Articles | Volume 18, issue 10
https://doi.org/10.5194/acp-18-7625-2018
© Author(s) 2018. 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-18-7625-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| Highlight paper
| 
01 Jun 2018
Research article | Highlight paper |
| 01 Jun 2018
| 01 Jun 2018
On ozone trend detection: using coupled chemistry–climate simulations to investigate early signs of total column ozone recovery
James Keeble
CORRESPONDING AUTHOR
Department of Chemistry, University of Cambridge, Cambridge, UK
Hannah Brown
Department of Chemistry, University of Cambridge, Cambridge, UK
N. Luke Abraham
Department of Chemistry, University of Cambridge, Cambridge, UK
National Centre for Atmospheric Science, Cambridge, UK
Neil R. P. Harris
Centre for Environmental and Agricultural Informatics, Cranfield
University, Cranfield, UK
John A. Pyle
Department of Chemistry, University of Cambridge, Cambridge, UK
National Centre for Atmospheric Science, Cambridge, UK
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We analyzed the ozone response under elevated CO2 using the data from CMIP6 DECK experiments. We then looked at the relations between ozone response and temperature and circulation changes to identify drivers of the ozone change. The climate feedback of ozone is investigated by doing offline calculations and comparing models with and without interactive chemistry. We find that ozone-climate interactions are important for Earth System Models, thus should be considered in future model development.
Alex T. Archibald, Bablu Sinha, Maria R. Russo, Emily Matthews, Freya A. Squires, N. Luke Abraham, Stephane J.-B. Bauguitte, Thomas J. Bannan, Thomas G. Bell, David Berry, Lucy J. Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian A. King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Bengamin I. Moat, Katie Read, Chris Reed, Malcolm J. Roberts, Reinhard Schiemann, David Schroeder, Timothy J. Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Mingxi Yang
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Here, we present an overview of the data generated as part of the North Atlantic Climate System Integrated Study (ACSIS) programme that are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA; www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC; bodc.ac.uk). The datasets described here cover the North Atlantic Ocean, the atmosphere above (it including its composition), and Arctic sea ice.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
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If reductions aren’t implemented to limit emissions of pollutants that produce ozone then we calculate that this will cause a warming of climate. We assess how the future warming from ozone is affected by changing meteorological variables such as clouds and atmospheric temperatures. We find that reductions in high cloud cover tend to slightly reduce the warming from ozone.
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Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Laura J. Wilcox, Robert J. Allen, Bjørn H. Samset, Massimo A. Bollasina, Paul T. Griffiths, James Keeble, Marianne T. Lund, Risto Makkonen, Joonas Merikanto, Declan O'Donnell, David J. Paynter, Geeta G. Persad, Steven T. Rumbold, Toshihiko Takemura, Kostas Tsigaridis, Sabine Undorf, and Daniel M. Westervelt
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Changes in anthropogenic aerosol emissions have strongly contributed to global and regional climate change. However, the size of these regional impacts and the way they arise are still uncertain. With large changes in aerosol emissions a possibility over the next few decades, it is important to better quantify the potential role of aerosol in future regional climate change. The Regional Aerosol Model Intercomparison Project will deliver experiments designed to facilitate this.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
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Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 3609–3627, https://doi.org/10.5194/acp-23-3609-2023, https://doi.org/10.5194/acp-23-3609-2023, 2023
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We use a machine learning technique called Gaussian mixture modeling (GMM) to classify vertical ozone profiles into groups based on how the ozone concentration changes with pressure. Even though the GMM algorithm was not provided with spatial information, the classes are geographically coherent. We also detect signatures of tropical broadening in UKESM1 future climate scenarios. GMM may be useful for understanding ozone structures in modeled and observed datasets.
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Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
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Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
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Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Fraser Dennison, James Keeble, Olaf Morgenstern, Guang Zeng, N. Luke Abraham, and Xin Yang
Geosci. Model Dev., 12, 1227–1239, https://doi.org/10.5194/gmd-12-1227-2019, https://doi.org/10.5194/gmd-12-1227-2019, 2019
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Two developments are made to the United Kingdom Chemistry and Aerosols (UKCA) model to improve simulation of stratospheric ozone. The first is the addition of a solar cycle. The influence on ozone from the solar cycle is found to be 1–2 %, which is consistent with other studies. The second is to the heterogeneous chemistry, the most significant change being the addition of reactions involving bromine species. This was shown to reduce ozone biases relative to observations in most regions.
James Keeble, Ewa M. Bednarz, Antara Banerjee, N. Luke Abraham, Neil R. P. Harris, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 17, 13801–13818, https://doi.org/10.5194/acp-17-13801-2017, https://doi.org/10.5194/acp-17-13801-2017, 2017
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In this study we explore the chemical and transport processes controlling ozone abundances in different altitude regions in the tropics for the present day and how these processes may change in the future in order to determine when total-column ozone values in the tropics will recover to pre-1980s values following the implementation of the Montreal Protocol and its subsequent amendments, which imposed bans on the use and emissions of CFCs.
Mingjin Tang, James Keeble, Paul J. Telford, Francis D. Pope, Peter Braesicke, Paul T. Griffiths, N. Luke Abraham, James McGregor, I. Matt Watson, R. Anthony Cox, John A. Pyle, and Markus Kalberer
Atmos. Chem. Phys., 16, 15397–15412, https://doi.org/10.5194/acp-16-15397-2016, https://doi.org/10.5194/acp-16-15397-2016, 2016
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We have investigated for the first time the heterogeneous hydrolysis of ClONO2 on TiO2 and SiO2 aerosol particles at room temperature and at different relative humidities (RHs), using an aerosol flow tube. The kinetic data reported in our current and previous studies have been included in the UKCA chemistry–climate model to assess the impact of TiO2 injection on stratospheric chemistry and stratospheric ozone in particular.
A. Orr, J. S. Hosking, L. Hoffmann, J. Keeble, S. M. Dean, H. K. Roscoe, N. L. Abraham, S. Vosper, and P. Braesicke
Atmos. Chem. Phys., 15, 1071–1086, https://doi.org/10.5194/acp-15-1071-2015, https://doi.org/10.5194/acp-15-1071-2015, 2015
J. Keeble, P. Braesicke, N. L. Abraham, H. K. Roscoe, and J. A. Pyle
Atmos. Chem. Phys., 14, 13705–13717, https://doi.org/10.5194/acp-14-13705-2014, https://doi.org/10.5194/acp-14-13705-2014, 2014
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 10431–10438, https://doi.org/10.5194/acp-14-10431-2014, https://doi.org/10.5194/acp-14-10431-2014, 2014
P. Braesicke, J. Keeble, X. Yang, G. Stiller, S. Kellmann, N. L. Abraham, A. Archibald, P. Telford, and J. A. Pyle
Atmos. Chem. Phys., 13, 10677–10688, https://doi.org/10.5194/acp-13-10677-2013, https://doi.org/10.5194/acp-13-10677-2013, 2013
Clara Orbe, Alison Ming, Gabriel Chiodo, Michael Prather, Mohamadou Diallo, Qi Tang, Andreas Chrysanthou, Hiroaki Naoe, Xin Zhou, Irina Thaler, Dillon Elsbury, Ewa Bednarz, Jonathon S. Wright, Aaron Match, Shingo Watanabe, James Anstey, Tobias Kerzenmacher, Stefan Versick, Marion Marchand, Feng Li, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2025-2761, https://doi.org/10.5194/egusphere-2025-2761, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
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The quasi-biennial oscillation (QBO) is the main source of wind fluctuations in the tropical stratosphere, which can couple to surface climate. However, models do a poor job of simulating the QBO in the lower stratosphere, for reasons that remain unclear. One possibility is that models do not completely represent how ozone influences the QBO-associated wind variations. Here we propose a multi-model framework for assessing how ozone influences the QBO in recent past and future climates.
Jingyu Wang, Gabriel Chiodo, Timofei Sukhodolov, Blanca Ayarzagüena, William T. Ball, Mohamadou Diallo, Birgit Hassler, James Keeble, Peer Nowack, Clara Orbe, and Sandro Vattioni
EGUsphere, https://doi.org/10.5194/egusphere-2025-340, https://doi.org/10.5194/egusphere-2025-340, 2025
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We analyzed the ozone response under elevated CO2 using the data from CMIP6 DECK experiments. We then looked at the relations between ozone response and temperature and circulation changes to identify drivers of the ozone change. The climate feedback of ozone is investigated by doing offline calculations and comparing models with and without interactive chemistry. We find that ozone-climate interactions are important for Earth System Models, thus should be considered in future model development.
Lauren R. Marshall, Anja Schmidt, Andrew P. Schurer, Nathan Luke Abraham, Lucie J. Lücke, Rob Wilson, Kevin J. Anchukaitis, Gabriele C. Hegerl, Ben Johnson, Bette L. Otto-Bliesner, Esther C. Brady, Myriam Khodri, and Kohei Yoshida
Clim. Past, 21, 161–184, https://doi.org/10.5194/cp-21-161-2025, https://doi.org/10.5194/cp-21-161-2025, 2025
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Large volcanic eruptions have caused temperature deviations over the past 1000 years; however, climate model results and reconstructions of surface cooling using tree rings do not match. We explore this mismatch using the latest models and find a better match to tree-ring reconstructions for some eruptions. Our results show that the way in which eruptions are simulated in models matters for the comparison to tree-rings, particularly regarding the spatial spread of volcanic aerosol.
