Articles | Volume 23, issue 21
https://doi.org/10.5194/acp-23-13701-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-23-13701-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
03 Nov 2023
Research article |
| 03 Nov 2023
| 03 Nov 2023
Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 2: Impacts on ozone
Lancaster Environment Centre, Lancaster University, Lancaster, UK
Cooperative Institute for Research in Environmental Science (CIRES), University of Colorado Boulder, Boulder, CO, USA
NOAA Chemical Sciences Laboratory (NOAA CSL), Boulder, CO, USA
Ryan Hossaini
Lancaster Environment Centre, Lancaster University, Lancaster, UK
Centre of Excellence in Environmental Data Science (CEEDS), Lancaster University, Lancaster, UK
Martyn P. Chipperfield
School of Earth and Environment, University of Leeds, Leeds, UK
National Centre for Earth Observation (NCEO), University of Leeds, Leeds, UK
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Yan Zhang, Douglas G. MacMartin, Daniele Visioni, Ewa M. Bednarz, and Ben Kravitz
Earth Syst. Dynam., 15, 191–213, https://doi.org/10.5194/esd-15-191-2024, https://doi.org/10.5194/esd-15-191-2024, 2024
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Injecting SO2 into the lower stratosphere can temporarily reduce global mean temperature and mitigate some risks associated with climate change, but injecting it at different latitudes and seasons would have different impacts. This study introduces new stratospheric aerosol injection (SAI) strategies and explores the importance of the choice of SAI strategy, demonstrating that it notably affects the distribution of aerosol cloud, injection efficiency, and various surface climate impacts.
Ewa M. Bednarz, Amy H. Butler, Daniele Visioni, Yan Zhang, Ben Kravitz, and Douglas G. MacMartin
Atmos. Chem. Phys., 23, 13665–13684, https://doi.org/10.5194/acp-23-13665-2023, https://doi.org/10.5194/acp-23-13665-2023, 2023
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We use a state-of-the-art Earth system model and a set of stratospheric aerosol injection (SAI) strategies to achieve the same level of global mean surface cooling through different combinations of location and/or timing of the injection. We demonstrate that the choice of SAI strategy can lead to contrasting impacts on stratospheric and tropospheric temperatures, circulation, and chemistry (including stratospheric ozone), thereby leading to different impacts on regional surface climate.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Matthew Henry, Jim Haywood, Andy Jones, Mohit Dalvi, Alice Wells, Daniele Visioni, Ewa M. Bednarz, Douglas G. MacMartin, Walker Lee, and Mari R. Tye
Atmos. Chem. Phys., 23, 13369–13385, https://doi.org/10.5194/acp-23-13369-2023, https://doi.org/10.5194/acp-23-13369-2023, 2023
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Solar climate interventions, such as injecting sulfur in the stratosphere, may be used to offset some of the adverse impacts of global warming. We use two independently developed Earth system models to assess the uncertainties around stratospheric sulfur injections. The injection locations and amounts are optimized to maintain the same pattern of surface temperature. While both models show reduced warming, the change in rainfall patterns (even without sulfur injections) is uncertain.
Daniele Visioni, Ewa M. Bednarz, Walker R. Lee, Ben Kravitz, Andy Jones, Jim M. Haywood, and Douglas G. MacMartin
Atmos. Chem. Phys., 23, 663–685, https://doi.org/10.5194/acp-23-663-2023, https://doi.org/10.5194/acp-23-663-2023, 2023
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The paper constitutes Part 1 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric sulfate aerosol injections (SAIs) at various latitudes as simulated by three state-of-the-art Earth system models. We identify similarities and differences in the modeled aerosol burden, investigate the differences in the aerosol approaches between the models, and ultimately show the differences produced in surface climate, temperature and precipitation.
Ewa M. Bednarz, Daniele Visioni, Ben Kravitz, Andy Jones, James M. Haywood, Jadwiga Richter, Douglas G. MacMartin, and Peter Braesicke
Atmos. Chem. Phys., 23, 687–709, https://doi.org/10.5194/acp-23-687-2023, https://doi.org/10.5194/acp-23-687-2023, 2023
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Building on Part 1 of this two-part study, we demonstrate the role of biases in climatological circulation and specific aspects of model microphysics in driving the differences in simulated sulfate distributions amongst three Earth system models. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface responses discussed in Part 1.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Simone Tilmes, Daniele Visioni, Andy Jones, James Haywood, Roland Séférian, Pierre Nabat, Olivier Boucher, Ewa Monica Bednarz, and Ulrike Niemeier
Atmos. Chem. Phys., 22, 4557–4579, https://doi.org/10.5194/acp-22-4557-2022, https://doi.org/10.5194/acp-22-4557-2022, 2022
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This study assesses the impacts of climate interventions, using stratospheric sulfate aerosol and solar dimming on stratospheric ozone, based on three Earth system models with interactive stratospheric chemistry. The climate interventions have been applied to a high emission (baseline) scenario in order to reach global surface temperatures of a medium emission scenario. We find significant increases and decreases in total column ozone, depending on regions and seasons.
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.
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.
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
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Richard J. Pope, Alexandru Rap, Matilda A. Pimlott, Brice Barret, Eric Le Flochmoen, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Anne Boynard, Christian Retscher, Wuhu Feng, Richard Rigby, Sandip S. Dhomse, Catherine Wespes, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 3613–3626, https://doi.org/10.5194/acp-24-3613-2024, https://doi.org/10.5194/acp-24-3613-2024, 2024
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Tropospheric ozone is an important short-lived climate forcer which influences the incoming solar short-wave radiation and the outgoing long-wave radiation in the atmosphere (8–15 km) where the balance between the two yields a net positive (i.e. warming) effect at the surface. Overall, we find that the tropospheric ozone radiative effect ranges between 1.21 and 1.26 W m−2 with a negligible trend (2008–2017), suggesting that tropospheric ozone influences on climate have remained stable with time.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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Yan Zhang, Douglas G. MacMartin, Daniele Visioni, Ewa M. Bednarz, and Ben Kravitz
Earth Syst. Dynam., 15, 191–213, https://doi.org/10.5194/esd-15-191-2024, https://doi.org/10.5194/esd-15-191-2024, 2024
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Injecting SO2 into the lower stratosphere can temporarily reduce global mean temperature and mitigate some risks associated with climate change, but injecting it at different latitudes and seasons would have different impacts. This study introduces new stratospheric aerosol injection (SAI) strategies and explores the importance of the choice of SAI strategy, demonstrating that it notably affects the distribution of aerosol cloud, injection efficiency, and various surface climate impacts.
Lily Gouldsbrough, Ryan Hossaini, Emma Eastoe, Paul J. Young, and Massimo Vieno
Atmos. Chem. Phys., 24, 3163–3196, https://doi.org/10.5194/acp-24-3163-2024, https://doi.org/10.5194/acp-24-3163-2024, 2024
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High-resolution spatial fields of surface ozone are used to understand spikes in ozone concentration and predict their impact on public health. Such fields are routinely output from complex mathematical models for atmospheric conditions. These outputs are on a coarse spatial resolution and the highest concentrations tend to be biased. Using a novel data-driven machine learning methodology, we show how such output can be corrected to produce fields with both lower bias and higher resolution.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn Chipperfield, Wuhu Feng, David Oram, Karina Adcock, Stephen Montzka, Isobel Simpson, Andrea Mazzeo, Amber Leeson, Elliot Atlas, and Charles C.-K. Chou
EGUsphere, https://doi.org/10.5194/egusphere-2024-560, https://doi.org/10.5194/egusphere-2024-560, 2024
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Ethylene dichloride (EDC) is an industrial chemical used to produce polyvinyl chloride (PVC). We analysed EDC production data to estimate global EDC emissions (2002 to 2020). The emissions were included in an atmospheric model and evaluated by comparing simulated EDC to EDC measurements in the troposphere. We show EDC contributes ozone-depleting chlorine to the stratosphere and this has increased with increasing EDC emissions. EDC’s impact on stratospheric ozone is currently small, but non-zero.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Ailish M. Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matilda Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
Atmos. Chem. Phys., 24, 789–806, https://doi.org/10.5194/acp-24-789-2024, https://doi.org/10.5194/acp-24-789-2024, 2024
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Our paper uses novel satellite datasets and high-resolution emissions datasets alongside a back-trajectory model to investigate the balance of local and external sources influencing NOx air pollution changes in Delhi. We find in the post-monsoon season that NOx from local and non-local transport emissions contributes most to poor air quality in Delhi. Therefore, air quality mitigation strategies in Delhi and surrounding regions are used to control this issue.
Richard J. Pope, Fiona M. O'Connor, Mohit Dalvi, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Brice Barret, Eric Le Flochmoen, Anne Boynard, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, Catherine Wespes, and Richard Rigby
EGUsphere, https://doi.org/10.5194/egusphere-2023-3109, https://doi.org/10.5194/egusphere-2023-3109, 2024
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Ozone is a potent air pollutant in the lower troposphere with adverse impacts on human health. Satellite records of tropospheric ozone currently show large-scale inconsistencies in their long-term trends. Our detailed study of the potential factors (e.g. satellite errors, where the satellite can observe ozone) potentially driving these inconsistencies found that in North America, Europe and East Asia, the underlying trends are typically small with large uncertainties.
