Articles | Volume 18, issue 21
https://doi.org/10.5194/acp-18-15743-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-15743-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Simulating secondary organic aerosol from anthropogenic and biogenic precursors: comparison to outdoor chamber experiments, effect of oligomerization on SOA formation and reactive uptake of aldehydes
Florian Couvidat
CORRESPONDING AUTHOR
Institut National de l'Environnement Industriel et des Risques, Verneuil-en-Halatte, France
Marta G. Vivanco
Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas (CIEMAT), Departamento de Medio Ambiente,
Av. Complutense 40, 28040-Madrid, Spain
Bertrand Bessagnet
Institut National de l'Environnement Industriel et des Risques, Verneuil-en-Halatte, France
now at: Hangzhou Futuris Environmental Technology Co. Ltd, Zhejiang Overseas High-Level
Talent Innovation Park, No. 998 WenYi Road, 311121, Hangzhou, Zhejiang, China
Related authors
Aurélien Le Bayon, Aliisa Ojala, Siddharth Iyer, Zhizhao Wang, Victor Lannuque, Florian Couvidat, Raluca Ciuraru, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2026-3391, https://doi.org/10.5194/egusphere-2026-3391, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Aromatics compounds emitted in the atmosphere, such as benzene and phenol, contribute to the formation of organic aerosols. This study presents and evaluates an updated description of benzene chemistry, in which the most influential pathways are identified, including one developed in this work. The resulting mechanism reproduces laboratory observation with great accuracy and is reduced for use in large-scale air quality models.
Karine Sartelet, Zhizhao Wang, Youngseob Kim, Victor Lannuque, and Florian Couvidat
Geosci. Model Dev., 19, 389–421, https://doi.org/10.5194/gmd-19-389-2026, https://doi.org/10.5194/gmd-19-389-2026, 2026
Short summary
Short summary
The model simulates the evolution of primary and secondary pollutants via gas-phase chemistry, aerosol dynamics (including ultrafine particles), and intra-particle reactions. It uses a sectional approach for size and composition, includes a wall-loss module, and links gas-phase mechanisms of different complexity to secondary organic aerosol formation. Representation of particle phase composition allows viscosity and non-ideality to be taken into account.
Marc Guevara, Augustin Colette, Antoine Guion, Valentin Petiot, Mario Adani, Joaquim Arteta, Anna Benedictow, Robert Bergström, Andrea Bolignano, Paula Camps, Ana C. Carvalho, Jesper Heile Christensen, Florian Couvidat, Ilaria D'Elia, Hugo Denier van der Gon, Gaël Descombes, John Douros, Hilde Fagerli, Yalda Fatahi, Elmar Friese, Lise Frohn, Michael Gauss, Camilla Geels, Risto Hänninen, Kaj Hansen, Oriol Jorba, Jacek W. Kaminski, Rostislav Kouznetsov, Richard Kranenburg, Jeroen Kuenen, Victor Lannuque, Frédérik Meleux, Agnes Nyíri, Yuliia Palamarchuk, Carlos Pérez García-Pando, Lennard Robertson, Felicita Russo, Arjo Segers, Mikhail Sofiev, Joanna Struzewska, Renske Timmermans, Andreas Uppstu, Alvaro Valdebenito, and Zhuyun Ye
Atmos. Chem. Phys., 25, 13245–13278, https://doi.org/10.5194/acp-25-13245-2025, https://doi.org/10.5194/acp-25-13245-2025, 2025
Short summary
Short summary
Air quality models require hourly emissions to accurately represent dispersion and physico-chemical processes in the atmosphere. Since emission inventories are typically provided at the annual level, emissions are downscaled to a refined temporal resolution using temporal profiles. This study quantifies the impact of using new anthropogenic temporal profiles on the performance of an European air quality multi-model ensemble. Overall, the findings indicate an improvement of the modelling results.
Augustin Colette, Gaëlle Collin, François Besson, Etienne Blot, Vincent Guidard, Frédérik Meleux, Adrien Royer, Valentin Petiot, Claire Miller, Oihana Fermond, Alizé Jeant, Mario Adani, Joaquim Arteta, Anna Benedictow, Robert Bergström, Dene Bowdalo, Jorgen Brandt, Gino Briganti, Ana C. Carvalho, Jesper Heile Christensen, Florian Couvidat, Ilaria D'Elia, Massimo D'Isidoro, Hugo Denier van der Gon, Gaël Descombes, Enza Di Tomaso, John Douros, Jeronimo Escribano, Henk Eskes, Hilde Fagerli, Yalda Fatahi, Johannes Flemming, Elmar Friese, Lise Frohn, Michael Gauss, Camilla Geels, Guido Guarnieri, Marc Guevara, Antoine Guion, Jonathan Guth, Risto Hänninen, Kaj Hansen, Ulas Im, Ruud Janssen, Marine Jeoffrion, Mathieu Joly, Luke Jones, Oriol Jorba, Evgeni Kadantsev, Michael Kahnert, Jacek W. Kaminski, Rostislav Kouznetsov, Richard Kranenburg, Jeroen Kuenen, Anne Caroline Lange, Joachim Langner, Victor Lannuque, Francesca Macchia, Astrid Manders, Mihaela Mircea, Agnes Nyiri, Miriam Olid, Carlos Pérez García-Pando, Yuliia Palamarchuk, Antonio Piersanti, Blandine Raux, Miha Razinger, Lennard Robertson, Arjo Segers, Martijn Schaap, Pilvi Siljamo, David Simpson, Mikhail Sofiev, Anders Stangel, Joanna Struzewska, Carles Tena, Renske Timmermans, Thanos Tsikerdekis, Svetlana Tsyro, Svyatoslav Tyuryakov, Anthony Ung, Andreas Uppstu, Alvaro Valdebenito, Peter van Velthoven, Lina Vitali, Zhuyun Ye, Vincent-Henri Peuch, and Laurence Rouïl
Geosci. Model Dev., 18, 6835–6883, https://doi.org/10.5194/gmd-18-6835-2025, https://doi.org/10.5194/gmd-18-6835-2025, 2025
Short summary
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The Copernicus Atmosphere Monitoring Service – Regional Production delivers daily forecasts, analyses, and reanalyses of air quality in Europe. The service relies on a distributed modelling production by 11 leading European modelling teams following stringent requirements with an operational design that has no equivalent in the world. All the products are free, open, and quality-assured and disseminated with a high level of reliability.
Hanrui Lang, Yunjiang Zhang, Sheng Zhong, Yongcai Rao, Minfeng Zhou, Jian Qiu, Jingyi Li, Diwen Liu, Florian Couvidat, Olivier Favez, Didier Hauglustaine, and Xinlei Ge
Atmos. Chem. Phys., 25, 10587–10601, https://doi.org/10.5194/acp-25-10587-2025, https://doi.org/10.5194/acp-25-10587-2025, 2025
Short summary
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This study investigates how dust pollution influences particulate nitrate formation. We found that dust pollution could reduce the effectiveness of ammonia emission controls by altering aerosol chemistry. Using field observations and modeling, we showed that dust particles affect nitrate distribution between gas and particle phases. Our findings highlight the need for pollution control strategies that consider both human emissions and dust sources for better urban air quality management.
