Articles | Volume 21, issue 22
https://doi.org/10.5194/acp-21-16955-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-16955-2021
© 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 Nov 2021
Research article |
| 23 Nov 2021
| 23 Nov 2021
Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
Norwegian Institute for Air Research (NILU), Kjeller, Norway
Centre National de Recherches Météorologiques, Université
de Toulouse, Météo-France, CNRS, Toulouse, France
Virginie Marécal
Centre National de Recherches Météorologiques, Université
de Toulouse, Météo-France, CNRS, Toulouse, France
Ryan Hossaini
Lancaster Environment Centre, Lancaster University, Lancaster, LA1
4YQ, UK
Michel Pirre
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace,
CNRS and University of Orléans, UMR7328, Orléans, France
retired
Gisèle Krysztofiak
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace,
CNRS and University of Orléans, UMR7328, Orléans, France
Franziska Ziska
GEOMAR Helmholtz Centre for Ocean Research Kiel, Kiel, Germany
Andreas Engel
Institute for Atmospheric and Environmental Sciences, University of
Frankfurt, Altenhöferallee 1, 60438 Frankfurt, Germany
Stephan Sala
Institute for Atmospheric and Environmental Sciences, University of
Frankfurt, Altenhöferallee 1, 60438 Frankfurt, Germany
Timo Keber
Institute for Atmospheric and Environmental Sciences, University of
Frankfurt, Altenhöferallee 1, 60438 Frankfurt, Germany
Harald Bönisch
Institute for Atmospheric and Environmental Sciences, University of
Frankfurt, Altenhöferallee 1, 60438 Frankfurt, Germany
Elliot Atlas
University of Miami, 4600 Rickenbacker Causeway, Miami, FL 33149, USA
Kirstin Krüger
Department of Geosciences, University of Oslo, Postboks 1022,
Blindern, 0315 Oslo, Norway
Martyn Chipperfield
School of Earth
and Environment, University of Leeds, Leeds, UK
Valery Catoire
Laboratoire de Physique et Chimie de l'Environnement et de l'Espace,
CNRS and University of Orléans, UMR7328, Orléans, France
Azizan A. Samah
National Antarctic Research Centre, University of Malaya, Kuala
Lumpur 50603, Malaysia
Institute of Ocean and Earth Sciences, University of Malaya, 50603
Kuala Lumpur, Malaysia
Marcel Dorf
Department of Atmospheric
Chemistry, Max Planck Institute for Chemistry, Mainz, Germany
Phang Siew Moi
Institute of Ocean and Earth Sciences, University of Malaya, 50603
Kuala Lumpur, Malaysia
Hans Schlager
Institut für Physik der Atmosphäre, Deutsches Zentrum für Luft- und Raumfahrt (DLR), Atmosphärische Spurenstoffe, Münchner
Straße 20, 82234 Oberpfaffenhofen-Wessling, Germany
Klaus Pfeilsticker
Institute of Environmental Physics, Ruprecht-Karls-Universität
Heidelberg, Im Neuenheimer Feld 229, 69120 Heidelberg, Germany
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Michael P. Cartwright, Jeremy J. Harrison, David P. Moore, Richard J. Pope, Martyn P. Chipperfield, Chris Wilson, and Wuhu Feng
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Douwang Li, Zhe Wang, Siyi Zhao, Jiankai Zhang, Wuhu Feng, and Martyn P. Chipperfield
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Tómas Zoëga, Trude Storelvmo, and Kirstin Krüger
Atmos. Chem. Phys., 25, 2989–3010, https://doi.org/10.5194/acp-25-2989-2025, https://doi.org/10.5194/acp-25-2989-2025, 2025
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Jamal Makkor, Mathias Palm, Matthias Buschmann, Emmanuel Mahieu, Martyn P. Chipperfield, and Justus Notholt
Atmos. Meas. Tech., 18, 1105–1114, https://doi.org/10.5194/amt-18-1105-2025, https://doi.org/10.5194/amt-18-1105-2025, 2025
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Johannes Schneider, Christiane Schulz, Florian Rubach, Anna Ludwig, Jonas Wilsch, Philipp Joppe, Christian Gurk, Sergej Molleker, Laurent Poulain, Florian Obersteiner, Torsten Gehrlein, Harald Bönisch, Andreas Zahn, Peter Hoor, Nicolas Emig, Heiko Bozem, Stephan Borrmann, and Markus Hermann
EGUsphere, https://doi.org/10.5194/egusphere-2024-3969, https://doi.org/10.5194/egusphere-2024-3969, 2025
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Joan Stude, Heinfried Aufmhoff, Hans Schlager, Markus Rapp, Carsten Baumann, Frank Arnold, and Boris Strelnikov
Atmos. Chem. Phys., 25, 383–396, https://doi.org/10.5194/acp-25-383-2025, https://doi.org/10.5194/acp-25-383-2025, 2025
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We used a mass spectrometer on a rocket to analyze natural ions at altitudes between 60 and 120 km. Our instrument was launched in 2018 and 2021 from Norway. The heaviest particles were detected around 80 km, while medium particles could be found even above 100 km. Our measurements show that different particles are formed and not just one predominating compound. The most likely compounds that form meteor smoke particles in our measurements are made up of oxides of iron, magnesium and silicon.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Wuhu Feng, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-3717, https://doi.org/10.5194/egusphere-2024-3717, 2024
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Tropospheric ozone (O3) is a harmful secondary atmospheric pollutant and an important greenhouse gas. Here, we present an in-depth analysis of lower-tropospheric sub-column O3 (LTCO3, surface – 6 km) records from three satellite products produced by the Rutherford Appleton Laboratory (RAL) over Europe between 1996 and 2017. Overall, we detect moderate negative trends in the satellite records, but corresponding model simulations and ozonesonde measurements show negligible trends.
Fang Li, Xiang Song, Sandy P. Harrison, Jennifer R. Marlon, Zhongda Lin, L. Ruby Leung, Jörg Schwinger, Virginie Marécal, Shiyu Wang, Daniel S. Ward, Xiao Dong, Hanna Lee, Lars Nieradzik, Sam S. Rabin, and Roland Séférian
Geosci. Model Dev., 17, 8751–8771, https://doi.org/10.5194/gmd-17-8751-2024, https://doi.org/10.5194/gmd-17-8751-2024, 2024
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This study provides the first comprehensive assessment of historical fire simulations from 19 Earth system models in phase 6 of the Coupled Model Intercomparison Project (CMIP6). Most models reproduce global totals, spatial patterns, seasonality, and regional historical changes well but fail to simulate the recent decline in global burned area and underestimate the fire response to climate variability. CMIP6 simulations address three critical issues of phase-5 models.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn P. Chipperfield, Wuhu Feng, David E. Oram, Karina E. Adcock, Stephen A. Montzka, Isobel J. Simpson, Andrea Mazzeo, Amber A. Leeson, Elliot Atlas, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 13457–13475, https://doi.org/10.5194/acp-24-13457-2024, https://doi.org/10.5194/acp-24-13457-2024, 2024
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DCE (1,2-dichloroethane) is an industrial chemical used to produce PVC (polyvinyl chloride). We analysed DCE production data to estimate global DCE emissions (2002–2020). The emissions were included in an atmospheric model and evaluated by comparing simulated DCE to DCE measurements in the troposphere. We show that DCE contributes ozone-depleting Cl to the stratosphere and that this has increased with increasing DCE emissions. DCE’s impact on stratospheric O3 is currently small but non-zero.