Andrea Pazmiño, Florence Goutail, Sophie Godin-Beekmann, Alain Hauchecorne, Jean-Pierre Pommereau, Martyn P. Chipperfield, Wuhu Feng, Franck Lefèvre, Audrey Lecouffe, Michel Van Roozendael, Nis Jepsen, Georg Hansen, Rigel Kivi, Kimberly Strong, and Kaley A. Walker
Atmos. Chem. Phys., 23, 15655–15670, https://doi.org/10.5194/acp-23-15655-2023, https://doi.org/10.5194/acp-23-15655-2023, 2023
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The vortex-averaged ozone loss over the last 3 decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from the SAOZ network and MSR2 reanalysis. Three metrics were developed to compute ozone trends since 2000. The study confirms the ozone recovery in the Antarctic and shows a potential sign of quantitative detection of ozone recovery in the Arctic that needs to be robustly confirmed in the future.
Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, and Richard Rigby
Atmos. Chem. Phys., 23, 14933–14947, https://doi.org/10.5194/acp-23-14933-2023, https://doi.org/10.5194/acp-23-14933-2023, 2023
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Ozone is a potent air pollutant, and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTCO3) from space. We have constructed a merged LTCO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTCO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small-scale differences.
Sandip S. Dhomse and Martyn P. Chipperfield
Earth Syst. Sci. Data, 15, 5105–5120, https://doi.org/10.5194/essd-15-5105-2023, https://doi.org/10.5194/essd-15-5105-2023, 2023
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There are no long-term stratospheric profile data sets for two very important greenhouse gases: methane (CH4) and nitrous oxide (N2O). Along with radiative feedback, these species play an important role in controlling ozone loss in the stratosphere. Here, we use machine learning to fuse satellite measurements with a chemical model to construct long-term gap-free profile data sets for CH4 and N2O. We aim to construct similar data sets for other important trace gases (e.g. O3, Cly, NOy species).
Chris Wilson, Brian J. Kerridge, Richard Siddans, David P. Moore, Lucy J. Ventress, Emily Dowd, Wuhu Feng, Martyn P. Chipperfield, and John J. Remedios
EGUsphere, https://doi.org/10.5194/egusphere-2023-1652, https://doi.org/10.5194/egusphere-2023-1652, 2023
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The leaks from the Nord Stream gas pipelines in September 2022 released a large amount of methane (CH4) to the atmosphere. We provide observational data from a satellite instrument, IASI, that shows a large CH4 plume over the North Sea off the coast of Scandinavia. We use this, together with atmospheric models, to quantify the CH4 leaked into the atmosphere from the pipelines. We find that 215–390 Gg CH4 was emitted, making this the largest individual fossil fuel-related CH4 leak on record.
Ewa M. Bednarz, Amy H. Butler, Daniele Visioni, Yan Zhang, Ben Kravitz, and Douglas G. MacMartin
Atmos. Chem. Phys., 23, 13665–13684, https://doi.org/10.5194/acp-23-13665-2023, https://doi.org/10.5194/acp-23-13665-2023, 2023
Short summary
Short summary
We use a state-of-the-art Earth system model and a set of stratospheric aerosol injection (SAI) strategies to achieve the same level of global mean surface cooling through different combinations of location and/or timing of the injection. We demonstrate that the choice of SAI strategy can lead to contrasting impacts on stratospheric and tropospheric temperatures, circulation, and chemistry (including stratospheric ozone), thereby leading to different impacts on regional surface climate.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
Short summary
Short summary
Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Matthew Henry, Jim Haywood, Andy Jones, Mohit Dalvi, Alice Wells, Daniele Visioni, Ewa M. Bednarz, Douglas G. MacMartin, Walker Lee, and Mari R. Tye
Atmos. Chem. Phys., 23, 13369–13385, https://doi.org/10.5194/acp-23-13369-2023, https://doi.org/10.5194/acp-23-13369-2023, 2023
Short summary
Short summary
Solar climate interventions, such as injecting sulfur in the stratosphere, may be used to offset some of the adverse impacts of global warming. We use two independently developed Earth system models to assess the uncertainties around stratospheric sulfur injections. The injection locations and amounts are optimized to maintain the same pattern of surface temperature. While both models show reduced warming, the change in rainfall patterns (even without sulfur injections) is uncertain.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys., 23, 13235–13253, https://doi.org/10.5194/acp-23-13235-2023, https://doi.org/10.5194/acp-23-13235-2023, 2023
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Yang Li, Wuhu Feng, Xin Zhou, Yajuan Li, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2023-1452, https://doi.org/10.5194/egusphere-2023-1452, 2023
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Tibetan Plateau (TP), the highest and largest plateau, experiences strong surface solar UV radiation, whose excess can cause harmful influences on the local biota. Hence, it is critical to study TP ozone. We find ENSO, the strongest interannual phenomenon, can induce tropospheric temperature change and thus cause tropopause movement, which in turn leads to ozone change. Our understanding implies that future more strong ENSO events will play a key role in ozone recovery and ecosystems of the TP.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Peter Joyce, Cristina Ruiz Villena, Yahui Huang, Alex Webb, Manuel Gloor, Fabien H. Wagner, Martyn P. Chipperfield, Rocío Barrio Guilló, Chris Wilson, and Hartmut Boesch
Atmos. Meas. Tech., 16, 2627–2640, https://doi.org/10.5194/amt-16-2627-2023, https://doi.org/10.5194/amt-16-2627-2023, 2023
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Methane emissions are responsible for a lot of the warming caused by the greenhouse effect, much of which comes from a small number of point sources. We can identify methane point sources by analysing satellite data, but it requires a lot of time invested by experts and is prone to very high errors. Here, we produce a neural network that can automatically identify methane point sources and estimate the mass of methane that is being released per hour and are able to do so with far smaller errors.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Daniele Visioni, Ewa M. Bednarz, Walker R. Lee, Ben Kravitz, Andy Jones, Jim M. Haywood, and Douglas G. MacMartin
Atmos. Chem. Phys., 23, 663–685, https://doi.org/10.5194/acp-23-663-2023, https://doi.org/10.5194/acp-23-663-2023, 2023
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The paper constitutes Part 1 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric sulfate aerosol injections (SAIs) at various latitudes as simulated by three state-of-the-art Earth system models. We identify similarities and differences in the modeled aerosol burden, investigate the differences in the aerosol approaches between the models, and ultimately show the differences produced in surface climate, temperature and precipitation.
Ewa M. Bednarz, Daniele Visioni, Ben Kravitz, Andy Jones, James M. Haywood, Jadwiga Richter, Douglas G. MacMartin, and Peter Braesicke
Atmos. Chem. Phys., 23, 687–709, https://doi.org/10.5194/acp-23-687-2023, https://doi.org/10.5194/acp-23-687-2023, 2023
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Building on Part 1 of this two-part study, we demonstrate the role of biases in climatological circulation and specific aspects of model microphysics in driving the differences in simulated sulfate distributions amongst three Earth system models. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface responses discussed in Part 1.