Antoine Guion, Florian Couvidat, Marc Guevara, and Augustin Colette
Atmos. Chem. Phys., 25, 2807–2827, https://doi.org/10.5194/acp-25-2807-2025, https://doi.org/10.5194/acp-25-2807-2025, 2025
Short summary
Short summary
The residential sector can cause high background levels of pollutants and pollution peaks in winter. Its emissions are dominated by space heating and show strong daily variations linked to changes in outside temperature. Using heating degree days, we provide country- and species-dependent parameters for the distribution of these emissions, improving the performance of the CHIMERE air quality model. This also allows annual residential emissions to be projected before official publications.
Hasna Chebaicheb, Joel F. de Brito, Tanguy Amodeo, Florian Couvidat, Jean-Eudes Petit, Emmanuel Tison, Gregory Abbou, Alexia Baudic, Mélodie Chatain, Benjamin Chazeau, Nicolas Marchand, Raphaële Falhun, Florie Francony, Cyril Ratier, Didier Grenier, Romain Vidaud, Shouwen Zhang, Gregory Gille, Laurent Meunier, Caroline Marchand, Véronique Riffault, and Olivier Favez
Earth Syst. Sci. Data, 16, 5089–5109, https://doi.org/10.5194/essd-16-5089-2024, https://doi.org/10.5194/essd-16-5089-2024, 2024
Short summary
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Long-term (2015–2021) quasi-continuous measurements have been obtained at 13 French urban sites using online mass spectrometry, to acquire the comprehensive chemical composition of submicron particulate matter. The results show their spatial and temporal differences and confirm the predominance of organics in France (40–60 %). These measurements can be used for many future studies, such as trend and epidemiological analyses, or comparisons with chemical transport models.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
Short summary
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Rémy Lapere, Nicolás Huneeus, Sylvain Mailler, Laurent Menut, and Florian Couvidat
Atmos. Chem. Phys., 23, 1749–1768, https://doi.org/10.5194/acp-23-1749-2023, https://doi.org/10.5194/acp-23-1749-2023, 2023
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Glaciers in the Andes of central Chile are shrinking rapidly in response to global warming. This melting is accelerated by the deposition of opaque particles onto snow and ice. In this work, model simulations quantify typical deposition rates of soot on glaciers in summer and winter months and show that the contribution of emissions from Santiago is not as high as anticipated. Additionally, the combination of regional- and local-scale meteorology explains the seasonality in deposition.
Zhizhao Wang, Florian Couvidat, and Karine Sartelet
Geosci. Model Dev., 15, 8957–8982, https://doi.org/10.5194/gmd-15-8957-2022, https://doi.org/10.5194/gmd-15-8957-2022, 2022
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Air quality models need to reliably predict secondary organic aerosols (SOAs) at a reasonable computational cost. Thus, we developed GENOA v1.0, a mechanism reduction algorithm that preserves the accuracy of detailed gas-phase chemical mechanisms for SOA formation, thereby improving the practical use of actual chemistry in SOA models. With GENOA, a near-explicit chemical scheme was reduced to 2 % of its original size and computational time, with an average error of less than 3 %.
Karine Sartelet, Youngseob Kim, Florian Couvidat, Maik Merkel, Tuukka Petäjä, Jean Sciare, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 8579–8596, https://doi.org/10.5194/acp-22-8579-2022, https://doi.org/10.5194/acp-22-8579-2022, 2022
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A methodology is defined to estimate number emissions from an inventory providing mass emissions. Number concentrations are simulated over Greater Paris using different nucleation parameterisations (binary, ternary involving sulfuric acid and ammonia, and heteromolecular involving sulfuric acid and extremely low-volatility organics, ELVOCs). The comparisons show that ternary nucleation may not be a dominant process for new particle formation in cities, but they stress the role of ELVOCs.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
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Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Elsa Real, Florian Couvidat, Anthony Ung, Laure Malherbe, Blandine Raux, Alicia Gressent, and Augustin Colette
Earth Syst. Sci. Data, 14, 2419–2443, https://doi.org/10.5194/essd-14-2419-2022, https://doi.org/10.5194/essd-14-2419-2022, 2022
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This paper describes a 16-year (2000–2015) dataset of air pollution concentrations and air quality indicators over France combining background measurements and modeling. Hourly concentrations and regulatory indicators of NO2, O3, PM10 and PM2.5 are produced with 4 km spatial resolution. The overall dataset has been cross-validated and showed overall very good results. We hope that this open-access publication will facilitate further studies on the impacts of air pollution.
Laurent Menut, Bertrand Bessagnet, Régis Briant, Arineh Cholakian, Florian Couvidat, Sylvain Mailler, Romain Pennel, Guillaume Siour, Paolo Tuccella, Solène Turquety, and Myrto Valari
Geosci. Model Dev., 14, 6781–6811, https://doi.org/10.5194/gmd-14-6781-2021, https://doi.org/10.5194/gmd-14-6781-2021, 2021
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The CHIMERE chemistry-transport model is presented in its new version, V2020r1. Many changes are proposed compared to the previous version. These include online modeling, new parameterizations for aerosols, new emissions schemes, a new parameter file format, the subgrid-scale variability of urban concentrations and new transport schemes.
Aurélien Le Bayon, Aliisa Ojala, Siddharth Iyer, Zhizhao Wang, Victor Lannuque, Florian Couvidat, Raluca Ciuraru, and Karine Sartelet
EGUsphere, https://doi.org/10.5194/egusphere-2026-3391, https://doi.org/10.5194/egusphere-2026-3391, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Aromatics compounds emitted in the atmosphere, such as benzene and phenol, contribute to the formation of organic aerosols. This study presents and evaluates an updated description of benzene chemistry, in which the most influential pathways are identified, including one developed in this work. The resulting mechanism reproduces laboratory observation with great accuracy and is reduced for use in large-scale air quality models.
Tim Butler, Tabish Ansari, Claudio A. Belis, Elisa Bergas-Masso, Willem van Caspel, Hilde Fagerli, Johannes Flemming, Marta Garcia Vivanco, Paul Griffiths, Douglas S. Hamilton, Coralina Hernandez Trujillo, Lena Höglund-Isaksson, Vincent Huijnen, Matthew Kasoar, Johannes W. Kaiser, Gerbrand Koren, Zbigniew Klimont, Florian Lindl, Aura Lupascu, Mariano Mertens, Martijn Schaap, Steven T. Turnock, Oliver Wild, Philipp Weiss, Jacek Kaminski, Rosa Wu, and Terry Keating
EGUsphere, https://doi.org/10.5194/egusphere-2026-1367, https://doi.org/10.5194/egusphere-2026-1367, 2026
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Air pollution travels across continents, meaning emissions in one region can affect air quality far away. To better understand this, scientists from many groups are planning to run coordinated computer simulations of the atmosphere. By comparing results across models and emission scenarios, the planned study will show how pollution moves between regions and which sources matter most, helping governments design more effective air quality policies.
