Articles | Volume 22, issue 3
https://doi.org/10.5194/acp-22-2079-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-2079-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
15 Feb 2022
Research article |
| 15 Feb 2022
| 15 Feb 2022
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
Department of Earth System Science, University of California Irvine, Irvine, CA 92697-3100, USA
Michael J. Prather
Department of Earth System Science, University of California Irvine, Irvine, CA 92697-3100, USA
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Qi Tang, Michael J. Prather, Juno Hsu, Daniel J. Ruiz, Philip J. Cameron-Smith, Shaocheng Xie, and Jean-Christophe Golaz
Geosci. Model Dev., 14, 1219–1236, https://doi.org/10.5194/gmd-14-1219-2021, https://doi.org/10.5194/gmd-14-1219-2021, 2021
Calum P. Wilson and Michael J. Prather
Atmos. Meas. Tech., 18, 1757–1769, https://doi.org/10.5194/amt-18-1757-2025, https://doi.org/10.5194/amt-18-1757-2025, 2025
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We evaluated how well we can infer air pollutant levels (ozone, carbon monoxide, and nitrogen oxides) between air quality stations throughout South Korea, finding good representation in most densely measured cities in spite of intense small-scale emission hotspots. Comparing observed air quality with gridded model output is desirable, and so we created gridded datasets over South Korea using air quality station measurements, which agreed with airborne measurements around Seoul.
Maryam Ramezani Ziarani, Miriam Sinnhuber, Thomas Reddmann, Bernd Funke, Stefan Bender, and Michael Prather
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-227, https://doi.org/10.5194/gmd-2024-227, 2025
Preprint under review for GMD
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Our study aims to present a new method for incorporating top-down solar forcing into stratospheric ozone relying on linearized ozone scheme. The addition of geomagnetic forcing led to significant ozone losses in the polar upper stratosphere of both hemispheres due to the catalytic cycles involving NOy. In addition to the particle precipitation effect, accounting for solar UV variability in the ICON-ART model leads to the changes in ozone in the tropical stratosphere.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael J. Prather, Alexander T. Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Christopher J. Smith, Steven T. Turnock, Duncan Watson-Parris, and Paul J. Young
EGUsphere, https://doi.org/10.5194/egusphere-2024-2528, https://doi.org/10.5194/egusphere-2024-2528, 2024
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The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. In this paper, we review its contribution to AR6, and the wider understanding of the role of these species in climate and climate change. We identify remaining challenges concluding with recommendations aimed to improve the utility and uptake of climate model data to address the role of short-lived climate forcers in the Earth system.
Jinbo Xie, Qi Tang, Michael Prather, Jadwiga Richter, and Shixuan Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1927, https://doi.org/10.5194/egusphere-2024-1927, 2024
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Analysis of the interaction between the climate and ozone in the stratosphere is complicated by the in-ability climate model in simulating the Quasi-Biennial Oscillation (QBO) – an important climate mode in the stratosphere. We use a set of model simulation that realistically simulate QBO and a novel ozone diagnostic tool to separate the temperature and circulation-driven QBO impact. These are important for diagnosing model-model differences in the QBO-ozone responses for climate projections.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
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Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
Hsiang-He Lee, Qi Tang, and Michael Prather
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-203, https://doi.org/10.5194/gmd-2023-203, 2024
Revised manuscript not accepted
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The E3SM Chemistry diagnostics package (ChemDyg) is a software tool, which is designed for the global climate model (E3SM) chemistry development. ChemDyg generates several diagnostic plots and tables for model-to-model and model-to-observation comparison, including 2-dimentional contour mapping plots, diurnal and annual cycle, time-series plots, and comprehensive processing tables. This paper is to introduce the details of each diagnostics set and its required input data formats in ChemDyg.