Robert J. Parker, Chris Wilson, Edward Comyn-Platt, Garry Hayman, Toby R. Marthews, A. Anthony Bloom, Mark F. Lunt, Nicola Gedney, Simon J. Dadson, Joe McNorton, Neil Humpage, Hartmut Boesch, Martyn P. Chipperfield, Paul I. Palmer, and Dai Yamazaki
Biogeosciences, 19, 5779–5805, https://doi.org/10.5194/bg-19-5779-2022, https://doi.org/10.5194/bg-19-5779-2022, 2022
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Wetlands are the largest natural source of methane, one of the most important climate gases. The JULES land surface model simulates these emissions. We use satellite data to evaluate how well JULES reproduces the methane seasonal cycle over different tropical wetlands. It performs well for most regions; however, it struggles for some African wetlands influenced heavily by river flooding. We explain the reasons for these deficiencies and highlight how future development will improve these areas.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Simone Tilmes, Daniele Visioni, Andy Jones, James Haywood, Roland Séférian, Pierre Nabat, Olivier Boucher, Ewa Monica Bednarz, and Ulrike Niemeier
Atmos. Chem. Phys., 22, 4557–4579, https://doi.org/10.5194/acp-22-4557-2022, https://doi.org/10.5194/acp-22-4557-2022, 2022
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This study assesses the impacts of climate interventions, using stratospheric sulfate aerosol and solar dimming on stratospheric ozone, based on three Earth system models with interactive stratospheric chemistry. The climate interventions have been applied to a high emission (baseline) scenario in order to reach global surface temperatures of a medium emission scenario. We find significant increases and decreases in total column ozone, depending on regions and seasons.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Piera Raspollini, Enrico Arnone, Flavio Barbara, Massimo Bianchini, Bruno Carli, Simone Ceccherini, Martyn P. Chipperfield, Angelika Dehn, Stefano Della Fera, Bianca Maria Dinelli, Anu Dudhia, Jean-Marie Flaud, Marco Gai, Michael Kiefer, Manuel López-Puertas, David P. Moore, Alessandro Piro, John J. Remedios, Marco Ridolfi, Harjinder Sembhi, Luca Sgheri, and Nicola Zoppetti
Atmos. Meas. Tech., 15, 1871–1901, https://doi.org/10.5194/amt-15-1871-2022, https://doi.org/10.5194/amt-15-1871-2022, 2022
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The MIPAS instrument onboard the ENVISAT satellite provided 10 years of measurements of the atmospheric emission al limb that allow for the retrieval of latitude- and altitude-resolved atmospheric composition. We describe the improvements implemented in the retrieval algorithm used for the full mission reanalysis, which allows for the generation of the global distributions of 21 atmospheric constituents plus temperature with increased accuracy with respect to previously generated data.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Sandip S. Dhomse, Carlo Arosio, Wuhu Feng, Alexei Rozanov, Mark Weber, and Martyn P. Chipperfield
Earth Syst. Sci. Data, 13, 5711–5729, https://doi.org/10.5194/essd-13-5711-2021, https://doi.org/10.5194/essd-13-5711-2021, 2021
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High-quality long-term ozone profile data sets are key to estimating short- and long-term ozone variability. Almost all the satellite (and chemical model) data sets show some kind of bias with respect to each other. This is because of differences in measurement methodologies as well as simplified processes in the models. We use satellite data sets and chemical model output to generate 42 years of ozone profile data sets using a random-forest machine-learning algorithm that is named ML-TOMCAT.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Akash Biswal, Vikas Singh, Shweta Singh, Amit P. Kesarkar, Khaiwal Ravindra, Ranjeet S. Sokhi, Martyn P. Chipperfield, Sandip S. Dhomse, Richard J. Pope, Tanbir Singh, and Suman Mor
Atmos. Chem. Phys., 21, 5235–5251, https://doi.org/10.5194/acp-21-5235-2021, https://doi.org/10.5194/acp-21-5235-2021, 2021
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Satellite and surface observations show a reduction in NO2 levels over India during the lockdown compared to business-as-usual years. A substantial reduction, proportional to the population, was observed over the urban areas. The changes in NO2 levels at the surface during the lockdown appear to be present in the satellite observations. However, TROPOMI showed a better correlation with surface NO2 and was more sensitive to the changes than OMI because of the finer resolution.
Robert J. Parker, Chris Wilson, A. Anthony Bloom, Edward Comyn-Platt, Garry Hayman, Joe McNorton, Hartmut Boesch, and Martyn P. Chipperfield
Biogeosciences, 17, 5669–5691, https://doi.org/10.5194/bg-17-5669-2020, https://doi.org/10.5194/bg-17-5669-2020, 2020
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Wetlands contribute the largest uncertainty to the atmospheric methane budget. WetCHARTs is a simple, data-driven model that estimates wetland emissions using observations of precipitation and temperature. We perform the first detailed evaluation of WetCHARTs against satellite data and find it performs well in reproducing the observed wetland methane seasonal cycle for the majority of wetland regions. In regions where it performs poorly, we highlight incorrect wetland extent as a key reason.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Benjamin Birner, Martyn P. Chipperfield, Eric J. Morgan, Britton B. Stephens, Marianna Linz, Wuhu Feng, Chris Wilson, Jonathan D. Bent, Steven C. Wofsy, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Chem. Phys., 20, 12391–12408, https://doi.org/10.5194/acp-20-12391-2020, https://doi.org/10.5194/acp-20-12391-2020, 2020
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With new high-precision observations from nine aircraft campaigns and 3-D chemical transport modeling, we show that the argon-to-nitrogen ratio (Ar / N2) in the lowermost stratosphere provides a useful constraint on the “age of air” (the time elapsed since entry of an air parcel into the stratosphere). Therefore, Ar / N2 in combination with traditional age-of-air indicators, such as CO2 and N2O, could provide new insights into atmospheric mixing and transport.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
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.
Sarah A. Strode, James S. Wang, Michael Manyin, Bryan Duncan, Ryan Hossaini, Christoph A. Keller, Sylvia E. Michel, and James W. C. White
Atmos. Chem. Phys., 20, 8405–8419, https://doi.org/10.5194/acp-20-8405-2020, https://doi.org/10.5194/acp-20-8405-2020, 2020
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The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss of CH4 by reaction with OH and chlorine (Cl) also affects this ratio. Tropospheric Cl provides a small and uncertain sink for CH4 but has a large effect on its isotopic ratio. We use the GEOS model with several different Cl fields to test the sensitivity of methane's isotopic composition to tropospheric Cl. Cl affects the global mean, hemispheric gradient, and seasonal cycle of the isotopic ratio.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
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.
Andreas Chrysanthou, Amanda C. Maycock, and Martyn P. Chipperfield
Weather Clim. Dynam., 1, 155–174, https://doi.org/10.5194/wcd-1-155-2020, https://doi.org/10.5194/wcd-1-155-2020, 2020
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We perform 50-year-long time-slice experiments using the Met Office HadGEM3 global climate model in order to decompose the Brewer–Dobson circulation (BDC) response to an abrupt quadrupling of CO2 in three distinct components, (a) the rapid adjustment, associated with CO2 radiative effects; (b) a global uniform sea surface temperature warming; and (c) sea surface temperature patterns. This demonstrates a potential for fast and slow timescales of the response of the BDC to greenhouse gas forcing.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
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.
Andreas Chrysanthou, Amanda C. Maycock, Martyn P. Chipperfield, Sandip Dhomse, Hella Garny, Douglas Kinnison, Hideharu Akiyoshi, Makoto Deushi, Rolando R. Garcia, Patrick Jöckel, Oliver Kirner, Giovanni Pitari, David A. Plummer, Laura Revell, Eugene Rozanov, Andrea Stenke, Taichu Y. Tanaka, Daniele Visioni, and Yousuke Yamashita
Atmos. Chem. Phys., 19, 11559–11586, https://doi.org/10.5194/acp-19-11559-2019, https://doi.org/10.5194/acp-19-11559-2019, 2019
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We perform the first multi-model comparison of the impact of nudged meteorology on the stratospheric residual circulation (RC) in chemistry–climate models. Nudging meteorology does not constrain the mean strength of RC compared to free-running simulations, and despite the lack of agreement in the mean circulation, nudging tightly constrains the inter-annual variability in the tropical upward mass flux in the lower stratosphere. In summary, nudging strongly affects the representation of RC.
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.
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.
Matthew J. Rowlinson, Alexandru Rap, Stephen R. Arnold, Richard J. Pope, Martyn P. Chipperfield, Joe McNorton, Piers Forster, Hamish Gordon, Kirsty J. Pringle, Wuhu Feng, Brian J. Kerridge, Barry L. Latter, and Richard Siddans
Atmos. Chem. Phys., 19, 8669–8686, https://doi.org/10.5194/acp-19-8669-2019, https://doi.org/10.5194/acp-19-8669-2019, 2019
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Wildfires and meteorology have a substantial effect on atmospheric concentrations of greenhouse gases such as methane and ozone. During the 1997 El Niño event, unusually large fire emissions indirectly increased global methane through carbon monoxide emission, which decreased the oxidation capacity of the atmosphere. There were also large regional changes to tropospheric ozone concentrations, but contrasting effects of fire and meteorology resulted in a small change to global radiative forcing.
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.
Evgenia Galytska, Alexey Rozanov, Martyn P. Chipperfield, Sandip. S. Dhomse, Mark Weber, Carlo Arosio, Wuhu Feng, and John P. Burrows
Atmos. Chem. Phys., 19, 767–783, https://doi.org/10.5194/acp-19-767-2019, https://doi.org/10.5194/acp-19-767-2019, 2019
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In this study we analysed ozone changes in the tropical mid-stratosphere as observed by the SCIAMACHY instrument during 2004–2012. We used simulations from TOMCAT model with different chemical and dynamical forcings to reveal primary causes of ozone changes. We also considered measured NO2 and modelled NOx, NOx, and N2O data. With modelled AoA data we identified seasonal changes in the upwelling speed and explained how those changes affect N2O chemistry which leads to observed ozone changes.
Debora Griffin, Kaley A. Walker, Ingo Wohltmann, Sandip S. Dhomse, Markus Rex, Martyn P. Chipperfield, Wuhu Feng, Gloria L. Manney, Jane Liu, and David Tarasick
Atmos. Chem. Phys., 19, 577–601, https://doi.org/10.5194/acp-19-577-2019, https://doi.org/10.5194/acp-19-577-2019, 2019
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Ozone in the stratosphere is important to protect the Earth from UV radiation. Using measurements taken by the Atmospheric Chemistry Experiment satellite between 2005 and 2013, we examine different methods to calculate the ozone loss in the high Arctic and establish the altitude at which most of the ozone is destroyed. Our results show that the different methods agree within the uncertainties. Recommendations are made on which methods are most appropriate to use.