Karine Sartelet, Zhizhao Wang, Youngseob Kim, Victor Lannuque, and Florian Couvidat
Geosci. Model Dev., 19, 389–421, https://doi.org/10.5194/gmd-19-389-2026, https://doi.org/10.5194/gmd-19-389-2026, 2026
Short summary
Short summary
The model simulates the evolution of primary and secondary pollutants via gas-phase chemistry, aerosol dynamics (including ultrafine particles), and intra-particle reactions. It uses a sectional approach for size and composition, includes a wall-loss module, and links gas-phase mechanisms of different complexity to secondary organic aerosol formation. Representation of particle phase composition allows viscosity and non-ideality to be taken into account.
Bertrand Bessagnet, Narayan Thapa, Dikra Prasad Bajgai, Ravi Sahu, Arshini Saikia, Arineh Cholakian, Laurent Menut, Guillaume Siour, Tenzin Wangchuk, Monica Crippa, and Kamala Gurung
Atmos. Chem. Phys., 25, 18675–18696, https://doi.org/10.5194/acp-25-18675-2025, https://doi.org/10.5194/acp-25-18675-2025, 2025
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This study highlights the use of numerical tools at very high resolution to support the Air Quality monitoring strategy in the Himalayan valley which suffer from Air Pollution. For the first time ever, a high resolution simulation is performed in Bhutan showing the high PM2.5 concentrations within the valleys and potential contaminations up to the glaciers enhancing climate related risks.
Marc Guevara, Augustin Colette, Antoine Guion, Valentin Petiot, Mario Adani, Joaquim Arteta, Anna Benedictow, Robert Bergström, Andrea Bolignano, Paula Camps, Ana C. Carvalho, Jesper Heile Christensen, Florian Couvidat, Ilaria D'Elia, Hugo Denier van der Gon, Gaël Descombes, John Douros, Hilde Fagerli, Yalda Fatahi, Elmar Friese, Lise Frohn, Michael Gauss, Camilla Geels, Risto Hänninen, Kaj Hansen, Oriol Jorba, Jacek W. Kaminski, Rostislav Kouznetsov, Richard Kranenburg, Jeroen Kuenen, Victor Lannuque, Frédérik Meleux, Agnes Nyíri, Yuliia Palamarchuk, Carlos Pérez García-Pando, Lennard Robertson, Felicita Russo, Arjo Segers, Mikhail Sofiev, Joanna Struzewska, Renske Timmermans, Andreas Uppstu, Alvaro Valdebenito, and Zhuyun Ye
Atmos. Chem. Phys., 25, 13245–13278, https://doi.org/10.5194/acp-25-13245-2025, https://doi.org/10.5194/acp-25-13245-2025, 2025
Short summary
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Air quality models require hourly emissions to accurately represent dispersion and physico-chemical processes in the atmosphere. Since emission inventories are typically provided at the annual level, emissions are downscaled to a refined temporal resolution using temporal profiles. This study quantifies the impact of using new anthropogenic temporal profiles on the performance of an European air quality multi-model ensemble. Overall, the findings indicate an improvement of the modelling results.
Augustin Colette, Gaëlle Collin, François Besson, Etienne Blot, Vincent Guidard, Frédérik Meleux, Adrien Royer, Valentin Petiot, Claire Miller, Oihana Fermond, Alizé Jeant, Mario Adani, Joaquim Arteta, Anna Benedictow, Robert Bergström, Dene Bowdalo, Jorgen Brandt, Gino Briganti, Ana C. Carvalho, Jesper Heile Christensen, Florian Couvidat, Ilaria D'Elia, Massimo D'Isidoro, Hugo Denier van der Gon, Gaël Descombes, Enza Di Tomaso, John Douros, Jeronimo Escribano, Henk Eskes, Hilde Fagerli, Yalda Fatahi, Johannes Flemming, Elmar Friese, Lise Frohn, Michael Gauss, Camilla Geels, Guido Guarnieri, Marc Guevara, Antoine Guion, Jonathan Guth, Risto Hänninen, Kaj Hansen, Ulas Im, Ruud Janssen, Marine Jeoffrion, Mathieu Joly, Luke Jones, Oriol Jorba, Evgeni Kadantsev, Michael Kahnert, Jacek W. Kaminski, Rostislav Kouznetsov, Richard Kranenburg, Jeroen Kuenen, Anne Caroline Lange, Joachim Langner, Victor Lannuque, Francesca Macchia, Astrid Manders, Mihaela Mircea, Agnes Nyiri, Miriam Olid, Carlos Pérez García-Pando, Yuliia Palamarchuk, Antonio Piersanti, Blandine Raux, Miha Razinger, Lennard Robertson, Arjo Segers, Martijn Schaap, Pilvi Siljamo, David Simpson, Mikhail Sofiev, Anders Stangel, Joanna Struzewska, Carles Tena, Renske Timmermans, Thanos Tsikerdekis, Svetlana Tsyro, Svyatoslav Tyuryakov, Anthony Ung, Andreas Uppstu, Alvaro Valdebenito, Peter van Velthoven, Lina Vitali, Zhuyun Ye, Vincent-Henri Peuch, and Laurence Rouïl
Geosci. Model Dev., 18, 6835–6883, https://doi.org/10.5194/gmd-18-6835-2025, https://doi.org/10.5194/gmd-18-6835-2025, 2025
Short summary
Short summary
The Copernicus Atmosphere Monitoring Service – Regional Production delivers daily forecasts, analyses, and reanalyses of air quality in Europe. The service relies on a distributed modelling production by 11 leading European modelling teams following stringent requirements with an operational design that has no equivalent in the world. All the products are free, open, and quality-assured and disseminated with a high level of reliability.
Hanrui Lang, Yunjiang Zhang, Sheng Zhong, Yongcai Rao, Minfeng Zhou, Jian Qiu, Jingyi Li, Diwen Liu, Florian Couvidat, Olivier Favez, Didier Hauglustaine, and Xinlei Ge
Atmos. Chem. Phys., 25, 10587–10601, https://doi.org/10.5194/acp-25-10587-2025, https://doi.org/10.5194/acp-25-10587-2025, 2025
Short summary
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This study investigates how dust pollution influences particulate nitrate formation. We found that dust pollution could reduce the effectiveness of ammonia emission controls by altering aerosol chemistry. Using field observations and modeling, we showed that dust particles affect nitrate distribution between gas and particle phases. Our findings highlight the need for pollution control strategies that consider both human emissions and dust sources for better urban air quality management.
Antoine Guion, Florian Couvidat, Marc Guevara, and Augustin Colette
Atmos. Chem. Phys., 25, 2807–2827, https://doi.org/10.5194/acp-25-2807-2025, https://doi.org/10.5194/acp-25-2807-2025, 2025
Short summary
Short summary
The residential sector can cause high background levels of pollutants and pollution peaks in winter. Its emissions are dominated by space heating and show strong daily variations linked to changes in outside temperature. Using heating degree days, we provide country- and species-dependent parameters for the distribution of these emissions, improving the performance of the CHIMERE air quality model. This also allows annual residential emissions to be projected before official publications.
