Articles | Volume 16, issue 9
https://doi.org/10.5194/acp-16-5867-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-5867-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
13 May 2016
Research article |
| 13 May 2016
Modeling lightning-NOx chemistry on a sub-grid scale in a global chemical transport model
Alicia Gressent
CORRESPONDING AUTHOR
LA, CNRS, Université de Toulouse, Toulouse, France
Bastien Sauvage
LA, CNRS, Université de Toulouse, Toulouse, France
Daniel Cariolle
Météo France, Toulouse, France
Centre Européen de Recherche et de Formation Avancée en Calcul Scientifique, CERFACS, Toulouse, France
Mathew Evans
The Wolfson Atmospheric Chemistry Laboratories, University of York, York, UK
Maud Leriche
LA, CNRS, Université de Toulouse, Toulouse, France
Céline Mari
LA, CNRS, Université de Toulouse, Toulouse, France
Valérie Thouret
LA, CNRS, Université de Toulouse, Toulouse, France
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Atmos. Chem. Phys., 25, 7991–8028, https://doi.org/10.5194/acp-25-7991-2025, https://doi.org/10.5194/acp-25-7991-2025, 2025
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This study analyzes summertime ozone trends in East and Southeast Asia derived from a comprehensive observational database spanning from 1995 to 2019, incorporating aircraft observations, ozonesonde data, and measurements from 2500 surface sites. Multiple models are applied to attribute to changes in anthropogenic emissions and climate. The results highlight that increases in anthropogenic emissions are the primary driver of ozone increases both in the free troposphere and at the surface.
Nana Wei, Eloise A. Marais, Gongda Lu, Robert G. Ryan, and Bastien Sauvage
Atmos. Chem. Phys., 25, 7925–7940, https://doi.org/10.5194/acp-25-7925-2025, https://doi.org/10.5194/acp-25-7925-2025, 2025
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This study uses reactive nitrogen observations from NASA DC-8 research aircraft and the In-service Aircraft for a Global Observing System (IAGOS) campaigns to characterize reactive nitrogen seasonality and composition in the global upper troposphere and to diagnose the greatest knowledge gaps from comparison to a state-of-the-science model, GEOS-Chem, that need to be resolved for climate, nitrogen cycle, and air pollution assessments.
Matthew James Rowlinson, Lucy J. Carpenter, Mat J. Evans, James D. Lee, Simone Andersen, Tomas Sherwen, Anna B. Callaghan, Roberto Sommariva, William Bloss, Siqi Hou, Leigh R. Crilley, Klaus Pfeilsticker, Benjamin Weyland, Thomas B. Ryerson, Patrick R. Veres, Pedro Campuzano-Jost, Hongyu Guo, Benjamin A. Nault, Jose L. Jimenez, and Khanneh Wadinga Fomba
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Anne M. Thompson, Ryan M. Stauffer, Debra E. Kollonige, Jerald R. Ziemke, Maria Cazorla, Pawel Wolff, and Bastien Sauvage
EGUsphere, https://doi.org/10.5194/egusphere-2024-3761, https://doi.org/10.5194/egusphere-2024-3761, 2025
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Tropospheric ozone is a potent greenhouse gas; its anthropogenic levels rise contributes to climate change. We evaluate tropospheric ozone trends and climate impacts with aircraft data and a radiative model, comparing the baseline period (1994–2004) to 2011–2016 and 2019. Tropospheric ozone levels increased significantly but with a smaller trend in 2019 than in 2011–2016. However, ozone radiative forcing did not decrease between these periods because of different vertical distribution evolutions
Eric Martial Yao, Fabien Solmon, Marcellin Adon, Claire Delon, Corinne Galy-Lacaux, Graziano Giuliani, Bastien Sauvage, and Véronique Yoboue
EGUsphere, https://doi.org/10.5194/egusphere-2024-3179, https://doi.org/10.5194/egusphere-2024-3179, 2025
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As climate change and human activities intensify in Africa, understanding how air pollution, climate, and natural cycles interact is crucial. This study explores how nitrogen oxide emissions from African soils, especially in dry regions, contribute to atmospheric pollution. By using a climate-chemistry model, we show that considering these emissions improves predictions of nitrogen dioxide, nitric acid and ozone, although some discrepancies remain compared to observations.
Brice Barret, Pierre Loicq, Eric Le Flochmoën, Yasmine Bennouna, Juliette Hadji-Lazaro, Daniel Hurtmans, and Bastien Sauvage
Atmos. Meas. Tech., 18, 129–149, https://doi.org/10.5194/amt-18-129-2025, https://doi.org/10.5194/amt-18-129-2025, 2025
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Profiles of carbon monoxide (CO) retrieved from the Infrared Atmospheric Sounding Interferometer (IASI) with the SOftware for a Fast Retrieval of IASI Data (SOFRID) and Fast Optimal Retrievals on Layers for IASI (FORLI) are validated with 8500 observations at 33 airports from the In-service Aircraft for a Global Observing System (IAGOS) for 2008–2019. IASI retrievals underestimate CO, with stronger bias in the middle to upper troposphere for SOFRID and in the lower troposphere for FORLI.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Audrey Gaudel, Ilann Bourgeois, Meng Li, Kai-Lan Chang, Jerald Ziemke, Bastien Sauvage, Ryan M. Stauffer, Anne M. Thompson, Debra E. Kollonige, Nadia Smith, Daan Hubert, Arno Keppens, Juan Cuesta, Klaus-Peter Heue, Pepijn Veefkind, Kenneth Aikin, Jeff Peischl, Chelsea R. Thompson, Thomas B. Ryerson, Gregory J. Frost, Brian C. McDonald, and Owen R. Cooper
Atmos. Chem. Phys., 24, 9975–10000, https://doi.org/10.5194/acp-24-9975-2024, https://doi.org/10.5194/acp-24-9975-2024, 2024
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The study examines tropical tropospheric ozone changes. In situ data from 1994–2019 display increased ozone, notably over India, Southeast Asia, and Malaysia and Indonesia. Sparse in situ data limit trend detection for the 15-year period. In situ and satellite data, with limited sampling, struggle to consistently detect trends. Continuous observations are vital over the tropical Pacific Ocean, Indian Ocean, western Africa, and South Asia for accurate ozone trend estimation in these regions.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Lucas Pailler, Laurent Deguillaume, Hélène Lavanant, Isabelle Schmitz, Marie Hubert, Edith Nicol, Mickaël Ribeiro, Jean-Marc Pichon, Mickaël Vaïtilingom, Pamela Dominutti, Frédéric Burnet, Pierre Tulet, Maud Leriche, and Angelica Bianco
Atmos. Chem. Phys., 24, 5567–5584, https://doi.org/10.5194/acp-24-5567-2024, https://doi.org/10.5194/acp-24-5567-2024, 2024
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The composition of dissolved organic matter of cloud water has been investigated through non-targeted high-resolution mass spectrometry on only a few samples collected in the Northern Hemisphere. In this work, the chemical composition of samples collected at Réunion Island (SH) is investigated and compared to samples collected at Puy de Dôme (NH). Sampling, analysis and data treatment with the same methodology produced a unique dataset for investigating the molecular composition of clouds.
Maud Leriche, Pierre Tulet, Laurent Deguillaume, Frédéric Burnet, Aurélie Colomb, Agnès Borbon, Corinne Jambert, Valentin Duflot, Stéphan Houdier, Jean-Luc Jaffrezo, Mickaël Vaïtilingom, Pamela Dominutti, Manon Rocco, Camille Mouchel-Vallon, Samira El Gdachi, Maxence Brissy, Maroua Fathalli, Nicolas Maury, Bert Verreyken, Crist Amelynck, Niels Schoon, Valérie Gros, Jean-Marc Pichon, Mickael Ribeiro, Eric Pique, Emmanuel Leclerc, Thierry Bourrianne, Axel Roy, Eric Moulin, Joël Barrie, Jean-Marc Metzger, Guillaume Péris, Christian Guadagno, Chatrapatty Bhugwant, Jean-Mathieu Tibere, Arnaud Tournigand, Evelyn Freney, Karine Sellegri, Anne-Marie Delort, Pierre Amato, Muriel Joly, Jean-Luc Baray, Pascal Renard, Angelica Bianco, Anne Réchou, and Guillaume Payen
Atmos. Chem. Phys., 24, 4129–4155, https://doi.org/10.5194/acp-24-4129-2024, https://doi.org/10.5194/acp-24-4129-2024, 2024
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Aerosol particles in the atmosphere play a key role in climate change and air pollution. A large number of aerosol particles are formed from the oxidation of volatile organic compounds (VOCs and secondary organic aerosols – SOA). An important field campaign was organized on Réunion in March–April 2019 to understand the formation of SOA in a tropical atmosphere mostly influenced by VOCs emitted by forest and in the presence of clouds. This work synthesizes the results of this campaign.
Kelvin H. Bates, Mathew J. Evans, Barron H. Henderson, and Daniel J. Jacob
Geosci. Model Dev., 17, 1511–1524, https://doi.org/10.5194/gmd-17-1511-2024, https://doi.org/10.5194/gmd-17-1511-2024, 2024
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Accurate representation of rates and products of chemical reactions in atmospheric models is crucial for simulating concentrations of pollutants and climate forcers. We update the widely used GEOS-Chem atmospheric chemistry model with reaction parameters from recent compilations of experimental data and demonstrate the implications for key atmospheric chemical species. The updates decrease tropospheric CO mixing ratios and increase stratospheric nitrogen oxide mixing ratios, among other changes.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Maxime Perini, Laurent Terray, Daniel Cariolle, Saloua Peatier, and Marie-Pierre Moine
EGUsphere, https://doi.org/10.5194/egusphere-2023-2478, https://doi.org/10.5194/egusphere-2023-2478, 2023
Preprint archived
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Uncertainty about aviation radiative forcing is essentially due to uncertainties about non-CO2 forcing, especially for condensation trails (contrails). This study uses a new parameterization for ice-supersaturation and additional contrail coverage in the CNRM-CM6-1 atmospheric component to estimate contrail radiative forcing for the year 2000. The range of contrail radiative forcing due to parametric uncertainty is analyzed. Our contrail radiative forcing best estimate is 56 (38−70) mW.m-2.
Maria Tsivlidou, Bastien Sauvage, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Eric Le Flochmoën, Philippe Nédélec, Valérie Thouret, Pawel Wolff, and Brice Barret
Atmos. Chem. Phys., 23, 14039–14063, https://doi.org/10.5194/acp-23-14039-2023, https://doi.org/10.5194/acp-23-14039-2023, 2023
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The tropics are a region where the ozone increase has been most apparent since 1980 and where observations are sparse. Using aircraft, satellite, and model data, we document the characteristics of tropospheric ozone and CO over the whole tropics for the last 2 decades. We explore the origin of the observed CO anomalies and investigate transport processes driving the tropical CO and O3 distribution. Our study highlights the importance of anthropogenic emissions, mostly over the northern tropics.
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.
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.
Haolin Wang, Xiao Lu, Daniel J. Jacob, Owen R. Cooper, Kai-Lan Chang, Ke Li, Meng Gao, Yiming Liu, Bosi Sheng, Kai Wu, Tongwen Wu, Jie Zhang, Bastien Sauvage, Philippe Nédélec, Romain Blot, and Shaojia Fan
Atmos. Chem. Phys., 22, 13753–13782, https://doi.org/10.5194/acp-22-13753-2022, https://doi.org/10.5194/acp-22-13753-2022, 2022
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We report significant global tropospheric ozone increases in 1995–2017 based on extensive aircraft and ozonesonde observations. Using GEOS-Chem (Goddard Earth Observing System chemistry model) multi-decadal global simulations, we find that changes in global anthropogenic emissions, in particular the rapid increases in aircraft emissions, contribute significantly to the increases in tropospheric ozone and resulting radiative impact.
Graciela B. Raga, Darrel Baumgardner, Blanca Rios, Yanet Díaz-Esteban, Alejandro Jaramillo, Martin Gallagher, Bastien Sauvage, Pawel Wolff, and Gary Lloyd
Atmos. Chem. Phys., 22, 2269–2292, https://doi.org/10.5194/acp-22-2269-2022, https://doi.org/10.5194/acp-22-2269-2022, 2022
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The In-Service Aircraft for a Global Observing System (IAGOS) is a small fleet of commercial aircraft that carry a suite of meteorological, gas, aerosol, and cloud sensors and have been measuring worldwide for almost 9 years, since late 2011. Extreme ice events (EIEs) have been identified from the IAGOS cloud measurements and linked to surface emissions for biomass and fossil fuel consumption. The results reported here are highly relevant for climate change and flight operations forecasting.