Joe McNorton, Chris Wilson, Manuel Gloor, Rob J. Parker, Hartmut Boesch, Wuhu Feng, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 18149–18168, https://doi.org/10.5194/acp-18-18149-2018, https://doi.org/10.5194/acp-18-18149-2018, 2018
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Since 2007 atmospheric methane (CH4) has been unexpectedly increasing following a 6-year hiatus. We have used an atmospheric model to attribute regional sources and global sinks of CH4 using observations for the 2003–2015 period. Model results show the renewed growth is best explained by decreased atmospheric removal, decreased biomass burning emissions, and an increased energy sector (mainly from Africa–Middle East and Southern Asia–Oceania) and wetland emissions (mainly from northern Eurasia).
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.
Birgit Hassler, Stefanie Kremser, Greg E. Bodeker, Jared Lewis, Kage Nesbit, Sean M. Davis, Martyn P. Chipperfield, Sandip S. Dhomse, and Martin Dameris
Earth Syst. Sci. Data, 10, 1473–1490, https://doi.org/10.5194/essd-10-1473-2018, https://doi.org/10.5194/essd-10-1473-2018, 2018
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
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.
Richard J. Pope, Martyn P. Chipperfield, Stephen R. Arnold, Norbert Glatthor, Wuhu Feng, Sandip S. Dhomse, Brian J. Kerridge, Barry G. Latter, and Richard Siddans
Atmos. Chem. Phys., 18, 8389–8408, https://doi.org/10.5194/acp-18-8389-2018, https://doi.org/10.5194/acp-18-8389-2018, 2018
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.
Richard Hyde, Ryan Hossaini, and Amber A. Leeson
Geosci. Model Dev., 11, 2033–2048, https://doi.org/10.5194/gmd-11-2033-2018, https://doi.org/10.5194/gmd-11-2033-2018, 2018
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Clustering, the automated grouping of similar data, can provide powerful insight into large/complex data. We demonstrate the benefits of clustering applied to output from climate model inter-comparison initiatives. We focus on modelled tropospheric ozone from the ACCMIP project. Cluster-based subsampling of the model ensemble can (i) remove outlier data on a grid-cell basis, reducing model–observation bias and (ii) provide a useful framework in which to investigate and visualise model diversity.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
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.
Sarah A. Monks, Stephen R. Arnold, Michael J. Hollaway, Richard J. Pope, Chris Wilson, Wuhu Feng, Kathryn M. Emmerson, Brian J. Kerridge, Barry L. Latter, Georgina M. Miles, Richard Siddans, and Martyn P. Chipperfield
Geosci. Model Dev., 10, 3025–3057, https://doi.org/10.5194/gmd-10-3025-2017, https://doi.org/10.5194/gmd-10-3025-2017, 2017
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The TOMCAT chemical transport model has been updated with the chemical degradation of ethene, propene, toluene, butane and monoterpenes. The tropospheric chemical mechanism is documented and the model is evaluated against surface, balloon, aircraft and satellite data. The model is generally able to capture the main spatial and seasonal features of carbon monoxide, ozone, volatile organic compounds and reactive nitrogen. However,
some model biases are found that require further investigation.
Wenshou Tian, Yuanpu Li, Fei Xie, Jiankai Zhang, Martyn P. Chipperfield, Wuhu Feng, Yongyun Hu, Sen Zhao, Xin Zhou, Yun Yang, and Xuan Ma
Atmos. Chem. Phys., 17, 6705–6722, https://doi.org/10.5194/acp-17-6705-2017, https://doi.org/10.5194/acp-17-6705-2017, 2017
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Although the principal mechanisms responsible for the formation of the Antarctic ozone hole are well understood, the factors or processes that generate interannual variations in ozone levels in the southern high-latitude stratosphere remain under debate. This study finds that the SST variations across the East Asian marginal seas (5° S–35° N, 100–140° E) could modulate the southern high-latitude stratospheric ozone interannual changes.
Shreeya Verma, Julia Marshall, Mark Parrington, Anna Agustí-Panareda, Sebastien Massart, Martyn P. Chipperfield, Christopher Wilson, and Christoph Gerbig
Atmos. Chem. Phys., 17, 6663–6678, https://doi.org/10.5194/acp-17-6663-2017, https://doi.org/10.5194/acp-17-6663-2017, 2017
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Aircraft profiles are a useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, these are available only up to about 9–13 km altitude and therefore need to be extended synthetically into the stratosphere using other sources. In this study, we analyse three different data sources that are available for extension of CH4 profiles by comparing the error introduced by each into the total column and provide recommendations regarding the best approach.
Jochen Stutz, Bodo Werner, Max Spolaor, Lisa Scalone, James Festa, Catalina Tsai, Ross Cheung, Santo F. Colosimo, Ugo Tricoli, Rasmus Raecke, Ryan Hossaini, Martyn P. Chipperfield, Wuhu Feng, Ru-Shan Gao, Eric J. Hintsa, James W. Elkins, Fred L. Moore, Bruce Daube, Jasna Pittman, Steven Wofsy, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 1017–1042, https://doi.org/10.5194/amt-10-1017-2017, https://doi.org/10.5194/amt-10-1017-2017, 2017
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A new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument was developed for NASA’s Global Hawk unmanned aerial system during the Airborne Tropical TRopopause EXperiment to study trace gases in the tropical tropopause layer. A new technique that uses in situ and DOAS O3 observations together with radiative transfer calculations allows the retrieval of mixing ratios from the slant column densities of BrO and NO2 at high accuracies of 0.5 ppt and 15 ppt, respectively.
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.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
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.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, John J. Remedios, Carsten Warneke, James M. Roberts, Glenn S. Diskin, Lewis G. Huey, Armin Wisthaler, Eric C. Apel, Peter F. Bernath, and Wuhu Feng
Atmos. Chem. Phys., 16, 13541–13559, https://doi.org/10.5194/acp-16-13541-2016, https://doi.org/10.5194/acp-16-13541-2016, 2016
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.
Anna Totterdill, Tamás Kovács, Wuhu Feng, Sandip Dhomse, Christopher J. Smith, Juan Carlos Gómez-Martín, Martyn P. Chipperfield, Piers M. Forster, and John M. C. Plane
Atmos. Chem. Phys., 16, 11451–11463, https://doi.org/10.5194/acp-16-11451-2016, https://doi.org/10.5194/acp-16-11451-2016, 2016
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In this study we have experimentally determined the infrared absorption cross sections of NF3 and CFC-115, calculated the radiative forcing and efficiency using two radiative transfer models and identified the effect of clouds and stratospheric adjustment. We have also determined their atmospheric lifetimes using the Whole Atmosphere Community Climate Model.
Tamás Kovács, John M. C. Plane, Wuhu Feng, Tibor Nagy, Martyn P. Chipperfield, Pekka T. Verronen, Monika E. Andersson, David A. Newnham, Mark A. Clilverd, and Daniel R. Marsh
Geosci. Model Dev., 9, 3123–3136, https://doi.org/10.5194/gmd-9-3123-2016, https://doi.org/10.5194/gmd-9-3123-2016, 2016
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This study was completed on D-region atmospheric model development. The sophisticated 3-D Whole Atmosphere Community Climate Model (WACCM) and the 1-D Sodynkalä Ion and Neutral Chemistry Model (SIC) were combined in order to provide a detailed, accurate model (WACCM-SIC) that considers the processes taking place in solar proton events. The original SIC model was reduced by mechanism reduction, which provided an accurate sub-mechanism (rSIC, WACCM-rSIC) of the original model.
Jeremy J. Harrison, Martyn P. Chipperfield, Christopher D. Boone, Sandip S. Dhomse, Peter F. Bernath, Lucien Froidevaux, John Anderson, and James Russell III
Atmos. Chem. Phys., 16, 10501–10519, https://doi.org/10.5194/acp-16-10501-2016, https://doi.org/10.5194/acp-16-10501-2016, 2016
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HF, the dominant stratospheric fluorine reservoir, results from the atmospheric degradation of anthropogenic species such as CFCs, HCFCs, and HFCs. All are strong greenhouse gases, and CFCs and HCFCs deplete stratospheric ozone.
We report the comparison of HF global distributions and trends measured by the ACE-FTS and HALOE satellite instruments with the output of SLIMCAT, a chemical transport model. The global HF trends reveal a slowing down in the rate of increase of HF since the 1990s.
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
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
S. T. Lennartz, G. Krysztofiak, C. A. Marandino, B.-M. Sinnhuber, S. Tegtmeier, F. Ziska, R. Hossaini, K. Krüger, S. A. Montzka, E. Atlas, D. E. Oram, T. Keber, H. Bönisch, and B. Quack
Atmos. Chem. Phys., 15, 11753–11772, https://doi.org/10.5194/acp-15-11753-2015, https://doi.org/10.5194/acp-15-11753-2015, 2015
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Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact atmospheric chemistry. To assess this impact on ozone depletion and the radiative budget, it is critical that their marine emissions in atmospheric chemistry models are quantified as accurately as possible. We show that calculating emissions online with an interactive atmosphere improves the agreement with current observations and should be employed regularly in models where marine sources are important.
