Articles | Volume 14, issue 6
https://doi.org/10.5194/amt-14-4669-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-14-4669-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
23 Jun 2021
Research article |
| 23 Jun 2021
| 23 Jun 2021
An indirect-calibration method for non-target quantification of trace gases applied to a time series of fourth-generation synthetic halocarbons at the Taunus Observatory (Germany)
Fides Lefrancois
CORRESPONDING AUTHOR
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Markus Jesswein
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Markus Thoma
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Andreas Engel
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Kieran Stanley
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
Tanja Schuck
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt, Germany
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EGUsphere, https://doi.org/10.5194/egusphere-2026-2799, https://doi.org/10.5194/egusphere-2026-2799, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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In this study, we calculate the mean lifetime of carbonyl sulfide (COS) and methane (CH4) in the stratosphere from continuous vertical profiles sampled with balloon-borne instruments. We used two methods based on the stratospheric relationship of these gas species with N2O. The estimated stratospheric lifetime range is 69–90 years for COS and 146–172 years for CH4. These results are consistent with other studies and suggest no long-term trends in the stratospheric lifetime of these gas species.
Hélène De Longueville, Daniela B. Melo, Alison L. Redington, Alice Ramsden, Alexandre Danjou, Peter Andrews, Joseph Pitt, Brendan Murphy, Lionel Constantin, Kieran M. Stanley, Simon O'Doherty, Angelina Wenger, Dickon Young, Andreas Engel, Tanja Schuck, Katharina Meixner, Thomas Wagenhaeuser, Fides Gad, Martin K. Vollmer, Stefan Reimann, Michela Maoine, Jgor Arduini, Chris Lunder, Norbert Schmidtbauer, László Haszpra, Mihály Molnár, Arnoud Frumau, Cedric Couret, Matthew Rigby, Stephan Henne, Alistair Manning, and Anita L. Ganesan
Atmos. Chem. Phys., 26, 7647–7675, https://doi.org/10.5194/acp-26-7647-2026, https://doi.org/10.5194/acp-26-7647-2026, 2026
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This study estimates emissions of hydrofluorocarbons, potent greenhouse gases, in north-western Europe using atmospheric observations and atmospheric modelling. The estimates are compared with nationally reported emissions submitted to the United Nations. Overall, our results are consistent with reported values, although differences are found for some gases and countries. The findings indicate that emissions in north-western Europe are declining, reflecting the effects of climate regulations.
Emmal Safi, Joe Pitt, Grant Forster, Chris Rennick, Simon O’Doherty, Dickon Young, Kanokrat Charoenpornpukdee, Nick Garrard, Dafina Kikaj, Andrew Manning, Gerard Spain, Damien Martin, Morgan Lopez, Michel Ramonet, and Kieran Stanely
EGUsphere, https://doi.org/10.5194/egusphere-2026-1802, https://doi.org/10.5194/egusphere-2026-1802, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We compared whole and synthetic-air reference materials (RMs) for investigating offsets in greenhouse gas measurements so data from different sites/networks can be trusted when combined. By sending whole and synthetic-air (RMs) to six sites and measuring under routine field conditions, we found whole-air gives the most precise results, especially for carbon dioxide and nitrous oxide. Synthetic-air worked fairly well for methane but synthetic-air RMs needs lower uncertainty before wide use.
Martin K. Vollmer, Joseph R. Pitt, Dickon Young, Stephan Henne, Blagoj Mitrevski, Jens Mühle, Anita Ganesan, Jgor Arduini, Alistair J. Manning, Thomas Wagenhäuser, Alison L. Redington, Daniela B. Melo, Brendan Murphy, Ray Gluckmann, Kieran M. Stanley, Paul B. Krummel, Chris R. Lunder, Jaegeun Yun, Dominique Rust, Angelina Wenger, Myriam Guillevic, Jooil Kim, Ray H. J. Wang, Tae Siek Rhee, Lionel Constantin, Arnoud Frumau, Christina M. Harth, Peter K. Salameh, Ove Hermansen, Matthew Rigby, Luke M. Western, Andreas Engel, Simon O'Doherty, Sunyoung Park, Michela Maione, Paul J. Fraser, Ronald G. Prinn, Ray F. Weiss, and Stefan Reimann
Atmos. Chem. Phys., 26, 6993–7012, https://doi.org/10.5194/acp-26-6993-2026, https://doi.org/10.5194/acp-26-6993-2026, 2026
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Halogenated olefins (HFOs) are newly emerging compounds in the atmosphere. They are in reach of the definition of PFAS (Per- and polyfluoroalkyl substances) and some decay to the eternal chemical trifluoroacetate (TFA). We provide atmospheric measurements of three HFOs from the large Advanced Global Atmospheric Gases Experiment (AGAGE) network and estimate emissions for Northwest Europe for the first time. We find a quasi-ubiquitous presence in the atmosphere and rapidly increasing emissions.
