Articles | Volume 20, issue 18
https://doi.org/10.5194/acp-20-10889-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-10889-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
22 Sep 2020
Research article |
| 22 Sep 2020
CRI-HOM: A novel chemical mechanism for simulating highly oxygenated organic molecules (HOMs) in global chemistry–aerosol–climate models
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Cambridge, CB2 1EW, UK
Scott Archer-Nicholls
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Cambridge, CB2 1EW, UK
Paul Griffiths
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Cambridge, CB2 1EW, UK
National Centre for Atmospheric Science, Department of Chemistry,
University of Cambridge, CB2 1EW, UK
Torsten Berndt
Atmospheric Chemistry Department (ACD), Leibniz Institute for
Tropospheric Research (TROPOS), 04318 Leipzig, Germany
Michael Jenkin
Atmospheric Chemistry Services, Okehampton, Devon, EX20 4BQ, UK
Hamish Gordon
Engineering Research Accelerator and Center for Atmospheric Particle
Studies, Carnegie Mellon University, Pittsburgh, PA 15213, USA
Christoph Knote
Meteorologisches Institut, Ludwig-Maximilians-Universität
München, 80333 Munich, Germany
Alexander T. Archibald
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Cambridge, CB2 1EW, UK
National Centre for Atmospheric Science, Department of Chemistry,
University of Cambridge, CB2 1EW, UK
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Silke Trömel, Clemens Simmer, Ulrich Blahak, Armin Blanke, Sabine Doktorowski, Florian Ewald, Michael Frech, Mathias Gergely, Martin Hagen, Tijana Janjic, Heike Kalesse-Los, Stefan Kneifel, Christoph Knote, Jana Mendrok, Manuel Moser, Gregor Köcher, Kai Mühlbauer, Alexander Myagkov, Velibor Pejcic, Patric Seifert, Prabhakar Shrestha, Audrey Teisseire, Leonie von Terzi, Eleni Tetoni, Teresa Vogl, Christiane Voigt, Yuefei Zeng, Tobias Zinner, and Johannes Quaas
Atmos. Chem. Phys., 21, 17291–17314, https://doi.org/10.5194/acp-21-17291-2021, https://doi.org/10.5194/acp-21-17291-2021, 2021
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The article introduces the ACP readership to ongoing research in Germany on cloud- and precipitation-related process information inherent in polarimetric radar measurements, outlines pathways to inform atmospheric models with radar-based information, and points to remaining challenges towards an improved fusion of radar polarimetry and atmospheric modelling.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
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.
Caterina Mogno, Paul I. Palmer, Christoph Knote, Fei Yao, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 10881–10909, https://doi.org/10.5194/acp-21-10881-2021, https://doi.org/10.5194/acp-21-10881-2021, 2021
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We use a 3-D atmospheric chemistry model to investigate how seasonal emissions sources and meteorological conditions affect the surface distribution of fine particulate matter (PM2.5) and organic aerosol (OA) over the Indo-Gangetic Plain. We find that all seasonal mean values of PM2.5 still exceed safe air quality levels, with human emissions contributing to PM2.5 all year round, open fires during post- and pre-monsoon, and biogenic emissions during monsoon. OA contributes up to 30 % to PM2.5.
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
Julian Kostinek, Anke Roiger, Maximilian Eckl, Alina Fiehn, Andreas Luther, Norman Wildmann, Theresa Klausner, Andreas Fix, Christoph Knote, Andreas Stohl, and André Butz
Atmos. Chem. Phys., 21, 8791–8807, https://doi.org/10.5194/acp-21-8791-2021, https://doi.org/10.5194/acp-21-8791-2021, 2021
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Abundant mining and industrial activities in the Upper Silesian Coal Basin lead to large emissions of the potent greenhouse gas methane. This study quantifies these emissions with continuous, high-precision airborne measurements and dispersion modeling. Our emission estimates are in line with values reported in the European Pollutant Release and Transfer Register (E-PRTR 2017) but significantly lower than values reported in the Emissions Database for Global Atmospheric Research (EDGAR v4.3.2).
James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
Atmos. Chem. Phys., 21, 5015–5061, https://doi.org/10.5194/acp-21-5015-2021, https://doi.org/10.5194/acp-21-5015-2021, 2021
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Stratospheric ozone and water vapour are key components of the Earth system; changes to both have important impacts on global and regional climate. We evaluate changes to these species from 1850 to 2100 in the new generation of CMIP6 models. There is good agreement between the multi-model mean and observations, although there is substantial variation between the individual models. The future evolution of both ozone and water vapour is strongly dependent on the assumed future emissions scenario.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
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.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
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.
Jim M. Haywood, Steven J. Abel, Paul A. Barrett, Nicolas Bellouin, Alan Blyth, Keith N. Bower, Melissa Brooks, Ken Carslaw, Haochi Che, Hugh Coe, Michael I. Cotterell, Ian Crawford, Zhiqiang Cui, Nicholas Davies, Beth Dingley, Paul Field, Paola Formenti, Hamish Gordon, Martin de Graaf, Ross Herbert, Ben Johnson, Anthony C. Jones, Justin M. Langridge, Florent Malavelle, Daniel G. Partridge, Fanny Peers, Jens Redemann, Philip Stier, Kate Szpek, Jonathan W. Taylor, Duncan Watson-Parris, Robert Wood, Huihui Wu, and Paquita Zuidema
Atmos. Chem. Phys., 21, 1049–1084, https://doi.org/10.5194/acp-21-1049-2021, https://doi.org/10.5194/acp-21-1049-2021, 2021
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Every year, the seasonal cycle of biomass burning from agricultural practices in Africa creates a huge plume of smoke that travels many thousands of kilometres over the Atlantic Ocean. This study provides an overview of a measurement campaign called the cloud–aerosol–radiation interaction and forcing for year 2017 (CLARIFY-2017) and documents the rationale, deployment strategy, observations, and key results from the campaign which utilized the heavily equipped FAAM atmospheric research aircraft.
Haochi Che, Philip Stier, Hamish Gordon, Duncan Watson-Parris, and Lucia Deaconu
Atmos. Chem. Phys., 21, 17–33, https://doi.org/10.5194/acp-21-17-2021, https://doi.org/10.5194/acp-21-17-2021, 2021
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The south-eastern Atlantic is semi-permanently covered by some of the largest stratocumulus clouds and is influenced by one-third of the biomass burning emissions from African fires. A UKEMS1 model simulation shows that the absorption effect of biomass burning aerosols is the most significant on clouds and radiation. The dominate cooling and rapid adjustments induced by the radiative effects of biomass burning aerosols result in an overall cooling in the south-eastern Atlantic.