Phuc Thi Minh Ha, Yugo Kanaya, Kazuyo Yamaji, Syuichi Itahashi, Satoru Chatani, Takashi Sekiya, Maria Dolores Andrés Hernández, John Philip Burrows, Hans Schlager, Michael Lichtenstern, Mira Poehlker, and Bruna Holanda
EGUsphere, https://doi.org/10.5194/egusphere-2024-2064, https://doi.org/10.5194/egusphere-2024-2064, 2024
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Black carbon and CO are important to climate change. EMeRGe airborne observation can identify the suitability of emission inventories used in CMAQv5.0.2 model for Asian polluted regions. GFEDv4.1s is suitable for fire emissions. Anthropogenic BC and CO emissions from Philippines (REASv2.1) are insufficient. The estimated Chinese emissions in 2018 are 0.65±0.25 TgBC, 166±65 TgCO and 12.4±4.8 PgCO2, suggesting a reduction and increment for China's BC and CO emissions in the HTAPv2.2z inventory.
Theresa Harlass, Rebecca Dischl, Stefan Kaufmann, Raphael Märkl, Daniel Sauer, Monika Scheibe, Paul Stock, Tiziana Bräuer, Andreas Dörnbrack, Anke Roiger, Hans Schlager, Ulrich Schumann, Magdalena Pühl, Tobias Schripp, Tobias Grein, Linda Bondorf, Charles Renard, Maxime Gauthier, Mark Johnson, Darren Luff, Paul Madden, Peter Swann, Denise Ahrens, Reetu Sallinen, and Christiane Voigt
Atmos. Chem. Phys., 24, 11807–11822, https://doi.org/10.5194/acp-24-11807-2024, https://doi.org/10.5194/acp-24-11807-2024, 2024
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Emissions from aircraft have a direct impact on our climate. Here, we present airborne and ground-based measurement data of nitrogen oxides that were collected in the exhaust of an Airbus aircraft. We study the impact of burning fossil and sustainable aviation fuel on nitrogen oxide emissions at different engine settings related to combustor temperature, pressure and fuel flow. Further, we compare observations with engine emission models.
Chris Wilson, Brian J. Kerridge, Richard Siddans, David P. Moore, Lucy J. Ventress, Emily Dowd, Wuhu Feng, Martyn P. Chipperfield, and John J. Remedios
Atmos. Chem. Phys., 24, 10639–10653, https://doi.org/10.5194/acp-24-10639-2024, https://doi.org/10.5194/acp-24-10639-2024, 2024
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The leaks from the Nord Stream gas pipelines in September 2022 released a large amount of methane (CH4) into the atmosphere. We provide observational data from a satellite instrument that shows a large CH4 plume over the North Sea off the coast of Scandinavia. We use this together with atmospheric models to quantify the CH4 leaked into the atmosphere from the pipelines. We find that 219–427 Gg CH4 was emitted, making this the largest individual fossil-fuel-related CH4 leak on record.
Richard J. Pope, Fiona M. O'Connor, Mohit Dalvi, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Brice Barret, Eric Le Flochmoen, Anne Boynard, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, Catherine Wespes, and Richard Rigby
Atmos. Chem. Phys., 24, 9177–9195, https://doi.org/10.5194/acp-24-9177-2024, https://doi.org/10.5194/acp-24-9177-2024, 2024
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Ozone is a potent air pollutant in the lower troposphere, with adverse impacts on human health. Satellite records of tropospheric ozone currently show large-scale inconsistencies in long-term trends. Our detailed study of the potential factors (e.g. satellite errors, where the satellite can observe ozone) potentially driving these inconsistencies found that, in North America, Europe, and East Asia, the underlying trends are typically small with large uncertainties.
Karolin Voss, Philip Holzbeck, Klaus Pfeilsticker, Ralph Kleinschek, Gerald Wetzel, Blanca Fuentes Andrade, Michael Höpfner, Jörn Ungermann, Björn-Martin Sinnhuber, and André Butz
Atmos. Meas. Tech., 17, 4507–4528, https://doi.org/10.5194/amt-17-4507-2024, https://doi.org/10.5194/amt-17-4507-2024, 2024
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A novel balloon-borne instrument for direct sun and solar occultation measurements of several UV–Vis absorbing gases (e.g. O3, NO2, BrO, IO, and HONO) is described. Its major design features and performance during two stratospheric deployments are discussed. From the measured overhead BrO concentration and a suitable photochemical correction, total stratospheric bromine is inferred to (17.5 ± 2.2) ppt in air masses which entered the stratosphere around early 2017 ± 1 year.
Yang Li, Wuhu Feng, Xin Zhou, Yajuan Li, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 8277–8293, https://doi.org/10.5194/acp-24-8277-2024, https://doi.org/10.5194/acp-24-8277-2024, 2024
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The Tibetan Plateau (TP), the highest and largest plateau, experiences strong surface solar UV radiation, whose excess can cause harmful influences on local biota. Hence, it is critical to study TP ozone. We find ENSO, the strongest interannual phenomenon, tends to induce tropospheric temperature change and thus modulate tropopause variability, which in turn favours ozone change over the TP. Our results have implications for a better understanding of the interannual variability of TP ozone.
Nelson Bègue, Alexandre Baron, Gisèle Krysztofiak, Gwenaël Berthet, Corinna Kloss, Fabrice Jégou, Sergey Khaykin, Marion Ranaivombola, Tristan Millet, Thierry Portafaix, Valentin Duflot, Philippe Keckhut, Hélène Vérèmes, Guillaume Payen, Mahesh Kumar Sha, Pierre-François Coheur, Cathy Clerbaux, Michaël Sicard, Tetsu Sakai, Richard Querel, Ben Liley, Dan Smale, Isamu Morino, Osamu Uchino, Tomohiro Nagai, Penny Smale, John Robinson, and Hassan Bencherif
Atmos. Chem. Phys., 24, 8031–8048, https://doi.org/10.5194/acp-24-8031-2024, https://doi.org/10.5194/acp-24-8031-2024, 2024
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During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean basin experienced significant perturbations. Numerical models indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers.
Luis F. Millán, Peter Hoor, Michaela I. Hegglin, Gloria L. Manney, Harald Boenisch, Paul Jeffery, Daniel Kunkel, Irina Petropavlovskikh, Hao Ye, Thierry Leblanc, and Kaley Walker
Atmos. Chem. Phys., 24, 7927–7959, https://doi.org/10.5194/acp-24-7927-2024, https://doi.org/10.5194/acp-24-7927-2024, 2024
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In the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we have mapped multiplatform ozone datasets into coordinate systems to systematically evaluate the influence of these coordinates on binned climatological variability. This effort unifies the work of studies that focused on individual coordinate system variability. Our goal was to create the most comprehensive assessment of this topic.
