to reconcile simulated with observed AoA trends. We show that the positive AoA trend is due to the SF6 sinks themselves and provide a first approach for a correction to account for SF6 loss.
Michael Höpfner, Oliver Kirner, Gerald Wetzel, Björn-Martin Sinnhuber, Florian Haenel, Sören Johansson, Johannes Orphal, Roland Ruhnke, Gabriele Stiller, and Thomas von Clarmann
Atmos. Chem. Phys., 21, 18433–18464, https://doi.org/10.5194/acp-21-18433-2021, https://doi.org/10.5194/acp-21-18433-2021, 2021
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BrONO2 is an important reservoir gas for inorganic stratospheric bromine linked to the chemical cycles of stratospheric ozone depletion. Presently infrared limb sounding is the only way to measure BrONO2 in the atmosphere. We provide global distributions of BrONO2 derived from MIPAS observations 2002–2012. Comparisons with EMAC atmospheric modelling show an overall agreement and enable us to derive an independent estimate of stratospheric bromine of 21.2±1.4pptv based on the BrONO2 measurements.
Tyler Wizenberg, Kimberly Strong, Kaley Walker, Erik Lutsch, Tobias Borsdorff, and Jochen Landgraf
Atmos. Meas. Tech., 14, 7707–7728, https://doi.org/10.5194/amt-14-7707-2021, https://doi.org/10.5194/amt-14-7707-2021, 2021
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CO is an important atmospheric gas that influences both air quality and the climate. Here, we compare CO measurements from TROPOMI with those from ACE-FTS and an Arctic ground-based FTS at Eureka, Nunavut, to further characterize the accuracy of TROPOMI measurements. CO columns from the instruments agree well but show larger differences at high latitudes. Despite this, the results fall within the TROPOMI accuracy target, indicating good data quality at high latitudes.
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.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Nathaniel J. Livesey, William G. Read, Lucien Froidevaux, Alyn Lambert, Michelle L. Santee, Michael J. Schwartz, Luis F. Millán, Robert F. Jarnot, Paul A. Wagner, Dale F. Hurst, Kaley A. Walker, Patrick E. Sheese, and Gerald E. Nedoluha
Atmos. Chem. Phys., 21, 15409–15430, https://doi.org/10.5194/acp-21-15409-2021, https://doi.org/10.5194/acp-21-15409-2021, 2021
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The Microwave Limb Sounder (MLS), an instrument on NASA's Aura mission launched in 2004, measures vertical profiles of the temperature and composition of Earth's "middle atmosphere" (the region from ~12 to ~100 km altitude). We describe how, among the 16 trace gases measured by MLS, the measurements of water vapor (H2O) and nitrous oxide (N2O) have started to drift since ~2010. The paper also discusses the origins of this drift and work to ameliorate it in a new version of the MLS dataset.
Christoph Mahnke, Ralf Weigel, Francesco Cairo, Jean-Paul Vernier, Armin Afchine, Martina Krämer, Valentin Mitev, Renaud Matthey, Silvia Viciani, Francesco D'Amato, Felix Ploeger, Terry Deshler, and Stephan Borrmann
Atmos. Chem. Phys., 21, 15259–15282, https://doi.org/10.5194/acp-21-15259-2021, https://doi.org/10.5194/acp-21-15259-2021, 2021
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In 2017, in situ aerosol measurements were conducted aboard the M55 Geophysica in the Asian monsoon region. The vertical particle mixing ratio profiles show a distinct layer (15–18.5 km), the Asian tropopause aerosol layer (ATAL). The backscatter ratio (BR) was calculated based on the aerosol size distributions and compared with the BRs detected by a backscatter probe and a lidar aboard M55, and by the CALIOP lidar. All four methods show enhanced BRs in the ATAL altitude range (max. at 17.5 km).
Marta Abalos, Natalia Calvo, Samuel Benito-Barca, Hella Garny, Steven C. Hardiman, Pu Lin, Martin B. Andrews, Neal Butchart, Rolando Garcia, Clara Orbe, David Saint-Martin, Shingo Watanabe, and Kohei Yoshida
Atmos. Chem. Phys., 21, 13571–13591, https://doi.org/10.5194/acp-21-13571-2021, https://doi.org/10.5194/acp-21-13571-2021, 2021
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The stratospheric Brewer–Dobson circulation (BDC), responsible for transporting mass, tracers and heat globally in the stratosphere, is evaluated in a set of state-of-the-art climate models. The acceleration of the BDC in response to increasing greenhouse gases is most robust in the lower stratosphere. At higher levels, the well-known inconsistency between model and observational BDC trends can be partly reconciled by accounting for limited sampling and large uncertainties in the observations.