Michael J. Prather, Hao Guo, and Xin Zhu
Earth Syst. Sci. Data, 15, 3299–3349, https://doi.org/10.5194/essd-15-3299-2023, https://doi.org/10.5194/essd-15-3299-2023, 2023
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The Atmospheric Tomography Mission (ATom) measured the chemical composition in air parcels from 0–12 km altitude on 2 km horizontal by 80 m vertical scales for four seasons, resolving most scales of chemical heterogeneity. ATom is one of the first missions designed to calculate the chemical evolution of each parcel, providing semi-global diurnal budgets for ozone and methane. Observations covered the remote troposphere: Pacific and Atlantic Ocean basins, Southern Ocean, Arctic basin, Antarctica.
Michael J. Prather, Lucien Froidevaux, and Nathaniel J. Livesey
Atmos. Chem. Phys., 23, 843–849, https://doi.org/10.5194/acp-23-843-2023, https://doi.org/10.5194/acp-23-843-2023, 2023
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From satellite data for nitrous oxide (N2O), ozone and temperature, we calculate the monthly loss of N2O and find it is increasing faster than expected, resulting in a shorter lifetime, which reduces the impact of anthropogenic emissions. We identify the cause as enhanced vertical lofting of high-N2O air into the tropical middle stratosphere, where it is destroyed photochemically. Because global warming is due in part to N2O, this finding presents a new negative climate-chemistry feedback.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Michael J. Prather
Earth Syst. Dynam., 13, 703–709, https://doi.org/10.5194/esd-13-703-2022, https://doi.org/10.5194/esd-13-703-2022, 2022
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Atmospheric CO2 fluctuations point to changes in fossil fuel emissions plus natural and perturbed variations in the natural carbon cycle. One unstudied source of variability is the stratosphere, where the influx of aged CO2-depleted air can cause surface fluctuations. Using modeling and, separately, scaling the observed N2O variability, I find that stratosphere-driven surface variability in CO2 is not a significant uncertainty (at most 10 % of the observed interannual variability).
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Qi Tang, Michael J. Prather, Juno Hsu, Daniel J. Ruiz, Philip J. Cameron-Smith, Shaocheng Xie, and Jean-Christophe Golaz
Geosci. Model Dev., 14, 1219–1236, https://doi.org/10.5194/gmd-14-1219-2021, https://doi.org/10.5194/gmd-14-1219-2021, 2021
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Sarah A. Strode, Junhua Liu, Leslie Lait, Róisín Commane, Bruce Daube, Steven Wofsy, Austin Conaty, Paul Newman, and Michael Prather
Atmos. Chem. Phys., 18, 10955–10971, https://doi.org/10.5194/acp-18-10955-2018, https://doi.org/10.5194/acp-18-10955-2018, 2018
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The GEOS-5 atmospheric model provided forecasts for the Atmospheric Tomography Mission (ATom). GEOS-5 shows skill in simulating the carbon monoxide (CO) measured in ATom-1. African fires contribute to high CO over the tropical Atlantic, but non-fire sources are the main contributors elsewhere. ATom aims to provide a chemical climatology, so we consider whether ATom-1 occurred during a typical summer month. Satellite observations suggest ATom-1 occurred in a clean but not exceptional month.
Michael J. Prather, Clare M. Flynn, Xin Zhu, Stephen D. Steenrod, Sarah A. Strode, Arlene M. Fiore, Gustavo Correa, Lee T. Murray, and Jean-Francois Lamarque
Atmos. Meas. Tech., 11, 2653–2668, https://doi.org/10.5194/amt-11-2653-2018, https://doi.org/10.5194/amt-11-2653-2018, 2018
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A new protocol for merging in situ atmospheric chemistry measurements with 3-D models is developed. This technique can identify the most reactive air parcels in terms of tropospheric production/loss of O3 & CH4. This approach highlights differences in 6 global chemistry models even with composition specified. Thus in situ measurements from, e.g., NASA's ATom mission can be used to develop a chemical climatology of, not only the key species, but also the rates of key reactions in each air parcel.
