Articles | Volume 23, issue 24
https://doi.org/10.5194/acp-23-15537-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-15537-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
20 Dec 2023
Research article |
| 20 Dec 2023
| 20 Dec 2023
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
CEREA, École des Ponts ParisTech, EDF R&D, IPSL, 77455 Marne-la-Vallée, France
Aix Marseille Univ, CNRS, LCE, Marseille, France
Evangelia Kostenidou
Aix Marseille Univ, CNRS, LCE, Marseille, France
now at: Department of Environmental Engineering, Democritus University of Thrace, 67100 Xanthi, Greece
Florian Couvidat
National Institute for Industrial Environment and Risks (INERIS), 60 550 Verneuil-en-Halatte, France
Alvaro Martinez-Valiente
Aix Marseille Univ, CNRS, LCE, Marseille, France
Philipp Eichler
Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
now at: German Environment Agency, Dessau, Germany
Armin Wisthaler
Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
Department of Chemistry, University of Oslo, 0315 Oslo, Norway
Markus Müller
Ionicon Analytik GmbH, 6020 Innsbruck, Austria
Brice Temime-Roussel
Aix Marseille Univ, CNRS, LCE, Marseille, France
Richard Valorso
Univ Paris Est Creteil and Université Paris Cité, CNRS, LISA, 94010 Créteil, France
Karine Sartelet
CEREA, École des Ponts ParisTech, EDF R&D, IPSL, 77455 Marne-la-Vallée, France
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Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
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Brice Barret, Patrice Medina, Natalie Brett, Roman Pohorsky, Kathy Law, Slimane Bekki, Gilberto J. Fochesatto, Julia Schmale, Steve Arnold, Andrea Baccarini, Mauricio Busetto, Meeta Cesler-Maloney, Barbara D'Anna, Stefano Decesari, Jingqiu Mao, Gianluca Pappaccogli, Joel Savarino, Federico Scoto, and William R. Simpson
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Victor Lannuque and Karine Sartelet
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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
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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.
Alexis Squarcioni, Yelva Roustan, Myrto Valari, Youngseob Kim, Karine Sartelet, Lya Lugon, Fabrice Dugay, and Robin Voitot
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This study highlights the interest of using a street network model to estimate pollutant concentrations of NOx, NO2, and PM2.5 in heterogeneous urban areas, particularly those adjacent to highways, compared with the Subgrid approach embedded in the 3D eulerian model CHIMERE. However, the study also reveals comparable performance between the two approaches for the aforementioned pollutants in areas near the city centre, where urban characteristics are more uniform.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Karen E. Cady-Pereira, Xuehui Guo, Rui Wang, April B. Leytem, Chase Calkins, Elizabeth Berry, Kang Sun, Markus Müller, Armin Wisthaler, Vivienne H. Payne, Mark W. Shephard, Mark A. Zondlo, and Valentin Kantchev
Atmos. Meas. Tech., 17, 15–36, https://doi.org/10.5194/amt-17-15-2024, https://doi.org/10.5194/amt-17-15-2024, 2024
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Ammonia is a significant precursor of PM2.5 particles and thus contributes to poor air quality in many regions. Furthermore, ammonia concentrations are rising due to the increase of large-scale, intensive agricultural activities. Here we evaluate satellite measurements of ammonia against aircraft and surface network data, and show that there are differences in magnitude, but the satellite data are spatially and temporally well correlated with the in situ data.
Andreas Aktypis, Christos Kaltsonoudis, David Patoulias, Panayiotis Kalkavouras, Angeliki Matrali, Christina N. Vasilakopoulou, Evangelia Kostenidou, Kalliopi Florou, Nikos Kalivitis, Aikaterini Bougiatioti, Konstantinos Eleftheriadis, Stergios Vratolis, Maria I. Gini, Athanasios Kouras, Constantini Samara, Mihalis Lazaridis, Sofia-Eirini Chatoutsidou, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 65–84, https://doi.org/10.5194/acp-24-65-2024, https://doi.org/10.5194/acp-24-65-2024, 2024
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Extensive continuous particle number size distribution measurements took place during two summers (2020 and 2021) at 11 sites in Greece for the investigation of the frequency and the spatial extent of new particle formation. The frequency during summer varied from close to zero in southwestern Greece to more than 60 % in the northern, central, and eastern regions. The spatial variability can be explained by the proximity of the sites to coal-fired power plants and agricultural areas.