Andrea E. Gordon, Cameron R. Homeyer, Jessica B. Smith, Rei Ueyama, Jonathan M. Dean-Day, Elliot L. Atlas, Kate Smith, Jasna V. Pittman, David S. Sayres, David M. Wilmouth, Apoorva Pandey, Jason M. St. Clair, Thomas F. Hanisco, Jennifer Hare, Reem A. Hannun, Steven Wofsy, Bruce C. Daube, and Stephen Donnelly
Atmos. Chem. Phys., 24, 7591–7608, https://doi.org/10.5194/acp-24-7591-2024, https://doi.org/10.5194/acp-24-7591-2024, 2024
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In situ airborne observations of ongoing tropopause-overshooting convection and an above-anvil cirrus plume from the 31 May 2022 flight of the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) field campaign are examined. Upper troposphere and lower stratosphere composition changes are evaluated along with possible contributing dynamical and physical processes. Measurements reveal multiple changes in air mass composition and stratospheric hydration throughout the flight.
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, and Stephan Borrmann
Atmos. Chem. Phys., 24, 7499–7522, https://doi.org/10.5194/acp-24-7499-2024, https://doi.org/10.5194/acp-24-7499-2024, 2024
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From aircraft measurements in the upper troposphere/lower stratosphere, we find a correlation between the ozone and particulate sulfate in the lower stratosphere. The correlation exhibits some variability over the measurement period exceeding the background sulfate-to-ozone correlation. From our analysis, we conclude that gas-to-particle conversion of volcanic sulfur dioxide leads to observed enhanced sulfate aerosol mixing ratios.
Dennis Booge, Jerry F. Tjiputra, Dirk J. L. Olivié, Birgit Quack, and Kirstin Krüger
Earth Syst. Dynam., 15, 801–816, https://doi.org/10.5194/esd-15-801-2024, https://doi.org/10.5194/esd-15-801-2024, 2024
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Oceanic bromoform, produced by algae, is an important precursor of atmospheric bromine, highlighting the importance of implementing these emissions in climate models. The simulated mean oceanic concentrations align well with observations, while the mean atmospheric values are lower than the observed ones. Modelled annual mean emissions mostly occur from the sea to the air and are driven by oceanic concentrations, sea surface temperature, and wind speed, which depend on season and location.
Zhihong Zhuo, Herman F. Fuglestvedt, Matthew Toohey, and Kirstin Krüger
Atmos. Chem. Phys., 24, 6233–6249, https://doi.org/10.5194/acp-24-6233-2024, https://doi.org/10.5194/acp-24-6233-2024, 2024
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This work simulated volcanic eruptions with varied eruption source parameters under different initial conditions with a fully coupled Earth system model. We show that initial atmospheric conditions control the meridional distribution of volcanic volatiles and modulate volcanic forcing and subsequent climate and environmental impacts of tropical and Northern Hemisphere extratropical eruptions. This highlights the potential for predicting these impacts as early as the first post-eruption month.
Safae Oumami, Joaquim Arteta, Vincent Guidard, Pierre Tulet, and Paul David Hamer
Geosci. Model Dev., 17, 3385–3408, https://doi.org/10.5194/gmd-17-3385-2024, https://doi.org/10.5194/gmd-17-3385-2024, 2024
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In this paper, we coupled the SURFEX and MEGAN models. The aim of this coupling is to improve the estimation of biogenic fluxes by using the SURFEX canopy environment model. The coupled model results were validated and several sensitivity tests were performed. The coupled-model total annual isoprene flux is 442 Tg; this value is within the range of other isoprene estimates reported. The ultimate aim of this coupling is to predict the impact of climate change on biogenic 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
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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.
Santo Fedele Colosimo, Nathaniel Brockway, Vijay Natraj, Robert Spurr, Klaus Pfeilsticker, Lisa Scalone, Max Spolaor, Sarah Woods, and Jochen Stutz
Atmos. Meas. Tech., 17, 2367–2385, https://doi.org/10.5194/amt-17-2367-2024, https://doi.org/10.5194/amt-17-2367-2024, 2024
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Cirrus clouds are poorly understood components of the climate system, in part due to the challenge of observing thin, sub-visible ice clouds. We address this issue with a new observational approach that uses the remote sensing of near-infrared ice water absorption features from a high-altitude aircraft. We describe the underlying principle of this approach and present a new procedure to retrieve ice concentration in cirrus clouds. Our retrievals compare well with in situ observations.
Hella Garny, Roland Eichinger, Johannes C. Laube, Eric A. Ray, Gabriele P. Stiller, Harald Bönisch, Laura Saunders, and Marianna Linz
Atmos. Chem. Phys., 24, 4193–4215, https://doi.org/10.5194/acp-24-4193-2024, https://doi.org/10.5194/acp-24-4193-2024, 2024
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Transport circulation in the stratosphere is important for the distribution of tracers, but its strength is hard to measure. Mean transport times can be inferred from observations of trace gases with certain properties, such as sulfur hexafluoride (SF6). However, this gas has a chemical sink in the high atmosphere, which can lead to substantial biases in inferred transport times. In this paper we present a method to correct mean transport times derived from SF6 for the effects of chemical sinks.