Pamela A. Dominutti, Pascal Renard, Mickaël Vaïtilingom, Angelica Bianco, Jean-Luc Baray, Agnès Borbon, Thierry Bourianne, Frédéric Burnet, Aurélie Colomb, Anne-Marie Delort, Valentin Duflot, Stephan Houdier, Jean-Luc Jaffrezo, Muriel Joly, Martin Leremboure, Jean-Marc Metzger, Jean-Marc Pichon, Mickaël Ribeiro, Manon Rocco, Pierre Tulet, Anthony Vella, Maud Leriche, and Laurent Deguillaume
Atmos. Chem. Phys., 22, 505–533, https://doi.org/10.5194/acp-22-505-2022, https://doi.org/10.5194/acp-22-505-2022, 2022
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We present here the results obtained during an intensive field campaign conducted in March to April 2019 in Reunion. Our study integrates a comprehensive chemical and microphysical characterization of cloud water. Our investigations reveal that air mass history and cloud microphysical properties do not fully explain the variability observed in their chemical composition. This highlights the complexity of emission sources, multiphasic exchanges, and transformations in clouds.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Hannah Clark, Yasmine Bennouna, Maria Tsivlidou, Pawel Wolff, Bastien Sauvage, Brice Barret, Eric Le Flochmoën, Romain Blot, Damien Boulanger, Jean-Marc Cousin, Philippe Nédélec, Andreas Petzold, and Valérie Thouret
Atmos. Chem. Phys., 21, 16237–16256, https://doi.org/10.5194/acp-21-16237-2021, https://doi.org/10.5194/acp-21-16237-2021, 2021
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We examined 27 years of IAGOS (In-service Aircraft for a Global Observing System) profiles at Frankfurt to see if there were unusual features during the spring of 2020 related to COVID-19 lockdowns in Europe. Increased ozone near the surface was partly linked to the reduction in emissions. Carbon monoxide decreased near the surface, but the impact of the lockdowns was offset by polluted air masses from elsewhere. There were small reductions in ozone and carbon monoxide in the free troposphere.
Victor Lannuque, Bastien Sauvage, Brice Barret, Hannah Clark, Gilles Athier, Damien Boulanger, Jean-Pierre Cammas, Jean-Marc Cousin, Alain Fontaine, Eric Le Flochmoën, Philippe Nédélec, Hervé Petetin, Isabelle Pfaffenzeller, Susanne Rohs, Herman G. J. Smit, Pawel Wolff, and Valérie Thouret
Atmos. Chem. Phys., 21, 14535–14555, https://doi.org/10.5194/acp-21-14535-2021, https://doi.org/10.5194/acp-21-14535-2021, 2021
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The African intertropical troposphere is one of the world areas where the increase in ozone mixing ratio has been most pronounced since 1980 and where high carbon monoxide mixing ratios are found in altitude. In this article, IAGOS aircraft measurements, IASI satellite instrument observations, and SOFT-IO model products are used to explore the seasonal distribution variations and the origin of ozone and carbon monoxide over the African upper troposphere.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Romain Blot, Philippe Nedelec, Damien Boulanger, Pawel Wolff, Bastien Sauvage, Jean-Marc Cousin, Gilles Athier, Andreas Zahn, Florian Obersteiner, Dieter Scharffe, Hervé Petetin, Yasmine Bennouna, Hannah Clark, and Valérie Thouret
Atmos. Meas. Tech., 14, 3935–3951, https://doi.org/10.5194/amt-14-3935-2021, https://doi.org/10.5194/amt-14-3935-2021, 2021
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A lack of information about temporal changes in measurement uncertainties is an area of concern for long-term trend studies of the key compounds which have a direct or indirect impact on climate change. The IAGOS program has measured O3 and CO within the troposphere and lower stratosphere for more than 25 years. In this study, we demonstrated that the IAGOS database can be treated as one continuous program and is therefore appropriate for studies of long-term trends.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Keun-Ok Lee, Brice Barret, Eric L. Flochmoën, Pierre Tulet, Silvia Bucci, Marc von Hobe, Corinna Kloss, Bernard Legras, Maud Leriche, Bastien Sauvage, Fabrizio Ravegnani, and Alexey Ulanovsky
Atmos. Chem. Phys., 21, 3255–3274, https://doi.org/10.5194/acp-21-3255-2021, https://doi.org/10.5194/acp-21-3255-2021, 2021
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This paper focuses on the emission sources and pathways of pollution from the boundary layer to the Asian monsoon anticyclone (AMA) during the StratoClim aircraft campaign period. Simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of AMA and on the formation of the Asian tropopause aerosol layer during the StratoClim campaign.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Setigui Aboubacar Keita, Eric Girard, Jean-Christophe Raut, Maud Leriche, Jean-Pierre Blanchet, Jacques Pelon, Tatsuo Onishi, and Ana Cirisan
Geosci. Model Dev., 13, 5737–5755, https://doi.org/10.5194/gmd-13-5737-2020, https://doi.org/10.5194/gmd-13-5737-2020, 2020
Martin Cussac, Virginie Marécal, Valérie Thouret, Béatrice Josse, and Bastien Sauvage
Atmos. Chem. Phys., 20, 9393–9417, https://doi.org/10.5194/acp-20-9393-2020, https://doi.org/10.5194/acp-20-9393-2020, 2020
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Biomass burning emissions are a major source of carbon monoxide in the atmosphere. Here, the vertical transport that these emissions can undergo until the upper troposphere is investigated, as well as their contribution to carbon monoxide concentrations. It was found that boreal forest emissions were specific to the occurrence of pyroconvection directly above the fires, whereas biomass burning emissions from other regions of the globe relied more on the occurrence of deep convection.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Frank Roux, Hannah Clark, Kuo-Ying Wang, Susanne Rohs, Bastien Sauvage, and Philippe Nédélec
Atmos. Chem. Phys., 20, 3945–3963, https://doi.org/10.5194/acp-20-3945-2020, https://doi.org/10.5194/acp-20-3945-2020, 2020
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Ozone, carbon monoxide and relative humidity were measured by two China Airlines aircraft equipped with IAGOS instruments during the summer of 2016. We examined landing and take-off profiles near Taipei (Taiwan), in the vicinity of three typhoons, in relation to ERA-5 meteorological reanalyses. Upstream of the storms, these data suggest that air is transported downwards from the stratosphere. Downstream, the troposphere is cleaner and moister due to the uplift of marine boundary layer air.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Philipp Reutter, Patrick Neis, Susanne Rohs, and Bastien Sauvage
Atmos. Chem. Phys., 20, 787–804, https://doi.org/10.5194/acp-20-787-2020, https://doi.org/10.5194/acp-20-787-2020, 2020
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This study compares in situ measurements of temperature and humidity in the upper troposphere and lower stratosphere with reanalysis data from the ECMWF ERA-Interim data set. It is shown that temperature compares well between both data sets. However, extreme values of relative humidity with respect to ice (RHi) are missing in ERA-Interim, and hence the number and size of ice supersaturated regions differ strongly between both data sets.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Émilie Poirier, Julie M. Thériault, and Maud Leriche
Hydrol. Earth Syst. Sci., 23, 4097–4111, https://doi.org/10.5194/hess-23-4097-2019, https://doi.org/10.5194/hess-23-4097-2019, 2019
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The impact of phase changes aloft on the precipitation distribution in the Kananaskis Valley, Alberta, was studied. The model reproduces well the atmospheric conditions and precipitation pattern. In this region, sublimation has a greater impact on the evolution of the precipitation than melting. The trajectories of hydrometeors explain the precipitation distribution in the valley, which can impact snowpacks. The amount of snow at the surface also depends on the strength of the downslope flow.
Tomás Sherwen, Rosie J. Chance, Liselotte Tinel, Daniel Ellis, Mat J. Evans, and Lucy J. Carpenter
Earth Syst. Sci. Data, 11, 1239–1262, https://doi.org/10.5194/essd-11-1239-2019, https://doi.org/10.5194/essd-11-1239-2019, 2019
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Iodine plays an important role in the Earth system, as a nutrient to the biosphere and by changing the concentrations of climate and air-quality species. However, there are uncertainties on the magnitude of iodine’s role, and a key uncertainty is our understanding of iodide in the global sea-surface. Here we take a data-driven approach using a machine learning algorithm to convert a sparse set of sea-surface iodide observations into a spatially and temporally resolved dataset for use in models.
Franck Auguste, Géraldine Réa, Roberto Paoli, Christine Lac, Valery Masson, and Daniel Cariolle
Geosci. Model Dev., 12, 2607–2633, https://doi.org/10.5194/gmd-12-2607-2019, https://doi.org/10.5194/gmd-12-2607-2019, 2019
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The numerical implementation of an immersed boundary method in the atmospheric solver Meso-NH is presented. This technique models fluid–solid interaction and allows for the simulation of urban flows by considering buildings to be part of the resolved scales. This study constitutes a first robust step towards a better understanding of the interactions between weather and cities and better predictions of such interactions.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Kate R. Smith, Peter M. Edwards, Peter D. Ivatt, James D. Lee, Freya Squires, Chengliang Dai, Richard E. Peltier, Mat J. Evans, Yele Sun, and Alastair C. Lewis
Atmos. Meas. Tech., 12, 1325–1336, https://doi.org/10.5194/amt-12-1325-2019, https://doi.org/10.5194/amt-12-1325-2019, 2019
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Clusters of low-cost, low-power atmospheric gas sensors were built into a sensor instrument to monitor NO2 and O3 in Beijing, alongside reference instruments, aiming to improve the reliability of sensor measurements. Clustering identical sensors and using the median sensor signal was used to minimize drift over short and medium timescales. Three different machine learning techniques were used for all the sensor data in an attempt to correct for cross-interferences, which worked to some degree.
Federica Pacifico, Claire Delon, Corinne Jambert, Pierre Durand, Eleanor Morris, Mat J. Evans, Fabienne Lohou, Solène Derrien, Venance H. E. Donnou, Arnaud V. Houeto, Irene Reinares Martínez, and Pierre-Etienne Brilouet
Atmos. Chem. Phys., 19, 2299–2325, https://doi.org/10.5194/acp-19-2299-2019, https://doi.org/10.5194/acp-19-2299-2019, 2019
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Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in
June and July 2016.
Hervé Petetin, Bastien Sauvage, Mark Parrington, Hannah Clark, Alain Fontaine, Gilles Athier, Romain Blot, Damien Boulanger, Jean-Marc Cousin, Philippe Nédélec, and Valérie Thouret
Atmos. Chem. Phys., 18, 17277–17306, https://doi.org/10.5194/acp-18-17277-2018, https://doi.org/10.5194/acp-18-17277-2018, 2018
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This study derives a climatology of the impact of biomass burning versus anthropogenic emissions on the strongest CO plumes observed in the troposphere based on a dataset of about 30 000 in situ vertical profiles, combined with Lagrangian simulations coupled to CO emission. Results demonstrate the large contribution of biomass burning to the strongest CO plumes encountered in the troposphere in many locations of the world.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Hervé Petetin, Bastien Sauvage, Herman G. J. Smit, François Gheusi, Fabienne Lohou, Romain Blot, Hannah Clark, Gilles Athier, Damien Boulanger, Jean-Marc Cousin, Philippe Nedelec, Patrick Neis, Susanne Rohs, and Valérie Thouret
Atmos. Chem. Phys., 18, 9561–9581, https://doi.org/10.5194/acp-18-9561-2018, https://doi.org/10.5194/acp-18-9561-2018, 2018
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Based on the numerous profiles available since 1994, this paper investigates the vertical stratification of ozone, carbon monoxide and relative humidity in the lower part of the troposphere (planetary boundary layer, lower free troposphere). Such a characterization of the vertical distribution of pollution is notably important for better understanding vertical exchanges and evaluating models on the vertical dimension.
