Articles | Volume 24, issue 1
https://doi.org/10.5194/acp-24-689-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-24-689-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
17 Jan 2024
Research article |
| 17 Jan 2024
| 17 Jan 2024
The interhemispheric gradient of SF6 in the upper troposphere
Tanja J. Schuck
CORRESPONDING AUTHOR
Institute for Atmospheric and Environmental Sciences, University of Frankfurt, Frankfurt, Germany
Johannes Degen
Institute for Atmospheric and Environmental Sciences, University of Frankfurt, Frankfurt, Germany
Eric Hintsa
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, Colorado, United States
NOAA Global Monitoring Laboratory, Boulder, Colorado, United States
Peter Hoor
Institute for Atmospheric Physics, Johannes Gutenberg University of Mainz, Mainz, Germany
Markus Jesswein
Institute for Atmospheric and Environmental Sciences, University of Frankfurt, Frankfurt, Germany
Timo Keber
Institute for Atmospheric and Environmental Sciences, University of Frankfurt, Frankfurt, Germany
Daniel Kunkel
Institute for Atmospheric Physics, Johannes Gutenberg University of Mainz, Mainz, Germany
Fred Moore
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, Colorado, United States
NOAA Global Monitoring Laboratory, Boulder, Colorado, United States
Florian Obersteiner
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
Matt Rigby
School of Chemistry, University of Bristol, Bristol, United Kingdom
Thomas Wagenhäuser
Institute for Atmospheric and Environmental Sciences, University of Frankfurt, Frankfurt, Germany
Luke M. Western
NOAA Global Monitoring Laboratory, Boulder, Colorado, United States
Andreas Zahn
School of Chemistry, University of Bristol, Bristol, United Kingdom
Andreas Engel
Institute for Atmospheric and Environmental Sciences, University of Frankfurt, Frankfurt, Germany
Related authors
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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
Short summary
Short summary
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
Short summary
Short summary
The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
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
Short summary
Short summary
Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Madhuri Umbarkar and Daniel Kunkel
Atmos. Chem. Phys., 25, 10159–10182, https://doi.org/10.5194/acp-25-10159-2025, https://doi.org/10.5194/acp-25-10159-2025, 2025
Short summary
Short summary
Atmospheric gravity waves (GWs) significantly enhance vertical shear in the lowermost stratosphere (LMS), influencing turbulence and mixing in the extratropical transition layer. Using idealized baroclinic life cycle experiments with the ICON model, this study demonstrates that moisture and cloud processes amplify GW activity, driving strong shear and turbulence in the LMS. These findings highlight the critical role of GWs in shaping the dynamics in the LMS, particularly for clear air turbulence.
Kirstin Gerrand, Elena Fillola, Alistair J. Manning, Jgor Arduini, Paul B. Krummel, Chris R. Lunder, Jens Mühle, Simon O'Doherty, Sunyoung Park, Ronald G. Prinn, Stefan Reimann, Dickon Young, and Matthew Rigby
EGUsphere, https://doi.org/10.5194/egusphere-2025-4137, https://doi.org/10.5194/egusphere-2025-4137, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
To analyse long-term trends in atmospheric trace gas concentrations, it is important to identify data points minimally affected by local pollution sources or air masses carried from other latitudes or altitudes. Traditional methods for detecting these “baselines” are computationally expensive or lack a basis in physical principles. This paper introduces a machine-learning method that uses meteorological data and offers significantly lower computational costs compared to physics-based techniques.
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
Short summary
Short summary
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.
Rodrigo J. Seguel, Charlie Opazo, Yann Cohen, Owen R. Cooper, Laura Gallardo, Björn-Martin Sinnhuber, Florian Obersteiner, Andreas Zahn, Peter Hoor, Susanne Rohs, and Andreas Marsing
Atmos. Chem. Phys., 25, 8553–8573, https://doi.org/10.5194/acp-25-8553-2025, https://doi.org/10.5194/acp-25-8553-2025, 2025
Short summary
Short summary
We explored ozone differences between the Northern Hemisphere and Southern Hemispheres in the upper troposphere–lower stratosphere. We found lower ozone (with stratospheric origin) in the Southern Hemisphere, especially during years of severe ozone depletion. Sudden stratospheric warming events increased the ozone in each hemisphere, highlighting the relationship between stratospheric processes and ozone in the upper troposphere, where ozone is an important greenhouse gas.
Markus Jesswein, Valentin Lauther, Nicolas Emig, Peter Hoor, Timo Keber, Hans-Christoph Lachnitt, Linda Ort, Tanja Schuck, Johannes Strobel, Ronja Van Luijt, C. Michael Volk, Franziska Weyland, and Andreas Engel
Atmos. Chem. Phys., 25, 8107–8126, https://doi.org/10.5194/acp-25-8107-2025, https://doi.org/10.5194/acp-25-8107-2025, 2025
Short summary
Short summary
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.
Jasna V. Pittman, Bruce C. Daube, Steven C. Wofsy, Elliot L. Atlas, Maria A. Navarro, Eric J. Hintsa, Fred L. Moore, Geoff S. Dutton, James W. Elkins, Troy D. Thornberry, Andrew W. Rollins, Eric J. Jensen, Thaopaul Bui, Jonathan Dean-Day, and Leonhard Pfister
Atmos. Chem. Phys., 25, 7543–7562, https://doi.org/10.5194/acp-25-7543-2025, https://doi.org/10.5194/acp-25-7543-2025, 2025
Short summary
Short summary
Biomass fires emit aerosols and precursors that can provide a novel environment for initiating stratospheric ozone loss. The Airborne Tropical TRopopause EXperiment campaign sampled the western Pacific, the dominant longitudes for surface air lofted by convection to enter the global stratosphere. Aircraft measurements over multiple flights revealed persistent layers of biomass burning pollutants entering the lower stratosphere and originating from fires as far away as Africa and Indonesia.
Elena Fillola, Raul Santos-Rodriguez, Rachel Tunnicliffe, Jeffrey Clark, Nawid Keshtmand, Anita Ganesan, and Matthew Rigby
EGUsphere, https://doi.org/10.5194/egusphere-2025-2392, https://doi.org/10.5194/egusphere-2025-2392, 2025
Short summary
Short summary
Satellite-based greenhouse gas measurements can be used in “inverse models” to improve emissions reporting, but one of the key components, the simulations of atmospheric transport, struggle to scale to large datasets. We introduce GATES, an AI-driven emulator that outputs transport plumes about 1000× faster than traditional models. Applied to Brazil’s methane emissions, GATES produces estimates consistent with physics-based methods, offering a scalable path for timely emissions monitoring.
Anna Breuninger, Philipp Joppe, Jonas Wilsch, Cornelis Schwenk, Heiko Bozem, Nicolas Emig, Laurin Merkel, Rainer Rossberg, Timo Keber, Arthur Kutschka, Philipp Waleska, Stefan Hofmann, Sarah Richter, Florian Ungeheuer, Konstantin Dörholt, Thorsten Hoffmann, Annette Miltenberger, Johannes Schneider, Peter Hoor, and Alexander L. Vogel
EGUsphere, https://doi.org/10.5194/egusphere-2025-3129, https://doi.org/10.5194/egusphere-2025-3129, 2025
Short summary
Short summary
This study investigates molecular organic aerosol composition in the upper troposphere and lower stratosphere from an airborne campaign over Central Europe in summer 2024. Via ultra-high-performance liquid chromatography and high-resolution mass spectrometry of tropospheric and stratospheric filter samples, we identified various organic compounds. Our findings underscore the significant cross-tropopause transport of biogenic secondary organic aerosol and anthropogenic pollutants.
Heiko Bozem, Philipp Joppe, Yun Li, Nicolas Emig, Armin Afchine, Anna Breuninger, Joachim Curtius, Stefan Hofmann, Sadath Ismayil, Konrad Kandler, Daniel Kunkel, Arthur Kutschka, Hans-Christoph Lachnitt, Andreas Petzold, Sarah Richter, Timo Röschenthaler, Christian Rolf, Lisa Schneider, Johannes Schneider, Alexander Vogel, and Peter Hoor
EGUsphere, https://doi.org/10.5194/egusphere-2025-3175, https://doi.org/10.5194/egusphere-2025-3175, 2025
Short summary
Short summary
Deployed on a Learjet as a tandem measurement platform during TPEx I (TropoPause composition gradients and mixing Experiment) campaign in June 2024, the new TPC-TOSS (TropoPause Composition Towed Sensor Shuttle) system delivers high-resolution in situ data on ozone, aerosol, clouds, and key weather parameters. Laboratory and in-flight tests confirmed its precision and stability. Observed gradients near the tropopause reveal active mixing and transport processes in the tropopause region.
