Articles | Volume 23, issue 23
https://doi.org/10.5194/acp-23-14735-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-14735-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
29 Nov 2023
Research article |
| 29 Nov 2023
| 29 Nov 2023
Development, intercomparison, and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
Ben A. Cala
CORRESPONDING AUTHOR
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
now at: Department of Ocean Systems (OCS), NIOZ Royal Netherlands Institute for Sea Research, Texel, the Netherlands
Scott Archer-Nicholls
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
now at: IT Services, University of Manchester, Manchester, M13 9PL, UK
James Weber
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
now at: School of Biosciences, University of Sheffield, Sheffield, S10 2TN, UK
N. Luke Abraham
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
National Centre for Atmospheric Science, Cambridge, CB2 1EW, UK
Paul T. Griffiths
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
National Centre for Atmospheric Science, Cambridge, CB2 1EW, UK
Lorrie Jacob
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
Y. Matthew Shin
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
Laura E. Revell
School of Physical and Chemical Sciences, University of Canterbury, Christchurch, New Zealand
Matthew Woodhouse
CSIRO Oceans and Atmosphere, Aspendale, 3195, Australia
Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
National Centre for Atmospheric Science, Cambridge, CB2 1EW, UK
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Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-73, https://doi.org/10.5194/gmd-2024-73, 2024
Preprint under review for GMD
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Observational data and modelling capabilities are expanding in recent years, but there are still barriers preventing these two data sources to be used in synergy. Proper comparison requires generating, storing and handling a large amount of data. This manuscript describes the first step in the development of a new set of software tools, the ‘VISION toolkit’, which can enable the easy and efficient integration of observational and model data required for model evaluation.
Lauren R. Marshall, Anja Schmidt, Andrew P. Schurer, Nathan Luke Abraham, Lucie J. Lücke, Rob Wilson, Kevin Anchukaitis, Gabriele Hegerl, Ben Johnson, Bette L. Otto-Bliesner, Esther C. Brady, Myriam Khodri, and Kohei Yoshida
EGUsphere, https://doi.org/10.5194/egusphere-2024-1322, https://doi.org/10.5194/egusphere-2024-1322, 2024
This preprint is open for discussion and under review for Climate of the Past (CP).
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Large volcanic eruptions have caused temperature deviations over the past 1000 years, however climate model results and reconstructions of surface cooling using tree-rings do not match. We explore this mismatch using the latest models and find a better match to tree-ring reconstructions for some eruptions. Our results show that the way in which eruptions are simulated in models matters for the comparison to tree-rings, particularly regarding the spatial spread of volcanic aerosol.
Sonya L. Fiddes, Marc D. Mallet, Alain Protat, Matthew T. Woodhouse, Simon P. Alexander, and Kalli Furtado
Geosci. Model Dev., 17, 2641–2662, https://doi.org/10.5194/gmd-17-2641-2024, https://doi.org/10.5194/gmd-17-2641-2024, 2024
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In this study we present an evaluation that considers complex, non-linear systems in a holistic manner. This study uses XGBoost, a machine learning algorithm, to predict the simulated Southern Ocean shortwave radiation bias in the ACCESS model using cloud property biases as predictors. We then used a novel feature importance analysis to quantify the role that each cloud bias plays in predicting the radiative bias, laying the foundation for advanced Earth system model evaluation and development.
Stephanie Fiedler, Vaishali Naik, Fiona M. O'Connor, Christopher J. Smith, Paul Griffiths, Ryan J. Kramer, Toshihiko Takemura, Robert J. Allen, Ulas Im, Matthew Kasoar, Angshuman Modak, Steven Turnock, Apostolos Voulgarakis, Duncan Watson-Parris, Daniel M. Westervelt, Laura J. Wilcox, Alcide Zhao, William J. Collins, Michael Schulz, Gunnar Myhre, and Piers M. Forster
Geosci. Model Dev., 17, 2387–2417, https://doi.org/10.5194/gmd-17-2387-2024, https://doi.org/10.5194/gmd-17-2387-2024, 2024
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Climate scientists want to better understand modern climate change. Thus, climate model experiments are performed and compared. The results of climate model experiments differ, as assessed in the latest Intergovernmental Panel on Climate Change (IPCC) assessment report. This article gives insights into the challenges and outlines opportunities for further improving the understanding of climate change. It is based on views of a group of experts in atmospheric composition–climate interactions.
James A. King, James Weber, Peter Lawrence, Stephanie Roe, Abigail L. S. Swann, and Maria Val Martin
EGUsphere, https://doi.org/10.5194/egusphere-2024-710, https://doi.org/10.5194/egusphere-2024-710, 2024
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Tackling climate change by adding, restoring, or enhancing forests is gaining global support. However, it’s important to investigate the broader implications of this. We used a computer model of the Earth to investigate a future where tree cover expanded as much as possible. We found that some tropical areas were cooler because of trees pumping water into the atmosphere, but this also led to soil and rivers drying. This is important because it might be harder to maintain the forests as a result.
Lorrie Simone Denise Jacob, Chiara Giorio, and Alexander Thomas Archibald
Atmos. Chem. Phys., 24, 3329–3347, https://doi.org/10.5194/acp-24-3329-2024, https://doi.org/10.5194/acp-24-3329-2024, 2024
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Recent studies on DMS have provided new challenges to our mechanistic understanding. Here we synthesise a number of recent studies to further develop and extend a state-of-the-art mechanism. Our new mechanism is shown to outperform all existing mechanisms when compared over a wide set of conditions. The development of an improved DMS mechanism will help lead the way to better the understanding the climate impacts of DMS emissions in past, present, and future atmospheric conditions.
Alexander T. Archibald, Bablu Sinha, Maria Russo, Emily Matthews, Freya Squires, N. Luke Abraham, Stephane Bauguitte, Thomas Bannan, Thomas Bell, David Berry, Lucy Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Ben I. Moat, Katie Read, Chris Reed, Malcolm Roberts, Reinhard Schiemann, David Schroeder, Tim Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Ming-Xi Yang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-405, https://doi.org/10.5194/essd-2023-405, 2024
Preprint under review for ESSD
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Here we present an overview of the data generated as part of the North Atlantic Climate System Integrated Studies (ACSIS) programme which are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA, www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC, bodc.ac.uk). ACSIS data cover the full North Atlantic System comprising: the North Atlantic Ocean, the atmosphere above it including its composition, Arctic Sea Ice and the Greenland Ice Sheet.