Christine Lac, Jean-Pierre Chaboureau, Valéry Masson, Jean-Pierre Pinty, Pierre Tulet, Juan Escobar, Maud Leriche, Christelle Barthe, Benjamin Aouizerats, Clotilde Augros, Pierre Aumond, Franck Auguste, Peter Bechtold, Sarah Berthet, Soline Bielli, Frédéric Bosseur, Olivier Caumont, Jean-Martial Cohard, Jeanne Colin, Fleur Couvreux, Joan Cuxart, Gaëlle Delautier, Thibaut Dauhut, Véronique Ducrocq, Jean-Baptiste Filippi, Didier Gazen, Olivier Geoffroy, François Gheusi, Rachel Honnert, Jean-Philippe Lafore, Cindy Lebeaupin Brossier, Quentin Libois, Thibaut Lunet, Céline Mari, Tomislav Maric, Patrick Mascart, Maxime Mogé, Gilles Molinié, Olivier Nuissier, Florian Pantillon, Philippe Peyrillé, Julien Pergaud, Emilie Perraud, Joris Pianezze, Jean-Luc Redelsperger, Didier Ricard, Evelyne Richard, Sébastien Riette, Quentin Rodier, Robert Schoetter, Léo Seyfried, Joël Stein, Karsten Suhre, Marie Taufour, Odile Thouron, Sandra Turner, Antoine Verrelle, Benoît Vié, Florian Visentin, Vincent Vionnet, and Philippe Wautelet
Geosci. Model Dev., 11, 1929–1969, https://doi.org/10.5194/gmd-11-1929-2018, https://doi.org/10.5194/gmd-11-1929-2018, 2018
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This paper presents the Meso-NH model version 5.4, which is an atmospheric non-hydrostatic research model that is applied on synoptic to turbulent scales. The model includes advanced numerical techniques and state-of-the-art physics parameterization schemes. It has been expanded to provide capabilities for a range of Earth system prediction applications such as chemistry and aerosols, electricity and lightning, hydrology, wildland fires, volcanic eruptions, and cyclones with ocean coupling.
Fabien Brosse, Maud Leriche, Céline Mari, and Fleur Couvreux
Atmos. Chem. Phys., 18, 6601–6624, https://doi.org/10.5194/acp-18-6601-2018, https://doi.org/10.5194/acp-18-6601-2018, 2018
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The cleansing capacity of the atmosphere is studied through the hydroxyl radical (OH) chemical reactivity in numerical simulations of natural and urban environments. Turbulence-driven segregation of chemical compounds in the atmospheric boundary layer is explored and may partially explain discrepancies between observed and modeled OH reactivity in both environments.
Mike J. Newland, Andrew R. Rickard, Tomás Sherwen, Mathew J. Evans, Luc Vereecken, Amalia Muñoz, Milagros Ródenas, and William J. Bloss
Atmos. Chem. Phys., 18, 6095–6120, https://doi.org/10.5194/acp-18-6095-2018, https://doi.org/10.5194/acp-18-6095-2018, 2018
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Stabilised Criegee intermediates (SCIs) are formed in the reaction of alkenes with ozone, both of which are ubiquitous throughout the troposphere. We determine the fate and global distribution of SCI from monoterpene ozonolysis. One major fate of SCI is reaction with H2O, but for a fraction of SCIs, unimolecular reactions dominate. Concentrations of SCIs are high enough regionally to play a key role in the conversion of sulfur dioxide to aerosol, affecting air quality and climate.
Yann Cohen, Hervé Petetin, Valérie Thouret, Virginie Marécal, Béatrice Josse, Hannah Clark, Bastien Sauvage, Alain Fontaine, Gilles Athier, Romain Blot, Damien Boulanger, Jean-Marc Cousin, and Philippe Nédélec
Atmos. Chem. Phys., 18, 5415–5453, https://doi.org/10.5194/acp-18-5415-2018, https://doi.org/10.5194/acp-18-5415-2018, 2018
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Measurements of ozone and carbon monoxide were performed during 1994–2013 around the tropopause on board commercial aircraft. Seasonal cycles and trends were calculated above eight well-sampled regions in Northern Hemisphere midlatitudes. CO shows decreasing concentrations over the last 10 years, thus reflecting the impact of the legislation on anthropogenic emissions. Ozone amounts increased over the 20 years in the upper troposphere during different seasons, depending on the longitudes.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Clémence Rose, Nadine Chaumerliac, Laurent Deguillaume, Hélène Perroux, Camille Mouchel-Vallon, Maud Leriche, Luc Patryl, and Patrick Armand
Atmos. Chem. Phys., 18, 2225–2242, https://doi.org/10.5194/acp-18-2225-2018, https://doi.org/10.5194/acp-18-2225-2018, 2018
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A detailed aqueous phase mechanism CLEPS 1.1 is coupled with warm microphysics including activation of aerosol particles into cloud droplets. Simulated aqueous concentrations of carboxylic acids are close to the long-term measurements conducted at Puy de Dôme (France). Sensitivity tests show that formic and acetic acids mainly originate from the gas phase with highly variable aqueous-phase reactivity depending on cloud pH, while C3–C4 carboxylic acids mainly originate from the particulate phase.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Bastien Sauvage, Alain Fontaine, Sabine Eckhardt, Antoine Auby, Damien Boulanger, Hervé Petetin, Ronan Paugam, Gilles Athier, Jean-Marc Cousin, Sabine Darras, Philippe Nédélec, Andreas Stohl, Solène Turquety, Jean-Pierre Cammas, and Valérie Thouret
Atmos. Chem. Phys., 17, 15271–15292, https://doi.org/10.5194/acp-17-15271-2017, https://doi.org/10.5194/acp-17-15271-2017, 2017
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We provide the scientific community with a SOFT-IO tool based on the coupling of Lagrangian modeling with emission inventories and aircraft CO measurements, which is able to calculate the contribution of the sources and geographical origins of CO measurements, with good performances. Calculated CO added-value products will help scientists in interpreting large IAGOS CO data set. SOFT-IO could further be applied to other CO data sets or used to help validate emission inventories.
Ben Newsome and Mat Evans
Atmos. Chem. Phys., 17, 14333–14352, https://doi.org/10.5194/acp-17-14333-2017, https://doi.org/10.5194/acp-17-14333-2017, 2017
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We explore the uncertainty in the predictions of a chemical transport model (GEOS-Chem) from uncertainty in 60 inorganic rate constants and photolysis rates. We find uncertainty in the global mean ozone burden of 10 %, in global mean OH of 16 %, methane lifetimes of 16 %, and tropospheric ozone radiative forcings of 13 %. Reductions in the uncertainty of rate constants of these simple reactions would reduce uncertainty in our understanding of atmospheric composition.
Peter M. Edwards and Mathew J. Evans
Atmos. Chem. Phys., 17, 13669–13680, https://doi.org/10.5194/acp-17-13669-2017, https://doi.org/10.5194/acp-17-13669-2017, 2017
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Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
Peter Knippertz, Andreas H. Fink, Adrien Deroubaix, Eleanor Morris, Flore Tocquer, Mat J. Evans, Cyrille Flamant, Marco Gaetani, Christophe Lavaysse, Celine Mari, John H. Marsham, Rémi Meynadier, Abalo Affo-Dogo, Titike Bahaga, Fabien Brosse, Konrad Deetz, Ridha Guebsi, Issaou Latifou, Marlon Maranan, Philip D. Rosenberg, and Andreas Schlueter
Atmos. Chem. Phys., 17, 10893–10918, https://doi.org/10.5194/acp-17-10893-2017, https://doi.org/10.5194/acp-17-10893-2017, 2017
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In June–July 2016 DACCIWA (Dynamics–Aerosol–Chemistry–Cloud Interactions in West Africa), a large, EU-funded European–African project, organised an international field campaign in densely populated southern West Africa, including measurements from ground sites, research aircraft, weather balloons and urban sites. This paper gives an overview of the atmospheric evolution during this period focusing on meteorological (precipitation, cloudiness, winds) and composition (gases, particles) aspects.
Marine Claeys, Greg Roberts, Marc Mallet, Jovanna Arndt, Karine Sellegri, Jean Sciare, John Wenger, and Bastien Sauvage
Atmos. Chem. Phys., 17, 7891–7915, https://doi.org/10.5194/acp-17-7891-2017, https://doi.org/10.5194/acp-17-7891-2017, 2017
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Over a period of 5 days (summer 2013), the mass concentration of primary marine aerosols was dominant compared to other aerosols measured at a ground-based measuring site on Corsica. The characteristics of primary marine aerosols such as their size distribution, their optical properties and their direct radiative effect were studied as a function of their ageing and region of emission. These characteristics were compared to two other periods dominated by different aerosol regimes.
Daniel Cariolle, Philippe Moinat, Hubert Teyssèdre, Luc Giraud, Béatrice Josse, and Franck Lefèvre
Geosci. Model Dev., 10, 1467–1485, https://doi.org/10.5194/gmd-10-1467-2017, https://doi.org/10.5194/gmd-10-1467-2017, 2017
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This article reports on the development and tests of the adaptive semi-implicit scheme (ASIS) solver for the simulation of atmospheric chemistry. To solve the ordinary differential equations associated with the time evolution of the species concentrations, ASIS adopts a one-step linearized implicit scheme. It conserves mass and has a time-stepping module to control the accuracy of the numerical solution. ASIS was found competitive in terms of computation cost against higher-order schemes.
Camille Mouchel-Vallon, Laurent Deguillaume, Anne Monod, Hélène Perroux, Clémence Rose, Giovanni Ghigo, Yoann Long, Maud Leriche, Bernard Aumont, Luc Patryl, Patrick Armand, and Nadine Chaumerliac
Geosci. Model Dev., 10, 1339–1362, https://doi.org/10.5194/gmd-10-1339-2017, https://doi.org/10.5194/gmd-10-1339-2017, 2017
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The Cloud Explicit Physico-chemical Scheme (CLEPS 1.0) describes oxidation of water-soluble organic compounds resulting from isoprene oxidation. It is based on structure activity relationships (SARs) (global rate constants and branching ratios for HO• abstraction and addition) and GROMHE SAR (Henry's law constants for undocumented species). It is coupled to the MCM gas phase mechanism and is included in a model using the DSMACC model and KPP to analyze experimental and field data.
Chris Reed, Mathew J. Evans, Leigh R. Crilley, William J. Bloss, Tomás Sherwen, Katie A. Read, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 17, 4081–4092, https://doi.org/10.5194/acp-17-4081-2017, https://doi.org/10.5194/acp-17-4081-2017, 2017
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The source of ozone-depleting compounds in the remote troposphere has been thought to be long-range transport of secondary pollutants such as organic nitrates. Processing of organic nitrates to nitric acid and subsequent deposition on surfaces in the atmosphere was thought to remove these nitrates from the ozone–NOx–HOx cycle. We found through observation of NOx in the remote tropical troposphere at the Cape Verde Observatory that surface nitrates can be released back into the atmosphere.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Hervé Petetin, Valérie Thouret, Alain Fontaine, Bastien Sauvage, Giles Athier, Romain Blot, Damien Boulanger, Jean-Marc Cousin, and Philippe Nédélec
Atmos. Chem. Phys., 16, 15147–15163, https://doi.org/10.5194/acp-16-15147-2016, https://doi.org/10.5194/acp-16-15147-2016, 2016
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Ozone (O3) and carbon monoxide (CO) are two compounds of major importance in the atmosphere. In this paper we investigated their variability and trends at Frankfurt based on the MOZAIC–IAGOS dataset, a unique dataset of about 21 300 vertical profiles recorded by commercial aircraft. The CO concentrations have been decreasing since 2002, while no strong tendency is observed for O3 since 1994. However, the O3 seasonal variations are changing, with the spring maximum occurring earlier and earlier.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Mohammed K. Osman, David W. Tarasick, Jane Liu, Omid Moeini, Valerie Thouret, Vitali E. Fioletov, Mark Parrington, and Philippe Nédélec
Atmos. Chem. Phys., 16, 10263–10282, https://doi.org/10.5194/acp-16-10263-2016, https://doi.org/10.5194/acp-16-10263-2016, 2016
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A new 3-D gridded climatology of CO has been developed by trajectory mapping of global MOZAIC-IAGOS in situ aircraft measurements. The dataset is archived monthly from 2001–2012 on a grid of 5 × 5deg × 1 km altitude. The dataset facilitates comparison of different years and seasons and offers insight into the global variation and trends of CO. Major CO sources are clearly visible. The dataset can be used as an a priori data for satellite retrieval and for air quality model validation and initialization.