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).
Short summary
Short summary
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
Short summary
Short summary
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.
Luke M. Western, Matthew Rigby, Jens Mühle, Paul B. Krummel, Chris R. Lunder, Simon O'Doherty, Stefan Reimann, Martin K. Vollmer, Dickon Young, Ben Adam, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Ove Hermansen, Jooil Kim, Ray L. Langenfelds, Zoë M. Loh, Blagoj Mitrevski, Joseph R. Pitt, Peter K. Salameh, Roland Schmidt, Kieran Stanley, Ann R. Stavert, Hsiang-Jui Wang, Ray F. Weiss, and Ronald G. Prinn
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-348, https://doi.org/10.5194/essd-2025-348, 2025
Preprint under review for ESSD
Short summary
Short summary
We used global measurements and an atmospheric model to estimate how emissions and abundances of 42 chemically and radiatively important trace gases have changed over time. These gases affect the Earth's radiative balance and the ozone layer. Our data sets help track progress in reducing harmful. This work supports international efforts to protect the environment by providing clear, long-term, consistent data on how these gases are changing in the atmosphere.
Patrick Konjari, Christian Rolf, Martina Krämer, Armin Afchine, Nicole Spelten, Irene Bartolome Garcia, Annette Miltenberger, Nicolar Emig, Philipp Joppe, Johannes Schneider, Yun Li, Andreas Petzold, Heiko Bozem, and Peter Hoor
EGUsphere, https://doi.org/10.5194/egusphere-2025-2847, https://doi.org/10.5194/egusphere-2025-2847, 2025
Short summary
Short summary
We investigated how a powerful storm over southern Sweden in June 2024 transported ice particles and moist air into the normally dry stratosphere. We observed unusually high water vapor and ice levels up to 1.5 kilometers above the tropopause. Although the extra water vapor lasted only a few days to weeks, it shows how such storms can temporarily alter the upper atmosphere’s composition.
Piers M. Forster, Chris Smith, Tristram Walsh, William F. Lamb, Robin Lamboll, Christophe Cassou, Mathias Hauser, Zeke Hausfather, June-Yi Lee, Matthew D. Palmer, Karina von Schuckmann, Aimée B. A. Slangen, Sophie Szopa, Blair Trewin, Jeongeun Yun, Nathan P. Gillett, Stuart Jenkins, H. Damon Matthews, Krishnan Raghavan, Aurélien Ribes, Joeri Rogelj, Debbie Rosen, Xuebin Zhang, Myles Allen, Lara Aleluia Reis, Robbie M. Andrew, Richard A. Betts, Alex Borger, Jiddu A. Broersma, Samantha N. Burgess, Lijing Cheng, Pierre Friedlingstein, Catia M. Domingues, Marco Gambarini, Thomas Gasser, Johannes Gütschow, Masayoshi Ishii, Christopher Kadow, John Kennedy, Rachel E. Killick, Paul B. Krummel, Aurélien Liné, Didier P. Monselesan, Colin Morice, Jens Mühle, Vaishali Naik, Glen P. Peters, Anna Pirani, Julia Pongratz, Jan C. Minx, Matthew Rigby, Robert Rohde, Abhishek Savita, Sonia I. Seneviratne, Peter Thorne, Christopher Wells, Luke M. Western, Guido R. van der Werf, Susan E. Wijffels, Valérie Masson-Delmotte, and Panmao Zhai
Earth Syst. Sci. Data, 17, 2641–2680, https://doi.org/10.5194/essd-17-2641-2025, https://doi.org/10.5194/essd-17-2641-2025, 2025
Short summary
Short summary
In a rapidly changing climate, evidence-based decision-making benefits from up-to-date and timely information. Here we compile monitoring datasets to track real-world changes over time. To make our work relevant to policymakers, we follow methods from the Intergovernmental Panel on Climate Change (IPCC). Human activities are increasing the Earth's energy imbalance and driving faster sea-level rise compared to the IPCC assessment.
Yann Cohen, Didier Hauglustaine, Nicolas Bellouin, Marianne Tronstad Lund, Sigrun Matthes, Agnieszka Skowron, Robin Thor, Ulrich Bundke, Andreas Petzold, Susanne Rohs, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 25, 5793–5836, https://doi.org/10.5194/acp-25-5793-2025, https://doi.org/10.5194/acp-25-5793-2025, 2025
Short summary
Short summary
The chemical composition of the atmosphere near the tropopause is a key parameter for evaluating the climate impact of subsonic aviation pollutants. This study uses in situ data collected aboard passenger aircraft to assess the ability of four chemistry–climate models to reproduce (bi-)decadal climatologies of ozone, carbon monoxide, water vapour, and reactive nitrogen in this region. The models reproduce the very distinct ozone seasonality in the upper troposphere and in the lower stratosphere well.
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
Short summary
Short summary
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.
Philipp Joppe, Johannes Schneider, Jonas Wilsch, Heiko Bozem, Anna Breuninger, Joachim Curtius, Martin Ebert, Nicolas Emig, Peter Hoor, Sadath Ismayil, Konrad Kandler, Daniel Kunkel, Isabel Kurth, Hans-Christoph Lachnitt, Yun Li, Annette Miltenberger, Sarah Richter, Christian Rolf, Lisa Schneider, Cornelis Schwenk, Nicole Spelten, Alexander L. Vogel, Yafang Cheng, and Stephan Borrmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-1346, https://doi.org/10.5194/egusphere-2025-1346, 2025
Short summary
Short summary
We show measurements of a filament with biomass burning influence transported by a warm conveyor belt (WCB) into the tropopause region over Europe. The pollution originates from Canadian forest fires and is transported in the lower troposphere towards Europe. The WCB transport is followed by mixing with air masses of stratospheric chemical signatures. We hypothesize that this mixing leads to a change in the vertical gradient of the potential temperature.
Linda Ort, Andrea Pozzer, Peter Hoor, Florian Obersteiner, Andreas Zahn, Thomas B. Ryerson, Chelsea R. Thompson, Jeff Peischl, Róisín Commane, Bruce Daube, Ilann Bourgeois, Jos Lelieveld, and Horst Fischer
EGUsphere, https://doi.org/10.5194/egusphere-2025-1477, https://doi.org/10.5194/egusphere-2025-1477, 2025
Short summary
Short summary
This study investigates the role of lightning emissions on the O3–CO ratio in the northern subtropics. We used in situ observations and a global circulation model to show an effect of up to 40 % onto the subtropical O3–CO ratio by tropical air masses transported via the Hadley cell. This influence of lightning emissions and its photochemistry has a global effect on trace and greenhouse gases and needs to be considered for global chemical distributions.
Sophie Bauchinger, Andreas Engel, Markus Jesswein, Timo Keber, Harald Bönisch, Florian Obersteiner, Andreas Zahn, Nicolas Emig, Peter Hoor, Hans-Christoph Lachnitt, Franziska Weyland, Linda Ort, and Tanja J. Schuck
EGUsphere, https://doi.org/10.5194/egusphere-2025-1589, https://doi.org/10.5194/egusphere-2025-1589, 2025
Short summary
Short summary
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
Short summary
Short summary
A balloon was launched in 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km. One purpose was to compare measurement techniques. We focus on the major greenhouse gases. To measure these, air was sampled with the AirCore technique and with flask sampling, and samples were analysed after the flight. In flight, observations were done with an optical method. In a companion paper, we report on observations of chlorine and bromine containing trace gases.
Patrick Konjari, Christian Rolf, Michaela I. Hegglin, Susanne Rohs, Yun Li, Andreas Zahn, Harald Bönisch, Philippe Nedelec, Martina Krämer, and Andreas Petzold
Atmos. Chem. Phys., 25, 4269–4289, https://doi.org/10.5194/acp-25-4269-2025, https://doi.org/10.5194/acp-25-4269-2025, 2025
Short summary
Short summary
This study introduces a new method to derive adjusted water vapor (H2O) climatologies for the upper tropopshere and lower statosphere (UT/LS) using data from 60 000 flights under the IAGOS program. Biases in the IAGOS water vapour dataset are adjusted, based on the more accurate IAGOS-CARIBIC data. The resulting highly resolved H2O climatologies will contribute to a better understanding of the H2O variability in the UT/LS and its connection to various transport and mixing processes.
Laura N. Saunders, Kaley A. Walker, Gabriele P. Stiller, Thomas von Clarmann, Florian Haenel, Hella Garny, Harald Bönisch, Chris D. Boone, Ariana E. Castillo, Andreas Engel, Johannes C. Laube, Marianna Linz, Felix Ploeger, David A. Plummer, Eric A. Ray, and Patrick E. Sheese
Atmos. Chem. Phys., 25, 4185–4209, https://doi.org/10.5194/acp-25-4185-2025, https://doi.org/10.5194/acp-25-4185-2025, 2025
Short summary
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.