Abd El Rahman El Mais, Barbara D'Anna, Luka Drinovec, Andrew T. Lambe, Zhe Peng, Jean-Eudes Petit, Olivier Favez, Selim Aït-Aïssa, and Alexandre Albinet
Atmos. Chem. Phys., 23, 15077–15096, https://doi.org/10.5194/acp-23-15077-2023, https://doi.org/10.5194/acp-23-15077-2023, 2023
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Polycyclic aromatic hydrocarbons (PAHS) and furans are key precursors of secondary organic aerosols (SOAs) related to biomass burning emissions. We evaluated and compared the formation yields, and the physical and light absorption properties, of laboratory-generated SOAs from the oxidation of such compounds for both, day- and nighttime reactivities. The results illustrate that PAHs are large SOA precursors and may contribute significantly to the biomass burning brown carbon in the atmosphere.
Thibaud Sarica, Alice Maison, Yelva Roustan, Matthias Ketzel, Steen Solvang Jensen, Youngseob Kim, Christophe Chaillou, and Karine Sartelet
Geosci. Model Dev., 16, 5281–5303, https://doi.org/10.5194/gmd-16-5281-2023, https://doi.org/10.5194/gmd-16-5281-2023, 2023
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A new version of the Model of Urban Network of Intersecting Canyons and Highways (MUNICH) is developed to represent heterogeneities of concentrations in streets. The street volume is discretized vertically and horizontally to limit the artificial dilution of emissions and concentrations. This new version is applied to street networks in Copenhagen and Paris. The comparisons to observations are improved, with higher concentrations of pollutants emitted by traffic at the bottom of the street.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
Amir H. Souri, Matthew S. Johnson, Glenn M. Wolfe, James H. Crawford, Alan Fried, Armin Wisthaler, William H. Brune, Donald R. Blake, Andrew J. Weinheimer, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Corinne Vigouroux, Bavo Langerock, Sungyeon Choi, Lok Lamsal, Lei Zhu, Shuai Sun, Ronald C. Cohen, Kyung-Eun Min, Changmin Cho, Sajeev Philip, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 23, 1963–1986, https://doi.org/10.5194/acp-23-1963-2023, https://doi.org/10.5194/acp-23-1963-2023, 2023
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We have rigorously characterized different sources of error in satellite-based HCHO / NO2 tropospheric columns, a widely used metric for diagnosing near-surface ozone sensitivity. Specifically, the errors were categorized/quantified into (i) an inherent chemistry error, (ii) the decoupled relationship between columns and the near-surface concentration, (iii) the spatial representativeness error of ground satellite pixels, and (iv) the satellite retrieval errors.
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.
Chao Lin, Yunyi Wang, Ryozo Ooka, Cédric Flageul, Youngseob Kim, Hideki Kikumoto, Zhizhao Wang, and Karine Sartelet
Atmos. Chem. Phys., 23, 1421–1436, https://doi.org/10.5194/acp-23-1421-2023, https://doi.org/10.5194/acp-23-1421-2023, 2023
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In this study, SSH-aerosol, a modular box model that simulates the evolution of gas, primary, and secondary aerosols, is coupled with the computational fluid dynamics (CFD) software, OpenFOAM and Code_Saturne. The transient dispersion of pollutants emitted from traffic in a street canyon of Greater Paris is simulated. The coupled model achieved better agreement in NO2 and PM10 with measurement data than the conventional CFD simulation which regards pollutants as passive scalars.