Ruth M. Doherty, Clara Orbe, Guang Zeng, David A. Plummer, Michael J. Prather, Oliver Wild, Meiyun Lin, Drew T. Shindell, and Ian A. Mackenzie
Atmos. Chem. Phys., 17, 14219–14237, https://doi.org/10.5194/acp-17-14219-2017, https://doi.org/10.5194/acp-17-14219-2017, 2017
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We investigate how climate change impacts global air pollution transport. To study transport changes, we use a carbon monoxide (CO) tracer species emitted from global sources. We find robust and consistent changes in CO-tracer distributions in climate change simulations performed by four chemistry–climate models in different seasons. We highlight the importance of the co-location of emission source regions and controlling transport processes in determining future pollution transport.
Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
Atmos. Chem. Phys., 17, 9081–9102, https://doi.org/10.5194/acp-17-9081-2017, https://doi.org/10.5194/acp-17-9081-2017, 2017
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We present a new approach for comparing atmospheric chemistry models with measurements based on what these models are used to do, i.e., calculate changes in ozone and methane, prime greenhouse gases. This method anticipates a new type of measurements from the NASA Atmospheric Tomography (ATom) mission. In comparing the mixture of species within air parcels, we focus on those responsible for key chemical changes and weight these parcels by their chemical reactivity.
James Hansen, Makiko Sato, Pushker Kharecha, Karina von Schuckmann, David J. Beerling, Junji Cao, Shaun Marcott, Valerie Masson-Delmotte, Michael J. Prather, Eelco J. Rohling, Jeremy Shakun, Pete Smith, Andrew Lacis, Gary Russell, and Reto Ruedy
Earth Syst. Dynam., 8, 577–616, https://doi.org/10.5194/esd-8-577-2017, https://doi.org/10.5194/esd-8-577-2017, 2017
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Global temperature now exceeds +1.25 °C relative to 1880–1920, similar to warmth of the Eemian period. Keeping warming less than 1.5 °C or CO2 below 350 ppm now requires extraction of CO2 from the air. If rapid phaseout of fossil fuel emissions begins soon, most extraction can be via improved agricultural and forestry practices. In contrast, continued high emissions places a burden on young people of massive technological CO2 extraction with large risks, high costs and uncertain feasibility.
Juno Hsu, Michael J. Prather, Philip Cameron-Smith, Alex Veidenbaum, and Alex Nicolau
Geosci. Model Dev., 10, 2525–2545, https://doi.org/10.5194/gmd-10-2525-2017, https://doi.org/10.5194/gmd-10-2525-2017, 2017
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Solar-J is a high-fidelity solar radiative transfer Fortran 90 code. It has been developed for consistently calculating both the photolysis rates of important chemical species and the heating rates of the atmosphere and the Earth's surface. Its spectral range spans from 177 nm to 12 microns. It can be easily dropped in as a module in global climate–chemistry models.
Gunnar Myhre, Wenche Aas, Ribu Cherian, William Collins, Greg Faluvegi, Mark Flanner, Piers Forster, Øivind Hodnebrog, Zbigniew Klimont, Marianne T. Lund, Johannes Mülmenstädt, Cathrine Lund Myhre, Dirk Olivié, Michael Prather, Johannes Quaas, Bjørn H. Samset, Jordan L. Schnell, Michael Schulz, Drew Shindell, Ragnhild B. Skeie, Toshihiko Takemura, and Svetlana Tsyro
Atmos. Chem. Phys., 17, 2709–2720, https://doi.org/10.5194/acp-17-2709-2017, https://doi.org/10.5194/acp-17-2709-2017, 2017
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Over the past decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990–2015, as simulated by seven global atmospheric composition models. The global mean radiative forcing is more strongly positive than reported in IPCC AR5.
William J. Collins, Jean-François Lamarque, Michael Schulz, Olivier Boucher, Veronika Eyring, Michaela I. Hegglin, Amanda Maycock, Gunnar Myhre, Michael Prather, Drew Shindell, and Steven J. Smith
Geosci. Model Dev., 10, 585–607, https://doi.org/10.5194/gmd-10-585-2017, https://doi.org/10.5194/gmd-10-585-2017, 2017
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We have designed a set of climate model experiments called the Aerosol Chemistry Model Intercomparison Project (AerChemMIP). These are designed to quantify the climate and air quality impacts of aerosols and chemically reactive gases in the climate models that are used to simulate past and future climate. We hope that many climate modelling centres will choose to run these experiments to help understand the contribution of aerosols and chemistry to climate change.
