Articles | Volume 15, issue 19
https://doi.org/10.5194/acp-15-11201-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-15-11201-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
08 Oct 2015
Research article |
| 08 Oct 2015
The influence of synoptic weather regimes on UK air quality: regional model studies of tropospheric column NO2
R. J. Pope
CORRESPONDING AUTHOR
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Earth Observation, University of Leeds, Leeds, LS2 9JT, UK
N. H. Savage
Met Office, Exeter, UK
M. P. Chipperfield
School of Earth and Environment, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Earth Observation, University of Leeds, Leeds, LS2 9JT, UK
C. Ordóñez
Met Office, Exeter, UK
L. S. Neal
Met Office, Exeter, UK
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For the Aburrá Valley, Colombia, local emissions dominate aerosol concentrations, which degrade air quality (AQ) and impact human health. However, this can be exacerbated by the influx of external emissions from sources such as regional fires, Saharan dust, and volcanic degassing. While substantially increasing city-wide aerosols, these external sources can also degrade the aerosol chemical composition (i.e. their toxicity) and impact AQ, which we investigate in this study.
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Ozone is a potent air pollutant, and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTCO3) from space. We have constructed a merged LTCO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTCO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small-scale differences.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
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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.
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Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
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Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
Yajuan Li, Martyn P. Chipperfield, Wuhu Feng, Sandip S. Dhomse, Richard J. Pope, Faquan Li, and Dong Guo
Atmos. Chem. Phys., 20, 8627–8639, https://doi.org/10.5194/acp-20-8627-2020, https://doi.org/10.5194/acp-20-8627-2020, 2020
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Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Matthew J. Rowlinson, Alexandru Rap, Stephen R. Arnold, Richard J. Pope, Martyn P. Chipperfield, Joe McNorton, Piers Forster, Hamish Gordon, Kirsty J. Pringle, Wuhu Feng, Brian J. Kerridge, Barry L. Latter, and Richard Siddans
Atmos. Chem. Phys., 19, 8669–8686, https://doi.org/10.5194/acp-19-8669-2019, https://doi.org/10.5194/acp-19-8669-2019, 2019
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Wildfires and meteorology have a substantial effect on atmospheric concentrations of greenhouse gases such as methane and ozone. During the 1997 El Niño event, unusually large fire emissions indirectly increased global methane through carbon monoxide emission, which decreased the oxidation capacity of the atmosphere. There were also large regional changes to tropospheric ozone concentrations, but contrasting effects of fire and meteorology resulted in a small change to global radiative forcing.
Richard J. Pope, Martyn P. Chipperfield, Stephen R. Arnold, Norbert Glatthor, Wuhu Feng, Sandip S. Dhomse, Brian J. Kerridge, Barry G. Latter, and Richard Siddans
Atmos. Chem. Phys., 18, 8389–8408, https://doi.org/10.5194/acp-18-8389-2018, https://doi.org/10.5194/acp-18-8389-2018, 2018
Sarah A. Monks, Stephen R. Arnold, Michael J. Hollaway, Richard J. Pope, Chris Wilson, Wuhu Feng, Kathryn M. Emmerson, Brian J. Kerridge, Barry L. Latter, Georgina M. Miles, Richard Siddans, and Martyn P. Chipperfield
Geosci. Model Dev., 10, 3025–3057, https://doi.org/10.5194/gmd-10-3025-2017, https://doi.org/10.5194/gmd-10-3025-2017, 2017
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The TOMCAT chemical transport model has been updated with the chemical degradation of ethene, propene, toluene, butane and monoterpenes. The tropospheric chemical mechanism is documented and the model is evaluated against surface, balloon, aircraft and satellite data. The model is generally able to capture the main spatial and seasonal features of carbon monoxide, ozone, volatile organic compounds and reactive nitrogen. However,
some model biases are found that require further investigation.
Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, John J. Remedios, Carsten Warneke, James M. Roberts, Glenn S. Diskin, Lewis G. Huey, Armin Wisthaler, Eric C. Apel, Peter F. Bernath, and Wuhu Feng
Atmos. Chem. Phys., 16, 13541–13559, https://doi.org/10.5194/acp-16-13541-2016, https://doi.org/10.5194/acp-16-13541-2016, 2016
R. J. Pope, M. P. Chipperfield, N. H. Savage, C. Ordóñez, L. S. Neal, L. A. Lee, S. S. Dhomse, N. A. D. Richards, and T. D. Keslake
Atmos. Chem. Phys., 15, 5611–5626, https://doi.org/10.5194/acp-15-5611-2015, https://doi.org/10.5194/acp-15-5611-2015, 2015
Aishah Shittu, Kirsty Pringle, Stephen Arnold, Richard Pope, Ailish Graham, Carly Reddington, Richard Rigby, and James McQuaid
EGUsphere, https://doi.org/10.5194/egusphere-2024-1685, https://doi.org/10.5194/egusphere-2024-1685, 2024
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
The study highlighted the importance of data cleaning in improving the raw Atmotube Pro PM2.5 data. The data cleaning method was successful in improving the inter-sensor variability among the Atmotube Pro sensors data. This study showed 62.5 % of the sensors used for the study exhibited greater precision in their measurements. The overall performance showed the sensors passed the base testing recommended by USEPA using one-hour averaged data.
Maria P. Velásquez-García, K. Santiago Hernández, James A. Vergara-Correa, Richard J. Pope, Miriam Gómez-Marín, and Angela M. Rendón
EGUsphere, https://doi.org/10.5194/egusphere-2024-695, https://doi.org/10.5194/egusphere-2024-695, 2024
Short summary
Short summary
For the Aburrá Valley, Colombia, local emissions dominate aerosol concentrations, which degrade air quality (AQ) and impact human health. However, this can be exacerbated by the influx of external emissions from sources such as regional fires, Saharan dust, and volcanic degassing. While substantially increasing city-wide aerosols, these external sources can also degrade the aerosol chemical composition (i.e. their toxicity) and impact AQ, which we investigate in this study.
Richard J. Pope, Alexandru Rap, Matilda A. Pimlott, Brice Barret, Eric Le Flochmoen, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Anne Boynard, Christian Retscher, Wuhu Feng, Richard Rigby, Sandip S. Dhomse, Catherine Wespes, and Martyn P. Chipperfield
Atmos. Chem. Phys., 24, 3613–3626, https://doi.org/10.5194/acp-24-3613-2024, https://doi.org/10.5194/acp-24-3613-2024, 2024
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Short summary
Tropospheric ozone is an important short-lived climate forcer which influences the incoming solar short-wave radiation and the outgoing long-wave radiation in the atmosphere (8–15 km) where the balance between the two yields a net positive (i.e. warming) effect at the surface. Overall, we find that the tropospheric ozone radiative effect ranges between 1.21 and 1.26 W m−2 with a negligible trend (2008–2017), suggesting that tropospheric ozone influences on climate have remained stable with time.
Emma Sands, Richard Pope, Ruth M. Doherty, Fiona M. O'Connor, Chris Wilson, and Hugh Pumphrey
EGUsphere, https://doi.org/10.5194/egusphere-2024-503, https://doi.org/10.5194/egusphere-2024-503, 2024
Short summary
Short summary
Changes in vegetation alongside biomass burning impact regional atmospheric composition and air quality. Using satellite remote sensing, we find a clear linear relationship between forest cover and isoprene and a pronounced non-linear relationship between burned area and nitrogen dioxide in the southern Amazon, a region of substantial deforestation. These quantified relationships can be used for model evaluation and further exploration of biosphere-atmosphere interactions in Earth System Models.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn Chipperfield, Wuhu Feng, David Oram, Karina Adcock, Stephen Montzka, Isobel Simpson, Andrea Mazzeo, Amber Leeson, Elliot Atlas, and Charles C.-K. Chou
EGUsphere, https://doi.org/10.5194/egusphere-2024-560, https://doi.org/10.5194/egusphere-2024-560, 2024
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Ethylene dichloride (EDC) is an industrial chemical used to produce polyvinyl chloride (PVC). We analysed EDC production data to estimate global EDC emissions (2002 to 2020). The emissions were included in an atmospheric model and evaluated by comparing simulated EDC to EDC measurements in the troposphere. We show EDC contributes ozone-depleting chlorine to the stratosphere and this has increased with increasing EDC emissions. EDC’s impact on stratospheric ozone is currently small, but non-zero.