Helen Walter-Terrinoni, John S. Daniel, Chelsea R. Thompson, and Luke M. Western
EGUsphere, https://doi.org/10.5194/egusphere-2025-297, https://doi.org/10.5194/egusphere-2025-297, 2025
Short summary
Short summary
We have developed a model to improve our ability to estimate emissions of chemicals that are used as foam blowing agents. Some of these chemicals are ozone-depleting substances and some are greenhouse gases. For HCFC-141b, which is the focus of this study, we find that recent observations are inconsistent with our calculated emissions, with our emissions being lower. This mismatch is similar to previous findings and may have important implications for compliance with the Montreal Protocol.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Nicolas Emig, Annette K. Miltenberger, Peter M. Hoor, and Andreas Petzold
EGUsphere, https://doi.org/10.5194/egusphere-2024-3919, https://doi.org/10.5194/egusphere-2024-3919, 2025
Short summary
Short summary
This study presents in situ observations of cirrus occurrence from aircraft measurements in the extra-tropical transition layer (ExTL) using simultaneous measurements from two platforms. Lagrangian diagnostics based on high-resolution ICON simulations show long residence times of the cirrus in stratospheric air allowing to separate different diabatic processes during transit. The findings suggest that radiative diabatic cloud processes significantly impact the tropopause thermodynamic structure.
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
Short summary
Short summary
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.
Herman G.J. Smit, Torben Galle, Romain Blot, Florian Obersteiner, Philippe Nédélec, Andreas Zahn, Jean-Marc Cousin, Ulrich Bundke, Andreas Petzold, Valerie Thouret, and Hannah Clark
EGUsphere, https://doi.org/10.5194/egusphere-2024-3760, https://doi.org/10.5194/egusphere-2024-3760, 2025
Short summary
Short summary
The two ozone instruments of IAGOS (In-service Aircraft for a Global Observation System) have been compared with the Ozone PhotoMeter (OPM) of the World Calibration Center of Ozone Sondes (WCCOS) in an atmospheric simulation chamber under realistic flight conditions of pressure, temperature, and ozone concentrations. The two IAGOS-instruments showed good agreement with the OPM within 5–6 %. The observed differences are small but systematic and reproducible during the intercomparison.
Chun Hang Chau, Peter Hoor, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2024-3805, https://doi.org/10.5194/egusphere-2024-3805, 2024
Short summary
Short summary
This study examines how the turbulence in the upper troposphere/lower stratosphere could modify the tracer distribution under different situations. Using a multi-scale chemistry model, we find that both the pre-existing tracer gradient and the dynamical and thermodynamically forcing play a role in modifying the tracer distribution. These results allow further research on the UTLS turbulent mixing and its implications for the climate system.
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
Short summary
Short summary
The tropopause separates the troposphere, where many greenhouse gases originate, from the stratosphere. This study examines a tropopause defined by potential vorticity – an analogue for angular momentum that changes sharply in the subtropics, creating a transport barrier. Between 1980 and 2017, this tropopause shifted poleward at lower altitudes and equatorward above, suggesting height-dependent changes in atmospheric circulation that may affect greenhouse gas distribution and global warming.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
Short summary
Short summary
Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
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
Short summary
Short summary
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.
Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5731–5746, https://doi.org/10.5194/amt-17-5731-2024, https://doi.org/10.5194/amt-17-5731-2024, 2024
Short summary
Short summary
The ozone sink into oceans and marine clouds is seldom studied and highly uncertain. Calculations suggest O3 destruction at aqueous surfaces (ocean, droplets) may be strongly accelerated, but field evidence is missing. Here we compare three fast airborne O3 instruments to measure eddy covariance fluxes of O3 over the remote ocean, in clear and cloudy air. We find O3 fluxes below clouds are consistently directed into clouds, while O3 fluxes into oceans are much smaller and spatially variable.
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
Short summary
Short summary
In the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we have mapped multiplatform ozone datasets into coordinate systems to systematically evaluate the influence of these coordinates on binned climatological variability. This effort unifies the work of studies that focused on individual coordinate system variability. Our goal was to create the most comprehensive assessment of this topic.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
Short summary
Short summary
The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, and Stephan Borrmann
Atmos. Chem. Phys., 24, 7499–7522, https://doi.org/10.5194/acp-24-7499-2024, https://doi.org/10.5194/acp-24-7499-2024, 2024
Short summary
Short summary
From aircraft measurements in the upper troposphere/lower stratosphere, we find a correlation between the ozone and particulate sulfate in the lower stratosphere. The correlation exhibits some variability over the measurement period exceeding the background sulfate-to-ozone correlation. From our analysis, we conclude that gas-to-particle conversion of volcanic sulfur dioxide leads to observed enhanced sulfate aerosol mixing ratios.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
Short summary
Short summary
Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
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
Short summary
Short summary
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.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
Short summary
Short summary
The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
Short summary
Short summary
The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
Short summary
Short summary
The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
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
Short summary
Short summary
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.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
Short summary
Short summary
The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
Short summary
Short summary
Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
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
Short summary
Short summary
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.
Jianghanyang Li, Bianca C. Baier, Fred Moore, Tim Newberger, Sonja Wolter, Jack Higgs, Geoff Dutton, Eric Hintsa, Bradley Hall, and Colm Sweeney
Atmos. Meas. Tech., 16, 2851–2863, https://doi.org/10.5194/amt-16-2851-2023, https://doi.org/10.5194/amt-16-2851-2023, 2023
Short summary
Short summary
Monitoring a suite of trace gases in the stratosphere will help us better understand the stratospheric circulation and its impact on the earth's radiation balance. However, such measurements are rare and usually expensive. We developed an instrument that can measure stratospheric trace gases using a low-cost sampling platform (AirCore). The results showed expected agreement with aircraft measurements, demonstrating this technique provides a low-cost and robust way to observe the stratosphere.
Elena Fillola, Raul Santos-Rodriguez, Alistair Manning, Simon O'Doherty, and Matt Rigby
Geosci. Model Dev., 16, 1997–2009, https://doi.org/10.5194/gmd-16-1997-2023, https://doi.org/10.5194/gmd-16-1997-2023, 2023
Short summary
Short summary
Lagrangian particle dispersion models are used extensively for the estimation of greenhouse gas (GHG) fluxes using atmospheric observations. However, these models do not scale well as data volumes increase. Here, we develop a proof-of-concept machine learning emulator that can produce outputs similar to those of the dispersion model, but 50 000 times faster, using only meteorological inputs. This works demonstrates the potential of machine learning to accelerate GHG estimations across the globe.
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
Short summary
Short summary
A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
Short summary
Short summary
During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
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
Short summary
Short summary
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.
Hans-Christoph Lachnitt, Peter Hoor, Daniel Kunkel, Martina Bramberger, Andreas Dörnbrack, Stefan Müller, Philipp Reutter, Andreas Giez, Thorsten Kaluza, and Markus Rapp
Atmos. Chem. Phys., 23, 355–373, https://doi.org/10.5194/acp-23-355-2023, https://doi.org/10.5194/acp-23-355-2023, 2023
Short summary
Short summary
We present an analysis of high-resolution airborne measurements during a flight of the DEEPWAVE 2014 campaign in New Zealand. The focus of this flight was to study the effects of enhanced mountain wave activity over the Southern Alps. We discuss changes in the upstream and downstream distributions of N2O and CO and show that these changes are related to turbulence-induced trace gas fluxes which have persistent effects on the trace gas composition in the lower stratosphere.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
Short summary
Short summary
We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
Short summary
Short summary
The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
Short summary
Short summary
Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
Short summary
Short summary
We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.9 to 7.8 × 105 cm-3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
Short summary
Short summary
In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
Preprint withdrawn
Short summary
Short summary
The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
Short summary
Short summary
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.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
Short summary
Short summary
Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Vivienne H. Payne, Susan S. Kulawik, Emily V. Fischer, Jared F. Brewer, L. Gregory Huey, Kazuyuki Miyazaki, John R. Worden, Kevin W. Bowman, Eric J. Hintsa, Fred Moore, James W. Elkins, and Julieta Juncosa Calahorrano
Atmos. Meas. Tech., 15, 3497–3511, https://doi.org/10.5194/amt-15-3497-2022, https://doi.org/10.5194/amt-15-3497-2022, 2022
Short summary
Short summary
We compare new satellite measurements of peroxyacetyl nitrate (PAN) with reference aircraft measurements from two different instruments flown on the same platform. While there is a systematic difference between the two aircraft datasets, both show the same large-scale distribution of PAN and the discrepancy between aircraft datasets is small compared to the satellite uncertainties. The satellite measurements show skill in capturing large-scale variations in PAN.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
Short summary
Short summary
Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
Short summary
Short summary
The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
Short summary
Short summary
The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
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
Short summary
Short summary
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.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
Short summary
Short summary
Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
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
Short summary
Short summary
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.