Alex T. Archibald, Bablu Sinha, Maria R. Russo, Emily Matthews, Freya A. Squires, N. Luke Abraham, Stephane J.-B. Bauguitte, Thomas J. Bannan, Thomas G. Bell, David Berry, Lucy J. Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian A. King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Bengamin I. Moat, Katie Read, Chris Reed, Malcolm J. Roberts, Reinhard Schiemann, David Schroeder, Timothy J. Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Mingxi Yang
Earth Syst. Sci. Data, 17, 135–164, https://doi.org/10.5194/essd-17-135-2025, https://doi.org/10.5194/essd-17-135-2025, 2025
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Here, we present an overview of the data generated as part of the North Atlantic Climate System Integrated Study (ACSIS) programme that are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA; www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC; bodc.ac.uk). The datasets described here cover the North Atlantic Ocean, the atmosphere above (it including its composition), and Arctic sea ice.
Maria R. Russo, Sadie L. Bartholomew, David Hassell, Alex M. Mason, Erica Neininger, A. James Perman, David A. J. Sproson, Duncan Watson-Parris, and Nathan Luke Abraham
Geosci. Model Dev., 18, 181–191, https://doi.org/10.5194/gmd-18-181-2025, https://doi.org/10.5194/gmd-18-181-2025, 2025
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Observational data and modelling capabilities have expanded in recent years, but there are still barriers preventing these two data sources from being used in synergy. Proper comparison requires generating, storing, and handling a large amount of data. This work describes the first step in the development of a new set of software tools, the VISION toolkit, which can enable the easy and efficient integration of observational and model data required for model evaluation.
William J. Collins, Fiona M. O'Connor, Connor R. Barker, Rachael E. Byrom, Sebastian D. Eastham, Øivind Hodnebrog, Patrick Jöckel, Eloise A. Marais, Mariano Mertens, Gunnar Myhre, Matthias Nützel, Dirk Olivié, Ragnhild Bieltvedt Skeie, Laura Stecher, Larry W. Horowitz, Vaishali Naik, Gregory Faluvegi, Ulas Im, Lee T. Murray, Drew Shindell, Kostas Tsigaridis, Nathan Luke Abraham, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2024-3698, https://doi.org/10.5194/egusphere-2024-3698, 2024
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If reductions aren’t implemented to limit emissions of pollutants that produce ozone then we calculate that this will cause a warming of climate. We assess how the future warming from ozone is affected by changing meteorological variables such as clouds and atmospheric temperatures. We find that reductions in high cloud cover tend to slightly reduce the warming from ozone.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
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Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
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.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
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A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Laura J. Wilcox, Robert J. Allen, Bjørn H. Samset, Massimo A. Bollasina, Paul T. Griffiths, James Keeble, Marianne T. Lund, Risto Makkonen, Joonas Merikanto, Declan O'Donnell, David J. Paynter, Geeta G. Persad, Steven T. Rumbold, Toshihiko Takemura, Kostas Tsigaridis, Sabine Undorf, and Daniel M. Westervelt
Geosci. Model Dev., 16, 4451–4479, https://doi.org/10.5194/gmd-16-4451-2023, https://doi.org/10.5194/gmd-16-4451-2023, 2023
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Changes in anthropogenic aerosol emissions have strongly contributed to global and regional climate change. However, the size of these regional impacts and the way they arise are still uncertain. With large changes in aerosol emissions a possibility over the next few decades, it is important to better quantify the potential role of aerosol in future regional climate change. The Regional Aerosol Model Intercomparison Project will deliver experiments designed to facilitate this.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
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Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
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The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 3609–3627, https://doi.org/10.5194/acp-23-3609-2023, https://doi.org/10.5194/acp-23-3609-2023, 2023
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We use a machine learning technique called Gaussian mixture modeling (GMM) to classify vertical ozone profiles into groups based on how the ozone concentration changes with pressure. Even though the GMM algorithm was not provided with spatial information, the classes are geographically coherent. We also detect signatures of tropical broadening in UKESM1 future climate scenarios. GMM may be useful for understanding ozone structures in modeled and observed datasets.
Flossie Brown, Gerd A. Folberth, Stephen Sitch, Susanne Bauer, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Makoto Deushi, Inês Dos Santos Vieira, Corinne Galy-Lacaux, James Haywood, James Keeble, Lina M. Mercado, Fiona M. O'Connor, Naga Oshima, Kostas Tsigaridis, and Hans Verbeeck
Atmos. Chem. Phys., 22, 12331–12352, https://doi.org/10.5194/acp-22-12331-2022, https://doi.org/10.5194/acp-22-12331-2022, 2022
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Surface ozone can decrease plant productivity and impair human health. In this study, we evaluate the change in surface ozone due to climate change over South America and Africa using Earth system models. We find that if the climate were to change according to the worst-case scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of ozone exposure, but other areas will experience a climate benefit.
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.
Sebastian Landwehr, Michele Volpi, F. Alexander Haumann, Charlotte M. Robinson, Iris Thurnherr, Valerio Ferracci, Andrea Baccarini, Jenny Thomas, Irina Gorodetskaya, Christian Tatzelt, Silvia Henning, Rob L. Modini, Heather J. Forrer, Yajuan Lin, Nicolas Cassar, Rafel Simó, Christel Hassler, Alireza Moallemi, Sarah E. Fawcett, Neil Harris, Ruth Airs, Marzieh H. Derkani, Alberto Alberello, Alessandro Toffoli, Gang Chen, Pablo Rodríguez-Ros, Marina Zamanillo, Pau Cortés-Greus, Lei Xue, Conor G. Bolas, Katherine C. Leonard, Fernando Perez-Cruz, David Walton, and Julia Schmale
Earth Syst. Dynam., 12, 1295–1369, https://doi.org/10.5194/esd-12-1295-2021, https://doi.org/10.5194/esd-12-1295-2021, 2021
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The Antarctic Circumnavigation Expedition surveyed a large number of variables describing the dynamic state of ocean and atmosphere, freshwater cycle, atmospheric chemistry, ocean biogeochemistry, and microbiology in the Southern Ocean. To reduce the dimensionality of the dataset, we apply a sparse principal component analysis and identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and
hotspotsof interaction. Code and data are open access.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, https://doi.org/10.5194/acp-21-15901-2021, 2021
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Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
John Staunton-Sykes, Thomas J. Aubry, Youngsub M. Shin, James Weber, Lauren R. Marshall, Nathan Luke Abraham, Alex Archibald, and Anja Schmidt
Atmos. Chem. Phys., 21, 9009–9029, https://doi.org/10.5194/acp-21-9009-2021, https://doi.org/10.5194/acp-21-9009-2021, 2021
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
Atmos. Chem. Phys., 21, 5015–5061, https://doi.org/10.5194/acp-21-5015-2021, https://doi.org/10.5194/acp-21-5015-2021, 2021
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Stratospheric ozone and water vapour are key components of the Earth system; changes to both have important impacts on global and regional climate. We evaluate changes to these species from 1850 to 2100 in the new generation of CMIP6 models. There is good agreement between the multi-model mean and observations, although there is substantial variation between the individual models. The future evolution of both ozone and water vapour is strongly dependent on the assumed future emissions scenario.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
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The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
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This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Jane P. Mulcahy, Colin Johnson, Colin G. Jones, Adam C. Povey, Catherine E. Scott, Alistair Sellar, Steven T. Turnock, Matthew T. Woodhouse, Nathan Luke Abraham, Martin B. Andrews, Nicolas Bellouin, Jo Browse, Ken S. Carslaw, Mohit Dalvi, Gerd A. Folberth, Matthew Glover, Daniel P. Grosvenor, Catherine Hardacre, Richard Hill, Ben Johnson, Andy Jones, Zak Kipling, Graham Mann, James Mollard, Fiona M. O'Connor, Julien Palmiéri, Carly Reddington, Steven T. Rumbold, Mark Richardson, Nick A. J. Schutgens, Philip Stier, Marc Stringer, Yongming Tang, Jeremy Walton, Stephanie Woodward, and Andrew Yool
Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, https://doi.org/10.5194/gmd-13-6383-2020, 2020
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Aerosols are an important component of the Earth system. Here, we comprehensively document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 and UKESM1. This study provides a useful characterisation of the aerosol climatology in both models, facilitating the understanding of the numerous aerosol–climate interaction studies that will be conducted for CMIP6 and beyond.
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.
Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
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Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
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Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Conor G. Bolas, Valerio Ferracci, Andrew D. Robinson, Mohammed I. Mead, Mohd Shahrul Mohd Nadzir, John A. Pyle, Roderic L. Jones, and Neil R. P. Harris
Atmos. Meas. Tech., 13, 821–838, https://doi.org/10.5194/amt-13-821-2020, https://doi.org/10.5194/amt-13-821-2020, 2020
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Here we present the iDirac, a new instrument capable of making isoprene measurements in remote and challenging environments. The iDirac is a customisable and rugged field instrument for investigating emissions of volatile organic compounds from vegetation. It has been tested here in a series of experiments to ensure a high degree of technical precision, accuracy and repeatability. This new instrument allows us to ask and answer new questions about the influence of vegetation on the atmosphere.