Richard J. Pope, Alexandru Rap, Matilda A. Pimlott, Brice Barret, Eric Le Flochmoen, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Anne Boynard, Christian Retscher, Wuhu Feng, Richard Rigby, Sandip S. Dhomse, Catherine Wespes, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 3613–3626, https://doi.org/10.5194/acp-24-3613-2024, https://doi.org/10.5194/acp-24-3613-2024, 2024
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Tropospheric ozone is an important short-lived climate forcer which influences the incoming solar short-wave radiation and the outgoing long-wave radiation in the atmosphere (8–15 km) where the balance between the two yields a net positive (i.e. warming) effect at the surface. Overall, we find that the tropospheric ozone radiative effect ranges between 1.21 and 1.26 W m−2 with a negligible trend (2008–2017), suggesting that tropospheric ozone influences on climate have remained stable with time.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Lily Gouldsbrough, Ryan Hossaini, Emma Eastoe, Paul J. Young, and Massimo Vieno
Atmos. Chem. Phys., 24, 3163–3196, https://doi.org/10.5194/acp-24-3163-2024, https://doi.org/10.5194/acp-24-3163-2024, 2024
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High-resolution spatial fields of surface ozone are used to understand spikes in ozone concentration and predict their impact on public health. Such fields are routinely output from complex mathematical models for atmospheric conditions. These outputs are on a coarse spatial resolution and the highest concentrations tend to be biased. Using a novel data-driven machine learning methodology, we show how such output can be corrected to produce fields with both lower bias and higher resolution.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-516, https://doi.org/10.5194/egusphere-2024-516, 2024
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This study assesses atmospheric composition using air quality models during aircraft campaigns in Europe and Asia, focusing on carbonaceous aerosols and trace gases. While carbon monoxide is well modeled, other pollutants have moderate to weak agreement with observations. Wind speed modeling is reliable for identifying pollution plumes, where models tend to overestimate concentrations. This highlights challenges in accurately modeling aerosol and trace gas composition, particularly in cities.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-521, https://doi.org/10.5194/egusphere-2024-521, 2024
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This study explores the proportional relationships between carbonaceous aerosols (black and organic carbon) and trace gases using airborne measurements from two campaigns in Europe and East Asia. Differences between regions were found, but air quality models struggled to reproduce them accurately. We show that these proportional relationships can help to constrain models and can be used to infer aerosol concentrations from satellite observations of trace gases, especially in urban areas.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Ailish M. Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matilda Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
Atmos. Chem. Phys., 24, 789–806, https://doi.org/10.5194/acp-24-789-2024, https://doi.org/10.5194/acp-24-789-2024, 2024
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Our paper uses novel satellite datasets and high-resolution emissions datasets alongside a back-trajectory model to investigate the balance of local and external sources influencing NOx air pollution changes in Delhi. We find in the post-monsoon season that NOx from local and non-local transport emissions contributes most to poor air quality in Delhi. Therefore, air quality mitigation strategies in Delhi and surrounding regions are used to control this issue.
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.
Andrea Pazmiño, Florence Goutail, Sophie Godin-Beekmann, Alain Hauchecorne, Jean-Pierre Pommereau, Martyn P. Chipperfield, Wuhu Feng, Franck Lefèvre, Audrey Lecouffe, Michel Van Roozendael, Nis Jepsen, Georg Hansen, Rigel Kivi, Kimberly Strong, and Kaley A. Walker
Atmos. Chem. Phys., 23, 15655–15670, https://doi.org/10.5194/acp-23-15655-2023, https://doi.org/10.5194/acp-23-15655-2023, 2023
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The vortex-averaged ozone loss over the last 3 decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from the SAOZ network and MSR2 reanalysis. Three metrics were developed to compute ozone trends since 2000. The study confirms the ozone recovery in the Antarctic and shows a potential sign of quantitative detection of ozone recovery in the Arctic that needs to be robustly confirmed in the future.
Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, and Richard Rigby
Atmos. Chem. Phys., 23, 14933–14947, https://doi.org/10.5194/acp-23-14933-2023, https://doi.org/10.5194/acp-23-14933-2023, 2023
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Ozone is a potent air pollutant, and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTCO3) from space. We have constructed a merged LTCO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTCO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small-scale differences.
Sandip S. Dhomse and Martyn P. Chipperfield
Earth Syst. Sci. Data, 15, 5105–5120, https://doi.org/10.5194/essd-15-5105-2023, https://doi.org/10.5194/essd-15-5105-2023, 2023
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There are no long-term stratospheric profile data sets for two very important greenhouse gases: methane (CH4) and nitrous oxide (N2O). Along with radiative feedback, these species play an important role in controlling ozone loss in the stratosphere. Here, we use machine learning to fuse satellite measurements with a chemical model to construct long-term gap-free profile data sets for CH4 and N2O. We aim to construct similar data sets for other important trace gases (e.g. O3, Cly, NOy species).
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
James Barry, Stefanie Meilinger, Klaus Pfeilsticker, Anna Herman-Czezuch, Nicola Kimiaie, Christopher Schirrmeister, Rone Yousif, Tina Buchmann, Johannes Grabenstein, Hartwig Deneke, Jonas Witthuhn, Claudia Emde, Felix Gödde, Bernhard Mayer, Leonhard Scheck, Marion Schroedter-Homscheidt, Philipp Hofbauer, and Matthias Struck
Atmos. Meas. Tech., 16, 4975–5007, https://doi.org/10.5194/amt-16-4975-2023, https://doi.org/10.5194/amt-16-4975-2023, 2023
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Measured power data from solar photovoltaic (PV) systems contain information about the state of the atmosphere. In this work, power data from PV systems in the Allgäu region in Germany were used to determine the solar irradiance at each location, using state-of-the-art simulation and modelling. The results were validated using concurrent measurements of the incoming solar radiation in each case. If applied on a wider scale, this algorithm could help improve weather and climate models.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys., 23, 13235–13253, https://doi.org/10.5194/acp-23-13235-2023, https://doi.org/10.5194/acp-23-13235-2023, 2023
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
Chaoyang Xue, Gisèle Krysztofiak, Vanessa Brocchi, Stéphane Chevrier, Michel Chartier, Patrick Jacquet, Claude Robert, and Valéry Catoire
Earth Syst. Sci. Data, 15, 4553–4569, https://doi.org/10.5194/essd-15-4553-2023, https://doi.org/10.5194/essd-15-4553-2023, 2023
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To understand tropospheric air pollution at regional and global scales, an infrared laser spectrometer called SPIRIT was used on aircraft to rapidly and accurately measure carbon monoxide (CO), an important indicator of air pollution, during the last decade. Measurements were taken for more than 200 flight hours over three continents. Levels of CO are mapped with 3D trajectories for each flight. Additionally, this can be used to validate model performance and satellite measurements.
Frederik Harzer, Hella Garny, Felix Ploeger, Harald Bönisch, Peter Hoor, and Thomas Birner
Atmos. Chem. Phys., 23, 10661–10675, https://doi.org/10.5194/acp-23-10661-2023, https://doi.org/10.5194/acp-23-10661-2023, 2023
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We study the statistical relation between year-by-year fluctuations in winter-mean ozone and the strength of the stratospheric polar vortex. In the latitude–pressure plane, regression analysis shows that anomalously weak polar vortex years are associated with three pronounced local ozone maxima over the polar cap relative to the winter climatology. These response maxima primarily reflect the non-trivial combination of different ozone transport processes with varying relative contributions.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
Atmos. Chem. Phys., 23, 10533–10561, https://doi.org/10.5194/acp-23-10533-2023, https://doi.org/10.5194/acp-23-10533-2023, 2023
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Volcanic emissions emit large quantities of gases and primary aerosols that can play an important role in atmospheric chemistry. We present a study of the fate of volcanic bromine emissions from the eruption of Mount Etna around Christmas 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume and how it modifies the composition of the air over the whole Mediterranean basin, in particular on tropospheric ozone through the bromine-explosion cycle.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Valerian Hahn, Ralf Meerkötter, Christiane Voigt, Sonja Gisinger, Daniel Sauer, Valéry Catoire, Volker Dreiling, Hugh Coe, Cyrille Flamant, Stefan Kaufmann, Jonas Kleine, Peter Knippertz, Manuel Moser, Philip Rosenberg, Hans Schlager, Alfons Schwarzenboeck, and Jonathan Taylor
Atmos. Chem. Phys., 23, 8515–8530, https://doi.org/10.5194/acp-23-8515-2023, https://doi.org/10.5194/acp-23-8515-2023, 2023
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During the DACCIWA campaign in West Africa, we found a 35 % increase in the cloud droplet concentration that formed in a polluted compared with a less polluted environment and a decrease of 17 % in effective droplet diameter. Radiative transfer simulations, based on the measured cloud properties, reveal that these low-level polluted clouds radiate only 2.6 % more energy back to space, compared with a less polluted cloud. The corresponding additional decrease in temperature is rather small.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Luis F. Millán, Gloria L. Manney, Harald Boenisch, Michaela I. Hegglin, Peter Hoor, Daniel Kunkel, Thierry Leblanc, Irina Petropavlovskikh, Kaley Walker, Krzysztof Wargan, and Andreas Zahn
Atmos. Meas. Tech., 16, 2957–2988, https://doi.org/10.5194/amt-16-2957-2023, https://doi.org/10.5194/amt-16-2957-2023, 2023
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The determination of atmospheric composition trends in the upper troposphere and lower stratosphere (UTLS) is still highly uncertain. We present the creation of dynamical diagnostics to map several ozone datasets (ozonesondes, lidars, aircraft, and satellite measurements) in geophysically based coordinate systems. The diagnostics can also be used to analyze other greenhouse gases relevant to surface climate and UTLS chemistry.