Jens Mühle, Lambert J. M. Kuijpers, Kieran M. Stanley, Matthew Rigby, Luke M. Western, Jooil Kim, Sunyoung Park, Christina M. Harth, Paul B. Krummel, Paul J. Fraser, Simon O'Doherty, Peter K. Salameh, Roland Schmidt, Dickon Young, Ronald G. Prinn, Ray H. J. Wang, and Ray F. Weiss
Atmos. Chem. Phys., 22, 3371–3378, https://doi.org/10.5194/acp-22-3371-2022, https://doi.org/10.5194/acp-22-3371-2022, 2022
Short summary
Short summary
Emissions of the strong greenhouse gas perfluorocyclobutane (c-C4F8) into the atmosphere have been increasing sharply since the early 2000s. These c-C4F8 emissions are highly correlated with the amount of hydrochlorofluorocarbon-22 produced to synthesize polytetrafluoroethylene (known for its non-stick properties) and related chemicals. From this process, c-C4F8 by-product is vented to the atmosphere. Avoiding these unnecessary c-C4F8 emissions could reduce the climate impact of this industry.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
Short summary
Short summary
The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Valentin Lauther, Bärbel Vogel, Johannes Wintel, Andrea Rau, Peter Hoor, Vera Bense, Rolf Müller, and C. Michael Volk
Atmos. Chem. Phys., 22, 2049–2077, https://doi.org/10.5194/acp-22-2049-2022, https://doi.org/10.5194/acp-22-2049-2022, 2022
Short summary
Short summary
We show airborne in situ measurements of the very short-lived ozone-depleting substances CH2Cl2 and CHCl3, revealing particularly high concentrations of both species in the lower stratosphere. Back-trajectory calculations and 3D model simulations show that the air masses with high concentrations originated in the Asian boundary layer and were transported via the Asian summer monsoon. We also identify a fast transport pathway into the stratosphere via the North American monsoon and by hurricanes.
Andrew Zammit-Mangion, Michael Bertolacci, Jenny Fisher, Ann Stavert, Matthew Rigby, Yi Cao, and Noel Cressie
Geosci. Model Dev., 15, 45–73, https://doi.org/10.5194/gmd-15-45-2022, https://doi.org/10.5194/gmd-15-45-2022, 2022
Short summary
Short summary
We present a framework for estimating the sources and sinks (flux) of carbon dioxide from satellite data. The framework is statistical and yields measures of uncertainty alongside all estimates of flux and other parameters in the underlying model. It also allows us to generate other insights, such as the size of errors and biases in the data. The primary aim of this research was to develop a fully statistical flux inversion framework for use by atmospheric scientists.
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
Short summary
Short summary
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
Short summary
Short summary
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.
Jan C. Minx, William F. Lamb, Robbie M. Andrew, Josep G. Canadell, Monica Crippa, Niklas Döbbeling, Piers M. Forster, Diego Guizzardi, Jos Olivier, Glen P. Peters, Julia Pongratz, Andy Reisinger, Matthew Rigby, Marielle Saunois, Steven J. Smith, Efisio Solazzo, and Hanqin Tian
Earth Syst. Sci. Data, 13, 5213–5252, https://doi.org/10.5194/essd-13-5213-2021, https://doi.org/10.5194/essd-13-5213-2021, 2021
Short summary
Short summary
We provide a synthetic dataset on anthropogenic greenhouse gas (GHG) emissions for 1970–2018 with a fast-track extension to 2019. We show that GHG emissions continued to rise across all gases and sectors. Annual average GHG emissions growth slowed, but absolute decadal increases have never been higher in human history. We identify a number of data gaps and data quality issues in global inventories and highlight their importance for monitoring progress towards international climate goals.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
Short summary
Short summary
We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-788, https://doi.org/10.5194/acp-2021-788, 2021
Preprint withdrawn
Short summary
Short summary
By presenting an approach using EMeRGe-Asia airborne field measurements and surface observations, this study shows that the fraction of OH reactivity due to SO2-OH reaction has a significant correlation with the sulfate concentration. Approximately 30 % of sulfate is produced by SO2-OH reaction. Our results underline the importance of SO2-OH gas-phase oxidation in sulfate formation, and demonstrate that the method can be applied to other regions and under different meteorological conditions.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
Short summary
Short summary
We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
Short summary
Short summary
NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
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
Short summary
Short summary
Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
Short summary
Short summary
The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
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
Short summary
Short summary
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.
Thorsten Kaluza, Daniel Kunkel, and Peter Hoor
Weather Clim. Dynam., 2, 631–651, https://doi.org/10.5194/wcd-2-631-2021, https://doi.org/10.5194/wcd-2-631-2021, 2021
Short summary
Short summary
We present a 10-year analysis on the occurrence of strong wind shear in the Northern Hemisphere, focusing on the region around the transport barrier that separates the first two layers of the atmosphere. The major result of our analysis is that strong wind shear above a certain threshold occurs frequently and nearly exclusively in this region, which, as an indicator for turbulent mixing, might have major implications concerning the separation efficiency of the transport barrier.
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
Short summary
Short summary
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
Short summary
Short summary
A Rossby wave (RW) breaking event was observed over the North Atlantic during the WISE measurement campaign in October 2017. Infrared limb sounding measurements of trace gases in the lower stratosphere, including high-resolution 3-D tomographic reconstruction, revealed complex spatial structures in stratospheric tracers near the polar jet related to previous RW breaking events. Backward-trajectory analysis and tracer correlations were used to study mixing and stratosphere–troposphere exchange.
Fides Lefrancois, Markus Jesswein, Markus Thoma, Andreas Engel, Kieran Stanley, and Tanja Schuck
Atmos. Meas. Tech., 14, 4669–4687, https://doi.org/10.5194/amt-14-4669-2021, https://doi.org/10.5194/amt-14-4669-2021, 2021
Short summary
Short summary
Synthetic halocarbons can contribute to stratospheric ozone depletion or to climate change. In many applications they have been replaced over the last years. The presented non-target analysis shows an application approach to quantify those replacements retrospectively, using recorded data of air measurements with gas chromatography coupled to time-of-flight mass spectrometry. We focus on the retrospective analysis of the fourth-generation halocarbons, detected at Taunus Observatory in Germany.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412, https://doi.org/10.5194/acp-21-8393-2021, https://doi.org/10.5194/acp-21-8393-2021, 2021
Short summary
Short summary
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
Short summary
Short summary
AirCore samplers are increasingly deployed to weather balloons to collect continuous atmospheric samples. We introduce a technique that can be used in situ to evaluate different data processing methods that are required to derive vertical trace gas profiles from AirCore measurements after sample recovery. Results from two test flights with a specific AirCore configuration provide evidence for systematic deviations in altitude attribution for the upper levels, which can be empirically corrected.