Michal T. Filus, Elliot L. Atlas, Maria A. Navarro, Elena Meneguz, David Thomson, Matthew J. Ashfold, Lucy J. Carpenter, Stephen J. Andrews, and Neil R. P. Harris
Atmos. Chem. Phys., 20, 1163–1181, https://doi.org/10.5194/acp-20-1163-2020, https://doi.org/10.5194/acp-20-1163-2020, 2020
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The effectiveness of transport of short-lived halocarbons to the upper troposphere and lower stratosphere remains an important unknown in quantifying the supply of ozone-depleting substances to the stratosphere. In early 2014, a major field campaign in Guam in the western Pacific, involving UK and US research aircraft, sampled the tropical troposphere and lower stratosphere. The resulting measurements of CH3I, CHBr3 and CH2Br2 are compared here with calculations from a Lagrangian model.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Kuo-Ying Wang, Philippe Nedelec, Hannah Clark, and Neil Harris
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2019-156, https://doi.org/10.5194/essd-2019-156, 2019
Revised manuscript not accepted
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Atmospheric dispersion of radioactive materials following the accidents of the 11 March 2011 Fukushima Nuclear Power Plants contain very distinctive characteristics
over the land surface areas and over the oceanic atmosphere. Air dose rates measured over the land surface areas exhibit a combination of the effects from the deposited radioactive materials on the surface and the airborne radioactive materials. Air dose rates measured over the oceanic atmosphere were due to airborne particles.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
David C. Wade, Nathan Luke Abraham, Alexander Farnsworth, Paul J. Valdes, Fran Bragg, and Alexander T. Archibald
Clim. Past, 15, 1463–1483, https://doi.org/10.5194/cp-15-1463-2019, https://doi.org/10.5194/cp-15-1463-2019, 2019
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The amount of O2 in the atmosphere may have varied from as little as 10 % to as much as 35 % during the last 541 Myr. These changes are large enough to have led to changes in atmospheric mass, which may alter the radiative budget of the atmosphere. We present the first fully 3-D numerical model simulations to investigate the climate impacts of changes in O2 during different climate states. We identify a complex new mechanism causing increases in surface temperature when O2 levels were higher.
Ewa M. Bednarz, Amanda C. Maycock, Peter Braesicke, Paul J. Telford, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 9833–9846, https://doi.org/10.5194/acp-19-9833-2019, https://doi.org/10.5194/acp-19-9833-2019, 2019
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The atmospheric response to the amplitude of 11-year solar cycle in UM-UKCA is separated into the contributions from changes in direct radiative heating and photolysis rates, and the results compared with a control case with both effects included. We find that while the tropical responses are largely additive, this is not necessarily the case in the high latitudes. We suggest that solar-induced changes in ozone are important for modulating the SH dynamical response to the 11-year solar cycle.
Stuart N. Riddick, Denise L. Mauzerall, Michael Celia, Neil R. P. Harris, Grant Allen, Joseph Pitt, John Staunton-Sykes, Grant L. Forster, Mary Kang, David Lowry, Euan G. Nisbet, and Alistair J. Manning
Atmos. Chem. Phys., 19, 9787–9796, https://doi.org/10.5194/acp-19-9787-2019, https://doi.org/10.5194/acp-19-9787-2019, 2019
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Currently, bottom-up methods estimate that 0.13 % of methane produced by UK North Sea oil and gas installations is lost. Here we measure emissions from eight platforms in the North Sea and, when considered collectively, the methane loss is estimated at 0.19 % of gas production. As this ambient loss is not explicitly accounted for in the bottom-up approach, these measured emissions represent significant additional emissions above previous estimates.
Zainab Q. Hakim, Scott Archer-Nicholls, Gufran Beig, Gerd A. Folberth, Kengo Sudo, Nathan Luke Abraham, Sachin Ghude, Daven K. Henze, and Alexander T. Archibald
Atmos. Chem. Phys., 19, 6437–6458, https://doi.org/10.5194/acp-19-6437-2019, https://doi.org/10.5194/acp-19-6437-2019, 2019
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Surface ozone is an important air pollutant and recent work has calculated that large numbers of people die prematurely because of exposure to high levels of surface ozone in India. However, these calculations require model simulations of ozone as key inputs.
Here we perform the most thorough evaluation of global model surface ozone over India to date. These analyses of model simulations and observations highlight some successes and shortcomings and the need for further process-based studies.
Ewa M. Bednarz, Amanda C. Maycock, Paul J. Telford, Peter Braesicke, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 5209–5233, https://doi.org/10.5194/acp-19-5209-2019, https://doi.org/10.5194/acp-19-5209-2019, 2019
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Following model improvements, the atmospheric response to the 11-year solar cycle forcing simulated in the UM-UKCA chemistry–climate model is discussed for the first time. In contrast to most previous studies in the literature, we compare the results diagnosed using both a composite and a MLR methodology, and we show that apparently different signals can be diagnosed in the troposphere. In addition, we look at the role of internal atmospheric variability for the detection of the solar response.
Fraser Dennison, James Keeble, Olaf Morgenstern, Guang Zeng, N. Luke Abraham, and Xin Yang
Geosci. Model Dev., 12, 1227–1239, https://doi.org/10.5194/gmd-12-1227-2019, https://doi.org/10.5194/gmd-12-1227-2019, 2019
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Two developments are made to the United Kingdom Chemistry and Aerosols (UKCA) model to improve simulation of stratospheric ozone. The first is the addition of a solar cycle. The influence on ozone from the solar cycle is found to be 1–2 %, which is consistent with other studies. The second is to the heterogeneous chemistry, the most significant change being the addition of reactions involving bromine species. This was shown to reduce ozone biases relative to observations in most regions.
Sarah Connors, Alistair J. Manning, Andrew D. Robinson, Stuart N. Riddick, Grant L. Forster, Anita Ganesan, Aoife Grant, Stephen Humphrey, Simon O'Doherty, Dave E. Oram, Paul I. Palmer, Robert L. Skelton, Kieran Stanley, Ann Stavert, Dickon Young, and Neil R. P. Harris
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1187, https://doi.org/10.5194/acp-2018-1187, 2018
Preprint withdrawn
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Methane is an important greenhouse gas & reducing its emissions is a vital part of climate change mitigation to limit global temperature increase to 1.5 °C or 2.0 °C. This paper explains a way to estimate emitted methane over a sub-national area by combining measurements & computer dispersion modelling in a so-called
inversiontechnique. Compared with the current national inventory, our results show lower emissions for Cambridgeshire, possibly due to waste sector emission differences.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
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Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Liang Feng, Paul I. Palmer, Robyn Butler, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Ross J. Salawitch, Laura L. Pan, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 14787–14798, https://doi.org/10.5194/acp-18-14787-2018, https://doi.org/10.5194/acp-18-14787-2018, 2018
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We infer surface fluxes of bromoform (CHBr3) and dibromoform (CH2Br2) from CAST and CONTRAST aircraft observations over the western Pacific, using a tagged version of the GEOS-Chem global 3-D atmospheric chemistry model and a Maximum A Posteriori inverse model. Using the aircraft data, we estimate the regional fluxes about 20–40 % smaller than the prior inventories by Ordóñez et al. (2012). We find no evidence to support a robust linear relationship between CHBr3 and CH2Br2 oceanic emissions.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
Nathan Luke Abraham, Alexander T. Archibald, Paul Cresswell, Sam Cusworth, Mohit Dalvi, David Matthews, Steven Wardle, and Stuart Whitehouse
Geosci. Model Dev., 11, 3647–3657, https://doi.org/10.5194/gmd-11-3647-2018, https://doi.org/10.5194/gmd-11-3647-2018, 2018
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Using a virtual machine environment, a low-resolution configuration of the United Kingdom Chemistry and Aerosols (UKCA) composition-climate model has been developed. This configuration, while not suitable for long simulations, is an excellent test-bed for new model developments and can be used to train new users in how to use UKCA. This work was motivated by the desire to improve the usability of UKCA, and to encourage more users to become involved with the code development process.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Emre Esentürk, Nathan Luke Abraham, Scott Archer-Nicholls, Christina Mitsakou, Paul Griffiths, Alex Archibald, and John Pyle
Geosci. Model Dev., 11, 3089–3108, https://doi.org/10.5194/gmd-11-3089-2018, https://doi.org/10.5194/gmd-11-3089-2018, 2018
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An integral and expensive part of coupled climate model simulations is the gas-phase chemistry which gives rise to hundreds of coupled differential equations. We propose a method which improves the convergence and robustness properties of commonly used Newton–Raphson solvers. The method is flexible and can be appended to most algorithms. The approach can be useful for a broader community of computational scientists whose interests lie in solving systems with intensive interactive chemistry.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Valerio Ferracci, Ines Heimann, N. Luke Abraham, John A. Pyle, and Alexander T. Archibald
Atmos. Chem. Phys., 18, 7109–7129, https://doi.org/10.5194/acp-18-7109-2018, https://doi.org/10.5194/acp-18-7109-2018, 2018
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Hydroxyl radicals (OH) control the removal of species emitted in the atmosphere. Field campaigns reported a "missing" OH sink, not included in current atmospheric models. In this work a global model was used to establish the impact of additional OH sinks, based on both observations of the missing sink and newly discovered reactions of OH. Results show modest increases in global atmospheric lifetimes but pronounced regional effects on the abundance of some key species.
James Keeble, Ewa M. Bednarz, Antara Banerjee, N. Luke Abraham, Neil R. P. Harris, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 17, 13801–13818, https://doi.org/10.5194/acp-17-13801-2017, https://doi.org/10.5194/acp-17-13801-2017, 2017
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In this study we explore the chemical and transport processes controlling ozone abundances in different altitude regions in the tropics for the present day and how these processes may change in the future in order to determine when total-column ozone values in the tropics will recover to pre-1980s values following the implementation of the Montreal Protocol and its subsequent amendments, which imposed bans on the use and emissions of CFCs.