Johannes Degen, Nicole Bobrowski, Mélisende M. Bossard, Lucie Boucher, Huilin Chen, Andreas Engel, Bastien H. Geil, Giovanni B. Giuffrida, Steven van Heuven, Thorsten Hoffmann, Niklas Karbach, Gianluigi Ortenzi, and Tanja J. Schuck
EGUsphere, https://doi.org/10.5194/egusphere-2026-1865, https://doi.org/10.5194/egusphere-2026-1865, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Observations in volcanic plumes often rely on Uncrewed Aerial Systems (UAS). In July 2024, we used the active AirCore technique with UAS to probe the plumes of Mount Etna (Italy). This was the first time to use this technique inside volcanic plumes. AirCore samples are stored in long coils for laboratory analyses delivering high-quality trace gas measurements. We observed enhanced mole fractions of CO2 and often also of CO. allowing conclusions on oxidation processes inside the crater.
Joseph R. Pitt, Dominique Rust, Anita Ganesan, Luke M. Western, Martin K. Vollmer, Jens Mühle, Tobias Bühlmann, Christina M. Harth, Stephen A. Montzka, Brad D. Hall, Isaac J. Vimont, Alistair J. Manning, Alison L. Redington, Stephan Henne, Daniela B. Melo, Saurabh Annadate, Lionel Constantin, Brendan M. Murphy, Matthew Rigby, Dickon Young, Simon O'Doherty, Angelina Wenger, Chris R. Lunder, Ove Hermansen, Thomas Wagenhäuser, Andreas Engel, Jgor Arduini, Michela Maione, Jaegeun Yun, Blagoj Mitrevski, Paul B. Krummel, Paul J. Fraser, Jooil Kim, Ray H. J. Wang, Tae Siek Rhee, Peter K. Salameh, T. Gerard Spain, Stefan Reimann, Ronald G. Prinn, Ray F. Weiss, and Kieran M. Stanley
EGUsphere, https://doi.org/10.5194/egusphere-2026-1589, https://doi.org/10.5194/egusphere-2026-1589, 2026
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1,2‑Dichloroethane (DCE) can contribute to the depletion of the stratospheric ozone layer. Whether DCE reaches the stratosphere depends on where and when it is emitted. We present the ongoing measurements of DCE from the AGAGE and NOAA global monitoring networks. For the period 2017–2023, our modelled average global emissions based on these observations align with another study, while regional estimates differ. This suggests remaining uncertainty in the geographical distribution of emissions.
Alice Emily Ramsden, Anita Ganesan, Matthew Rigby, Chris Rennick, Tim Arnold, Emmal Safi, Edward Chung, Dafina Kikaj, Cameron Yeo, Dave Lowry, Pete Levy, Simon O'Doherty, Kieran Stanley, Dickon Young, Joe Pitt, Damien Martin, Morgan Lopez, Michel Ramonet, Grant Forster, Arnoud Frumau, and Alistair Manning
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Methane is emitted from a range of anthropogenic and natural sources, each with a characteristic isotope ratio signature. We present a method for estimating emissions from multiple sources using isotopic signatures and observations of atmospheric methane isotope ratios. We show the importance of considering isotopic signature uncertainty and demonstrate how our current understanding of these signatures may be limiting this method’s ability to reduce uncertainties in emissions estimates.
