Articles | Volume 22, issue 3
15 Feb 2022
Research article | 15 Feb 2022
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
Daniel J. Ruiz and Michael J. Prather
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,
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. Discuss.,
Revised manuscript under review for ACPShort summary
We have prepared from the recent ATom aircraft mission a unique and unusual result: 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, Lucien Froidevaux, and Nathaniel J. Livesey
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
From the 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. The cause of the increasing loss is enhanced vertical lofting of high-N2O air in the tropical middle stratosphere, where it is destroyed photochemically. This presents a new, distinct, but minor, negative climate-chemistry feedback.
Michael J. Prather
Earth Syst. Dynam., 13, 703–709,Short summary
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,Short summary
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,
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,
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,Short summary
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,Short summary
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,
C. D. Holmes, M. J. Prather, and G. C. M. Vinken
Atmos. Chem. Phys., 14, 6801–6812,
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,
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,
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,
C. D. Holmes, M. J. Prather, O. A. Søvde, and G. Myhre
Atmos. Chem. Phys., 13, 285–302,
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,
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)Atmospheric impacts of chlorinated very short-lived substances over the recent past – Part 1: Stratospheric chlorine budget and the role of transportEffects of reanalysis forcing fields on ozone trends and age of air from a chemical transport modelThe historical ozone trends simulated with the SOCOLv4 and their comparison with observations and reanalysisThe influence of energetic particle precipitation on Antarctic stratospheric chlorine and ozone over the 20th centuryAn Arctic ozone hole in 2020 if not for the Montreal ProtocolEffects of enhanced downwelling of NOx on Antarctic upper-stratospheric ozone in the 21st centuryProcesses influencing lower stratospheric water vapour in monsoon anticyclones: insights from Lagrangian modellingEvaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100Slow feedbacks resulting from strongly enhanced atmospheric methane mixing ratios in a chemistry–climate model with mixed-layer oceanImpact of the eruption of Mt Pinatubo on the chemical composition of the stratosphereProjecting ozone hole recovery using an ensemble of chemistry–climate models weighted by model performance and independenceInconsistencies between chemistry–climate models and observed lower stratospheric ozone trends since 1998Reformulating the bromine alpha factor and equivalent effective stratospheric chlorine (EESC): evolution of ozone destruction rates of bromine and chlorine in future climate scenariosAnalysis and attribution of total column ozone changes over the Tibetan Plateau during 1979–2017Seasonal impact of biogenic very short-lived bromocarbons on lowermost stratospheric ozone between 60° N and 60° S during the 21st centuryModelling the potential impacts of the recent, unexpected increase in CFC-11 emissions on total column ozone recoveryThe potential impacts of a sulfur- and halogen-rich supereruption such as Los Chocoyos on the atmosphere and climateTechnical note: Intermittent reduction of the stratospheric ozone over northern Europe caused by a storm in the Atlantic OceanPossible implications of enhanced chlorofluorocarbon-11 concentrations on ozoneTechnical note: Reanalysis of Aura MLS chemical observationsSeparating the role of direct radiative heating and photolysis in modulating the atmospheric response to the amplitude of the 11-year solar cycle forcingReactive nitrogen (NOy) and ozone responses to energetic electron precipitation during Southern Hemisphere winterImplication of strongly increased atmospheric methane concentrations for chemistry–climate connectionsMultitimescale variations in modeled stratospheric water vapor derived from three modern reanalysis productsHow 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 recordsChlorine nitrate in the atmosphereLinking uncertainty in simulated Arctic ozone loss to uncertainties in modelled tropical stratospheric water vapourImportance of seasonally resolved oceanic emissions for bromoform delivery from the tropical Indian Ocean and west Pacific to the stratosphereThe representation of solar cycle signals in stratospheric ozone – Part 2: Analysis of global modelsInvestigating the yield of H2O and H2 from methane oxidation in the stratosphereComparison of ECHAM5/MESSy Atmospheric Chemistry (EMAC) simulations of the Arctic winter 2009/2010 and 2010/2011 with Envisat/MIPAS and Aura/MLS observationsOn the discrepancy of HCl processing in the core of the wintertime polar vorticesEstimates of ozone return dates from Chemistry-Climate Model Initiative simulationsTrend differences in lower stratospheric water vapour between Boulder and the zonal mean and their role in understanding fundamental observational discrepanciesOn ozone trend detection: using coupled chemistry–climate simulations to investigate early signs of total column ozone recoveryFuture changes in the stratosphere-to-troposphere ozone mass flux and the contribution from climate change and ozone recoveryThe maintenance of elevated active chlorine levels in the Antarctic lower stratosphere through HCl null cyclesChemical and climatic drivers of radiative forcing due to changes in stratospheric and tropospheric ozone over the 21st centuryOzone sensitivity to varying greenhouse gases and ozone-depleting substances in CCMI-1 simulationsDiagnosing the radiative and chemical contributions to future changes in tropical column ozone with the UM-UKCA chemistry–climate modelDenitrification, dehydration and ozone loss during the 2015/2016 Arctic winterAssessment of upper tropospheric and stratospheric water vapor and ozone in reanalyses as part of S-RIPA quantitative analysis of the reactions involved in stratospheric ozone depletion in the polar vortex coreAn assessment of ozone mini-hole representation in reanalyses over the Northern HemisphereImpact of biogenic very short-lived bromine on the Antarctic ozone hole during the 21st centuryInfluence of enhanced Asian NOx emissions on ozone in the upper troposphere and lower stratosphere in chemistry–climate model simulationsDetermination of the atmospheric lifetime and global warming potential of sulfur hexafluoride using a three-dimensional modelAntarctic ozone depletion between 1960 and 1980 in observations and chemistry–climate model simulationsSeasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676,Short summary
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,Short summary
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.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Jan Sedlacek, William Ball, and Thomas Peter
Applying DLM, we confirm near-global ozone recovery [55N–55S] in the mesosphere, upper and middle stratosphere, as well as a steady increase in tropospheric ozone. We also show that modern CCMs, such as SOCOLv4, still cannot properly reproduce the observed trends in extratropical low stratospheric ozone, exhibiting weak and non-significant trends. Nevertheless, the obtained pattern of ozone trends in SOCOLv4 is generally consistent with observations and reanalysis data sets.