Hannah Sonderfeld, Hartmut Bösch, Antoine P. R. Jeanjean, Stuart N. Riddick, Grant Allen, Sébastien Ars, Stewart Davies, Neil Harris, Neil Humpage, Roland Leigh, and Joseph Pitt
Atmos. Meas. Tech., 10, 3931–3946, https://doi.org/10.5194/amt-10-3931-2017, https://doi.org/10.5194/amt-10-3931-2017, 2017
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The waste sector is the second largest source of methane in the UK. However, uncertainties of methane emissions from landfill sites still remain. In this study we present a new approach for the estimation of methane emissions from a landfill site by applying a computational fluid dynamics (CFD) model for precise measurements of methane with in situ Fourier-transform infrared (FTIR) spectroscopy. Different source areas could be distinguished with this method and their emissions were assessed.
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma C. Leedham Elvidge, Grant L. Forster, Neil R. P. Harris, Mohammed Iqbal Mead, Azizan Abu Samah, Siew Moi Phang, Chang-Feng Ou-Yang, Neng-Huei Lin, Jia-Lin Wang, Angela K. Baker, Carl A. M. Brenninkmeijer, and David Sherry
Atmos. Chem. Phys., 17, 11929–11941, https://doi.org/10.5194/acp-17-11929-2017, https://doi.org/10.5194/acp-17-11929-2017, 2017
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We have observed large amounts of man-made chlorine compounds in E and SE Asia and in the upper tropical troposphere. These relatively short-lived compounds are not controlled by the Montreal Protocol, but if significant quantities were able to reach the stratosphere, the long-term recovery of stratospheric ozone would be delayed. We have also identified an important atmospheric transport mechanism that can rapidly transport these chemicals from E Asia to the upper troposphere via the tropics.
Wolfgang Steinbrecht, Lucien Froidevaux, Ryan Fuller, Ray Wang, John Anderson, Chris Roth, Adam Bourassa, Doug Degenstein, Robert Damadeo, Joe Zawodny, Stacey Frith, Richard McPeters, Pawan Bhartia, Jeannette Wild, Craig Long, Sean Davis, Karen Rosenlof, Viktoria Sofieva, Kaley Walker, Nabiz Rahpoe, Alexei Rozanov, Mark Weber, Alexandra Laeng, Thomas von Clarmann, Gabriele Stiller, Natalya Kramarova, Sophie Godin-Beekmann, Thierry Leblanc, Richard Querel, Daan Swart, Ian Boyd, Klemens Hocke, Niklaus Kämpfer, Eliane Maillard Barras, Lorena Moreira, Gerald Nedoluha, Corinne Vigouroux, Thomas Blumenstock, Matthias Schneider, Omaira García, Nicholas Jones, Emmanuel Mahieu, Dan Smale, Michael Kotkamp, John Robinson, Irina Petropavlovskikh, Neil Harris, Birgit Hassler, Daan Hubert, and Fiona Tummon
Atmos. Chem. Phys., 17, 10675–10690, https://doi.org/10.5194/acp-17-10675-2017, https://doi.org/10.5194/acp-17-10675-2017, 2017
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Thanks to the 1987 Montreal Protocol and its amendments, ozone-depleting chlorine (and bromine) in the stratosphere has declined slowly since the late 1990s. Improved and extended long-term ozone profile observations from satellites and ground-based stations confirm that ozone is responding as expected and has increased by about 2 % per decade since 2000 in the upper stratosphere, around 40 km altitude. At lower altitudes, however, ozone has not changed significantly since 2000.
Stuart N. Riddick, Sarah Connors, Andrew D. Robinson, Alistair J. Manning, Pippa S. D. Jones, David Lowry, Euan Nisbet, Robert L. Skelton, Grant Allen, Joseph Pitt, and Neil R. P. Harris
Atmos. Chem. Phys., 17, 7839–7851, https://doi.org/10.5194/acp-17-7839-2017, https://doi.org/10.5194/acp-17-7839-2017, 2017
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High methane mixing ratios occurred at our long-term measurement site. Isotopic measurements show the source is a landfill 7 km away; the emissions were estimated using three different approaches. The emission estimates made by near-source and middle-distance methods agree well for a period of intense observation. The estimate of the inverse modelling is similar to the labour-intensive middle-distance approach, which shows it can be used to identify point sources within an emission landscape.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Mingjin Tang, James Keeble, Paul J. Telford, Francis D. Pope, Peter Braesicke, Paul T. Griffiths, N. Luke Abraham, James McGregor, I. Matt Watson, R. Anthony Cox, John A. Pyle, and Markus Kalberer
Atmos. Chem. Phys., 16, 15397–15412, https://doi.org/10.5194/acp-16-15397-2016, https://doi.org/10.5194/acp-16-15397-2016, 2016
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We have investigated for the first time the heterogeneous hydrolysis of ClONO2 on TiO2 and SiO2 aerosol particles at room temperature and at different relative humidities (RHs), using an aerosol flow tube. The kinetic data reported in our current and previous studies have been included in the UKCA chemistry–climate model to assess the impact of TiO2 injection on stratospheric chemistry and stratospheric ozone in particular.
Ewa M. Bednarz, Amanda C. Maycock, N. Luke Abraham, Peter Braesicke, Olivier Dessens, and John A. Pyle
Atmos. Chem. Phys., 16, 12159–12176, https://doi.org/10.5194/acp-16-12159-2016, https://doi.org/10.5194/acp-16-12159-2016, 2016
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Future trends in springtime Arctic ozone, and its chemical dynamical and radiative drivers, are analysed using a 7-member ensemble of chemistry–climate model integrations, allowing for a detailed assessment of interannual variability. Despite the future long-term recovery of Arctic ozone, there is large interannual variability and episodic reductions in springtime Arctic column ozone. Halogen chemistry will become a smaller but non-negligible driver of Arctic ozone variability over the century.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Peer Johannes Nowack, Nathan Luke Abraham, Peter Braesicke, and John Adrian Pyle
Atmos. Chem. Phys., 16, 4191–4203, https://doi.org/10.5194/acp-16-4191-2016, https://doi.org/10.5194/acp-16-4191-2016, 2016
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Various forms of solar radiation management (SRM) have been proposed to counteract man-made climate change. However, all these countermeasures could have unintended side-effects. We add a novel perspective to this discussion by showing how atmospheric ozone changes under solar geoengineering could affect UV exposure and air pollution. This would have implications for human health and ecology. Atmospheric composition changes are therefore important to consider in the evaluation of any SRM scheme.
Antara Banerjee, Amanda C. Maycock, Alexander T. Archibald, N. Luke Abraham, Paul Telford, Peter Braesicke, and John A. Pyle
Atmos. Chem. Phys., 16, 2727–2746, https://doi.org/10.5194/acp-16-2727-2016, https://doi.org/10.5194/acp-16-2727-2016, 2016
M. R. Russo, M. J. Ashfold, N. R. P. Harris, and J. A. Pyle
Atmos. Chem. Phys., 15, 14031–14040, https://doi.org/10.5194/acp-15-14031-2015, https://doi.org/10.5194/acp-15-14031-2015, 2015
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We find a strong regional element to the uplift of CHBr3 from the ocean to the upper troposphere and lower stratosphere. The strongest uplift occurs when the largest emission and the most intense convection are co-located which is over the Maritime Continent in northern winter. Estimates of CHBr3 emissions based on aircraft measurements will be sensitive to where the available aircraft campaigns took place.
R. S. Humphries, R. Schofield, M. D. Keywood, J. Ward, J. R. Pierce, C. M. Gionfriddo, M. T. Tate, D. P. Krabbenhoft, I. E. Galbally, S. B. Molloy, A. R. Klekociuk, P. V. Johnston, K. Kreher, A. J. Thomas, A. D. Robinson, N. R. P. Harris, R. Johnson, and S. R. Wilson
Atmos. Chem. Phys., 15, 13339–13364, https://doi.org/10.5194/acp-15-13339-2015, https://doi.org/10.5194/acp-15-13339-2015, 2015
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An atmospheric new particle formation event that was observed in the pristine East Antarctic pack ice during a springtime voyage in 2012 is characterised in terms of formation and growth rates. Known nucleation mechanisms (e.g. those involving sulfate, iodine and organics) were unable to explain observations; however, correlations with total gaseous mercury were found, leading to the suggestion of a possible mercury-driven nucleation mechanism not previously described.
N. R. P. Harris, B. Hassler, F. Tummon, G. E. Bodeker, D. Hubert, I. Petropavlovskikh, W. Steinbrecht, J. Anderson, P. K. Bhartia, C. D. Boone, A. Bourassa, S. M. Davis, D. Degenstein, A. Delcloo, S. M. Frith, L. Froidevaux, S. Godin-Beekmann, N. Jones, M. J. Kurylo, E. Kyrölä, M. Laine, S. T. Leblanc, J.-C. Lambert, B. Liley, E. Mahieu, A. Maycock, M. de Mazière, A. Parrish, R. Querel, K. H. Rosenlof, C. Roth, C. Sioris, J. Staehelin, R. S. Stolarski, R. Stübi, J. Tamminen, C. Vigouroux, K. A. Walker, H. J. Wang, J. Wild, and J. M. Zawodny
Atmos. Chem. Phys., 15, 9965–9982, https://doi.org/10.5194/acp-15-9965-2015, https://doi.org/10.5194/acp-15-9965-2015, 2015
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Trends in the vertical distribution of ozone are reported for new and recently revised data sets. The amount of ozone-depleting compounds in the stratosphere peaked in the second half of the 1990s. We examine the trends before and after that peak to see if any change in trend is discernible. The previously reported decreases are confirmed. Furthermore, the downward trend in upper stratospheric ozone has not continued. The possible significance of any increase is discussed in detail.