Dongqi Lin, Jiawei Zhang, Basit Khan, Marwan Katurji, and Laura E. Revell
Geosci. Model Dev., 17, 815–845, https://doi.org/10.5194/gmd-17-815-2024, https://doi.org/10.5194/gmd-17-815-2024, 2024
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GEO4PALM is an open-source tool to generate static input for the Parallelized Large-Eddy Simulation (PALM) model system. Geospatial static input is essential for realistic PALM simulations. However, existing tools fail to generate PALM's geospatial static input for most regions. GEO4PALM is compatible with diverse geospatial data sources and provides access to free data sets. In addition, this paper presents two application examples, which show successful PALM simulations using GEO4PALM.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Dongqi Lin, Marwan Katurji, Laura E. Revell, Basit Khan, and Andrew Sturman
Atmos. Chem. Phys., 23, 14451–14479, https://doi.org/10.5194/acp-23-14451-2023, https://doi.org/10.5194/acp-23-14451-2023, 2023
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Accurate fog forecasting is difficult in a complex environment. Spatial variations in soil moisture could impact fog. Here, we carried out fog simulations with spatially different soil moisture in complex topography. The soil moisture was calculated using satellite observations. The results show that the spatial variations in soil moisture do not have a significant impact on where fog occurs but do impact how long fog lasts. This finding could improve fog forecasts in the future.
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.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
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A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Laura J. Wilcox, Robert J. Allen, Bjørn H. Samset, Massimo A. Bollasina, Paul T. Griffiths, James Keeble, Marianne T. Lund, Risto Makkonen, Joonas Merikanto, Declan O'Donnell, David J. Paynter, Geeta G. Persad, Steven T. Rumbold, Toshihiko Takemura, Kostas Tsigaridis, Sabine Undorf, and Daniel M. Westervelt
Geosci. Model Dev., 16, 4451–4479, https://doi.org/10.5194/gmd-16-4451-2023, https://doi.org/10.5194/gmd-16-4451-2023, 2023
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Changes in anthropogenic aerosol emissions have strongly contributed to global and regional climate change. However, the size of these regional impacts and the way they arise are still uncertain. With large changes in aerosol emissions a possibility over the next few decades, it is important to better quantify the potential role of aerosol in future regional climate change. The Regional Aerosol Model Intercomparison Project will deliver experiments designed to facilitate this.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
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Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
James Weber, James A. King, Katerina Sindelarova, and Maria Val Martin
Geosci. Model Dev., 16, 3083–3101, https://doi.org/10.5194/gmd-16-3083-2023, https://doi.org/10.5194/gmd-16-3083-2023, 2023
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The emissions of volatile organic compounds from vegetation (BVOCs) influence atmospheric composition and contribute to certain gases and aerosols (tiny airborne particles) which play a role in climate change. BVOC emissions are likely to change in the future due to changes in climate and land use. Therefore, accurate simulation of BVOC emission is important, and this study describes an update to the simulation of BVOC emissions in the United Kingdom Earth System Model (UKESM).
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
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The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 3609–3627, https://doi.org/10.5194/acp-23-3609-2023, https://doi.org/10.5194/acp-23-3609-2023, 2023
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We use a machine learning technique called Gaussian mixture modeling (GMM) to classify vertical ozone profiles into groups based on how the ozone concentration changes with pressure. Even though the GMM algorithm was not provided with spatial information, the classes are geographically coherent. We also detect signatures of tropical broadening in UKESM1 future climate scenarios. GMM may be useful for understanding ozone structures in modeled and observed datasets.
Sonya L. Fiddes, Alain Protat, Marc D. Mallet, Simon P. Alexander, and Matthew T. Woodhouse
Atmos. Chem. Phys., 22, 14603–14630, https://doi.org/10.5194/acp-22-14603-2022, https://doi.org/10.5194/acp-22-14603-2022, 2022
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Climate models have difficulty simulating Southern Ocean clouds, impacting how much sunlight reaches the surface. We use machine learning to group different cloud types observed from satellites and simulated in a climate model. We find the model does a poor job of simulating the same cloud type as what the satellite shows and, even when it does, the cloud properties and amount of reflected sunlight are incorrect. We have a lot of work to do to model clouds correctly over the Southern Ocean.
Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Archer-Nicholls, Steve Dorling, Claire E. Reeves, and Tim Butler
Atmos. Chem. Phys., 22, 13797–13815, https://doi.org/10.5194/acp-22-13797-2022, https://doi.org/10.5194/acp-22-13797-2022, 2022
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As ozone can be transported across countries, efficient air quality management and regulatory policies rely on the assessment of local ozone production vs. transport. In our study, we investigate the origin of surface ozone in the UK and the contribution of the different source regions to regulatory ozone metrics. It is shown that emission controls would be necessary over western Europe to improve health-related metrics and over larger areas to reduce impacts on ecosystems.
Ashok K. Luhar, Ian E. Galbally, and Matthew T. Woodhouse
Atmos. Chem. Phys., 22, 13013–13033, https://doi.org/10.5194/acp-22-13013-2022, https://doi.org/10.5194/acp-22-13013-2022, 2022
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Recent improvements to global parameterisations of oceanic ozone dry deposition and lightning-generated oxides of nitrogen (LNOx) have consequent impacts on earth's radiative fluxes. Uncertainty in radiative fluxes arising from uncertainty in LNOx is of significant magnitude in comparison with the
present-dayIPCC AR6 anthropogenic effective radiative forcing (ERF) due to ozone. Hence, uncertainty in LNOx needs to be explicitly addressed in relation to the GWP and ERF of anthropogenic methane.
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.
Le Yuan, Olalekan A. M. Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys., 22, 8617–8637, https://doi.org/10.5194/acp-22-8617-2022, https://doi.org/10.5194/acp-22-8617-2022, 2022
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Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing inventories using air quality models and routine in situ observations. Using this approach, we derived improved estimates of NOx emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Alex R. Aves, Laura E. Revell, Sally Gaw, Helena Ruffell, Alex Schuddeboom, Ngaire E. Wotherspoon, Michelle LaRue, and Adrian J. McDonald
The Cryosphere, 16, 2127–2145, https://doi.org/10.5194/tc-16-2127-2022, https://doi.org/10.5194/tc-16-2127-2022, 2022
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This study confirms the presence of microplastics in Antarctic snow, highlighting the extent of plastic pollution globally. Fresh snow was collected from Ross Island, Antarctica, and subsequent analysis identified an average of 29 microplastic particles per litre of melted snow. The most likely source of these airborne microplastics is local scientific research stations; however, modelling shows their origin could have been up to 6000 km away.