Benjamin Püschel, Martin Vojta, Luise Kandler, Molly Crotwell, Andreas Engel, Paul B. Krummel, Chris R. Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Thomas Wagenhäuser, Ray F. Weiss, Dickon Young, and Andreas Stohl
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We present global and regionally resolved emissions of the two highly potent greenhouse gases CF4 and C2F6 from 2006 to 2023, based on atmospheric measurements and transport modeling. In nearly all regions studied, our results show that national reports and industry-based data underestimate emissions. While emissions in Europe and the U.S. declined, we find rising emissions in South, Southeast, and East Asia. China and India are the major contributors to global emissions in recent years.
Luke M. Western, Stephen Bourguet, Molly Crotwell, Lei Hu, Paul B. Krummel, Hélène De Longueville, Alistair J. Manning, Jens Mühle, Dominique Rust, Isaac Vimont, Martin K. Vollmer, Minde An, Jgor Arduini, Andreas Engel, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Chris Lunder, Michela Maione, Stephen A. Montzka, David Nance, Simon O'Doherty, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Roland Schmidt, Kieran M. Stanley, Thomas Wagenhäuser, Dickon Young, Matt Rigby, Ronald G. Prinn, and Ray F. Weiss
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Earth Syst. Sci. Data, 17, 6557–6582, https://doi.org/10.5194/essd-17-6557-2025, https://doi.org/10.5194/essd-17-6557-2025, 2025
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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 emissions of these gases to the atmosphere. 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.
Johannes Degen, Bianca C. Baier, Patrick Jöckel, J. Moritz Menken, Tanja J. Schuck, Colm Sweeney, and Andreas Engel
Atmos. Chem. Phys., 25, 15741–15763, https://doi.org/10.5194/acp-25-15741-2025, https://doi.org/10.5194/acp-25-15741-2025, 2025
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We investigate the distribution of CO2 in the upper troposphere and lower stratosphere using both, observations and an atmospheric model. Simulating an artificial tracer, we separate CO2 seasonality from long-term trend and transport variability. We found that patterns in the seasonal signal are attributable to large-scale transport features like the subtropical jet or the Brewer-Dobson circulation. Being a powerful diagnostic tool we recommend to use this tracer for model intercomparisons.
Martin Vojta, Andreas Plach, Rona L. Thompson, Pallav Purohit, Kieran Stanley, Simon O'Doherty, Dickon Young, Joe Pitt, Jgor Arduini, Xin Lan, and Andreas Stohl
Atmos. Chem. Phys., 25, 15197–15243, https://doi.org/10.5194/acp-25-15197-2025, https://doi.org/10.5194/acp-25-15197-2025, 2025
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We determine European emissions of the highly potent greenhouse gas sulfur hexafluoride from 2005 to 2021 – focusing on high-emitting countries and the aggregated EU-27 emissions. Emissions declined in most regions, likely due to EU F-gas regulations. However, our results reveal that most studied countries underestimate their emissions in their national reports. Our sensitivity tests highlight the importance of dense observational networks for reliable inversion-based emission estimates.
Gerald Wetzel, Anne Kleinert, Sören Johansson, Felix Friedl-Vallon, Michael Höpfner, Jörn Ungermann, Tom Neubert, Valéry Catoire, Cyril Crevoisier, Andreas Engel, Thomas Gulde, Patrick Jacquet, Oliver Kirner, Erik Kretschmer, Thomas Kulessa, Johannes C. Laube, Guido Maucher, Hans Nordmeyer, Christof Piesch, Peter Preusse, Markus Retzlaff, Georg Schardt, Johan Schillings, Herbert Schneider, Axel Schönfeld, Tanja Schuck, Wolfgang Woiwode, Martin Riese, and Peter Braesicke
Atmos. Meas. Tech., 18, 5873–5894, https://doi.org/10.5194/amt-18-5873-2025, https://doi.org/10.5194/amt-18-5873-2025, 2025
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We present vertical trace gas profiles from the first balloon flight of the newly developed GLORIA-B limb-imaging Fourier-Transform spectrometer. Longer-lived gases are compared to external measurements to assess the quality of the GLORIA-B observations. Diurnal changes of photochemically active species are compared to model simulations. GLORIA-B demonstrates the capability of balloon-borne limb imaging to provide high-resolution vertical profiles of trace gases up to the middle stratosphere.