Francesca Gallo, Kevin J. Sanchez, Bruce E. Anderson, Ryan Bennett, Matthew D. Brown, Ewan C. Crosbie, Chris Hostetler, Carolyn Jordan, Melissa Yang Martin, Claire E. Robinson, Lynn M. Russell, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Elizabeth B. Wiggins, Edward L. Winstead, Armin Wisthaler, Luke D. Ziemba, and Richard H. Moore
Atmos. Chem. Phys., 23, 1465–1490, https://doi.org/10.5194/acp-23-1465-2023, https://doi.org/10.5194/acp-23-1465-2023, 2023
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We integrate in situ ship- and aircraft-based measurements of aerosol, trace gases, and meteorological parameters collected during the NASA North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) field campaigns in the western North Atlantic Ocean region. A comprehensive characterization of the vertical profiles of aerosol properties under different seasonal regimes is provided for improving the understanding of aerosol key processes and aerosol–cloud interactions in marine regions.
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 %.
Alexander Håland, Tomáš Mikoviny, Elisabeth Emilie Syse, and Armin Wisthaler
Atmos. Meas. Tech., 15, 6297–6307, https://doi.org/10.5194/amt-15-6297-2022, https://doi.org/10.5194/amt-15-6297-2022, 2022
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PTR-MS is widely used in atmospheric sciences for the detection of non-methane organic trace gases. The two most widely used types of PTR-MS instruments differ in their ion source and drift tube design. We herein present a new prototype PTR-MS instrument that hybridizes these designs and combines a conventional hollow cathode glow discharge ion source with a focusing ion–molecule reactor. We also show how this new instrument performs in detecting atmospheric amines.
Youngseob Kim, Lya Lugon, Alice Maison, Thibaud Sarica, Yelva Roustan, Myrto Valari, Yang Zhang, Michel André, and Karine Sartelet
Geosci. Model Dev., 15, 7371–7396, https://doi.org/10.5194/gmd-15-7371-2022, https://doi.org/10.5194/gmd-15-7371-2022, 2022
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This paper presents the latest version of the street-network model MUNICH, v2.0. The description of MUNICH v1.0, which models gas-phase pollutants in a street network, was published in GMD in 2018. Since then, major modifications have been made to MUNICH. The comprehensive aerosol model SSH-aerosol is now coupled to MUNICH to simulate primary and secondary aerosol concentrations. New parameterisations have also been introduced. Test cases are defined to illustrate the new model functionalities.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Etienne Terrenoire, Didier A. Hauglustaine, Yann Cohen, Anne Cozic, Richard Valorso, Franck Lefèvre, and Sigrun Matthes
Atmos. Chem. Phys., 22, 11987–12023, https://doi.org/10.5194/acp-22-11987-2022, https://doi.org/10.5194/acp-22-11987-2022, 2022
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Aviation NOx emissions not only have an impact on global climate by changing ozone and methane levels in the atmosphere, but also contribute to the deterioration of local air quality. The LMDZ-INCA global model is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. We investigate the impact of present-day and future (2050) aircraft emissions on atmospheric composition and the associated radiative forcings of climate for ozone, methane and aerosol direct forcings.
Alice Maison, Cédric Flageul, Bertrand Carissimo, Yunyi Wang, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 22, 9369–9388, https://doi.org/10.5194/acp-22-9369-2022, https://doi.org/10.5194/acp-22-9369-2022, 2022
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This paper presents a parameterization of the tree crown effect on air flow and pollutant dispersion in a street network model used to simulate air quality at the street level. The new parameterization is built using a finer-scale model (computational fluid dynamics). The tree effect increases with the leaf area index and the crown volume fraction of the trees; the street horizontal velocity is reduced by up to 68 % and the vertical transfer into or out of the street by up to 23 %.
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.
Junteng Wu, Nicolas Brun, Juan Miguel González-Sánchez, Badr R'Mili, Brice Temime Roussel, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Meas. Tech., 15, 3859–3874, https://doi.org/10.5194/amt-15-3859-2022, https://doi.org/10.5194/amt-15-3859-2022, 2022
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This work quantified and tentatively identified the organic impurities on ammonium sulfate aerosols generated in the laboratory. They are likely low volatile and high mass molecules containing oxygen, nitrogen, and/or sulfur. Our results show that these organic impurities likely originate from the commercial AS crystals. It is recommended to use AS seeds with caution, especially when small particles are used, in terms of AS purity and water purity when aqueous solutions are used for atomization.