Sonya L. Fiddes, Matthew T. Woodhouse, Steve Utembe, Robyn Schofield, Simon P. Alexander, Joel Alroe, Scott D. Chambers, Zhenyi Chen, Luke Cravigan, Erin Dunne, Ruhi S. Humphries, Graham Johnson, Melita D. Keywood, Todd P. Lane, Branka Miljevic, Yuko Omori, Alain Protat, Zoran Ristovski, Paul Selleck, Hilton B. Swan, Hiroshi Tanimoto, Jason P. Ward, and Alastair G. Williams
Atmos. Chem. Phys., 22, 2419–2445, https://doi.org/10.5194/acp-22-2419-2022, https://doi.org/10.5194/acp-22-2419-2022, 2022
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Coral reefs have been found to produce the climatically relevant chemical compound dimethyl sulfide (DMS). It has been suggested that corals can modify their environment via the production of DMS. We use an atmospheric chemistry model to test this theory at a regional scale for the first time. We find that it is unlikely that coral-reef-derived DMS has an influence over local climate, in part due to the proximity to terrestrial and anthropogenic aerosol sources.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, https://doi.org/10.5194/acp-21-15901-2021, 2021
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Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 13011–13018, https://doi.org/10.5194/acp-21-13011-2021, https://doi.org/10.5194/acp-21-13011-2021, 2021
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The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
John Staunton-Sykes, Thomas J. Aubry, Youngsub M. Shin, James Weber, Lauren R. Marshall, Nathan Luke Abraham, Alex Archibald, and Anja Schmidt
Atmos. Chem. Phys., 21, 9009–9029, https://doi.org/10.5194/acp-21-9009-2021, https://doi.org/10.5194/acp-21-9009-2021, 2021
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
Dongqi Lin, Basit Khan, Marwan Katurji, Leroy Bird, Ricardo Faria, and Laura E. Revell
Geosci. Model Dev., 14, 2503–2524, https://doi.org/10.5194/gmd-14-2503-2021, https://doi.org/10.5194/gmd-14-2503-2021, 2021
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We present an open-source toolbox WRF4PALM, which enables weather dynamics simulation within urban landscapes. WRF4PALM passes meteorological information from the popular Weather Research and Forecasting (WRF) model to the turbulence-resolving PALM model system 6.0. WRF4PALM can potentially extend the use of WRF and PALM with realistic boundary conditions to any part of the world. WRF4PALM will help study air pollution dispersion, wind energy prospecting, and high-impact wind forecasting.
Sonya L. Fiddes, Matthew T. Woodhouse, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 21, 5883–5903, https://doi.org/10.5194/acp-21-5883-2021, https://doi.org/10.5194/acp-21-5883-2021, 2021
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Coral reefs are known to produce the aerosol precursor dimethyl sulfide (DMS). Currently, this source of coral DMS is unaccounted for in climate modelling, and the impact of coral reef extinction on aerosol and climate is unknown. In this study, we address this problem using a coupled chemistry–climate model for the first time. We find that coral reefs make a minimal contribution to the aerosol population and are unlikely to play a role in climate modulation.
James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
Atmos. Chem. Phys., 21, 5015–5061, https://doi.org/10.5194/acp-21-5015-2021, https://doi.org/10.5194/acp-21-5015-2021, 2021
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Stratospheric ozone and water vapour are key components of the Earth system; changes to both have important impacts on global and regional climate. We evaluate changes to these species from 1850 to 2100 in the new generation of CMIP6 models. There is good agreement between the multi-model mean and observations, although there is substantial variation between the individual models. The future evolution of both ozone and water vapour is strongly dependent on the assumed future emissions scenario.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
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The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
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This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Gillian Thornhill, William Collins, Dirk Olivié, Ragnhild B. Skeie, Alex Archibald, Susanne Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry Horowitz, Jean-Francois Lamarque, Martine Michou, Jane Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M. O'Connor, Fabien Paulot, Michael Schulz, Catherine E. Scott, Roland Séférian, Chris Smith, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, and James Weber
Atmos. Chem. Phys., 21, 1105–1126, https://doi.org/10.5194/acp-21-1105-2021, https://doi.org/10.5194/acp-21-1105-2021, 2021
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We find that increased temperatures affect aerosols and reactive gases by changing natural emissions and their rates of removal from the atmosphere. Changing the composition of these species in the atmosphere affects the radiative budget of the climate system and therefore amplifies or dampens the climate response of climate models of the Earth system. This study found that the largest effect is a dampening of climate change as warmer temperatures increase the emissions of cooling aerosols.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Jane P. Mulcahy, Colin Johnson, Colin G. Jones, Adam C. Povey, Catherine E. Scott, Alistair Sellar, Steven T. Turnock, Matthew T. Woodhouse, Nathan Luke Abraham, Martin B. Andrews, Nicolas Bellouin, Jo Browse, Ken S. Carslaw, Mohit Dalvi, Gerd A. Folberth, Matthew Glover, Daniel P. Grosvenor, Catherine Hardacre, Richard Hill, Ben Johnson, Andy Jones, Zak Kipling, Graham Mann, James Mollard, Fiona M. O'Connor, Julien Palmiéri, Carly Reddington, Steven T. Rumbold, Mark Richardson, Nick A. J. Schutgens, Philip Stier, Marc Stringer, Yongming Tang, Jeremy Walton, Stephanie Woodward, and Andrew Yool
Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, https://doi.org/10.5194/gmd-13-6383-2020, 2020
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Aerosols are an important component of the Earth system. Here, we comprehensively document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 and UKESM1. This study provides a useful characterisation of the aerosol climatology in both models, facilitating the understanding of the numerous aerosol–climate interaction studies that will be conducted for CMIP6 and beyond.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
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Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
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Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Rebecca L. Jackson, Albert J. Gabric, Roger Cropp, and Matthew T. Woodhouse
Biogeosciences, 17, 2181–2204, https://doi.org/10.5194/bg-17-2181-2020, https://doi.org/10.5194/bg-17-2181-2020, 2020
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Coral reefs are a strong source of atmospheric sulfur through stress-induced emissions of dimethylsulfide (DMS). This biogenic sulfur can influence aerosol and cloud properties and, consequently, the radiative balance over the ocean. DMS emissions may therefore help to mitigate coral physiological stress via increased low-level cloud cover and reduced sea surface temperature. The importance of DMS in coral physiology and climate is reviewed and the implications for coral bleaching are discussed.
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.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Ying Chen, Oliver Wild, Edmund Ryan, Saroj Kumar Sahu, Douglas Lowe, Scott Archer-Nicholls, Yu Wang, Gordon McFiggans, Tabish Ansari, Vikas Singh, Ranjeet S. Sokhi, Alex Archibald, and Gufran Beig
Atmos. Chem. Phys., 20, 499–514, https://doi.org/10.5194/acp-20-499-2020, https://doi.org/10.5194/acp-20-499-2020, 2020
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PM2.5 and O3 are two major air pollutants. Some mitigation strategies focusing on reducing PM2.5 may lead to substantial increase in O3. We use statistical emulation combined with atmospheric transport model to perform thousands of sensitivity numerical studies to identify the major sources of PM2.5 and O3 and to develop strategies targeted at both pollutants. Our scientific evidence suggests that regional coordinated emission control is required to mitigate PM2.5 whilst preventing O3 increase.
Le Kuai, Kevin W. Bowman, Kazuyuki Miyazaki, Makoto Deushi, Laura Revell, Eugene Rozanov, Fabien Paulot, Sarah Strode, Andrew Conley, Jean-François Lamarque, Patrick Jöckel, David A. Plummer, Luke D. Oman, Helen Worden, Susan Kulawik, David Paynter, Andrea Stenke, and Markus Kunze
Atmos. Chem. Phys., 20, 281–301, https://doi.org/10.5194/acp-20-281-2020, https://doi.org/10.5194/acp-20-281-2020, 2020
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The tropospheric ozone increase from pre-industrial to the present day leads to a radiative forcing. The top-of-atmosphere outgoing fluxes at the ozone band are controlled by ozone, water vapor, and temperature. We demonstrate a method to attribute the models’ flux biases to these key players using satellite-constrained instantaneous radiative kernels. The largest spread between models is found in the tropics, mainly driven by ozone and then water vapor.