Martyn P. Chipperfield and Slimane Bekki
Atmos. Chem. Phys., 24, 2783–2802, https://doi.org/10.5194/acp-24-2783-2024, https://doi.org/10.5194/acp-24-2783-2024, 2024
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga–Hunga Ha'apai volcano in January 2022.
Ailish M. Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matilda Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
Atmos. Chem. Phys., 24, 789–806, https://doi.org/10.5194/acp-24-789-2024, https://doi.org/10.5194/acp-24-789-2024, 2024
Short summary
Short summary
Our paper uses novel satellite datasets and high-resolution emissions datasets alongside a back-trajectory model to investigate the balance of local and external sources influencing NOx air pollution changes in Delhi. We find in the post-monsoon season that NOx from local and non-local transport emissions contributes most to poor air quality in Delhi. Therefore, air quality mitigation strategies in Delhi and surrounding regions are used to control this issue.
Richard J. Pope, Fiona M. O'Connor, Mohit Dalvi, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Brice Barret, Eric Le Flochmoen, Anne Boynard, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, Catherine Wespes, and Richard Rigby
EGUsphere, https://doi.org/10.5194/egusphere-2023-3109, https://doi.org/10.5194/egusphere-2023-3109, 2024
Short summary
Short summary
Ozone is a potent air pollutant in the lower troposphere with adverse impacts on human health. Satellite records of tropospheric ozone currently show large-scale inconsistencies in their long-term trends. Our detailed study of the potential factors (e.g. satellite errors, where the satellite can observe ozone) potentially driving these inconsistencies found that in North America, Europe and East Asia, the underlying trends are typically small with large uncertainties.
Andrea Pazmiño, Florence Goutail, Sophie Godin-Beekmann, Alain Hauchecorne, Jean-Pierre Pommereau, Martyn P. Chipperfield, Wuhu Feng, Franck Lefèvre, Audrey Lecouffe, Michel Van Roozendael, Nis Jepsen, Georg Hansen, Rigel Kivi, Kimberly Strong, and Kaley A. Walker
Atmos. Chem. Phys., 23, 15655–15670, https://doi.org/10.5194/acp-23-15655-2023, https://doi.org/10.5194/acp-23-15655-2023, 2023
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The vortex-averaged ozone loss over the last 3 decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from the SAOZ network and MSR2 reanalysis. Three metrics were developed to compute ozone trends since 2000. The study confirms the ozone recovery in the Antarctic and shows a potential sign of quantitative detection of ozone recovery in the Arctic that needs to be robustly confirmed in the future.
Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, and Richard Rigby
Atmos. Chem. Phys., 23, 14933–14947, https://doi.org/10.5194/acp-23-14933-2023, https://doi.org/10.5194/acp-23-14933-2023, 2023
Short summary
Short summary
Ozone is a potent air pollutant, and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTCO3) from space. We have constructed a merged LTCO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTCO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small-scale differences.
Sandip S. Dhomse and Martyn P. Chipperfield
Earth Syst. Sci. Data, 15, 5105–5120, https://doi.org/10.5194/essd-15-5105-2023, https://doi.org/10.5194/essd-15-5105-2023, 2023
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There are no long-term stratospheric profile data sets for two very important greenhouse gases: methane (CH4) and nitrous oxide (N2O). Along with radiative feedback, these species play an important role in controlling ozone loss in the stratosphere. Here, we use machine learning to fuse satellite measurements with a chemical model to construct long-term gap-free profile data sets for CH4 and N2O. We aim to construct similar data sets for other important trace gases (e.g. O3, Cly, NOy species).
Chris Wilson, Brian J. Kerridge, Richard Siddans, David P. Moore, Lucy J. Ventress, Emily Dowd, Wuhu Feng, Martyn P. Chipperfield, and John J. Remedios
EGUsphere, https://doi.org/10.5194/egusphere-2023-1652, https://doi.org/10.5194/egusphere-2023-1652, 2023
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The leaks from the Nord Stream gas pipelines in September 2022 released a large amount of methane (CH4) to the atmosphere. We provide observational data from a satellite instrument, IASI, that shows a large CH4 plume over the North Sea off the coast of Scandinavia. We use this, together with atmospheric models, to quantify the CH4 leaked into the atmosphere from the pipelines. We find that 215–390 Gg CH4 was emitted, making this the largest individual fossil fuel-related CH4 leak on record.
Ewa M. Bednarz, 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.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys., 23, 13235–13253, https://doi.org/10.5194/acp-23-13235-2023, https://doi.org/10.5194/acp-23-13235-2023, 2023
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Yang Li, Wuhu Feng, Xin Zhou, Yajuan Li, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2023-1452, https://doi.org/10.5194/egusphere-2023-1452, 2023
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Tibetan Plateau (TP), the highest and largest plateau, experiences strong surface solar UV radiation, whose excess can cause harmful influences on the local biota. Hence, it is critical to study TP ozone. We find ENSO, the strongest interannual phenomenon, can induce tropospheric temperature change and thus cause tropopause movement, which in turn leads to ozone change. Our understanding implies that future more strong ENSO events will play a key role in ozone recovery and ecosystems of the TP.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Peter Joyce, Cristina Ruiz Villena, Yahui Huang, Alex Webb, Manuel Gloor, Fabien H. Wagner, Martyn P. Chipperfield, Rocío Barrio Guilló, Chris Wilson, and Hartmut Boesch
Atmos. Meas. Tech., 16, 2627–2640, https://doi.org/10.5194/amt-16-2627-2023, https://doi.org/10.5194/amt-16-2627-2023, 2023
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Methane emissions are responsible for a lot of the warming caused by the greenhouse effect, much of which comes from a small number of point sources. We can identify methane point sources by analysing satellite data, but it requires a lot of time invested by experts and is prone to very high errors. Here, we produce a neural network that can automatically identify methane point sources and estimate the mass of methane that is being released per hour and are able to do so with far smaller errors.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Zixuan Jia, Carlos Ordóñez, Ruth M. Doherty, Oliver Wild, Steven T. Turnock, and Fiona M. O'Connor
Atmos. Chem. Phys., 23, 2829–2842, https://doi.org/10.5194/acp-23-2829-2023, https://doi.org/10.5194/acp-23-2829-2023, 2023
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This study investigates the influence of the winter large-scale circulation on daily concentrations of PM2.5 and their sensitivity to emissions. The new proposed circulation index can effectively distinguish different levels of air pollution and explain changes in PM2.5 sensitivity to emissions from local and surrounding regions. We then project future changes in PM2.5 concentrations using this index and find an increase in PM2.5 concentrations over the region due to climate change.