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.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Ben Silver, Luke Conibear, Carly L. Reddington, Christoph Knote, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 20, 11683–11695, https://doi.org/10.5194/acp-20-11683-2020, https://doi.org/10.5194/acp-20-11683-2020, 2020
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China suffers from serious air pollution, which is thought to cause millions of early deaths each year. Measurements on the ground show that overall air quality is improving. Air quality is also affected by weather conditions, which can vary from year to year. We conduct computer simulations to show it is the reduction of the amount of pollution emitted, rather than weather conditions, which caused air quality to improve during 2015–2017. We then estimate that 150 000 fewer people die early.
Yohei Shinozuka, Pablo E. Saide, Gonzalo A. Ferrada, Sharon P. Burton, Richard Ferrare, Sarah J. Doherty, Hamish Gordon, Karla Longo, Marc Mallet, Yan Feng, Qiaoqiao Wang, Yafang Cheng, Amie Dobracki, Steffen Freitag, Steven G. Howell, Samuel LeBlanc, Connor Flynn, Michal Segal-Rosenhaimer, Kristina Pistone, James R. Podolske, Eric J. Stith, Joseph Ryan Bennett, Gregory R. Carmichael, Arlindo da Silva, Ravi Govindaraju, Ruby Leung, Yang Zhang, Leonhard Pfister, Ju-Mee Ryoo, Jens Redemann, Robert Wood, and Paquita Zuidema
Atmos. Chem. Phys., 20, 11491–11526, https://doi.org/10.5194/acp-20-11491-2020, https://doi.org/10.5194/acp-20-11491-2020, 2020
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In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016.
Hamish Gordon, Paul R. Field, Steven J. Abel, Paul Barrett, Keith Bower, Ian Crawford, Zhiqiang Cui, Daniel P. Grosvenor, Adrian A. Hill, Jonathan Taylor, Jonathan Wilkinson, Huihui Wu, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 10997–11024, https://doi.org/10.5194/acp-20-10997-2020, https://doi.org/10.5194/acp-20-10997-2020, 2020
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The Met Office's Unified Model is widely used both for weather forecasting and climate prediction. We present the first version of the model in which both aerosol and cloud particle mass and number concentrations are allowed to evolve separately and independently, which is important for studying how aerosols affect weather and climate. We test the model against aircraft observations near Ascension Island in the Atlantic, focusing on how aerosols can "activate" to become cloud droplets.
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.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
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.
Bruna A. Holanda, Mira L. Pöhlker, David Walter, Jorge Saturno, Matthias Sörgel, Jeannine Ditas, Florian Ditas, Christiane Schulz, Marco Aurélio Franco, Qiaoqiao Wang, Tobias Donth, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Ramon Braga, Joel Brito, Yafang Cheng, Maximilian Dollner, Johannes W. Kaiser, Thomas Klimach, Christoph Knote, Ovid O. Krüger, Daniel Fütterer, Jošt V. Lavrič, Nan Ma, Luiz A. T. Machado, Jing Ming, Fernando G. Morais, Hauke Paulsen, Daniel Sauer, Hans Schlager, Johannes Schneider, Hang Su, Bernadett Weinzierl, Adrian Walser, Manfred Wendisch, Helmut Ziereis, Martin Zöger, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 20, 4757–4785, https://doi.org/10.5194/acp-20-4757-2020, https://doi.org/10.5194/acp-20-4757-2020, 2020
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Biomass burning smoke from African savanna and grassland is transported across the South Atlantic Ocean in defined layers within the free troposphere. The combination of in situ aircraft and ground-based measurements aided by satellite observations showed that these layers are transported into the Amazon Basin during the early dry season. The influx of aged smoke, enriched in black carbon and cloud condensation nuclei, has important implications for the Amazonian aerosol and cloud cycling.
Daniel T. McCoy, Paul Field, Hamish Gordon, Gregory S. Elsaesser, and Daniel P. Grosvenor
Atmos. Chem. Phys., 20, 4085–4103, https://doi.org/10.5194/acp-20-4085-2020, https://doi.org/10.5194/acp-20-4085-2020, 2020
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Incomplete understanding of how aerosol affects clouds degrades our ability to predict future climate. In particular, it is unclear how aerosol affects the lifetime of clouds. Does it increase or decrease it? This confusion is partially because causality flows from aerosol to clouds and clouds to aerosol, and it is hard to tell what is happening in observations. Here, we use simulations to tell us about how clouds affect aerosol and use this to interpret observations, showing increased lifetime.
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.
Pascal Polonik, Christoph Knote, Tobias Zinner, Florian Ewald, Tobias Kölling, Bernhard Mayer, Meinrat O. Andreae, Tina Jurkat-Witschas, Thomas Klimach, Christoph Mahnke, Sergej Molleker, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Ralf Weigel, and Manfred Wendisch
Atmos. Chem. Phys., 20, 1591–1605, https://doi.org/10.5194/acp-20-1591-2020, https://doi.org/10.5194/acp-20-1591-2020, 2020
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A realistic representation of cloud–aerosol interactions is central to accurate climate projections. Here we combine observations collected during the ACRIDICON-CHUVA campaign with chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysics. We find an upper limit for the model sensitivity on cloud condensation nuclei concentrations well below the levels reached during the burning season in the Amazon Basin.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
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.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Carly L. Reddington, Luke Conibear, Christoph Knote, Ben J. Silver, Yong J. Li, Chak K. Chan, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 19, 11887–11910, https://doi.org/10.5194/acp-19-11887-2019, https://doi.org/10.5194/acp-19-11887-2019, 2019
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We use a high-resolution model over South and East Asia to explore air quality and human health benefits of eliminating emissions from six man-made pollution sources. We find that preventing emissions from either residential energy use, industry, or open biomass burning yields the largest reductions in ground-level particulate matter pollution and its associated disease burden over this region. We also summarize previous estimates of the source-specific disease burden in China and India.
Laura Kiely, Dominick V. Spracklen, Christine Wiedinmyer, Luke Conibear, Carly L. Reddington, Scott Archer-Nicholls, Douglas Lowe, Stephen R. Arnold, Christoph Knote, Md Firoz Khan, Mohd Talib Latif, Mikinori Kuwata, Sri Hapsari Budisulistiorini, and Lailan Syaufina
Atmos. Chem. Phys., 19, 11105–11121, https://doi.org/10.5194/acp-19-11105-2019, https://doi.org/10.5194/acp-19-11105-2019, 2019
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In 2015, a large fire episode occurred in Indonesia, reducing air quality. Fires occurred predominantly on peatland, where large uncertainties are associated with emissions. Current fire emissions datasets underestimate peat fire emissions. We created new fire emissions data, with data specific to Indonesian peat fires. Using these emissions in simulations of particulate matter and aerosol optical depth shows an improvement over simulations using current data, when compared with observations.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
David C. Wade, Nathan Luke Abraham, Alexander Farnsworth, Paul J. Valdes, Fran Bragg, and Alexander T. Archibald
Clim. Past, 15, 1463–1483, https://doi.org/10.5194/cp-15-1463-2019, https://doi.org/10.5194/cp-15-1463-2019, 2019
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The amount of O2 in the atmosphere may have varied from as little as 10 % to as much as 35 % during the last 541 Myr. These changes are large enough to have led to changes in atmospheric mass, which may alter the radiative budget of the atmosphere. We present the first fully 3-D numerical model simulations to investigate the climate impacts of changes in O2 during different climate states. We identify a complex new mechanism causing increases in surface temperature when O2 levels were higher.