Laura E. Revell, Stefanie Kremser, Sean Hartery, Mike Harvey, Jane P. Mulcahy, Jonny Williams, Olaf Morgenstern, Adrian J. McDonald, Vidya Varma, Leroy Bird, and Alex Schuddeboom
Atmos. Chem. Phys., 19, 15447–15466, https://doi.org/10.5194/acp-19-15447-2019, https://doi.org/10.5194/acp-19-15447-2019, 2019
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Aerosols over the Southern Ocean consist primarily of sea salt and sulfate, yet are seasonally biased in our model. We test three sulfate chemistry schemes to investigate DMS oxidation, which forms sulfate aerosol. Simulated cloud droplet number concentrations improve using more complex sulfate chemistry. We also show that a new sea spray aerosol source function, developed from measurements made on a recent Southern Ocean research voyage, improves the model's simulation of aerosol optical depth.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
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.
Laura Kiely, Dominick V. Spracklen, Christine Wiedinmyer, Luke Conibear, Carly L. Reddington, Scott Archer-Nicholls, Douglas Lowe, Stephen R. Arnold, Christoph Knote, Md Firoz Khan, Mohd Talib Latif, Mikinori Kuwata, Sri Hapsari Budisulistiorini, and Lailan Syaufina
Atmos. Chem. Phys., 19, 11105–11121, https://doi.org/10.5194/acp-19-11105-2019, https://doi.org/10.5194/acp-19-11105-2019, 2019
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In 2015, a large fire episode occurred in Indonesia, reducing air quality. Fires occurred predominantly on peatland, where large uncertainties are associated with emissions. Current fire emissions datasets underestimate peat fire emissions. We created new fire emissions data, with data specific to Indonesian peat fires. Using these emissions in simulations of particulate matter and aerosol optical depth shows an improvement over simulations using current data, when compared with observations.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
David C. Wade, Nathan Luke Abraham, Alexander Farnsworth, Paul J. Valdes, Fran Bragg, and Alexander T. Archibald
Clim. Past, 15, 1463–1483, https://doi.org/10.5194/cp-15-1463-2019, https://doi.org/10.5194/cp-15-1463-2019, 2019
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The amount of O2 in the atmosphere may have varied from as little as 10 % to as much as 35 % during the last 541 Myr. These changes are large enough to have led to changes in atmospheric mass, which may alter the radiative budget of the atmosphere. We present the first fully 3-D numerical model simulations to investigate the climate impacts of changes in O2 during different climate states. We identify a complex new mechanism causing increases in surface temperature when O2 levels were higher.
Ewa M. Bednarz, Amanda C. Maycock, Peter Braesicke, Paul J. Telford, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 9833–9846, https://doi.org/10.5194/acp-19-9833-2019, https://doi.org/10.5194/acp-19-9833-2019, 2019
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The atmospheric response to the amplitude of 11-year solar cycle in UM-UKCA is separated into the contributions from changes in direct radiative heating and photolysis rates, and the results compared with a control case with both effects included. We find that while the tropical responses are largely additive, this is not necessarily the case in the high latitudes. We suggest that solar-induced changes in ozone are important for modulating the SH dynamical response to the 11-year solar cycle.
Zainab Q. Hakim, Scott Archer-Nicholls, Gufran Beig, Gerd A. Folberth, Kengo Sudo, Nathan Luke Abraham, Sachin Ghude, Daven K. Henze, and Alexander T. Archibald
Atmos. Chem. Phys., 19, 6437–6458, https://doi.org/10.5194/acp-19-6437-2019, https://doi.org/10.5194/acp-19-6437-2019, 2019
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Surface ozone is an important air pollutant and recent work has calculated that large numbers of people die prematurely because of exposure to high levels of surface ozone in India. However, these calculations require model simulations of ozone as key inputs.
Here we perform the most thorough evaluation of global model surface ozone over India to date. These analyses of model simulations and observations highlight some successes and shortcomings and the need for further process-based studies.
Ewa M. Bednarz, Amanda C. Maycock, Paul J. Telford, Peter Braesicke, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 5209–5233, https://doi.org/10.5194/acp-19-5209-2019, https://doi.org/10.5194/acp-19-5209-2019, 2019
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Following model improvements, the atmospheric response to the 11-year solar cycle forcing simulated in the UM-UKCA chemistry–climate model is discussed for the first time. In contrast to most previous studies in the literature, we compare the results diagnosed using both a composite and a MLR methodology, and we show that apparently different signals can be diagnosed in the troposphere. In addition, we look at the role of internal atmospheric variability for the detection of the solar response.
Fraser Dennison, James Keeble, Olaf Morgenstern, Guang Zeng, N. Luke Abraham, and Xin Yang
Geosci. Model Dev., 12, 1227–1239, https://doi.org/10.5194/gmd-12-1227-2019, https://doi.org/10.5194/gmd-12-1227-2019, 2019
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Two developments are made to the United Kingdom Chemistry and Aerosols (UKCA) model to improve simulation of stratospheric ozone. The first is the addition of a solar cycle. The influence on ozone from the solar cycle is found to be 1–2 %, which is consistent with other studies. The second is to the heterogeneous chemistry, the most significant change being the addition of reactions involving bromine species. This was shown to reduce ozone biases relative to observations in most regions.
Roland Eichinger, Simone Dietmüller, Hella Garny, Petr Šácha, Thomas Birner, Harald Bönisch, Giovanni Pitari, Daniele Visioni, Andrea Stenke, Eugene Rozanov, Laura Revell, David A. Plummer, Patrick Jöckel, Luke Oman, Makoto Deushi, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 921–940, https://doi.org/10.5194/acp-19-921-2019, https://doi.org/10.5194/acp-19-921-2019, 2019
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To shed more light upon the changes in stratospheric circulation in the 21st century, climate projection simulations of 10 state-of-the-art global climate models, spanning from 1960 to 2100, are analyzed. The study shows that in addition to changes in transport, mixing also plays an important role in stratospheric circulation and that the properties of mixing vary over time. Furthermore, the influence of mixing is quantified and a dynamical framework is provided to understand the changes.