Peter Joyce, Cristina Ruiz Villena, Yahui Huang, Alex Webb, Manuel Gloor, Fabien H. Wagner, Martyn P. Chipperfield, Rocío Barrio Guilló, Chris Wilson, and Hartmut Boesch
Atmos. Meas. Tech., 16, 2627–2640, https://doi.org/10.5194/amt-16-2627-2023, https://doi.org/10.5194/amt-16-2627-2023, 2023
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Methane emissions are responsible for a lot of the warming caused by the greenhouse effect, much of which comes from a small number of point sources. We can identify methane point sources by analysing satellite data, but it requires a lot of time invested by experts and is prone to very high errors. Here, we produce a neural network that can automatically identify methane point sources and estimate the mass of methane that is being released per hour and are able to do so with far smaller errors.
Virginie Marécal, Ronan Voisin-Plessis, Tjarda Jane Roberts, Alessandro Aiuppa, Herizo Narivelo, Paul David Hamer, Béatrice Josse, Jonathan Guth, Luke Surl, and Lisa Grellier
Geosci. Model Dev., 16, 2873–2898, https://doi.org/10.5194/gmd-16-2873-2023, https://doi.org/10.5194/gmd-16-2873-2023, 2023
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We implemented a halogen volcanic chemistry scheme in a one-dimensional modelling framework preparing for further use in a three-dimensional global chemistry-transport model. The results of the simulations for an eruption of Mt Etna in 2008, including various sensitivity tests, show a good consistency with previous modelling studies.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
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During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
Phuc Thi Minh Ha, Yugo Kanaya, Fumikazu Taketani, Maria Dolores Andrés Hernández, Benjamin Schreiner, Klaus Pfeilsticker, and Kengo Sudo
Geosci. Model Dev., 16, 927–960, https://doi.org/10.5194/gmd-16-927-2023, https://doi.org/10.5194/gmd-16-927-2023, 2023
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HONO affects tropospheric oxidizing capacity; thus, it is implemented into the chemistry–climate model CHASER. The model substantially underpredicts daytime HONO, while nitrate photolysis on surfaces can supplement the daytime HONO budget. Current HONO chemistry predicts reductions of 20.4 % for global tropospheric NOx, 40–67 % for OH, and 30–45 % for O3 in the summer North Pacific. In contrast, OH and O3 winter levels in China are greatly enhanced.
Evelien van Dijk, Ingar Mørkestøl Gundersen, Anna de Bode, Helge Høeg, Kjetil Loftsgarden, Frode Iversen, Claudia Timmreck, Johann Jungclaus, and Kirstin Krüger
Clim. Past, 19, 357–398, https://doi.org/10.5194/cp-19-357-2023, https://doi.org/10.5194/cp-19-357-2023, 2023
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The mid-6th century was one of the coldest periods of the last 2000 years as characterized by great societal changes. Here, we study the effect of the volcanic double event in 536 CE and 540 CE on climate and society in southern Norway. The combined climate and growing degree day models and high-resolution pollen and archaeological records reveal that the northern and western sites are vulnerable to crop failure with possible abandonment of farms, whereas the southeastern site is more resilient.
Eric Förster, Harald Bönisch, Marco Neumaier, Florian Obersteiner, Andreas Zahn, Andreas Hilboll, Anna B. Kalisz Hedegaard, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Mihalis Vrekoussis, Michael Lichtenstern, and Peter Braesicke
Atmos. Chem. Phys., 23, 1893–1918, https://doi.org/10.5194/acp-23-1893-2023, https://doi.org/10.5194/acp-23-1893-2023, 2023
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The airborne megacity campaign EMeRGe provided an unprecedented amount of trace gas measurements. We combine measured volatile organic compounds (VOCs) with trajectory-modelled emission uptakes to identify potential source regions of pollution. We also characterise the chemical fingerprints (e.g. biomass burning and anthropogenic signatures) of the probed air masses to corroborate the contributing source regions. Our approach is the first large-scale study of VOCs originating from megacities.
Flora Kluge, Tilman Hüneke, Christophe Lerot, Simon Rosanka, Meike K. Rotermund, Domenico Taraborrelli, Benjamin Weyland, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 1369–1401, https://doi.org/10.5194/acp-23-1369-2023, https://doi.org/10.5194/acp-23-1369-2023, 2023
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Using airborne glyoxal concentration and vertical column density measurements, vertical profiles are inferred for eight global regions in aged biomass burning plumes and the tropical marine boundary layer. Using TROPOMI observations, an analysis of space- and airborne measurements is performed. A comparison to EMAC simulations shows a general glyoxal underprediction, which points to various missing sources and precursors from anthropogenic activities, biomass burning, and the sea surface.
Robert J. Parker, Chris Wilson, Edward Comyn-Platt, Garry Hayman, Toby R. Marthews, A. Anthony Bloom, Mark F. Lunt, Nicola Gedney, Simon J. Dadson, Joe McNorton, Neil Humpage, Hartmut Boesch, Martyn P. Chipperfield, Paul I. Palmer, and Dai Yamazaki
Biogeosciences, 19, 5779–5805, https://doi.org/10.5194/bg-19-5779-2022, https://doi.org/10.5194/bg-19-5779-2022, 2022
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Wetlands are the largest natural source of methane, one of the most important climate gases. The JULES land surface model simulates these emissions. We use satellite data to evaluate how well JULES reproduces the methane seasonal cycle over different tropical wetlands. It performs well for most regions; however, it struggles for some African wetlands influenced heavily by river flooding. We explain the reasons for these deficiencies and highlight how future development will improve these areas.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Shih-Wei Fang, Claudia Timmreck, Johann Jungclaus, Kirstin Krüger, and Hauke Schmidt
Earth Syst. Dynam., 13, 1535–1555, https://doi.org/10.5194/esd-13-1535-2022, https://doi.org/10.5194/esd-13-1535-2022, 2022
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The early 19th century was the coldest period over the past 500 years, when strong tropical volcanic events and a solar minimum coincided. This study quantifies potential surface cooling from the solar and volcanic forcing in the early 19th century with large ensemble simulations, and identifies the regions that their impacts cannot be simply additive. The cooling perspective of Arctic amplification exists in both solar and post-volcano period with the albedo feedback as the main contribution.