M. J. Ashfold, J. A. Pyle, A. D. Robinson, E. Meneguz, M. S. M. Nadzir, S. M. Phang, A. A. Samah, S. Ong, H. E. Ung, L. K. Peng, S. E. Yong, and N. R. P. Harris
Atmos. Chem. Phys., 15, 3565–3573, https://doi.org/10.5194/acp-15-3565-2015, https://doi.org/10.5194/acp-15-3565-2015, 2015
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We use observations and model calculations to show that "cold surges" occurring during Northern Hemisphere winter can rapidly transport East Asian pollution to equatorial Southeast Asia. As well as affecting atmospheric composition near the surface, we argue that strong convection can subsequently lift the polluted air masses to the tropical upper troposphere. This suggests a potentially important connection between midlatitude pollution sources and the lower stratosphere.
F. Tummon, B. Hassler, N. R. P. Harris, J. Staehelin, W. Steinbrecht, J. Anderson, G. E. Bodeker, A. Bourassa, S. M. Davis, D. Degenstein, S. M. Frith, L. Froidevaux, E. Kyrölä, M. Laine, C. Long, A. A. Penckwitt, C. E. Sioris, K. H. Rosenlof, C. Roth, H.-J. Wang, and J. Wild
Atmos. Chem. Phys., 15, 3021–3043, https://doi.org/10.5194/acp-15-3021-2015, https://doi.org/10.5194/acp-15-3021-2015, 2015
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Understanding ozone trends in the vertical is vital in terms of assessing the success of the Montreal Protocol. This paper compares and analyses the long-term trends in stratospheric ozone from seven new merged satellite data sets. The data sets largely agree well with each other, particularly for the negative trends seen in the early period 1984-1997. For the 1998-2011 period there is less agreement, but a clear shift from negative to mostly positive trends.
A. Orr, J. S. Hosking, L. Hoffmann, J. Keeble, S. M. Dean, H. K. Roscoe, N. L. Abraham, S. Vosper, and P. Braesicke
Atmos. Chem. Phys., 15, 1071–1086, https://doi.org/10.5194/acp-15-1071-2015, https://doi.org/10.5194/acp-15-1071-2015, 2015
J. Keeble, P. Braesicke, N. L. Abraham, H. K. Roscoe, and J. A. Pyle
Atmos. Chem. Phys., 14, 13705–13717, https://doi.org/10.5194/acp-14-13705-2014, https://doi.org/10.5194/acp-14-13705-2014, 2014
S. S. Dhomse, K. M. Emmerson, G. W. Mann, N. Bellouin, K. S. Carslaw, M. P. Chipperfield, R. Hommel, N. L. Abraham, P. Telford, P. Braesicke, M. Dalvi, C. E. Johnson, F. O'Connor, O. Morgenstern, J. A. Pyle, T. Deshler, J. M. Zawodny, and L. W. Thomason
Atmos. Chem. Phys., 14, 11221–11246, https://doi.org/10.5194/acp-14-11221-2014, https://doi.org/10.5194/acp-14-11221-2014, 2014
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 10431–10438, https://doi.org/10.5194/acp-14-10431-2014, https://doi.org/10.5194/acp-14-10431-2014, 2014
A. Banerjee, A. T. Archibald, A. C. Maycock, P. Telford, N. L. Abraham, X. Yang, P. Braesicke, and J. A. Pyle
Atmos. Chem. Phys., 14, 9871–9881, https://doi.org/10.5194/acp-14-9871-2014, https://doi.org/10.5194/acp-14-9871-2014, 2014
A. D. Robinson, N. R. P. Harris, M. J. Ashfold, B. Gostlow, N. J. Warwick, L. M. O'Brien, E. J. Beardmore, M. S. M. Nadzir, S. M. Phang, A. A. Samah, S. Ong, H. E. Ung, L. K. Peng, S. E. Yong, M. Mohamad, and J. A. Pyle
Atmos. Chem. Phys., 14, 8369–8388, https://doi.org/10.5194/acp-14-8369-2014, https://doi.org/10.5194/acp-14-8369-2014, 2014
M. J. Ashfold, N. R. P. Harris, A. J. Manning, A. D. Robinson, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 979–994, https://doi.org/10.5194/acp-14-979-2014, https://doi.org/10.5194/acp-14-979-2014, 2014
P. Braesicke, J. Keeble, X. Yang, G. Stiller, S. Kellmann, N. L. Abraham, A. Archibald, P. Telford, and J. A. Pyle
Atmos. Chem. Phys., 13, 10677–10688, https://doi.org/10.5194/acp-13-10677-2013, https://doi.org/10.5194/acp-13-10677-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)
Protection without poison: why tropical ozone maximizes in the interior of the atmosphere
Ozone trends in homogenized Umkehr, ozonesonde, and COH overpass records
Evaluating reanalysis representations of climatological trace gas distributions in the Asian monsoon tropopause layer
On the atmospheric budget of 1,2-dichloroethane and its impact on stratospheric chlorine and ozone (2002–2020)
Quantifying the decay rate of volcanic sulfur dioxide in the stratosphere
The return to 1980 stratospheric halogen levels: a moving target in ozone assessments from 2006 to 2022
The impact of dehydration and extremely low HCl values in the Antarctic stratospheric vortex in mid-winter on ozone loss in spring
Beyond self-healing: stabilizing and destabilizing photochemical adjustment of the ozone layer
Solar FTIR measurements of NOx vertical distributions – Part 2: Experiment-based scaling factors describing the daytime variation in stratospheric NOx
Technical note: Evaluation of the Copernicus Atmosphere Monitoring Service Cy48R1 upgrade of June 2023
Analysis of a newly homogenised ozonesonde dataset from Lauder, New Zealand
Correction of stratospheric age of air (AoA) derived from sulfur hexafluoride (SF6) for the effect of chemical sinks
Opinion: Stratospheric ozone – depletion, recovery and new challenges
Quantum yields of CHDO above 300 nm
Sensitivities of atmospheric composition and climate to altitude and latitude of hypersonic aircraft emissions
Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 2: Impacts on ozone
N2O as a regression proxy for dynamical variability in stratospheric trace gas trends
The influence of future changes in springtime Arctic ozone on stratospheric and surface climate
Weakening of springtime Arctic ozone depletion with climate change
The impact of an extreme solar event on the middle atmosphere: a case study
The future ozone trends in changing climate simulated with SOCOLv4
Atmospheric distribution of HCN from satellite observations and 3-D model simulations
Indicators of the ozone recovery for selected sites in the Northern Hemisphere mid-latitudes derived from various total column ozone datasets (1980–2020)
The historical ozone trends simulated with the SOCOLv4 and their comparison with observations and reanalyses
Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 1: Stratospheric chlorine budget and the role of transport
Effects of reanalysis forcing fields on ozone trends and age of air from a chemical transport model
The influence of energetic particle precipitation on Antarctic stratospheric chlorine and ozone over the 20th century
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
An Arctic ozone hole in 2020 if not for the Montreal Protocol
Effects of enhanced downwelling of NOx on Antarctic upper-stratospheric ozone in the 21st century
Processes influencing lower stratospheric water vapour in monsoon anticyclones: insights from Lagrangian modelling
Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100
Slow feedbacks resulting from strongly enhanced atmospheric methane mixing ratios in a chemistry–climate model with mixed-layer ocean
Impact of the eruption of Mt Pinatubo on the chemical composition of the stratosphere
Projecting ozone hole recovery using an ensemble of chemistry–climate models weighted by model performance and independence
Inconsistencies between chemistry–climate models and observed lower stratospheric ozone trends since 1998
Reformulating the bromine alpha factor and equivalent effective stratospheric chlorine (EESC): evolution of ozone destruction rates of bromine and chlorine in future climate scenarios
Analysis and attribution of total column ozone changes over the Tibetan Plateau during 1979–2017
Seasonal impact of biogenic very short-lived bromocarbons on lowermost stratospheric ozone between 60° N and 60° S during the 21st century
Modelling the potential impacts of the recent, unexpected increase in CFC-11 emissions on total column ozone recovery
The potential impacts of a sulfur- and halogen-rich supereruption such as Los Chocoyos on the atmosphere and climate
Technical note: Intermittent reduction of the stratospheric ozone over northern Europe caused by a storm in the Atlantic Ocean
Possible implications of enhanced chlorofluorocarbon-11 concentrations on ozone
Technical note: Reanalysis of Aura MLS chemical observations
Separating the role of direct radiative heating and photolysis in modulating the atmospheric response to the amplitude of the 11-year solar cycle forcing
Reactive nitrogen (NOy) and ozone responses to energetic electron precipitation during Southern Hemisphere winter
Implication of strongly increased atmospheric methane concentrations for chemistry–climate connections
Multitimescale variations in modeled stratospheric water vapor derived from three modern reanalysis products
How robust are stratospheric age of air trends from different reanalyses?