Christa Fittschen, Mohamad Al Ajami, Sebastien Batut, Valerio Ferracci, Scott Archer-Nicholls, Alexander T. Archibald, and Coralie Schoemaecker
Atmos. Chem. Phys., 19, 349–362, https://doi.org/10.5194/acp-19-349-2019, https://doi.org/10.5194/acp-19-349-2019, 2019
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Concentrations of OH, the main oxidant in the atmosphere, were measured in biogenic environments up to a factor of 10 higher than predicted by models. This was interpreted as a major lack in our understanding of biogenic volatile organic compound chemistry. But interferences of unknown origin have also been discovered, and we present experimental and modelling evidence that the interference might be due to the unexpected decomposition of a new class of molecule, ROOOH, in the FAGE instruments.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
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Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Nathan Luke Abraham, Alexander T. Archibald, Paul Cresswell, Sam Cusworth, Mohit Dalvi, David Matthews, Steven Wardle, and Stuart Whitehouse
Geosci. Model Dev., 11, 3647–3657, https://doi.org/10.5194/gmd-11-3647-2018, https://doi.org/10.5194/gmd-11-3647-2018, 2018
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Using a virtual machine environment, a low-resolution configuration of the United Kingdom Chemistry and Aerosols (UKCA) composition-climate model has been developed. This configuration, while not suitable for long simulations, is an excellent test-bed for new model developments and can be used to train new users in how to use UKCA. This work was motivated by the desire to improve the usability of UKCA, and to encourage more users to become involved with the code development process.
Amanda C. Maycock, Katja Matthes, Susann Tegtmeier, Hauke Schmidt, Rémi Thiéblemont, Lon Hood, Hideharu Akiyoshi, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Oliver Kirner, Markus Kunze, Marion Marchand, Daniel R. Marsh, Martine Michou, David Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Yousuke Yamashita, and Kohei Yoshida
Atmos. Chem. Phys., 18, 11323–11343, https://doi.org/10.5194/acp-18-11323-2018, https://doi.org/10.5194/acp-18-11323-2018, 2018
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The 11-year solar cycle is an important driver of climate variability. Changes in incoming solar ultraviolet radiation affect atmospheric ozone, which in turn influences atmospheric temperatures. Constraining the impact of the solar cycle on ozone is therefore important for understanding climate variability. This study examines the representation of the solar influence on ozone in numerical models used to simulate past and future climate. We highlight important differences among model datasets.
Blanca Ayarzagüena, Lorenzo M. Polvani, Ulrike Langematz, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Dameris, Makoto Deushi, Steven C. Hardiman, Patrick Jöckel, Andrew Klekociuk, Marion Marchand, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, David A. Plummer, Laura Revell, Eugene Rozanov, David Saint-Martin, John Scinocca, Andrea Stenke, Kane Stone, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Atmos. Chem. Phys., 18, 11277–11287, https://doi.org/10.5194/acp-18-11277-2018, https://doi.org/10.5194/acp-18-11277-2018, 2018
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Stratospheric sudden warmings (SSWs) are natural major disruptions of the polar stratospheric circulation that also affect surface weather. In the literature there are conflicting claims as to whether SSWs will change in the future. The confusion comes from studies using different models and methods. Here we settle the question by analysing 12 models with a consistent methodology, to show that no robust changes in frequency and other features are expected over the 21st century.
Emre Esentürk, Nathan Luke Abraham, Scott Archer-Nicholls, Christina Mitsakou, Paul Griffiths, Alex Archibald, and John Pyle
Geosci. Model Dev., 11, 3089–3108, https://doi.org/10.5194/gmd-11-3089-2018, https://doi.org/10.5194/gmd-11-3089-2018, 2018
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An integral and expensive part of coupled climate model simulations is the gas-phase chemistry which gives rise to hundreds of coupled differential equations. We propose a method which improves the convergence and robustness properties of commonly used Newton–Raphson solvers. The method is flexible and can be appended to most algorithms. The approach can be useful for a broader community of computational scientists whose interests lie in solving systems with intensive interactive chemistry.
Sonya L. Fiddes, Matthew T. Woodhouse, Zebedee Nicholls, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 18, 10177–10198, https://doi.org/10.5194/acp-18-10177-2018, https://doi.org/10.5194/acp-18-10177-2018, 2018
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The role of natural aerosol in the climate system is uncertain. A key contributor to marine aerosol is dimethyl sulfide (DMS), released by phytoplankton in the oceans. We study the effect of DMS on clouds and rain using a climate model with a detailed aerosol scheme. We show that DMS acts to reduce rainfall in cloud deck regions, leading to longer lived clouds and a large impact on solar energy reaching the surface. Further study of these areas will improve future climate projections.
Timofei Sukhodolov, Jian-Xiong Sheng, Aryeh Feinberg, Bei-Ping Luo, Thomas Peter, Laura Revell, Andrea Stenke, Debra K. Weisenstein, and Eugene Rozanov
Geosci. Model Dev., 11, 2633–2647, https://doi.org/10.5194/gmd-11-2633-2018, https://doi.org/10.5194/gmd-11-2633-2018, 2018
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The Pinatubo eruption in 1991 is the strongest directly observed volcanic event. In a series of experiments, we simulate its influence on the stratospheric aerosol layer using a state-of-the-art aerosol–chemistry–climate model, SOCOL-AERv1.0, and compare our results to observations. We show that SOCOL-AER reproduces the most important atmospheric effects and can therefore be used to study the climate effects of future volcanic eruptions and geoengineering by artificial sulfate aerosol.
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.
James Keeble, Hannah Brown, N. Luke Abraham, Neil R. P. Harris, and John A. Pyle
Atmos. Chem. Phys., 18, 7625–7637, https://doi.org/10.5194/acp-18-7625-2018, https://doi.org/10.5194/acp-18-7625-2018, 2018
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2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the stratospheric ozone layer from the harmful effects of synthetic ozone depleting substances. Since the late 1990s atmospheric concentrations of these species have begun to decline, and as a result ozone concentrations are expected to increase. In this study we use an ensemble of chemistry–climate simulations to investigate recent ozone trends and search for early signs of ozone recovery.
Clara Orbe, Huang Yang, Darryn W. Waugh, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, John F. Scinocca, Beatrice Josse, Virginie Marecal, Patrick Jöckel, Luke D. Oman, Susan E. Strahan, Makoto Deushi, Taichu Y. Tanaka, Kohei Yoshida, Hideharu Akiyoshi, Yousuke Yamashita, Andreas Stenke, Laura Revell, Timofei Sukhodolov, Eugene Rozanov, Giovanni Pitari, Daniele Visioni, Kane A. Stone, Robyn Schofield, and Antara Banerjee
Atmos. Chem. Phys., 18, 7217–7235, https://doi.org/10.5194/acp-18-7217-2018, https://doi.org/10.5194/acp-18-7217-2018, 2018
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In this study we compare a few atmospheric transport properties among several numerical models that are used to study the influence of atmospheric chemistry on climate. We show that there are large differences among models in terms of the timescales that connect the Northern Hemisphere midlatitudes, where greenhouse gases and ozone-depleting substances are emitted, to the Southern Hemisphere. Our results may have important implications for how models represent atmospheric composition.