Matthew J. Rowlinson, Alexandru Rap, Stephen R. Arnold, Richard J. Pope, Martyn P. Chipperfield, Joe McNorton, Piers Forster, Hamish Gordon, Kirsty J. Pringle, Wuhu Feng, Brian J. Kerridge, Barry L. Latter, and Richard Siddans
Atmos. Chem. Phys., 19, 8669–8686, https://doi.org/10.5194/acp-19-8669-2019, https://doi.org/10.5194/acp-19-8669-2019, 2019
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Wildfires and meteorology have a substantial effect on atmospheric concentrations of greenhouse gases such as methane and ozone. During the 1997 El Niño event, unusually large fire emissions indirectly increased global methane through carbon monoxide emission, which decreased the oxidation capacity of the atmosphere. There were also large regional changes to tropospheric ozone concentrations, but contrasting effects of fire and meteorology resulted in a small change to global radiative forcing.
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.
John T. Sullivan, Thomas J. McGee, Ryan M. Stauffer, Anne M. Thompson, Andrew Weinheimer, Christoph Knote, Scott Janz, Armin Wisthaler, Russell Long, James Szykman, Jinsoo Park, Youngjae Lee, Saewung Kim, Daun Jeong, Dianne Sanchez, Laurence Twigg, Grant Sumnicht, Travis Knepp, and Jason R. Schroeder
Atmos. Chem. Phys., 19, 5051–5067, https://doi.org/10.5194/acp-19-5051-2019, https://doi.org/10.5194/acp-19-5051-2019, 2019
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During the May–June 2016 International Cooperative Air Quality Field Study in Korea (KORUS-AQ), pollution reached the remote Taehwa Research Forest (TRF) site. Two case studies are examined and observations clearly identify TRF and the surrounding rural areas as long-term receptor sites for severe urban pollution events. In summary, domestic emissions may be causing more pollution than by transboundary pathways, which have been historically believed to be the major source of air pollution.
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.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
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.
Hamish Gordon, Paul R. Field, Steven J. Abel, Mohit Dalvi, Daniel P. Grosvenor, Adrian A. Hill, Ben T. Johnson, Annette K. Miltenberger, Masaru Yoshioka, and Ken S. Carslaw
Atmos. Chem. Phys., 18, 15261–15289, https://doi.org/10.5194/acp-18-15261-2018, https://doi.org/10.5194/acp-18-15261-2018, 2018
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Smoke from African fires is frequently transported across the Atlantic Ocean, where it interacts with clouds. We simulate the interaction of the smoke with the clouds, and the consequences of this for the solar radiation the clouds reflect. The simulations use a new regional configuration of the UK Met Office climate model. Our simulations indicate that the properties of the clouds, in particular their height and reflectivity, and the fractional cloud cover, are strongly affected by the smoke.
Christiane Schulz, Johannes Schneider, Bruna Amorim Holanda, Oliver Appel, Anja Costa, Suzane S. de Sá, Volker Dreiling, Daniel Fütterer, Tina Jurkat-Witschas, Thomas Klimach, Christoph Knote, Martina Krämer, Scot T. Martin, Stephan Mertes, Mira L. Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Bernadett Weinzierl, Helmut Ziereis, Martin Zöger, Meinrat O. Andreae, Paulo Artaxo, Luiz A. T. Machado, Ulrich Pöschl, Manfred Wendisch, and Stephan Borrmann
Atmos. Chem. Phys., 18, 14979–15001, https://doi.org/10.5194/acp-18-14979-2018, https://doi.org/10.5194/acp-18-14979-2018, 2018
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Aerosol chemical composition measurements in the tropical upper troposphere over the Amazon region show that 78 % of the aerosol in the upper troposphere consists of organic matter. Up to 20 % of the organic aerosol can be attributed to isoprene epoxydiol secondary organic aerosol (IEPOX-SOA). Furthermore, organic nitrates were identified, suggesting a connection to the IEPOX-SOA formation.
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.
Christoph Knote, Jérôme Barré, and Max Eckl
Geosci. Model Dev., 11, 561–573, https://doi.org/10.5194/gmd-11-561-2018, https://doi.org/10.5194/gmd-11-561-2018, 2018
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The Background Error Analysis Testbed with Box Models (BEATBOX) is a toy model to investigate the effects of data assimilation on systems like tropospheric photochemistry in a box model fashion. We present the model system and show its application in a case study using data from a recent field campaign and employing commonly used tropospheric chemistry mechanisms.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
Atmos. Chem. Phys., 18, 921–961, https://doi.org/10.5194/acp-18-921-2018, https://doi.org/10.5194/acp-18-921-2018, 2018
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We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Kathrin Gatzsche, Yoshiteru Iinuma, Andreas Tilgner, Anke Mutzel, Torsten Berndt, and Ralf Wolke
Atmos. Chem. Phys., 17, 13187–13211, https://doi.org/10.5194/acp-17-13187-2017, https://doi.org/10.5194/acp-17-13187-2017, 2017
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Secondary organic aerosol (SOA) represents an important fraction of the particulate matter and, thus, an advanced treatment of SOA processes in models is necessary. Therefore, this investigation aims at sensitivity studies of a kinetic description of SOA formation. The results reveal that the particle-phase state and the reactivity of the organic solutes are key parameters in the SOA formation. Overall, the results show that an advanced kinetic treatment enables improved model predictions.
Huan Yao, Yu Song, Mingxu Liu, Scott Archer-Nicholls, Douglas Lowe, Gordon McFiggans, Tingting Xu, Pin Du, Jianfeng Li, Yusheng Wu, Min Hu, Chun Zhao, and Tong Zhu
Atmos. Chem. Phys., 17, 5205–5219, https://doi.org/10.5194/acp-17-5205-2017, https://doi.org/10.5194/acp-17-5205-2017, 2017
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
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.
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
Stefanie Richters, Hartmut Herrmann, and Torsten Berndt
Atmos. Chem. Phys., 16, 9831–9845, https://doi.org/10.5194/acp-16-9831-2016, https://doi.org/10.5194/acp-16-9831-2016, 2016
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New reaction pathways of highly oxidized multifunctional organic compounds (HOMs) from the ozonolysis of the sesquiterpene (C15H24) beta-caryophyllene were elucidated based on experiments using isotopically labelled ozone and H/D exchange experiments. These new insights in reaction pathways of unsaturated RO2 radicals are responsible for the production of about two-thirds of the detected HOMs from beta-caryophyllene and extend the knowledge of HOM formation mechanisms in the atmosphere.