Romain Blot, Philippe Nedelec, Damien Boulanger, Pawel Wolff, Bastien Sauvage, Jean-Marc Cousin, Gilles Athier, Andreas Zahn, Florian Obersteiner, Dieter Scharffe, Hervé Petetin, Yasmine Bennouna, Hannah Clark, and Valérie Thouret
Atmos. Meas. Tech., 14, 3935–3951, https://doi.org/10.5194/amt-14-3935-2021, https://doi.org/10.5194/amt-14-3935-2021, 2021
Short summary
Short summary
A lack of information about temporal changes in measurement uncertainties is an area of concern for long-term trend studies of the key compounds which have a direct or indirect impact on climate change. The IAGOS program has measured O3 and CO within the troposphere and lower stratosphere for more than 25 years. In this study, we demonstrated that the IAGOS database can be treated as one continuous program and is therefore appropriate for studies of long-term trends.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
Short summary
Short summary
Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
Short summary
Short summary
Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Hannes Schulz, Daniel Kunkel, Heiko Bozem, Peter Hoor, Thomas Klimach, Frank Helleis, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 21, 6509–6539, https://doi.org/10.5194/acp-21-6509-2021, https://doi.org/10.5194/acp-21-6509-2021, 2021
Short summary
Short summary
We present in situ observations of vertically resolved particle chemical composition in the summertime Arctic lower troposphere. Our analysis demonstrates the strong vertical contrast between particle properties within the boundary layer and aloft. Emissions from vegetation fires and anthropogenic sources in northern Canada, Europe, and East Asia influenced particle composition in the free troposphere. Organics detected in Arctic aerosol particles can partly be identified as dicarboxylic acids.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
Short summary
Short summary
Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
Short summary
Short summary
Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
Short summary
Short summary
During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067, https://doi.org/10.5194/acp-20-13041-2020, https://doi.org/10.5194/acp-20-13041-2020, 2020
Short summary
Short summary
This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
Short summary
Short summary
During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Guillaume Monteil, Grégoire Broquet, Marko Scholze, Matthew Lang, Ute Karstens, Christoph Gerbig, Frank-Thomas Koch, Naomi E. Smith, Rona L. Thompson, Ingrid T. Luijkx, Emily White, Antoon Meesters, Philippe Ciais, Anita L. Ganesan, Alistair Manning, Michael Mischurow, Wouter Peters, Philippe Peylin, Jerôme Tarniewicz, Matt Rigby, Christian Rödenbeck, Alex Vermeulen, and Evie M. Walton
Atmos. Chem. Phys., 20, 12063–12091, https://doi.org/10.5194/acp-20-12063-2020, https://doi.org/10.5194/acp-20-12063-2020, 2020
Short summary
Short summary
The paper presents the first results from the EUROCOM project, a regional atmospheric inversion intercomparison exercise involving six European research groups. It aims to produce an estimate of the net carbon flux between the European terrestrial ecosystems and the atmosphere for the period 2006–2015, based on constraints provided by observed CO2 concentrations and using inverse modelling techniques. The use of six different models enables us to investigate the robustness of the results.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
Short summary
Short summary
With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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
Cited articles
Belikov, D. A., Saitoh, N., and Patra, P. K.: An Analysis of Interhemispheric Transport Pathways Based on Three-Dimensional Methane Data by GOSAT Observations and Model Simulations, J. Geophys. Res.-Atmos., 127, e2021JD035688, https://doi.org/10.1029/2021JD035688, 2022. a, b
Bischof, W., Borchers, R., Fabian, P., and Krüger, B.: Increased concentration and vertical distribution of carbon dioxide in the stratosphere, Nature, 316, 708–710, https://doi.org/10.1038/316708a0, 1985. a
Bönisch, H., Engel, A., Birner, Th., Hoor, P., Tarasick, D. W., and Ray, E. A.: On the structural changes in the Brewer-Dobson circulation after 2000, Atmos. Chem. Phys., 11, 3937–3948, https://doi.org/10.5194/acp-11-3937-2011, 2011. a
Brenninkmeijer, C. A. M., Crutzen, P., Boumard, F., Dauer, T., Dix, B., Ebinghaus, R., Filippi, D., Fischer, H., Franke, H., Frieβ, U., Heintzenberg, J., Helleis, F., Hermann, M., Kock, H. H., Koeppel, C., Lelieveld, J., Leuenberger, M., Martinsson, B. G., Miemczyk, S., Moret, H. P., Nguyen, H. N., Nyfeler, P., Oram, D., O'Sullivan, D., Penkett, S., Platt, U., Pupek, M., Ramonet, M., Randa, B., Reichelt, M., Rhee, T. S., Rohwer, J., Rosenfeld, K., Scharffe, D., Schlager, H., Schumann, U., Slemr, F., Sprung, D., Stock, P., Thaler, R., Valentino, F., van Velthoven, P., Waibel, A., Wandel, A., Waschitschek, K., Wiedensohler, A., Xueref-Remy, I., Zahn, A., Zech, U., and Ziereis, H.: Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system, Atmos. Chem. Phys., 7, 4953–4976, https://doi.org/10.5194/acp-7-4953-2007, 2007. a
Chen, G., Orbe, C., and Waugh, D.: The role of monsoon-like zonally asymmetric heating in interhemispheric transport, J. Geophys. Res.-Atmos., 122, 3282–3298, https://doi.org/10.1002/2016JD026427, 2017. a
Crippa, M., Guizzardi, D., Solazzo, E., Muntean, M., Schaaf, E., Monforti-Ferrario, F., Banja, M., Olivier, J., Grassi, G., Rossi, S., and Vignati, E.: GHG emissions of all world: 2021 report, Publications Office of the European Union, https://doi.org/10.2760/173513, 2021. a
Cunnold, D. M., Prinn, R. G., Rasmussen, R. A., Simmonds, P. G., Alyea, F. N., Cardelino, C. A., Crawford, A. J., Fraser, P. J., and Rosen, R. D.: The Atmospheric Lifetime Experiment: 3. Lifetime methodology and application to three years of CFCl3 data, J. Geophys. Res.-Oceans, 88, 8379–8400, https://doi.org/10.1029/JC088iC13p08379, 1983. a, b, c
Cunnold, D. M., Fraser, P. J., Weiss, R. F., Prinn, R. G., Simmonds, P. G., Miller, B. R., Alyea, F. N., and Crawford, A. J.: Global trends and annual releases of CCl3F and CCl2F2 estimated from ALE/GAGE and other measurements from July 1978 to June 1991, J. Geophys. Res.-Atmos., 99, 1107–1126, https://doi.org/10.1029/93JD02715, 1994. a
Cunnold, D. M., Weiss, R. F., Prinn, R. G., Hartley, D., Simmonds, P. G., Fraser, P. J., Miller, B., Alyea, F. N., and Porter, L.: GAGE/AGAGE measurements indicating reductions in global emissions of CCl3F and CCl2F2 in 1992–1994, J. Geophys. Res.-Atmos., 102, 1259–1269, https://doi.org/10.1029/96JD02973, 1997. a
Cunnold, D. M., Steele, L. P., Fraser, P. J., Simmonds, P. G., Prinn, R. G., Weiss, R. F., Porter, L. W., O'Doherty, S., Langenfelds, R. L., Krummel, P. B., Wang, H. J., Emmons, L., Tie, X. X., and Dlugokencky, E. J.: In situ measurements of atmospheric methane at GAGE/AGAGE sites during 1985–2000 and resulting source inferences, J. Geophys. Res.-Atmos., 107, ACH 20–1–ACH 20–18, https://doi.org/10.1029/2001JD001226, 2002. a
Deutsches Zentrum für Luft- und Raumfahrt: HALO database, https://halo-db.pa.op.dlr.de/search?page=47&texts=&missions=1&missions=116, last access: 12 January 2024. a