Bojan Sič, Laaziz El Amraoui, Andrea Piacentini, Virginie Marécal, Emanuele Emili, Daniel Cariolle, Michael Prather, and Jean-Luc Attié
Atmos. Meas. Tech., 9, 5535–5554, https://doi.org/10.5194/amt-9-5535-2016, https://doi.org/10.5194/amt-9-5535-2016, 2016
J. L. Schnell, M. J. Prather, B. Josse, V. Naik, L. W. Horowitz, P. Cameron-Smith, D. Bergmann, G. Zeng, D. A. Plummer, K. Sudo, T. Nagashima, D. T. Shindell, G. Faluvegi, and S. A. Strode
Atmos. Chem. Phys., 15, 10581–10596, https://doi.org/10.5194/acp-15-10581-2015, https://doi.org/10.5194/acp-15-10581-2015, 2015
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We test global chemistry--climate models in their ability to simulate present-day surface ozone. Models are tested against observed hourly ozone from 4217 stations in North America and Europe that are averaged over 1°x1° grid cells. Using novel metrics, we find most models match the shape but not the amplitude of regional summertime diurnal and annual cycles and match the pattern but not the magnitude of summer ozone enhancement. Most also match the observed distribution of extreme episode sizes
M. J. Prather
Geosci. Model Dev., 8, 2587–2595, https://doi.org/10.5194/gmd-8-2587-2015, https://doi.org/10.5194/gmd-8-2587-2015, 2015
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A new approach for modeling photolysis rates (J values) in atmospheres with fractional cloud cover has been developed and is implemented as Cloud-J – a multi-scattering eight-stream radiative transfer model for solar radiation based on Fast-J. Using observations of the vertical correlation of cloud layers, Cloud-J provides a practical and accurate method for modeling atmospheric chemistry, which can be extended to solar heating rates.
J. L. Schnell, C. D. Holmes, A. Jangam, and M. J. Prather
Atmos. Chem. Phys., 14, 7721–7739, https://doi.org/10.5194/acp-14-7721-2014, https://doi.org/10.5194/acp-14-7721-2014, 2014
C. D. Holmes, M. J. Prather, and G. C. M. Vinken
Atmos. Chem. Phys., 14, 6801–6812, https://doi.org/10.5194/acp-14-6801-2014, https://doi.org/10.5194/acp-14-6801-2014, 2014
P. H. Lauritzen, P. A. Ullrich, C. Jablonowski, P. A. Bosler, D. Calhoun, A. J. Conley, T. Enomoto, L. Dong, S. Dubey, O. Guba, A. B. Hansen, E. Kaas, J. Kent, J.-F. Lamarque, M. J. Prather, D. Reinert, V. V. Shashkin, W. C. Skamarock, B. Sørensen, M. A. Taylor, and M. A. Tolstykh
Geosci. Model Dev., 7, 105–145, https://doi.org/10.5194/gmd-7-105-2014, https://doi.org/10.5194/gmd-7-105-2014, 2014
V. Naik, A. Voulgarakis, A. M. Fiore, L. W. Horowitz, J.-F. Lamarque, M. Lin, M. J. Prather, P. J. Young, D. Bergmann, P. J. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, T. P. C. van Noije, D. A. Plummer, M. Righi, S. T. Rumbold, R. Skeie, D. T. Shindell, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, https://doi.org/10.5194/acp-13-5277-2013, 2013
A. Voulgarakis, V. Naik, J.-F. Lamarque, D. T. Shindell, P. J. Young, M. J. Prather, O. Wild, R. D. Field, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, L. W. Horowitz, B. Josse, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, D. S. Stevenson, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2563–2587, https://doi.org/10.5194/acp-13-2563-2013, https://doi.org/10.5194/acp-13-2563-2013, 2013
C. D. Holmes, M. J. Prather, O. A. Søvde, and G. Myhre
Atmos. Chem. Phys., 13, 285–302, https://doi.org/10.5194/acp-13-285-2013, https://doi.org/10.5194/acp-13-285-2013, 2013
Ø. Hodnebrog, T. K. Berntsen, O. Dessens, M. Gauss, V. Grewe, I. S. A. Isaksen, B. Koffi, G. Myhre, D. Olivié, M. J. Prather, F. Stordal, S. Szopa, Q. Tang, P. van Velthoven, and J. E. Williams