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
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
Scott Archer-Nicholls, Douglas Lowe, David M. Schultz, and Gordon McFiggans
Atmos. Chem. Phys., 16, 5573–5594, https://doi.org/10.5194/acp-16-5573-2016, https://doi.org/10.5194/acp-16-5573-2016, 2016
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The response of the Weather Research and Forecasting model with Chemistry to forcings by biomass burning aerosol were investigated in high-resolution nested domains over Brazil. The aerosol-layer was found to have a negative direct effect at the top of the atmosphere, but this was largely cancelled by a semi-direct effect which inhibited afternoon cloud formation. The cloud response to the aerosol was found to be highly sensitive to model resolution and the use of convective parameterisation.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
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
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
Y. Zheng, N. Unger, A. Hodzic, L. Emmons, C. Knote, S. Tilmes, J.-F. Lamarque, and P. Yu
Atmos. Chem. Phys., 15, 13487–13506, https://doi.org/10.5194/acp-15-13487-2015, https://doi.org/10.5194/acp-15-13487-2015, 2015
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Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
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.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
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.
O. J. Squire, A. T. Archibald, P. T. Griffiths, M. E. Jenkin, D. Smith, and J. A. Pyle
Atmos. Chem. Phys., 15, 5123–5143, https://doi.org/10.5194/acp-15-5123-2015, https://doi.org/10.5194/acp-15-5123-2015, 2015
S. Archer-Nicholls, D. Lowe, E. Darbyshire, W. T. Morgan, M. M. Bela, G. Pereira, J. Trembath, J. W. Kaiser, K. M. Longo, S. R. Freitas, H. Coe, and G. McFiggans
Geosci. Model Dev., 8, 549–577, https://doi.org/10.5194/gmd-8-549-2015, https://doi.org/10.5194/gmd-8-549-2015, 2015
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The regional WRF-Chem model was used to study aerosol particles from biomass burning in South America. The modelled estimates of fire plume injection heights were found to be too high, with serious implications for modelled aerosol vertical distribution, transport and impacts on local climate. A modified emission scenario was developed which improved the predicted injection height. Model results were compared and evaluated against in situ measurements from the 2012 SAMBBA flight campaign.
D. Lowe, S. Archer-Nicholls, W. Morgan, J. Allan, S. Utembe, B. Ouyang, E. Aruffo, M. Le Breton, R. A. Zaveri, P. Di Carlo, C. Percival, H. Coe, R. Jones, and G. McFiggans
Atmos. Chem. Phys., 15, 1385–1409, https://doi.org/10.5194/acp-15-1385-2015, https://doi.org/10.5194/acp-15-1385-2015, 2015
C. Knote, A. Hodzic, and J. L. Jimenez
Atmos. Chem. Phys., 15, 1–18, https://doi.org/10.5194/acp-15-1-2015, https://doi.org/10.5194/acp-15-1-2015, 2015
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Organic material found in ambient aerosol is mostly formed through the oxidation of gaseous precursors. It is semi-volatile under atmospheric conditions, and it continuously partitions between the gas and particle phases. At the same time, it is also highly water soluble. We show that wet and especially dry deposition of semi-volatile organic compounds in the gas phase are major indirect removal pathways for the particle phase, and hence need to be accurately accounted for in modeling studies.
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
S. Archer-Nicholls, D. Lowe, S. Utembe, J. Allan, R. A. Zaveri, J. D. Fast, Ø. Hodnebrog, H. Denier van der Gon, and G. McFiggans
Geosci. Model Dev., 7, 2557–2579, https://doi.org/10.5194/gmd-7-2557-2014, https://doi.org/10.5194/gmd-7-2557-2014, 2014
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
R. Kumar, M. C. Barth, S. Madronich, M. Naja, G. R. Carmichael, G. G. Pfister, C. Knote, G. P. Brasseur, N. Ojha, and T. Sarangi
Atmos. Chem. Phys., 14, 6813–6834, https://doi.org/10.5194/acp-14-6813-2014, https://doi.org/10.5194/acp-14-6813-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 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
T. Berndt, M. Sipilä, F. Stratmann, T. Petäjä, J. Vanhanen, J. Mikkilä, J. Patokoski, R. Taipale, R. L. Mauldin III, and M. Kulmala
Atmos. Chem. Phys., 14, 751–764, https://doi.org/10.5194/acp-14-751-2014, https://doi.org/10.5194/acp-14-751-2014, 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
C. Knote and D. Brunner
Atmos. Chem. Phys., 13, 1177–1192, https://doi.org/10.5194/acp-13-1177-2013, https://doi.org/10.5194/acp-13-1177-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Constraining the budget of atmospheric carbonyl sulfide using a 3-D chemical transport model
Atmospheric CO2 inversion reveals the Amazon as a minor carbon source caused by fire emissions, with forest uptake offsetting about half of these emissions
Rapid O3 assimilations – Part 2: Tropospheric O3 changes accompanied by declining NOx emissions in the USA and Europe in 2005–2020
High-resolution air quality simulations of ozone exceedance events during the Lake Michigan Ozone Study
Simulations of winter ozone in the Upper Green River basin, Wyoming, using WRF-Chem
Measurement report: Assessment of Asian emissions of ethane and propane with a chemistry transport model based on observations from the island of Hateruma
Sensitivity of northeastern US surface ozone predictions to the representation of atmospheric chemistry in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0)
Daytime isoprene nitrates under changing NOx and O3
Atmospheric data support a multi-decadal shift in the global methane budget towards natural tropical emissions
Air quality and related health impact in the UNECE region: source attribution and scenario analysis
East Asian methane emissions inferred from high-resolution inversions of GOSAT and TROPOMI observations: a comparative and evaluative analysis
Towards near-real-time air pollutant and greenhouse gas emissions: lessons learned from multiple estimates during the COVID-19 pandemic
Spatiotemporal variation of radionuclide dispersion from nuclear power plant accidents using FLEXPART mini-ensemble modeling
Continuous weekly monitoring of methane emissions from the Permian Basin by inversion of TROPOMI satellite observations
Western European emission estimates of CFC-11, CFC-12 and CCl4 derived from atmospheric measurements from 2008 to 2021
Estimating methane emissions in the Arctic nations using surface observations from 2008 to 2019
Background nitrogen dioxide (NO2) over the United States and its implications for satellite observations and trends: effects of nitrate photolysis, aircraft, and open fires
Seasonal, interannual and decadal variability of tropospheric ozone in the North Atlantic: comparison of UM-UKCA and remote sensing observations for 2005–2018
Quantification of oil and gas methane emissions in the Delaware and Marcellus basins using a network of continuous tower-based measurements
Global sensitivities of reactive N and S gas and particle concentrations and deposition to precursor emissions reductions
Large simulated future changes in the nitrate radical under the CMIP6 SSP scenarios: implications for oxidation chemistry
Impact of HO2 aerosol uptake on radical levels and O3 production during summertime in Beijing
Source attribution of near-surface ozone trends in the United States during 1995–2019
What controls ozone sensitivity in the upper tropical troposphere?