Hasna Chebaicheb, Joel F. de Brito, Tanguy Amodeo, Florian Couvidat, Jean-Eudes Petit, Emmanuel Tison, Gregory Abbou, Alexia Baudic, Mélodie Chatain, Benjamin Chazeau, Nicolas Marchand, Raphaële Falhun, Florie Francony, Cyril Ratier, Didier Grenier, Romain Vidaud, Shouwen Zhang, Gregory Gille, Laurent Meunier, Caroline Marchand, Véronique Riffault, and Olivier Favez
Earth Syst. Sci. Data, 16, 5089–5109, https://doi.org/10.5194/essd-16-5089-2024, https://doi.org/10.5194/essd-16-5089-2024, 2024
Short summary
Short summary
Long-term (2015–2021) quasi-continuous measurements have been obtained at 13 French urban sites using online mass spectrometry, to acquire the comprehensive chemical composition of submicron particulate matter. The results show their spatial and temporal differences and confirm the predominance of organics in France (40–60 %). These measurements can be used for many future studies, such as trend and epidemiological analyses, or comparisons with chemical transport models.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Philippe Thunis, Jeroen Kuenen, Enrico Pisoni, Bertrand Bessagnet, Manjola Banja, Lech Gawuc, Karol Szymankiewicz, Diego Guizardi, Monica Crippa, Susana Lopez-Aparicio, Marc Guevara, Alexander De Meij, Sabine Schindlbacher, and Alain Clappier
Geosci. Model Dev., 17, 3631–3643, https://doi.org/10.5194/gmd-17-3631-2024, https://doi.org/10.5194/gmd-17-3631-2024, 2024
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An ensemble emission inventory is created with the aim of monitoring the status and progress made with the development of EU-wide inventories. This emission ensemble serves as a common benchmark for the screening and allows for the comparison of more than two inventories at a time. Because the emission “truth” is unknown, the approach does not tell which inventory is the closest to reality, but it identifies inconsistencies that require special attention.
Laurent Menut, Bertrand Bessagnet, Arineh Cholakian, Guillaume Siour, Sylvain Mailler, and Romain Pennel
Geosci. Model Dev., 17, 3645–3665, https://doi.org/10.5194/gmd-17-3645-2024, https://doi.org/10.5194/gmd-17-3645-2024, 2024
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This study is about the modelling of the atmospheric composition in Europe during the summer of 2022, when massive wildfires were observed. It is a sensitivity study dedicated to the relative impacts of two modelling processes that are able to modify the meteorology used for the calculation of the atmospheric chemistry and transport of pollutants.
Alexander de Meij, Cornelis Cuvelier, Philippe Thunis, Enrico Pisoni, and Bertrand Bessagnet
Geosci. Model Dev., 17, 587–606, https://doi.org/10.5194/gmd-17-587-2024, https://doi.org/10.5194/gmd-17-587-2024, 2024
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In our study the robustness of the model responses to emission reductions in the EU is assessed when the emission data are changed. Our findings are particularly important to better understand the uncertainties associated to the emission inventories and how these uncertainties impact the level of accuracy of the resulting air quality modelling, which is a key for designing air quality plans. Also crucial is the choice of indicator to avoid misleading interpretations of the results.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Laurent Menut, Arineh Cholakian, Guillaume Siour, Rémy Lapere, Romain Pennel, Sylvain Mailler, and Bertrand Bessagnet
Atmos. Chem. Phys., 23, 7281–7296, https://doi.org/10.5194/acp-23-7281-2023, https://doi.org/10.5194/acp-23-7281-2023, 2023
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This study is about the wildfires occurring in France during the summer 2022. We study the forest fires that took place in the Landes during the summer of 2022. We show the direct impact of these fires on the air quality, especially downstream of the smoke plume towards the Paris region. We quantify the impact of these fires on the pollutants peak concentrations and the possible exceedance of thresholds.
Rémy Lapere, Nicolás Huneeus, Sylvain Mailler, Laurent Menut, and Florian Couvidat
Atmos. Chem. Phys., 23, 1749–1768, https://doi.org/10.5194/acp-23-1749-2023, https://doi.org/10.5194/acp-23-1749-2023, 2023
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Glaciers in the Andes of central Chile are shrinking rapidly in response to global warming. This melting is accelerated by the deposition of opaque particles onto snow and ice. In this work, model simulations quantify typical deposition rates of soot on glaciers in summer and winter months and show that the contribution of emissions from Santiago is not as high as anticipated. Additionally, the combination of regional- and local-scale meteorology explains the seasonality in deposition.
Zhizhao Wang, Florian Couvidat, and Karine Sartelet
Geosci. Model Dev., 15, 8957–8982, https://doi.org/10.5194/gmd-15-8957-2022, https://doi.org/10.5194/gmd-15-8957-2022, 2022
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Air quality models need to reliably predict secondary organic aerosols (SOAs) at a reasonable computational cost. Thus, we developed GENOA v1.0, a mechanism reduction algorithm that preserves the accuracy of detailed gas-phase chemical mechanisms for SOA formation, thereby improving the practical use of actual chemistry in SOA models. With GENOA, a near-explicit chemical scheme was reduced to 2 % of its original size and computational time, with an average error of less than 3 %.
Philippe Thunis, Alain Clappier, Enrico Pisoni, Bertrand Bessagnet, Jeroen Kuenen, Marc Guevara, and Susana Lopez-Aparicio
Geosci. Model Dev., 15, 5271–5286, https://doi.org/10.5194/gmd-15-5271-2022, https://doi.org/10.5194/gmd-15-5271-2022, 2022
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In this work, we propose a screening method to improve the quality of emission inventories, which are responsible for large uncertainties in air-quality modeling. The first step of screening consists of keeping only emission contributions that are relevant enough. In a second step, the method identifies large differences that provide evidence of methodological divergence or errors. We used the approach to compare two versions of the CAMS-REG European-scale inventory over 150 European cities.
Karine Sartelet, Youngseob Kim, Florian Couvidat, Maik Merkel, Tuukka Petäjä, Jean Sciare, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 8579–8596, https://doi.org/10.5194/acp-22-8579-2022, https://doi.org/10.5194/acp-22-8579-2022, 2022
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A methodology is defined to estimate number emissions from an inventory providing mass emissions. Number concentrations are simulated over Greater Paris using different nucleation parameterisations (binary, ternary involving sulfuric acid and ammonia, and heteromolecular involving sulfuric acid and extremely low-volatility organics, ELVOCs). The comparisons show that ternary nucleation may not be a dominant process for new particle formation in cities, but they stress the role of ELVOCs.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
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Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Elsa Real, Florian Couvidat, Anthony Ung, Laure Malherbe, Blandine Raux, Alicia Gressent, and Augustin Colette
Earth Syst. Sci. Data, 14, 2419–2443, https://doi.org/10.5194/essd-14-2419-2022, https://doi.org/10.5194/essd-14-2419-2022, 2022
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This paper describes a 16-year (2000–2015) dataset of air pollution concentrations and air quality indicators over France combining background measurements and modeling. Hourly concentrations and regulatory indicators of NO2, O3, PM10 and PM2.5 are produced with 4 km spatial resolution. The overall dataset has been cross-validated and showed overall very good results. We hope that this open-access publication will facilitate further studies on the impacts of air pollution.
