Articles | Volume 18, issue 10
Atmos. Chem. Phys., 18, 7625–7637, 2018
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.
Atmos. Chem. Phys., 18, 7625–7637, 2018
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
On ozone trend detection: using coupled chemistry–climate simulations to investigate early signs of total column ozone recovery
James Keeble et al.
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Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-423, https://doi.org/10.5194/acp-2022-423, 2022
Preprint under review for ACP
Short summary
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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, Marijin Bauters, Pascal Boeckx, Alexander W. Cheesman, Makoto Deushi, Inês Dos Santos, Corinne Galy-Lacaux, James Haywood, James Keeble, Lina M. Mercado, Fiona M. O'Connor, Naga Oshima, Kostas Tsigaridis, and Hans Verbeeck
EGUsphere, https://doi.org/10.5194/egusphere-2022-218, https://doi.org/10.5194/egusphere-2022-218, 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.
Maria R. Russo, Brian J. Kerridge, Nathan L. Abraham, James Keeble, Barry G. Latter, Richard Siddans, James Weber, Paul T. Griffiths, John A. Pyle, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-99, https://doi.org/10.5194/acp-2022-99, 2022
Preprint under review for ACP
Short summary
Short summary
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.
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
Short summary
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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.
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.
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.
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
Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-423, https://doi.org/10.5194/acp-2022-423, 2022
Preprint under review for ACP
Short summary
Short summary
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, Marijin Bauters, Pascal Boeckx, Alexander W. Cheesman, Makoto Deushi, Inês Dos Santos, Corinne Galy-Lacaux, James Haywood, James Keeble, Lina M. Mercado, Fiona M. O'Connor, Naga Oshima, Kostas Tsigaridis, and Hans Verbeeck
EGUsphere, https://doi.org/10.5194/egusphere-2022-218, https://doi.org/10.5194/egusphere-2022-218, 2022
Short summary
Short summary
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.
Maria R. Russo, Brian J. Kerridge, Nathan L. Abraham, James Keeble, Barry G. Latter, Richard Siddans, James Weber, Paul T. Griffiths, John A. Pyle, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-99, https://doi.org/10.5194/acp-2022-99, 2022
Preprint under review for ACP
Short summary
Short summary
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.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-34, https://doi.org/10.5194/acp-2022-34, 2022
Revised manuscript accepted for ACP
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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 setup with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running setup. 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
Short summary
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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 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 | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)
The influence of energetic particle precipitation on Antarctic stratospheric chlorine and ozone over the 20th century
Effects of Reanalysis Forcing Fields on Ozone Trends from a Chemical Transport Model
Atmospheric impacts of chlorinated very short-lived substances over the recent past. Part 1: the role of transport
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
Chlorine nitrate in the atmosphere
Linking uncertainty in simulated Arctic ozone loss to uncertainties in modelled tropical stratospheric water vapour
Importance of seasonally resolved oceanic emissions for bromoform delivery from the tropical Indian Ocean and west Pacific to the stratosphere
The representation of solar cycle signals in stratospheric ozone – Part 2: Analysis of global models
Investigating the yield of H2O and H2 from methane oxidation in the stratosphere
Comparison of ECHAM5/MESSy Atmospheric Chemistry (EMAC) simulations of the Arctic winter 2009/2010 and 2010/2011 with Envisat/MIPAS and Aura/MLS observations
On the discrepancy of HCl processing in the core of the wintertime polar vortices
Estimates of ozone return dates from Chemistry-Climate Model Initiative simulations
Trend differences in lower stratospheric water vapour between Boulder and the zonal mean and their role in understanding fundamental observational discrepancies
Future changes in the stratosphere-to-troposphere ozone mass flux and the contribution from climate change and ozone recovery
The maintenance of elevated active chlorine levels in the Antarctic lower stratosphere through HCl null cycles
Chemical and climatic drivers of radiative forcing due to changes in stratospheric and tropospheric ozone over the 21st century
Ozone sensitivity to varying greenhouse gases and ozone-depleting substances in CCMI-1 simulations
Diagnosing the radiative and chemical contributions to future changes in tropical column ozone with the UM-UKCA chemistry–climate model
Denitrification, dehydration and ozone loss during the 2015/2016 Arctic winter
Assessment of upper tropospheric and stratospheric water vapor and ozone in reanalyses as part of S-RIP
A quantitative analysis of the reactions involved in stratospheric ozone depletion in the polar vortex core
An assessment of ozone mini-hole representation in reanalyses over the Northern Hemisphere
Impact of biogenic very short-lived bromine on the Antarctic ozone hole during the 21st century
Influence of enhanced Asian NOx emissions on ozone in the upper troposphere and lower stratosphere in chemistry–climate model simulations
Determination of the atmospheric lifetime and global warming potential of sulfur hexafluoride using a three-dimensional model
Antarctic ozone depletion between 1960 and 1980 in observations and chemistry–climate model simulations
Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
The role of methane in projections of 21st century stratospheric water vapour
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.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-182, https://doi.org/10.5194/acp-2022-182, 2022
Preprint under review for ACP
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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.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-34, https://doi.org/10.5194/acp-2022-34, 2022
Revised manuscript accepted for ACP
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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 setup with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running setup. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
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).