R. J. Pope, N. H. Savage, M. P. Chipperfield, C. Ordóñez, and L. S. Neal
Atmos. Chem. Phys., 15, 11201–11215, https://doi.org/10.5194/acp-15-11201-2015, https://doi.org/10.5194/acp-15-11201-2015, 2015
R. J. Pope, M. P. Chipperfield, N. H. Savage, C. Ordóñez, L. S. Neal, L. A. Lee, S. S. Dhomse, N. A. D. Richards, and T. D. Keslake
Atmos. Chem. Phys., 15, 5611–5626, https://doi.org/10.5194/acp-15-5611-2015, https://doi.org/10.5194/acp-15-5611-2015, 2015
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
G. D. Hayman, F. M. O'Connor, M. Dalvi, D. B. Clark, N. Gedney, C. Huntingford, C. Prigent, M. Buchwitz, O. Schneising, J. P. Burrows, C. Wilson, N. Richards, and M. Chipperfield
Atmos. Chem. Phys., 14, 13257–13280, https://doi.org/10.5194/acp-14-13257-2014, https://doi.org/10.5194/acp-14-13257-2014, 2014
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Globally, wetlands are a major source of methane, which is the second most important greenhouse gas. We find the JULES wetland methane scheme to perform well in general, although there is a tendency for it to overpredict emissions in the tropics and underpredict them in northern latitudes. Our study highlights novel uses of satellite data as a major tool to constrain land-atmosphere methane flux models in a warming world.
J. J. Harrison, M. P. Chipperfield, A. Dudhia, S. Cai, S. Dhomse, C. D. Boone, and P. F. Bernath
Atmos. Chem. Phys., 14, 11915–11933, https://doi.org/10.5194/acp-14-11915-2014, https://doi.org/10.5194/acp-14-11915-2014, 2014
C. Wilson, M. P. Chipperfield, M. Gloor, and F. Chevallier
Geosci. Model Dev., 7, 2485–2500, https://doi.org/10.5194/gmd-7-2485-2014, https://doi.org/10.5194/gmd-7-2485-2014, 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
L. Kritten, A. Butz, M. P. Chipperfield, M. Dorf, S. Dhomse, R. Hossaini, H. Oelhaf, C. Prados-Roman, G. Wetzel, and K. Pfeilsticker
Atmos. Chem. Phys., 14, 9555–9566, https://doi.org/10.5194/acp-14-9555-2014, https://doi.org/10.5194/acp-14-9555-2014, 2014
R. L. Thompson, P. K. Patra, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, C. Wilson, P. Bergamaschi, E. Dlugokencky, C. Sweeney, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, M. Saunois, M. Chipperfield, and P. Bousquet
Atmos. Chem. Phys., 14, 4349–4368, https://doi.org/10.5194/acp-14-4349-2014, https://doi.org/10.5194/acp-14-4349-2014, 2014
A. T. Brown, M. P. Chipperfield, N. A. D. Richards, C. Boone, and P. F. Bernath
Atmos. Chem. Phys., 14, 267–282, https://doi.org/10.5194/acp-14-267-2014, https://doi.org/10.5194/acp-14-267-2014, 2014
S. Tegtmeier, K. Krüger, B. Quack, E. Atlas, D. R. Blake, H. Boenisch, A. Engel, H. Hepach, R. Hossaini, M. A. Navarro, S. Raimund, S. Sala, Q. Shi, and F. Ziska
Atmos. Chem. Phys., 13, 11869–11886, https://doi.org/10.5194/acp-13-11869-2013, https://doi.org/10.5194/acp-13-11869-2013, 2013
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
S. S. Dhomse, M. P. Chipperfield, W. Feng, W. T. Ball, Y. C. Unruh, J. D. Haigh, N. A. Krivova, S. K. Solanki, and A. K. Smith
Atmos. Chem. Phys., 13, 10113–10123, https://doi.org/10.5194/acp-13-10113-2013, https://doi.org/10.5194/acp-13-10113-2013, 2013
R. Locatelli, P. Bousquet, F. Chevallier, A. Fortems-Cheney, S. Szopa, M. Saunois, A. Agusti-Panareda, D. Bergmann, H. Bian, P. Cameron-Smith, M. P. Chipperfield, E. Gloor, S. Houweling, S. R. Kawa, M. Krol, P. K. Patra, R. G. Prinn, M. Rigby, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 9917–9937, https://doi.org/10.5194/acp-13-9917-2013, https://doi.org/10.5194/acp-13-9917-2013, 2013
A. T. Brown, M. P. Chipperfield, S. Dhomse, C. Boone, and P. F. Bernath
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-23491-2013, https://doi.org/10.5194/acpd-13-23491-2013, 2013
Revised manuscript has not been submitted
P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, Emma C. Leedham Elvidge, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-20611-2013, https://doi.org/10.5194/acpd-13-20611-2013, 2013
Revised manuscript not accepted
S. Kreycy, C. Camy-Peyret, M. P. Chipperfield, M. Dorf, W. Feng, R. Hossaini, L. Kritten, B. Werner, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 6263–6274, https://doi.org/10.5194/acp-13-6263-2013, https://doi.org/10.5194/acp-13-6263-2013, 2013
N. A. D. Richards, S. R. Arnold, M. P. Chipperfield, G. Miles, A. Rap, R. Siddans, S. A. Monks, and M. J. Hollaway
Atmos. Chem. Phys., 13, 2331–2345, https://doi.org/10.5194/acp-13-2331-2013, https://doi.org/10.5194/acp-13-2331-2013, 2013
D. A. Belikov, S. Maksyutov, M. Krol, A. Fraser, M. Rigby, H. Bian, A. Agusti-Panareda, D. Bergmann, P. Bousquet, P. Cameron-Smith, M. P. Chipperfield, A. Fortems-Cheiney, E. Gloor, K. Haynes, P. Hess, S. Houweling, S. R. Kawa, R. M. Law, Z. Loh, L. Meng, P. I. Palmer, P. K. Patra, R. G. Prinn, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 1093–1114, https://doi.org/10.5194/acp-13-1093-2013, https://doi.org/10.5194/acp-13-1093-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)
Correction of stratospheric age of air (AoA) derived from sulfur hexafluoride (SF6) for the effect of chemical sinks
Opinion: Stratospheric ozone – depletion, recovery and new challenges
Quantum yields of CHDO above 300 nm
Sensitivities of atmospheric composition and climate to altitude and latitude of hypersonic aircraft emissions
Analysis of a newly homogenised ozonesonde dataset from Lauder, New Zealand
N2O as a regression proxy for dynamical variability in stratospheric trace gas trends
The influence of future changes in springtime Arctic ozone on stratospheric and surface climate
Weakening of springtime Arctic ozone depletion with climate change
The impact of an extreme solar event on the middle atmosphere: a case study
The future ozone trends in changing climate simulated with SOCOLv4
Atmospheric distribution of HCN from satellite observations and 3-D model simulations
Indicators of the ozone recovery for selected sites in the Northern Hemisphere mid-latitudes derived from various total column ozone datasets (1980–2020)
The historical ozone trends simulated with the SOCOLv4 and their comparison with observations and reanalyses
Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 1: Stratospheric chlorine budget and the role of transport
Effects of reanalysis forcing fields on ozone trends and age of air from a chemical transport model
The influence of energetic particle precipitation on Antarctic stratospheric chlorine and ozone over the 20th century
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
An Arctic ozone hole in 2020 if not for the Montreal Protocol
Effects of enhanced downwelling of NOx on Antarctic upper-stratospheric ozone in the 21st century
Processes influencing lower stratospheric water vapour in monsoon anticyclones: insights from Lagrangian modelling
Evaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100
Slow feedbacks resulting from strongly enhanced atmospheric methane mixing ratios in a chemistry–climate model with mixed-layer ocean
Impact of the eruption of Mt Pinatubo on the chemical composition of the stratosphere
Projecting ozone hole recovery using an ensemble of chemistry–climate models weighted by model performance and independence
Inconsistencies between chemistry–climate models and observed lower stratospheric ozone trends since 1998
Reformulating the bromine alpha factor and equivalent effective stratospheric chlorine (EESC): evolution of ozone destruction rates of bromine and chlorine in future climate scenarios
Analysis and attribution of total column ozone changes over the Tibetan Plateau during 1979–2017
Seasonal impact of biogenic very short-lived bromocarbons on lowermost stratospheric ozone between 60° N and 60° S during the 21st century
Modelling the potential impacts of the recent, unexpected increase in CFC-11 emissions on total column ozone recovery
The potential impacts of a sulfur- and halogen-rich supereruption such as Los Chocoyos on the atmosphere and climate
Technical note: Intermittent reduction of the stratospheric ozone over northern Europe caused by a storm in the Atlantic Ocean
Possible implications of enhanced chlorofluorocarbon-11 concentrations on ozone
Technical note: Reanalysis of Aura MLS chemical observations
Separating the role of direct radiative heating and photolysis in modulating the atmospheric response to the amplitude of the 11-year solar cycle forcing
Reactive nitrogen (NOy) and ozone responses to energetic electron precipitation during Southern Hemisphere winter
Implication of strongly increased atmospheric methane concentrations for chemistry–climate connections
Multitimescale variations in modeled stratospheric water vapor derived from three modern reanalysis products
How robust are stratospheric age of air trends from different reanalyses?