Ville Maliniemi, Pavle Arsenovic, Annika Seppälä, and Hilde Nesse Tyssøy
Atmos. Chem. Phys., 22, 8137–8149,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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,Short summary
2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the stratospheric ozone layer from the harmful effects of synthetic ozone depleting substances. Since the late 1990s atmospheric concentrations of these species have begun to decline, and as a result ozone concentrations are expected to increase. In this study we use an ensemble of chemistry–climate simulations to investigate recent ozone trends and search for early signs of ozone recovery.
Stefanie Meul, Ulrike Langematz, Philipp Kröger, Sophie Oberländer-Hayn, and Patrick Jöckel
Atmos. Chem. Phys., 18, 7721–7738,Short summary
Using a chemistry--climate model future changes in the stratosphere-to-troposphere ozone mass flux, their drivers, and the future distribution of stratospheric ozone in the troposphere are investigated. In an extreme greenhouse gas (GHG) scenario, the global influx of stratospheric ozone into the troposphere is projected to grow between 2000 and 2100 by 53%. The increase is due to the recovery of stratospheric ozone owing to declining halogens and GHG induced circulation and temperature changes.
Rolf Müller, Jens-Uwe Grooß, Abdul Mannan Zafar, Sabine Robrecht, and Ralph Lehmann
Atmos. Chem. Phys., 18, 2985–2997,Short summary
This paper revisits the chemistry leading to strong ozone depletion in the Antarctic. We focus on the heart of the ozone layer in the lowermost stratosphere in the core of the vortex. We argue that chemical cycles (referred to as HCl null cycles) that have hitherto been largely neglected counteract the deactivation of chlorine and are therefore key to ozone depletion in the core of the Antarctic vortex. The key process to full activation of chlorine is the photolysis of formaldehyde.
Antara Banerjee, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 18, 2899–2911,Short summary
This study quantifies the radiative forcing (RF) of future ozone changes. Under climate change, even the sign of the ozone RF can change depending on the greenhouse gas emissions scenario followed. Stratosphere–troposphere exchange plays an important role in driving ozone RF due to reductions in ozone-depleting substances (ODSs) and increases in methane abundance. These could negate the ozone-derived climate benefits of air-quality controls on non-methane ozone precursor emissions.
Olaf Morgenstern, Kane A. Stone, Robyn Schofield, Hideharu Akiyoshi, Yousuke Yamashita, Douglas E. Kinnison, Rolando R. Garcia, Kengo Sudo, David A. Plummer, John Scinocca, Luke D. Oman, Michael E. Manyin, Guang Zeng, Eugene Rozanov, Andrea Stenke, Laura E. Revell, Giovanni Pitari, Eva Mancini, Glauco Di Genova, Daniele Visioni, Sandip S. Dhomse, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 1091–1114,Short summary
We assess how ozone as simulated by a group of chemistry–climate models responds to variations in man-made climate gases and ozone-depleting substances. We find some agreement, particularly in the middle and upper stratosphere, but also considerable disagreement elsewhere. Such disagreement affects the reliability of future ozone projections based on these models, and also constitutes a source of uncertainty in climate projections using prescribed ozone derived from these simulations.
James Keeble, Ewa M. Bednarz, Antara Banerjee, N. Luke Abraham, Neil R. P. Harris, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 17, 13801–13818,Short summary
In this study we explore the chemical and transport processes controlling ozone abundances in different altitude regions in the tropics for the present day and how these processes may change in the future in order to determine when total-column ozone values in the tropics will recover to pre-1980s values following the implementation of the Montreal Protocol and its subsequent amendments, which imposed bans on the use and emissions of CFCs.