Brice Barret, Bastien Sauvage, Yasmine Bennouna, and Eric Le Flochmoen
Atmos. Chem. Phys., 16, 9129–9147, https://doi.org/10.5194/acp-16-9129-2016, https://doi.org/10.5194/acp-16-9129-2016, 2016
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During the Asian Monsoon, pollutants are uplifted to the upper troposphere where they are trapped within the large scale Asian monsoon anticyclone. Among these pollutants are O3 precursors such as nitrogen oxides (NOx) and carbon monoxide (CO). Based on satellite observations and model simulations, we have estimated the impact of anthropogenic and natural sources on O3 in the monsoon anticyclone. Our results show that Asian pollution and LiNOx have comparable contributions.
Dene R. Bowdalo, Mathew J. Evans, and Eric D. Sofen
Atmos. Chem. Phys., 16, 8295–8308, https://doi.org/10.5194/acp-16-8295-2016, https://doi.org/10.5194/acp-16-8295-2016, 2016
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We introduce a new methodology for the assessment of atmospheric models with observations. We apply a spectral analysis methodology to hourly ozone observations and the equivalent model output. The spectrally transformed observational data show significant peaks on daily and annual timescales. Comparison between the amplitude and phase of these peaks introduces a new comparison methodology between model and measurements. We find the model shows significant biases on an annual timescale.
Xuewu Fu, Nicolas Marusczak, Lars-Eric Heimbürger, Bastien Sauvage, François Gheusi, Eric M. Prestbo, and Jeroen E. Sonke
Atmos. Chem. Phys., 16, 5623–5639, https://doi.org/10.5194/acp-16-5623-2016, https://doi.org/10.5194/acp-16-5623-2016, 2016
Chris Reed, Mathew J. Evans, Piero Di Carlo, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 16, 4707–4724, https://doi.org/10.5194/acp-16-4707-2016, https://doi.org/10.5194/acp-16-4707-2016, 2016
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The self-cleaning capacity of the atmosphere in places like Antarctica can be measured by quantifying very low amounts of combustion products that exist in a well-known ratio. When this ratio deviates from 1 it points to the existence of unknown compounds. Several unknown compounds have been theorized to exist but never measured. We have found the method for measuring the ratio of combustion products suffers a bias in remote places, which when taken into account disproves any unknown compounds.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
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We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
B. Vié, J.-P. Pinty, S. Berthet, and M. Leriche
Geosci. Model Dev., 9, 567–586, https://doi.org/10.5194/gmd-9-567-2016, https://doi.org/10.5194/gmd-9-567-2016, 2016
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LIMA, a new quasi two-moment, mixed-phase microphysical scheme, is introduced. LIMA relies on the prognostic evolution of a multimodal aerosol population and the careful description of their nucleating properties that enable cloud droplets and pristine ice to form. This paper describes LIMA and illustrates its ability to represent aerosol-cloud interactions for 2-D idealized simulations of a squall line and orographic cold clouds.
E. D. Sofen, D. Bowdalo, and M. J. Evans
Atmos. Chem. Phys., 16, 1445–1457, https://doi.org/10.5194/acp-16-1445-2016, https://doi.org/10.5194/acp-16-1445-2016, 2016
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We explore the global representativeness of a global surface ozone data set from a range of perspectives (area, biomes, chemical regimes, model uncertainty, model trends). We conclude that the current network fails to provide sufficient constraints for important regions/regimes, leading to uncertainty for a range of atmospheric composition challenges. We suggest 20 new locations for making surface ozone observations, which would significantly enhance our observational capability.
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
E. D. Sofen, M. J. Evans, and A. C. Lewis
Atmos. Chem. Phys., 15, 13627–13632, https://doi.org/10.5194/acp-15-13627-2015, https://doi.org/10.5194/acp-15-13627-2015, 2015
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As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
Atmos. Chem. Phys., 15, 9983–9996, https://doi.org/10.5194/acp-15-9983-2015, https://doi.org/10.5194/acp-15-9983-2015, 2015
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Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
P. S. Monks, A. T. Archibald, A. Colette, O. Cooper, M. Coyle, R. Derwent, D. Fowler, C. Granier, K. S. Law, G. E. Mills, D. S. Stevenson, O. Tarasova, V. Thouret, E. von Schneidemesser, R. Sommariva, O. Wild, and M. L. Williams
Atmos. Chem. Phys., 15, 8889–8973, https://doi.org/10.5194/acp-15-8889-2015, https://doi.org/10.5194/acp-15-8889-2015, 2015
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Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, and yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
S. G. Sivia, F. Gheusi, C. Mari, and A. Di Muro
Geosci. Model Dev., 8, 1427–1443, https://doi.org/10.5194/gmd-8-1427-2015, https://doi.org/10.5194/gmd-8-1427-2015, 2015
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A sub-grid shallow convection scheme is adapted such that the size and intensity of the ground heat source provided by an eruption is initialised for modelling the sub-grid updraft. This parameterisation is tested on a 1-D single column model with a 1km resolution for an eruption observed at PdF in January 2010. The modelled plume agrees well with the SO2 concentrations found with LES and the adapted scheme emphasizes the sensitivity of the parameterisation to entrainment at the plume base.
A. Inness, A.-M. Blechschmidt, I. Bouarar, S. Chabrillat, M. Crepulja, R. J. Engelen, H. Eskes, J. Flemming, A. Gaudel, F. Hendrick, V. Huijnen, L. Jones, J. Kapsomenakis, E. Katragkou, A. Keppens, B. Langerock, M. de Mazière, D. Melas, M. Parrington, V. H. Peuch, M. Razinger, A. Richter, M. G. Schultz, M. Suttie, V. Thouret, M. Vrekoussis, A. Wagner, and C. Zerefos
Atmos. Chem. Phys., 15, 5275–5303, https://doi.org/10.5194/acp-15-5275-2015, https://doi.org/10.5194/acp-15-5275-2015, 2015
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The paper presents results from data assimilation studies with the new Composition-IFS model developed in the MACC project. This system was used in MACC to produce daily analyses and 5-day forecasts of atmospheric composition and is now run daily in the EU’s Copernicus Atmosphere Monitoring Service. The paper looks at the quality of the CO, O3 and NO2 analysis fields obtained with this system, comparing them against observations, a control run and an older version of the model.
J. Huang, H. Liu, J. H. Crawford, C. Chan, D. B. Considine, Y. Zhang, X. Zheng, C. Zhao, V. Thouret, S. J. Oltmans, S. C. Liu, D. B. A. Jones, S. D. Steenrod, and M. R. Damon
Atmos. Chem. Phys., 15, 5161–5179, https://doi.org/10.5194/acp-15-5161-2015, https://doi.org/10.5194/acp-15-5161-2015, 2015
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High ozone concentrations (up to 94.7ppbv) were frequently observed at an altitude of ~1.5--2km over Beijing during April--May 2005. Ozone due to Asian anthropogenic pollution made major contributions to the observed ozone enhancements. These enhancements typically occurred under southerly wind and warmer conditions. An earlier onset of the Asian summer monsoon would cause more ozone enhancement events in the lower troposphere over the North China Plain in late spring and early summer.
C. Barbet, L. Deguillaume, N. Chaumerliac, M. Leriche, A. Berger, E. Freney, A. Colomb, K. Sellegri, L. Patryl, and P. Armand
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-13395-2015, https://doi.org/10.5194/acpd-15-13395-2015, 2015
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J.-F. Léon, P. Augustin, M. Mallet, T. Bourrianne, V. Pont, F. Dulac, M. Fourmentin, D. Lambert, and B. Sauvage
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-9507-2015, https://doi.org/10.5194/acpd-15-9507-2015, 2015
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This paper presents the aerosol vertical distribution observed by lidar soundings in Corsica (western Mediterranean) between February 2012 and August 2013. A seasonal cycle is observed in the extinction coefficient profiles and aerosol optical thickness with minima in winter and maxima in spring-summer. Less than 10% of the daily observations show high AOD corresponding to the large-scale advection of desert dust from Northern Africa or pollution aerosols from Europe.
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
R. Paoli, O. Thouron, J. Escobar, J. Picot, and D. Cariolle
Atmos. Chem. Phys., 14, 5037–5055, https://doi.org/10.5194/acp-14-5037-2014, https://doi.org/10.5194/acp-14-5037-2014, 2014
V. Leroy-Cancellieri, P. Augustin, J. B. Filippi, C. Mari, M. Fourmentin, F. Bosseur, F. Morandini, and H. Delbarre
Nat. Hazards Earth Syst. Sci., 14, 509–523, https://doi.org/10.5194/nhess-14-509-2014, https://doi.org/10.5194/nhess-14-509-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
M. Leriche, J.-P. Pinty, C. Mari, and D. Gazen
Geosci. Model Dev., 6, 1275–1298, https://doi.org/10.5194/gmd-6-1275-2013, https://doi.org/10.5194/gmd-6-1275-2013, 2013
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
S. Strada, S. R. Freitas, C. Mari, K. M. Longo, and R. Paugam
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmdd-6-721-2013, https://doi.org/10.5194/gmdd-6-721-2013, 2013
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A. C. Lewis, M. J. Evans, J. R. Hopkins, S. Punjabi, K. A. Read, R. M. Purvis, S. J. Andrews, S. J. Moller, L. J. Carpenter, J. D. Lee, A. R. Rickard, P. I. Palmer, and M. Parrington
Atmos. Chem. Phys., 13, 851–867, https://doi.org/10.5194/acp-13-851-2013, https://doi.org/10.5194/acp-13-851-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Influence of nitrogen oxides and volatile organic compounds emission changes on tropospheric ozone variability, trends and radiative effect
Tropospheric ozone trends and attributions over East and Southeast Asia in 1995–2019: an integrated assessment using statistical methods, machine learning models, and multiple chemical transport models
Characterization of reactive oxidized nitrogen in the global upper troposphere using recent and historic commercial and research aircraft campaigns and GEOS-Chem
Soil deposition of atmospheric hydrogen constrained using planetary-scale observations
Comparative ozone production sensitivity to NOx and VOCs in Quito, Ecuador, and Santiago, Chile
South Asia anthropogenic ammonia emission inversion through assimilating IASI observations
A new parameterization of photolysis rates for oxygenated volatile organic compounds (OVOCs)
Constraining the budget of NOx and volatile organic compounds at a remote tropical island using multi-platform observations and WRF-Chem model simulations
Multi-observational estimation of regional and sectoral emission contributions to the persistent high growth rate of atmospheric CH4 for 2020–2022
Representing improved tropospheric ozone distribution over the Northern Hemisphere by including lightning NOx emissions in CHIMERE
Assessing the ability to quantify the decrease in NOx anthropogenic emissions in 2019 compared to 2005 using OMI and TROPOMI satellite observations
Tracking daily NOx emissions from an urban agglomeration based on TROPOMI NO2 and a local ensemble transform Kalman filter
Evaluation of O3, H2O, CO, and NOy climatologies simulated by four global models in the upper troposphere–lower stratosphere with IAGOS measurements
Source contribution to ozone pollution during June 2021 fire events in Arizona: insights from WRF-Chem-tagged O3 and CO
High-resolution mapping of on-road vehicle emissions with real-time traffic datasets based on big data
Sensitivity of climate–chemistry model simulated atmospheric composition to the application of an inverse relationship between NOx emission and lightning flash frequency
Regional and sectoral contributions of NOx and reactive carbon emission sources to global trends in tropospheric ozone during the 2000–2018 period
Underappreciated contributions of biogenic volatile organic compounds from urban green spaces to ozone pollution
Chemistry–climate feedback of atmospheric methane in a methane-emission-flux-driven chemistry–climate model
Surface ozone trend variability across the United States and the impact of heat waves (1990–2023)
Influence of Various Criteria on Identifying the Springtime Tropospheric Ozone Depletion Events (ODEs) at Utqiagvik, Arctic
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over south and east Asia
The role of the tropical carbon balance in determining the large atmospheric CO2 growth rate in 2023
Shifts in global atmospheric oxidant chemistry from land cover change
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations – a case study of the 2019 Raikoke eruption
Revisiting the high tropospheric ozone over southern Africa: role of biomass burning and anthropogenic emissions
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Local and transboundary contributions to NOy loadings across East Asia using CMAQ-ISAM and a GEMS-informed emission inventory during the winter–spring transition
Estimating the variability in NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
Effects of enhancing nitrogen use efficiency in cropland and livestock systems on agricultural ammonia emissions and particulate matter air quality in China
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Tropospheric ozone responses to the El Niño-Southern Oscillation (ENSO): quantification of individual processes and future projections from multiple chemical models
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Contributions of lightning to long-term trends and inter-annual variability in global atmospheric chemistry constrained by Schumann Resonance observations
Simulated photochemical response to observational constraints on aerosol vertical distribution over North China
Impacts of wildfire smoke aerosols on near-surface ozone photochemistry
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Effectiveness of Emission Controls on Atmospheric Oxidation and Air Pollutant Concentrations: Uncertainties due to Chemical Mechanisms and Inventories
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
The 21st-century wetting inhibits growing surface ozone in Northwestern China
Effects of different emission inventories on tropospheric ozone and methane lifetime
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Global atmospheric inversion of the NH3 emissions over 2019–2022 using the LMDZ-INCA chemistry-transport model and the IASI NH3 observations
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
The impact of sea spray aerosol on photochemical ozone formation over eastern China: heterogeneous reaction of chlorine particles and radiative effect
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Improving the computation efficiency of a source-oriented chemical mechanism for the simultaneous source apportionment of ozone and secondary particulate pollutants
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Suvarna Fadnavis, Yasin Elshorbany, Jerald Ziemke, Brice Barret, Alexandru Rap, P. R. Satheesh Chandran, Richard J. Pope, Vijay Sagar, Domenico Taraborrelli, Eric Le Flochmoen, Juan Cuesta, Catherine Wespes, Folkert Boersma, Isolde Glissenaar, Isabelle De Smedt, Michel Van Roozendael, Hervé Petetin, and Isidora Anglou
Atmos. Chem. Phys., 25, 8229–8254, https://doi.org/10.5194/acp-25-8229-2025, https://doi.org/10.5194/acp-25-8229-2025, 2025
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Satellites and model simulations show enhancement in tropospheric ozone, which is highly impacted by human-produced nitrous oxides compared to volatile organic compounds. The increased amount of ozone enhances ozone radiative forcing. The ozone enhancement and associated radiative forcing are the highest over South and East Asia. The emissions of nitrous oxides show a higher influence on shifting ozone photochemical regimes than volatile organic compounds.
