Articles | Volume 15, issue 9
Atmos. Chem. Phys., 15, 5123–5143, 2015
https://doi.org/10.5194/acp-15-5123-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 15, 5123–5143, 2015
https://doi.org/10.5194/acp-15-5123-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
07 May 2015
Research article
| 07 May 2015
Influence of isoprene chemical mechanism on modelled changes in tropospheric ozone due to climate and land use over the 21st century
O. J. Squire et al.
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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.
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
Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-423, https://doi.org/10.5194/acp-2022-423, 2022
Preprint under review for ACP
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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.
Ernesto Reyes-Villegas, Doug Lowe, Jill 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. Discuss., https://doi.org/10.5194/acp-2022-463, https://doi.org/10.5194/acp-2022-463, 2022
Preprint under review for ACP
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Organic aerosols (OA), their sources and 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 POA production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations taken at Delhi, India in 2018.
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.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Maria R. Russo, Brian J. Kerridge, Nathan L. Abraham, James Keeble, Barry G. Latter, Richard Siddans, James Weber, Paul T. Griffiths, John A. Pyle, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-99, https://doi.org/10.5194/acp-2022-99, 2022
Preprint under review for ACP
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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.
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
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.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
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Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric 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.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
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Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 20, 13497–13519, https://doi.org/10.5194/acp-20-13497-2020, https://doi.org/10.5194/acp-20-13497-2020, 2020
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Criegee intermediates, formed from alkene–ozone reactions, play a potentially important role as tropospheric oxidants. Evaluated kinetic data are provided for reactions governing their formation and removal for use in atmospheric models. These include their formation from reactions of simple and complex alkenes and removal by decomposition and reaction with a number of atmospheric species (e.g. H2O, SO2). An overview of the tropospheric chemistry of Criegee intermediates is also provided.
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.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Mike J. Newland, and Andrew R. Rickard
Atmos. Chem. Phys., 20, 12921–12937, https://doi.org/10.5194/acp-20-12921-2020, https://doi.org/10.5194/acp-20-12921-2020, 2020
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Unsaturated organic compounds are emitted in large quantities from natural and human-influenced sources. Atmospheric removal occurs significantly by reaction with ozone, initiating reaction sequences forming free radicals and organic pollutants in the gaseous and particulate phases. Due to their very large number, it is impossible to study the reaction rate for every compound, and most have to be estimated. Updated and extended estimation methods are reported for use in atmospheric models.
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.
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.
Conor G. Bolas, Valerio Ferracci, Andrew D. Robinson, Mohammed I. Mead, Mohd Shahrul Mohd Nadzir, John A. Pyle, Roderic L. Jones, and Neil R. P. Harris
Atmos. Meas. Tech., 13, 821–838, https://doi.org/10.5194/amt-13-821-2020, https://doi.org/10.5194/amt-13-821-2020, 2020
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Here we present the iDirac, a new instrument capable of making isoprene measurements in remote and challenging environments. The iDirac is a customisable and rugged field instrument for investigating emissions of volatile organic compounds from vegetation. It has been tested here in a series of experiments to ensure a high degree of technical precision, accuracy and repeatability. This new instrument allows us to ask and answer new questions about the influence of vegetation on the atmosphere.
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.
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.
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.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, and Andrew R. Rickard
Atmos. Chem. Phys., 19, 7691–7717, https://doi.org/10.5194/acp-19-7691-2019, https://doi.org/10.5194/acp-19-7691-2019, 2019
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Organic compounds are emitted in large amounts from natural and human-influenced sources. Peroxy radicals are key intermediates formed during oxidation of organic compounds, and play a central role in mechanisms forming pollutants such as ozone and organic particles. Due to the large number of different peroxy radicals formed, it is impossible to study the rates of all of their reactions, and most have to be estimated. Updated and new estimation methods are reported for use in atmospheric models
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.
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.