Valerio Ferracci, Ines Heimann, N. Luke Abraham, John A. Pyle, and Alexander T. Archibald
Atmos. Chem. Phys., 18, 7109–7129, https://doi.org/10.5194/acp-18-7109-2018, https://doi.org/10.5194/acp-18-7109-2018, 2018
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Hydroxyl radicals (OH) control the removal of species emitted in the atmosphere. Field campaigns reported a "missing" OH sink, not included in current atmospheric models. In this work a global model was used to establish the impact of additional OH sinks, based on both observations of the missing sink and newly discovered reactions of OH. Results show modest increases in global atmospheric lifetimes but pronounced regional effects on the abundance of some key species.
Simone Dietmüller, Roland Eichinger, Hella Garny, Thomas Birner, Harald Boenisch, Giovanni Pitari, Eva Mancini, Daniele Visioni, Andrea Stenke, Laura Revell, Eugene Rozanov, David A. Plummer, John Scinocca, Patrick Jöckel, Luke Oman, Makoto Deushi, Shibata Kiyotaka, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 18, 6699–6720, https://doi.org/10.5194/acp-18-6699-2018, https://doi.org/10.5194/acp-18-6699-2018, 2018
Ashok K. Luhar, Matthew T. Woodhouse, and Ian E. Galbally
Atmos. Chem. Phys., 18, 4329–4348, https://doi.org/10.5194/acp-18-4329-2018, https://doi.org/10.5194/acp-18-4329-2018, 2018
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Dry deposition at the Earth’s surface is an important sink of atmospheric ozone. A new parameterisation for ozone dry deposition to the ocean that accounts for relevant chemical and physical processes is developed and tested. It results in an ocean deposition loss that is only about a third of the current model estimates and corresponds to an increase of 5 % in the tropospheric ozone burden. This is important for tropospheric ozone budget, associated radiative forcing, and ozone mixing ratios.
Olaf Morgenstern, Kane A. Stone, Robyn Schofield, Hideharu Akiyoshi, Yousuke Yamashita, Douglas E. Kinnison, Rolando R. Garcia, Kengo Sudo, David A. Plummer, John Scinocca, Luke D. Oman, Michael E. Manyin, Guang Zeng, Eugene Rozanov, Andrea Stenke, Laura E. Revell, Giovanni Pitari, Eva Mancini, Glauco Di Genova, Daniele Visioni, Sandip S. Dhomse, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 1091–1114, https://doi.org/10.5194/acp-18-1091-2018, https://doi.org/10.5194/acp-18-1091-2018, 2018
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We assess how ozone as simulated by a group of chemistry–climate models responds to variations in man-made climate gases and ozone-depleting substances. We find some agreement, particularly in the middle and upper stratosphere, but also considerable disagreement elsewhere. Such disagreement affects the reliability of future ozone projections based on these models, and also constitutes a source of uncertainty in climate projections using prescribed ozone derived from these simulations.
James Keeble, Ewa M. Bednarz, Antara Banerjee, N. Luke Abraham, Neil R. P. Harris, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 17, 13801–13818, https://doi.org/10.5194/acp-17-13801-2017, https://doi.org/10.5194/acp-17-13801-2017, 2017
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In this study we explore the chemical and transport processes controlling ozone abundances in different altitude regions in the tropics for the present day and how these processes may change in the future in order to determine when total-column ozone values in the tropics will recover to pre-1980s values following the implementation of the Montreal Protocol and its subsequent amendments, which imposed bans on the use and emissions of CFCs.
Laura E. Revell, Andrea Stenke, Beiping Luo, Stefanie Kremser, Eugene Rozanov, Timofei Sukhodolov, and Thomas Peter
Atmos. Chem. Phys., 17, 13139–13150, https://doi.org/10.5194/acp-17-13139-2017, https://doi.org/10.5194/acp-17-13139-2017, 2017
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Compiling stratospheric aerosol data sets after a major volcanic eruption is difficult as the stratosphere becomes too optically opaque for satellite instruments to measure accurately. We performed ensemble chemistry–climate model simulations with two stratospheric aerosol data sets compiled for two international modelling activities and compared the simulated volcanic aerosol-induced effects from the 1991 Mt Pinatubo eruption on tropical stratospheric temperature and ozone with observations.
Huan Yao, Yu Song, Mingxu Liu, Scott Archer-Nicholls, Douglas Lowe, Gordon McFiggans, Tingting Xu, Pin Du, Jianfeng Li, Yusheng Wu, Min Hu, Chun Zhao, and Tong Zhu
Atmos. Chem. Phys., 17, 5205–5219, https://doi.org/10.5194/acp-17-5205-2017, https://doi.org/10.5194/acp-17-5205-2017, 2017
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Marcus Thatcher
Atmos. Chem. Phys., 17, 3749–3767, https://doi.org/10.5194/acp-17-3749-2017, https://doi.org/10.5194/acp-17-3749-2017, 2017
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Dry deposition of tropospheric ozone relates to its destruction at the Earth’s surface. An improved model scheme for such deposition to the ocean is formulated backed up by field data. It results in the oceanic dry deposition of ozone to be 12 % of the global total, which is much lower than the current model estimate of about 30 %. This result has implications for modelling global tropospheric ozone budget and its radiative forcing, and ozone mixing ratios, especially in the Southern Hemisphere.
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.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
William T. Ball, Aleš Kuchař, Eugene V. Rozanov, Johannes Staehelin, Fiona Tummon, Anne K. Smith, Timofei Sukhodolov, Andrea Stenke, Laura Revell, Ancelin Coulon, Werner Schmutz, and Thomas Peter
Atmos. Chem. Phys., 16, 15485–15500, https://doi.org/10.5194/acp-16-15485-2016, https://doi.org/10.5194/acp-16-15485-2016, 2016
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We find monthly, mid-latitude temperature changes above 40 km are related to ozone and temperature variations throughout the middle atmosphere. We develop an index to represent this atmospheric variability. In statistical analysis, the index can account for up to 60 % of variability in tropical temperature and ozone above 27 km. The uncertainties can be reduced by up to 35 % and 20 % in temperature and ozone, respectively. This index is an important tool to quantify current and future ozone recovery.
Mingjin Tang, James Keeble, Paul J. Telford, Francis D. Pope, Peter Braesicke, Paul T. Griffiths, N. Luke Abraham, James McGregor, I. Matt Watson, R. Anthony Cox, John A. Pyle, and Markus Kalberer
Atmos. Chem. Phys., 16, 15397–15412, https://doi.org/10.5194/acp-16-15397-2016, https://doi.org/10.5194/acp-16-15397-2016, 2016
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We have investigated for the first time the heterogeneous hydrolysis of ClONO2 on TiO2 and SiO2 aerosol particles at room temperature and at different relative humidities (RHs), using an aerosol flow tube. The kinetic data reported in our current and previous studies have been included in the UKCA chemistry–climate model to assess the impact of TiO2 injection on stratospheric chemistry and stratospheric ozone in particular.