Xiao Lu, Yiming Liu, Jiayin Su, Xiang Weng, Tabish Ansari, Yuqiang Zhang, Guowen He, Yuqi Zhu, Haolin Wang, Ganquan Zeng, Jingyu Li, Cheng He, Shuai Li, Teerachai Amnuaylojaroen, Tim Butler, Qi Fan, Shaojia Fan, Grant L. Forster, Meng Gao, Jianlin Hu, Yugo Kanaya, Mohd Talib Latif, Keding Lu, Philippe Nédélec, Peer Nowack, Bastien Sauvage, Xiaobin Xu, Lin Zhang, Ke Li, Ja-Ho Koo, and Tatsuya Nagashima
Atmos. Chem. Phys., 25, 7991–8028, https://doi.org/10.5194/acp-25-7991-2025, https://doi.org/10.5194/acp-25-7991-2025, 2025
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This study analyzes summertime ozone trends in East and Southeast Asia derived from a comprehensive observational database spanning from 1995 to 2019, incorporating aircraft observations, ozonesonde data, and measurements from 2500 surface sites. Multiple models are applied to attribute to changes in anthropogenic emissions and climate. The results highlight that increases in anthropogenic emissions are the primary driver of ozone increases both in the free troposphere and at the surface.
Nana Wei, Eloise A. Marais, Gongda Lu, Robert G. Ryan, and Bastien Sauvage
Atmos. Chem. Phys., 25, 7925–7940, https://doi.org/10.5194/acp-25-7925-2025, https://doi.org/10.5194/acp-25-7925-2025, 2025
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This study uses reactive nitrogen observations from NASA DC-8 research aircraft and the In-service Aircraft for a Global Observing System (IAGOS) campaigns to characterize reactive nitrogen seasonality and composition in the global upper troposphere and to diagnose the greatest knowledge gaps from comparison to a state-of-the-science model, GEOS-Chem, that need to be resolved for climate, nitrogen cycle, and air pollution assessments.
Alexander K. Tardito Chaudhri and David S. Stevenson
Atmos. Chem. Phys., 25, 7369–7385, https://doi.org/10.5194/acp-25-7369-2025, https://doi.org/10.5194/acp-25-7369-2025, 2025
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There remains a large uncertainty in the global warming potential of atmospheric hydrogen due to poor constraints on its soil deposition and, therefore, its lifetime. A new analysis of the latitudinal variation in the observed seasonality of hydrogen is used to constrain its surface fluxes. This is complemented with a simple latitude–height model where surface fluxes are adjusted from a prototype deposition scheme.
María Cazorla, Melissa Trujillo, Rodrigo Seguel, and Laura Gallardo
Atmos. Chem. Phys., 25, 7087–7109, https://doi.org/10.5194/acp-25-7087-2025, https://doi.org/10.5194/acp-25-7087-2025, 2025
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The current climate and environmental crises impose the need to take actions in cities to curb ozone as a pollutant and a climate forcer. This endeavor is challenging in understudied regions. In this work we analyze how reducing levels of precursor chemicals would affect ozone formation in Quito, Ecuador, and Santiago, Chile.
Ji Xia, Yi Zhou, Li Fang, Yingfei Qi, Dehao Li, Hong Liao, and Jianbing Jin
Atmos. Chem. Phys., 25, 7071–7086, https://doi.org/10.5194/acp-25-7071-2025, https://doi.org/10.5194/acp-25-7071-2025, 2025
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This study established an ammonia emission inventory for South Asia via an assimilation-based inversion system. The posterior emissions, calculated by integrating the anthropogenic inventory and satellite observations, showed significant improvement over the prior. Validation against various measurements supports our results. The study offers a deep understanding of ammonia emissions for policymakers and researchers aiming to develop air quality management and mitigation strategies for South Asia.
Yuwen Peng, Bin Yuan, Sihang Wang, Xin Song, Zhe Peng, Wenjie Wang, Suxia Yang, Jipeng Qi, Xianjun He, Yibo Huangfu, Xiao-Bing Li, and Min Shao
Atmos. Chem. Phys., 25, 7037–7052, https://doi.org/10.5194/acp-25-7037-2025, https://doi.org/10.5194/acp-25-7037-2025, 2025
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A structural-based parameterization for the photolysis rates of oxygenated volatile organic compounds (OVOCs) was integrated into an updated chemical mechanism. This method links photolysis rates to species' structure, bypassing limitations of insufficient quantum yield data. Box model results show that non-HCHO OVOCs, particularly multifunctional carbonyl compounds, significantly contribute to radical production, with alkene and aromatic oxidation products playing key roles.
Catalina Poraicu, Jean-François Müller, Trissevgeni Stavrakou, Crist Amelynck, Bert W. D. Verreyken, Niels Schoon, Corinne Vigouroux, Nicolas Kumps, Jérôme Brioude, Pierre Tulet, and Camille Mouchel-Vallon
Atmos. Chem. Phys., 25, 6903–6941, https://doi.org/10.5194/acp-25-6903-2025, https://doi.org/10.5194/acp-25-6903-2025, 2025
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We investigated the sources and impacts of nitrogen oxides and organic compounds over a remote tropical island. Simulations of the high-resolution Weather Research and Forecasting model coupled with chemistry (WRF-Chem) were evaluated using in situ Fourier transform infrared spectroscopy (FTIR) and satellite measurements. This work highlights gaps in current models, like missing sources of key organic compounds and inaccuracies in emission inventories, emphasizing the importance of improving chemical and dynamical processes in atmospheric modelling for budget estimates in tropical regions.
Yosuke Niwa, Yasunori Tohjima, Yukio Terao, Tazu Saeki, Akihiko Ito, Taku Umezawa, Kyohei Yamada, Motoki Sasakawa, Toshinobu Machida, Shin-Ichiro Nakaoka, Hideki Nara, Hiroshi Tanimoto, Hitoshi Mukai, Yukio Yoshida, Shinji Morimoto, Shinya Takatsuji, Kazuhiro Tsuboi, Yousuke Sawa, Hidekazu Matsueda, Kentaro Ishijima, Ryo Fujita, Daisuke Goto, Xin Lan, Kenneth Schuldt, Michal Heliasz, Tobias Biermann, Lukasz Chmura, Jarsolaw Necki, Irène Xueref-Remy, and Damiano Sferlazzo
Atmos. Chem. Phys., 25, 6757–6785, https://doi.org/10.5194/acp-25-6757-2025, https://doi.org/10.5194/acp-25-6757-2025, 2025
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This study estimated regional and sectoral emission contributions to the unprecedented surge of atmospheric methane for 2020–2022. The methane is the second most important greenhouse gas, and its emissions reduction is urgently required to mitigate global warming. Numerical modeling-based estimates with three different sets of atmospheric observations consistently suggested large contributions of biogenic emissions from South Asia and Southeast Asia to the surge of atmospheric methane.
Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut
Atmos. Chem. Phys., 25, 6273–6297, https://doi.org/10.5194/acp-25-6273-2025, https://doi.org/10.5194/acp-25-6273-2025, 2025
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In this study, we evaluate the present state of modelling lightning flashes over the Northern Hemisphere, using the classical CTH (cloud-top height) scheme and the ICEFLUX scheme with the CHIMERE model. Our study provides a comprehensive 3D comparison of model outputs to assess the robustness and applicability of these schemes. An improvement in O3 distribution in the tropical free troposphere is observed due to inclusion of LNOx (nitrogen oxide emissions from lightning) in the model. Inclusion of LNOx also reduces the lifetime of trace gas CH4.
Audrey Fortems-Cheiney, Grégoire Broquet, Elise Potier, Antoine Berchet, Isabelle Pison, Adrien Martinez, Robin Plauchu, Rimal Abeed, Aurélien Sicsik-Paré, Gaelle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, Henk Eskes, Hugo A. C. Denier van der Gon, and Stijn N. C. Dellaert
Atmos. Chem. Phys., 25, 6047–6068, https://doi.org/10.5194/acp-25-6047-2025, https://doi.org/10.5194/acp-25-6047-2025, 2025
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This study assesses the potential of the Ozone Monitoring Instrument (OMI) and the TROPOspheric Monitoring Instrument (TROPOMI) satellite observations to inform about the decrease in anthropogenic emissions of nitrogen oxides (NOx) in 2019 compared with 2005 at regional to national scales in Europe. Both the OMI and TROPOMI inversions show decreases in European NOx anthropogenic emission budgets in 2019 compared to 2005 but with different magnitudes.
Yawen Kong, Bo Zheng, and Yuxi Liu
Atmos. Chem. Phys., 25, 5959–5976, https://doi.org/10.5194/acp-25-5959-2025, https://doi.org/10.5194/acp-25-5959-2025, 2025
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Current high-resolution satellite remote sensing technologies provide a unique opportunity to derive timely high-resolution emission data. We developed an emission inversion system to assimilate satellite NO2 data to obtain daily kilometer-scale NOx emission inventories. Our results enhance inventory accuracy, allowing us to capture the effects of pollution control policies on daily emissions (e.g., during COVID-19 lockdowns) and improve fine-scale air quality modeling.
Yann Cohen, Didier Hauglustaine, Nicolas Bellouin, Marianne Tronstad Lund, Sigrun Matthes, Agnieszka Skowron, Robin Thor, Ulrich Bundke, Andreas Petzold, Susanne Rohs, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 25, 5793–5836, https://doi.org/10.5194/acp-25-5793-2025, https://doi.org/10.5194/acp-25-5793-2025, 2025
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The chemical composition of the atmosphere near the tropopause is a key parameter for evaluating the climate impact of subsonic aviation pollutants. This study uses in situ data collected aboard passenger aircraft to assess the ability of four chemistry–climate models to reproduce (bi-)decadal climatologies of ozone, carbon monoxide, water vapour, and reactive nitrogen in this region. The models reproduce the very distinct ozone seasonality in the upper troposphere and in the lower stratosphere well.