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.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Andrew R. Rickard, and Timothy J. Wallington
Atmos. Chem. Phys., 18, 9297–9328, https://doi.org/10.5194/acp-18-9297-2018, https://doi.org/10.5194/acp-18-9297-2018, 2018
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Organic compounds are emitted in large quantities from natural and human-influenced sources. Removal from the atmosphere occurs mainly by reaction with hydroxyl (OH) radicals, and initiates reaction sequences forming pollutants such as ozone and organic particles. Due to their very large number, it is impossible to measure the removal rate for all compounds, and most have to be estimated. An updated and extended estimation method is reported for use in atmospheric models and impact assessments.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Andrew R. Rickard, and Timothy J. Wallington
Atmos. Chem. Phys., 18, 9329–9349, https://doi.org/10.5194/acp-18-9329-2018, https://doi.org/10.5194/acp-18-9329-2018, 2018
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Organic compounds are emitted in large quantities from natural and human-influenced sources. Removal from the atmosphere occurs mainly by reaction with hydroxyl (OH) radicals, and initiates reaction sequences forming pollutants such as ozone and organic particles. Due to their very large number, it is impossible to measure the removal rate for all compounds, and most have to be estimated. An updated and extended estimation method is reported for use in atmospheric models and impact assessments.
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.
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.
Antara Banerjee, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 18, 2899–2911, https://doi.org/10.5194/acp-18-2899-2018, https://doi.org/10.5194/acp-18-2899-2018, 2018
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This study quantifies the radiative forcing (RF) of future ozone changes. Under climate change, even the sign of the ozone RF can change depending on the greenhouse gas emissions scenario followed. Stratosphere–troposphere exchange plays an important role in driving ozone RF due to reductions in ozone-depleting substances (ODSs) and increases in methane abundance. These could negate the ozone-derived climate benefits of air-quality controls on non-methane ozone precursor emissions.
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.
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.
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.
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.
Nicola J. Warwick, Michelle L. Cain, Rebecca Fisher, James L. France, David Lowry, Sylvia E. Michel, Euan G. Nisbet, Bruce H. Vaughn, James W. C. White, and John A. Pyle
Atmos. Chem. Phys., 16, 14891–14908, https://doi.org/10.5194/acp-16-14891-2016, https://doi.org/10.5194/acp-16-14891-2016, 2016
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Methane is an important greenhouse gas. Methane emissions from Arctic wetlands are poorly quantified and may increase in a warming climate. Using a global atmospheric model and atmospheric observations of methane and its isotopologues, we find that isotopologue data are useful in constraining Arctic wetland emissions. Our results suggest that the seasonal cycle of these emissions may be incorrectly simulated in land process models, with implications for our understanding of future emissions.
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
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
J. R. Pitt, M. Le Breton, G. Allen, C. J. Percival, M. W. Gallagher, S. J.-B. Bauguitte, S. J. O'Shea, J. B. A. Muller, M. S. Zahniser, J. Pyle, and P. I. Palmer
Atmos. Meas. Tech., 9, 63–77, https://doi.org/10.5194/amt-9-63-2016, https://doi.org/10.5194/amt-9-63-2016, 2016
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We present details of an Aerodyne quantum cascade laser absorption spectrometer (QCLAS) used to make airborne measurements of N2O and CH4, including its configuration for use on board an aircraft. Two different methods to correct for the influence of water vapour on the measurements are evaluated. We diagnose a sensitivity of the instrument to changes in pressure, introduce a new calibration procedure to account for this effect, and assess its performance.
M. R. Russo, M. J. Ashfold, N. R. P. Harris, and J. A. Pyle
Atmos. Chem. Phys., 15, 14031–14040, https://doi.org/10.5194/acp-15-14031-2015, https://doi.org/10.5194/acp-15-14031-2015, 2015
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We find a strong regional element to the uplift of CHBr3 from the ocean to the upper troposphere and lower stratosphere. The strongest uplift occurs when the largest emission and the most intense convection are co-located which is over the Maritime Continent in northern winter. Estimates of CHBr3 emissions based on aircraft measurements will be sensitive to where the available aircraft campaigns took place.
M. E. Jenkin, J. C. Young, and A. R. Rickard
Atmos. Chem. Phys., 15, 11433–11459, https://doi.org/10.5194/acp-15-11433-2015, https://doi.org/10.5194/acp-15-11433-2015, 2015
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Atmospheric isoprene oxidation has an important effect on the formation of pollutants such as ozone and particles. A reliable representation is an essential component of climate change/air quality models. Systematic updates to the detailed chemistry in the MCM are described, with reference to recently reported kinetic/mechanistic data. Results of box model calculations are used to illustrate the impacts of the updates, with particular focus on the key atmospheric cycles involving HOx and NOx.