Thomas von Clarmann and Sören Johansson
Atmos. Chem. Phys., 18, 15363–15386, https://doi.org/10.5194/acp-18-15363-2018, https://doi.org/10.5194/acp-18-15363-2018, 2018
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This review article compiles the characteristics of the gas chlorine nitrate and discusses its role in atmospheric chemistry. Chlorine nitrate is a reservoir of both stratospheric chlorine and nitrogen. Formation and sink processes are discussed, as well as spectral features and spectroscopic studies. Remote sensing, fluorescence, and mass spectroscopic measurement techniques are introduced, and global distributions and the annual cycle are discussed in the context of chlorine de-/activation.
Laura Thölix, Alexey Karpechko, Leif Backman, and Rigel Kivi
Atmos. Chem. Phys., 18, 15047–15067, https://doi.org/10.5194/acp-18-15047-2018, https://doi.org/10.5194/acp-18-15047-2018, 2018
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We analyse the impact of water vapour (WV) on Arctic ozone loss and find the strongest impact during intermediately cold stratospheric winters when chlorine activation increases with increasing PSCs and WV. In colder winters the impact is limited because chlorine activation becomes complete at relatively low WV values, so further addition of WV does not affect ozone loss. Our results imply that improved simulations of WV are needed for more reliable projections of ozone layer recovery.
Alina Fiehn, Birgit Quack, Irene Stemmler, Franziska Ziska, and Kirstin Krüger
Atmos. Chem. Phys., 18, 11973–11990, https://doi.org/10.5194/acp-18-11973-2018, https://doi.org/10.5194/acp-18-11973-2018, 2018
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Oceanic very short-lived substances, VSLS, contribute to stratospheric halogen loading and ozone depletion. We created bromoform emission inventories with monthly resolution for the tropical Indian Ocean and west Pacific and modeled the atmospheric transport of bromoform with the particle dispersion model FLEXPART/ERA-Interim. Results underline that the seasonal and regional stratospheric bromine entrainment critically depends on the seasonality and spatial distribution of the VSLS emissions.
Amanda C. Maycock, Katja Matthes, Susann Tegtmeier, Hauke Schmidt, Rémi Thiéblemont, Lon Hood, Hideharu Akiyoshi, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Oliver Kirner, Markus Kunze, Marion Marchand, Daniel R. Marsh, Martine Michou, David Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Yousuke Yamashita, and Kohei Yoshida
Atmos. Chem. Phys., 18, 11323–11343, https://doi.org/10.5194/acp-18-11323-2018, https://doi.org/10.5194/acp-18-11323-2018, 2018
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The 11-year solar cycle is an important driver of climate variability. Changes in incoming solar ultraviolet radiation affect atmospheric ozone, which in turn influences atmospheric temperatures. Constraining the impact of the solar cycle on ozone is therefore important for understanding climate variability. This study examines the representation of the solar influence on ozone in numerical models used to simulate past and future climate. We highlight important differences among model datasets.
Franziska Frank, Patrick Jöckel, Sergey Gromov, and Martin Dameris
Atmos. Chem. Phys., 18, 9955–9973, https://doi.org/10.5194/acp-18-9955-2018, https://doi.org/10.5194/acp-18-9955-2018, 2018
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It is frequently assumed that one methane molecule produces two water molecules. Applying various modeling concepts, we find that the yield of water from methane is vertically not constantly 2. In the upper stratosphere and lower mesosphere, transport of intermediate H2 molecules even led to a yield greater than 2. We conclude that for a realistic chemical source of stratospheric water vapor, one must also take other sources (H2), intermediates and the chemical removal of water into account.