Exploring the drivers of tropospheric hydroxyl radical trends in the Geophysical Fluid Dynamics Laboratory AM4.1 atmospheric chemistry–climate model
Impacts of land cover changes on biogenic emission and its contribution to ozone and secondary organic aerosol in China
High-resolution regional emission inventory contributes to the evaluation of policy effectiveness: a case study in Jiangsu Province, China
Why is ozone in South Korea and the Seoul metropolitan area so high and increasing?
Vehicular ammonia emissions: an underappreciated emission source in densely populated areas
Improving ozone simulations in Asia via multisource data assimilation: results from an observing system simulation experiment with GEMS geostationary satellite observations
A three-dimensional simulation and process analysis of tropospheric ozone depletion events (ODEs) during the springtime in the Arctic using CMAQ (Community Multiscale Air Quality Modeling System)
A high-resolution satellite-based map of global methane emissions reveals missing wetland, fossil fuel, and monsoon sources
Global impact of the COVID-19 lockdown on surface concentration and health risk of atmospheric benzene
Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity and pollution transport over the Catalonia region
Variable effects of spatial resolution on modeling of nitrogen oxides
Atmospheric composition and climate impacts of a future hydrogen economy
Tropospheric NO2 vertical profiles over South Korea and their relation to oxidant chemistry: implications for geostationary satellite retrievals and the observation of NO2 diurnal variation from space
A regional modelling study of halogen chemistry within a volcanic plume of Mt Etna’s Christmas 2018 eruption
Assessment of isoprene and near surface ozone sensitivities to water stress over the Euro-Mediterranean region
Simulating impacts on UK air quality from net-zero forest planting scenarios
Potential impact of shipping on air pollution in the Mediterranean region – a multimodel evaluation: comparison of photooxidants NO2 and O3
Development, intercomparison and evaluation of an improved mechanism for the oxidation of dimethyl sulfide in the UKCA model
Summertime ozone pollution in China affected by stratospheric quasi-biennial oscillation
Declining, seasonal-varying emissions of sulfur hexafluoride from the United States
Nitrogen oxides in the free troposphere: implications for tropospheric oxidants and the interpretation of satellite NO2 measurements
Climate-driven deterioration of future ozone pollution in Asia predicted by machine learning with multi-source data
Reconciling the bottom-up and top-down estimates of the methane chemical sink using multiple observations
Arctic tropospheric ozone: assessment of current knowledge and model performance
Chloride (HCl ∕ Cl−) dominates inorganic aerosol formation from ammonia in the Indo-Gangetic Plain during winter: modeling and comparison with observations
Inferring and evaluating satellite-based constraints on NOx emissions estimates in air quality simulations
Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
Atmos. Chem. Phys., 23, 10035–10056, https://doi.org/10.5194/acp-23-10035-2023, https://doi.org/10.5194/acp-23-10035-2023, 2023
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A 3-D chemical transport model, TOMCAT, is used to simulate global atmospheric carbonyl sulfide (OCS) distribution. Modelled OCS compares well with satellite observations of OCS from limb-sounding satellite observations. Model simulations also compare adequately with surface and atmospheric observations and suitably capture the seasonality of OCS and background concentrations.
Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
Atmos. Chem. Phys., 23, 9685–9723, https://doi.org/10.5194/acp-23-9685-2023, https://doi.org/10.5194/acp-23-9685-2023, 2023
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The Amazon’s carbon balance may have changed due to forest degradation, deforestation and warmer climate. We used an atmospheric model and atmospheric CO2 observations to quantify Amazonian carbon emissions (2010–2018). The region was a small carbon source to the atmosphere, mostly due to fire emissions. Forest uptake compensated for ~ 50 % of the fire emissions, meaning that the remaining forest is still a small carbon sink. We found no clear evidence of weakening carbon uptake over the period.
Rui Zhu, Zhaojun Tang, Xiaokang Chen, Xiong Liu, and Zhe Jiang
Atmos. Chem. Phys., 23, 9745–9763, https://doi.org/10.5194/acp-23-9745-2023, https://doi.org/10.5194/acp-23-9745-2023, 2023
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Ozone Monitoring Instrument (OMI) and surface O3 observations are used to investigate the changes in tropospheric O3 in the USA and Europe in 2005–2020. The surface-based assimilations show limited changes in surface and tropospheric column O3. The OMI-based assimilations show larger decreases in tropospheric O3 columns in 2010–2014, related to a decline in free-tropospheric NO2. Analysis suggests limited impacts of local emissions decline on tropospheric O3 over the USA and Europe in 2005–2020.
R. Bradley Pierce, Monica Harkey, Allen Lenzen, Lee M. Cronce, Jason A. Otkin, Jonathan L. Case, David S. Henderson, Zac Adelman, Tsengel Nergui, and Christopher R. Hain
Atmos. Chem. Phys., 23, 9613–9635, https://doi.org/10.5194/acp-23-9613-2023, https://doi.org/10.5194/acp-23-9613-2023, 2023
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We evaluate two high-resolution model simulations with different meteorological inputs but identical chemistry and anthropogenic emissions, with the goal of identifying a model configuration best suited for characterizing air quality in locations where lake breezes commonly affect local air quality along the Lake Michigan shoreline. This analysis complements other studies in evaluating the impact of meteorological inputs and parameterizations on air quality in a complex environment.
Shreta Ghimire, Zachary J. Lebo, Shane Murphy, Stefan Rahimi, and Trang Tran
Atmos. Chem. Phys., 23, 9413–9438, https://doi.org/10.5194/acp-23-9413-2023, https://doi.org/10.5194/acp-23-9413-2023, 2023
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High wintertime ozone levels have occurred often in recent years in mountain basins with oil and gas production facilities. Photochemical modeling of ozone production serves as a basis for understanding the mechanism by which it occurs and for predictive capability. We present photochemical model simulations of ozone formation and accumulation in the Upper Green River basin, Wyoming, demonstrating the model's ability to simulate wintertime ozone and the sensitivity of ozone to its precursors.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Alfred W. Mayhew, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 23, 8473–8485, https://doi.org/10.5194/acp-23-8473-2023, https://doi.org/10.5194/acp-23-8473-2023, 2023
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper investigates modelled changes to daytime isoprene nitrate concentrations resulting from changes in NOx and O3. The results highlight the complex, nonlinear chemistry of this group of species under typical conditions for megacities such as Beijing, with many species showing increased concentrations when NOx is decreased and/or ozone is increased.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452, https://doi.org/10.5194/acp-23-8429-2023, https://doi.org/10.5194/acp-23-8429-2023, 2023
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Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Claudio A. Belis and Rita Van Dingenen
Atmos. Chem. Phys., 23, 8225–8240, https://doi.org/10.5194/acp-23-8225-2023, https://doi.org/10.5194/acp-23-8225-2023, 2023
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The study assesses the influence that abating emissions in the rest of the world have on exposure and mortality due to ozone and fine particulate matter in the region covered by the Gothenburg protocol (UNECE, mainly Europe and North America). To that end, the impacts of pollutants derived from different geographic areas and anthropogenic sources are analysed in a series of scenarios including measures to abate air pollutants and greenhouse gas emissions with different levels of ambition.