Yafang Guo, Mohammad Amin Mirrezaei, Armin Sorooshian, and Avelino F. Arellano
Atmos. Chem. Phys., 25, 5591–5616, https://doi.org/10.5194/acp-25-5591-2025, https://doi.org/10.5194/acp-25-5591-2025, 2025
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We assess the contributions of fire and anthropogenic emissions to O3 levels in Phoenix, Arizona, during a period of intense heat and drought conditions. We find that fire exacerbates O3 pollution and that interactions between weather, climate, and air chemistry are important to consider. This has implications for activities related to formulating emission reduction strategies in areas that are currently understudied yet becoming relevant due to reports of increasing global aridity.
Yujia Wang, Hongbin Wang, Bo Zhang, Peng Liu, Xinfeng Wang, Shuchun Si, Likun Xue, Qingzhu Zhang, and Qiao Wang
Atmos. Chem. Phys., 25, 5537–5555, https://doi.org/10.5194/acp-25-5537-2025, https://doi.org/10.5194/acp-25-5537-2025, 2025
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This study established a bottom-up approach that employs real-time traffic flows and interpolation to obtain a spatially continuous on-road vehicle emission mapping for the main urban area of Jinan. The diurnal variation, spatial distribution, and emission hotspots were analyzed with clustering and hotspot analysis, showing unique fine-scale variation characteristics of on-road vehicle emissions. Future scenario analysis demonstrates remarkable benefits of electrification on emission reduction.
Francisco J. Pérez-Invernón, Francisco J. Gordillo-Vázquez, Heidi Huntrieser, Patrick Jöckel, and Eric J. Bucsela
Atmos. Chem. Phys., 25, 5557–5575, https://doi.org/10.5194/acp-25-5557-2025, https://doi.org/10.5194/acp-25-5557-2025, 2025
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Lightning plays a significant role in tropospheric chemistry by producing substantial amounts of nitrogen oxides. According to recent estimates, thunderstorms that produce a higher lightning frequency rate also produce less nitrogen oxide per flash. We implemented the dependency of nitrogen oxide production per flash on lightning flash frequency in a chemical atmospheric model.
Aditya Nalam, Aura Lupaşcu, Tabish Ansari, and Tim Butler
Atmos. Chem. Phys., 25, 5287–5311, https://doi.org/10.5194/acp-25-5287-2025, https://doi.org/10.5194/acp-25-5287-2025, 2025
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Tropospheric O3 molecules are labeled with the identity of their precursor source to simulate contributions from various emission sources to the global tropospheric O3 burden (TOB) and its trends. With an equatorward shift, anthropogenic NOx emissions become significantly more efficient at producing O3 and play a major role in driving TOB trends, mainly due to larger convection at the tropics effectively lifting O3 and its precursors to the free troposphere, where O3 lifetime is longer.
Haofan Wang, Yuejin Li, Yiming Liu, Xiao Lu, Yang Zhang, Qi Fan, Chong Shen, Senchao Lai, Yan Zhou, Tao Zhang, and Dingli Yue
Atmos. Chem. Phys., 25, 5233–5250, https://doi.org/10.5194/acp-25-5233-2025, https://doi.org/10.5194/acp-25-5233-2025, 2025
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This study explores how urban green spaces (UGSs) in Guangzhou influence ozone levels. By using advanced models, we found that natural emissions from these areas can significantly affect air quality. Our results suggest that the design and planning of UGSs should not only consider aesthetics and social factors but also their environmental impacts on air quality.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
Atmos. Chem. Phys., 25, 5133–5158, https://doi.org/10.5194/acp-25-5133-2025, https://doi.org/10.5194/acp-25-5133-2025, 2025
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry–climate model to assess the feedback of atmospheric methane induced by changes in the chemical sink in a warming climate and its implications for the chemical composition and the surface air temperature change.
Kai-Lan Chang, Brian C. McDonald, Colin Harkins, and Owen R. Cooper
Atmos. Chem. Phys., 25, 5101–5132, https://doi.org/10.5194/acp-25-5101-2025, https://doi.org/10.5194/acp-25-5101-2025, 2025
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Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over the period from 1990 to 2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heat wave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Xiaochun Zhu, Le Cao, Xin Yang, Simeng Li, Jiandong Wang, and Tianliang Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-3873, https://doi.org/10.5194/egusphere-2024-3873, 2025
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We applied various criteria to identify springtime ODEs at Utqiagvik, Arctic, and investigated the influences of using different criteria on conclusions regarding the characteristics of ODEs. We found criteria using a constant threshold and using thresholds based on the monthly averaged ozone more suitable for identifying ODEs than the others. Applying a threshold varying with the monthly average or stricter thresholds also signifies a more significant reduction in the ODE occurrences.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
Atmos. Chem. Phys., 25, 4929–4942, https://doi.org/10.5194/acp-25-4929-2025, https://doi.org/10.5194/acp-25-4929-2025, 2025
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs with different amounts of leakages and with where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Martyn P. Chipperfield
Atmos. Chem. Phys., 25, 4785–4802, https://doi.org/10.5194/acp-25-4785-2025, https://doi.org/10.5194/acp-25-4785-2025, 2025
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane, and aerosols. Satellite instruments can quantify column NO2 and, by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over south and east Asia is assessed, showing that the model captures not only many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Liang Feng, Paul Palmer, Luke Smallman, Jingfeng Xiao, Paulo Cristofanelli, Ove Hermansen, John Lee, Casper Labuschagne, Simonetta Montaguti, Steffen Noe, Stephen Platt, Xinrong Ren, Martin Steinbacher, and Irene Xueref-Remy
EGUsphere, https://doi.org/10.5194/egusphere-2025-1793, https://doi.org/10.5194/egusphere-2025-1793, 2025
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2023 saw an unexpectedly high global atmospheric CO2 growth. Satellite data reveal a role for increased emissions over the tropics. Larger emissions over eastern Brazil can be explained by warmer temperatures, while changes in rainfall and soil moisture play more of a role in emission increases elsewhere in the tropics.
Ryan Vella, Sergey Gromov, Clara M. Nussbaumer, Laura Stecher, Matthias Kohl, Samuel Ruhl, Holger Tost, Jos Lelieveld, and Andrea Pozzer
EGUsphere, https://doi.org/10.5194/egusphere-2025-1800, https://doi.org/10.5194/egusphere-2025-1800, 2025
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We evaluated how replacing forests with farmland and grazing areas affects atmospheric composition. Using a global climate-chemistry model, we found that deforestation reduces BVOCs, increases farming pollutants, and shifts ozone chemistry. These changes lead to a small cooling effect on the climate. Restoring natural vegetation could reverse some of these effects.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
Atmos. Chem. Phys., 25, 4403–4418, https://doi.org/10.5194/acp-25-4403-2025, https://doi.org/10.5194/acp-25-4403-2025, 2025
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 25, 4455–4475, https://doi.org/10.5194/acp-25-4455-2025, https://doi.org/10.5194/acp-25-4455-2025, 2025
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The impacts of biomass burning and anthropogenic emissions on high tropospheric ozone levels are not well studied in southern Africa. We combined model simulations with recent observations at the surface and from space to quantify tropospheric ozone and its drivers in southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in southern Africa.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
Atmos. Chem. Phys., 25, 4313–4331, https://doi.org/10.5194/acp-25-4313-2025, https://doi.org/10.5194/acp-25-4313-2025, 2025
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants that may influence future approaches to modelling climate.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
Atmos. Chem. Phys., 25, 4291–4311, https://doi.org/10.5194/acp-25-4291-2025, https://doi.org/10.5194/acp-25-4291-2025, 2025
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We investigated NOx emission contributions to NOy loadings across five regions of East Asia during the 2022 winter–spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
Atmos. Chem. Phys., 25, 3313–3326, https://doi.org/10.5194/acp-25-3313-2025, https://doi.org/10.5194/acp-25-3313-2025, 2025
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Biao Luo, Lei Liu, David H. Y. Yung, Tiangang Yuan, Jingwei Zhang, Leo T. H. Ng, and Amos P. K. Tai
EGUsphere, https://doi.org/10.5194/egusphere-2025-72, https://doi.org/10.5194/egusphere-2025-72, 2025
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Through a combination of emission models and air quality model, we aimed to address the pressing issue of poor nitrogen management while promoting sustainable food systems and public health in China. We discovered that improving nitrogen management of crop and livestock can substantially reduce air pollutant emissions, particularly in North China Plain. Our findings further provide the benefits of such interventions on PM2.5 reductions, offering valuable insights for policymakers.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
Atmos. Chem. Phys., 25, 3029–3048, https://doi.org/10.5194/acp-25-3029-2025, https://doi.org/10.5194/acp-25-3029-2025, 2025
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of surface ozone and large-scale circulations such as atmospheric blocking. Besides local heat waves, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation in regional air quality.
Jingyu Li, Haolin Wang, Qi Fan, and Xiao Lu
EGUsphere, https://doi.org/10.5194/egusphere-2025-782, https://doi.org/10.5194/egusphere-2025-782, 2025
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We use multiple global chemical models to quantify processes contributing the ozone response to ENSO. We find that changes in transport patterns are the dominant factor in the overall ozone-ENSO responses, with the opposing effects of chemical depletion and increased biomass burning on ozone largely offsetting each other. Models consistently project an increase in tropical ozone-ENSO response associated with strengthening anomalous circulation and more abundant water vapor with global warming.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Xiaobo Wang, Yuzhong Zhang, Tamás Bozóki, Ruosi Liang, Xinchun Xie, Shutao Zhao, Rui Wang, Yujia Zhao, and Shuai Sun
EGUsphere, https://doi.org/10.5194/egusphere-2025-370, https://doi.org/10.5194/egusphere-2025-370, 2025
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Schumann Resonance observations are used to parameterize lightning NOx emissions for better capturing global lightning trend and variability. Updated simulations reveal insignificant trend but greater variability in lightning NOx emissions, impacting tropospheric NOx, O3 and OH. Lightning generally counteracts non-lightning factors, reducing the inter-annua variability of tropospheric O3 and OH. Variations of global lightning play important role in understanding the atmospheric methane budget.
Xi Chen, Ke Li, Ting Yang, Xipeng Jin, Lei Chen, Yang Yang, Shuman Zhao, Bo Hu, Bin Zhu, Zifa Wang, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2025-430, https://doi.org/10.5194/egusphere-2025-430, 2025
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Aerosol vertical distribution that plays a crucial role in aerosol-photolysis interaction (API) remains underrepresented in chemical models. We integrated lidar and radiosonde observations to constrain the simulated aerosol profiles over North China and quantified the photochemical responses. The increased photolysis rates in the lower layers led to increased ozone and accounted for a 36 %–56 % reduction in API effects, resulting in enhanced atmospheric oxidizing capacity and aerosol formation.
Jiaqi Shen, Ronald C. Cohen, Glenn M. Wolfe, and Xiaomeng Jin
EGUsphere, https://doi.org/10.5194/egusphere-2025-706, https://doi.org/10.5194/egusphere-2025-706, 2025
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This study shows large chemical and radiative effects of smoke aerosols from fires on near-surface ozone production. Aerosol loading and NOx levels are identified as the primary factors influencing these effects. Furthermore, we show that the surface PM2.5 to NO2 column ratio can be used as an indicator for identifying aerosol-dominated regimes, facilitating the assessments of aerosol impacts on ozone formation through satellite observations.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Mingjie Kang, Hongliang Zhang, and Qi Ying
EGUsphere, https://doi.org/10.5194/egusphere-2025-255, https://doi.org/10.5194/egusphere-2025-255, 2025
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This study examines the impacts of reducing nitrogen oxides and volatile organic compounds on ozone (O3), secondary inorganic aerosols (SIA), and OH and NO3 radicals. The results show similar predictions for 8-h O3 but significant variability for SIA and radicals, with differences up to 30 % for SIA and 200 % for radicals across chemical mechanisms and inventories. The findings highlight that evaluating control strategies for SIA and atmospheric oxidation capacity requires an ensemble approach.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Xiaodong Zhang, Yu Yan, Ning Zhang, Wenpeng Wang, Huabing Suo, Xiaohu Jian, Chao Wang, Haibo Ma, Hong Gao, Zhaoli Yang, Tao Huang, and Jianmin Ma
EGUsphere, https://doi.org/10.5194/egusphere-2025-258, https://doi.org/10.5194/egusphere-2025-258, 2025
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This study performed comprehensive sensitivity model simulations to explore the surface O3 responses to historical and projected climate change in Northwestern China (NW). Our results reveal that substantial wetting trends since the 21st century have mitigated O3 growth in this region, with the influence of wetting on O3 evolution outweighing the warming effect. These findings should be taken into account in future policymaking aimed at scientifically reducing O3 pollution in NW.