Sophie Bauchinger, Andreas Engel, Markus Jesswein, Timo Keber, Harald Bönisch, Florian Obersteiner, Andreas Zahn, Nicolas Emig, Peter Hoor, Hans-Christoph Lachnitt, Franziska Weyland, Linda Ort, and Tanja J. Schuck
Atmos. Chem. Phys., 25, 14167–14186, https://doi.org/10.5194/acp-25-14167-2025, https://doi.org/10.5194/acp-25-14167-2025, 2025
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We compared different ways to define the upper barrier of the troposphere in the extra-tropics, the “tropopause”. By analysing ozone distributions sorted by different definitions, we found that the traditional temperature-based tropopause works less well than dynamic or tracer-based definitions. We saw a sharper transition of ozone across the tropopause using a higher value of potential vorticity than often used and recommend this value for future studies of exchange processes in this region.
Johannes C. Laube, Tanja J. Schuck, Sophie Baartman, Huilin Chen, Markus Geldenhuys, Steven van Heuven, Timo Keber, Maria Elena Popa, Elinor Tuffnell, Florian Voet, Bärbel Vogel, Thomas Wagenhäuser, Alessandro Zanchetta, and Andreas Engel
Atmos. Meas. Tech., 18, 4087–4102, https://doi.org/10.5194/amt-18-4087-2025, https://doi.org/10.5194/amt-18-4087-2025, 2025
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A large balloon was launched in summer 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km, above the reach of aircraft. The main aims were to evaluate different techniques and atmospheric processes. We focus on halogenated greenhouse gases and ozone-depleting substances. For this, air was collected with the AirCore technique and a cryogenic air sampler and measured after the flight. A companion paper reports observations of major greenhouse gases.
Markus Jesswein, Valentin Lauther, Nicolas Emig, Peter Hoor, Timo Keber, Hans-Christoph Lachnitt, Linda Ort, Tanja Schuck, Johannes Strobel, Ronja Van Luijt, C. Michael Volk, Franziska Weyland, and Andreas Engel
Atmos. Chem. Phys., 25, 8107–8126, https://doi.org/10.5194/acp-25-8107-2025, https://doi.org/10.5194/acp-25-8107-2025, 2025
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The study investigates transport within the Asian Summer Monsoon, focusing on how CH2Cl2 reaches the subarctic tropopause region. Using data from the PHILEAS campaign in 2023, events with increased mixing ratios were detected. Their origin, the transport paths to the tropopause region, and the potential entry into the stratosphere were analyzed. The East Asian Summer Monsoon was identified as the main transport pathway, with only a small contribution to the stratosphere in the following days.
Tanja J. Schuck, Johannes Degen, Timo Keber, Katharina Meixner, Thomas Wagenhäuser, Mélanie Ghysels, Georges Durry, Nadir Amarouche, Alessandro Zanchetta, Steven van Heuven, Huilin Chen, Johannes C. Laube, Sophie L. Baartman, Carina van der Veen, Maria Elena Popa, and Andreas Engel
Atmos. Chem. Phys., 25, 4333–4348, https://doi.org/10.5194/acp-25-4333-2025, https://doi.org/10.5194/acp-25-4333-2025, 2025
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A balloon was launched in 2021 in the Arctic to carry instruments for trace gas measurements up to 32 km. One purpose was to compare measurement techniques. We focus on the major greenhouse gases. To measure these, air was sampled with the AirCore technique and with flask sampling, and samples were analysed after the flight. In flight, observations were done with an optical method. In a companion paper, we report on observations of chlorine and bromine containing trace gases.
Laura N. Saunders, Kaley A. Walker, Gabriele P. Stiller, Thomas von Clarmann, Florian Haenel, Hella Garny, Harald Bönisch, Chris D. Boone, Ariana E. Castillo, Andreas Engel, Johannes C. Laube, Marianna Linz, Felix Ploeger, David A. Plummer, Eric A. Ray, and Patrick E. Sheese
Atmos. Chem. Phys., 25, 4185–4209, https://doi.org/10.5194/acp-25-4185-2025, https://doi.org/10.5194/acp-25-4185-2025, 2025
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We present a 17-year stratospheric age-of-air dataset derived from ACE-FTS satellite measurements of sulfur hexafluoride. This is the longest continuous, global, and vertically resolved age of air time series available to date. In this paper, we show that this dataset agrees well with age-of-air datasets based on measurements from other instruments. We also present trends in the midlatitude lower stratosphere that indicate changes in the global circulation that are predicted by climate models.