Robert J. Parker, Chris Wilson, Edward Comyn-Platt, Garry Hayman, Toby R. Marthews, A. Anthony Bloom, Mark F. Lunt, Nicola Gedney, Simon J. Dadson, Joe McNorton, Neil Humpage, Hartmut Boesch, Martyn P. Chipperfield, Paul I. Palmer, and Dai Yamazaki
Biogeosciences, 19, 5779–5805, https://doi.org/10.5194/bg-19-5779-2022, https://doi.org/10.5194/bg-19-5779-2022, 2022
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Wetlands are the largest natural source of methane, one of the most important climate gases. The JULES land surface model simulates these emissions. We use satellite data to evaluate how well JULES reproduces the methane seasonal cycle over different tropical wetlands. It performs well for most regions; however, it struggles for some African wetlands influenced heavily by river flooding. We explain the reasons for these deficiencies and highlight how future development will improve these areas.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Zixuan Jia, Ruth M. Doherty, Carlos Ordóñez, Chaofan Li, Oliver Wild, Shipra Jain, and Xiao Tang
Atmos. Chem. Phys., 22, 6471–6487, https://doi.org/10.5194/acp-22-6471-2022, https://doi.org/10.5194/acp-22-6471-2022, 2022
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This study investigates the modulation of daily PM2.5 over three major populated regions in China by regional meteorology and large-scale circulation during winter. These results demonstrate the benefits of considering the large-scale circulation for air quality studies. The novel circulation indices proposed here can explain a considerable fraction of the day-to-day variability of PM2.5 and can be combined with regional meteorology to improve our capability to predict the variability of PM2.5.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Piera Raspollini, Enrico Arnone, Flavio Barbara, Massimo Bianchini, Bruno Carli, Simone Ceccherini, Martyn P. Chipperfield, Angelika Dehn, Stefano Della Fera, Bianca Maria Dinelli, Anu Dudhia, Jean-Marie Flaud, Marco Gai, Michael Kiefer, Manuel López-Puertas, David P. Moore, Alessandro Piro, John J. Remedios, Marco Ridolfi, Harjinder Sembhi, Luca Sgheri, and Nicola Zoppetti
Atmos. Meas. Tech., 15, 1871–1901, https://doi.org/10.5194/amt-15-1871-2022, https://doi.org/10.5194/amt-15-1871-2022, 2022
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The MIPAS instrument onboard the ENVISAT satellite provided 10 years of measurements of the atmospheric emission al limb that allow for the retrieval of latitude- and altitude-resolved atmospheric composition. We describe the improvements implemented in the retrieval algorithm used for the full mission reanalysis, which allows for the generation of the global distributions of 21 atmospheric constituents plus temperature with increased accuracy with respect to previously generated data.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Sandip S. Dhomse, Carlo Arosio, Wuhu Feng, Alexei Rozanov, Mark Weber, and Martyn P. Chipperfield
Earth Syst. Sci. Data, 13, 5711–5729, https://doi.org/10.5194/essd-13-5711-2021, https://doi.org/10.5194/essd-13-5711-2021, 2021
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High-quality long-term ozone profile data sets are key to estimating short- and long-term ozone variability. Almost all the satellite (and chemical model) data sets show some kind of bias with respect to each other. This is because of differences in measurement methodologies as well as simplified processes in the models. We use satellite data sets and chemical model output to generate 42 years of ozone profile data sets using a random-forest machine-learning algorithm that is named ML-TOMCAT.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Jacob W. Maddison, Marta Abalos, David Barriopedro, Ricardo García-Herrera, Jose M. Garrido-Perez, and Carlos Ordóñez
Weather Clim. Dynam., 2, 675–694, https://doi.org/10.5194/wcd-2-675-2021, https://doi.org/10.5194/wcd-2-675-2021, 2021
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Air stagnation occurs when an air mass becomes settled over a region and precipitation is suppressed. Pollutant levels can rise during stagnation. The synoptic- to large-scale influence on European air stagnation and pollution is explored here. We show that around 60 % of the monthly variability in air stagnation and pollutants can be explained by dynamical indices describing the atmospheric circulation. The weather systems most related to stagnation are different for regions across Europe.
Johannes de Leeuw, Anja Schmidt, Claire S. Witham, Nicolas Theys, Isabelle A. Taylor, Roy G. Grainger, Richard J. Pope, Jim Haywood, Martin Osborne, and Nina I. Kristiansen
Atmos. Chem. Phys., 21, 10851–10879, https://doi.org/10.5194/acp-21-10851-2021, https://doi.org/10.5194/acp-21-10851-2021, 2021
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Using the NAME dispersion model in combination with high-resolution SO2 satellite data from TROPOMI, we investigate the dispersion of volcanic SO2 from the 2019 Raikoke eruption. NAME accurately simulates the dispersion of SO2 during the first 2–3 weeks after the eruption and illustrates the potential of using high-resolution satellite data to identify potential limitations in dispersion models, which will ultimately help to improve efforts to forecast the dispersion of volcanic clouds.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
Akash Biswal, Vikas Singh, Shweta Singh, Amit P. Kesarkar, Khaiwal Ravindra, Ranjeet S. Sokhi, Martyn P. Chipperfield, Sandip S. Dhomse, Richard J. Pope, Tanbir Singh, and Suman Mor
Atmos. Chem. Phys., 21, 5235–5251, https://doi.org/10.5194/acp-21-5235-2021, https://doi.org/10.5194/acp-21-5235-2021, 2021
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Satellite and surface observations show a reduction in NO2 levels over India during the lockdown compared to business-as-usual years. A substantial reduction, proportional to the population, was observed over the urban areas. The changes in NO2 levels at the surface during the lockdown appear to be present in the satellite observations. However, TROPOMI showed a better correlation with surface NO2 and was more sensitive to the changes than OMI because of the finer resolution.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Robert J. Parker, Chris Wilson, A. Anthony Bloom, Edward Comyn-Platt, Garry Hayman, Joe McNorton, Hartmut Boesch, and Martyn P. Chipperfield
Biogeosciences, 17, 5669–5691, https://doi.org/10.5194/bg-17-5669-2020, https://doi.org/10.5194/bg-17-5669-2020, 2020
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Wetlands contribute the largest uncertainty to the atmospheric methane budget. WetCHARTs is a simple, data-driven model that estimates wetland emissions using observations of precipitation and temperature. We perform the first detailed evaluation of WetCHARTs against satellite data and find it performs well in reproducing the observed wetland methane seasonal cycle for the majority of wetland regions. In regions where it performs poorly, we highlight incorrect wetland extent as a key reason.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Benjamin Birner, Martyn P. Chipperfield, Eric J. Morgan, Britton B. Stephens, Marianna Linz, Wuhu Feng, Chris Wilson, Jonathan D. Bent, Steven C. Wofsy, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Chem. Phys., 20, 12391–12408, https://doi.org/10.5194/acp-20-12391-2020, https://doi.org/10.5194/acp-20-12391-2020, 2020
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With new high-precision observations from nine aircraft campaigns and 3-D chemical transport modeling, we show that the argon-to-nitrogen ratio (Ar / N2) in the lowermost stratosphere provides a useful constraint on the “age of air” (the time elapsed since entry of an air parcel into the stratosphere). Therefore, Ar / N2 in combination with traditional age-of-air indicators, such as CO2 and N2O, could provide new insights into atmospheric mixing and transport.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
Yajuan Li, Martyn P. Chipperfield, Wuhu Feng, Sandip S. Dhomse, Richard J. Pope, Faquan Li, and Dong Guo
Atmos. Chem. Phys., 20, 8627–8639, https://doi.org/10.5194/acp-20-8627-2020, https://doi.org/10.5194/acp-20-8627-2020, 2020
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The Tibetan Plateau (TP) exerts important thermal and dynamical effects on atmospheric circulation, climate change as well as the ozone distribution. In this study, we use updated observations and model simulations to investigate the ozone trends and variations over the TP. Wintertime TP ozone variations are largely controlled by tropical to high-latitude transport processes, whereas summertime concentrations are a combined effect of photochemical decay and tropical processes.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
Preprint withdrawn
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Andreas Chrysanthou, Amanda C. Maycock, and Martyn P. Chipperfield
Weather Clim. Dynam., 1, 155–174, https://doi.org/10.5194/wcd-1-155-2020, https://doi.org/10.5194/wcd-1-155-2020, 2020
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We perform 50-year-long time-slice experiments using the Met Office HadGEM3 global climate model in order to decompose the Brewer–Dobson circulation (BDC) response to an abrupt quadrupling of CO2 in three distinct components, (a) the rapid adjustment, associated with CO2 radiative effects; (b) a global uniform sea surface temperature warming; and (c) sea surface temperature patterns. This demonstrates a potential for fast and slow timescales of the response of the BDC to greenhouse gas forcing.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
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Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Andreas Chrysanthou, Amanda C. Maycock, Martyn P. Chipperfield, Sandip Dhomse, Hella Garny, Douglas Kinnison, Hideharu Akiyoshi, Makoto Deushi, Rolando R. Garcia, Patrick Jöckel, Oliver Kirner, Giovanni Pitari, David A. Plummer, Laura Revell, Eugene Rozanov, Andrea Stenke, Taichu Y. Tanaka, Daniele Visioni, and Yousuke Yamashita
Atmos. Chem. Phys., 19, 11559–11586, https://doi.org/10.5194/acp-19-11559-2019, https://doi.org/10.5194/acp-19-11559-2019, 2019
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We perform the first multi-model comparison of the impact of nudged meteorology on the stratospheric residual circulation (RC) in chemistry–climate models. Nudging meteorology does not constrain the mean strength of RC compared to free-running simulations, and despite the lack of agreement in the mean circulation, nudging tightly constrains the inter-annual variability in the tropical upward mass flux in the lower stratosphere. In summary, nudging strongly affects the representation of RC.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
Matthew J. Rowlinson, Alexandru Rap, Stephen R. Arnold, Richard J. Pope, Martyn P. Chipperfield, Joe McNorton, Piers Forster, Hamish Gordon, Kirsty J. Pringle, Wuhu Feng, Brian J. Kerridge, Barry L. Latter, and Richard Siddans
Atmos. Chem. Phys., 19, 8669–8686, https://doi.org/10.5194/acp-19-8669-2019, https://doi.org/10.5194/acp-19-8669-2019, 2019
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Wildfires and meteorology have a substantial effect on atmospheric concentrations of greenhouse gases such as methane and ozone. During the 1997 El Niño event, unusually large fire emissions indirectly increased global methane through carbon monoxide emission, which decreased the oxidation capacity of the atmosphere. There were also large regional changes to tropospheric ozone concentrations, but contrasting effects of fire and meteorology resulted in a small change to global radiative forcing.