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.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Boris Vansevenant, Cédric Louis, Corinne Ferronato, Ludovic Fine, Patrick Tassel, Pascal Perret, Evangelia Kostenidou, Brice Temime-Roussel, Barbara D'Anna, Karine Sartelet, Véronique Cerezo, and Yao Liu
Atmos. Meas. Tech., 14, 7627–7655, https://doi.org/10.5194/amt-14-7627-2021, https://doi.org/10.5194/amt-14-7627-2021, 2021
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A new method was developed to correct wall losses of particles on Teflon walls using a new environmental chamber. It was applied to experiments with six diesel vehicles (Euro 3 to 6), tested on a chassis dynamometer. Emissions of particles and precursors were obtained under urban and motorway conditions. The chamber experiments help understand the role of physical processes in diesel particle evolutions in the dark. These results can be applied to situations such as tunnels or winter rush hours.
Lya Lugon, Jérémy Vigneron, Christophe Debert, Olivier Chrétien, and Karine Sartelet
Geosci. Model Dev., 14, 7001–7019, https://doi.org/10.5194/gmd-14-7001-2021, https://doi.org/10.5194/gmd-14-7001-2021, 2021
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The multiscale Street-in-Grid model is used to simulate black carbon (BC) concentrations in streets. To respect street-surface mass balance, particle resuspension is estimated with a new approach based on deposited mass. The contribution of resuspension is low, but non-exhaust emissions from tyre wear may largely contribute to BC concentrations. The impact of the two-way dynamic coupling between scales on BC concentrations varies depending on the street geometry and traffic emission intensity.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
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.
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.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
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We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Eve-Agnès Fiorentino, Henri Wortham, and Karine Sartelet
Geosci. Model Dev., 14, 2747–2780, https://doi.org/10.5194/gmd-14-2747-2021, https://doi.org/10.5194/gmd-14-2747-2021, 2021
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Indoor air quality (IAQ) is strongly influenced by reactivity with surfaces, which is called heterogeneous reactivity. To date, this reactivity is barely integrated into numerical models due to the strong uncertainties it is subjected to. In this work, an open-source IAQ model, called the H2I model, is developed to consider both gas-phase and heterogeneous reactivity and simulate indoor concentrations of inorganic compounds.
Benjamin Chazeau, Brice Temime-Roussel, Grégory Gille, Boualem Mesbah, Barbara D'Anna, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 21, 7293–7319, https://doi.org/10.5194/acp-21-7293-2021, https://doi.org/10.5194/acp-21-7293-2021, 2021
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The temporal trends in the chemical composition and particle number of the submicron aerosols in a Mediterranean city, Marseille, are investigated over 14 months. Fifteen days were found to exceed the WHO PM2.5 daily limit (25 µg m−3) only during the cold period, with two distinct origins: local pollution events with an increased fraction of the carbonaceous fraction due to domestic wood burning and long-range pollution events with a high level of oxygenated organic aerosol and ammonium nitrate.
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Julien Morin, Brice Temime-Roussel, Sylvain Ravier, Camille Mouchel-Vallon, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 21, 4915–4937, https://doi.org/10.5194/acp-21-4915-2021, https://doi.org/10.5194/acp-21-4915-2021, 2021
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Organic nitrates play a crucial role in air pollution as they are considered NOx reservoirs. This work lights up the importance of their reactions with OH radicals in the aqueous phase (cloud/fog, wet aerosol), which is slower than in the gas phase. For compounds that significantly partition in water such as polyfunctional biogenic nitrates, these aqueous-phase reactions should drive their atmospheric removal, leading to a broader spatial distribution of NOx than previously accounted for.