Dutton, G., Elkin, J., Hall, B., and NOAA ESRL: Earth System Research Laboratory Halocarbons and Other Atmospheric Trace Gases Chromatograph for Atmospheric Trace Species (CATS) Measurements, version: 2021-03, US National Centers for Environmental Information [data set], https://doi.org/10.7289/V5X0659V, 2017. a
Engel, A., Möbius, T., Bönisch, H., Schmidt, U., Heinz, R., Levin, I., Atlas, E., Aoki, S., Nakazawa, T., Sugawara, S., Moore, F., Hurst, D., Elkins, J., Schauffler, S., Andrews, A., and Boering, K.: Age of stratospheric air unchanged within uncertainties over the past 30 years, Nat. Geosci., 2, 28–31, https://doi.org/10.1038/ngeo388, 2009. a
Gloor, M., Dlugokencky, E., Brenninkmeijer, C., Horowitz, L., Hurst, D. F., Dutton, G., Crevoisier, C., Machida, T., and Tans, P.: Three-dimensional SF6 data and tropospheric transport simulations: Signals, modeling accuracy, and implications for inverse modeling, J. Geophys. Res.-Atmos., 112, D15112, https://doi.org/10.1029/2006JD007973, 2007. a, b, c, d
Hall, T. M. and Waugh, D. W.: Influence of nonlocal chemistry on tracer distributions: Inferring the mean age of air from SF6, J. Geophys. Res.-Atmos., 103, 13327–13336, https://doi.org/10.1029/98JD00170, 1998. a
Hauck, M., Bönisch, H., Hoor, P., Keber, T., Ploeger, F., Schuck, T. J., and Engel, A.: A convolution of observational and model data to estimate age of air spectra in the northern hemispheric lower stratosphere, Atmos. Chem. Phys., 20, 8763–8785, https://doi.org/10.5194/acp-20-8763-2020, 2020. a
Hintsa, E. J., Moore, F. L., Hurst, D. F., Dutton, G. S., Hall, B. D., Nance, J. D., Miller, B. R., Montzka, S. A., Wolton, L. P., McClure-Begley, A., Elkins, J. W., Hall, E. G., Jordan, A. F., Rollins, A. W., Thornberry, T. D., Watts, L. A., Thompson, C. R., Peischl, J., Bourgeois, I., Ryerson, T. B., Daube, B. C., Gonzalez Ramos, Y., Commane, R., Santoni, G. W., Pittman, J. V., Wofsy, S. C., Kort, E., Diskin, G. S., and Bui, T. P.: UAS Chromatograph for Atmospheric Trace Species (UCATS) – a versatile instrument for trace gas measurements on airborne platforms, Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, 2021. a, b, c, d, e, f, g
Holzer, M. and Waugh, D. W.: Interhemispheric transit time distributions and path-dependent lifetimes constrained by measurements of SF6, CFCs, and CFC replacements, Geophys. Res. Lett., 42, 4581–4589, https://doi.org/10.1002/2015GL064172, 2015. a
Hu, L., Ottinger, D., Bogle, S., Montzka, S. A., DeCola, P. L., Dlugokencky, E., Andrews, A., Thoning, K., Sweeney, C., Dutton, G., Aepli, L., and Crotwell, A.: Declining, seasonal-varying emissions of sulfur hexafluoride from the United States, Atmos. Chem. Phys., 23, 1437–1448, https://doi.org/10.5194/acp-23-1437-2023, 2023. a, b
IAGOS-CARIBIC: Data access, https://www.caribic-atmospheric.com/Data.php, last access: 12 January 2024. a
Jesswein, M., Bozem, H., Lachnitt, H.-C., Hoor, P., Wagenhäuser, T., Keber, T., Schuck, T., and Engel, A.: Comparison of inorganic chlorine in the Antarctic and Arctic lowermost stratosphere by separate late winter aircraft measurements, Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, 2021. a, b
Keber, T., Bönisch, H., Hartick, C., Hauck, M., Lefrancois, F., Obersteiner, F., Ringsdorf, A., Schohl, N., Schuck, T., Hossaini, R., Graf, P., Jöckel, P., and Engel, A.: Bromine from short-lived source gases in the extratropical northern hemispheric upper troposphere and lower stratosphere (UTLS), Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, 2020. a
Ko, M. K. W., Sze, N. D., Wang, W.-C., Shia, G., Goldman, A., Murcray, F. J., Murcray, D. G., and Rinsland, C. P.: Atmospheric sulfur hexafluoride: Sources, sinks and greenhouse warming, J. Geophys. Res.-Atmos., 98, 10499–10507, https://doi.org/10.1029/93JD00228, 1993. a
Kovács, T., Feng, W., Totterdill, A., Plane, J. M. C., Dhomse, S., Gómez-Martín, J. C., Stiller, G. P., Haenel, F. J., Smith, C., Forster, P. M., García, R. R., Marsh, D. R., and Chipperfield, M. P.: Determination of the atmospheric lifetime and global warming potential of sulfur hexafluoride using a three-dimensional model, Atmos. Chem. Phys., 17, 883–898, https://doi.org/10.5194/acp-17-883-2017, 2017. a
Krol, M., de Bruine, M., Killaars, L., Ouwersloot, H., Pozzer, A., Yin, Y., Chevallier, F., Bousquet, P., Patra, P., Belikov, D., Maksyutov, S., Dhomse, S., Feng, W., and Chipperfield, M. P.: Age of air as a diagnostic for transport timescales in global models, Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, 2018. a, b, c
Kunkel, D., Hoor, P., Kaluza, T., Ungermann, J., Kluschat, B., Giez, A., Lachnitt, H.-C., Kaufmann, M., and Riese, M.: Evidence of small-scale quasi-isentropic mixing in ridges of extratropical baroclinic waves, Atmos. Chem. Phys., 19, 12607–12630, https://doi.org/10.5194/acp-19-12607-2019, 2019. a, b, c
Lan, X., Tans, P., Thoning, K., and NOAA Global Monitoring Laboratory: NOAA Greenhouse Gas Marine Boundary Layer Reference – SF6, 1997–2020, version: 2021-08, https://doi.org/10.15138/JYP5-0335, 2021. a, b
Levin, I., Naegler, T., Heinz, R., Osusko, D., Cuevas, E., Engel, A., Ilmberger, J., Langenfelds, R. L., Neininger, B., Rohden, C. v., Steele, L. P., Weller, R., Worthy, D. E., and Zimov, S. A.: The global SF6 source inferred from long-term high precision atmospheric measurements and its comparison with emission inventories, Atmos. Chem. Phys., 10, 2655–2662, https://doi.org/10.5194/acp-10-2655-2010, 2010. a, b
Liang, Q., Newman, P. A., Daniel, J. S., Reimann, S., Hall, B. D., Dutton, G., and Kuijpers, L. J. M.: Constraining the carbon tetrachloride (CCl4) budget using its global trend and inter-hemispheric gradient, Geophys. Res. Lett., 41, 5307–5315, https://doi.org/10.1002/2014GL060754, 2014. a
Miyazaki, K., Machida, T., Patra, P. K., Iwasaki, T., Sawa, Y., Matsueda, H., and Nakazawa, T.: Formation mechanisms of latitudinal CO2 gradients in the upper troposphere over the subtropics and tropics, J. Geophys. Res.-Atmos., 114, D03306, https://doi.org/10.1029/2008JD010545, 2009. a
Montzka, S. A., Dutton, G. S., Yu, P., Ray, E., Portmann, R. W., Daniel, J. S., Kuijpers, L., Hall, B. D., Mondeel, D., Siso, C., Nance, J. D., Rigby, M., Manning, A. J., Hu, L., Moore, F., Miller, B. R., and Elkins, J. W.: An unexpected and persistent increase in global emissions of ozone-depleting CFC-11, Nature, 557, 413–417, https://doi.org/10.1038/s41586-018-0106-2, 2018. a
Müller, S., Hoor, P., Bozem, H., Gute, E., Vogel, B., Zahn, A., Bönisch, H., Keber, T., Krämer, M., Rolf, C., Riese, M., Schlager, H., and Engel, A.: Impact of the Asian monsoon on the extratropical lower stratosphere: trace gas observations during TACTS over Europe 2012, Atmos. Chem. Phys., 16, 10573–10589, https://doi.org/10.5194/acp-16-10573-2016, 2016. a, b, c
Müller, S., Hoor, P., Berkes, F., Bozem, H., Klingebiel, M., Reutter, P., Smit, H. G. J., Wendisch, M., Spichtinger, P., and Borrmann, S.: In situ detection of stratosphere-troposphere exchange of cirrus particles in the midlatitudes, Geophys. Res. Lett., 42, 949–955, https://doi.org/10.1002/2014GL062556, 2015. a, b, c
Orbe, C., Waugh, D. W., Newman, P. A., and Steenrod, S.: The Transit-Time Distribution from the Northern Hemisphere Midlatitude Surface, J. Atmos. Sci., 73, 3785–3802, https://doi.org/10.1175/JAS-D-15-0289.1, 2016. a, b