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.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
K. P. Wyche, P. S. Monks, K. L. Smallbone, J. F. Hamilton, M. R. Alfarra, A. R. Rickard, G. B. McFiggans, M. E. Jenkin, W. J. Bloss, A. C. Ryan, C. N. Hewitt, and A. R. MacKenzie
Atmos. Chem. Phys., 15, 8077–8100, https://doi.org/10.5194/acp-15-8077-2015, https://doi.org/10.5194/acp-15-8077-2015, 2015
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This paper describes a new ensemble methodology for the statistical analysis of atmospheric gas- & particle-phase composition data sets. The methodology reduces the huge amount of data derived from many chamber experiments to show that organic reactivity & resultant particle formation can be mapped into unique clusters in statistical space. The model generated is used to map more realistic plant mesocosm oxidation data, the projection of which gives insight into reactive pathways & precursors.
M. J. Ashfold, J. A. Pyle, A. D. Robinson, E. Meneguz, M. S. M. Nadzir, S. M. Phang, A. A. Samah, S. Ong, H. E. Ung, L. K. Peng, S. E. Yong, and N. R. P. Harris
Atmos. Chem. Phys., 15, 3565–3573, https://doi.org/10.5194/acp-15-3565-2015, https://doi.org/10.5194/acp-15-3565-2015, 2015
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We use observations and model calculations to show that "cold surges" occurring during Northern Hemisphere winter can rapidly transport East Asian pollution to equatorial Southeast Asia. As well as affecting atmospheric composition near the surface, we argue that strong convection can subsequently lift the polluted air masses to the tropical upper troposphere. This suggests a potentially important connection between midlatitude pollution sources and the lower stratosphere.
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. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
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This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
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
M. S. Mohd Nadzir, S. M. Phang, M. R. Abas, N. Abdul Rahman, A. Abu Samah, W. T. Sturges, D. E. Oram, G. P. Mills, E. C. Leedham, J. A. Pyle, N. R. P. Harris, A. D. Robinson, M. J. Ashfold, M. I. Mead, M. T. Latif, M. F. Khan, A. M. Amiruddin, N. Banan, and M. M. Hanafiah
Atmos. Chem. Phys., 14, 8137–8148, https://doi.org/10.5194/acp-14-8137-2014, https://doi.org/10.5194/acp-14-8137-2014, 2014
M. J. Tang, P. J. Telford, F. D. Pope, L. Rkiouak, N. L. Abraham, A. T. Archibald, P. Braesicke, J. A. Pyle, J. McGregor, I. M. Watson, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 14, 6035–6048, https://doi.org/10.5194/acp-14-6035-2014, https://doi.org/10.5194/acp-14-6035-2014, 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
F. M. O'Connor, C. E. Johnson, O. Morgenstern, N. L. Abraham, P. Braesicke, M. Dalvi, G. A. Folberth, M. G. Sanderson, P. J. Telford, A. Voulgarakis, P. J. Young, G. Zeng, W. J. Collins, and J. A. Pyle
Geosci. Model Dev., 7, 41–91, https://doi.org/10.5194/gmd-7-41-2014, https://doi.org/10.5194/gmd-7-41-2014, 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. Ammann, R. A. Cox, J. N. Crowley, M. E. Jenkin, A. Mellouki, M. J. Rossi, J. Troe, and T. J. Wallington
Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, https://doi.org/10.5194/acp-13-8045-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 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 | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
A renewed rise in global HCFC-141b emissions between 2017–2021
A model for simultaneous evaluation of NO2, O3, and PM10 pollution in urban and rural areas: handling incomplete data sets with multivariate curve resolution analysis
Technical note: Entrainment-limited kinetics of bimolecular reactions in clouds
Improving NOx emission estimates in Beijing using network observations and a perturbed emissions ensemble
Observation-based analysis of ozone production sensitivity for two persistent ozone episodes in Guangdong, China
A machine learning approach to quantify meteorological drivers of ozone pollution in China from 2015 to 2019
Discrepancy in assimilated atmospheric CO over East Asia in 2015–2020 by assimilating satellite and surface CO measurements
Potential environmental impact of bromoform from Asparagopsis farming in Australia
Satellite soil moisture data assimilation impacts on modeling weather variables and ozone in the southeastern US – Part 2: Sensitivity to dry-deposition parameterizations
The impacts of marine-emitted halogens on OH radicals in East Asia during summer
Impact of eastern and central Pacific El Niño on lower tropospheric ozone in China
Contribution of Asian emissions to upper tropospheric CO over the remote Pacific
Impact of a subtropical high and a typhoon on a severe ozone pollution episode in the Pearl River Delta, China
An ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievals
A process-oriented evaluation of CAMS reanalysis ozone during tropopause folds over Europe for the period 2003–2018
Estimation of mechanistic parameters in the gas-phase reactions of ozone with alkenes for use in automated mechanism construction
Projections of hydrofluorocarbon (HFC) emissions and the resulting global warming based on recent trends in observed abundances and current policies