Catherine Acquah, Laura Stecher, Mariano Mertens, and Patrick Jöckel
EGUsphere, https://doi.org/10.5194/egusphere-2025-294, https://doi.org/10.5194/egusphere-2025-294, 2025
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Short-lived ozone precursor species influence the formation of ozone and also the atmospheric lifetime of methane. Our study assesses the effect of two widely used emission inventories of these species on ozone and the methane lifetime. Our results indicate tropospheric ozone and methane lifetime differences of around 4 % even though both emission inventories aim at representing present-day conditions. We further attribute the differences to emissions of individual sectors, e.g. land traffic.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Pramod Kumar, Grégoire Broquet, Didier Hauglustaine, Maureen Beaudor, Lieven Clarisse, Martin Van Damme, Pierre Coheur, Anne Cozic, Bo Zheng, Beatriz Revilla Romero, Antony Delavois, and Philippe Ciais
EGUsphere, https://doi.org/10.5194/egusphere-2025-162, https://doi.org/10.5194/egusphere-2025-162, 2025
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Global maps of the NH3 emissions over 2019–2022 are derived using IASI NH3 spaceborne observations, the LMDZ-INCA chemistry-transport model at 1.27°×2.5° resolution and mass balance approach. The average global NH3 emissions over the period are ~98 Tg NH3 yr-1, which is significantly higher than three reference inventories. The analysis provides confidence in the seasonal variability and regional budgets, and provides new insights into NH3 emissions at global and regional scales.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yingying Hong, Yuqi Zhu, Yuxuan Huang, Yiming Liu, Chuqi Xiong, and Qi Fan
EGUsphere, https://doi.org/10.5194/egusphere-2024-4132, https://doi.org/10.5194/egusphere-2024-4132, 2025
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This study investigates the impact of sea spray aerosol on ozone formation across Eastern China, highlighting its complex influence through both chemical reactions and radiative effects, which vary seasonally and geographically.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Qixiang Xu, Fangcheng Su, Ke Wang, Ruiqin Zhang, Qi Ying, and Michael J. Kleeman
EGUsphere, https://doi.org/10.5194/egusphere-2025-44, https://doi.org/10.5194/egusphere-2025-44, 2025
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This manuscript introduces a novel approach for improving the computational efficiency and scalability of source-oriented chemical mechanisms by simplifying the representation of reactions involving source-tagged species and implementing a source-oriented Euler Backward Iterative (EBI) solver. These advancements reduce simulation times by up to 74 % while maintaining accuracy, offering significant practical benefits for long-term source apportionment studies.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Cited articles
Amos, H. M., Jacob, D. J., Holmes, C. D., Fisher, J. A., Wang, Q., Yantosca, R. M., Corbitt, E. S., Galarneau, E., Rutter, A. P., Gustin, M. S., Steffen, A., Schauer, J. J., Graydon, J. A., Louis, V. L. St., Talbot, R. W., Edgerton, E. S., Zhang, Y., and Sunderland, E. M.: Gas-particle partitioning of atmospheric Hg(II) and its effect on global mercury deposition, Atmos. Chem. Phys., 12, 591–603, https://doi.org/10.5194/acp-12-591-2012, 2012.
Aumont, B.: Modélisation de la chimie troposphérique, Manuscript presented for the degree of “Habilitation a diriger les recherches”, Université Paris 12, Val de Marne, UFR de Sciences et Technologie, 2005.
Banerjee, A., Archibald, A. T., Maycock, A. C., Telford, P., Abraham, N. L., Yang, X., Braesicke, P., and Pyle, J. A.: Lightning NOx, a key chemistry-climate interaction: impacts of future climate change and consequences for tropospheric oxidising capacity, Atmos. Chem. Phys., 14, 9871–9881, https://doi.org/10.5194/acp-14-9871-2014, 2014.
Bechtold, P., Bazile, E., Guichard, F., Mascart, P., and Richard, E.: A mass-flux convection scheme for regional and global models, Q. J. Roy. Meteor. Soc., 127, 869–886, 2000.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of tropospheric chemistry with assimilated meteorology: model description and evaluation, J. Geophys. Res., 106, 23073–23095, 2001.
Bian, H. and Prather, M. J.: Fast-J2: Accurate simulation of stratospheric photolysis in global chemical models, J. Atmos. Chem., 41, 281–296, 2002.
Cariolle, D., Caro, D., Paoli, R., Hauglustaine, D. A., Cuénot, B., Cozic, A., and Paugam, R.: Parametrization of plume chemistry into large-scale atmospheric models: application to aicraft NOx emissions, J. Geophys. Res., 114, D19302, https://doi.org/10.1029/2009JD011873, 2009.
Choi, Y., Kim, J., Eldering, A., Osterman, G., Yung, Y. L., Gu, Y., and Liou, K. N.: Lightning and anthropogenic NOx sources over the United States and the western North Atlantic Ocean: impact on OLR and radiative effects, Geophys. Res. Lett., 36, L17806, https://doi.org/10.1029/2009GL039381, 2009.
Christian, H. J., Blakeslee, R. J., Boccippio, D. J., Boeck, W. L., Buechler, D. E., Driscoll, K. T., Goodman, S. J., Hall, J. M., Koshak, W. J., Mach, D. M., and Stewart, M. F.: Global frequency and distribution of lightning as observed from space by the Optical Transient Detector, J. Geophys. Res., 108, 4005, https://doi.org/10.1029/2002JD002347, 2003.
Cohard, J.-M. and Pinty, J. P.: A comprehensive two-moment warm microphysical bulk scheme. I: Description and tests, Q. J. Roy. Meteor. Soc., 126, 1815–1842, 2000.
Cooper, M., Martin, R. V., Wespes, C., Coheur, P.-F., Clerbaux, C., and Murray L. T.: Tropospheric nitric acid columns from the IASI satellite instrument interpreted with a chemical transport model: implications for parameterizations of nitric oxide production by lightning, J. Geophys. Res., 119, 10068–10079, 2014.
Cuxart, J., Bougeault, P., and Redelsperger, J. L.: A turbulence scheme allowing for mesoscale and large-eddy simulations, Q. J. Roy. Meteor. Soc., 126, 1–30, 1999.
Damian, V., Sandu, A., Damian, M., Potra, F., and Camichael, G. R.: The kinetic preprocessor KPP – a software environment for solving chemical kinectics, Comput. Chem. Eng., 26, 1567–1579, 2002.
Dye, J. E., Ridley, B. A., Skamarock, W., Barth, M., and Venticinque, M.: An overview of the Stratospheric-Tropospheric experiment: radiation, aerosols, and ozone (STERAO)-Deep convection experiment with results for the July 10, 1996 storm, J. Geophys. Res., 105, 10023–10045, 2000.
Emmerson, K. M. and Evans, M. J.: Comparison of tropospheric gas-phase chemistry schemes for use within global models, Atmos. Chem. Phys., 9, 1831–1845, https://doi.org/10.5194/acp-9-1831-2009, 2009.
Evans, M. J. and Jacob, D. J.: Impact of new laboratory studies of N2O5 hydrolysis on global model budgets of tropospheric nitrogen oxides, ozone, and OH, Geophys. Res. Lett., 32, L09813, https://doi.org/10.1029/2005GL022469, 2005.
Franzblau, E.: Electrical discharges involving the formation of NO, NO2, HNO3 and O3, J. Geophys. Res., 96, 22337–22345, 1991.
Gregory, D., Morcrette J.-J., Jakob, C., Beljaars, A. C. M., and Stockdale, T.: Revision of convection, radiation and cloud schemes in the ECMWF Integrated Forecasting System, Q. J. Roy. Meteor. Soc., 126, 1685–1710, 2000.
Grewe, V.: Impact of climate variability on tropospheric ozone, Sci. Total Environ., 374, 167–181, 2007.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Hauglustaine, D. A., Granier, C., and Brasseur, G. P.: Impact of present aircraft emissions of nitrogen oxides on troposheric ozone and climate forcing, Geophys. Res. Lett., 21, 2031–2034, 1994.
Hauglustaine, D., Emmons, L., Newchurch, M., Brasseur, G., Takao, T., Matsubara, K., Johnson, J., Ridley, B., Stith, J., and Dye, J.: On the role of lightning NOx in the formation of tropospheric ozone plumes: a global model perspective, J. Atmos. Chem., 38, 277–294, 2001.
Hudman, R. C., Jacob, D. J., Turquety, S., Leibensperger, E. M., Murray, L. T., Wu, S., Gilliland, A. B., Avery, M., Bertram, T. H., Brune, W., Cohen, R. C., Dibb, J. E., Flocke, F. M., Fried, A., Holloway, J., Neuman, J. A., Orville, R., Perring, A., Ren, X., Sachse, G. W., Singh, H. B., Swanson, A., and Wooldridge, P. J.: Surface and lightning sources of nitrogen oxides over the United States: Magnitudes, chemical evolution, and outflow, J. Geophys. Res., 112, D12S05, https://doi.org/10.1029/2006JD007912, 2007.
Huntrieser, H., Schlager, H., Feigl, C., and Höller, H.: Transport and production of NOx in electrified thunderstorms: survey of previous studies and new observations at midlatitudes, J. Geophys. Res., 103, 28247–28264, 1998.
Huntrieser, H., Feigl, C., Schlager, H., Schröder, F., Gerbig, C., and van Velthoven, P.: Airborne measurements of NOx, tracer species, and small particles during the European Lightning Nitrogen Oxides Experiment, J. Geophys. Res., 107, 4113, https://doi.org/10.1029/2000JD000209, 2002.
Huszar, P., Cariolle, D., Paoli, R., Halenka, T., Belda, M., Schlager, H., Miksovsky, J., and Pisoft, P.: Modeling the regional impact of ship emissions on NOx and ozone levels over the Eastern Atlantic and Western Europe using ship plume parameterization, Atmos. Chem. Phys., 10, 6645–6660, https://doi.org/10.5194/acp-10-6645-2010, 2010.
Jacobson, M. Z. and Turco, R. P.: SMVGEAR: a sparse-matrix, vectorized gear code for atmospheric models, Atmos. Environ., 28, 273–284, 1994.
Jaéglé, L., Jacob, D. J., Wang, Y., Weinheimer, A. J., Ridley, B. A., Campos, T. L., Sachse, G. W., and Hagen, D. E.: Soucres and chemistry of NOx in the upper troposphere over the United Sates, Geophys. Res. Lett., 25, 1705–1708, 1998.
Jenkin, M. E., Saunders, S. M., and Pilling, M. J.: The tropospheric degradation of volatile organic compounds: a protocol for mechanism development, Atmos. Environ., 31, 81–104, 1997.
Klemp, J. B. and Wilhelmson, R. B.: The simulation of three-dimensional convective storm dynamics, J. Atmos. Sci., 35, 1070–1096, 1978.
Knollenberg, R. G.: Measurements of the growth of the ice budget in a persisting contrail, J. Atmos. Sci., 29, 1367–1374, 1972.
Knollenberg, R. G., Kelly, K., and Wilson, J. C.: Measurements of high number densities of ice crystals in the tops of tropical cumulonimbus, J. Geophys. Res., 98, 8639–8664, 1993.
Labrador, L. J., von Kuhlmann, R., and Lawrence, M. G.: Strong sensitivity of the global mean OH concentration and te tropospheric oxidizing efficiency to the source of NOx from lightning, Geophys. Res. Lett., 31, L06102, https://doi.org/10.1029/2003GL019229, 2004.
Lafore, J. P., Stein, J., Asencio, N., Bougeault, P., Ducrocq, V., Duron, J., Fischer, C., Héreil, P., Mascart, P., Masson, V., Pinty, J. P., Redelsperger, J. L., Richard, E., and Vilà-Guerau de Arellano, J.: The Meso-NH Atmospheric Simulation System. Part I: adiabatic formulation and control simulations, Ann. Geophys., 16, 90–109, https://doi.org/10.1007/s00585-997-0090-6, 1998.
Lange, L., Hoor, P., Helas, G., Fischer, H., Brunner, D., Scheeren, B., Williams, J., Wong, S., Wohlfrom, K.-H., Arnold F., Strom, J., Krejci, R., Lelieveld, J., and Andreae, M. O.: Detection of lightning-produced NO in the midlatitude upper troposphere during STREAM 1998, J. Geophys. Res., 106, 27777–27785, 2001.