Francesco Grieco, Kristell Pérot, Donal Murtagh, Patrick Eriksson, Bengt Rydberg, Michael Kiefer, Maya Garcia-Comas, Alyn Lambert, and Kaley A. Walker
Atmos. Meas. Tech., 14, 5823–5857, https://doi.org/10.5194/amt-14-5823-2021, https://doi.org/10.5194/amt-14-5823-2021, 2021
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We present improved Odin/SMR mesospheric H2O concentration and temperature data sets, reprocessed assuming a bigger sideband leakage of the instrument. The validation study shows how the improved SMR data sets agree better with other instruments' observations than the old SMR version did. Given their unique time extension and geographical coverage, and H2O being a good tracer of mesospheric circulation, the new data sets are valuable for the study of dynamical processes and multi-year trends.
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.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
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.
Nuria Pilar Plaza, Aurélien Podglajen, Cristina Peña-Ortiz, and Felix Ploeger
Atmos. Chem. Phys., 21, 9585–9607, https://doi.org/10.5194/acp-21-9585-2021, https://doi.org/10.5194/acp-21-9585-2021, 2021
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We study the role of different processes in setting the lower stratospheric water vapour. We find that mechanisms involving ice microphysics and small-scale mixing produce the strongest increase in water vapour, in particular over the Asian Monsoon. Small-scale mixing has a special relevance as it improves the agreement with observations at seasonal and intra-seasonal timescales, contrary to the North American Monsoon case, in which large-scale temperatures still dominate its variability.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
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.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Thomas von Clarmann, Udo Grabowski, Gabriele P. Stiller, Beatriz M. Monge-Sanz, Norbert Glatthor, and Sylvia Kellmann
Atmos. Chem. Phys., 21, 8823–8843, https://doi.org/10.5194/acp-21-8823-2021, https://doi.org/10.5194/acp-21-8823-2021, 2021
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Measurements of long-lived trace gases (SF6, CFC-11, CFC-12, HCFC-12, CCl4, N2O, CH4, H2O, and CO) performed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) have been used to infer the stratospheric and mesospheric meridional circulation. The MIPAS data set covers the time period from July 2002 to April 2012. The method used for this purpose was the direct inversion of the two-dimensional continuity equation. Multiannual monthly mean circulation fields are presented.
Michael Kiefer, Thomas von Clarmann, Bernd Funke, Maya García-Comas, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Anne Kleinert, Alexandra Laeng, Andrea Linden, Manuel López-Puertas, Daniel R. Marsh, and Gabriele P. Stiller
Atmos. Meas. Tech., 14, 4111–4138, https://doi.org/10.5194/amt-14-4111-2021, https://doi.org/10.5194/amt-14-4111-2021, 2021
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An improved dataset of vertical temperature profiles of the Earth's atmosphere in the altitude range 5–70 km is presented. These profiles are derived from measurements of the MIPAS instrument onboard ESA's Envisat satellite. The overall improvements are based on upgrades in the input data and several improvements in the data processing approach. Both of these are discussed, and an extensive error discussion is included. Enhancements of the new dataset are demonstrated by means of examples.
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.