Ruosi Liang, Yuzhong Zhang, Wei Chen, Peixuan Zhang, Jingran Liu, Cuihong Chen, Huiqin Mao, Guofeng Shen, Zhen Qu, Zichong Chen, Minqiang Zhou, Pucai Wang, Robert J. Parker, Hartmut Boesch, Alba Lorente, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 8039–8057, https://doi.org/10.5194/acp-23-8039-2023, https://doi.org/10.5194/acp-23-8039-2023, 2023
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We compare and evaluate East Asian methane emissions inferred from different satellite observations (GOSAT and TROPOMI). The results show discrepancies over northern India and eastern China. Independent ground-based observations are more consistent with TROPOMI-derived emissions in northern India and GOSAT-derived emissions in eastern China.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Claire Granier, Thierno Doumbia, Philippe Ciais, Zhu Liu, Robin D. Lamboll, Sabine Schindlbacher, Bradley Matthews, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8081–8101, https://doi.org/10.5194/acp-23-8081-2023, https://doi.org/10.5194/acp-23-8081-2023, 2023
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This study provides an intercomparison of European 2020 emission changes derived from official inventories, which are reported by countries under the framework of several international conventions and directives, and non-official near-real-time estimates, the use of which has significantly grown since the COVID-19 outbreak. The results of the work are used to produce recommendations on how best to approach and make use of near-real-time emissions for modelling and monitoring applications.
Seyed Omid Nabavi, Theodoros Christoudias, Yiannis Proestos, Christos Fountoukis, Huda Al-Sulaiti, and Jos Lelieveld
Atmos. Chem. Phys., 23, 7719–7739, https://doi.org/10.5194/acp-23-7719-2023, https://doi.org/10.5194/acp-23-7719-2023, 2023
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The objective of our study is to comprehensively assess the timing of radioactive material transportation and deposition, along with the associated population exposure in the designated region. We employed diverse meteorological inputs, emission specifics, and simulation codes, aiming to quantify the level of uncertainty.
Daniel J. Varon, Daniel J. Jacob, Benjamin Hmiel, Ritesh Gautam, David R. Lyon, Mark Omara, Melissa Sulprizio, Lu Shen, Drew Pendergrass, Hannah Nesser, Zhen Qu, Zachary R. Barkley, Natasha L. Miles, Scott J. Richardson, Kenneth J. Davis, Sudhanshu Pandey, Xiao Lu, Alba Lorente, Tobias Borsdorff, Joannes D. Maasakkers, and Ilse Aben
Atmos. Chem. Phys., 23, 7503–7520, https://doi.org/10.5194/acp-23-7503-2023, https://doi.org/10.5194/acp-23-7503-2023, 2023
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We use TROPOMI satellite observations to quantify weekly methane emissions from the US Permian oil and gas basin from May 2018 to October 2020. We find that Permian emissions are highly variable, with diverse economic and activity drivers. The most important drivers during our study period were new well development and natural gas price. Permian methane intensity averaged 4.6 % and decreased by 1 % per year.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
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Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, Joël Thanwerdas, Adrien Martinez, Jean-Daniel Paris, Toshinobu Machida, Motoki Sasakawa, Douglas E. J. Worthy, Xin Lan, Rona L. Thompson, Espen Sollum, and Mikhail Arshinov
Atmos. Chem. Phys., 23, 6457–6485, https://doi.org/10.5194/acp-23-6457-2023, https://doi.org/10.5194/acp-23-6457-2023, 2023
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Here, an inverse modelling approach is applied to estimate CH4 sources and sinks in the Arctic from 2008 to 2019. We study the magnitude, seasonal patterns and trends from different sources during recent years. We also assess how the current observation network helps to constrain fluxes. We find that constraints are only significant for North America and, to a lesser extent, West Siberia, where the observation network is relatively dense. We find no clear trend over the period of inversion.
Ruijun Dang, Daniel J. Jacob, Viral Shah, Sebastian D. Eastham, Thibaud M. Fritz, Loretta J. Mickley, Tianjia Liu, Yi Wang, and Jun Wang
Atmos. Chem. Phys., 23, 6271–6284, https://doi.org/10.5194/acp-23-6271-2023, https://doi.org/10.5194/acp-23-6271-2023, 2023
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We use the GEOS-Chem model to better understand the magnitude and trend in free tropospheric NO2 over the contiguous US. Model underestimate of background NO2 is largely corrected by considering aerosol nitrate photolysis. Increase in aircraft emissions affects satellite retrievals by altering the NO2 shape factor, and this effect is expected to increase in future. We show the importance of properly accounting for the free tropospheric background in interpreting NO2 observations from space.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
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Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Zachary Barkley, Kenneth Davis, Natasha Miles, Scott Richardson, Aijun Deng, Benjamin Hmiel, David Lyon, and Thomas Lauvaux
Atmos. Chem. Phys., 23, 6127–6144, https://doi.org/10.5194/acp-23-6127-2023, https://doi.org/10.5194/acp-23-6127-2023, 2023
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Using methane monitoring instruments attached to towers, we measure methane concentrations and quantify methane emissions coming from the Marcellus and Permian oil and gas basins. In the Marcellus, emissions were 3 times higher than the state inventory across the entire monitoring period. In the Permian, we see a sharp decline in emissions aligning with the onset of the COVID-19 pandemic. Tower observational networks can be utilized in other basins for long-term monitoring of emissions.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 23, 6083–6112, https://doi.org/10.5194/acp-23-6083-2023, https://doi.org/10.5194/acp-23-6083-2023, 2023
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The sensitivity of fine particles and reactive N and S species to reductions in precursor emissions is investigated using the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) atmospheric chemistry transport model. This study reveals that the individual emissions reduction has multiple and geographically varying co-benefits and small disbenefits on different species, demonstrating the importance of prioritizing regional emissions controls.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
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The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Pengwei Li, Yang Yang, Hailong Wang, Su Li, Ke Li, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 23, 5403–5417, https://doi.org/10.5194/acp-23-5403-2023, https://doi.org/10.5194/acp-23-5403-2023, 2023
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We use a novel technique that can attribute O3 to precursors to investigate O3 changes in the United States during 1995–2019. We found that the US domestic energy and surface transportation emission reductions are primarily responsible for the O3 decrease in summer. In winter, factors such as nitrogen oxide emission reduction in the context of its inhibition of ozone production, increased aviation and shipping activities, and large-scale circulation changes contribute to the O3 increases.