Juan Cuesta, Lorenzo Costantino, Matthias Beekmann, Guillaume Siour, Laurent Menut, Bertrand Bessagnet, Tony C. Landi, Gaëlle Dufour, and Maxim Eremenko
Atmos. Chem. Phys., 22, 4471–4489, https://doi.org/10.5194/acp-22-4471-2022, https://doi.org/10.5194/acp-22-4471-2022, 2022
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We present the first comprehensive study integrating satellite observations of near-surface ozone pollution, surface in situ measurements, and a chemistry-transport model for quantifying the role of anthropogenic emission reductions during the COVID-19 lockdown in spring 2020. It confirms the occurrence of a net enhancement of ozone in central Europe and a reduction elsewhere, except for some hotspots, linked with the reduction of precursor emissions from Europe and the Northern Hemisphere.
Philippe Thunis, Alain Clappier, Alexander de Meij, Enrico Pisoni, Bertrand Bessagnet, and Leonor Tarrason
Atmos. Chem. Phys., 21, 18195–18212, https://doi.org/10.5194/acp-21-18195-2021, https://doi.org/10.5194/acp-21-18195-2021, 2021
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Air pollution's origin in cities is still a point of discussion, and approaches to assess the city's responsibility for its pollution are not harmonized and thus not comparable, resulting in sometimes contradicting interpretations. We show that methodological choices can easily lead to differences of a factor of 2 in terms of responsibility outcome and stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility.
Laurent Menut, Bertrand Bessagnet, Régis Briant, Arineh Cholakian, Florian Couvidat, Sylvain Mailler, Romain Pennel, Guillaume Siour, Paolo Tuccella, Solène Turquety, and Myrto Valari
Geosci. Model Dev., 14, 6781–6811, https://doi.org/10.5194/gmd-14-6781-2021, https://doi.org/10.5194/gmd-14-6781-2021, 2021
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The CHIMERE chemistry-transport model is presented in its new version, V2020r1. Many changes are proposed compared to the previous version. These include online modeling, new parameterizations for aerosols, new emissions schemes, a new parameter file format, the subgrid-scale variability of urban concentrations and new transport schemes.
Gaëlle Dufour, Didier Hauglustaine, Yunjiang Zhang, Maxim Eremenko, Yann Cohen, Audrey Gaudel, Guillaume Siour, Mathieu Lachatre, Axel Bense, Bertrand Bessagnet, Juan Cuesta, Jerry Ziemke, Valérie Thouret, and Bo Zheng
Atmos. Chem. Phys., 21, 16001–16025, https://doi.org/10.5194/acp-21-16001-2021, https://doi.org/10.5194/acp-21-16001-2021, 2021
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The IASI observations and the LMDZ-OR-INCA model simulations show negative ozone trends in the Central East China region in the lower free (3–6 km column) and the upper free (6–9 km column) troposphere. Sensitivity studies from the model show that the Chinese anthropogenic emissions contribute to more than 50 % in the trend. The reduction in NOx emissions that has occurred since 2013 in China seems to lead to a decrease in ozone in the free troposphere, contrary to the increase at the surface.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Cited articles
Bian, Q., May, A. A., Kreidenweis, S. M., and Pierce, J. R.: Investigation of particle and vapor wall-loss effects on controlled wood-smoke smog-chamber experiments, Atmos. Chem. Phys., 15, 11027–11045, https://doi.org/10.5194/acp-15-11027-2015, 2015.
Cappa, C. D., Jathar, S. H., Kleeman, M. J., Docherty, K. S., Jimenez, J. L., Seinfeld, J. H., and Wexler, A. S.: Simulating secondary organic aerosol in a regional air quality model using the statistical oxidation model – Part 2: Assessing the influence of vapor wall losses, Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, 2016.
Carlton, A. G., Bhave, P. V., Napelenok, S. L., Edney, E. O., Sarwar, G., Pinder, R. W., Pouliot, G. A., and Houyoux, M.: Model Representation of Secondary Organic Aerosol in CMAQv4.7, Environ. Sci. Tech., 44, 8553–8560, https://doi.org/10.1021/es100636q, 2010.
Chacon-Madrid, H. J., Henry, K. M., and Donahue, N. M.: Photo-oxidation of pinonaldehyde at low NOx: from chemistry to organic aerosol formation, Atmos. Chem. Phys., 13, 3227–3236, https://doi.org/10.5194/acp-13-3227-2013, 2013.
Cocker III, D. R., Mader, B. T., Kalberer, M., Flagan, R. C., and Seinfeld, J. H.: The effect of water on gas-particle partitioning of secondary organic aerosol: II. m-xylene and 1,3,5-trimethylbenzene photooxidation systems, Atmos. Environ., 35, 6073–6085, https://doi.org/10.1016/S1352-2310(01)00405-8, 2001.
Couvidat, F. and Sartelet, K.: The Secondary Organic Aerosol Processor (SOAP v1.0) model: a unified model with different ranges of complexity based on the molecular surrogate approach, Geosci. Model Dev., 8, 1111–1138, https://doi.org/10.5194/gmd-8-1111-2015, 2015.
Couvidat, F. and Seigneur, C.: Modeling secondary organic aerosol formation from isoprene oxidation under dry and humid conditions, Atmos. Chem. Phys., 11, 893–909, https://doi.org/10.5194/acp-11-893-2011, 2011.
Couvidat, F., Debry, É., Sartelet, K., and Seigneur, C.: A Hydrophilic/Hydrophobic Organic (H2O) model: Model development, evaluation and sensitivity analysis, J. Geophys. Res., 117, D10304, https://doi.org/10.1029/2011JD017214, 2012.
Couvidat, F., Bessagnet, B., Garcia-Vivanco, M., Real, E., Menut, L., and Colette, A.: Development of an inorganic and organic aerosol model (CHIMERE 2017β v1.0): seasonal and spatial evaluation over Europe, Geosci. Model Dev., 11, 165–194, https://doi.org/10.5194/gmd-11-165-2018, 2018.
DePalma, J. W., Horan, A. J., Hall IV, W. A., and Johnston, M. V.: Thermodynamics of oligomer formation: implications for secondary organic aerosol formation and reactivity, Phys. Chem. Chem. Phys., 15, 6935–6944, https://doi.org/10.1039/C3cp44586k, 2013.
Donahue, N. M., Robinson, A. L., Stanier, C. O., and Pandis, S. N.: Coupled Partitioning, Dilution, and Chemical Aging of Semivolatile Organics, Environ. Sci. Technol., 40, 2635–2643, https://doi.org/10.1021/es052297c, 2006.
Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, https://doi.org/10.5194/acp-11-3303-2011, 2011
Fountoukis, C. and Nenes, A.: ISORROPIA II: a computationally efficient thermodynamic equilibrium model for K+–Ca2+–Mg2+–NH+4–Na+–SO42−–NO3−–Cl−–H2O aerosols, Atmos. Chem. Phys., 7, 4639–4659, https://doi.org/10.5194/acp-7-4639-2007, 2007.
Fry, J. L., Draper, D. C., Barsanti, K. C., Smith, J. N., Ortega, J., Winkler, P. M., Lawler, M. J., Brown, S. S., Edwards, P. M., Cohen, R. C., and Lee, L.: Secondary Organic Aerosol Formation and Organic Nitrate Yield from NO3 Oxidation of Biogenic Hydrocarbons, Environ. Sci. Technol., 48, 11944–11953, https://doi.org/10.1021/es502204x, 2014.