Quantification of methane emissions from hotspots and during COVID-19 using a global atmospheric inversion
Model evaluation of short-lived climate forcers for the Arctic Monitoring and Assessment Programme: a multi-species, multi-model study
Global simulations of monoterpene-derived peroxy radical fates and the distributions of highly oxygenated organic molecules (HOMs) and accretion products
Impact of present and future aircraft NOx and aerosol emissions on atmospheric composition and associated direct radiative forcing of climate
Influence of photochemical loss of volatile organic compounds on understanding ozone formation mechanism
North China Plain as a hot spot of ozone pollution exacerbated by extreme high temperatures
Bayesian assessment of chlorofluorocarbon (CFC), hydrochlorofluorocarbon (HCFC) and halon banks suggest large reservoirs still present in old equipment
Photochemical evolution of the 2013 California Rim Fire: synergistic impacts of reactive hydrocarbons and enhanced oxidants
Impact of biomass burning and stratospheric intrusions in the remote South Pacific Ocean troposphere
Global and regional carbon budget 2015–2020 inferred from OCO-2 based on an ensemble Kalman filter coupled with GEOS-Chem
Influence of total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODEs) in the Antarctic
Changes in anthropogenic precursor emissions drive shifts in the ozone seasonal cycle throughout the northern midlatitude troposphere
Changing Ozone Sensitivity in the South Coast Air Basin during the COVID-19 Period
Amplified role of potential HONO sources in O3 formation in North China Plain during autumn haze aggravating processes
Continental-scale contributions to the global CFC-11 emission increase between 2012 and 2017
Surface ozone impacts on major crop production in China from 2010 to 2017
Enhanced summertime ozone and SOA from biogenic volatile organic compound (BVOC) emissions due to vegetation biomass variability during 1981–2018 in China
Pyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation
Tropospheric ozone changes and ozone sensitivity from the present day to the future under shared socio-economic pathways
An integrated analysis of contemporary methane emissions and concentration trends over China using in situ and satellite observations and model simulations
An assessment of the tropospherically accessible photo-initiated ground state chemistry of organic carbonyls
Methane emissions in the United States, Canada, and Mexico: evaluation of national methane emission inventories and 2010–2017 sectoral trends by inverse analysis of in situ (GLOBALVIEWplus CH4 ObsPack) and satellite (GOSAT) atmospheric observations
Evaluation of SO2, SO42− and an updated SO2 dry deposition parameterization in the United Kingdom Earth System Model
Development and evaluation of a new compact mechanism for aromatic oxidation in atmospheric models
Ozone deposition impact assessments for forest canopies require accurate ozone flux partitioning on diurnal timescales
Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI
Model Output Statistics (MOS) applied to CAMS O3 forecasts: trade-offs between continuous and categorical skill scores
Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
Improving predictability of high-ozone episodes through dynamic boundary conditions, emission refresh and chemical data assimilation during the Long Island Sound Tropospheric Ozone Study (LISTOS) field campaign
Atmospheric observations consistent with reported decline in the UK's methane emissions (2013–2020)
Influence of atmospheric in-cloud aqueous-phase chemistry on the global simulation of SO2 in CESM2
Technical note: Quality assessment of ozone reanalysis products and gap-filling over subarctic Europe for vegetation risk mapping
Evolution of OH reactivity in NO-free volatile organic compound photooxidation investigated by the fully explicit GECKO-A model
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
Atmos. Chem. Phys., 22, 9111–9127, https://doi.org/10.5194/acp-22-9111-2022, https://doi.org/10.5194/acp-22-9111-2022, 2022
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A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easily interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants, even when having missing data.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
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.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416, https://doi.org/10.5194/acp-22-8403-2022, https://doi.org/10.5194/acp-22-8403-2022, 2022
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We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402, https://doi.org/10.5194/acp-22-8385-2022, https://doi.org/10.5194/acp-22-8385-2022, 2022
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We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826, https://doi.org/10.5194/acp-22-7815-2022, https://doi.org/10.5194/acp-22-7815-2022, 2022
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We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351, https://doi.org/10.5194/acp-22-7331-2022, https://doi.org/10.5194/acp-22-7331-2022, 2022
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We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.