Clara M. Nussbaumer, Horst Fischer, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2023-816, https://doi.org/10.5194/egusphere-2023-816, 2023
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Ozone is a greenhouse gas and contributes to the earth’s radiative energy budget and therefore to global warming. This effect is largest in the upper troposphere. In this study, we investigate the processes controlling ozone formation and the sensitivity to its precursors in the upper tropical troposphere based on model simulations by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) model. We find that NOx emissions from lightning most importantly affect ozone chemistry at these altitudes.
Glen Chua, Vaishali Naik, and Larry Wayne Horowitz
Atmos. Chem. Phys., 23, 4955–4975, https://doi.org/10.5194/acp-23-4955-2023, https://doi.org/10.5194/acp-23-4955-2023, 2023
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The hydroxyl radical (OH) is an atmospheric
detergent, removing air pollutants and greenhouse gases like methane from the atmosphere. Thus, understanding how it is changing and responding to its various drivers is important for air quality and climate. We found that OH has increased by about 5 % globally from 1980 to 2014 in our model, mostly driven by increasing nitrogen oxide (NOx) emissions. This suggests potential climate tradeoffs from air quality policies solely targeting NOx emissions.
Jinlong Ma, Shengqiang Zhu, Siyu Wang, Peng Wang, Jianmin Chen, and Hongliang Zhang
Atmos. Chem. Phys., 23, 4311–4325, https://doi.org/10.5194/acp-23-4311-2023, https://doi.org/10.5194/acp-23-4311-2023, 2023
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An updated version of the CMAQ model with biogenic volatile organic compound (BVOC) emissions from MEGAN was applied to study the impacts of different land cover inputs on O3 and secondary organic aerosol (SOA) in China. The estimated BVOC emissions ranged from 25.42 to 37.39 Tg using different leaf area index (LAI) and land cover (LC) inputs. Those differences further induced differences of 4.8–6.9 ppb in O3 concentrations and differences of 5.3–8.4 µg m−3 in SOA concentrations in China.
Chen Gu, Lei Zhang, Zidie Xu, Sijia Xia, Yutong Wang, Li Li, Zeren Wang, Qiuyue Zhao, Hanying Wang, and Yu Zhao
Atmos. Chem. Phys., 23, 4247–4269, https://doi.org/10.5194/acp-23-4247-2023, https://doi.org/10.5194/acp-23-4247-2023, 2023
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We demonstrated the development of a high-resolution emission inventory and its application to evaluate the effectiveness of emission control actions, by incorporating the improved methodology, the best available data, and air quality modeling. We show that substantial efforts for emission controls indeed played an important role in air quality improvement even with worsened meteorological conditions and that the contributions of individual measures to emission reduction were greatly changing.
Nadia K. Colombi, Daniel J. Jacob, Laura Hyesung Yang, Shixian Zhai, Viral Shah, Stuart K. Grange, Robert M. Yantosca, Soontae Kim, and Hong Liao
Atmos. Chem. Phys., 23, 4031–4044, https://doi.org/10.5194/acp-23-4031-2023, https://doi.org/10.5194/acp-23-4031-2023, 2023
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Surface ozone, detrimental to human and ecosystem health, is very high and increasing in South Korea. Using a global model of the atmosphere, we found that emissions from South Korea and China contribute equally to the high ozone observed. We found that in the absence of all anthropogenic emissions over East Asia, ozone is still very high, implying that the air quality standard in South Korea is not practically achievable unless this background external to East Asia can be decreased.
Yifan Wen, Shaojun Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 23, 3819–3828, https://doi.org/10.5194/acp-23-3819-2023, https://doi.org/10.5194/acp-23-3819-2023, 2023
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This study established a high-resolution vehicular NH3 emission inventory for mainland China to quantify the absolute value and relative importance of on-road NH3 emissions for different regions, seasons and population densities. Our results indicate that the significant role of on-road NH3 emissions in populated urban areas may have been underappreciated, suggesting the control of vehicular NH3 emission can be a feasible and cost-effective way of mitigating haze pollution in urban areas.
Lei Shu, Lei Zhu, Juseon Bak, Peter Zoogman, Han Han, Song Liu, Xicheng Li, Shuai Sun, Juan Li, Yuyang Chen, Dongchuan Pu, Xiaoxing Zuo, Weitao Fu, Xin Yang, and Tzung-May Fu
Atmos. Chem. Phys., 23, 3731–3748, https://doi.org/10.5194/acp-23-3731-2023, https://doi.org/10.5194/acp-23-3731-2023, 2023
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We quantify the benefit of multisource observations (GEMS, LEO satellite, and surface) on ozone simulations in Asia. Data assimilation improves the monitoring of exceedance, spatial pattern, and diurnal variation of surface ozone, with the regional mean bias reduced from −2.1 to −0.2 ppbv. Data assimilation also better represents ozone vertical distributions in the middle to upper troposphere at low latitudes. Our results offer a valuable reference for future ozone simulations.
Le Cao, Simeng Li, Yicheng Gu, and Yuhan Luo
Atmos. Chem. Phys., 23, 3363–3382, https://doi.org/10.5194/acp-23-3363-2023, https://doi.org/10.5194/acp-23-3363-2023, 2023
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We performed a 3-D mesoscale model study on ozone depletion events (ODEs) occurring in the spring of 2019 at Barrow using an air quality model, CMAQ. Many ODEs observed at Barrow were captured by the model, and the contribution from each physical or chemical process to ozone and bromine species during ODEs was quantitatively evaluated. We found the ODEs at Barrow to be strongly influenced by horizontal transport. In contrast, over the sea, local chemistry significantly reduced the surface ozone.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
Atmos. Chem. Phys., 23, 3325–3346, https://doi.org/10.5194/acp-23-3325-2023, https://doi.org/10.5194/acp-23-3325-2023, 2023
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We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
Chaohao Ling, Lulu Cui, and Rui Li
Atmos. Chem. Phys., 23, 3311–3324, https://doi.org/10.5194/acp-23-3311-2023, https://doi.org/10.5194/acp-23-3311-2023, 2023
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An ensemble machine-learning model coupled with chemical transport models (CTMs) was applied to assess the impact of COVID-19 on ambient benzene. The change ratio of the deweathered benzene concentration from the pre-lockdown to lockdown period was in the order of India (−23.6 %) > Europe (−21.9 %) > the United States (−16.2 %) > China (−15.6 %), which might be associated with local serious benzene pollution and substantial emission reduction in the industrial and transportation sectors.