Ganbavale, G., Zuend, A., Marcolli, C., and Peter, T.: Improved AIOMFAC model parameterisation of the temperature dependence of activity coefficients for aqueous organic mixtures, Atmos. Chem. Phys., 15, 447–493, https://doi.org/10.5194/acp-15-447-2015, 2015.
Gao, S., Keywood, M., Ng, N. L., Surratt, J., Varutbangkul, V., Bahreini, R., Flagan, R. C., and Seinfeld, J. H.: Low-Molecular-Weight and Oligomeric Components in Secondary Organic Aerosol from the Ozonolysis of Cycloalkenes and α-pinene, J. Phys. Chem. A, 108, 10147–10164, https://doi.org/10.1021/jp047466e, 2004a.
Gao, S., Ng, N. L., Keywood, M., Varutbangkul, V., Bahreini, R., Nenes, A., He, J., Yoo, K. Y., Beauchamp, J. L., Hodyss, R. P., Flagan, R. C., and Seinfeld, J. H.: Particle phase acidity and oligomer formation in secondary organic aerosol, Environ. Sci. Technol., 38, 6582–6589, https://doi.org/10.1021/es049125k, 2004b.
Goliff, W. S., Stockwell, W. R., and Lawson, C. V.: The Regional Atmospheric Chemistry Mechanism, Version 2, Atmos. Environ., 68, 174–185, 2013.
Griffin, R. J., Nguyen, K., Dabdub, D., and Seinfeld, J. H.: A coupled hydrophobic-hydrophilic model for predicting secondary organic aerosol formation, J. Atmos. Chem., 44, 171–190, https://doi.org/10.1023/A:1022436813699, 2003.
Hakola, H., Arey, J., Aschmann, S. M., and Atkinson, R.: Product formation from the gas-phase reactions of OH radicals and O3 with a series of monoterpenes, J. Atmos. Chem., 18, 75–102, https://doi.org/10.1007/BF00694375, 1994.
Hall IV, W. A. and Johnston, M. V.: Oligomer Content of α-Pinene Secondary Organic Aerosol, Aerosol Sci. Tech., 45, 37–45, https://doi.org/10.1080/02786826.2010.517580, 2011.
Hallquist, M., Wängberg, I., Ljungström, E., Barnes, I., and Becher, K.-H.: Aerosol and product yield from NO3 radical-initiated oxidation of selected monoterpenes, Environ. Sci. Technol., 33, 553–559, https://doi.org/10.1021/es980292s, 1999.
Han, Z., Xie, Z., Wang, G., Zhang, R., and Tao, J.: Modeling organic aerosols over east China using a volatility basis-set approach with aging mechanism in a regional air quality model, Atmos. Environ., 124, 186–198, https://doi.org/10.1016/j.atmosenv.2015.05.045, 2016.
Healy, R. M., Temine, B., Kuprovskyte, K., and Wenger, J. C.: Effect of Relative Humidity on Gas/Particle Partitioning and Aerosol Mass Yield in the Photooxidation of p-Xylene, Environ. Sci. Technol., 43, 1884–1889, https://doi.org/10.1021/es802404z, 2009.
Im, Y., Jang, M., and Beardsley, R. L.: Simulation of aromatic SOA formation using the lumping model integrated with explicit gas-phase kinetic mechanisms and aerosol-phase reactions, Atmos. Chem. Phys., 14, 4013–4027, https://doi.org/10.5194/acp-14-4013-2014, 2014.
Jathar, S. H., Cappa, C. D., Wexler, A. S., Seinfeld, J. H., and Kleeman, M. J.: Multi-generational oxidation model to simulate secondary organic aerosol in a 3-D air quality model, Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, 2015.
Jathar, S. H., Cappa, C. D., Wexler, A. S., Seinfeld, J. H., and Kleeman, M. J.: Simulating secondary organic aerosol in a regional air quality model using the statistical oxidation model – Part 1: Assessing the influence of constrained multi-generational ageing, Atmos. Chem. Phys., 16, 2309–2322, https://doi.org/10.5194/acp-16-2309-2016, 2016.
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.
Kalberer, M., Paulsen, D., Sax, M., Steinbacher, M., Dommen, J., Prevot, A. S. H., Fisseha, R., Weingartner, E., Frankevich, V., Zenobi, R., and Baltensperger, U.: Identification of Polymers as Major Components of Atmospheric Organic Aerosols, Science, 303, 1659–1662, https://doi.org/10.1126/science.1092185, 2004.
Kalberer, M., Sax, M., and Samburova, V.: Molecular size evolution of oligomers in organic aerosols collected in urban atmospheres and generated in a smog chamber, Environ. Sci. Technol., 40, 5917–5922, https://doi.org/10.1021/es0525760, 2006.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Keene, W. C., Pszenny, A. A. P., Maben, J. R., Stevenson, E., and Wall, A.: Closure evaluation of size-resolved aerosol pH in the New England coastal atmosphere during summer, J. Geophys. Res., 109, D23307, https://doi.org/10.1029/2004JD004801, 2004.
Kim, H., Liu, S., Russell, J. M., and Paulson, S. E.: Dependence of Real Refractive Indices on O : C, H : C and Mass Fragments of Secondary Organic Aerosol Generated from Ozonolysis and Photooxidation of Limonene and α-Pinene, Aerosol Sci. Tech., 48, 498–507, https://doi.org/10.1080/02786826.2014.893278, 2014.
Kim, Y., Sartelet, K., and Seigneur, C.: Comparison of two gas-phase chemical kinetic mechanisms of ozone formation over Europe, J. Atmos. Chem., 62, 82–119, https://doi.org/10.1007/s10874-009-9142-5, 2009.
Koo, B., Knipping, E., and Yarwood, G.: 1.5-Dimensional volatility basis set approach for modeling organic aerosol in CAMx and CMAQ, Atmos. Environ., 95, 158–164, https://doi.org/10.1016/j.atmosenv.2014.06.031, 2014.
Kristensen, K., Cui, T., Zhang, H., Gold, A., Glasius, M., and Surratt, J. D.: Dimers in α-pinene secondary organic aerosol: effect of hydroxyl radical, ozone, relative humidity and aerosol acidity, Atmos. Chem. Phys., 14, 4201–4218, https://doi.org/10.5194/acp-14-4201-2014, 2014.
Lane, T. E., Donahue, N. M., and Pandis, S. N.: Simulating secondary organic aerosol formation using the volatility basis-set approach in a chemical transport model, Atmos. Environ., 42, 7439–7451, https://doi.org/10.1016/j.atmosenv.2008.06.026, 2008.
Lee, B.-H., Pierce, J. R., Engelhart, G. J., and Pandis, S. N.: Volatility of secondary organic aerosol from the ozonolysis of monoterpenes, Atmos. Environ., 45, 2443–2452, https://doi.org/10.1016/j.atmosenv.2011.02.004, 2011.
Lemaire, V., Coll, I., Couvidat, F., Mouchel-Vallon, C., Seigneur, C., and Siour, G.: Oligomer formation in the troposphere: from experimental knowledge to 3-D modeling, Geosci. Model Dev., 9, 1361–1382, https://doi.org/10.5194/gmd-9-1361-2016, 2016.