Dafina Kikaj, Edward Chung, Alan D. Griffiths, Scott D. Chambers, Grant Forster, Angelina Wenger, Penelope Pickers, Chris Rennick, Simon O'Doherty, Joseph Pitt, Kieran Stanley, Dickon Young, Leigh S. Fleming, Karina Adcock, Emmal Safi, and Tim Arnold
Atmos. Meas. Tech., 18, 151–175, https://doi.org/10.5194/amt-18-151-2025, https://doi.org/10.5194/amt-18-151-2025, 2025
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We present a protocol to improve confidence in atmospheric radon measurements, enabling site comparisons and integration with greenhouse gas data. As a natural tracer, radon provides an independent check of transport model performance. This standardized method enhances radon’s use as a metric for model evaluation. Beyond UK observatories, it can support broader networks like ICOS and WMO/GAW, advancing global atmospheric research.
Felicia Kolonjari, Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, David A. Plummer, Andreas Engel, Stephen A. Montzka, David E. Oram, Tanja Schuck, Gabriele P. Stiller, and Geoffrey C. Toon
Atmos. Meas. Tech., 17, 2429–2449, https://doi.org/10.5194/amt-17-2429-2024, https://doi.org/10.5194/amt-17-2429-2024, 2024
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The Canadian Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) satellite instrument is currently providing the only vertically resolved chlorodifluoromethane (HCFC-22) measurements from space. This study assesses the most current ACE-FTS HCFC-22 data product in the upper troposphere and lower stratosphere, as well as modelled HCFC-22 from a 39-year run of the Canadian Middle Atmosphere Model (CMAM39) in the same region.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
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
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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.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
Markus Thoma, Franziska Bachmeier, Felix Leonard Gottwald, Mario Simon, and Alexander Lucas Vogel
Atmos. Meas. Tech., 15, 7137–7154, https://doi.org/10.5194/amt-15-7137-2022, https://doi.org/10.5194/amt-15-7137-2022, 2022
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We introduce the aerosolomics database and apply it to particulate matter samples. Nine VOCs were oxidized under various conditions in an oxidation flow reactor, and the formed SOA was measured using liquid chromatography mass spectrometry. With the database, an unambiguous top-down attribution of atmospheric oxidation products to their parent VOCs is now possible. Combining the database with hierarchical clustering enables a better understanding of sources, formation, and partitioning of SOA.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
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
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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
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Airborne observations were conducted in the lowermost Arctic stratosphere during the winter of 2015/2016. The observed distribution of reactive nitrogen shows clear indications of nitrification in mid-winter and denitrification in late winter. This was caused by the formation of polar stratospheric cloud particles, which were observed during several flights. The sedimentation and evaporation of these particles and the descent of air masses cause a redistribution of reactive nitrogen.
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
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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.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
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
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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.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Alistair J. Manning, Alison L. Redington, Daniel Say, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Martin K. Vollmer, Jens Mühle, Jgor Arduini, Gerard Spain, Adam Wisher, Michela Maione, Tanja J. Schuck, Kieran Stanley, Stefan Reimann, Andreas Engel, Paul B. Krummel, Paul J. Fraser, Christina M. Harth, Peter K. Salameh, Ray F. Weiss, Ray Gluckman, Peter N. Brown, John D. Watterson, and Tim Arnold
Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, https://doi.org/10.5194/acp-21-12739-2021, 2021
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This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs)) using high-quality atmospheric observations and atmospheric modelling. We compare these estimates with those submitted by the UK to the United Nations. We conclude that global concentrations of these gases are still increasing. Our estimates for the UK are 73 % of those reported and that the UK emissions are now falling, demonstrating an impact of UK government policy.
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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.
Synthetic halocarbons can contribute to stratospheric ozone depletion or to climate change. In...