Farahnaz Khosrawi, Oliver Kirner, Gabriele Stiller, Michael Höpfner, Michelle L. Santee, Sylvia Kellmann, and Peter Braesicke
Atmos. Chem. Phys., 18, 8873–8892, https://doi.org/10.5194/acp-18-8873-2018, https://doi.org/10.5194/acp-18-8873-2018, 2018
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An extensive assessment of the performance of the chemistry–climate model EMAC is given for Arctic winters 2009/2010 and 2010/2011. The EMAC simulations are compared to satellite observations. The comparisons between EMAC simulations and satellite observations show that model and measurements compare well for these two Arctic winters. However, differences between model and observations are found that need improvements in the model in the future.
Jens-Uwe Grooß, Rolf Müller, Reinhold Spang, Ines Tritscher, Tobias Wegner, Martyn P. Chipperfield, Wuhu Feng, Douglas E. Kinnison, and Sasha Madronich
Atmos. Chem. Phys., 18, 8647–8666, https://doi.org/10.5194/acp-18-8647-2018, https://doi.org/10.5194/acp-18-8647-2018, 2018
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We investigate a discrepancy between model simulations and observations of HCl in the dark polar stratosphere. In early winter, the less-well-studied period of the onset of chlorine activation, observations show a much faster depletion of HCl than simulations of three models. This points to some unknown process that is currently not represented in the models. Various hypotheses for potential causes are investigated that partly reduce the discrepancy. The impact on polar ozone depletion is low.
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.
Stefan Lossow, Dale F. Hurst, Karen H. Rosenlof, Gabriele P. Stiller, Thomas von Clarmann, Sabine Brinkop, Martin Dameris, Patrick Jöckel, Doug E. Kinnison, Johannes Plieninger, David A. Plummer, Felix Ploeger, William G. Read, Ellis E. Remsberg, James M. Russell, and Mengchu Tao
Atmos. Chem. Phys., 18, 8331–8351, https://doi.org/10.5194/acp-18-8331-2018, https://doi.org/10.5194/acp-18-8331-2018, 2018
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Trend estimates of lower stratospheric H2O derived from the FPH observations at Boulder and a merged zonal mean satellite data set clearly differ for the time period from the late 1980s to 2010. We investigate if a sampling bias between Boulder and the zonal mean around the Boulder latitude can explain these trend discrepancies. Typically they are small and not sufficient to explain the trend discrepancies in the observational database.
Stefanie Meul, Ulrike Langematz, Philipp Kröger, Sophie Oberländer-Hayn, and Patrick Jöckel
Atmos. Chem. Phys., 18, 7721–7738, https://doi.org/10.5194/acp-18-7721-2018, https://doi.org/10.5194/acp-18-7721-2018, 2018
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Using a chemistry--climate model future changes in the stratosphere-to-troposphere ozone mass flux, their drivers, and the future distribution of stratospheric ozone in the troposphere are investigated. In an extreme greenhouse gas (GHG) scenario, the global influx of stratospheric ozone into the troposphere is projected to grow between 2000 and 2100 by 53%. The increase is due to the recovery of stratospheric ozone owing to declining halogens and GHG induced circulation and temperature changes.
Rolf Müller, Jens-Uwe Grooß, Abdul Mannan Zafar, Sabine Robrecht, and Ralph Lehmann
Atmos. Chem. Phys., 18, 2985–2997, https://doi.org/10.5194/acp-18-2985-2018, https://doi.org/10.5194/acp-18-2985-2018, 2018
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This paper revisits the chemistry leading to strong ozone depletion in the Antarctic. We focus on the heart of the ozone layer in the lowermost stratosphere in the core of the vortex. We argue that chemical cycles (referred to as HCl null cycles) that have hitherto been largely neglected counteract the deactivation of chlorine and are therefore key to ozone depletion in the core of the Antarctic vortex. The key process to full activation of chlorine is the photolysis of formaldehyde.
Antara Banerjee, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 18, 2899–2911, https://doi.org/10.5194/acp-18-2899-2018, https://doi.org/10.5194/acp-18-2899-2018, 2018
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This study quantifies the radiative forcing (RF) of future ozone changes. Under climate change, even the sign of the ozone RF can change depending on the greenhouse gas emissions scenario followed. Stratosphere–troposphere exchange plays an important role in driving ozone RF due to reductions in ozone-depleting substances (ODSs) and increases in methane abundance. These could negate the ozone-derived climate benefits of air-quality controls on non-methane ozone precursor emissions.