Evgenia Galytska, Alexey Rozanov, Martyn P. Chipperfield, Sandip. S. Dhomse, Mark Weber, Carlo Arosio, Wuhu Feng, and John P. Burrows
Atmos. Chem. Phys., 19, 767–783, https://doi.org/10.5194/acp-19-767-2019, https://doi.org/10.5194/acp-19-767-2019, 2019
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In this study we analysed ozone changes in the tropical mid-stratosphere as observed by the SCIAMACHY instrument during 2004–2012. We used simulations from TOMCAT model with different chemical and dynamical forcings to reveal primary causes of ozone changes. We also considered measured NO2 and modelled NOx, NOx, and N2O data. With modelled AoA data we identified seasonal changes in the upwelling speed and explained how those changes affect N2O chemistry which leads to observed ozone changes.
Debora Griffin, Kaley A. Walker, Ingo Wohltmann, Sandip S. Dhomse, Markus Rex, Martyn P. Chipperfield, Wuhu Feng, Gloria L. Manney, Jane Liu, and David Tarasick
Atmos. Chem. Phys., 19, 577–601, https://doi.org/10.5194/acp-19-577-2019, https://doi.org/10.5194/acp-19-577-2019, 2019
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Ozone in the stratosphere is important to protect the Earth from UV radiation. Using measurements taken by the Atmospheric Chemistry Experiment satellite between 2005 and 2013, we examine different methods to calculate the ozone loss in the high Arctic and establish the altitude at which most of the ozone is destroyed. Our results show that the different methods agree within the uncertainties. Recommendations are made on which methods are most appropriate to use.
Joe McNorton, Chris Wilson, Manuel Gloor, Rob J. Parker, Hartmut Boesch, Wuhu Feng, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 18149–18168, https://doi.org/10.5194/acp-18-18149-2018, https://doi.org/10.5194/acp-18-18149-2018, 2018
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Since 2007 atmospheric methane (CH4) has been unexpectedly increasing following a 6-year hiatus. We have used an atmospheric model to attribute regional sources and global sinks of CH4 using observations for the 2003–2015 period. Model results show the renewed growth is best explained by decreased atmospheric removal, decreased biomass burning emissions, and an increased energy sector (mainly from Africa–Middle East and Southern Asia–Oceania) and wetland emissions (mainly from northern Eurasia).
Rocío Baró, Pedro Jiménez-Guerrero, Martin Stengel, Dominik Brunner, Gabriele Curci, Renate Forkel, Lucy Neal, Laura Palacios-Peña, Nicholas Savage, Martijn Schaap, Paolo Tuccella, Hugo Denier van der Gon, and Stefano Galmarini
Atmos. Chem. Phys., 18, 15183–15199, https://doi.org/10.5194/acp-18-15183-2018, https://doi.org/10.5194/acp-18-15183-2018, 2018
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Particles in the atmosphere, such as pollution, desert dust, and volcanic ash, have an impact on meteorology. They interact with incoming radiation resulting in a cooling effect of the atmosphere. Today, the use of meteorology and chemistry models help us to understand these processes, but there are a lot of uncertainties. The goal of this work is to evaluate how these interactions are represented in the models by comparing them to satellite data to see how close they are to reality.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Birgit Hassler, Stefanie Kremser, Greg E. Bodeker, Jared Lewis, Kage Nesbit, Sean M. Davis, Martyn P. Chipperfield, Sandip S. Dhomse, and Martin Dameris
Earth Syst. Sci. Data, 10, 1473–1490, https://doi.org/10.5194/essd-10-1473-2018, https://doi.org/10.5194/essd-10-1473-2018, 2018
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
Jens-Uwe Grooß, Rolf Müller, Reinhold Spang, Ines Tritscher, Tobias Wegner, Martyn P. Chipperfield, Wuhu Feng, Douglas E. Kinnison, and Sasha Madronich
Atmos. Chem. Phys., 18, 8647–8666, https://doi.org/10.5194/acp-18-8647-2018, https://doi.org/10.5194/acp-18-8647-2018, 2018
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We investigate a discrepancy between model simulations and observations of HCl in the dark polar stratosphere. In early winter, the less-well-studied period of the onset of chlorine activation, observations show a much faster depletion of HCl than simulations of three models. This points to some unknown process that is currently not represented in the models. Various hypotheses for potential causes are investigated that partly reduce the discrepancy. The impact on polar ozone depletion is low.
Richard J. Pope, Martyn P. Chipperfield, Stephen R. Arnold, Norbert Glatthor, Wuhu Feng, Sandip S. Dhomse, Brian J. Kerridge, Barry G. Latter, and Richard Siddans
Atmos. Chem. Phys., 18, 8389–8408, https://doi.org/10.5194/acp-18-8389-2018, https://doi.org/10.5194/acp-18-8389-2018, 2018
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
Lucy S. Neal, Mohit Dalvi, Gerd Folberth, Rachel N. McInnes, Paul Agnew, Fiona M. O'Connor, Nicholas H. Savage, and Marie Tilbee
Geosci. Model Dev., 10, 3941–3962, https://doi.org/10.5194/gmd-10-3941-2017, https://doi.org/10.5194/gmd-10-3941-2017, 2017
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This paper concerns aspects of downscaling global atmospheric composition and chemistry model predictions on the continental and UK national scale. A two-step nested model configuration was developed and used to simulate UK air quality for a 5-year period under present-day conditions. The results show some benefits associated with higher-resolution modelling for primary emitted pollutants, but also highlight the importance of consistency between the nested models.