Atmos. Chem. Phys., 12, 12211–12225, https://doi.org/10.5194/acp-12-12211-2012, https://doi.org/10.5194/acp-12-12211-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)
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Aaron Match, Edwin P. Gerber, and Stephan Fueglistaler
Atmos. Chem. Phys., 25, 4349–4366, https://doi.org/10.5194/acp-25-4349-2025, https://doi.org/10.5194/acp-25-4349-2025, 2025
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The ozone concentration in the tropical stratosphere peaks at 26 km, protecting life from harmful ultraviolet light without poisoning it. Climate models reproduce this peak, but textbook explanations yield errors of 10 km. Simplifying the well-understood sources and sinks of ozone, we develop a theory explaining that tropical ozone peaks where its dominant sink transitions from damping of atomic oxygen aloft (mainly via catalytic chemistry) to damping of ozone below (mainly via transport).
Irina Petropavlovskikh, Jeannette D. Wild, Kari Abromitis, Peter Effertz, Koji Miyagawa, Lawrence E. Flynn, Eliane Maillard Barras, Robert Damadeo, Glen McConville, Bryan Johnson, Patrick Cullis, Sophie Godin-Beekmann, Gerard Ancellet, Richard Querel, Roeland Van Malderen, and Daniel Zawada
Atmos. Chem. Phys., 25, 2895–2936, https://doi.org/10.5194/acp-25-2895-2025, https://doi.org/10.5194/acp-25-2895-2025, 2025
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Observational records show that stratospheric ozone is recovering in accordance with the implementation of the Montreal Protocol and its amendments. Natural ozone variability complicates the detection of small trends. This study optimizes a statistical model fit in ground-station-based observational records by adding parameters that interpret seasonal and long-term changes in atmospheric circulation and airmass mixing, which reduces uncertainties in detecting the stratospheric ozone recovery.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn P. Chipperfield, Wuhu Feng, David E. Oram, Karina E. Adcock, Stephen A. Montzka, Isobel J. Simpson, Andrea Mazzeo, Amber A. Leeson, Elliot Atlas, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 13457–13475, https://doi.org/10.5194/acp-24-13457-2024, https://doi.org/10.5194/acp-24-13457-2024, 2024
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DCE (1,2-dichloroethane) is an industrial chemical used to produce PVC (polyvinyl chloride). We analysed DCE production data to estimate global DCE emissions (2002–2020). The emissions were included in an atmospheric model and evaluated by comparing simulated DCE to DCE measurements in the troposphere. We show that DCE contributes ozone-depleting Cl to the stratosphere and that this has increased with increasing DCE emissions. DCE’s impact on stratospheric O3 is currently small but non-zero.
Megan J. Lickley, John S. Daniel, Laura A. McBride, Ross J. Salawitch, and Guus J. M. Velders
Atmos. Chem. Phys., 24, 13081–13099, https://doi.org/10.5194/acp-24-13081-2024, https://doi.org/10.5194/acp-24-13081-2024, 2024
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The expected ozone recovery date was delayed by 17 years between the 2006 and 2022 international scientific assessments of ozone depletion. We quantify the primary drivers of this delay. Changes in the metric used to estimate ozone recovery explain ca. 5 years of this delay. Of the remaining 12 years, changes in estimated banks, atmospheric lifetimes, and emission projections explain 4, 3.5, and 3 years of this delay, respectively.