Zhongjing Jiang and Jing Li
Atmos. Chem. Phys., 22, 7273–7285, https://doi.org/10.5194/acp-22-7273-2022, https://doi.org/10.5194/acp-22-7273-2022, 2022
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This study investigates the changes of tropospheric ozone in China associated with EP and CP El Niño, using satellite observations and the GEOS-Chem model. We found that El Niño generally leads to lower tropospheric ozone (LTO) decrease over most parts of China; La Niña acts the opposite. The difference between LTO changes during EP and CP El Niño primarily lies in southern China. Regional transport and chemical processes play the leading and secondary roles in driving the LTO changes.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Shanshan Ouyang, Tao Deng, Run Liu, Jingyang Chen, Guowen He, Jeremy Cheuk-Hin Leung, Nan Wang, and Shaw Chen Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-290, https://doi.org/10.5194/acp-2022-290, 2022
Revised manuscript accepted for ACP
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A record-breaking severe O3 pollution episode occurred under the influence of a Pacific subtropical high followed by Typhoon Mina in the Pearl River Delta (PRD) in early Autumn 2019. Through the WRF-CMAQ model simulations, we propose that the enhanced photochemical production of O3 during the episode is a major cause of the most severe O3 pollution year since the official O3 observation started in PRD in 2006.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624, https://doi.org/10.5194/acp-22-6595-2022, https://doi.org/10.5194/acp-22-6595-2022, 2022
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Luca Cantarello, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 5961–5981, https://doi.org/10.5194/acp-22-5961-2022, https://doi.org/10.5194/acp-22-5961-2022, 2022
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Concentrations of atmospheric methane continue to grow, in recent years at an increasing rate, for unknown reasons. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high resolution. Results show that the system can accurately report on biases in national inventories and is used to conclude that the early COVID-19 slowdown period (March–June 2020) had little impact on global methane emissions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Etienne Terrenoire, Didier Hauglustaine, Yann Cohen, Anne Cozic, Richard Valorso, Franck Lefèvre, and Sigrun Matthes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-222, https://doi.org/10.5194/acp-2022-222, 2022
Revised manuscript accepted for ACP
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Aviation NOx emissions have not only an impact on global climate by changing ozone and methane levels in the atmosphere but also contribute to deteriorate local air quality. The LMDZ-INCA global model is applied to reevaluate the impact of aircraft NOx and aerosol emissions on climate. We investigate the impact of present-day and future (2050) aircraft emissions on atmospheric composition and the associated radiative forcings of climate of ozone, methane and the aerosol direct forcings.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-240, https://doi.org/10.5194/acp-2022-240, 2022
Revised manuscript accepted for ACP
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Halocarbons contained in equipment continue to be emitted after production has ceased. These ‘banks’ must be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone hole recovery if left unrecovered.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Yawen Kong, Bo Zheng, Qiang Zhang, and Kebin He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-183, https://doi.org/10.5194/acp-2022-183, 2022
Revised manuscript accepted for ACP
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We developed a Bayesian atmospheric inversion system based on the 4D-LETKF algorithm coupled with GEOS-Chem, constrained by OCO-2 XCO2. This work represents the first time the 4D-LETKF algorithm was adapted to a global carbon inversion system that assimilated OCO-2 data. We inferred global gridded carbon fluxes from the latest OCO-2 V10r retrievals and investigated their magnitudes, variations, and partitioning schemes to understand the global and regional carbon budgets between 2015 and 2020.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890, https://doi.org/10.5194/acp-22-3875-2022, https://doi.org/10.5194/acp-22-3875-2022, 2022
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We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524, https://doi.org/10.5194/acp-22-3507-2022, https://doi.org/10.5194/acp-22-3507-2022, 2022
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A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Jason Schroeder, Chenxia Cai, Jin Xu, David Ridley, Jin Lu, Nancy Bui, Fang Yan, and Jeremy Avise
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-178, https://doi.org/10.5194/acp-2022-178, 2022
Revised manuscript accepted for ACP
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Ozone, a key component of smog, has plagued the Los Angeles region for decades. Ozone is created by complex chemical reactions that can be greatly impacted by anthropogenic emissions. This study makes use of the COVID-19 period to study the sensitivity of ozone chemistry in LA to certain anthropogenic emissions, notably from vehicles. We find that vehicular emissions of key pollutants dropped by up to 25 % during COVID-19, which caused a fundamental shift in ozone chemistry in the region.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364, https://doi.org/10.5194/acp-22-2351-2022, https://doi.org/10.5194/acp-22-2351-2022, 2022
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Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963, https://doi.org/10.5194/acp-22-1951-2022, https://doi.org/10.5194/acp-22-1951-2022, 2022
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227, https://doi.org/10.5194/acp-22-1209-2022, https://doi.org/10.5194/acp-22-1209-2022, 2022
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Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
Keiran N. Rowell, Scott H. Kable, and Meredith J. T. Jordan
Atmos. Chem. Phys., 22, 929–949, https://doi.org/10.5194/acp-22-929-2022, https://doi.org/10.5194/acp-22-929-2022, 2022
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Sunlight drives chemical reactions in the atmosphere by breaking chemical bonds. Motivated by the knowledge that if we can better understand the fundamental chemistry, we will be better able to predict atmospheric composition and model any future changes, we use quantum chemistry to investigate new classes of atmospheric reactions. We identify several potentially important reaction classes that will have implications for the atmospheric production of organic acids and molecular hydrogen.