Evangelia Kostenidou, Alvaro Martinez-Valiente, Badr R'Mili, Baptiste Marques, Brice Temime-Roussel, Amandine Durand, Michel André, Yao Liu, Cédric Louis, Boris Vansevenant, Daniel Ferry, Carine Laffon, Philippe Parent, and Barbara D'Anna
Atmos. Chem. Phys., 21, 4779–4796, https://doi.org/10.5194/acp-21-4779-2021, https://doi.org/10.5194/acp-21-4779-2021, 2021
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Passenger vehicle emissions can be a significant source of particulate matter in urban areas. In this study the particle-phase emissions of seven Euro 5 passenger vehicles were characterized. Changes in engine technologies and after-treatment devices can alter the chemical composition and the size of the emitted particulate matter. The condition of the diesel particle filter (DPF) plays an important role in the emitted pollutants.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Felix Piel, Markus Müller, Klaus Winkler, Jenny Skytte af Sätra, and Armin Wisthaler
Atmos. Meas. Tech., 14, 1355–1363, https://doi.org/10.5194/amt-14-1355-2021, https://doi.org/10.5194/amt-14-1355-2021, 2021
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Proton-transfer-reaction mass spectrometry (PTR-MS) instruments are widely used in the atmospheric community for measuring organic trace substances in the Earth's atmosphere. Some of these substances
stickonto and slowly come off surfaces in the PTR-MS analyzer, which makes it impossible to measure rapid changes in the atmosphere. Herein, we present a new type of PTR-MS instrument with a specially treated surface that mitigates this problem.
Betty Croft, Randall V. Martin, Richard H. Moore, Luke D. Ziemba, Ewan C. Crosbie, Hongyu Liu, Lynn M. Russell, Georges Saliba, Armin Wisthaler, Markus Müller, Arne Schiller, Martí Galí, Rachel Y.-W. Chang, Erin E. McDuffie, Kelsey R. Bilsback, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 1889–1916, https://doi.org/10.5194/acp-21-1889-2021, https://doi.org/10.5194/acp-21-1889-2021, 2021
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North Atlantic Aerosols and Marine Ecosystems Study measurements combined with GEOS-Chem-TOMAS modeling suggest that several not-well-understood key factors control northwest Atlantic aerosol number and size. These synergetic and climate-relevant factors include particle formation near and above the marine boundary layer top, particle growth by marine secondary organic aerosol on descent, particle formation/growth related to dimethyl sulfide, sea spray aerosol, and ship emissions.
Audrey Fortems-Cheiney, Gaëlle Dufour, Karine Dufossé, Florian Couvidat, Jean-Marc Gilliot, Guillaume Siour, Matthias Beekmann, Gilles Foret, Frederik Meleux, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Cathy Clerbaux, and Sophie Génermont
Atmos. Chem. Phys., 20, 13481–13495, https://doi.org/10.5194/acp-20-13481-2020, https://doi.org/10.5194/acp-20-13481-2020, 2020
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Studies have suggested the importance of ammonia emissions on pollution particle formation over Europe, whose main atmospheric source is agriculture. In this study, we performed an inter-comparison of two alternative inventories, both with a reference inventory, that quantify the French ammonia emissions during spring 2011. Over regions with large mineral fertilizer use, like over northeastern France, NH3 emissions are probably considerably underestimated by the reference inventory.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Mike J. Newland, and Andrew R. Rickard
Atmos. Chem. Phys., 20, 12921–12937, https://doi.org/10.5194/acp-20-12921-2020, https://doi.org/10.5194/acp-20-12921-2020, 2020
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Unsaturated organic compounds are emitted in large quantities from natural and human-influenced sources. Atmospheric removal occurs significantly by reaction with ozone, initiating reaction sequences forming free radicals and organic pollutants in the gaseous and particulate phases. Due to their very large number, it is impossible to study the reaction rate for every compound, and most have to be estimated. Updated and extended estimation methods are reported for use in atmospheric models.
James Brean, David C. S. Beddows, Zongbo Shi, Brice Temime-Roussel, Nicolas Marchand, Xavier Querol, Andrés Alastuey, María Cruz Minguillón, and Roy M. Harrison
Atmos. Chem. Phys., 20, 10029–10045, https://doi.org/10.5194/acp-20-10029-2020, https://doi.org/10.5194/acp-20-10029-2020, 2020
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New particle formation is a key process influencing both local air quality and climatically active cloud condensation nuclei concentrations. This study has carried out fundamental measurements of nucleation processes in Barcelona, Spain, and concludes that a mechanism involving stabilisation of sulfuric acid clusters by low molecular weight amines is primarily responsible for new particle formation events.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Eve-Agnès Fiorentino, Henri Wortham, and Karine Sartelet
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-192, https://doi.org/10.5194/gmd-2020-192, 2020
Preprint withdrawn
Lya Lugon, Karine Sartelet, Youngseob Kim, Jérémy Vigneron, and Olivier Chrétien
Atmos. Chem. Phys., 20, 7717–7740, https://doi.org/10.5194/acp-20-7717-2020, https://doi.org/10.5194/acp-20-7717-2020, 2020
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This study presents a new version of the multi-scale model Street-in-Grid (SinG) that interconnects regional and local scales in air-quality modeling in urban areas. The new version of SinG performs the finest coupling between transport and chemistry, leading to a numerically stable partitioning between NO and NO2. Multi-scale, local-scale and regional-scale simulations of NO, NO2 and NOx over Paris are compared to observations, and SinG shows good performance for both local and regional scales.