Yiran Zhang-Liu, Rolf Müller, Jens-Uwe Grooß, Sabine Robrecht, Bärbel Vogel, Abdul Mannan Zafar, and Ralph Lehmann
Atmos. Chem. Phys., 24, 12557–12574, https://doi.org/10.5194/acp-24-12557-2024, https://doi.org/10.5194/acp-24-12557-2024, 2024
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HCl null cycles in Antarctica are important for maintaining high values of ozone-destroying chlorine in Antarctic spring. These HCl null cycles are not affected by (1) using the most recent recommendations of chemical kinetics (compared to older recommendations), (2) accounting for dehydration in the Antarctic winter vortex, and (3) considering the observed (but unexplained) depletion of HCl in mid-winter in the Antarctic vortex throughout Antarctic winter.
Aaron Match, Edwin P. Gerber, and Stephan Fueglistaler
Atmos. Chem. Phys., 24, 10305–10322, https://doi.org/10.5194/acp-24-10305-2024, https://doi.org/10.5194/acp-24-10305-2024, 2024
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Earth's ozone layer absorbs incoming UV light, protecting life. Removing ozone aloft allows UV light to penetrate deeper, where it is known to produce new ozone, leading to "self-healing" that partially stabilizes total ozone. However, a photochemistry model shows that, above 40 km in the tropics, deeper-penetrating UV destroys ozone, destabilizing the total ozone. Photochemical theory reveals that this destabilizing regime occurs where overhead ozone is below a key threshold.
Pinchas Nürnberg, Sarah A. Strode, and Ralf Sussmann
Atmos. Chem. Phys., 24, 10001–10012, https://doi.org/10.5194/acp-24-10001-2024, https://doi.org/10.5194/acp-24-10001-2024, 2024
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We created a set of scaling factors describing the diurnal increase in stratospheric nitrogen oxides above Zugspitze, Germany. We used these factors to validate recently published model simulation data. On the one hand, this validation enables the use of the validated data to better understand the stratospheric photochemistry. On the other hand, it can improve satellite validation, which has implications for the understanding of urban smog events and other pollution events in the troposphere.
Henk Eskes, Athanasios Tsikerdekis, Melanie Ades, Mihai Alexe, Anna Carlin Benedictow, Yasmine Bennouna, Lewis Blake, Idir Bouarar, Simon Chabrillat, Richard Engelen, Quentin Errera, Johannes Flemming, Sebastien Garrigues, Jan Griesfeller, Vincent Huijnen, Luka Ilić, Antje Inness, John Kapsomenakis, Zak Kipling, Bavo Langerock, Augustin Mortier, Mark Parrington, Isabelle Pison, Mikko Pitkänen, Samuel Remy, Andreas Richter, Anja Schoenhardt, Michael Schulz, Valerie Thouret, Thorsten Warneke, Christos Zerefos, and Vincent-Henri Peuch
Atmos. Chem. Phys., 24, 9475–9514, https://doi.org/10.5194/acp-24-9475-2024, https://doi.org/10.5194/acp-24-9475-2024, 2024
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The Copernicus Atmosphere Monitoring Service (CAMS) provides global analyses and forecasts of aerosols and trace gases in the atmosphere. On 27 June 2023 a major upgrade, Cy48R1, became operational. Comparisons with in situ, surface remote sensing, aircraft, and balloon and satellite observations show that the new CAMS system is a significant improvement. The results quantify the skill of CAMS to forecast impactful events, such as wildfires, dust storms and air pollution peaks.
Guang Zeng, Richard Querel, Hisako Shiona, Deniz Poyraz, Roeland Van Malderen, Alex Geddes, Penny Smale, Dan Smale, John Robinson, and Olaf Morgenstern
Atmos. Chem. Phys., 24, 6413–6432, https://doi.org/10.5194/acp-24-6413-2024, https://doi.org/10.5194/acp-24-6413-2024, 2024
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We present a homogenised ozonesonde record (1987–2020) for Lauder, a Southern Hemisphere mid-latitude site; identify factors driving ozone trends; and attribute them to anthropogenic forcings using statistical analysis and model simulations. We find that significant negative lower-stratospheric ozone trends identified at Lauder are associated with an increase in tropopause height and that CO2-driven dynamical changes have played an increasingly important role in driving ozone trends.