Laura E. Revell, Andrea Stenke, Eugene Rozanov, William Ball, Stefan Lossow, and Thomas Peter
Atmos. Chem. Phys., 16, 13067–13080, https://doi.org/10.5194/acp-16-13067-2016, https://doi.org/10.5194/acp-16-13067-2016, 2016
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Water vapour in the stratosphere plays an important role in atmospheric chemistry and the Earth's radiative balance. We have analysed trends in stratospheric water vapour through the 21st century as simulated by a coupled chemistry–climate model following a range of greenhouse gas emission scenarios. We have also quantified the contribution that methane oxidation in the stratosphere makes to projected water vapour trends.
Ewa M. Bednarz, Amanda C. Maycock, N. Luke Abraham, Peter Braesicke, Olivier Dessens, and John A. Pyle
Atmos. Chem. Phys., 16, 12159–12176, https://doi.org/10.5194/acp-16-12159-2016, https://doi.org/10.5194/acp-16-12159-2016, 2016
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Future trends in springtime Arctic ozone, and its chemical dynamical and radiative drivers, are analysed using a 7-member ensemble of chemistry–climate model integrations, allowing for a detailed assessment of interannual variability. Despite the future long-term recovery of Arctic ozone, there is large interannual variability and episodic reductions in springtime Arctic column ozone. Halogen chemistry will become a smaller but non-negligible driver of Arctic ozone variability over the century.
Ivan Kourtchev, Ricardo H. M. Godoi, Sarah Connors, James G. Levine, Alex T. Archibald, Ana F. L. Godoi, Sarah L. Paralovo, Cybelli G. G. Barbosa, Rodrigo A. F. Souza, Antonio O. Manzi, Roger Seco, Steve Sjostedt, Jeong-Hoo Park, Alex Guenther, Saewung Kim, James Smith, Scot T. Martin, and Markus Kalberer
Atmos. Chem. Phys., 16, 11899–11913, https://doi.org/10.5194/acp-16-11899-2016, https://doi.org/10.5194/acp-16-11899-2016, 2016
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Scott Archer-Nicholls, Douglas Lowe, David M. Schultz, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5573–5594, https://doi.org/10.5194/acp-16-5573-2016, https://doi.org/10.5194/acp-16-5573-2016, 2016
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The response of the Weather Research and Forecasting model with Chemistry to forcings by biomass burning aerosol were investigated in high-resolution nested domains over Brazil. The aerosol-layer was found to have a negative direct effect at the top of the atmosphere, but this was largely cancelled by a semi-direct effect which inhibited afternoon cloud formation. The cloud response to the aerosol was found to be highly sensitive to model resolution and the use of convective parameterisation.
Peer Johannes Nowack, Nathan Luke Abraham, Peter Braesicke, and John Adrian Pyle
Atmos. Chem. Phys., 16, 4191–4203, https://doi.org/10.5194/acp-16-4191-2016, https://doi.org/10.5194/acp-16-4191-2016, 2016
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Various forms of solar radiation management (SRM) have been proposed to counteract man-made climate change. However, all these countermeasures could have unintended side-effects. We add a novel perspective to this discussion by showing how atmospheric ozone changes under solar geoengineering could affect UV exposure and air pollution. This would have implications for human health and ecology. Atmospheric composition changes are therefore important to consider in the evaluation of any SRM scheme.
Antara Banerjee, Amanda C. Maycock, Alexander T. Archibald, N. Luke Abraham, Paul Telford, Peter Braesicke, and John A. Pyle
Atmos. Chem. Phys., 16, 2727–2746, https://doi.org/10.5194/acp-16-2727-2016, https://doi.org/10.5194/acp-16-2727-2016, 2016
E. W. Butt, A. Rap, A. Schmidt, C. E. Scott, K. J. Pringle, C. L. Reddington, N. A. D. Richards, M. T. Woodhouse, J. Ramirez-Villegas, H. Yang, V. Vakkari, E. A. Stone, M. Rupakheti, P. S. Praveen, P. G. van Zyl, J. P. Beukes, M. Josipovic, E. J. S. Mitchell, S. M. Sallu, P. M. Forster, and D. V. Spracklen
Atmos. Chem. Phys., 16, 873–905, https://doi.org/10.5194/acp-16-873-2016, https://doi.org/10.5194/acp-16-873-2016, 2016
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We estimate the impact of residential emissions (cooking and heating) on atmospheric aerosol, human health, and climate. We find large contributions to annual mean ambient PM2.5 in residential sources regions resulting in significant but uncertain global premature mortality when key uncertainties in emission flux are considered. We show that residential emissions exert an uncertain global radiative effect and suggest more work is needed to characterise residential emissions climate importance.
J. G. Levine, A. R. MacKenzie, O. J. Squire, A. T. Archibald, P. T. Griffiths, N. L. Abraham, J. A. Pyle, D. E. Oram, G. Forster, J. F. Brito, J. D. Lee, J. R. Hopkins, A. C. Lewis, S. J. B. Bauguitte, C. F. Demarco, P. Artaxo, P. Messina, J. Lathière, D. A. Hauglustaine, E. House, C. N. Hewitt, and E. Nemitz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-24251-2015, https://doi.org/10.5194/acpd-15-24251-2015, 2015
Revised manuscript has not been submitted
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This study explores our ability to simulate atmospheric chemistry stemming from isoprene emissions—a reactive gas emitted from vegetation—in pristine and polluted regions of the Amazon basin. We explore how two contrasting models fare in reproducing recent airborne measurements in the region. Their differing treatments of transport and mixing are found to: profoundly affect their performance; and yield very different pictures of the exposure of the rainforest to harmful ozone concentrations.
S. T. Turnock, D. V. Spracklen, K. S. Carslaw, G. W. Mann, M. T. Woodhouse, P. M. Forster, J. Haywood, C. E. Johnson, M. Dalvi, N. Bellouin, and A. Sanchez-Lorenzo
Atmos. Chem. Phys., 15, 9477–9500, https://doi.org/10.5194/acp-15-9477-2015, https://doi.org/10.5194/acp-15-9477-2015, 2015
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We evaluate HadGEM3-UKCA over Europe for the period 1960-2009 against observations of aerosol mass and number, aerosol optical depth (AOD) and surface solar radiation (SSR). The model underestimates aerosol mass and number but is less biased if compared to AOD and SSR. Observed trends in aerosols are well simulated by the model and necessary for reproducing the observed increase in SSR since 1990. European all-sky top of atmosphere aerosol radiative forcing increased by > 3 Wm-2 from 1970 to 2009.
L. E. Revell, F. Tummon, A. Stenke, T. Sukhodolov, A. Coulon, E. Rozanov, H. Garny, V. Grewe, and T. Peter
Atmos. Chem. Phys., 15, 5887–5902, https://doi.org/10.5194/acp-15-5887-2015, https://doi.org/10.5194/acp-15-5887-2015, 2015
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We have examined the effects of ozone precursor emissions and climate change on the tropospheric ozone budget. Under RCP 6.0, ozone in the future is governed primarily by changes in nitrogen oxides (NOx). Methane is also important, and induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. This study highlights the critical role that emission policies globally have to play in determining tropospheric ozone evolution through the 21st century.