Lascaux, F., Richard, E., and Pinty, J. P.: Numerical simulations of three different MAP IOPs and the associated microphysical processes, Q. J. Roy. Meteor. Soc., 132, 1907–1926, 2006.
Lin, J.-T. and McElroy, M. B.: Impacts of boundary layer mixing on pollutant vertical profiles in the lower troposphere: implications to satellite remote sensing, Atmos. Environ., 44, 1726–1739, 2010.
Lin, S.-J. and Rood, R. B.: Multidimensional flux-form semi-lagrangian transport scheme, Mon. Weather Rev., 124, 2046–2070, 1996.
Lin, X., Trainer, M., and Liu, S. C.: On the nonlinearity of the tropospheric ozone production, J. Geophys. Res., 93, 15879–15888, 1988.
Liu, H., Jacob, D. J., Rey, I., and Yantosca, R. M.: Constraints from 210Pb and 7Be on wet deposition and transport in a global three-dimensional chemical tracer model driven by assimilated meteorological fields, J. Geophys. Res., 106, 12109–12128, 2001.
Madronich, S. and Flocke, S.: Environmental Photochemistry, https://doi.org/10.1007/978-3-540-69044-3, Springer Berlin Heidelberg, 1999.
Martin, R. V., Jacob, D. J., Logan, J. A., Bey, I., Yantosca, R. M., Staudt, A. C., Li, Q., Fiore, A. M., Duncan, B. N., and Liu, H.: Interpretation of TOMS observations of tropical tropospheric ozone with a global model and in situ observations, J. Geophys. Res., 107, 4351, https://doi.org/10.1029/2001JD001480, 2002.
Martin, R. V., Jacob, D. J., Yantosca, R. M., Chin, M., and Ginoux, P.: Global and Regional Decreases in Tropospheric Oxidants from Photochemical Effects of Aerosols, J. Geophys. Res., 108, 4097, https://doi.org/10.1029/2002jd002622, 2003.
Martin, R. V., Sauvage, B., Folkins, I., Sioris, C. E., Boone, C., Bernath, P., and Ziemke, J.: Space-based constraints on the production of nitric oxide by lightning, J. Geophys. Res., 112, D09309, https://doi.org/10.1029/2006JD007831, 2007.
Monks, P. S.: Gas-phase radical chemistry in the tropopshere, Chem. Soc. Rev., 34, 376–395, 2005.
Moorthi, S. and Suarez, M. J.: Relaxed Arakawa-Schubert: a parameterization of moist convection for general circulation models, Mon. Weather Rev., 120, 978–1002, 1991.
Murray, L. T., Jacob, D. J., Logan, J. A., Hudman, R. C., and Koshak, J.: Optimized regional and interannual variability of lightning in a global chemical transport model constrained by LIS/OTD satelite data, J. Geophys. Res., 117, D20307, https://doi.org/10.1029/2012JD017934, 2012.
Olivier, J. G. J.: Recent trends in global greenhouse gas emissions: regional trends and spatial distribution of key sources, Environ. Sci., 2, 81–89, 2005.
Ott, L. E., Pickering, K. E., Stenchikov, G. L., Allen, D. J., DeCaria, A. J., Ridley, B., Lin, R.-F., Lang, S., and Tao, W.-K.: Production of lightning NOx and its vertical distribution calculated from three-dimensional cloud-scale chemical transport model simulations, J. Geophys. Res., 115, D04301, https://doi.org/10.1029/2009JD011880, 2010.
Paoli, R., Cariolle, D., and Sausen, R.: Review of effective emissions modeling and computation, Geosci. Model Dev., 4, 643–667, https://doi.org/10.5194/gmd-4-643-2011, 2011.
Pickering, K. E., Thompson, A. M., Dickerson, R. R., Luke, W. T., MacNamara, D. P., Greenberg, J. P., and Zimmerman, P. R.: Model calculations of tropospheric ozone production potentiel following observed convective events, J. Geophys. Res., 95, 14049–14062, 1990.
Pinty, J. P. and Jabouille, P.: A mixed-phase cloud parameterization for use in a mesoscale non-hydrostatic model: simulations of a squall line and of orographic precipitation, in: Proceedings of Conference on Cloud Physics, 17–21 August 1998, Everett, USA, 217–220, 1998.
Price, C. and Rind, D.: A simple lightning parameterization for calculating global lightning distributions, J. Geophys. Res., 97, 9919–9933, 1992.
Price, C. and Rind, D.: Possible implications of global climate change on global lightning distributions and frequencies, J. Geophys. Res., 99, 10823–10831, 1994.
Sander, S. P., Friedl, R. R., Golden, D. M., Kurylo, M. J., Moortgat, G. K., Wine, P. H., Ravishankara, A. R., Kolb, C. E., Molina, M. J., Finlayson-Pitts, B. J., Huie, R. E., and Orkin, V. L.: Chemical kinetics and photochemical data for use in atmosperic studies, evaluation number 15, Tech. rep., NASA, 2006.
Saunders, S. M., Jenkin, M. E., Derwent, R. G., and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part A): tropospheric degradation of non-aromatic volatile organic compounds, Atmos. Chem. Phys., 3, 161–180, https://doi.org/10.5194/acp-3-161-2003, 2003.
Sauvage, B., Martin, R. V., van Donkelaa, A., and Ziemke, J. R.: Quantification of the factors controlling tropical tropopsheric ozone and the South Atlantic maximum, J. Geophys. Res., 112, D11309, https://doi.org/10.1029/2006JD008008, 2007a.
Sauvage, B., Martin, R. V., van Donkelaar, A., Liu, X., Chance, K., Jaeglé, L., Palmer, P. I., Wu, S., and Fu, T.-M.: Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone, Atmos. Chem. Phys., 7, 815–838, https://doi.org/10.5194/acp-7-815-2007, 2007b.
Schumann, U. and Huntrieser, H.: The global lightning-induced nitrogen oxides source, Atmos. Chem. Phys., 7, 3823–3907, https://doi.org/10.5194/acp-7-3823-2007, 2007.
Stark, M. S., Harrison, J. T. H., and Anastasi, C.: Formation of nitrogen oxides by electrical discharges and implications for atmospheric lightning, J. Geophys. Res., 101, 6963–6969, 1996.
Stith, J., Dye, J., Ridley, B., Laroche, P., Defer, E., Hübler, G., Zerr, R., and Venticinque, M.: NO signatures from lightning flashes, J. Geophys. Res., 104, 16081–16089, 1999.
Stockwell, D. Z., Giannakopoulos, C., Plantevin, P. H., Carver, G. D., Chipperfield, M. P., Law, K. S., Pyle, J. A., Shallcross, D. E., and Wang, K. Y.: Modelling NOx from lightning and its impact on global chemical fields, Atmos. Environ., 33, 4477–4493, 1999.
Streets, D. G., Zhang, Q., Wang, L., He, L., Hao., J., Wu, Y., Tang, Y., and Carmichael, G. R.: Revisting China's CO emissions after the Transport and Chemical evolution over the Pacific (TRACE-P) mission: Synthesis of inventories, atmospheric modeling, and observations, J. Geophys. Res., 111, D14306, https://doi.org/10.1029/2006JD007118, 2006.
Teyssèdre, H., Michou, M., Clark, H. L., Josse, B., Karcher, F., Olivié, D., Peuch, V.-H., Saint-Martin, D., Cariolle, D., Attié, J.-L., Nédélec, P., Ricaud, P., Thouret, V., van der A, R. J., Volz-Thomas, A., and Chéroux, F.: A new tropospheric and stratospheric Chemistry and Transport Model MOCAGE-Climat for multi-year studies: evaluation of the present-day climatology and sensitivity to surface processes, Atmos. Chem. Phys., 7, 5815–5860, https://doi.org/10.5194/acp-7-5815-2007, 2007.
Tost, H., Jöckel, P., and Lelieveld, J.: Lightning and convection parameterisations – uncertainties in global modelling, Atmos. Chem. Phys., 7, 4553–4568, https://doi.org/10.5194/acp-7-4553-2007, 2007.
Trier, S. B. and Sharman, R. D.: Convection-permitting simulations of the environment supporting widespread turbulence within the upper-level outflow of a mesoscale convective system, American Meteorological Society, 137, 1972–1990, 2008.
Tulet, P., Crassier, V., Solmon, F., Guedalia, D., and Rosset, R.: Description of the Mesoscale Nonhydrostatic chemistry model and application to a transboundary pollution episode between northern France and southern England, J. Geophys. Res., 108, 4021, https://doi.org/10.1029/2000JD000301, 2003.
Tulet, P., Grini, A., Griffin, R. J., and Petitcol, S.: ORILAM-SOA: A compitationnaly efficient model for predicting secondary organic aerosols in three-dimensional atmospheric models, J. Geophys. Res., 111, D23208, https://doi.org/10.1029/2006JD007152, 2006.
van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Mu, M., Kasibhatla, P. S., Morton, D. C., DeFries, R. S., Jin, Y., and van Leeuwen, T. T.: Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997–2009), Atmos. Chem. Phys., 10, 11707–11735, https://doi.org/10.5194/acp-10-11707-2010, 2010.
Wang, Q., Jacob, D. J., Fisher, J. A., Mao, J., Leibensperger, E. M., Carouge, C. C., Le Sager, P., Kondo, Y., Jimenez, J. L., Cubison, M. J., and Doherty, S. J.: Sources of carbonaceous aerosols and deposited black carbon in the Arctic in winter-spring: implications for radiative forcing, Atmos. Chem. Phys., 11, 12453–12473, https://doi.org/10.5194/acp-11-12453-2011, 2011.
Wang, Y., Jacob, D. J., and Logan, J. A.: Global simulation of tropospheric O3-NOx-hydrocarbon chemistry – 1. Model formulation, J. Geophys. Res., 103, 10713–10725, 1998.
Wennberg, P. O., Hanisco, T. F., Jaegle, L., Jacob, D. J., Hintsa, E. J., Lanzendorf, E. J., Anderson, J. G., Gao, R.-S., Keim, E. J., Donnelly, S. G., Del Negro, L. A., Fahey, D. W., McKeen, S. A., Salawitch, R. J., Webster, C. R., May, R. D., Herman, R. L., Proffitt, M. H., Margitan, J. J., Atlas, E. L., Schauffler, S. M., Flocke, F., McElroy, C. T., and Bui, T. P.: Hydrogen radicals, nitrogen radicals and the production of O3 in the upper troposphere, Science, 279, 49–53, https://doi.org/10.1126/science.279.5347.49, 1998.
Wesely, M. L.: Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models, Atmos. Environ., 23, 1293–1304, 1989.
World Meteorological Organization (WMO): Scientific Assessment of Ozone Depletion: 1998, Tech. rep., World Meteorological Organization, Geneva, Switzerland, 1999.
Yevich, R. and Logan, J. A.: An assessment of biofuel use and burning of agricultural waste in the developing world, Global Biogeochem. Cy., 17, 1095, https://doi.org/10.1029/2002GB001952, 2003.
Yienger, J. J. and Levy, H.: Empirical model of global soil-biogenic NOx emissions, J. Geophys. Res., 100, 11447–11464, 1995.
Zhang, Q., Streets, D. G., Carmichael, G. R., He, K. B., Huo, H., Kannari, A., Klimont, Z., Park, I. S., Reddy, S., Fu, J. S., Chen, D., Duan, L., Lei, Y., Wang, L. T., and Yao, Z. L.: Asian emissions in 2006 for the NASA INTEX-B mission, Atmos. Chem. Phys., 9, 5131–5153, https://doi.org/10.5194/acp-9-5131-2009, 2009.
Zhang, R., Tie, X., and Bond, D. W.: Impacts of anthropogenic and natural NOx sources over the U.S. on tropospheric chemistry, P. Natl. Acad. Sci. USA, 100, 1505–1509, 2003.
Short summary
In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into the grid. A plume-in-grid parameterization to account for the sub-grid chemistry of LNOx is presented. This approach was implemented into the GEOS-Chem model and leads to a relative increase of NOx and O3 (18 % and 2 %, respectively, in July) on a large scale downwind of lightning emissions and a relative decrease (25 % and 8 %, respectively, over central Africa in July) over the regions of emissions.
In chemical transport models, NOx emitted by lightning (LNOx) is instantaneously diluted into...
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