Evaluation of CESM1 (WACCM) free-running and specified dynamics atmospheric composition simulations using global multispecies satellite data records
Aaron Match, Edwin P. Gerber, and Stephan Fueglistaler
Atmos. Chem. Phys., 25, 4349–4366, https://doi.org/10.5194/acp-25-4349-2025, https://doi.org/10.5194/acp-25-4349-2025, 2025
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The ozone concentration in the tropical stratosphere peaks at 26 km, protecting life from harmful ultraviolet light without poisoning it. Climate models reproduce this peak, but textbook explanations yield errors of 10 km. Simplifying the well-understood sources and sinks of ozone, we develop a theory explaining that tropical ozone peaks where its dominant sink transitions from damping of atomic oxygen aloft (mainly via catalytic chemistry) to damping of ozone below (mainly via transport).
Irina Petropavlovskikh, Jeannette D. Wild, Kari Abromitis, Peter Effertz, Koji Miyagawa, Lawrence E. Flynn, Eliane Maillard Barras, Robert Damadeo, Glen McConville, Bryan Johnson, Patrick Cullis, Sophie Godin-Beekmann, Gerard Ancellet, Richard Querel, Roeland Van Malderen, and Daniel Zawada
Atmos. Chem. Phys., 25, 2895–2936, https://doi.org/10.5194/acp-25-2895-2025, https://doi.org/10.5194/acp-25-2895-2025, 2025
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Observational records show that stratospheric ozone is recovering in accordance with the implementation of the Montreal Protocol and its amendments. Natural ozone variability complicates the detection of small trends. This study optimizes a statistical model fit in ground-station-based observational records by adding parameters that interpret seasonal and long-term changes in atmospheric circulation and airmass mixing, which reduces uncertainties in detecting the stratospheric ozone recovery.
Jonathon S. Wright, Shenglong Zhang, Jiao Chen, Sean M. Davis, Paul Konopka, Mengqian Lu, Xiaolu Yan, and Guang J. Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-135, https://doi.org/10.5194/egusphere-2025-135, 2025
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Atmospheric reanalysis products reconstruct the past states of the atmosphere. These products are often used to study winds and temperatures in the upper-level monsoon circulation, but their ability to reproduce composition fields like water vapor and ozone has been questionable at best. Here we report clear signs of improvement in both consistency across reanalyses and agreement with satellite observations, outline limitations and suggest steps to further enhance the usefulness of these fields.
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.
Paul A. Nicknish, Kane Stone, Susan Solomon, and Simon A. Carn
EGUsphere, https://doi.org/10.5194/egusphere-2024-3525, https://doi.org/10.5194/egusphere-2024-3525, 2024
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Large volcanic eruptions can inject teragrams of sulfur dioxide (SO2) into the stratosphere, influencing stratospheric chemistry and Earth's climate. This work calculates lifetime of volcanic, gas-phase SO2 in the stratosphere using data from three satellite products. SO2 lifetimes vary significantly between the different products, and this uncertainty limits our ability to attribute an observed SO2 lifetime following an eruption to a specific chemical process.
Megan J. Lickley, John S. Daniel, Laura A. McBride, Ross J. Salawitch, and Guus J. M. Velders
Atmos. Chem. Phys., 24, 13081–13099, https://doi.org/10.5194/acp-24-13081-2024, https://doi.org/10.5194/acp-24-13081-2024, 2024
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The expected ozone recovery date was delayed by 17 years between the 2006 and 2022 international scientific assessments of ozone depletion. We quantify the primary drivers of this delay. Changes in the metric used to estimate ozone recovery explain ca. 5 years of this delay. Of the remaining 12 years, changes in estimated banks, atmospheric lifetimes, and emission projections explain 4, 3.5, and 3 years of this delay, respectively.
Yiran Zhang-Liu, Rolf Müller, Jens-Uwe Grooß, Sabine Robrecht, Bärbel Vogel, Abdul Mannan Zafar, and Ralph Lehmann
Atmos. Chem. Phys., 24, 12557–12574, https://doi.org/10.5194/acp-24-12557-2024, https://doi.org/10.5194/acp-24-12557-2024, 2024
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HCl null cycles in Antarctica are important for maintaining high values of ozone-destroying chlorine in Antarctic spring. These HCl null cycles are not affected by (1) using the most recent recommendations of chemical kinetics (compared to older recommendations), (2) accounting for dehydration in the Antarctic winter vortex, and (3) considering the observed (but unexplained) depletion of HCl in mid-winter in the Antarctic vortex throughout Antarctic winter.
Aaron Match, Edwin P. Gerber, and Stephan Fueglistaler
Atmos. Chem. Phys., 24, 10305–10322, https://doi.org/10.5194/acp-24-10305-2024, https://doi.org/10.5194/acp-24-10305-2024, 2024
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Earth's ozone layer absorbs incoming UV light, protecting life. Removing ozone aloft allows UV light to penetrate deeper, where it is known to produce new ozone, leading to "self-healing" that partially stabilizes total ozone. However, a photochemistry model shows that, above 40 km in the tropics, deeper-penetrating UV destroys ozone, destabilizing the total ozone. Photochemical theory reveals that this destabilizing regime occurs where overhead ozone is below a key threshold.
Pinchas Nürnberg, Sarah A. Strode, and Ralf Sussmann
Atmos. Chem. Phys., 24, 10001–10012, https://doi.org/10.5194/acp-24-10001-2024, https://doi.org/10.5194/acp-24-10001-2024, 2024
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We created a set of scaling factors describing the diurnal increase in stratospheric nitrogen oxides above Zugspitze, Germany. We used these factors to validate recently published model simulation data. On the one hand, this validation enables the use of the validated data to better understand the stratospheric photochemistry. On the other hand, it can improve satellite validation, which has implications for the understanding of urban smog events and other pollution events in the troposphere.
Henk Eskes, Athanasios Tsikerdekis, Melanie Ades, Mihai Alexe, Anna Carlin Benedictow, Yasmine Bennouna, Lewis Blake, Idir Bouarar, Simon Chabrillat, Richard Engelen, Quentin Errera, Johannes Flemming, Sebastien Garrigues, Jan Griesfeller, Vincent Huijnen, Luka Ilić, Antje Inness, John Kapsomenakis, Zak Kipling, Bavo Langerock, Augustin Mortier, Mark Parrington, Isabelle Pison, Mikko Pitkänen, Samuel Remy, Andreas Richter, Anja Schoenhardt, Michael Schulz, Valerie Thouret, Thorsten Warneke, Christos Zerefos, and Vincent-Henri Peuch
Atmos. Chem. Phys., 24, 9475–9514, https://doi.org/10.5194/acp-24-9475-2024, https://doi.org/10.5194/acp-24-9475-2024, 2024
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The Copernicus Atmosphere Monitoring Service (CAMS) provides global analyses and forecasts of aerosols and trace gases in the atmosphere. On 27 June 2023 a major upgrade, Cy48R1, became operational. Comparisons with in situ, surface remote sensing, aircraft, and balloon and satellite observations show that the new CAMS system is a significant improvement. The results quantify the skill of CAMS to forecast impactful events, such as wildfires, dust storms and air pollution peaks.
Guang Zeng, Richard Querel, Hisako Shiona, Deniz Poyraz, Roeland Van Malderen, Alex Geddes, Penny Smale, Dan Smale, John Robinson, and Olaf Morgenstern
Atmos. Chem. Phys., 24, 6413–6432, https://doi.org/10.5194/acp-24-6413-2024, https://doi.org/10.5194/acp-24-6413-2024, 2024
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We present a homogenised ozonesonde record (1987–2020) for Lauder, a Southern Hemisphere mid-latitude site; identify factors driving ozone trends; and attribute them to anthropogenic forcings using statistical analysis and model simulations. We find that significant negative lower-stratospheric ozone trends identified at Lauder are associated with an increase in tropopause height and that CO2-driven dynamical changes have played an increasingly important role in driving ozone trends.
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.
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.
Ernst-Peter Röth and Luc Vereecken
Atmos. Chem. Phys., 24, 2625–2638, https://doi.org/10.5194/acp-24-2625-2024, https://doi.org/10.5194/acp-24-2625-2024, 2024
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The paper presents the radical and molecular product quantum yields in the photolysis reaction of CHDO at wavelengths above 300 nm. Two different approaches based on literature data are used, with results falling within both approaches' uncertainty ranges. Simple functional forms are presented for use in photochemical models of the atmosphere.
Johannes Pletzer and Volker Grewe
Atmos. Chem. Phys., 24, 1743–1775, https://doi.org/10.5194/acp-24-1743-2024, https://doi.org/10.5194/acp-24-1743-2024, 2024
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Very fast aircraft can travel at 30–40 km altitude and are designed to use liquid hydrogen as fuel instead of kerosene. Depending on their flight altitude, the impact of these aircraft on the atmosphere and climate can change very much. Our results show that a variation inflight latitude can have a considerably higher change in impact compared to a variation in flight altitude. Atmospheric air transport and polar stratospheric clouds play an important role in hypersonic aircraft emissions.
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.
Kimberlee Dubé, Susann Tegtmeier, Adam Bourassa, Daniel Zawada, Douglas Degenstein, Patrick E. Sheese, Kaley A. Walker, and William Randel
Atmos. Chem. Phys., 23, 13283–13300, https://doi.org/10.5194/acp-23-13283-2023, https://doi.org/10.5194/acp-23-13283-2023, 2023
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This paper presents a technique for understanding the causes of long-term changes in stratospheric composition. By using N2O as a proxy for stratospheric circulation in the model used to calculated trends, it is possible to separate the effects of dynamics and chemistry on observed trace gas trends. We find that observed HCl increases are due to changes in the stratospheric circulation, as are O3 decreases above 30 hPa in the Northern Hemisphere.