O. J. Squire, A. T. Archibald, P. T. Griffiths, M. E. Jenkin, D. Smith, and J. A. Pyle
Atmos. Chem. Phys., 15, 5123–5143, https://doi.org/10.5194/acp-15-5123-2015, https://doi.org/10.5194/acp-15-5123-2015, 2015
S. Archer-Nicholls, D. Lowe, E. Darbyshire, W. T. Morgan, M. M. Bela, G. Pereira, J. Trembath, J. W. Kaiser, K. M. Longo, S. R. Freitas, H. Coe, and G. McFiggans
Geosci. Model Dev., 8, 549–577, https://doi.org/10.5194/gmd-8-549-2015, https://doi.org/10.5194/gmd-8-549-2015, 2015
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The regional WRF-Chem model was used to study aerosol particles from biomass burning in South America. The modelled estimates of fire plume injection heights were found to be too high, with serious implications for modelled aerosol vertical distribution, transport and impacts on local climate. A modified emission scenario was developed which improved the predicted injection height. Model results were compared and evaluated against in situ measurements from the 2012 SAMBBA flight campaign.
D. Lowe, S. Archer-Nicholls, W. Morgan, J. Allan, S. Utembe, B. Ouyang, E. Aruffo, M. Le Breton, R. A. Zaveri, P. Di Carlo, C. Percival, H. Coe, R. Jones, and G. McFiggans
Atmos. Chem. Phys., 15, 1385–1409, https://doi.org/10.5194/acp-15-1385-2015, https://doi.org/10.5194/acp-15-1385-2015, 2015
J. Keeble, P. Braesicke, N. L. Abraham, H. K. Roscoe, and J. A. Pyle
Atmos. Chem. Phys., 14, 13705–13717, https://doi.org/10.5194/acp-14-13705-2014, https://doi.org/10.5194/acp-14-13705-2014, 2014
S. Archer-Nicholls, D. Lowe, S. Utembe, J. Allan, R. A. Zaveri, J. D. Fast, Ø. Hodnebrog, H. Denier van der Gon, and G. McFiggans
Geosci. Model Dev., 7, 2557–2579, https://doi.org/10.5194/gmd-7-2557-2014, https://doi.org/10.5194/gmd-7-2557-2014, 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
T. J. Roberts, L. Jourdain, P. T. Griffiths, and M. Pirre
Atmos. Chem. Phys., 14, 11185–11199, https://doi.org/10.5194/acp-14-11185-2014, https://doi.org/10.5194/acp-14-11185-2014, 2014
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 10431–10438, https://doi.org/10.5194/acp-14-10431-2014, https://doi.org/10.5194/acp-14-10431-2014, 2014
A. Banerjee, A. T. Archibald, A. C. Maycock, P. Telford, N. L. Abraham, X. Yang, P. Braesicke, and J. A. Pyle
Atmos. Chem. Phys., 14, 9871–9881, https://doi.org/10.5194/acp-14-9871-2014, https://doi.org/10.5194/acp-14-9871-2014, 2014
O. J. Squire, A. T. Archibald, N. L. Abraham, D. J. Beerling, C. N. Hewitt, J. Lathière, R. C. Pike, P. J. Telford, and J. A. Pyle
Atmos. Chem. Phys., 14, 1011–1024, https://doi.org/10.5194/acp-14-1011-2014, https://doi.org/10.5194/acp-14-1011-2014, 2014
S. J. O'Shea, G. Allen, M. W. Gallagher, S. J.-B. Bauguitte, S. M. Illingworth, M. Le Breton, J. B. A. Muller, C. J. Percival, A. T. Archibald, D. E. Oram, M. Parrington, P. I. Palmer, and A. C. Lewis
Atmos. Chem. Phys., 13, 12451–12467, https://doi.org/10.5194/acp-13-12451-2013, https://doi.org/10.5194/acp-13-12451-2013, 2013
Z. S. Stock, M. R. Russo, T. M. Butler, A. T. Archibald, M. G. Lawrence, P. J. Telford, N. L. Abraham, and J. A. Pyle
Atmos. Chem. Phys., 13, 12215–12231, https://doi.org/10.5194/acp-13-12215-2013, https://doi.org/10.5194/acp-13-12215-2013, 2013
A. M. Foley, D. Dalmonech, A. D. Friend, F. Aires, A. T. Archibald, P. Bartlein, L. Bopp, J. Chappellaz, P. Cox, N. R. Edwards, G. Feulner, P. Friedlingstein, S. P. Harrison, P. O. Hopcroft, C. D. Jones, J. Kolassa, J. G. Levine, I. C. Prentice, J. Pyle, N. Vázquez Riveiros, E. W. Wolff, and S. Zaehle
Biogeosciences, 10, 8305–8328, https://doi.org/10.5194/bg-10-8305-2013, https://doi.org/10.5194/bg-10-8305-2013, 2013
P. Braesicke, J. Keeble, X. Yang, G. Stiller, S. Kellmann, N. L. Abraham, A. Archibald, P. Telford, and J. A. Pyle
Atmos. Chem. Phys., 13, 10677–10688, https://doi.org/10.5194/acp-13-10677-2013, https://doi.org/10.5194/acp-13-10677-2013, 2013
N. J. Warwick, A. T. Archibald, K. Ashworth, J. Dorsey, P. M. Edwards, D. E. Heard, B. Langford, J. Lee, P. K. Misztal, L. K. Whalley, and J. A. Pyle
Atmos. Chem. Phys., 13, 9183–9194, https://doi.org/10.5194/acp-13-9183-2013, https://doi.org/10.5194/acp-13-9183-2013, 2013
M. T. Woodhouse, G. W. Mann, K. S. Carslaw, and O. Boucher
Atmos. Chem. Phys., 13, 2723–2733, https://doi.org/10.5194/acp-13-2723-2013, https://doi.org/10.5194/acp-13-2723-2013, 2013
P. J. Young, A. T. Archibald, K. W. Bowman, J.-F. Lamarque, V. Naik, D. S. Stevenson, S. Tilmes, A. Voulgarakis, O. Wild, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, L. W. Horowitz, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, R. B. Skeie, D. T. Shindell, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2063–2090, https://doi.org/10.5194/acp-13-2063-2013, https://doi.org/10.5194/acp-13-2063-2013, 2013
P. J. Telford, N. L. Abraham, A. T. Archibald, P. Braesicke, M. Dalvi, O. Morgenstern, F. M. O'Connor, N. A. D. Richards, and J. A. Pyle
Geosci. Model Dev., 6, 161–177, https://doi.org/10.5194/gmd-6-161-2013, https://doi.org/10.5194/gmd-6-161-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
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
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
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
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
Aggravated surface O3 pollution primarily driven by meteorological variation in China during the early COVID-19 pandemic lockdown period
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (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.
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.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
EGUsphere, https://doi.org/10.5194/egusphere-2024-470, https://doi.org/10.5194/egusphere-2024-470, 2024
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Tropospheric ozone is a major air pollutant, greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side-by-side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
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.
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.
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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Short summary
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.
Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting...
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