Evaluation of CESM1 (WACCM) free-running and specified dynamics atmospheric composition simulations using global multispecies satellite data records
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
On ozone trend detection: using coupled chemistry–climate simulations to investigate early signs of total column ozone recovery
Future changes in the stratosphere-to-troposphere ozone mass flux and the contribution from climate change and ozone recovery
Hella Garny, Roland Eichinger, Johannes C. Laube, Eric A. Ray, Gabriele P. Stiller, Harald Bönisch, Laura Saunders, and Marianna Linz
Atmos. Chem. Phys., 24, 4193–4215, https://doi.org/10.5194/acp-24-4193-2024, https://doi.org/10.5194/acp-24-4193-2024, 2024
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Transport circulation in the stratosphere is important for the distribution of tracers, but its strength is hard to measure. Mean transport times can be inferred from observations of trace gases with certain properties, such as sulfur hexafluoride (SF6). However, this gas has a chemical sink in the high atmosphere, which can lead to substantial biases in inferred transport times. In this paper we present a method to correct mean transport times derived from SF6 for the effects of chemical sinks.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Ernst-Peter Röth and Luc Vereecken
Atmos. Chem. Phys., 24, 2625–2638, https://doi.org/10.5194/acp-24-2625-2024, https://doi.org/10.5194/acp-24-2625-2024, 2024
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The paper presents the radical and molecular product quantum yields in the photolysis reaction of CHDO at wavelengths above 300 nm. Two different approaches based on literature data are used, with results falling within both approaches' uncertainty ranges. Simple functional forms are presented for use in photochemical models of the atmosphere.
Johannes Pletzer and Volker Grewe
Atmos. Chem. Phys., 24, 1743–1775, https://doi.org/10.5194/acp-24-1743-2024, https://doi.org/10.5194/acp-24-1743-2024, 2024
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Very fast aircraft can travel at 30–40 km altitude and are designed to use liquid hydrogen as fuel instead of kerosene. Depending on their flight altitude, the impact of these aircraft on the atmosphere and climate can change very much. Our results show that a variation inflight latitude can have a considerably higher change in impact compared to a variation in flight altitude. Atmospheric air transport and polar stratospheric clouds play an important role in hypersonic aircraft emissions.
Guang Zeng, Richard Querel, Hisako Shiona, Deniz Poyraz, Roeland Van Malderen, Alex Geddes, Penny Smale, Dan Smale, John Robinson, and Olaf Morgenstern
EGUsphere, https://doi.org/10.5194/egusphere-2023-2534, https://doi.org/10.5194/egusphere-2023-2534, 2023
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We present a homogenised ozonesonde record (1987–2020) for Lauder, New Zealand, identify factors driving ozone trends, and attribute them to anthropogenic forcings using statistical analysis and model simulations. We find that significant negative stratospheric ozone trends identified at Lauder are associated with an increase in tropopause height and that CO2-driven dynamical changes have had an increasingly important role in driving ozone trends, offsetting effects of methane and nitrous oxide.
Kimberlee Dubé, Susann Tegtmeier, Adam Bourassa, Daniel Zawada, Douglas Degenstein, Patrick E. Sheese, Kaley A. Walker, and William Randel
Atmos. Chem. Phys., 23, 13283–13300, https://doi.org/10.5194/acp-23-13283-2023, https://doi.org/10.5194/acp-23-13283-2023, 2023
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This paper presents a technique for understanding the causes of long-term changes in stratospheric composition. By using N2O as a proxy for stratospheric circulation in the model used to calculated trends, it is possible to separate the effects of dynamics and chemistry on observed trace gas trends. We find that observed HCl increases are due to changes in the stratospheric circulation, as are O3 decreases above 30 hPa in the Northern Hemisphere.
Gabriel Chiodo, Marina Friedel, Svenja Seeber, Daniela Domeisen, Andrea Stenke, Timofei Sukhodolov, and Franziska Zilker
Atmos. Chem. Phys., 23, 10451–10472, https://doi.org/10.5194/acp-23-10451-2023, https://doi.org/10.5194/acp-23-10451-2023, 2023
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Stratospheric ozone protects the biosphere from harmful UV radiation. Anthropogenic activity has led to a reduction in the ozone layer in the recent past, but thanks to the implementation of the Montreal Protocol, the ozone layer is projected to recover. In this study, we show that projected future changes in Arctic ozone abundances during springtime will influence stratospheric climate and thereby actively modulate large-scale circulation changes in the Northern Hemisphere.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Thomas Reddmann, Miriam Sinnhuber, Jan Maik Wissing, Olesya Yakovchuk, and Ilya Usoskin
Atmos. Chem. Phys., 23, 6989–7000, https://doi.org/10.5194/acp-23-6989-2023, https://doi.org/10.5194/acp-23-6989-2023, 2023
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Recent analyses of isotopic records of ice cores and sediments have shown that very strong explosions may occur on the Sun, perhaps about one such explosion every 1000 years. Such explosions pose a real threat to humankind. It is therefore of great interest to study the impact of such explosions on Earth. We analyzed how the explosions would affect the chemistry of the middle atmosphere and show that the related ozone loss is not dramatic and that the atmosphere will recover within 1 year.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, and Thomas Peter
Atmos. Chem. Phys., 23, 4801–4817, https://doi.org/10.5194/acp-23-4801-2023, https://doi.org/10.5194/acp-23-4801-2023, 2023
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The future ozone evolution in SOCOLv4 simulations under SSP2-4.5 and SSP5-8.5 scenarios has been assessed for the period 2015–2099 and subperiods using the DLM approach. The SOCOLv4 projects a decline in tropospheric ozone in the 2030s in SSP2-4.5 and in the 2060s in SSP5-8.5. The stratospheric ozone increase is ~3 times higher in SSP5-8.5, confirming the important role of GHGs in ozone evolution. We also showed that tropospheric ozone strongly impacts the total column in the tropics.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Janusz Krzyścin
Atmos. Chem. Phys., 23, 3119–3132, https://doi.org/10.5194/acp-23-3119-2023, https://doi.org/10.5194/acp-23-3119-2023, 2023
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We propose indices to obtain the current stage of total column ozone (TCO3) recovery attributed to ozone-depleting substance (ODS) changes in the stratosphere. The indices are calculated using TCO3 values in key years of the ODS changes. The ozone recovery stage is derived for 16 sites in the NH mid-latitudes using results from ground and satellite measurements and reanalysis data. In Europe, there is a slow TCO3 recovery. A continuous TCO3 decline has been occurring in some sites since 1980.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, William Ball, and Thomas Peter
Atmos. Chem. Phys., 22, 15333–15350, https://doi.org/10.5194/acp-22-15333-2022, https://doi.org/10.5194/acp-22-15333-2022, 2022
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Applying the dynamic linear model, we confirm near-global ozone recovery (55°N–55°S) in the mesosphere, upper and middle stratosphere, and a steady increase in the troposphere. We also show that modern chemistry–climate models (CCMs) like SOCOLv4 may reproduce the observed trend distribution of lower stratospheric ozone, despite exhibiting a lower magnitude and statistical significance. The obtained ozone trend pattern in SOCOLv4 is generally consistent with observations and reanalysis datasets.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Ville Maliniemi, Pavle Arsenovic, Annika Seppälä, and Hilde Nesse Tyssøy
Atmos. Chem. Phys., 22, 8137–8149, https://doi.org/10.5194/acp-22-8137-2022, https://doi.org/10.5194/acp-22-8137-2022, 2022
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We simulate the effect of energetic particle precipitation (EPP) on Antarctic stratospheric ozone chemistry over the whole 20th century. We find a significant increase of reactive nitrogen due to EP, which can deplete ozone via a catalytic reaction. Furthermore, significant modulation of active chlorine is obtained related to EPP, which impacts ozone depletion by both active chlorine and EPP. Our results show that EPP has been a significant modulator of ozone chemistry during the CFC era.
Daniel J. Ruiz and Michael J. Prather
Atmos. Chem. Phys., 22, 2079–2093, https://doi.org/10.5194/acp-22-2079-2022, https://doi.org/10.5194/acp-22-2079-2022, 2022
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The stratosphere is an important source of tropospheric ozone, which affects climate, chemistry, and air quality, but is extremely difficult to quantify given the large production and loss terms in the troposphere. Here, we use other gases that are well observed and quantified as a reference to test our simulations of ozone transport in the atmosphere. This allows us to better constrain the stratospheric source of ozone and also offers guidance to improve future simulations of ozone transport.