Sarah A. Monks, Stephen R. Arnold, Michael J. Hollaway, Richard J. Pope, Chris Wilson, Wuhu Feng, Kathryn M. Emmerson, Brian J. Kerridge, Barry L. Latter, Georgina M. Miles, Richard Siddans, and Martyn P. Chipperfield
Geosci. Model Dev., 10, 3025–3057, https://doi.org/10.5194/gmd-10-3025-2017, https://doi.org/10.5194/gmd-10-3025-2017, 2017
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The TOMCAT chemical transport model has been updated with the chemical degradation of ethene, propene, toluene, butane and monoterpenes. The tropospheric chemical mechanism is documented and the model is evaluated against surface, balloon, aircraft and satellite data. The model is generally able to capture the main spatial and seasonal features of carbon monoxide, ozone, volatile organic compounds and reactive nitrogen. However,
some model biases are found that require further investigation.
Wenshou Tian, Yuanpu Li, Fei Xie, Jiankai Zhang, Martyn P. Chipperfield, Wuhu Feng, Yongyun Hu, Sen Zhao, Xin Zhou, Yun Yang, and Xuan Ma
Atmos. Chem. Phys., 17, 6705–6722, https://doi.org/10.5194/acp-17-6705-2017, https://doi.org/10.5194/acp-17-6705-2017, 2017
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Although the principal mechanisms responsible for the formation of the Antarctic ozone hole are well understood, the factors or processes that generate interannual variations in ozone levels in the southern high-latitude stratosphere remain under debate. This study finds that the SST variations across the East Asian marginal seas (5° S–35° N, 100–140° E) could modulate the southern high-latitude stratospheric ozone interannual changes.
Shreeya Verma, Julia Marshall, Mark Parrington, Anna Agustí-Panareda, Sebastien Massart, Martyn P. Chipperfield, Christopher Wilson, and Christoph Gerbig
Atmos. Chem. Phys., 17, 6663–6678, https://doi.org/10.5194/acp-17-6663-2017, https://doi.org/10.5194/acp-17-6663-2017, 2017
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Aircraft profiles are a useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, these are available only up to about 9–13 km altitude and therefore need to be extended synthetically into the stratosphere using other sources. In this study, we analyse three different data sources that are available for extension of CH4 profiles by comparing the error introduced by each into the total column and provide recommendations regarding the best approach.
Jochen Stutz, Bodo Werner, Max Spolaor, Lisa Scalone, James Festa, Catalina Tsai, Ross Cheung, Santo F. Colosimo, Ugo Tricoli, Rasmus Raecke, Ryan Hossaini, Martyn P. Chipperfield, Wuhu Feng, Ru-Shan Gao, Eric J. Hintsa, James W. Elkins, Fred L. Moore, Bruce Daube, Jasna Pittman, Steven Wofsy, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 1017–1042, https://doi.org/10.5194/amt-10-1017-2017, https://doi.org/10.5194/amt-10-1017-2017, 2017
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A new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument was developed for NASA’s Global Hawk unmanned aerial system during the Airborne Tropical TRopopause EXperiment to study trace gases in the tropical tropopause layer. A new technique that uses in situ and DOAS O3 observations together with radiative transfer calculations allows the retrieval of mixing ratios from the slant column densities of BrO and NO2 at high accuracies of 0.5 ppt and 15 ppt, respectively.
Carlos Ordóñez, David Barriopedro, Ricardo García-Herrera, Pedro M. Sousa, and Jordan L. Schnell
Atmos. Chem. Phys., 17, 3111–3131, https://doi.org/10.5194/acp-17-3111-2017, https://doi.org/10.5194/acp-17-3111-2017, 2017
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Blocks and ridges are synoptic patterns associated with an anticyclonic circulation. They also divert the atmospheric flow. This work proves that near-surface ozone in Europe is sensitive to these patterns. This quantitative assessment has been performed on a seasonal basis for a 15-year period. The results can be exploited in the future to evaluate modelled ozone responses to atmospheric circulation changes and to understand the contribution of dynamic effects to air quality projections.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Tamás Kovács, Wuhu Feng, Anna Totterdill, John M. C. Plane, Sandip Dhomse, Juan Carlos Gómez-Martín, Gabriele P. Stiller, Florian J. Haenel, Christopher Smith, Piers M. Forster, Rolando R. García, Daniel R. Marsh, and Martyn P. Chipperfield
Atmos. Chem. Phys., 17, 883–898, https://doi.org/10.5194/acp-17-883-2017, https://doi.org/10.5194/acp-17-883-2017, 2017
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Sulfur hexafluoride (SF6) is a very potent greenhouse gas, which is present in the atmosphere only through its industrial use, for example as an electrical insulator. To estimate accurately the impact of SF6 emissions on climate we need to know how long it persists in the atmosphere before being removed. Previous estimates of the SF6 lifetime indicate a large degree of uncertainty. Here we use a detailed atmospheric model to calculate a current best estimate of the SF6 lifetime.
Ioannis Kioutsioukis, Ulas Im, Efisio Solazzo, Roberto Bianconi, Alba Badia, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Dominik Brunner, Charles Chemel, Gabriele Curci, Hugo Denier van der Gon, Johannes Flemming, Renate Forkel, Lea Giordano, Pedro Jiménez-Guerrero, Marcus Hirtl, Oriol Jorba, Astrid Manders-Groot, Lucy Neal, Juan L. Pérez, Guidio Pirovano, Roberto San Jose, Nicholas Savage, Wolfram Schroder, Ranjeet S. Sokhi, Dimiter Syrakov, Paolo Tuccella, Johannes Werhahn, Ralf Wolke, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 16, 15629–15652, https://doi.org/10.5194/acp-16-15629-2016, https://doi.org/10.5194/acp-16-15629-2016, 2016
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Four ensemble methods are applied to two annual AQMEII datasets and their performance is compared for O3, NO2 and PM10. The goal of the study is to quantify to what extent we can extract predictable signals from an ensemble with superior skill at each station over the single models and the ensemble mean. The promotion of the right amount of accuracy and diversity within the ensemble results in an average additional skill of up to 31 % compared to using the full ensemble in an unconditional way.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, John J. Remedios, Carsten Warneke, James M. Roberts, Glenn S. Diskin, Lewis G. Huey, Armin Wisthaler, Eric C. Apel, Peter F. Bernath, and Wuhu Feng
Atmos. Chem. Phys., 16, 13541–13559, https://doi.org/10.5194/acp-16-13541-2016, https://doi.org/10.5194/acp-16-13541-2016, 2016
Anna Totterdill, Tamás Kovács, Wuhu Feng, Sandip Dhomse, Christopher J. Smith, Juan Carlos Gómez-Martín, Martyn P. Chipperfield, Piers M. Forster, and John M. C. Plane
Atmos. Chem. Phys., 16, 11451–11463, https://doi.org/10.5194/acp-16-11451-2016, https://doi.org/10.5194/acp-16-11451-2016, 2016
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In this study we have experimentally determined the infrared absorption cross sections of NF3 and CFC-115, calculated the radiative forcing and efficiency using two radiative transfer models and identified the effect of clouds and stratospheric adjustment. We have also determined their atmospheric lifetimes using the Whole Atmosphere Community Climate Model.
Tamás Kovács, John M. C. Plane, Wuhu Feng, Tibor Nagy, Martyn P. Chipperfield, Pekka T. Verronen, Monika E. Andersson, David A. Newnham, Mark A. Clilverd, and Daniel R. Marsh
Geosci. Model Dev., 9, 3123–3136, https://doi.org/10.5194/gmd-9-3123-2016, https://doi.org/10.5194/gmd-9-3123-2016, 2016
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This study was completed on D-region atmospheric model development. The sophisticated 3-D Whole Atmosphere Community Climate Model (WACCM) and the 1-D Sodynkalä Ion and Neutral Chemistry Model (SIC) were combined in order to provide a detailed, accurate model (WACCM-SIC) that considers the processes taking place in solar proton events. The original SIC model was reduced by mechanism reduction, which provided an accurate sub-mechanism (rSIC, WACCM-rSIC) of the original model.