Gabriel Chiodo, Marina Friedel, Svenja Seeber, Daniela Domeisen, Andrea Stenke, Timofei Sukhodolov, and Franziska Zilker
Atmos. Chem. Phys., 23, 10451–10472, https://doi.org/10.5194/acp-23-10451-2023, https://doi.org/10.5194/acp-23-10451-2023, 2023
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Stratospheric ozone protects the biosphere from harmful UV radiation. Anthropogenic activity has led to a reduction in the ozone layer in the recent past, but thanks to the implementation of the Montreal Protocol, the ozone layer is projected to recover. In this study, we show that projected future changes in Arctic ozone abundances during springtime will influence stratospheric climate and thereby actively modulate large-scale circulation changes in the Northern Hemisphere.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Thomas Reddmann, Miriam Sinnhuber, Jan Maik Wissing, Olesya Yakovchuk, and Ilya Usoskin
Atmos. Chem. Phys., 23, 6989–7000, https://doi.org/10.5194/acp-23-6989-2023, https://doi.org/10.5194/acp-23-6989-2023, 2023
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Recent analyses of isotopic records of ice cores and sediments have shown that very strong explosions may occur on the Sun, perhaps about one such explosion every 1000 years. Such explosions pose a real threat to humankind. It is therefore of great interest to study the impact of such explosions on Earth. We analyzed how the explosions would affect the chemistry of the middle atmosphere and show that the related ozone loss is not dramatic and that the atmosphere will recover within 1 year.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, and Thomas Peter
Atmos. Chem. Phys., 23, 4801–4817, https://doi.org/10.5194/acp-23-4801-2023, https://doi.org/10.5194/acp-23-4801-2023, 2023
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The future ozone evolution in SOCOLv4 simulations under SSP2-4.5 and SSP5-8.5 scenarios has been assessed for the period 2015–2099 and subperiods using the DLM approach. The SOCOLv4 projects a decline in tropospheric ozone in the 2030s in SSP2-4.5 and in the 2060s in SSP5-8.5. The stratospheric ozone increase is ~3 times higher in SSP5-8.5, confirming the important role of GHGs in ozone evolution. We also showed that tropospheric ozone strongly impacts the total column in the tropics.
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.
Janusz Krzyścin
Atmos. Chem. Phys., 23, 3119–3132, https://doi.org/10.5194/acp-23-3119-2023, https://doi.org/10.5194/acp-23-3119-2023, 2023
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We propose indices to obtain the current stage of total column ozone (TCO3) recovery attributed to ozone-depleting substance (ODS) changes in the stratosphere. The indices are calculated using TCO3 values in key years of the ODS changes. The ozone recovery stage is derived for 16 sites in the NH mid-latitudes using results from ground and satellite measurements and reanalysis data. In Europe, there is a slow TCO3 recovery. A continuous TCO3 decline has been occurring in some sites since 1980.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, William Ball, and Thomas Peter
Atmos. Chem. Phys., 22, 15333–15350, https://doi.org/10.5194/acp-22-15333-2022, https://doi.org/10.5194/acp-22-15333-2022, 2022
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Applying the dynamic linear model, we confirm near-global ozone recovery (55°N–55°S) in the mesosphere, upper and middle stratosphere, and a steady increase in the troposphere. We also show that modern chemistry–climate models (CCMs) like SOCOLv4 may reproduce the observed trend distribution of lower stratospheric ozone, despite exhibiting a lower magnitude and statistical significance. The obtained ozone trend pattern in SOCOLv4 is generally consistent with observations and reanalysis datasets.
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.
Ville Maliniemi, Pavle Arsenovic, Annika Seppälä, and Hilde Nesse Tyssøy
Atmos. Chem. Phys., 22, 8137–8149, https://doi.org/10.5194/acp-22-8137-2022, https://doi.org/10.5194/acp-22-8137-2022, 2022
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We simulate the effect of energetic particle precipitation (EPP) on Antarctic stratospheric ozone chemistry over the whole 20th century. We find a significant increase of reactive nitrogen due to EP, which can deplete ozone via a catalytic reaction. Furthermore, significant modulation of active chlorine is obtained related to EPP, which impacts ozone depletion by both active chlorine and EPP. Our results show that EPP has been a significant modulator of ozone chemistry during the CFC era.
Daniel J. Ruiz and Michael J. Prather
Atmos. Chem. Phys., 22, 2079–2093, https://doi.org/10.5194/acp-22-2079-2022, https://doi.org/10.5194/acp-22-2079-2022, 2022
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The stratosphere is an important source of tropospheric ozone, which affects climate, chemistry, and air quality, but is extremely difficult to quantify given the large production and loss terms in the troposphere. Here, we use other gases that are well observed and quantified as a reference to test our simulations of ozone transport in the atmosphere. This allows us to better constrain the stratospheric source of ozone and also offers guidance to improve future simulations of ozone transport.
Catherine Wilka, Susan Solomon, Doug Kinnison, and David Tarasick
Atmos. Chem. Phys., 21, 15771–15781, https://doi.org/10.5194/acp-21-15771-2021, https://doi.org/10.5194/acp-21-15771-2021, 2021
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We use satellite and balloon measurements to evaluate modeled ozone loss seen in the unusually cold Arctic of 2020 in the real world and compare it to simulations of a world avoided. We show that extensive denitrification in 2020 provides an important test case for stratospheric model process representations. If the Montreal Protocol had not banned ozone-depleting substances, an Arctic ozone hole would have emerged for the first time in spring 2020 that is comparable to those in the Antarctic.
Ville Maliniemi, Hilde Nesse Tyssøy, Christine Smith-Johnsen, Pavle Arsenovic, and Daniel R. Marsh
Atmos. Chem. Phys., 21, 11041–11052, https://doi.org/10.5194/acp-21-11041-2021, https://doi.org/10.5194/acp-21-11041-2021, 2021
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We simulate ozone variability over the 21st century with different greenhouse gas scenarios. Our results highlight a novel mechanism of additional reactive nitrogen species descending to the Antarctic stratosphere from the thermosphere/upper mesosphere due to the accelerated residual circulation under climate change. This excess descending NOx can potentially prevent a super recovery of ozone in the Antarctic upper stratosphere.
Nuria Pilar Plaza, Aurélien Podglajen, Cristina Peña-Ortiz, and Felix Ploeger
Atmos. Chem. Phys., 21, 9585–9607, https://doi.org/10.5194/acp-21-9585-2021, https://doi.org/10.5194/acp-21-9585-2021, 2021
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We study the role of different processes in setting the lower stratospheric water vapour. We find that mechanisms involving ice microphysics and small-scale mixing produce the strongest increase in water vapour, in particular over the Asian Monsoon. Small-scale mixing has a special relevance as it improves the agreement with observations at seasonal and intra-seasonal timescales, contrary to the North American Monsoon case, in which large-scale temperatures still dominate its variability.
James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
Atmos. Chem. Phys., 21, 5015–5061, https://doi.org/10.5194/acp-21-5015-2021, https://doi.org/10.5194/acp-21-5015-2021, 2021
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Stratospheric ozone and water vapour are key components of the Earth system; changes to both have important impacts on global and regional climate. We evaluate changes to these species from 1850 to 2100 in the new generation of CMIP6 models. There is good agreement between the multi-model mean and observations, although there is substantial variation between the individual models. The future evolution of both ozone and water vapour is strongly dependent on the assumed future emissions scenario.
Laura Stecher, Franziska Winterstein, Martin Dameris, Patrick Jöckel, Michael Ponater, and Markus Kunze
Atmos. Chem. Phys., 21, 731–754, https://doi.org/10.5194/acp-21-731-2021, https://doi.org/10.5194/acp-21-731-2021, 2021
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This study investigates the impact of strongly increased atmospheric methane mixing ratios on the Earth's climate. An interactive model system including atmospheric dynamics, chemistry, and a mixed-layer ocean model is used to analyse the effect of doubled and quintupled methane mixing ratios. We assess feedbacks on atmospheric chemistry and changes in the stratospheric circulation, focusing on the impact of tropospheric warming, and their relevance for the model's climate sensitivity.
Markus Kilian, Sabine Brinkop, and Patrick Jöckel
Atmos. Chem. Phys., 20, 11697–11715, https://doi.org/10.5194/acp-20-11697-2020, https://doi.org/10.5194/acp-20-11697-2020, 2020
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After the volcanic eruption of Mt Pinatubo in 1991, ozone decreased in the tropics and increased in the midlatitudes and polar regions for 1 year. The change in the ozone column is solely a result of the volcanic heating, followed by an ozone decrease in the higher latitudes. This is caused by the volcanic aerosol, which changes the heterogeneous chemistry and thus the catalytic ozone loss cycles. Vertical transport of water vapour is enhanced by volcanic heating and increases methane.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
William T. Ball, Gabriel Chiodo, Marta Abalos, Justin Alsing, and Andrea Stenke
Atmos. Chem. Phys., 20, 9737–9752, https://doi.org/10.5194/acp-20-9737-2020, https://doi.org/10.5194/acp-20-9737-2020, 2020
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Recent lower stratospheric ozone decreases remain unexplained. We show that chemistry–climate models are not generally able to reproduce mid-latitude ozone and water vapour changes. Our analysis of observations provides evidence that climate change may be responsible for the ozone trends. While model projections suggest that extratropical ozone should recover by 2100, our study raises questions about their efficacy in simulating lower stratospheric changes in this region.