Xiao Lu, Daniel J. Jacob, Haolin Wang, Joannes D. Maasakkers, Yuzhong Zhang, Tia R. Scarpelli, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Hannah Nesser, A. Anthony Bloom, Shuang Ma, John R. Worden, Shaojia Fan, Robert J. Parker, Hartmut Boesch, Ritesh Gautam, Deborah Gordon, Michael D. Moran, Frances Reuland, Claudia A. Octaviano Villasana, and Arlyn Andrews
Atmos. Chem. Phys., 22, 395–418, https://doi.org/10.5194/acp-22-395-2022, https://doi.org/10.5194/acp-22-395-2022, 2022
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We evaluate methane emissions and trends for 2010–2017 in the gridded national emission inventories for the United States, Canada, and Mexico by inversion of in situ and satellite methane observations. We find that anthropogenic methane emissions for all three countries are underestimated in the national inventories, largely driven by oil emissions. Anthropogenic methane emissions in the US peak in 2014, in contrast to the report of a steadily decreasing trend over 2010–2017 from the US EPA.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245, https://doi.org/10.5194/acp-21-18227-2021, https://doi.org/10.5194/acp-21-18227-2021, 2021
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The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-864, https://doi.org/10.5194/acp-2021-864, 2021
Revised manuscript accepted for ACP
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This study investigates to which extent ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts, while highlighting at the same time the complexity of improving the detection of highest O3 concentrations.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Wendong Ge, Junfeng Liu, Kan Yi, Jiayu Xu, Yizhou Zhang, Xiurong Hu, Jianmin Ma, Xuejun Wang, Yi Wan, Jianying Hu, Zhaobin Zhang, Xilong Wang, and Shu Tao
Atmos. Chem. Phys., 21, 16093–16120, https://doi.org/10.5194/acp-21-16093-2021, https://doi.org/10.5194/acp-21-16093-2021, 2021
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Compared with the observations, the results incorporating detailed cloud aqueous-phase chemistry greatly reduced SO2 overestimation. The biases in annual simulated SO2 concentrations (or mixing ratios) decreased by 46 %, 41 %, and 22 % in Europe, the USA, and China, respectively. Fe chemistry and HOx chemistry contributed more to SO2 oxidation than N chemistry. Higher concentrations of soluble Fe and higher pH values could further enhance the oxidation capacity.
Stefanie Falk, Ane V. Vollsnes, Aud B. Eriksen, Frode Stordal, and Terje Koren Berntsen
Atmos. Chem. Phys., 21, 15647–15661, https://doi.org/10.5194/acp-21-15647-2021, https://doi.org/10.5194/acp-21-15647-2021, 2021
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We evaluate regional and global models for ozone modeling and damage risk mapping of vegetation over subarctic Europe. Our analysis suggests that low-resolution global models do not reproduce the observed ozone seasonal cycle at ground level, underestimating ozone by 30–50 %. High-resolution regional models capture the seasonal cycle well, still underestimating ozone by up to 20 %. Our proposed gap-filling method for site observations shows a 76 % accuracy compared to the regional model (80 %).
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
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Archibald, A. T., Jenkin, M. E., and Shallcross, D. E.: An isoprene mechanism intercomparison, Atmos. Environ., 44, 5356–5364, https://doi.org/10.1016/j.atmosenv.2009.09.016, 2010b.
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