Liggio, J. and Li, S.-M.: Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols, Geophys. Res. Lett., 33, L13808, https://doi.org/10.1029/2006GL026079, 2006a.
Liggio, J. and Li, S.-M.: Reactive uptake of pinonaldehyde on acidic aerosols, J. Geophys. Res., 111, 1111–1138, https://doi.org/10.1029/2005JD006978, 2006b.
Lim, Y. B. and Ziemann, P. J.: Products and Mechanism of Secondary Organic Aerosol Formation from Reactions of n-Alkanes with OH Radicals in the Presence of NOx, Environ. Sci. Technol., 39, 9229–9236, https://doi.org/10.1021/es051447g, 2005.
Ludwig, J. and Klemm, O.: Acidity of size-fractionated aerosol particles, Water Air Soil Poll., 49, 35–50, https://doi.org/10.1007/BF00279508, 1990.
Madon, R. J. and Iglesia, E.: Catalytic reaction rates in thermodynamically non-ideal systems, J. Mol. Catal. A-Chem., 163, 189–204, 2000.
McMurry, P. H. and Grosjean, D.: Gas and aerosol wall losses in Teflon film smog chambers, Environ. Sci. Technol., 19, 1176–1182, https://doi.org/10.1021/es00142a006, 1985.
Menut, L., Bessagnet, B., Khvorostyanov, D., Beekmann, M., Blond, N., Colette, A., Coll, I., Curci, G., Foret, G., Hodzic, A., Mailler, S., Meleux, F., Monge, J.-L., Pison, I., Siour, G., Turquety, S., Valari, M., Vautard, R., and Vivanco, M. G.: CHIMERE 2013: a model for regional atmospheric composition modelling, Geosci. Model Dev., 6, 981–1028, https://doi.org/10.5194/gmd-6-981-2013, 2013.
Müller, L., Reinnig, M.-C., Naumann, K. H., Saathoff, H., Mentel, T. F., Donahue, N. M., and Hoffmann, T.: Formation of 3-methyl-1,2,3-butanetricarboxylic acid via gas phase oxidation of pinonic acid – a mass spectrometric study of SOA aging, Atmos. Chem. Phys., 12, 1483–1496, https://doi.org/10.5194/acp-12-1483-2012, 2012.
Murphy, B. N. and Pandis, S. N.: Simulating the formation of semivolatile primary and secondary organic aerosol in a regional chemical transport model, Environ. Sci. Technol., 43, 4722–4728, https://doi.org/10.1021/es803168a, 2009.
Mutzel, A., Rodigast, M., Iinuma, Y., Böge, O., and Herrmann, H.: Monoterpene SOA – Contribution of first-generation oxidation products to formation and chemical composition, Atmos. Environ., 130, 136–144, https://doi.org/10.1016/j.atmosenv.2015.10.080, 2016.
Ng, N. L., Chhabra, P. S., Chan, A. W. H., Surratt, J. D., Kroll, J. H., Kwan, A. J., McCabe, D. C., Wennberg, P. O., Sorooshian, A., Murphy, S. M., Dalleska, N. F., Flagan, R. C., and Seinfeld, J. H.: Effect of NOx level on secondary organic aerosol (SOA) formation from the photooxidation of terpenes, Atmos. Chem. Phys., 7, 5159–5174, https://doi.org/10.5194/acp-7-5159-2007, 2007a.
Ng, N. L., Kroll, J. H., Chan, A. W. H., Chhabra, P. S., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from m-xylene, toluene, and benzene, Atmos. Chem. Phys., 7, 3909–3922, https://doi.org/10.5194/acp-7-3909-2007, 2007b.
Odum, J. R., Hoffmann, F., Bowman, D., Collins, D., Flagan, R. C., and Seinfeld, J. H.: Gas/particle partitioning and secondary organic aerosol yields, Environ. Sci. Technol., 30, 2580–2585, https://doi.org/10.1021/es950943+, 1996.
Pankow, J. F.: An absorption model of gas/particle partitioning of organic compounds in the atmosphere, Atmos. Environ., 28, 185–188, 1994.
Pun, B. K. and Seigneur, C.: Investigative modeling of new pathways for secondary organic aerosol formation, Atmos. Chem. Phys., 7, 2199–2216, https://doi.org/10.5194/acp-7-2199-2007, 2007.
Pun, B. K., Griffin, R. J., Seigneur, C., and Seinfeld, J. H.: Secondary organic aerosol. 2. Thermodynamic model for gas/particle partitioning of molecular constituents, J. Geophys. Res., 107, 4333, https://doi.org/10.1029/2001JD000542, 2002.
Pun, B. K., Seigneur, C., and Lohman, K.: Modeling secondary organic aerosol formation via multiphase partitioning with molecular data, Environ. Sci. Technol., 40, 4722–4731, https://doi.org/10.1021/es0522736, 2006.
Rahimpour, M. R.: A non-ideal rate-based model for industrial urea thermal hydrolyser, Chem. Eng. Process., 43, 1299–1307, https://doi.org/10.1016/j.cep.2003.12.005, 2004.
Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging, Science, 315, 1259–1262, https://doi.org/10.1126/science.1133061, 2007.
Roldin, P., Eriksson, A. C., Nordin, E. Z., Hermansson, E., Mogensen, D., Rusanen, A., Boy, M., Swietlicki, E., Svenningsson, B., Zelenyuk, A., and Pagels, J.: Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM, Atmos. Chem. Phys., 14, 7953–7993, https://doi.org/10.5194/acp-14-7953-2014, 2014.
Santiago, M., Garcia Vivanco, M., and Stein, A.: SO2 effect on secondary organic aerosol from a mixture of anthropogenic VOCs: experimental and modelled results, Int. J. Environ. Pollut., 50, 224–233, 2012a.
Santiago, M., Vivanco, M. G., and Stein, A. F.: Evaluation of CMAQ parameterizations for SOA formation from the photooxidation of alpha-pinene and limonene against smog chamber data, Atmos. Environ., 56, 236–245, https://doi.org/10.1016/j.atmosenv.2012.04.011, 2012b.
Sato, K., Takami, A., Kato, Y., Seta, T., Fujitani, Y., Hikida, T., Shimono, A., and Imamura, T.: AMS and LC/MS analyses of SOA from the photooxidation of benzene and 1,3,5-trimethylbenzene in the presence of NOx: effects of chemical structure on SOA aging, Atmos. Chem. Phys., 12, 4667–4682, https://doi.org/10.5194/acp-12-4667-2012, 2012.
Sato, K., Jia, T., Tanabe, K., Morino, Y., Yoshizumi Kajii, Y., and Imamura, T.: Terpenylic acid and nine-carbon multifunctional compounds formed during the aging of β-pinene ozonolysis secondary organic aerosol, Atmos. Environ., 130, 127–135, https://doi.org/10.1016/j.atmosenv.2015.08.047, 2016.
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.
Schell, B., Ackermann, I. J., Hass, H., Binkowski, F. S., and Ebel, A.: Modeling the formation of secondary organic aerosol within a comprehensive air quality model system, J. Geophys. Res., 106, 28275–28293, https://doi.org/10.1029/2001JD000384, 2001.