Mohamadou Diallo, Manfred Ern, and Felix Ploeger
Atmos. Chem. Phys., 21, 7515–7544, https://doi.org/10.5194/acp-21-7515-2021, https://doi.org/10.5194/acp-21-7515-2021, 2021
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Despite good agreement in the spatial structure, there are substantial differences in the strength of the Brewer–Dobson circulation (BDC) and its modulations in the UTLS and upper stratosphere. The tropical upwelling is generally weaker in ERA5 than in ERAI due to weaker planetary and gravity wave breaking in the UTLS. Analysis of the BDC trend shows an acceleration of the BDC of about 1.5 % decade-1 due to the long-term intensification in wave breaking, consistent with climate predictions.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Simone Dietmüller, Hella Garny, Roland Eichinger, and William T. Ball
Atmos. Chem. Phys., 21, 6811–6837, https://doi.org/10.5194/acp-21-6811-2021, https://doi.org/10.5194/acp-21-6811-2021, 2021
Michaela I. Hegglin, Susann Tegtmeier, John Anderson, Adam E. Bourassa, Samuel Brohede, Doug Degenstein, Lucien Froidevaux, Bernd Funke, John Gille, Yasuko Kasai, Erkki T. Kyrölä, Jerry Lumpe, Donal Murtagh, Jessica L. Neu, Kristell Pérot, Ellis E. Remsberg, Alexei Rozanov, Matthew Toohey, Joachim Urban, Thomas von Clarmann, Kaley A. Walker, Hsiang-Jui Wang, Carlo Arosio, Robert Damadeo, Ryan A. Fuller, Gretchen Lingenfelser, Christopher McLinden, Diane Pendlebury, Chris Roth, Niall J. Ryan, Christopher Sioris, Lesley Smith, and Katja Weigel
Earth Syst. Sci. Data, 13, 1855–1903, https://doi.org/10.5194/essd-13-1855-2021, https://doi.org/10.5194/essd-13-1855-2021, 2021
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An overview of the SPARC Data Initiative is presented, to date the most comprehensive assessment of stratospheric composition measurements spanning 1979–2018. Measurements of 26 chemical constituents obtained from an international suite of space-based limb sounders were compiled into vertically resolved, zonal monthly mean time series. The quality and consistency of these gridded datasets are then evaluated using a climatological validation approach and a range of diagnostics.
Viktoria F. Sofieva, Monika Szeląg, Johanna Tamminen, Erkki Kyrölä, Doug Degenstein, Chris Roth, Daniel Zawada, Alexei Rozanov, Carlo Arosio, John P. Burrows, Mark Weber, Alexandra Laeng, Gabriele P. Stiller, Thomas von Clarmann, Lucien Froidevaux, Nathaniel Livesey, Michel van Roozendael, and Christian Retscher
Atmos. Chem. Phys., 21, 6707–6720, https://doi.org/10.5194/acp-21-6707-2021, https://doi.org/10.5194/acp-21-6707-2021, 2021
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The MErged GRIdded Dataset of Ozone Profiles is a long-term (2001–2018) stratospheric ozone profile climate data record with resolved longitudinal structure that combines the data from six limb satellite instruments. The dataset can be used for various analyses, some of which are discussed in the paper. In particular, regionally and vertically resolved ozone trends are evaluated, including trends in the polar regions.
Xiaolu Yan, Paul Konopka, Marius Hauck, Aurélien Podglajen, and Felix Ploeger
Atmos. Chem. Phys., 21, 6627–6645, https://doi.org/10.5194/acp-21-6627-2021, https://doi.org/10.5194/acp-21-6627-2021, 2021
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Inter-hemispheric transport is important for understanding atmospheric tracers because of the asymmetry in emissions between the Southern Hemisphere (SH) and Northern Hemisphere (NH). This study finds that the air masses from the NH extratropics to the atmosphere are about 5 times larger than those from the SH extratropics. The interplay between the Asian summer monsoon and westerly ducts triggers the cross-Equator transport from the NH to the SH in boreal summer and fall.
Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, Doug A. Degenstein, Felicia Kolonjari, David Plummer, Douglas E. Kinnison, Patrick Jöckel, and Thomas von Clarmann
Atmos. Meas. Tech., 14, 1425–1438, https://doi.org/10.5194/amt-14-1425-2021, https://doi.org/10.5194/amt-14-1425-2021, 2021
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Output from climate chemistry models (CMAM, EMAC, and WACCM) is used to estimate the expected geophysical variability of ozone concentrations between coincident satellite instrument measurement times and geolocations. We use the Canadian ACE-FTS and OSIRIS instruments as a case study. Ensemble mean estimates are used to optimize coincidence criteria between the two instruments, allowing for the use of more coincident profiles while providing an estimate of the geophysical variation.
Emily M. Gordon, Annika Seppälä, Bernd Funke, Johanna Tamminen, and Kaley A. Walker
Atmos. Chem. Phys., 21, 2819–2836, https://doi.org/10.5194/acp-21-2819-2021, https://doi.org/10.5194/acp-21-2819-2021, 2021
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Energetic particle precipitation (EPP) is the rain of solar energetic particles into the Earth's atmosphere. EPP is known to deplete O3 in the polar mesosphere–upper stratosphere via the formation of NOx. NOx also causes chlorine deactivation in the lower stratosphere and has, thus, been proposed to potentially result in reduced ozone depletion in the spring. We provide the first evidence to show that NOx formed by EPP is able to remove active chlorine, resulting in enhanced total ozone column.