Hella Garny, Roland Eichinger, Johannes C. Laube, Eric A. Ray, Gabriele P. Stiller, Harald Bönisch, Laura Saunders, and Marianna Linz
Atmos. Chem. Phys., 24, 4193–4215, https://doi.org/10.5194/acp-24-4193-2024, https://doi.org/10.5194/acp-24-4193-2024, 2024
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Transport circulation in the stratosphere is important for the distribution of tracers, but its strength is hard to measure. Mean transport times can be inferred from observations of trace gases with certain properties, such as sulfur hexafluoride (SF6). However, this gas has a chemical sink in the high atmosphere, which can lead to substantial biases in inferred transport times. In this paper we present a method to correct mean transport times derived from SF6 for the effects of chemical sinks.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Ernst-Peter Röth and Luc Vereecken
Atmos. Chem. Phys., 24, 2625–2638, https://doi.org/10.5194/acp-24-2625-2024, https://doi.org/10.5194/acp-24-2625-2024, 2024
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The paper presents the radical and molecular product quantum yields in the photolysis reaction of CHDO at wavelengths above 300 nm. Two different approaches based on literature data are used, with results falling within both approaches' uncertainty ranges. Simple functional forms are presented for use in photochemical models of the atmosphere.
Johannes Pletzer and Volker Grewe
Atmos. Chem. Phys., 24, 1743–1775, https://doi.org/10.5194/acp-24-1743-2024, https://doi.org/10.5194/acp-24-1743-2024, 2024
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Very fast aircraft can travel at 30–40 km altitude and are designed to use liquid hydrogen as fuel instead of kerosene. Depending on their flight altitude, the impact of these aircraft on the atmosphere and climate can change very much. Our results show that a variation inflight latitude can have a considerably higher change in impact compared to a variation in flight altitude. Atmospheric air transport and polar stratospheric clouds play an important role in hypersonic aircraft emissions.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Kimberlee Dubé, Susann Tegtmeier, Adam Bourassa, Daniel Zawada, Douglas Degenstein, Patrick E. Sheese, Kaley A. Walker, and William Randel
Atmos. Chem. Phys., 23, 13283–13300, https://doi.org/10.5194/acp-23-13283-2023, https://doi.org/10.5194/acp-23-13283-2023, 2023
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This paper presents a technique for understanding the causes of long-term changes in stratospheric composition. By using N2O as a proxy for stratospheric circulation in the model used to calculated trends, it is possible to separate the effects of dynamics and chemistry on observed trace gas trends. We find that observed HCl increases are due to changes in the stratospheric circulation, as are O3 decreases above 30 hPa in the Northern Hemisphere.
Gabriel Chiodo, Marina Friedel, Svenja Seeber, Daniela Domeisen, Andrea Stenke, Timofei Sukhodolov, and Franziska Zilker
Atmos. Chem. Phys., 23, 10451–10472, https://doi.org/10.5194/acp-23-10451-2023, https://doi.org/10.5194/acp-23-10451-2023, 2023
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Stratospheric ozone protects the biosphere from harmful UV radiation. Anthropogenic activity has led to a reduction in the ozone layer in the recent past, but thanks to the implementation of the Montreal Protocol, the ozone layer is projected to recover. In this study, we show that projected future changes in Arctic ozone abundances during springtime will influence stratospheric climate and thereby actively modulate large-scale circulation changes in the Northern Hemisphere.
Marina Friedel, Gabriel Chiodo, Timofei Sukhodolov, James Keeble, Thomas Peter, Svenja Seeber, Andrea Stenke, Hideharu Akiyoshi, Eugene Rozanov, David Plummer, Patrick Jöckel, Guang Zeng, Olaf Morgenstern, and Béatrice Josse
Atmos. Chem. Phys., 23, 10235–10254, https://doi.org/10.5194/acp-23-10235-2023, https://doi.org/10.5194/acp-23-10235-2023, 2023
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Previously, it has been suggested that springtime Arctic ozone depletion might worsen in the coming decades due to climate change, which might counteract the effect of reduced ozone-depleting substances. Here, we show with different chemistry–climate models that springtime Arctic ozone depletion will likely decrease in the future. Further, we explain why models show a large spread in the projected development of Arctic ozone depletion and use the model spread to constrain future projections.