Schilling, K. A.: Secondary Organic Aerosol Composition Studies Using Mass Spectrometry, PhD thesis, California Institute of Technology, https://doi.org/10.7907/Z93F4MJR, 2015.
Seinfeld, J. and Pandis, S.: Atmospheric chemistry and physics: from air pollution to climate change, A Wiley interscience publication, Wiley, 1998.
Shrivastava, M., Fast, J., Easter, R., Gustafson Jr., W. I., Zaveri, R. A., Jimenez, J. L., Saide, P., and Hodzic, A.: Modeling organic aerosols in a megacity: comparison of simple and complex representations of the volatility basis set approach, Atmos. Chem. Phys., 11, 6639–6662, https://doi.org/10.5194/acp-11-6639-2011, 2011.
Shrivastava, M. K., Lane, T. E., Donahue, N. M., Pandis, S. N., and Robinson, A. L.: Effects of gas particle partitioning and aging of primary emissions on urban and regional organic aerosol concentrations, J. Geophys. Res., 113, D18301, https://doi.org/10.1029/2007JD009735, 2008.
Song, M., Liu, P. F., Hanna, S. J., Zaveri, R. A., Potter, K., You, Y., Martin, S. T., and Bertram, A. K.: Relative humidity-dependent viscosity of secondary organic material from toluene photo-oxidation and possible implications for organic particulate matter over megacities, Atmos. Chem. Phys., 16, 8817–8830, https://doi.org/10.5194/acp-16-8817-2016, 2016.
Surratt, J. D., Murphy, S. M., Kroll, J. H., Ng, N. L., Hildebrandt, L., Sorooshian, A., Szmigielski, R., Vermeylen, R., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Chemical composition of secondary organic aerosol formed from the photooxidation of isoprene, J. Phys. Chem. A, 110, 9665–9690, https://doi.org/10.1021/jp061734m, 2006.
Svendby, T. M., Lazaridis, M., and Tørseth, K.: Temperature dependent secondary organic aerosol formation from terpenes and aromatics, J. Atmos. Chem., 59, 25–46, https://doi.org/10.1007/s10874-007-9093-7, 2008.
Trump, E. R. and Donahue, N. M.: Oligomer formation within secondary organic aerosols: equilibrium and dynamic considerations, Atmos. Chem. Phys., 14, 3691–3701, https://doi.org/10.5194/acp-14-3691-2014, 2014.
Tulet, P., Grini, A., Griffin, R. J., and Petitcol, S.: ORILAM-SOA: A computationally efficient model for predicting secondary organic aerosols in three-dimensional atmospheric models, J. Geophys. Res., 111, D23208, https://doi.org/10.1029/2006JD007152, 2006.
Verwer, J. G., Spee, E. J., Bloom, J. G., and Hundsdorfer, W.: A second-order rosenbrock method applied to photochemical dispersion problems, SIAM J. Sci. Comput., 20, 1456–1480, https://doi.org/10.1137/S1064827597326651, 1999.
Vivanco, M. G., Santiago, M., Martínez-Tarifa, A., Borrás, E., Ródenas, M., García-Diego, C., and Sánchez, M.: SOA formation in a photoreactor from a mixture of organic gases and HONO for different experimental conditions, Atmos. Environ., 45, 708–715, https://doi.org/10.1016/j.atmosenv.2010.09.059, 2011.
Vivanco, M. G., Santiago, M., Sánchez, M., Clavero, M. A., Borrás, E., Ródenas, M., Alacreu, F., Vásquez, M., Clemente, E., Porras, R., Muñoz, A., and Stein, A.: Experimental data on SOA formation from mixtures of anthropogenic and biogenic organic compounds, Atmósfera, 26, 59–73, 2013.
Vivanco, M. G., Couvidat, F., Seigneur, C., Jang, M., Santiago, M., and Bessagnet, B.: Evaluation of some SOA formation schemes for the oxidation of anthropogenic gases against experiments in two outdoor chambers, Int. J. Environ. Pollut., 59, 43–55, https://doi.org/10.1504/IJEP.2016.078062, 2016.
Volkamer, R., Platt, U., and Wirtz, K.: Primary and secondary glyoxal formation from aromatics: experimental evidence for the bicycloalkyl-radical pathway from benzene, toluene, and p-xylene, J. Phys. Chem. A, 105, 7865–7874, https://doi.org/10.1021/jp010152w, 2001.
WHO: Health Aspects of Air Pollution with Particulate Matter, Ozone and Nitrogen Dioxide, WHO Working Group, Bonn, Germany, Tech. rep., WHO EUR/03/5042688, 2003.
Yu, S., Bhave, P. V., Dennis, R. L., and Marthur, R.: Seasonal and regional variations of primary and secondary organic aerosols over the Continental United States: Semi-empirical estimates and model evaluation, Environ. Sci. Technol., 41, 4690–4697, https://doi.org/10.1021/es061535g, 2007.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J., Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influence Northern Hemisphere mildlatitudes, Geophys. Res. Lett., 34, L13801, https://doi.org/10.1029/2007GL029979, 2007.
Zhang, X., Cappa, C. D., Jathar, S. H., Mcvay, R. C., Ensberg, J. J., Kleeman, M. J., and Seinfeld, J. H.: Influence of vapor wall loss in laboratory chambers on yields of secondary organic aerosol, P. Natl. Acad. Sci. USA, 111, 5802–5807, https://doi.org/10.1073/pnas.1404727111, 2014.
Zhang, X., Schwantes, R. H., McVay, R. C., Lignell, H., Coggon, M. M., Flagan, R. C., and Seinfeld, J. H.: Vapor wall deposition in Teflon chambers, Atmos. Chem. Phys., 15, 4197–4214, https://doi.org/10.5194/acp-15-4197-2015, 2015.
Zuend, A. and Seinfeld, J. H.: Modeling the gas-particle partitioning of secondary organic aerosol: the importance of liquid-liquid phase separation, Atmos. Chem. Phys., 12, 3857–3882, https://doi.org/10.5194/acp-12-3857-2012, 2012.
Zuend, A., Marcolli, C., Luo, B. P., and Peter, T.: A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients, Atmos. Chem. Phys., 8, 4559–4593, https://doi.org/10.5194/acp-8-4559-2008, 2008.
Zuend, A., Marcolli, C., Booth, A. M., Lienhard, D. M., Soonsin, V., Krieger, U. K., Topping, D. O., McFiggans, G., Peter, T., and Seinfeld, J. H.: New and extended parameterization of the thermodynamic model AIOMFAC: calculation of activity coefficients for organic-inorganic mixtures containing carboxyl, hydroxyl, carbonyl, ether, ester, alkenyl, alkyl, and aromatic functional groups, Atmos. Chem. Phys., 11, 9155–9206, https://doi.org/10.5194/acp-11-9155-2011, 2011.
Short summary
Several new parameterizations and mechanisms for SOA formation are developed based on available experimental results. To evaluate the parameterizations, a box model was developed to simulate SOA formation from monoterpenes and aromatics in the environmental chamber EUPHORE. This box model takes oligomerization, nonideality of the aerosol, multiphase partitioning, aging, vapor wall losses and particle-phase diffusion into account. All these phenomena are rarely taken into account together.
Several new parameterizations and mechanisms for SOA formation are developed based on available...
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