Orbe, C., Yang, H., Waugh, D. W., Zeng, G., Morgenstern, O., Kinnison, D. E., Lamarque, J.-F., Tilmes, S., Plummer, D. A., Scinocca, J. F., Josse, B., Marecal, V., Jöckel, P., Oman, L. D., Strahan, S. E., Deushi, M., Tanaka, T. Y., Yoshida, K., Akiyoshi, H., Yamashita, Y., Stenke, A., Revell, L., Sukhodolov, T., Rozanov, E., Pitari, G., Visioni, D., Stone, K. A., Schofield, R., and Banerjee, A.: Large-scale tropospheric transport in the Chemistry–Climate Model Initiative (CCMI) simulations, Atmos. Chem. Phys., 18, 7217–7235, https://doi.org/10.5194/acp-18-7217-2018, 2018. a, b
Orbe, C., Waugh, D. W., Montzka, S., Dlugokencky, E. J., Strahan, S., Steenrod, S. D., Strode, S., Elkins, J. W., Hall, B., Sweeney, C., Hintsa, E. J., Moore, F. L., and Penafiel, E.: Tropospheric Age-of-Air: Influence of SF6 Emissions on Recent Surface Trends and Model Biases, J. Geophys. Res.-Atmos., 126, e2021JD035451, https://doi.org/10.1029/2021JD035451, 2021. a, b, c, d, e, f, g
Patra, P. K., Takigawa, M., Dutton, G. S., Uhse, K., Ishijima, K., Lintner, B. R., Miyazaki, K., and Elkins, J. W.: Transport mechanisms for synoptic, seasonal and interannual SF6 variations and ”age” of air in troposphere, Atmos. Chem. Phys., 9, 1209–1225, https://doi.org/10.5194/acp-9-1209-2009, 2009. a, b, c
Petzold, A., Thouret, V., Gerbig, C., Zahn, A., Brenninkmeijer, C. A. M., Gallagher, M., Hermann, M., Pontaud, M., Ziereis, H., Boulanger, D., Marshall, J., Nédélec, P., Smit, H. G. J., Friess, U., Flaud, J.-M., Wahner, A., Cammas, J.-P., Volz-Thomas, A., and TEAM, I.: Global-scale atmosphere monitoring by in-service aircraft – current achievements and future prospects of the European Research Infrastructure IAGOS, Tellus B, 67, 28452, https://doi.org/10.3402/tellusb.v67.28452, 2015. a
Prinn, R. G., Weiss, R. F., Arduini, J., Arnold, T., DeWitt, H. L., Fraser, P. J., Ganesan, A. L., Gasore, J., Harth, C. M., Hermansen, O., Kim, J., Krummel, P. B., Li, S., Loh, Z. M., Lunder, C. R., Maione, M., Manning, A. J., Miller, B. R., Mitrevski, B., Mühle, J., O'Doherty, S., Park, S., Reimann, S., Rigby, M., Saito, T., Salameh, P. K., Schmidt, R., Simmonds, P. G., Steele, L. P., Vollmer, M. K., Wang, R. H., Yao, B., Yokouchi, Y., Young, D., and Zhou, L.: History of chemically and radiatively important atmospheric gases from the Advanced Global Atmospheric Gases Experiment (AGAGE), Earth Syst. Sci. Data, 10, 985–1018, https://doi.org/10.5194/essd-10-985-2018, 2018. a
Randel, W. J. and Park, M.: Deep convective influence on the Asian summer monsoon anticyclone and associated tracer variability observed with Atmospheric Infrared Sounder (AIRS), J. Geophys. Res.-Atmos., 111, D12314, https://doi.org/10.1029/2005JD006490, 2006. a
Ray, E. A., Moore, F. L., Rosenlof, K. H., Davis, S. M., Sweeney, C., Tans, P., Wang, T., Elkins, J. W., Bönisch, H., Engel, A., Sugawara, S., Nakazawa, T., and Aoki, S.: Improving stratospheric transport trend analysis based on SF6 and CO2 measurements, J. Geophys. Res.-Atmos., 119, 14110–14128, https://doi.org/10.1002/2014JD021802, 2014. a
Ray, E. A., Moore, F. L., Elkins, J. W., Rosenlof, K. H., Laube, J. C., Röckmann, T., Marsh, D. R., and Andrews, A. E.: Quantification of the SF6 lifetime based on mesospheric loss measured in the stratospheric polar vortex, J. Geophys. Res.-Atmos., 122, 4626–4638, https://doi.org/10.1002/2016JD026198, 2017. a
Rigby, M. and Western, L.: mrghg/py12box: v0.2.1, Zenodo [code], https://doi.org/10.5281/zenodo.6857447, 2022. a
Rigby, M., Mühle, J., Miller, B. R., Prinn, R. G., Krummel, P. B., Steele, L. P., Fraser, P. J., Salameh, P. K., Harth, C. M., Weiss, R. F., Greally, B. R., O'Doherty, S., Simmonds, P. G., Vollmer, M. K., Reimann, S., Kim, J., Kim, K.-R., Wang, H. J., Olivier, J. G. J., Dlugokencky, E. J., Dutton, G. S., Hall, B. D., and Elkins, J. W.: History of atmospheric SF6 from 1973 to 2008, Atmos. Chem. Phys., 10, 10305–10320, https://doi.org/10.5194/acp-10-10305-2010, 2010. a, b
Rigby, M., Prinn, R. G., O'Doherty, S., Montzka, S. A., McCulloch, A., Harth, C. M., Mühle, J., Salameh, P. K., Weiss, R. F., Young, D., Simmonds, P. G., Hall, B. D., Dutton, G. S., Nance, D., Mondeel, D. J., Elkins, J. W., Krummel, P. B., Steele, L. P., and Fraser, P. J.: Re-evaluation of the lifetimes of the major CFCs and CH3CCl3 using atmospheric trends, Atmos. Chem. Phys., 13, 2691–2702, https://doi.org/10.5194/acp-13-2691-2013, 2013. a, b, c, d
Scharffe, D., Slemr, F., Brenninkmeijer, C. A. M., and Zahn, A.: Carbon monoxide measurements onboard the CARIBIC passenger aircraft using UV resonance fluorescence, Atmos. Meas. Tech., 5, 1753–1760, https://doi.org/10.5194/amt-5-1753-2012, 2012. a, b
Schuck, T.: Mixing ratios of sulfur hexafluoride (SF6) in the upper troposphere, Zenodo [data set], https://doi.org/10.5281/zenodo.10018398, 2023. a
Schuck, T. J., Brenninkmeijer, C. A. M., Slemr, F., Xueref-Remy, I., and Zahn, A.: Greenhouse gas analysis of air samples collected onboard the CARIBIC passenger aircraft, Atmos. Meas. Tech., 2, 449–464, https://doi.org/10.5194/amt-2-449-2009, 2009. a, b, c, d
Schuck, T. J., Brenninkmeijer, C. A. M., Baker, A. K., Slemr, F., von Velthoven, P. F. J., and Zahn, A.: Greenhouse gas relationships in the Indian summer monsoon plume measured by the CARIBIC passenger aircraft, Atmos. Chem. Phys., 10, 3965–3984, https://doi.org/10.5194/acp-10-3965-2010, 2010. a
Schuck, T. J., Ishijima, K., Patra, P. K., Baker, A. K., Machida, T., Matsueda, H., Sawa, Y., Umezawa, T., Brenninkmeijer, C. A. M., and Lelieveld, J.: Distribution of methane in the tropical upper troposphere measured by CARIBIC and CONTRAIL aircraft, J. Geophys. Res.-Atmos., 117, D19304, https://doi.org/10.1029/2012JD018199, 2012. a, b, c
Schuck, T. J., Lefrancois, F., Gallmann, F., Wang, D., Jesswein, M., Hoker, J., Bönisch, H., and Engel, A.: Establishing long-term measurements of halocarbons at Taunus Observatory, Atmos. Chem. Phys., 18, 16553–16569, https://doi.org/10.5194/acp-18-16553-2018, 2018. a
Simmonds, P. G., Rigby, M., Manning, A. J., Park, S., Stanley, K. M., McCulloch, A., Henne, S., Graziosi, F., Maione, M., Arduini, J., Reimann, S., Vollmer, M. K., Mühle, J., O'Doherty, S., Young, D., Krummel, P. B., Fraser, P. J., Weiss, R. F., Salameh, P. K., Harth, C. M., Park, M.-K., Park, H., Arnold, T., Rennick, C., Steele, L. P., Mitrevski, B., Wang, R. H. J., and Prinn, R. G.: The increasing atmospheric burden of the greenhouse gas sulfur hexafluoride (SF6), Atmos. Chem. Phys., 20, 7271–7290, https://doi.org/10.5194/acp-20-7271-2020, 2020. a, b, c
Smith, C., Nicholls, Z., Armour, K., Collins, W., Forster, P., Meinshausen, M., Palmer, M., and Watanabe, M.: The Earth’s Energy Budget, Climate Feedbacks, and Climate Sensitivity Supplementary Material, Book section 7, Cambridge University Press, https://doi.org/10.1017/9781009157896.009, 2021. a
Spivakovsky, C. M., Logan, J. A., Montzka, S. A., Balkanski, Y. J., Foreman-Fowler, M., Jones, D. B. A., Horowitz, L. W., Fusco, A. C., Brenninkmeijer, C. A. M., Prather, M. J., Wofsy, S. C., and McElroy, M. B.: Three-dimensional climatological distribution of tropospheric OH: Update and evaluation, J. Geophys. Res.-Atmos., 105, 8931–8980, https://doi.org/10.1029/1999JD901006, 2000. a