Jeremy J. Harrison, Martyn P. Chipperfield, Christopher D. Boone, Sandip S. Dhomse, Peter F. Bernath, Lucien Froidevaux, John Anderson, and James Russell III
Atmos. Chem. Phys., 16, 10501–10519, https://doi.org/10.5194/acp-16-10501-2016, https://doi.org/10.5194/acp-16-10501-2016, 2016
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HF, the dominant stratospheric fluorine reservoir, results from the atmospheric degradation of anthropogenic species such as CFCs, HCFCs, and HFCs. All are strong greenhouse gases, and CFCs and HCFCs deplete stratospheric ozone.
We report the comparison of HF global distributions and trends measured by the ACE-FTS and HALOE satellite instruments with the output of SLIMCAT, a chemical transport model. The global HF trends reveal a slowing down in the rate of increase of HF since the 1990s.
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
R. J. Pope, M. P. Chipperfield, N. H. Savage, C. Ordóñez, L. S. Neal, L. A. Lee, S. S. Dhomse, N. A. D. Richards, and T. D. Keslake
Atmos. Chem. Phys., 15, 5611–5626, https://doi.org/10.5194/acp-15-5611-2015, https://doi.org/10.5194/acp-15-5611-2015, 2015
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
G. D. Hayman, F. M. O'Connor, M. Dalvi, D. B. Clark, N. Gedney, C. Huntingford, C. Prigent, M. Buchwitz, O. Schneising, J. P. Burrows, C. Wilson, N. Richards, and M. Chipperfield
Atmos. Chem. Phys., 14, 13257–13280, https://doi.org/10.5194/acp-14-13257-2014, https://doi.org/10.5194/acp-14-13257-2014, 2014
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Globally, wetlands are a major source of methane, which is the second most important greenhouse gas. We find the JULES wetland methane scheme to perform well in general, although there is a tendency for it to overpredict emissions in the tropics and underpredict them in northern latitudes. Our study highlights novel uses of satellite data as a major tool to constrain land-atmosphere methane flux models in a warming world.
A. Saiz-Lopez, R. P. Fernandez, C. Ordóñez, D. E. Kinnison, J. C. Gómez Martín, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 14, 13119–13143, https://doi.org/10.5194/acp-14-13119-2014, https://doi.org/10.5194/acp-14-13119-2014, 2014
J. J. Harrison, M. P. Chipperfield, A. Dudhia, S. Cai, S. Dhomse, C. D. Boone, and P. F. Bernath
Atmos. Chem. Phys., 14, 11915–11933, https://doi.org/10.5194/acp-14-11915-2014, https://doi.org/10.5194/acp-14-11915-2014, 2014
C. Wilson, M. P. Chipperfield, M. Gloor, and F. Chevallier
Geosci. Model Dev., 7, 2485–2500, https://doi.org/10.5194/gmd-7-2485-2014, https://doi.org/10.5194/gmd-7-2485-2014, 2014
S. S. Dhomse, K. M. Emmerson, G. W. Mann, N. Bellouin, K. S. Carslaw, M. P. Chipperfield, R. Hommel, N. L. Abraham, P. Telford, P. Braesicke, M. Dalvi, C. E. Johnson, F. O'Connor, O. Morgenstern, J. A. Pyle, T. Deshler, J. M. Zawodny, and L. W. Thomason
Atmos. Chem. Phys., 14, 11221–11246, https://doi.org/10.5194/acp-14-11221-2014, https://doi.org/10.5194/acp-14-11221-2014, 2014
L. Kritten, A. Butz, M. P. Chipperfield, M. Dorf, S. Dhomse, R. Hossaini, H. Oelhaf, C. Prados-Roman, G. Wetzel, and K. Pfeilsticker
Atmos. Chem. Phys., 14, 9555–9566, https://doi.org/10.5194/acp-14-9555-2014, https://doi.org/10.5194/acp-14-9555-2014, 2014
R. L. Thompson, P. K. Patra, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, C. Wilson, P. Bergamaschi, E. Dlugokencky, C. Sweeney, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, M. Saunois, M. Chipperfield, and P. Bousquet
Atmos. Chem. Phys., 14, 4349–4368, https://doi.org/10.5194/acp-14-4349-2014, https://doi.org/10.5194/acp-14-4349-2014, 2014
A. Baklanov, K. Schlünzen, P. Suppan, J. Baldasano, D. Brunner, S. Aksoyoglu, G. Carmichael, J. Douros, J. Flemming, R. Forkel, S. Galmarini, M. Gauss, G. Grell, M. Hirtl, S. Joffre, O. Jorba, E. Kaas, M. Kaasik, G. Kallos, X. Kong, U. Korsholm, A. Kurganskiy, J. Kushta, U. Lohmann, A. Mahura, A. Manders-Groot, A. Maurizi, N. Moussiopoulos, S. T. Rao, N. Savage, C. Seigneur, R. S. Sokhi, E. Solazzo, S. Solomos, B. Sørensen, G. Tsegas, E. Vignati, B. Vogel, and Y. Zhang
Atmos. Chem. Phys., 14, 317–398, https://doi.org/10.5194/acp-14-317-2014, https://doi.org/10.5194/acp-14-317-2014, 2014
A. T. Brown, M. P. Chipperfield, N. A. D. Richards, C. Boone, and P. F. Bernath
Atmos. Chem. Phys., 14, 267–282, https://doi.org/10.5194/acp-14-267-2014, https://doi.org/10.5194/acp-14-267-2014, 2014
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
S. S. Dhomse, M. P. Chipperfield, W. Feng, W. T. Ball, Y. C. Unruh, J. D. Haigh, N. A. Krivova, S. K. Solanki, and A. K. Smith
Atmos. Chem. Phys., 13, 10113–10123, https://doi.org/10.5194/acp-13-10113-2013, https://doi.org/10.5194/acp-13-10113-2013, 2013
R. Locatelli, P. Bousquet, F. Chevallier, A. Fortems-Cheney, S. Szopa, M. Saunois, A. Agusti-Panareda, D. Bergmann, H. Bian, P. Cameron-Smith, M. P. Chipperfield, E. Gloor, S. Houweling, S. R. Kawa, M. Krol, P. K. Patra, R. G. Prinn, M. Rigby, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 9917–9937, https://doi.org/10.5194/acp-13-9917-2013, https://doi.org/10.5194/acp-13-9917-2013, 2013
A. T. Brown, M. P. Chipperfield, S. Dhomse, C. Boone, and P. F. Bernath
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-23491-2013, https://doi.org/10.5194/acpd-13-23491-2013, 2013
Revised manuscript has not been submitted
P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, Emma C. Leedham Elvidge, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-20611-2013, https://doi.org/10.5194/acpd-13-20611-2013, 2013
Revised manuscript not accepted
S. Kreycy, C. Camy-Peyret, M. P. Chipperfield, M. Dorf, W. Feng, R. Hossaini, L. Kritten, B. Werner, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 6263–6274, https://doi.org/10.5194/acp-13-6263-2013, https://doi.org/10.5194/acp-13-6263-2013, 2013
N. H. Savage, P. Agnew, L. S. Davis, C. Ordóñez, R. Thorpe, C. E. Johnson, F. M. O'Connor, and M. Dalvi
Geosci. Model Dev., 6, 353–372, https://doi.org/10.5194/gmd-6-353-2013, https://doi.org/10.5194/gmd-6-353-2013, 2013
N. A. D. Richards, S. R. Arnold, M. P. Chipperfield, G. Miles, A. Rap, R. Siddans, S. A. Monks, and M. J. Hollaway
Atmos. Chem. Phys., 13, 2331–2345, https://doi.org/10.5194/acp-13-2331-2013, https://doi.org/10.5194/acp-13-2331-2013, 2013
D. A. Belikov, S. Maksyutov, M. Krol, A. Fraser, M. Rigby, H. Bian, A. Agusti-Panareda, D. Bergmann, P. Bousquet, P. Cameron-Smith, M. P. Chipperfield, A. Fortems-Cheiney, E. Gloor, K. Haynes, P. Hess, S. Houweling, S. R. Kawa, R. M. Law, Z. Loh, L. Meng, P. I. Palmer, P. K. Patra, R. G. Prinn, R. Saito, and C. Wilson
Atmos. Chem. Phys., 13, 1093–1114, https://doi.org/10.5194/acp-13-1093-2013, https://doi.org/10.5194/acp-13-1093-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Development of a detailed gaseous oxidation scheme of naphthalene for SOA formation and speciation
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Enhancing Long-Term Trend Simulation of Global Tropospheric OH and Its Drivers from 2005–2019: A Synergistic Integration of Model Simulations and Satellite Observations
Large contribution of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
NOx emissions in France in 2019–2021 as estimated by the high spatial resolution assimilation of TROPOMI NO2 observations
Estimating NOx emissions of stack plumes using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
Revisiting day-of-week ozone patterns in an era of evolving US air quality
Changes in South American Surface Ozone Trends: Exploring the Influences of Precursors and Extreme Events
Air quality and radiative impacts of downward-propagating sudden stratospheric warmings (SSWs)
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
Investigating the differences in calculating global mean surface CO2 abundance: the impact of analysis methodologies and site selection
Meteorological characteristics of extreme ozone pollution events in China and their future predictions