Victor Lannuque, Florian Couvidat, Marie Camredon, Bernard Aumont, and Bertrand Bessagnet
Atmos. Chem. Phys., 20, 4905–4931, https://doi.org/10.5194/acp-20-4905-2020, https://doi.org/10.5194/acp-20-4905-2020, 2020
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Large uncertainties remain in modeling secondary organic aerosol (SOA) and evolution and properties in air quality models. In this article, the recently developed VBS-GECKO parameterization for SOA formation has been implemented in the air quality model CHIMERE. Simulations have been driven to identify the main SOA sources and to evaluate the sensitivity of simulated SOA concentrations to (i) secondary organic compound properties and (ii) emissions from traffic and transportation sources.
Laurent Menut, Guillaume Siour, Bertrand Bessagnet, Florian Couvidat, Emilie Journet, Yves Balkanski, and Karine Desboeufs
Geosci. Model Dev., 13, 2051–2071, https://doi.org/10.5194/gmd-13-2051-2020, https://doi.org/10.5194/gmd-13-2051-2020, 2020
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Modelling of mineral dust is often done using one single mean species. In this study, differentiated mineral species with their chemical composition are implemented in the CHIMERE regional chemistry-transport model by using global databases. Simulations are carried out to quantify the realism and gain of such mineralogy.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Giancarlo Ciarelli, Mark R. Theobald, Marta G. Vivanco, Matthias Beekmann, Wenche Aas, Camilla Andersson, Robert Bergström, Astrid Manders-Groot, Florian Couvidat, Mihaela Mircea, Svetlana Tsyro, Hilde Fagerli, Kathleen Mar, Valentin Raffort, Yelva Roustan, Maria-Teresa Pay, Martijn Schaap, Richard Kranenburg, Mario Adani, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Cornelis Cuvelier, Arineh Cholakian, Bertrand Bessagnet, Peter Wind, and Augustin Colette
Geosci. Model Dev., 12, 4923–4954, https://doi.org/10.5194/gmd-12-4923-2019, https://doi.org/10.5194/gmd-12-4923-2019, 2019
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The novel multi-model EURODELTA-Trends exercise provided 21 years of continuous PM components and their gas-phase precursor concentrations over Europe from the year 1990. The models’ capabilities to reproduce PM components and gas-phase PM precursor trends over the 1990–2010 period is the key focus of this study. The models were able to reproduce the observed trends relatively well, indicating a possible shift in the thermodynamic equilibrium between gas and particle phases.
Felix Piel, Markus Müller, Tomas Mikoviny, Sally E. Pusede, and Armin Wisthaler
Atmos. Meas. Tech., 12, 5947–5958, https://doi.org/10.5194/amt-12-5947-2019, https://doi.org/10.5194/amt-12-5947-2019, 2019
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Herein we report on the first successful airborne deployment of a CHARON PTR–ToF–MS instrument aboard the NASA DC–8 research aircraft. The analyzer is capable of chemically characterizing submicrometer atmospheric particles in a quantitative manner, at the near–molecular level, in real time. This brings a new and unprecedented measurement capability to the airborne atmospheric science community.