J. Eric Klobas, Debra K. Weisenstein, Ross J. Salawitch, and David M. Wilmouth
Atmos. Chem. Phys., 20, 9459–9471, https://doi.org/10.5194/acp-20-9459-2020, https://doi.org/10.5194/acp-20-9459-2020, 2020
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The rates of important ozone-destroying chemical reactions in the stratosphere are likely to change in the future. We employ a computer model to evaluate how the rates of ozone destruction by chlorine and bromine may evolve in four climate change scenarios with the introduction of the eta factor. We then show how these changing rates will impact the ozone-depleting power of the stratosphere with a new metric known as Equivalent Effective Stratospheric Benchmark-normalized Chlorine (EESBnC).
Yajuan Li, Martyn P. Chipperfield, Wuhu Feng, Sandip S. Dhomse, Richard J. Pope, Faquan Li, and Dong Guo
Atmos. Chem. Phys., 20, 8627–8639, https://doi.org/10.5194/acp-20-8627-2020, https://doi.org/10.5194/acp-20-8627-2020, 2020
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The Tibetan Plateau (TP) exerts important thermal and dynamical effects on atmospheric circulation, climate change as well as the ozone distribution. In this study, we use updated observations and model simulations to investigate the ozone trends and variations over the TP. Wintertime TP ozone variations are largely controlled by tropical to high-latitude transport processes, whereas summertime concentrations are a combined effect of photochemical decay and tropical processes.
Javier Alejandro Barrera, Rafael Pedro Fernandez, Fernando Iglesias-Suarez, Carlos Alberto Cuevas, Jean-Francois Lamarque, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 8083–8102, https://doi.org/10.5194/acp-20-8083-2020, https://doi.org/10.5194/acp-20-8083-2020, 2020
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The inclusion of biogenic very short-lived bromocarbons (VSLBr) in the CAM-chem model improves the model–satellite agreement of the total ozone columns at mid-latitudes and drives a persistent hemispheric asymmetry in lowermost stratospheric ozone loss. The seasonal VSLBr impact on mid-latitude lowermost stratospheric ozone is influenced by the heterogeneous reactivation processes of inorganic chlorine on ice crystals, with a clear increase in ozone destruction during spring and winter.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Hans Brenna, Steffen Kutterolf, Michael J. Mills, and Kirstin Krüger
Atmos. Chem. Phys., 20, 6521–6539, https://doi.org/10.5194/acp-20-6521-2020, https://doi.org/10.5194/acp-20-6521-2020, 2020
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The Los Chocoyos supereruption (84 000 years ago) in Guatemala was one of the largest volcanic events of the last 100 000 years. This eruption released enormous amounts of sulfur, which cooled the climate, as well as chlorine and bromine, which destroyed the ozone in the stratosphere. We have simulated this eruption by using an advanced chemistry–climate model. We found a collapse in the ozone layer lasting more than 10 years, increased surface–UV radiation, and a 30-year climate-cooling period.
Mikhail Sofiev, Rostislav Kouznetsov, Risto Hänninen, and Viktoria F. Sofieva
Atmos. Chem. Phys., 20, 1839–1847, https://doi.org/10.5194/acp-20-1839-2020, https://doi.org/10.5194/acp-20-1839-2020, 2020
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An episode of anomalously low ozone concentrations in the stratosphere over northern Europe occurred on 3–5 November 2018. The 30 % reduction of the ozone layer was predicted by the global chemistry-transport model of the Finnish Meteorological Institute driven by weather forecasts of ECMWF. The reduction was subsequently observed by ozone monitoring satellites. The episode was caused by a storm in the northern Atlantic, which uplifted air from the troposphere to stratosphere.
Martin Dameris, Patrick Jöckel, and Matthias Nützel
Atmos. Chem. Phys., 19, 13759–13771, https://doi.org/10.5194/acp-19-13759-2019, https://doi.org/10.5194/acp-19-13759-2019, 2019
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A chemistry–climate model (CCM) study is performed, investigating the consequences of a constant CFC-11 surface mixing ratio for stratospheric ozone in the future. The total column ozone is particularly affected in both polar regions in winter and spring. It turns out that the calculated ozone changes, especially in the upper stratosphere, are smaller than expected. In this attitudinal region the additional ozone depletion due to the catalysis by reactive chlorine is partly compensated for.
Quentin Errera, Simon Chabrillat, Yves Christophe, Jonas Debosscher, Daan Hubert, William Lahoz, Michelle L. Santee, Masato Shiotani, Sergey Skachko, Thomas von Clarmann, and Kaley Walker
Atmos. Chem. Phys., 19, 13647–13679, https://doi.org/10.5194/acp-19-13647-2019, https://doi.org/10.5194/acp-19-13647-2019, 2019
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BRAM2 is a 13-year reanalysis of the chemical composition from the upper troposphere to the lower mesosphere based on the assimilation of the Microwave Limb Sounder observations where eight species are assimilated: O3, H2O, N2O, HNO3, HCl, ClO, CH3Cl and CO. BRAM2 agrees generally well with independent observations in the middle stratosphere, the polar vortex and the upper troposphere–lower stratosphere but also shows several issues in the model and in the observations.
Ewa M. Bednarz, Amanda C. Maycock, Peter Braesicke, Paul J. Telford, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 9833–9846, https://doi.org/10.5194/acp-19-9833-2019, https://doi.org/10.5194/acp-19-9833-2019, 2019
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The atmospheric response to the amplitude of 11-year solar cycle in UM-UKCA is separated into the contributions from changes in direct radiative heating and photolysis rates, and the results compared with a control case with both effects included. We find that while the tropical responses are largely additive, this is not necessarily the case in the high latitudes. We suggest that solar-induced changes in ozone are important for modulating the SH dynamical response to the 11-year solar cycle.
Pavle Arsenovic, Alessandro Damiani, Eugene Rozanov, Bernd Funke, Andrea Stenke, and Thomas Peter
Atmos. Chem. Phys., 19, 9485–9494, https://doi.org/10.5194/acp-19-9485-2019, https://doi.org/10.5194/acp-19-9485-2019, 2019
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Low-energy electrons (LEE) are the dominant source of odd nitrogen, which destroys ozone, in the mesosphere and stratosphere in polar winter in the geomagnetically active periods. However, the observed stratospheric ozone anomalies can be reproduced only when accounting for both low- and middle-range energy electrons (MEE) in the chemistry-climate model. Ozone changes may induce further dynamical and thermal changes in the atmosphere. We recommend including both LEE and MEE in climate models.
Franziska Winterstein, Fabian Tanalski, Patrick Jöckel, Martin Dameris, and Michael Ponater
Atmos. Chem. Phys., 19, 7151–7163, https://doi.org/10.5194/acp-19-7151-2019, https://doi.org/10.5194/acp-19-7151-2019, 2019
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The atmospheric concentrations of the anthropogenic greenhouse gas methane are predicted to rise in the future. In this paper we investigate how very strong methane concentrations will impact the atmosphere. We analyse two experiments, one with doubled and one with quintupled methane concentrations and focus on the rapid atmospheric changes before the ocean adjusts to the induced
forcing. In particular these are changes in temperature, ozone, the hydroxyl radical and stratospheric water vapour.
Mengchu Tao, Paul Konopka, Felix Ploeger, Xiaolu Yan, Jonathon S. Wright, Mohamadou Diallo, Stephan Fueglistaler, and Martin Riese
Atmos. Chem. Phys., 19, 6509–6534, https://doi.org/10.5194/acp-19-6509-2019, https://doi.org/10.5194/acp-19-6509-2019, 2019
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This paper examines the annual and interannual variations as well as long-term trend of modeled stratospheric water vapor with a Lagrangian chemical transport model driven by ERA-I, MERRA-2 and JRA-55. We find reasonable consistency among the annual cycle, QBO and the variabilities induced by ENSO and volcanic aerosols. The main discrepancies are linked to the differences in reanalysis upwelling rates in the lower stratosphere. The trends are sensitive to the reanalyses that drives the model.
Felix Ploeger, Bernard Legras, Edward Charlesworth, Xiaolu Yan, Mohamadou Diallo, Paul Konopka, Thomas Birner, Mengchu Tao, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 19, 6085–6105, https://doi.org/10.5194/acp-19-6085-2019, https://doi.org/10.5194/acp-19-6085-2019, 2019
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We analyse the change in the circulation of the middle atmosphere based on current generation meteorological reanalysis data sets. We find that long-term changes from 1989 to 2015 are similar for the chosen reanalyses, mainly resembling the forced response in climate model simulations to climate change. For shorter periods circulation changes are less robust, and the representation of decadal variability appears to be a major uncertainty for modelling the circulation of the middle atmosphere.
Lucien Froidevaux, Douglas E. Kinnison, Ray Wang, John Anderson, and Ryan A. Fuller
Atmos. Chem. Phys., 19, 4783–4821, https://doi.org/10.5194/acp-19-4783-2019, https://doi.org/10.5194/acp-19-4783-2019, 2019
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This work evaluates two versions of a 3-D global model of upper-atmospheric composition for recent decades. The two versions differ mainly in their dynamical (wind) constraints. Model–data differences, variability, and trends in five gases (ozone, H2O, HCl, HNO3, and N2O) are compared. While the match between models and observations is impressive, a few areas of discrepancy are noted. This work also updates trends in composition based on recent satellite-based measurements (through 2018).
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Short summary
2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the stratospheric ozone layer from the harmful effects of synthetic ozone depleting substances. Since the late 1990s atmospheric concentrations of these species have begun to decline, and as a result ozone concentrations are expected to increase. In this study we use an ensemble of chemistry–climate simulations to investigate recent ozone trends and search for early signs of ozone recovery.
2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the...
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