Marc von Hobe, Felix Ploeger, Paul Konopka, Corinna Kloss, Alexey Ulanowski, Vladimir Yushkov, Fabrizio Ravegnani, C. Michael Volk, Laura L. Pan, Shawn B. Honomichl, Simone Tilmes, Douglas E. Kinnison, Rolando R. Garcia, and Jonathon S. Wright
Atmos. Chem. Phys., 21, 1267–1285, https://doi.org/10.5194/acp-21-1267-2021, https://doi.org/10.5194/acp-21-1267-2021, 2021
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The Asian summer monsoon (ASM) is known to foster transport of polluted tropospheric air into the stratosphere. To test and amend our picture of ASM vertical transport, we analyse distributions of airborne trace gas observations up to 20 km altitude near the main ASM vertical conduit south of the Himalayas. We also show that a new high-resolution version of the global chemistry climate model WACCM is able to reproduce the observations well.
Corinna Kloss, Gwenaël Berthet, Pasquale Sellitto, Felix Ploeger, Ghassan Taha, Mariam Tidiga, Maxim Eremenko, Adriana Bossolasco, Fabrice Jégou, Jean-Baptiste Renard, and Bernard Legras
Atmos. Chem. Phys., 21, 535–560, https://doi.org/10.5194/acp-21-535-2021, https://doi.org/10.5194/acp-21-535-2021, 2021
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The year 2019 was particularly rich for the stratospheric aerosol layer due to two volcanic eruptions (at Raikoke and Ulawun) and wildfire events. With satellite observations and models, we describe the exceptionally complex situation following the Raikoke eruption. The respective plume overwhelmed the Northern Hemisphere stratosphere in terms of aerosol load and resulted in the highest climate impact throughout the past decade.
Yuming Jin, Ralph F. Keeling, Eric J. Morgan, Eric Ray, Nicholas C. Parazoo, and Britton B. Stephens
Atmos. Chem. Phys., 21, 217–238, https://doi.org/10.5194/acp-21-217-2021, https://doi.org/10.5194/acp-21-217-2021, 2021
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We propose a new atmospheric coordinate (Mθe) based on equivalent potential temperature (θe) but with mass as the unit. This coordinate is useful in studying the spatial and temporal distribution of long-lived chemical tracers (CO2, CH4, O2 / N2, etc.) from sparse data, like airborne observation. Using this coordinate and sparse airborne observation (HIPPO and ATom), we resolve the Northern Hemisphere mass-weighted average CO2 seasonal cycle with high accuracy.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Ales Kuchar, William Ball, Pavle Arsenovic, Ellis Remsberg, Patrick Jöckel, Markus Kunze, David A. Plummer, Andrea Stenke, Daniel Marsh, Doug Kinnison, and Thomas Peter
Atmos. Chem. Phys., 21, 201–216, https://doi.org/10.5194/acp-21-201-2021, https://doi.org/10.5194/acp-21-201-2021, 2021
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The solar signal in the mesospheric H2O and CO was extracted from the CCMI-1 model simulations and satellite observations using multiple linear regression (MLR) analysis. MLR analysis shows a pronounced and statistically robust solar signal in both H2O and CO. The model results show a general agreement with observations reproducing a negative/positive solar signal in H2O/CO. The pattern of the solar signal varies among the considered models, reflecting some differences in the model setup.
Seidai Nara, Tomohiro O. Sato, Takayoshi Yamada, Tamaki Fujinawa, Kota Kuribayashi, Takeshi Manabe, Lucien Froidevaux, Nathaniel J. Livesey, Kaley A. Walker, Jian Xu, Franz Schreier, Yvan J. Orsolini, Varavut Limpasuvan, Nario Kuno, and Yasuko Kasai
Atmos. Meas. Tech., 13, 6837–6852, https://doi.org/10.5194/amt-13-6837-2020, https://doi.org/10.5194/amt-13-6837-2020, 2020
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In the atmosphere, more than 80 % of chlorine compounds are anthropogenic. Hydrogen chloride (HCl), the main stratospheric chlorine reservoir, is useful to estimate the total budget of the atmospheric chlorine compounds. We report, for the first time, the HCl vertical distribution from the middle troposphere to the lower thermosphere using a high-sensitivity SMILES measurement; the data quality is quantified by comparisons with other measurements and via theoretical error analysis.