Olaf Morgenstern, Kane A. Stone, Robyn Schofield, Hideharu Akiyoshi, Yousuke Yamashita, Douglas E. Kinnison, Rolando R. Garcia, Kengo Sudo, David A. Plummer, John Scinocca, Luke D. Oman, Michael E. Manyin, Guang Zeng, Eugene Rozanov, Andrea Stenke, Laura E. Revell, Giovanni Pitari, Eva Mancini, Glauco Di Genova, Daniele Visioni, Sandip S. Dhomse, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 1091–1114, https://doi.org/10.5194/acp-18-1091-2018, https://doi.org/10.5194/acp-18-1091-2018, 2018
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We assess how ozone as simulated by a group of chemistry–climate models responds to variations in man-made climate gases and ozone-depleting substances. We find some agreement, particularly in the middle and upper stratosphere, but also considerable disagreement elsewhere. Such disagreement affects the reliability of future ozone projections based on these models, and also constitutes a source of uncertainty in climate projections using prescribed ozone derived from these simulations.
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.
Farahnaz Khosrawi, Oliver Kirner, Björn-Martin Sinnhuber, Sören Johansson, Michael Höpfner, Michelle L. Santee, Lucien Froidevaux, Jörn Ungermann, Roland Ruhnke, Wolfgang Woiwode, Hermann Oelhaf, and Peter Braesicke
Atmos. Chem. Phys., 17, 12893–12910, https://doi.org/10.5194/acp-17-12893-2017, https://doi.org/10.5194/acp-17-12893-2017, 2017
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The 2015/2016 Arctic winter was one of the coldest winters in recent years, allowing extensive PSC formation and chlorine activation. Model simulations of the 2015/2016 Arctic winter were performed with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). We find that ozone loss was quite strong but not as strong as in 2010/2011; denitrification and dehydration were so far the strongest observed in the Arctic stratosphere in at least the past 10 years.
Sean M. Davis, Michaela I. Hegglin, Masatomo Fujiwara, Rossana Dragani, Yayoi Harada, Chiaki Kobayashi, Craig Long, Gloria L. Manney, Eric R. Nash, Gerald L. Potter, Susann Tegtmeier, Tao Wang, Krzysztof Wargan, and Jonathon S. Wright
Atmos. Chem. Phys., 17, 12743–12778, https://doi.org/10.5194/acp-17-12743-2017, https://doi.org/10.5194/acp-17-12743-2017, 2017
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Ozone and water vapor in the stratosphere are important gases that affect surface climate and absorb incoming solar ultraviolet radiation. These gases are represented in reanalyses, which create a complete picture of the state of Earth's atmosphere using limited observations. We evaluate reanalysis water vapor and ozone fidelity by intercomparing them, and comparing them to independent observations. Generally reanalyses do a good job at representing ozone, but have problems with water vapor.
Ingo Wohltmann, Ralph Lehmann, and Markus Rex
Atmos. Chem. Phys., 17, 10535–10563, https://doi.org/10.5194/acp-17-10535-2017, https://doi.org/10.5194/acp-17-10535-2017, 2017
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We present a quantitative analysis of the chemical reactions involved in polar ozone depletion in the stratosphere, and of the relevant reaction pathways and cycles. We show time series of reaction rates averaged over the core of the polar vortex in winter and spring for all relevant reactions. An emphasis is put on the partitioning of the relevant chemical families (nitrogen, hydrogen, chlorine, bromine and odd oxygen) and activation and deactivation of chlorine.
Luis F. Millán and Gloria L. Manney
Atmos. Chem. Phys., 17, 9277–9289, https://doi.org/10.5194/acp-17-9277-2017, https://doi.org/10.5194/acp-17-9277-2017, 2017
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An ozone mini-hole is a synoptic-scale region with strongly decreased total column ozone resulting from dynamical processes. Using total column measurements from the Ozone Monitoring Instrument and ozone profile measurements from the Microwave Limb Sounder, we evaluate the accuracy of mini-hole representation in five reanalyses.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688, https://doi.org/10.5194/acp-17-1673-2017, https://doi.org/10.5194/acp-17-1673-2017, 2017
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The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Chaitri Roy, Suvarna Fadnavis, Rolf Müller, D. C. Ayantika, Felix Ploeger, and Alexandru Rap
Atmos. Chem. Phys., 17, 1297–1311, https://doi.org/10.5194/acp-17-1297-2017, https://doi.org/10.5194/acp-17-1297-2017, 2017
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In the monsoon season, Asian NOx emissions are rapidly transported to the UTLS and can impact ozone in the UTLS. From chemistry–climate model simulations, we show that increasing Asian NOx emissions have enhanced ozone radiative forcing over Southeast Asia, which leads to significant warming over the Tibetan Plateau and increase precipitation over India. However, a further increase in NOx emissions elicited negative precipitation due to reversal of monsoon Hadley circulation.