Catherine Wilka, Susan Solomon, Doug Kinnison, and David Tarasick
Atmos. Chem. Phys., 21, 15771–15781, https://doi.org/10.5194/acp-21-15771-2021, https://doi.org/10.5194/acp-21-15771-2021, 2021
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We use satellite and balloon measurements to evaluate modeled ozone loss seen in the unusually cold Arctic of 2020 in the real world and compare it to simulations of a world avoided. We show that extensive denitrification in 2020 provides an important test case for stratospheric model process representations. If the Montreal Protocol had not banned ozone-depleting substances, an Arctic ozone hole would have emerged for the first time in spring 2020 that is comparable to those in the Antarctic.
Ville Maliniemi, Hilde Nesse Tyssøy, Christine Smith-Johnsen, Pavle Arsenovic, and Daniel R. Marsh
Atmos. Chem. Phys., 21, 11041–11052, https://doi.org/10.5194/acp-21-11041-2021, https://doi.org/10.5194/acp-21-11041-2021, 2021
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We simulate ozone variability over the 21st century with different greenhouse gas scenarios. Our results highlight a novel mechanism of additional reactive nitrogen species descending to the Antarctic stratosphere from the thermosphere/upper mesosphere due to the accelerated residual circulation under climate change. This excess descending NOx can potentially prevent a super recovery of ozone in the Antarctic upper stratosphere.
Nuria Pilar Plaza, Aurélien Podglajen, Cristina Peña-Ortiz, and Felix Ploeger
Atmos. Chem. Phys., 21, 9585–9607, https://doi.org/10.5194/acp-21-9585-2021, https://doi.org/10.5194/acp-21-9585-2021, 2021
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We study the role of different processes in setting the lower stratospheric water vapour. We find that mechanisms involving ice microphysics and small-scale mixing produce the strongest increase in water vapour, in particular over the Asian Monsoon. Small-scale mixing has a special relevance as it improves the agreement with observations at seasonal and intra-seasonal timescales, contrary to the North American Monsoon case, in which large-scale temperatures still dominate its variability.
James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
Atmos. Chem. Phys., 21, 5015–5061, https://doi.org/10.5194/acp-21-5015-2021, https://doi.org/10.5194/acp-21-5015-2021, 2021
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Stratospheric ozone and water vapour are key components of the Earth system; changes to both have important impacts on global and regional climate. We evaluate changes to these species from 1850 to 2100 in the new generation of CMIP6 models. There is good agreement between the multi-model mean and observations, although there is substantial variation between the individual models. The future evolution of both ozone and water vapour is strongly dependent on the assumed future emissions scenario.
Laura Stecher, Franziska Winterstein, Martin Dameris, Patrick Jöckel, Michael Ponater, and Markus Kunze
Atmos. Chem. Phys., 21, 731–754, https://doi.org/10.5194/acp-21-731-2021, https://doi.org/10.5194/acp-21-731-2021, 2021
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This study investigates the impact of strongly increased atmospheric methane mixing ratios on the Earth's climate. An interactive model system including atmospheric dynamics, chemistry, and a mixed-layer ocean model is used to analyse the effect of doubled and quintupled methane mixing ratios. We assess feedbacks on atmospheric chemistry and changes in the stratospheric circulation, focusing on the impact of tropospheric warming, and their relevance for the model's climate sensitivity.
Markus Kilian, Sabine Brinkop, and Patrick Jöckel
Atmos. Chem. Phys., 20, 11697–11715, https://doi.org/10.5194/acp-20-11697-2020, https://doi.org/10.5194/acp-20-11697-2020, 2020
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After the volcanic eruption of Mt Pinatubo in 1991, ozone decreased in the tropics and increased in the midlatitudes and polar regions for 1 year. The change in the ozone column is solely a result of the volcanic heating, followed by an ozone decrease in the higher latitudes. This is caused by the volcanic aerosol, which changes the heterogeneous chemistry and thus the catalytic ozone loss cycles. Vertical transport of water vapour is enhanced by volcanic heating and increases methane.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
William T. Ball, Gabriel Chiodo, Marta Abalos, Justin Alsing, and Andrea Stenke
Atmos. Chem. Phys., 20, 9737–9752, https://doi.org/10.5194/acp-20-9737-2020, https://doi.org/10.5194/acp-20-9737-2020, 2020
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Recent lower stratospheric ozone decreases remain unexplained. We show that chemistry–climate models are not generally able to reproduce mid-latitude ozone and water vapour changes. Our analysis of observations provides evidence that climate change may be responsible for the ozone trends. While model projections suggest that extratropical ozone should recover by 2100, our study raises questions about their efficacy in simulating lower stratospheric changes in this region.
J. Eric Klobas, Debra K. Weisenstein, Ross J. Salawitch, and David M. Wilmouth
Atmos. Chem. Phys., 20, 9459–9471, https://doi.org/10.5194/acp-20-9459-2020, https://doi.org/10.5194/acp-20-9459-2020, 2020
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The rates of important ozone-destroying chemical reactions in the stratosphere are likely to change in the future. We employ a computer model to evaluate how the rates of ozone destruction by chlorine and bromine may evolve in four climate change scenarios with the introduction of the eta factor. We then show how these changing rates will impact the ozone-depleting power of the stratosphere with a new metric known as Equivalent Effective Stratospheric Benchmark-normalized Chlorine (EESBnC).
Yajuan Li, Martyn P. Chipperfield, Wuhu Feng, Sandip S. Dhomse, Richard J. Pope, Faquan Li, and Dong Guo
Atmos. Chem. Phys., 20, 8627–8639, https://doi.org/10.5194/acp-20-8627-2020, https://doi.org/10.5194/acp-20-8627-2020, 2020
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The Tibetan Plateau (TP) exerts important thermal and dynamical effects on atmospheric circulation, climate change as well as the ozone distribution. In this study, we use updated observations and model simulations to investigate the ozone trends and variations over the TP. Wintertime TP ozone variations are largely controlled by tropical to high-latitude transport processes, whereas summertime concentrations are a combined effect of photochemical decay and tropical processes.
Javier Alejandro Barrera, Rafael Pedro Fernandez, Fernando Iglesias-Suarez, Carlos Alberto Cuevas, Jean-Francois Lamarque, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 8083–8102, https://doi.org/10.5194/acp-20-8083-2020, https://doi.org/10.5194/acp-20-8083-2020, 2020
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The inclusion of biogenic very short-lived bromocarbons (VSLBr) in the CAM-chem model improves the model–satellite agreement of the total ozone columns at mid-latitudes and drives a persistent hemispheric asymmetry in lowermost stratospheric ozone loss. The seasonal VSLBr impact on mid-latitude lowermost stratospheric ozone is influenced by the heterogeneous reactivation processes of inorganic chlorine on ice crystals, with a clear increase in ozone destruction during spring and winter.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Hans Brenna, Steffen Kutterolf, Michael J. Mills, and Kirstin Krüger
Atmos. Chem. Phys., 20, 6521–6539, https://doi.org/10.5194/acp-20-6521-2020, https://doi.org/10.5194/acp-20-6521-2020, 2020
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The Los Chocoyos supereruption (84 000 years ago) in Guatemala was one of the largest volcanic events of the last 100 000 years. This eruption released enormous amounts of sulfur, which cooled the climate, as well as chlorine and bromine, which destroyed the ozone in the stratosphere. We have simulated this eruption by using an advanced chemistry–climate model. We found a collapse in the ozone layer lasting more than 10 years, increased surface–UV radiation, and a 30-year climate-cooling period.
Mikhail Sofiev, Rostislav Kouznetsov, Risto Hänninen, and Viktoria F. Sofieva
Atmos. Chem. Phys., 20, 1839–1847, https://doi.org/10.5194/acp-20-1839-2020, https://doi.org/10.5194/acp-20-1839-2020, 2020
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An episode of anomalously low ozone concentrations in the stratosphere over northern Europe occurred on 3–5 November 2018. The 30 % reduction of the ozone layer was predicted by the global chemistry-transport model of the Finnish Meteorological Institute driven by weather forecasts of ECMWF. The reduction was subsequently observed by ozone monitoring satellites. The episode was caused by a storm in the northern Atlantic, which uplifted air from the troposphere to stratosphere.
Martin Dameris, Patrick Jöckel, and Matthias Nützel
Atmos. Chem. Phys., 19, 13759–13771, https://doi.org/10.5194/acp-19-13759-2019, https://doi.org/10.5194/acp-19-13759-2019, 2019
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A chemistry–climate model (CCM) study is performed, investigating the consequences of a constant CFC-11 surface mixing ratio for stratospheric ozone in the future. The total column ozone is particularly affected in both polar regions in winter and spring. It turns out that the calculated ozone changes, especially in the upper stratosphere, are smaller than expected. In this attitudinal region the additional ozone depletion due to the catalysis by reactive chlorine is partly compensated for.
Quentin Errera, Simon Chabrillat, Yves Christophe, Jonas Debosscher, Daan Hubert, William Lahoz, Michelle L. Santee, Masato Shiotani, Sergey Skachko, Thomas von Clarmann, and Kaley Walker
Atmos. Chem. Phys., 19, 13647–13679, https://doi.org/10.5194/acp-19-13647-2019, https://doi.org/10.5194/acp-19-13647-2019, 2019
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BRAM2 is a 13-year reanalysis of the chemical composition from the upper troposphere to the lower mesosphere based on the assimilation of the Microwave Limb Sounder observations where eight species are assimilated: O3, H2O, N2O, HNO3, HCl, ClO, CH3Cl and CO. BRAM2 agrees generally well with independent observations in the middle stratosphere, the polar vortex and the upper troposphere–lower stratosphere but also shows several issues in the model and in the observations.