Thomas Reddmann, Miriam Sinnhuber, Jan Maik Wissing, Olesya Yakovchuk, and Ilya Usoskin
Atmos. Chem. Phys., 23, 6989–7000, https://doi.org/10.5194/acp-23-6989-2023, https://doi.org/10.5194/acp-23-6989-2023, 2023
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Recent analyses of isotopic records of ice cores and sediments have shown that very strong explosions may occur on the Sun, perhaps about one such explosion every 1000 years. Such explosions pose a real threat to humankind. It is therefore of great interest to study the impact of such explosions on Earth. We analyzed how the explosions would affect the chemistry of the middle atmosphere and show that the related ozone loss is not dramatic and that the atmosphere will recover within 1 year.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, and Thomas Peter
Atmos. Chem. Phys., 23, 4801–4817, https://doi.org/10.5194/acp-23-4801-2023, https://doi.org/10.5194/acp-23-4801-2023, 2023
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The future ozone evolution in SOCOLv4 simulations under SSP2-4.5 and SSP5-8.5 scenarios has been assessed for the period 2015–2099 and subperiods using the DLM approach. The SOCOLv4 projects a decline in tropospheric ozone in the 2030s in SSP2-4.5 and in the 2060s in SSP5-8.5. The stratospheric ozone increase is ~3 times higher in SSP5-8.5, confirming the important role of GHGs in ozone evolution. We also showed that tropospheric ozone strongly impacts the total column in the tropics.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Janusz Krzyścin
Atmos. Chem. Phys., 23, 3119–3132, https://doi.org/10.5194/acp-23-3119-2023, https://doi.org/10.5194/acp-23-3119-2023, 2023
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We propose indices to obtain the current stage of total column ozone (TCO3) recovery attributed to ozone-depleting substance (ODS) changes in the stratosphere. The indices are calculated using TCO3 values in key years of the ODS changes. The ozone recovery stage is derived for 16 sites in the NH mid-latitudes using results from ground and satellite measurements and reanalysis data. In Europe, there is a slow TCO3 recovery. A continuous TCO3 decline has been occurring in some sites since 1980.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, William Ball, and Thomas Peter
Atmos. Chem. Phys., 22, 15333–15350, https://doi.org/10.5194/acp-22-15333-2022, https://doi.org/10.5194/acp-22-15333-2022, 2022
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Applying the dynamic linear model, we confirm near-global ozone recovery (55°N–55°S) in the mesosphere, upper and middle stratosphere, and a steady increase in the troposphere. We also show that modern chemistry–climate models (CCMs) like SOCOLv4 may reproduce the observed trend distribution of lower stratospheric ozone, despite exhibiting a lower magnitude and statistical significance. The obtained ozone trend pattern in SOCOLv4 is generally consistent with observations and reanalysis datasets.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Ville Maliniemi, Pavle Arsenovic, Annika Seppälä, and Hilde Nesse Tyssøy
Atmos. Chem. Phys., 22, 8137–8149, https://doi.org/10.5194/acp-22-8137-2022, https://doi.org/10.5194/acp-22-8137-2022, 2022
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We simulate the effect of energetic particle precipitation (EPP) on Antarctic stratospheric ozone chemistry over the whole 20th century. We find a significant increase of reactive nitrogen due to EP, which can deplete ozone via a catalytic reaction. Furthermore, significant modulation of active chlorine is obtained related to EPP, which impacts ozone depletion by both active chlorine and EPP. Our results show that EPP has been a significant modulator of ozone chemistry during the CFC era.
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.
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Short summary
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.
The stratosphere is an important source of tropospheric ozone, which affects climate, chemistry,...
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