Tamás Kovács, Wuhu Feng, Anna Totterdill, John M. C. Plane, Sandip Dhomse, Juan Carlos Gómez-Martín, Gabriele P. Stiller, Florian J. Haenel, Christopher Smith, Piers M. Forster, Rolando R. García, Daniel R. Marsh, and Martyn P. Chipperfield
Atmos. Chem. Phys., 17, 883–898, https://doi.org/10.5194/acp-17-883-2017, https://doi.org/10.5194/acp-17-883-2017, 2017
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Sulfur hexafluoride (SF6) is a very potent greenhouse gas, which is present in the atmosphere only through its industrial use, for example as an electrical insulator. To estimate accurately the impact of SF6 emissions on climate we need to know how long it persists in the atmosphere before being removed. Previous estimates of the SF6 lifetime indicate a large degree of uncertainty. Here we use a detailed atmospheric model to calculate a current best estimate of the SF6 lifetime.
Ulrike Langematz, Franziska Schmidt, Markus Kunze, Gregory E. Bodeker, and Peter Braesicke
Atmos. Chem. Phys., 16, 15619–15627, https://doi.org/10.5194/acp-16-15619-2016, https://doi.org/10.5194/acp-16-15619-2016, 2016
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The extent of anthropogenically driven Antarctic ozone depletion prior to 1980 is examined using transient chemistry–climate model simulations from 1960 to 2000 with prescribed changes of ozone depleting substances in conjunction with observations. All models show a long-term, halogen-induced negative trend in Antarctic ozone from 1960 to 1980, ranging between 26 and 50 % of the total anthropogenic ozone depletion from 1960 to 2000. A stronger ozone decline of 56 % was estimated from observation.
Katherine M. Saad, Debra Wunch, Nicholas M. Deutscher, David W. T. Griffith, Frank Hase, Martine De Mazière, Justus Notholt, David F. Pollard, Coleen M. Roehl, Matthias Schneider, Ralf Sussmann, Thorsten Warneke, and Paul O. Wennberg
Atmos. Chem. Phys., 16, 14003–14024, https://doi.org/10.5194/acp-16-14003-2016, https://doi.org/10.5194/acp-16-14003-2016, 2016
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Current approaches to constrain the global methane budget assimilate total column measurements into models, but model biases can impact results. We use tropospheric methane columns to evaluate model transport errors and identify a seasonal time lag in the Northern Hemisphere troposphere masked by stratospheric compensating effects. We find systematic biases in the stratosphere will alias into model-derived emissions estimates, especially those in the high Northern latitudes that vary seasonally.
Laura E. Revell, Andrea Stenke, Eugene Rozanov, William Ball, Stefan Lossow, and Thomas Peter
Atmos. Chem. Phys., 16, 13067–13080, https://doi.org/10.5194/acp-16-13067-2016, https://doi.org/10.5194/acp-16-13067-2016, 2016
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Water vapour in the stratosphere plays an important role in atmospheric chemistry and the Earth's radiative balance. We have analysed trends in stratospheric water vapour through the 21st century as simulated by a coupled chemistry–climate model following a range of greenhouse gas emission scenarios. We have also quantified the contribution that methane oxidation in the stratosphere makes to projected water vapour trends.
Cited articles
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Avallone, L. M. and Prather, M. J.: Photochemical evolution of ozone in the lower tropical stratosphere, J. Geophys. Res., 101, 1457–1461, https://doi.org/10.1029/95JD03010, 1996.
Baldwin, M. P., Gray, L. J., Dunkerton, T. J., Hamilton, K., Haynes, P. H., Randel, W. J., Holton, J. R., Alexander, M. J., Hirota, I., Horinouchi, T., Jones, D. B. A., Kinnersley, J. S., Marquardt, C., Sato, K., and Takahashi, M.: The quasi–biennial oscillation, Rev. Geophys., 39, 179–229, 2001.
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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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