Oliver Appel, Franziska Köllner, Antonis Dragoneas, Andreas Hünig, Sergej Molleker, Hans Schlager, Christoph Mahnke, Ralf Weigel, Max Port, Christiane Schulz, Frank Drewnick, Bärbel Vogel, Fred Stroh, and Stephan Borrmann
Atmos. Chem. Phys., 22, 13607–13630, https://doi.org/10.5194/acp-22-13607-2022, https://doi.org/10.5194/acp-22-13607-2022, 2022
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This paper clarifies the chemical composition of the Asian tropopause aerosol layer (ATAL) by means of airborne in situ aerosol mass spectrometry (AMS). Ammonium nitrate and organics are found to significantly contribute to the particle layer, while sulfate does not show a layered structure. An analysis of the single-particle mass spectra suggests that secondary particle formation and subsequent growth dominate the particle composition, rather than condensation on pre-existing primary particles.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.9 to 7.8 × 105 cm-3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
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The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Evelien van Dijk, Johann Jungclaus, Stephan Lorenz, Claudia Timmreck, and Kirstin Krüger
Clim. Past, 18, 1601–1623, https://doi.org/10.5194/cp-18-1601-2022, https://doi.org/10.5194/cp-18-1601-2022, 2022
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A double volcanic eruption in 536 and 540 CE caused one of the coldest decades during the last 2000 years. We analyzed new climate model simulations from that period and found a cooling of up to 2°C and a sea-ice extent up to 200 km further south. Complex interactions between sea ice and ocean circulation lead to a reduction in the northward ocean heat transport, which makes the sea ice extend further south; this in turn leads to a surface cooling up to 20 years after the eruptions.
Jason E. Williams, Vincent Huijnen, Idir Bouarar, Mehdi Meziane, Timo Schreurs, Sophie Pelletier, Virginie Marécal, Beatrice Josse, and Johannes Flemming
Geosci. Model Dev., 15, 4657–4687, https://doi.org/10.5194/gmd-15-4657-2022, https://doi.org/10.5194/gmd-15-4657-2022, 2022
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The global CAMS air quality model is used for providing tropospheric ozone information to end users. This paper updates the chemical mechanism employed (CBA) and compares it against two other mechanisms (MOCAGE, MOZART) and a multi-decadal dataset based on a previous version of CBA. We perform extensive validation for the US using multiple surface and aircraft datasets, providing an assessment of biases and the extent of correlation across different seasons during 2014.
Eric A. Ray, Elliot L. Atlas, Sue Schauffler, Sofia Chelpon, Laura Pan, Harald Bönisch, and Karen H. Rosenlof
Atmos. Chem. Phys., 22, 6539–6558, https://doi.org/10.5194/acp-22-6539-2022, https://doi.org/10.5194/acp-22-6539-2022, 2022
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The movement of air masses and the trace gases they contain from the Earth’s surface into the upper troposphere and lower stratosphere (UTLS) can have important implications for the radiative and chemical balance of the atmosphere. In this study we build on recent techniques and use new ones to estimate a range of transport diagnostics based on simultaneously measured trace gases in the UTLS during the monsoon season in North America.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Piera Raspollini, Enrico Arnone, Flavio Barbara, Massimo Bianchini, Bruno Carli, Simone Ceccherini, Martyn P. Chipperfield, Angelika Dehn, Stefano Della Fera, Bianca Maria Dinelli, Anu Dudhia, Jean-Marie Flaud, Marco Gai, Michael Kiefer, Manuel López-Puertas, David P. Moore, Alessandro Piro, John J. Remedios, Marco Ridolfi, Harjinder Sembhi, Luca Sgheri, and Nicola Zoppetti
Atmos. Meas. Tech., 15, 1871–1901, https://doi.org/10.5194/amt-15-1871-2022, https://doi.org/10.5194/amt-15-1871-2022, 2022
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The MIPAS instrument onboard the ENVISAT satellite provided 10 years of measurements of the atmospheric emission al limb that allow for the retrieval of latitude- and altitude-resolved atmospheric composition. We describe the improvements implemented in the retrieval algorithm used for the full mission reanalysis, which allows for the generation of the global distributions of 21 atmospheric constituents plus temperature with increased accuracy with respect to previously generated data.
Christine D. Groot Zwaaftink, Wenche Aas, Sabine Eckhardt, Nikolaos Evangeliou, Paul Hamer, Mona Johnsrud, Arve Kylling, Stephen M. Platt, Kerstin Stebel, Hilde Uggerud, and Karl Espen Yttri
Atmos. Chem. Phys., 22, 3789–3810, https://doi.org/10.5194/acp-22-3789-2022, https://doi.org/10.5194/acp-22-3789-2022, 2022
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We investigate causes of a poor-air-quality episode in northern Europe in October 2020 during which EU health limits for air quality were vastly exceeded. Such episodes may trigger measures to improve air quality. Analysis based on satellite observations, transport simulations, and surface observations revealed two sources of pollution. Emissions of mineral dust in Central Asia and biomass burning in Ukraine arrived almost simultaneously in Norway, and transport continued into the Arctic.
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.
Guangyu Liu, Toshihiko Hirooka, Nawo Eguchi, and Kirstin Krüger
Atmos. Chem. Phys., 22, 3493–3505, https://doi.org/10.5194/acp-22-3493-2022, https://doi.org/10.5194/acp-22-3493-2022, 2022
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The sudden stratospheric warming (SSW) event that occurred in September 2019 in the Southern Hemisphere was analyzed. A large warming and decelerated westerly winds were observed in the southern polar region. Since a reversal from westerly to easterly winds did not take place SSW2019 was classified as a minor SSW. The total wave forcing and the contribution from PW1 were larger in 2019. The strong and long-lasting planetary-scale waves with zonal wavenumber 1 played a role in SSW2019.
Chaoyang Xue, Can Ye, Jörg Kleffmann, Chenglong Zhang, Valéry Catoire, Fengxia Bao, Abdelwahid Mellouki, Likun Xue, Jianmin Chen, Keding Lu, Yong Zhao, Hengde Liu, Zhaoxin Guo, and Yujing Mu
Atmos. Chem. Phys., 22, 3149–3167, https://doi.org/10.5194/acp-22-3149-2022, https://doi.org/10.5194/acp-22-3149-2022, 2022
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Summertime measurements of nitrous acid (HONO) and related parameters were conducted at the foot and the summit of Mt. Tai (1534 m above sea level). We proposed a rapid vertical air mass exchange between the foot and the summit level, which enhances the role of HONO in the oxidizing capacity of the upper boundary layer. Kinetics for aerosol-derived HONO sources were constrained. HONO formation from different paths was quantified and discussed.