Manuel Baumgartner, Ralf Weigel, Allan H. Harvey, Felix Plöger, Ulrich Achatz, and Peter Spichtinger
Atmos. Chem. Phys., 20, 15585–15616, https://doi.org/10.5194/acp-20-15585-2020, https://doi.org/10.5194/acp-20-15585-2020, 2020
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The potential temperature is routinely used in atmospheric science. We review its derivation and suggest a new potential temperature, based on a temperature-dependent parameterization of the dry air's specific heat capacity. Moreover, we compare the new potential temperature to the common one and discuss the differences which become more important at higher altitudes. Finally, we indicate some consequences of using the new potential temperature in typical applications.
Edward J. Charlesworth, Ann-Kristin Dugstad, Frauke Fritsch, Patrick Jöckel, and Felix Plöger
Atmos. Chem. Phys., 20, 15227–15245, https://doi.org/10.5194/acp-20-15227-2020, https://doi.org/10.5194/acp-20-15227-2020, 2020
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Modeling the stratosphere requires models with good representations of chemical transport. To do this, nearly all models divide the atmosphere into boxes. This creates some unwanted problems. However, the only other option is to divide the atmosphere into balloons, and this method is very complicated. Here, we use a model which uses this balloon-like method to estimate the impacts of this method on chemical transport. We find significant differences in sensitive regions of the stratosphere.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
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Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
Hella Garny, Roland Walz, Matthias Nützel, and Thomas Birner
Geosci. Model Dev., 13, 5229–5257, https://doi.org/10.5194/gmd-13-5229-2020, https://doi.org/10.5194/gmd-13-5229-2020, 2020
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Numerical models of Earth's climate system have been gaining more and more complexity over the last decades. Therefore, it is important to establish simplified models to improve process understanding. In our study, we present and document the development of a new simplified model setup within the framework of a complex climate model system that uses the same routines to calculate atmospheric dynamics as the complex model but is simplified in the representation of clouds and radiation.
Benjamin Birner, Martyn P. Chipperfield, Eric J. Morgan, Britton B. Stephens, Marianna Linz, Wuhu Feng, Chris Wilson, Jonathan D. Bent, Steven C. Wofsy, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Chem. Phys., 20, 12391–12408, https://doi.org/10.5194/acp-20-12391-2020, https://doi.org/10.5194/acp-20-12391-2020, 2020
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With new high-precision observations from nine aircraft campaigns and 3-D chemical transport modeling, we show that the argon-to-nitrogen ratio (Ar / N2) in the lowermost stratosphere provides a useful constraint on the “age of air” (the time elapsed since entry of an air parcel into the stratosphere). Therefore, Ar / N2 in combination with traditional age-of-air indicators, such as CO2 and N2O, could provide new insights into atmospheric mixing and transport.
Francesco Grieco, Kristell Pérot, Donal Murtagh, Patrick Eriksson, Peter Forkman, Bengt Rydberg, Bernd Funke, Kaley A. Walker, and Hugh C. Pumphrey
Atmos. Meas. Tech., 13, 5013–5031, https://doi.org/10.5194/amt-13-5013-2020, https://doi.org/10.5194/amt-13-5013-2020, 2020
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We present a unique – by time extension and geographical coverage – dataset of satellite observations of carbon monoxide (CO) in the mesosphere which will allow us to study dynamical processes, since CO is a very good tracer of circulation in the mesosphere. Previously, the dataset was unusable due to instrumental artefacts that affected the measurements. We identify the cause of the artefacts, eliminate them and prove the quality of the results by comparing with other instrument measurements.
Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Kenneth C. Aikin, Teresa Campos, Hannah Clark, Róisín Commane, Bruce Daube, Glenn W. Diskin, James W. Elkins, Ru-Shan Gao, Audrey Gaudel, Eric J. Hintsa, Bryan J. Johnson, Rigel Kivi, Kathryn McKain, Fred L. Moore, David D. Parrish, Richard Querel, Eric Ray, Ricardo Sánchez, Colm Sweeney, David W. Tarasick, Anne M. Thompson, Valérie Thouret, Jacquelyn C. Witte, Steve C. Wofsy, and Thomas B. Ryerson
Atmos. Chem. Phys., 20, 10611–10635, https://doi.org/10.5194/acp-20-10611-2020, https://doi.org/10.5194/acp-20-10611-2020, 2020
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Short summary
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.
We present a 17-year stratospheric age-of-air dataset derived from ACE-FTS satellite...
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