Evaluating modelled tropospheric columns of CH4, CO, and O3 in the Arctic using ground-based Fourier transform infrared (FTIR) measurements
Evaluation of modelled versus observed NMVOC compounds at EMEP sites in Europe
The high-resolution Global Aviation emissions Inventory based on ADS-B (GAIA) for 2019–2021
Zonal variability of methane trends derived from satellite data
Weekly derived top-down volatile-organic-compound fluxes over Europe from TROPOMI HCHO data from 2018 to 2021
Revealing the significant acceleration of Hydrofluorocarbon (HFCs) emissions in eastern Asia through long-term atmospheric observations
Current status of model predictions of volatile organic compounds and impacts on surface ozone predictions during summer in China
Utility of Geostationary Lightning Mapper-derived lightning NO emission estimates in air quality modeling studies
Constraint of non-methane volatile organic compound emissions with TROPOMI HCHO observations and its impact on summertime surface ozone simulation over China
The suitability of atmospheric oxygen measurements to constrain western European fossil-fuel CO2 emissions and their trends
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Future tropospheric ozone budget and distribution over east Asia under a net-zero scenario
Why Did Ozone Concentrations Increase During Shanghai’s Static Management? A Statistical and Radical Chemistry Perspective
Comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA: implications for atmospheric oxidative capacity
Insights into soil NO emissions and the contribution to surface ozone formation in China
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
Aggravated surface O3 pollution primarily driven by meteorological variation in China during the early COVID-19 pandemic lockdown period
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
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Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
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Chemistry–climate models show biases compared to surface ozone observations and thus require bias correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Victor Lannuque and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2024-711, https://doi.org/10.5194/egusphere-2024-711, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH including kinetic and mechanistic data and able to reproduce most of the experimentally identified products in both gas and particle phases.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
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In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
EGUsphere, https://doi.org/10.5194/egusphere-2024-410, https://doi.org/10.5194/egusphere-2024-410, 2024
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We explore a new method to make use of the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, along with MERRA2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-359, https://doi.org/10.5194/egusphere-2024-359, 2024
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By using an updated soil reactive nitrogen emission scheme in the UI-WRF-Chem model, we investigate the underappreciated role of soil NO and HONO (Nr) emissions on air quality and temperature rise in North China. The significant contributions of soil Nr emissions to O3 and secondary pollutants, exceeding the effects of soil NOx or HONO emission alone. And soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
EGUsphere, https://doi.org/10.5194/egusphere-2024-103, https://doi.org/10.5194/egusphere-2024-103, 2024
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Over 2019–2021, our study used satellite data to assess NOx emissions in France. National budgets decreased due to effective policies, but COVID-19 lockdowns in 2020 didn't uniformly reduce emissions. Focusing on urban areas revealed varied impacts, with challenges like cloud coverage and model errors limiting precision. These findings contribute valuable insights into factors influencing emission assessments, informing future research.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
EGUsphere, https://doi.org/10.5194/egusphere-2023-2519, https://doi.org/10.5194/egusphere-2023-2519, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen-dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
EGUsphere, https://doi.org/10.5194/egusphere-2024-328, https://doi.org/10.5194/egusphere-2024-328, 2024
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Our research found that surface ozone trends in major South American cities increase or remain steady but show no signs of decreasing. Extra-tropical cities (Santiago and São Paulo), in particular, face the highest risk of ozone exposure. Furthermore, we found that prolonged heat waves and large fires explain many of the most extreme ozone values.
Ryan S. Williams, Michaela I. Hegglin, Patrick Jöckel, Hella Garny, and Keith P. Shine
Atmos. Chem. Phys., 24, 1389–1413, https://doi.org/10.5194/acp-24-1389-2024, https://doi.org/10.5194/acp-24-1389-2024, 2024
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During winter, a brief but abrupt reversal of the mean stratospheric westerly flow (~30 km high) around the Arctic occurs ~6 times a decade. Using a chemistry–climate model, about half of these events are shown to induce large anomalies in Arctic ozone (>25 %) and water vapour (>±25 %) around ~8–12 km altitude for up to 2–3 months, important for weather forecasting. We also calculate a doubling to trebling of the risk in breaches of mid-latitude surface air quality (ozone) standards (~60 ppbv).
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Zhendong Wu, Alex Vermeulen, Yousuke Sawa, Ute Karstens, Wouter Peters, Remco de Kok, Xin Lan, Yasuyuki Nagai, Akinori Ogi, and Oksana Tarasova
Atmos. Chem. Phys., 24, 1249–1264, https://doi.org/10.5194/acp-24-1249-2024, https://doi.org/10.5194/acp-24-1249-2024, 2024
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This study focuses on exploring the differences in calculating global surface CO2 and its growth rate, considering the impact of analysis methodologies and site selection. Our study reveals that the current global CO2 network has a good capacity to represent global surface CO2 and its growth rate, as well as trends in atmospheric CO2 mass changes. However, small differences exist in different analyses due to the impact of methodology and site selection.
Yang Yang, Yang Zhou, Hailong Wang, Mengyun Li, Huimin Li, Pinya Wang, Xu Yue, Ke Li, Jia Zhu, and Hong Liao
Atmos. Chem. Phys., 24, 1177–1191, https://doi.org/10.5194/acp-24-1177-2024, https://doi.org/10.5194/acp-24-1177-2024, 2024
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This study reveals that extreme ozone pollution over the North China Plain and Yangtze River Delta is due to the chemical production related to hot and dry conditions, and the regional transport explains the ozone pollution over the Sichuan Basin and Pearl River Delta. The frequency of meteorological conditions of the extreme ozone pollution increases from the past to the future. The sustainable scenario is the optimal path to retaining clean air in China in the future.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
Atmos. Chem. Phys., 24, 1079–1118, https://doi.org/10.5194/acp-24-1079-2024, https://doi.org/10.5194/acp-24-1079-2024, 2024
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models generally underpredict the concentrations of these gases in the Arctic troposphere.
Yao Ge, Sverre Solberg, Mathew Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
EGUsphere, https://doi.org/10.5194/egusphere-2023-3102, https://doi.org/10.5194/egusphere-2023-3102, 2024
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Atmospheric volatile organic compounds (VOC) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species, and underscore potential inaccuracies in total and sector-specific emission estimates.