Yanan Zhao, Dennis Booge, Christa A. Marandino, Cathleen Schlundt, Astrid Bracher, Elliot L. Atlas, Jonathan Williams, and Hermann W. Bange
Biogeosciences, 19, 701–714, https://doi.org/10.5194/bg-19-701-2022, https://doi.org/10.5194/bg-19-701-2022, 2022
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We present here, for the first time, simultaneously measured dimethylsulfide (DMS) seawater concentrations and DMS atmospheric mole fractions from the Peruvian upwelling region during two cruises in December 2012 and October 2015. Our results indicate low oceanic DMS concentrations and atmospheric DMS molar fractions in surface waters and the atmosphere, respectively. In addition, the Peruvian upwelling region was identified as an insignificant source of DMS emissions during both periods.
Chaoyang Xue, Can Ye, Jörg Kleffmann, Wenjin Zhang, Xiaowei He, Pengfei Liu, Chenglong Zhang, Xiaoxi Zhao, Chengtang Liu, Zhuobiao Ma, Junfeng Liu, Jinhe Wang, Keding Lu, Valéry Catoire, Abdelwahid Mellouki, and Yujing Mu
Atmos. Chem. Phys., 22, 1035–1057, https://doi.org/10.5194/acp-22-1035-2022, https://doi.org/10.5194/acp-22-1035-2022, 2022
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Nitrous acid (HONO) and related parameters were measured at the foot and the summit of Mt. Tai in the summer of 2018. Based on measurements at the foot station, we utilized a box model to explore the roles of different sources in the HONO budget. We also studied radical chemistry in this high-ozone region.
Abhinna K. Behera, Emmanuel D. Rivière, Sergey M. Khaykin, Virginie Marécal, Mélanie Ghysels, Jérémie Burgalat, and Gerhard Held
Atmos. Chem. Phys., 22, 881–901, https://doi.org/10.5194/acp-22-881-2022, https://doi.org/10.5194/acp-22-881-2022, 2022
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Deep convection overshooting the stratosphere's contribution to the global stratospheric water budget is still being quantified. We ran three different cloud-resolving simulations of an observed case of overshoots in Bauru during the TRO-Pico balloon campaign in the context of upscaling the impact of overshoots at a large scale. These simulations, which have been validated with balloon-borne and S-band radar measurements, shed light on the local-scale variability and composition of overshoots.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Sandip S. Dhomse, Carlo Arosio, Wuhu Feng, Alexei Rozanov, Mark Weber, and Martyn P. Chipperfield
Earth Syst. Sci. Data, 13, 5711–5729, https://doi.org/10.5194/essd-13-5711-2021, https://doi.org/10.5194/essd-13-5711-2021, 2021
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High-quality long-term ozone profile data sets are key to estimating short- and long-term ozone variability. Almost all the satellite (and chemical model) data sets show some kind of bias with respect to each other. This is because of differences in measurement methodologies as well as simplified processes in the models. We use satellite data sets and chemical model output to generate 42 years of ozone profile data sets using a random-forest machine-learning algorithm that is named ML-TOMCAT.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
Tiziana Bräuer, Christiane Voigt, Daniel Sauer, Stefan Kaufmann, Valerian Hahn, Monika Scheibe, Hans Schlager, Felix Huber, Patrick Le Clercq, Richard H. Moore, and Bruce E. Anderson
Atmos. Chem. Phys., 21, 16817–16826, https://doi.org/10.5194/acp-21-16817-2021, https://doi.org/10.5194/acp-21-16817-2021, 2021
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Over half of aviation climate impact is caused by contrails. Biofuels can reduce the ice crystal numbers in contrails and mitigate the climate impact. The experiment ECLIF II/NDMAX in 2018 assessed the effects of biofuels on contrails and aviation emissions. The NASA DC-8 aircraft performed measurements inside the contrail of the DLR A320. One reference fuel and two blends of the biofuel HEFA and kerosene are analysed. We find a max reduction of contrail ice numbers through biofuel use of 40 %.
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
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By presenting an approach using EMeRGe-Asia airborne field measurements and surface observations, this study shows that the fraction of OH reactivity due to SO2-OH reaction has a significant correlation with the sulfate concentration. Approximately 30 % of sulfate is produced by SO2-OH reaction. Our results underline the importance of SO2-OH gas-phase oxidation in sulfate formation, and demonstrate that the method can be applied to other regions and under different meteorological conditions.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
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.
Claire Lamotte, Jonathan Guth, Virginie Marécal, Martin Cussac, Paul David Hamer, Nicolas Theys, and Philipp Schneider
Atmos. Chem. Phys., 21, 11379–11404, https://doi.org/10.5194/acp-21-11379-2021, https://doi.org/10.5194/acp-21-11379-2021, 2021
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Improvements are made in a global chemical transfer model by considering a new volcanic SO2 emissions inventory, with more volcanoes referenced and more information on the altitude of injection. Better constraining volcanic emissions with this inventory improves the global, but mostly local, tropospheric sulfur composition. The tropospheric sulfur budget shows a nonlinearity to the volcanic contribution, especially to the sulfate aerosol burden and sulfur wet deposition.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Fides Lefrancois, Markus Jesswein, Markus Thoma, Andreas Engel, Kieran Stanley, and Tanja Schuck
Atmos. Meas. Tech., 14, 4669–4687, https://doi.org/10.5194/amt-14-4669-2021, https://doi.org/10.5194/amt-14-4669-2021, 2021
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Synthetic halocarbons can contribute to stratospheric ozone depletion or to climate change. In many applications they have been replaced over the last years. The presented non-target analysis shows an application approach to quantify those replacements retrospectively, using recorded data of air measurements with gas chromatography coupled to time-of-flight mass spectrometry. We focus on the retrospective analysis of the fourth-generation halocarbons, detected at Taunus Observatory in Germany.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412, https://doi.org/10.5194/acp-21-8393-2021, https://doi.org/10.5194/acp-21-8393-2021, 2021
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We investigate the global stratospheric circulation (Brewer–Dobson circulation) in the new ECMWF ERA5 reanalysis based on age of air simulations, and we compare it to results from the preceding ERA-Interim reanalysis. Our results show a slower stratospheric circulation and higher age for ERA5. The age of air trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, related to multi-annual variability and a potential contribution from changes in the reanalysis system.
Thomas Wagenhäuser, Andreas Engel, and Robert Sitals
Atmos. Meas. Tech., 14, 3923–3934, https://doi.org/10.5194/amt-14-3923-2021, https://doi.org/10.5194/amt-14-3923-2021, 2021
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AirCore samplers are increasingly deployed to weather balloons to collect continuous atmospheric samples. We introduce a technique that can be used in situ to evaluate different data processing methods that are required to derive vertical trace gas profiles from AirCore measurements after sample recovery. Results from two test flights with a specific AirCore configuration provide evidence for systematic deviations in altitude attribution for the upper levels, which can be empirically corrected.