Strahan, S. E., Duncan, B. N., and Hoor, P.: Observationally derived transport diagnostics for the lowermost stratosphere and their application to the GMI chemistry and transport model, Atmos. Chem. Phys., 7, 2435–2445, https://doi.org/10.5194/acp-7-2435-2007, 2007. a
Strahan, S. E., Douglass, A. R., and Steenrod, S. D.: Chemical and dynamical impacts of stratospheric sudden warmings on Arctic ozone variability, J. Geophys. Res.-Atmos., 121, 11836–11851, https://doi.org/10.1002/2016JD025128, 2016. a
Thompson, C. R., Wofsy, S. C., Prather, M. J., Newman, P. A., Hanisco, T. F., Ryerson, T. B., Fahey, D. W., Apel, E. C., Brock, C. A., Brune, W. H., Froyd, K., Katich, J. M., Nicely, J. M., Peischl, J., Ray, E., Veres, P. R., Wang, S., Allen, H. M., Asher, E., Bian, H., Blake, D., Bourgeois, I., Budney, J., Bui, T. P., Butler, A., Campuzano-Jost, P., Chang, C., Chin, M., Commane, R., Correa, G., Crounse, J. D., Daube, B., Dibb, J. E., DiGangi, J. P., Diskin, G. S., Dollner, M., Elkins, J. W., Fiore, A. M., Flynn, C. M., Guo, H., Hall, S. R., Hannun, R. A., Hills, A., Hintsa, E. J., Hodzic, A., Hornbrook, R. S., Huey, L. G., Jimenez, J. L., Keeling, R. F., Kim, M. J., Kupc, A., Lacey, F., Lait, L. R., Lamarque, J.-F., Liu, J., McKain, K., Meinardi, S., Miller, D. O., Montzka, S. A., Moore, F. L., Morgan, E. J., Murphy, D. M., Murray, L. T., Nault, B. A., Neuman, J. A., Nguyen, L., Gonzalez, Y., Rollins, A., Rosenlof, K., Sargent, M., Schill, G., Schwarz, J. P., Clair, J. M. S., Steenrod, S. D., Stephens, B. B., Strahan, S. E., Strode, S. A., Sweeney, C., Thames, A. B., Ullmann, K., Wagner, N., Weber, R., Weinzierl, B., Wennberg, P. O., Williamson, C. J., Wolfe, G. M., and Zeng, L.: The NASA Atmospheric Tomography (ATom) Mission: Imaging the Chemistry of the Global Atmosphere, B. Am. Meteorol. Soc., 103, E761–E790, https://doi.org/10.1175/BAMS-D-20-0315.1, 2022. a
Thorenz, U., Baker, A., Leedham Elvidge, E., Sauvage, C., Riede, H., van Velthoven, P., Hermann, M., Weigelt, A., Oram, D., Brenninkmeijer, C., Zahn, A., and Williams, J.: Investigating African trace gas sources, vertical transport, and oxidation using IAGOS-CARIBIC measurements between Germany and South Africa between 2009 and 2011, Atmos. Environ., 158, 11–26, https://doi.org/10.1016/j.atmosenv.2017.03.021, 2017. a, b
Vogel, B., Günther, G., Müller, R., Grooß, J.-U., Afchine, A., Bozem, H., Hoor, P., Krämer, M., Müller, S., Riese, M., Rolf, C., Spelten, N., Stiller, G. P., Ungermann, J., and Zahn, A.: Long-range transport pathways of tropospheric source gases originating in Asia into the northern lower stratosphere during the Asian monsoon season 2012, Atmos. Chem. Phys., 16, 15301–15325, https://doi.org/10.5194/acp-16-15301-2016, 2016. a
Volk, C. M., Elkins, J. W., Fahey, D. W., Dutton, G. S., Gilligan, J. M., Loewenstein, M., Podolske, J. R., Chan, K. R., and Gunson, M. R.: Evaluation of source gas lifetimes from stratospheric observations, J. Geophys. Res.-Atmos., 102, 25543–25564, https://doi.org/10.1029/97JD02215, 1997. a
Wagenhäuser, T., Jesswein, M., Keber, T., Schuck, T., and Engel, A.: Mean age from observations in the lowermost stratosphere: an improved method and interhemispheric differences, Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, 2023. a
Waugh, D. W., Crotwell, A. M., Dlugokencky, E. J., Dutton, G. S., Elkins, J. W., Hall, B. D., Hintsa, E. J., Hurst, D. F., Montzka, S. A., Mondeel, D. J., Moore, F. L., Nance, J. D., Ray, E. A., Steenrod, S. D., Strahan, S. E., and Sweeney, C.: Tropospheric SF6: Age of air from the Northern Hemisphere midlatitude surface, J. Geophys. Res.-Atmos., 118, 11429–11441, https://doi.org/10.1002/jgrd.50848, 2013. a, b, c, d
Wofsy, S., Daube, B., Jimenez, R., Kort, E., Pittman, J., Park, S., Commane, R., Xiang, B., Santoni, G., Jacob, D., Fisher, J., Pickett-Heaps, C., Wang, H., Wecht, K., Wang, Q., Stephens, B., Shertz, S., Watt, A., Romashkin, P., Campos, T., Haggerty, J., Cooper, W., Rogers, D., Beaton, S., Hendershot, R., Elkins, J., Fahey, D., Gao, R., Schwarz, J., Moore, F., Montzka, S., Perring, A., Hurst, D., Miller, B., Sweeney, C., Oltmans, S., Hintsa, E., Nance, D., Dutton, G., Watts, L., Spackman, J., Rosenlof, K., Ray, E., Hall, B., Zondlo, M., Diao, M., Keeling, R., Bent, J., Atlas, E., Lueb, R., and Mahoney, M.: HIPPO Combined Discrete Flask and GC Sample GHG, Halocarbon, and Hydrocarbon Data, version 1.0, Earth Observing Laboratory (EOL) data archive [data set], https://doi.org/10.3334/CDIAC/HIPPO_012, 2017. a
Wofsy, S., Afshar, S., Allen, H., Apel, E., Asher, E., Barletta, B., Bent, J., Bian, H., Biggs, B., Blake, D., Blake, N., Bourgeois, I., Brock, C., Brune, W., Budney, J., Bui, T., Butler, A., Campuzano-Jost, P., Chang, C., Chin, M., Commane, R., Correa, G., Crounse, J., Cullis, P. D., Daube, B., Day, D., Dean-Day, J., Dibb, J., DiGangi, J., Diskin, G., Dollner, M., Elkins, J., Erdesz, F., Fiore, A., Flynn, C., Froyd, K., Gesler, D., Hall, S., Hanisco, T., Hannun, R., Hills, A., Hintsa, E., Hoffman, A., Hornbrook, R., Huey, L., Hughes, S., Jimenez, J., Johnson, B., Katich, J., Keeling, R., Kim, M., Kupc, A., Lait, L., McKain, K., Mclaughlin, R., Meinardi, S., Miller, D., Montzka, S., Moore, F., Morgan, E., Murphy, D., Murray, L., Nault, B., Neuman, J., Newman, P., Nicely, J., Pan, X., Paplawsky, W., Peischl, J., Prather, M., Price, D., Ray, E., Reeves, J., Richardson, M., Rollins, A., Rosenlof, K., Ryerson, T., Scheuer, E., Schill, G., Schroder, J., Schwarz, J., St.Clair, J., Steenrod, S., Stephens, B., Strode, S., Sweeney, C., Tanner, D., Teng, A., Thames, A., Thompson, C., Ullmann, K., Veres, P., Wagner, N., Watt, A., Weber, R., Weinzierl, B., Wennberg, P., Williamson, C., Wilson, J., Wolfe, G., Woods, C., Zeng, L., and Vieznor, N.: ATom: Merged Atmospheric Chemistry, Trace Gases, and Aerosols, version 2, Earth Science Data Systems (ESDS) Program [data set], https://doi.org/10.3334/ORNLDAAC/1925, 2021. a
Wofsy, S. C.: HIAPER Pole-to-Pole Observations (HIPPO): fine-grained, global-scale measurements of climatically important atmospheric gases and aerosols, Philos. T. R. Soc. A., 369, 2073–2086, https://doi.org/10.1098/rsta.2010.0313, 2011. a
Yan, X., Konopka, P., Hauck, M., Podglajen, A., and Ploeger, F.: Asymmetry and pathways of inter-hemispheric transport in the upper troposphere and lower stratosphere, Atmos. Chem. Phys., 21, 6627–6645, https://doi.org/10.5194/acp-21-6627-2021, 2021. a
Yang, H., Waugh, D. W., Orbe, C., Patra, P. K., Jöckel, P., Lamarque, J.-F., Tilmes, S., Kinnison, D., Elkins, J. W., and Dlugokencky, E. J.: Evaluating Simulations of Interhemispheric Transport: Interhemispheric Exchange Time Versus SF6 Age, Geophys. Res. Lett., 46, 1113–1120, https://doi.org/10.1029/2018GL080960, 2019. a, b, c, d
Zahn, A., Weppner, J., Widmann, H., Schlote-Holubek, K., Burger, B., Kühner, T., and Franke, H.: A fast and precise chemiluminescence ozone detector for eddy flux and airborne application, Atmos. Meas. Tech., 5, 363–375, https://doi.org/10.5194/amt-5-363-2012, 2012. a
Short summary
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.
We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived...
Altmetrics
Final-revised paper
Preprint