Alba Badia, Veronica Vidal, Sergi Ventura, Roger Curcoll, Ricard Segura, and Gara Villalba
EGUsphere, https://doi.org/10.5194/egusphere-2023-160, https://doi.org/10.5194/egusphere-2023-160, 2023
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Improving air quality is a top priority in urban areas. In this study, we used an air quality model to analyse the air quality changes occurring over the Metropolitan Area of Barcelona and other rural areas affected by transport of the atmospheric plume from the city during mobility restrictions. Our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, particular ozone chemistry of the urban area.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Atmos. Chem. Phys., 23, 3031–3049, https://doi.org/10.5194/acp-23-3031-2023, https://doi.org/10.5194/acp-23-3031-2023, 2023
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Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate the variability of NOx resolution-dependent simulation biases; how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and how these biases affect the interpretation of satellite observations. High-resolution simulations are thus critical to accurately interpret NOx and its relevance to air quality.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2023-29, https://doi.org/10.5194/acp-2023-29, 2023
Revised manuscript accepted for ACP
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We have used a chemistry-climate model to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. We find that leakage of hydrogen results in an indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Herizo Narivelo, Paul David Hamer, Virginie Marécal, Luke Surl, Tjarda Roberts, Sophie Pelletier, Béatrice Josse, Jonathan Guth, Mickaël Bacles, Simon Warnach, Thomas Wagner, Stefano Corradini, Giuseppe Salerno, and Lorenzo Guerrieri
EGUsphere, https://doi.org/10.5194/egusphere-2023-184, https://doi.org/10.5194/egusphere-2023-184, 2023
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Volcanic emissions provide large amounts of gases and particles that can have important effects on the atmosphere. This is why the paper presents a study of the fate of the volcanic emissions from the Mt Etna’s eruption from 24 to 30 December 2018. Using a numerical model and satellite observations, we analyse the impact of the volcanic plume as it travels and how it modifies the air composition over the whole Mediterranean basin.
Susanna Strada, Andrea Pozzer, Filippo Giorgi, Graziano Giuliani, Erika Coppola, Fabien Solmon, Xiaoyan Jiang, and Alex Guenther
EGUsphere, https://doi.org/10.5194/egusphere-2022-1522, https://doi.org/10.5194/egusphere-2022-1522, 2023
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Water deficit modifies emissions of isoprene, an aromatic compound released by plants that influence the production of a pollutant such as surface ozone. Numerical modeling shows that, during the warmest and driest summers, isoprene decreases between −20 to −60 % over the Euro-Mediterranean region, while surface ozone only diminishes by few percents. Decreases in isoprene emissions not only happen simultaneously of dry conditions, but could also occur after prolonged or repeated water deficit.
Gemma Purser, Mathew R. Heal, Edward J. Carnell, Stephen Bathgate, Julia Drewer, James I. L. Morison, and Massimo Vieno
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-782, https://doi.org/10.5194/acp-2022-782, 2023
Revised manuscript accepted for ACP
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Forest expansion is a ‘net zero’ pathway, but change in landcover alters air quality in many ways. This study combines data on tree planting suitability with UK-specific emissions of biogenic volatile organic compound to simulate spatial and temporal changes in atmospheric composition for planting scenarios of four species. Decreases in fine particulate matter are relatively larger than increases in ozone which may indicate a net benefit of tree planting on human health aspects of air quality.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Jana Moldanova, Sara Jutterström, Jukka-Pekka Jalkanen, and Elisa Majamäki
Atmos. Chem. Phys., 23, 1825–1862, https://doi.org/10.5194/acp-23-1825-2023, https://doi.org/10.5194/acp-23-1825-2023, 2023
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Potential ship impact on air pollution in the Mediterranean Sea was simulated with five chemistry transport models. An evaluation of the results for NO2 and O3 air concentrations and dry deposition is presented. Emission data, modeled year and domain were the same. Model run outputs were compared to measurements from background stations. We focused on comparing model outputs regarding the concentration of regulatory pollutants and the relative ship impact on total air pollution concentrations.
Ben A. Cala, Scott Archer-Nicholls, James Weber, Nathan Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2023-42, https://doi.org/10.5194/acp-2023-42, 2023
Revised manuscript accepted for ACP
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DMS is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background. But its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop & compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our global model studies show our updated DMS scheme is a significant improvement. However, sensitivity studies underscore need for further lab & observational constraints.
Mengyun Li, Yang Yang, Hailong Wang, Huimin Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1533–1544, https://doi.org/10.5194/acp-23-1533-2023, https://doi.org/10.5194/acp-23-1533-2023, 2023
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Using the GEOS-Chem model, the impact of the quasi-biennial oscillation (QBO) on summertime tropospheric O3 in China is investigated. In the warm phases of sea surface temperature anomalies over the eastern tropical Pacific, the QBO has a significant positive correlation with near-surface O3 concentrations over central China. The QBO impacts on O3 pollution in China are mainly a result of changing vertical transport of O3.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448, https://doi.org/10.5194/acp-23-1437-2023, https://doi.org/10.5194/acp-23-1437-2023, 2023
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Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Huimin Li, Yang Yang, Jianbing Jin, Hailong Wang, Ke Li, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 23, 1131–1145, https://doi.org/10.5194/acp-23-1131-2023, https://doi.org/10.5194/acp-23-1131-2023, 2023
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Future climate change will aggravate ozone pollution in Asia, especially in high-forcing scenarios. Ozone pollution in China will expand from North China to South China and extend into the cold season in a warmer future. The emphasis of this work is to quantify the impacts of future climate change on O3 pollution in Asia, which is of great significance for future O3 pollution mitigation strategies.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, and Bo Zheng
Atmos. Chem. Phys., 23, 789–807, https://doi.org/10.5194/acp-23-789-2023, https://doi.org/10.5194/acp-23-789-2023, 2023
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The large uncertainties in OH simulated by atmospheric chemistry models hinder accurate estimates of CH4 chemical loss through the bottom-up method. This study presents a new approach based on OH precursor observations and a chemical box model to improve the tropospheric OH distributions simulated by atmospheric chemistry models. Through this approach, both the global OH burden and the corresponding methane chemical loss reach consistency with the top-down method based on MCF inversions.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Pooja V. Pawar, Sachin D. Ghude, Gaurav Govardhan, Prodip Acharja, Rachana Kulkarni, Rajesh Kumar, Baerbel Sinha, Vinayak Sinha, Chinmay Jena, Preeti Gunwani, Tapan Kumar Adhya, Eiko Nemitz, and Mark A. Sutton
Atmos. Chem. Phys., 23, 41–59, https://doi.org/10.5194/acp-23-41-2023, https://doi.org/10.5194/acp-23-41-2023, 2023
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In this study, for the first time in South Asia we compare simulated ammonia, ammonium, and total ammonia using the WRF-Chem model and MARGA measurements during winter in the Indo-Gangetic Plain region. Since observations show HCl promotes the fraction of high chlorides in Delhi, we added HCl / Cl emissions to the model. We conducted three sensitivity experiments with changes in HCl emissions, and improvements are reported in accurately simulating ammonia, ammonium, and total ammonia.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001, https://doi.org/10.5194/acp-22-15981-2022, https://doi.org/10.5194/acp-22-15981-2022, 2022
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We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
Cited articles
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Short summary
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.
Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle...
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