Ewa M. Bednarz, Amanda C. Maycock, Peter Braesicke, Paul J. Telford, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 9833–9846, https://doi.org/10.5194/acp-19-9833-2019, https://doi.org/10.5194/acp-19-9833-2019, 2019
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The atmospheric response to the amplitude of 11-year solar cycle in UM-UKCA is separated into the contributions from changes in direct radiative heating and photolysis rates, and the results compared with a control case with both effects included. We find that while the tropical responses are largely additive, this is not necessarily the case in the high latitudes. We suggest that solar-induced changes in ozone are important for modulating the SH dynamical response to the 11-year solar cycle.
Pavle Arsenovic, Alessandro Damiani, Eugene Rozanov, Bernd Funke, Andrea Stenke, and Thomas Peter
Atmos. Chem. Phys., 19, 9485–9494, https://doi.org/10.5194/acp-19-9485-2019, https://doi.org/10.5194/acp-19-9485-2019, 2019
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Low-energy electrons (LEE) are the dominant source of odd nitrogen, which destroys ozone, in the mesosphere and stratosphere in polar winter in the geomagnetically active periods. However, the observed stratospheric ozone anomalies can be reproduced only when accounting for both low- and middle-range energy electrons (MEE) in the chemistry-climate model. Ozone changes may induce further dynamical and thermal changes in the atmosphere. We recommend including both LEE and MEE in climate models.
Franziska Winterstein, Fabian Tanalski, Patrick Jöckel, Martin Dameris, and Michael Ponater
Atmos. Chem. Phys., 19, 7151–7163, https://doi.org/10.5194/acp-19-7151-2019, https://doi.org/10.5194/acp-19-7151-2019, 2019
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The atmospheric concentrations of the anthropogenic greenhouse gas methane are predicted to rise in the future. In this paper we investigate how very strong methane concentrations will impact the atmosphere. We analyse two experiments, one with doubled and one with quintupled methane concentrations and focus on the rapid atmospheric changes before the ocean adjusts to the induced
forcing. In particular these are changes in temperature, ozone, the hydroxyl radical and stratospheric water vapour.
Mengchu Tao, Paul Konopka, Felix Ploeger, Xiaolu Yan, Jonathon S. Wright, Mohamadou Diallo, Stephan Fueglistaler, and Martin Riese
Atmos. Chem. Phys., 19, 6509–6534, https://doi.org/10.5194/acp-19-6509-2019, https://doi.org/10.5194/acp-19-6509-2019, 2019
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This paper examines the annual and interannual variations as well as long-term trend of modeled stratospheric water vapor with a Lagrangian chemical transport model driven by ERA-I, MERRA-2 and JRA-55. We find reasonable consistency among the annual cycle, QBO and the variabilities induced by ENSO and volcanic aerosols. The main discrepancies are linked to the differences in reanalysis upwelling rates in the lower stratosphere. The trends are sensitive to the reanalyses that drives the model.
Felix Ploeger, Bernard Legras, Edward Charlesworth, Xiaolu Yan, Mohamadou Diallo, Paul Konopka, Thomas Birner, Mengchu Tao, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 19, 6085–6105, https://doi.org/10.5194/acp-19-6085-2019, https://doi.org/10.5194/acp-19-6085-2019, 2019
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We analyse the change in the circulation of the middle atmosphere based on current generation meteorological reanalysis data sets. We find that long-term changes from 1989 to 2015 are similar for the chosen reanalyses, mainly resembling the forced response in climate model simulations to climate change. For shorter periods circulation changes are less robust, and the representation of decadal variability appears to be a major uncertainty for modelling the circulation of the middle atmosphere.
Lucien Froidevaux, Douglas E. Kinnison, Ray Wang, John Anderson, and Ryan A. Fuller
Atmos. Chem. Phys., 19, 4783–4821, https://doi.org/10.5194/acp-19-4783-2019, https://doi.org/10.5194/acp-19-4783-2019, 2019
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This work evaluates two versions of a 3-D global model of upper-atmospheric composition for recent decades. The two versions differ mainly in their dynamical (wind) constraints. Model–data differences, variability, and trends in five gases (ozone, H2O, HCl, HNO3, and N2O) are compared. While the match between models and observations is impressive, a few areas of discrepancy are noted. This work also updates trends in composition based on recent satellite-based measurements (through 2018).
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.
James Keeble, Hannah Brown, N. Luke Abraham, Neil R. P. Harris, and John A. Pyle
Atmos. Chem. Phys., 18, 7625–7637, https://doi.org/10.5194/acp-18-7625-2018, https://doi.org/10.5194/acp-18-7625-2018, 2018
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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.
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.
Cited articles
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Archibald, A. T., O'Connor, F. M., Abraham, N. L., Archer-Nicholls, S., Chipperfield, M. P., Dalvi, M., Folberth, G. A., Dennison, F., Dhomse, S. S., Griffiths, P. T., Hardacre, C., Hewitt, A. J., Hill, R. S., Johnson, C. E., Keeble, J., Köhler, M. O., Morgenstern, O., Mulcahy, J. P., Ordóñez, C., Pope, R. J., Rumbold, S. T., Russo, M. R., Savage, N. H., Sellar, A., Stringer, M., Turnock, S. T., Wild, O., and Zeng, G.: Description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in UKESM1, Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, 2020.
Ball, W. T., Alsing, J., Mortlock, D. J., Staehelin, J., Haigh, J. D., Peter, T., Tummon, F., Stübi, R., Stenke, A., Anderson, J., Bourassa, A., Davis, S. M., Degenstein, D., Frith, S., Froidevaux, L., Roth, C., Sofieva, V., Wang, R., Wild, J., Yu, P., Ziemke, J. R., and Rozanov, E. V.: Evidence for a continuous decline in lower stratospheric ozone offsetting ozone layer recovery, Atmos. Chem. Phys., 18, 1379–1394, https://doi.org/10.5194/acp-18-1379-2018, 2018.
Ball, W. T., Alsing, J., Staehelin, J., Davis, S. M., Froidevaux, L., and Peter, T.: Stratospheric ozone trends for 1985–2018: sensitivity to recent large variability, Atmos. Chem. Phys., 19, 12731–12748, https://doi.org/10.5194/acp-19-12731-2019, 2019.
Ball, W. T., Chiodo, G., Abalos, M., Alsing, J., and Stenke, A.: Inconsistencies between chemistry–climate models and observed lower stratospheric ozone trends since 1998, Atmos. Chem. Phys., 20, 9737–9752, https://doi.org/10.5194/acp-20-9737-2020, 2020.
Barrera, J. A., Fernandez, R. P., Iglesias-Suarez, F., Cuevas, C. A., Lamarque, J.-F., and Saiz-Lopez, A.: Seasonal impact of biogenic very short-lived bromocarbons on lowermost stratospheric ozone between 60∘ N and 60∘ S during the 21st century, Atmos. Chem. Phys., 20, 8083–8102, https://doi.org/10.5194/acp-20-8083-2020, 2020.
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Bednarz, E. M., Hossaini, R., Chipperfield, M. P., Abraham, N. L., and Braesicke, P.: Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 1: Stratospheric chlorine budget and the role of transport, Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, 2022.
Bednarz, E. M., Hossaini, R., Abraham, N. L., and Chipperfield, M. P.: Description and evaluation of the new UM–UKCA (vn11.0) Double Extended Stratospheric–Tropospheric (DEST vn1.0) scheme for comprehensive modelling of halogen chemistry in the stratosphere, Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, 2023.
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Claxton, T., Hossaini, R., Wild, O., Chipperfield, M. P., and Wilson, C.: On the regional and seasonal ozone depletion potential of chlorinated very short-lived substances, Geophys. Res. Lett., 46, 5489–5498, https://doi.org/10.1029/2018GL081455, 2019.
Claxton, T., Hossaini, R., Wilson, C., Montzka, S. A., Chipperfield, M. P., Wild, O., Bednarz, E. M., Carpenter, L. J., Andrews, S. J., Hackenberg, S. C., Mühle, J., Oram, D., Park, S., Park, M.-K., Atlas, E., Navarro, M., Schauffler, S., Sherry, D., Vollmer, M., Schuck, T., Engel, A., Krummel, P. B., Maione, M., Arduini, J., Saito, T., Yokouchi, Y., O'Doherty, S., Young, D., and Lunder, C.: A synthesis inversion to constrain global emissions of two very short lived chlorocarbons: dichloromethane, and perchloroethylene, J. Geophys. Res.-Atmos., 125, e2019JD031818, https://doi.org/10.1029/2019JD031818, 2020.
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Short summary
We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
We quantify, for the first time, the time-varying impact of uncontrolled emissions of...
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