Yann Cohen, Virginie Marécal, Béatrice Josse, and Valérie Thouret
Geosci. Model Dev., 14, 2659–2689, https://doi.org/10.5194/gmd-14-2659-2021, https://doi.org/10.5194/gmd-14-2659-2021, 2021
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Assessing long-term chemistry–climate simulations with in situ and frequent observations near the tropopause is possible with the IAGOS commercial aircraft data set. This study presents a method that distributes the IAGOS data (ozone and CO) on a monthly model grid, limiting the impact of resolution for the evaluation of the modelled chemical fields. We applied it to the CCMI REF-C1SD simulation from the MOCAGE CTM and notably highlighted well-reproduced O3 behaviour in the lower stratosphere.
Maxi Boettcher, Andreas Schäfler, Michael Sprenger, Harald Sodemann, Stefan Kaufmann, Christiane Voigt, Hans Schlager, Donato Summa, Paolo Di Girolamo, Daniele Nerini, Urs Germann, and Heini Wernli
Atmos. Chem. Phys., 21, 5477–5498, https://doi.org/10.5194/acp-21-5477-2021, https://doi.org/10.5194/acp-21-5477-2021, 2021
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Warm conveyor belts (WCBs) are important airstreams in extratropical cyclones, often leading to the formation of intense precipitation. We present a case study that involves aircraft, lidar and radar observations of water and clouds in a WCB ascending from western Europe across the Alps towards the Baltic Sea during the field campaigns HyMeX and T-NAWDEX-Falcon in October 2012. A probabilistic trajectory measure and an airborne tracer experiment were used to confirm the long pathway of the WCB.
Akash Biswal, Vikas Singh, Shweta Singh, Amit P. Kesarkar, Khaiwal Ravindra, Ranjeet S. Sokhi, Martyn P. Chipperfield, Sandip S. Dhomse, Richard J. Pope, Tanbir Singh, and Suman Mor
Atmos. Chem. Phys., 21, 5235–5251, https://doi.org/10.5194/acp-21-5235-2021, https://doi.org/10.5194/acp-21-5235-2021, 2021
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Satellite and surface observations show a reduction in NO2 levels over India during the lockdown compared to business-as-usual years. A substantial reduction, proportional to the population, was observed over the urban areas. The changes in NO2 levels at the surface during the lockdown appear to be present in the satellite observations. However, TROPOMI showed a better correlation with surface NO2 and was more sensitive to the changes than OMI because of the finer resolution.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
Joan Stude, Heinfried Aufmhoff, Hans Schlager, Markus Rapp, Frank Arnold, and Boris Strelnikov
Atmos. Meas. Tech., 14, 983–993, https://doi.org/10.5194/amt-14-983-2021, https://doi.org/10.5194/amt-14-983-2021, 2021
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In this paper we describe the instrument ROMARA and show data from the first flight on a research rocket.
On the way through the atmosphere, the instrument detects positive and negative, natural occurring ions before returning back to ground.
ROMARA was successfully launched together with other instruments into a special radar echo.
We detected typical, light ions of positive and negative charge and heavy negative ions, but no heavy positive ions.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Robert J. Parker, Chris Wilson, A. Anthony Bloom, Edward Comyn-Platt, Garry Hayman, Joe McNorton, Hartmut Boesch, and Martyn P. Chipperfield
Biogeosciences, 17, 5669–5691, https://doi.org/10.5194/bg-17-5669-2020, https://doi.org/10.5194/bg-17-5669-2020, 2020
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Wetlands contribute the largest uncertainty to the atmospheric methane budget. WetCHARTs is a simple, data-driven model that estimates wetland emissions using observations of precipitation and temperature. We perform the first detailed evaluation of WetCHARTs against satellite data and find it performs well in reproducing the observed wetland methane seasonal cycle for the majority of wetland regions. In regions where it performs poorly, we highlight incorrect wetland extent as a key reason.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Benjamin Birner, Martyn P. Chipperfield, Eric J. Morgan, Britton B. Stephens, Marianna Linz, Wuhu Feng, Chris Wilson, Jonathan D. Bent, Steven C. Wofsy, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Chem. Phys., 20, 12391–12408, https://doi.org/10.5194/acp-20-12391-2020, https://doi.org/10.5194/acp-20-12391-2020, 2020
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With new high-precision observations from nine aircraft campaigns and 3-D chemical transport modeling, we show that the argon-to-nitrogen ratio (Ar / N2) in the lowermost stratosphere provides a useful constraint on the “age of air” (the time elapsed since entry of an air parcel into the stratosphere). Therefore, Ar / N2 in combination with traditional age-of-air indicators, such as CO2 and N2O, could provide new insights into atmospheric mixing and transport.
Flora Kluge, Tilman Hüneke, Matthias Knecht, Michael Lichtenstern, Meike Rotermund, Hans Schlager, Benjamin Schreiner, and Klaus Pfeilsticker
Atmos. Chem. Phys., 20, 12363–12389, https://doi.org/10.5194/acp-20-12363-2020, https://doi.org/10.5194/acp-20-12363-2020, 2020
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The presented study reports on airborne measurements of formaldehyde, glyoxal, methylglyoxal, and CO over the Amazon basin and lays a special focus on the influence of biomass burning emissions on the atmospheric profiles of these carbonyl compounds within the planetary boundary layer as well as in the free and upper troposphere.
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
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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.
Hirofumi Ohyama, Isamu Morino, Voltaire A. Velazco, Theresa Klausner, Gerry Bagtasa, Matthäus Kiel, Matthias Frey, Akihiro Hori, Osamu Uchino, Tsuneo Matsunaga, Nicholas M. Deutscher, Joshua P. DiGangi, Yonghoon Choi, Glenn S. Diskin, Sally E. Pusede, Alina Fiehn, Anke Roiger, Michael Lichtenstern, Hans Schlager, Pao K. Wang, Charles C.-K. Chou, Maria Dolores Andrés-Hernández, and John P. Burrows
Atmos. Meas. Tech., 13, 5149–5163, https://doi.org/10.5194/amt-13-5149-2020, https://doi.org/10.5194/amt-13-5149-2020, 2020
Short summary
Short summary
Column-averaged dry-air mole fractions of CO2 and CH4 measured by a solar viewing portable Fourier transform spectrometer (EM27/SUN) were validated with in situ profile data obtained during the transfer flights of two aircraft campaigns. Atmospheric dynamical properties based on ERA5 and WRF-Chem were used as criteria for selecting the best aircraft profiles for the validation. The resulting air-mass-independent correction factors for the EM27/SUN data were 0.9878 for CO2 and 0.9829 for CH4.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
Short summary
Short summary
Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
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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.
Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported...
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