Farahnaz Khosrawi, Oliver Kirner, Björn-Martin Sinnhuber, Sören Johansson, Michael Höpfner, Michelle L. Santee, Lucien Froidevaux, Jörn Ungermann, Roland Ruhnke, Wolfgang Woiwode, Hermann Oelhaf, and Peter Braesicke
Atmos. Chem. Phys., 17, 12893–12910,Short summary
The 2015/2016 Arctic winter was one of the coldest winters in recent years, allowing extensive PSC formation and chlorine activation. Model simulations of the 2015/2016 Arctic winter were performed with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). We find that ozone loss was quite strong but not as strong as in 2010/2011; denitrification and dehydration were so far the strongest observed in the Arctic stratosphere in at least the past 10 years.
Sean M. Davis, Michaela I. Hegglin, Masatomo Fujiwara, Rossana Dragani, Yayoi Harada, Chiaki Kobayashi, Craig Long, Gloria L. Manney, Eric R. Nash, Gerald L. Potter, Susann Tegtmeier, Tao Wang, Krzysztof Wargan, and Jonathon S. Wright
Atmos. Chem. Phys., 17, 12743–12778,Short summary
Ozone and water vapor in the stratosphere are important gases that affect surface climate and absorb incoming solar ultraviolet radiation. These gases are represented in reanalyses, which create a complete picture of the state of Earth's atmosphere using limited observations. We evaluate reanalysis water vapor and ozone fidelity by intercomparing them, and comparing them to independent observations. Generally reanalyses do a good job at representing ozone, but have problems with water vapor.
Ingo Wohltmann, Ralph Lehmann, and Markus Rex
Atmos. Chem. Phys., 17, 10535–10563,Short summary
We present a quantitative analysis of the chemical reactions involved in polar ozone depletion in the stratosphere, and of the relevant reaction pathways and cycles. We show time series of reaction rates averaged over the core of the polar vortex in winter and spring for all relevant reactions. An emphasis is put on the partitioning of the relevant chemical families (nitrogen, hydrogen, chlorine, bromine and odd oxygen) and activation and deactivation of chlorine.
Luis F. Millán and Gloria L. Manney
Atmos. Chem. Phys., 17, 9277–9289,Short summary
An ozone mini-hole is a synoptic-scale region with strongly decreased total column ozone resulting from dynamical processes. Using total column measurements from the Ozone Monitoring Instrument and ozone profile measurements from the Microwave Limb Sounder, we evaluate the accuracy of mini-hole representation in five reanalyses.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688,Short summary
The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Chaitri Roy, Suvarna Fadnavis, Rolf Müller, D. C. Ayantika, Felix Ploeger, and Alexandru Rap
Atmos. Chem. Phys., 17, 1297–1311,Short summary
In the monsoon season, Asian NOx emissions are rapidly transported to the UTLS and can impact ozone in the UTLS. From chemistry–climate model simulations, we show that increasing Asian NOx emissions have enhanced ozone radiative forcing over Southeast Asia, which leads to significant warming over the Tibetan Plateau and increase precipitation over India. However, a further increase in NOx emissions elicited negative precipitation due to reversal of monsoon Hadley circulation.
Tamás Kovács, Wuhu Feng, Anna Totterdill, John M. C. Plane, Sandip Dhomse, Juan Carlos Gómez-Martín, Gabriele P. Stiller, Florian J. Haenel, Christopher Smith, Piers M. Forster, Rolando R. García, Daniel R. Marsh, and Martyn P. Chipperfield
Atmos. Chem. Phys., 17, 883–898,Short summary
Sulfur hexafluoride (SF6) is a very potent greenhouse gas, which is present in the atmosphere only through its industrial use, for example as an electrical insulator. To estimate accurately the impact of SF6 emissions on climate we need to know how long it persists in the atmosphere before being removed. Previous estimates of the SF6 lifetime indicate a large degree of uncertainty. Here we use a detailed atmospheric model to calculate a current best estimate of the SF6 lifetime.
Ulrike Langematz, Franziska Schmidt, Markus Kunze, Gregory E. Bodeker, and Peter Braesicke
Atmos. Chem. Phys., 16, 15619–15627,Short summary
The extent of anthropogenically driven Antarctic ozone depletion prior to 1980 is examined using transient chemistry–climate model simulations from 1960 to 2000 with prescribed changes of ozone depleting substances in conjunction with observations. All models show a long-term, halogen-induced negative trend in Antarctic ozone from 1960 to 1980, ranging between 26 and 50 % of the total anthropogenic ozone depletion from 1960 to 2000. A stronger ozone decline of 56 % was estimated from observation.
Katherine M. Saad, Debra Wunch, Nicholas M. Deutscher, David W. T. Griffith, Frank Hase, Martine De Mazière, Justus Notholt, David F. Pollard, Coleen M. Roehl, Matthias Schneider, Ralf Sussmann, Thorsten Warneke, and Paul O. Wennberg
Atmos. Chem. Phys., 16, 14003–14024,Short summary
Current approaches to constrain the global methane budget assimilate total column measurements into models, but model biases can impact results. We use tropospheric methane columns to evaluate model transport errors and identify a seasonal time lag in the Northern Hemisphere troposphere masked by stratospheric compensating effects. We find systematic biases in the stratosphere will alias into model-derived emissions estimates, especially those in the high Northern latitudes that vary seasonally.
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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.
The stratosphere is an important source of tropospheric ozone, which affects climate, chemistry,...