Roger Teoh, Zebediah Engberg, Marc Shapiro, Lynnette Dray, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 725–744, https://doi.org/10.5194/acp-24-725-2024, https://doi.org/10.5194/acp-24-725-2024, 2024
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Emissions from aircraft contribute to climate change and degrade air quality. We describe an up-to-date 4D emissions inventory of global aviation from 2019 to 2021 based on actual flown trajectories. In 2019, 40.2 million flights collectively travelled 61 billion kilometres using 283 Tg of fuel. Long-haul flights were responsible for 43 % of CO2. The emissions inventory is made available for use in future studies to evaluate the negative externalities arising from global aviation.
Jonas Hachmeister, Oliver Schneising, Michael Buchwitz, John P. Burrows, Justus Notholt, and Matthias Buschmann
Atmos. Chem. Phys., 24, 577–595, https://doi.org/10.5194/acp-24-577-2024, https://doi.org/10.5194/acp-24-577-2024, 2024
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We quantified changes in atmospheric methane concentrations using satellite data and a dynamic linear model approach. We calculated global annual methane increases for the years 2019–2022, which are in good agreement with other sources. For zonal methane growth rates, we identified strong inter-hemispheric differences in 2019 and 2022. For 2022, we could attribute decreases in the global growth rate to the Northern Hemisphere, possibly related to a reduction in anthropogenic emissions.
Glenn-Michael Oomen, Jean-François Müller, Trissevgeni Stavrakou, Isabelle De Smedt, Thomas Blumenstock, Rigel Kivi, Maria Makarova, Mathias Palm, Amelie Röhling, Yao Té, Corinne Vigouroux, Martina M. Friedrich, Udo Frieß, François Hendrick, Alexis Merlaud, Ankie Piters, Andreas Richter, Michel Van Roozendael, and Thomas Wagner
Atmos. Chem. Phys., 24, 449–474, https://doi.org/10.5194/acp-24-449-2024, https://doi.org/10.5194/acp-24-449-2024, 2024
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Natural emissions from vegetation have a profound impact on air quality for their role in the formation of harmful tropospheric ozone and organic aerosols, yet these emissions are highly uncertain. In this study, we quantify emissions of organic gases over Europe using high-quality satellite measurements of formaldehyde. These satellite observations suggest that emissions from vegetation are much higher than predicted by models, especially in southern Europe.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Tompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistari J. Manning, and Sunyoung Park
EGUsphere, https://doi.org/10.5194/egusphere-2023-3144, https://doi.org/10.5194/egusphere-2023-3144, 2024
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We analyzed with an inversion model the atmospheric abundance of HFCs, potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
Yongliang She, Jingyi Li, Xiaopu Lyu, Hai Guo, Momei Qin, Xiaodong Xie, Kangjia Gong, Fei Ye, Jianjiong Mao, Lin Huang, and Jianlin Hu
Atmos. Chem. Phys., 24, 219–233, https://doi.org/10.5194/acp-24-219-2024, https://doi.org/10.5194/acp-24-219-2024, 2024
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In this study, we use multi-site volatile organic compound (VOC) measurements to evaluate the CMAQ-model-predicted VOCs and assess the impacts of VOC bias on O3 simulation. Our results demonstrate that current modeling setups and emission inventories are likely to underpredict VOC concentrations, and this underprediction of VOCs contributes to lower O3 predictions in China.
Peiyang Cheng, Arastoo Pour-Biazar, Yuling Wu, Shi Kuang, Richard T. McNider, and William J. Koshak
Atmos. Chem. Phys., 24, 41–63, https://doi.org/10.5194/acp-24-41-2024, https://doi.org/10.5194/acp-24-41-2024, 2024
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Lightning-induced nitrogen monoxide (LNO) emission can be estimated from geostationary satellite observations. The present study uses the LNO emission estimates derived from geostationary satellite observations in an air quality modeling system to investigate the impact of LNO on air quality. Results indicate that significant ozone increase could be due to long-distance chemical transport, lightning activity in the upwind direction, and the mixing of high LNO (or ozone) plumes.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
EGUsphere, https://doi.org/10.5194/egusphere-2023-2654, https://doi.org/10.5194/egusphere-2023-2654, 2024
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We developed a multi-air pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Christian Rödenbeck, Karina E. Adcock, Markus Eritt, Maksym Gachkivskyi, Christoph Gerbig, Samuel Hammer, Armin Jordan, Ralph F. Keeling, Ingeborg Levin, Fabian Maier, Andrew C. Manning, Heiko Moossen, Saqr Munassar, Penelope A. Pickers, Michael Rothe, Yasunori Tohjima, and Sönke Zaehle
Atmos. Chem. Phys., 23, 15767–15782, https://doi.org/10.5194/acp-23-15767-2023, https://doi.org/10.5194/acp-23-15767-2023, 2023
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The carbon dioxide content of the Earth atmosphere is increasing due to human emissions from burning of fossil fuels, causing global climate change. The strength of the fossil-fuel emissions is estimated by inventories based on energy data, but independent validation of these inventories has been recommended by the Intergovernmental Panel on Climate Change. Here we investigate the potential to validate inventories based on measurements of small changes in the atmospheric oxygen content.
Xiaohong Yao and Leiming Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2968, https://doi.org/10.5194/egusphere-2023-2968, 2023
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and (NO2+O3) measured in ten Canadian cities during the last two to three decades and associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, and changes in O3 sources and sinks.
Xuewei Hou, Oliver Wild, Bin Zhu, and James Lee
Atmos. Chem. Phys., 23, 15395–15411, https://doi.org/10.5194/acp-23-15395-2023, https://doi.org/10.5194/acp-23-15395-2023, 2023
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In response to the climate crisis, many countries have committed to net zero in a certain future year. The impacts of net-zero scenarios on tropospheric O3 are less well studied and remain unclear. In this study, we quantified the changes of tropospheric O3 budgets, spatiotemporal distributions of future surface O3 in east Asia and regional O3 source contributions for 2060 under a net-zero scenario using the NCAR Community Earth System Model (CESM) and online O3-tagging methods.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
EGUsphere, https://doi.org/10.5194/egusphere-2023-2142, https://doi.org/10.5194/egusphere-2023-2142, 2023
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a change to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Meghna Soni, Rolf Sander, Lokesh K. Sahu, Domenico Taraborrelli, Pengfei Liu, Ankit Patel, Imran A. Girach, Andrea Pozzer, Sachin S. Gunthe, and Narendra Ojha
Atmos. Chem. Phys., 23, 15165–15180, https://doi.org/10.5194/acp-23-15165-2023, https://doi.org/10.5194/acp-23-15165-2023, 2023
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The study presents the implementation of comprehensive multiphase chlorine chemistry in the box model CAABA/MECCA. Simulations for contrasting urban environments of Asia and Europe highlight the significant impacts of chlorine on atmospheric oxidation capacity and composition. Chemical processes governing the production and loss of chlorine-containing species has been discussed. The updated chemical mechanism will be useful to interpret field measurements and for future air quality studies.
Ling Huang, Jiong Fang, Jiaqiang Liao, Greg Yarwood, Hui Chen, Yangjun Wang, and Li Li
Atmos. Chem. Phys., 23, 14919–14932, https://doi.org/10.5194/acp-23-14919-2023, https://doi.org/10.5194/acp-23-14919-2023, 2023
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Surface ozone concentrations have emerged as a major environmental issue in China. Although control strategies aimed at reducing NOx emissions from conventional combustion sources are widely recognized, soil NOx emissions have received little attention. The impact of soil NO emissions on ground-level ozone concentration is yet to be evaluated. In this study, we estimated the soil NO emissions and evaluated its impact on ozone formation in China.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
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Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
EGUsphere, https://doi.org/10.5194/egusphere-2023-2723, https://doi.org/10.5194/egusphere-2023-2723, 2023
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In contrast with the past work showing the reduction of emission as the dominant factor for nation-wide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) and calibrated with surface observation.
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