Marc D. Mallet, Barbara D'Anna, Aurélie Même, Maria Chiara Bove, Federico Cassola, Giandomenico Pace, Karine Desboeufs, Claudia Di Biagio, Jean-Francois Doussin, Michel Maille, Dario Massabò, Jean Sciare, Pascal Zapf, Alcide Giorgio di Sarra, and Paola Formenti
Atmos. Chem. Phys., 19, 11123–11142, https://doi.org/10.5194/acp-19-11123-2019, https://doi.org/10.5194/acp-19-11123-2019, 2019
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We present findings from a summertime field campaign at the remote island of Lampedusa in the central Mediterranean Sea. We show that the aerosol loading is similar to coastal sites around the Mediterranean. We observe higher loadings of sulfate and aged organic aerosol from air masses transported over the central and eastern Mediterranean in comparison to those from the western Mediterranean. These results highlight the rarity of pristine air masses, even in remote marine environments.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, and Andrew R. Rickard
Atmos. Chem. Phys., 19, 7691–7717, https://doi.org/10.5194/acp-19-7691-2019, https://doi.org/10.5194/acp-19-7691-2019, 2019
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Organic compounds are emitted in large amounts from natural and human-influenced sources. Peroxy radicals are key intermediates formed during oxidation of organic compounds, and play a central role in mechanisms forming pollutants such as ozone and organic particles. Due to the large number of different peroxy radicals formed, it is impossible to study the rates of all of their reactions, and most have to be estimated. Updated and new estimation methods are reported for use in atmospheric models
Marwa Majdi, Karine Sartelet, Grazia Maria Lanzafame, Florian Couvidat, Youngseob Kim, Mounir Chrit, and Solene Turquety
Atmos. Chem. Phys., 19, 5543–5569, https://doi.org/10.5194/acp-19-5543-2019, https://doi.org/10.5194/acp-19-5543-2019, 2019
John T. Sullivan, Thomas J. McGee, Ryan M. Stauffer, Anne M. Thompson, Andrew Weinheimer, Christoph Knote, Scott Janz, Armin Wisthaler, Russell Long, James Szykman, Jinsoo Park, Youngjae Lee, Saewung Kim, Daun Jeong, Dianne Sanchez, Laurence Twigg, Grant Sumnicht, Travis Knepp, and Jason R. Schroeder
Atmos. Chem. Phys., 19, 5051–5067, https://doi.org/10.5194/acp-19-5051-2019, https://doi.org/10.5194/acp-19-5051-2019, 2019
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During the May–June 2016 International Cooperative Air Quality Field Study in Korea (KORUS-AQ), pollution reached the remote Taehwa Research Forest (TRF) site. Two case studies are examined and observations clearly identify TRF and the surrounding rural areas as long-term receptor sites for severe urban pollution events. In summary, domestic emissions may be causing more pollution than by transboundary pathways, which have been historically believed to be the major source of air pollution.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Youngseob Kim, Karine Sartelet, and Florian Couvidat
Atmos. Chem. Phys., 19, 1241–1261, https://doi.org/10.5194/acp-19-1241-2019, https://doi.org/10.5194/acp-19-1241-2019, 2019
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Assumptions (ideality and thermodynamic equilibrium) commonly made in 3-dimensional air quality models were reconsidered to evaluate their impacts on secondary organic aerosol (SOA) formation. Non-ideality (short-, medium- and long-range interactions of organics and inorganics) influences SOA concentrations by about 30 % over Europe. If SOA are highly viscous rather than inviscid, hydrophobic SOA concentrations increase by 6 % but can increase by an order of magnitude for volatile compounds.
Marwa Majdi, Solene Turquety, Karine Sartelet, Carole Legorgeu, Laurent Menut, and Youngseob Kim
Atmos. Chem. Phys., 19, 785–812, https://doi.org/10.5194/acp-19-785-2019, https://doi.org/10.5194/acp-19-785-2019, 2019
Mark R. Theobald, Marta G. Vivanco, Wenche Aas, Camilla Andersson, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Mihaela Mircea, Maria-Teresa Pay, Svetlana Tsyro, Mario Adani, Robert Bergström, Bertrand Bessagnet, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Hilde Fagerli, Kathleen Mar, Noelia Otero, Valentin Raffort, Yelva Roustan, Martijn Schaap, Peter Wind, and Augustin Colette
Atmos. Chem. Phys., 19, 379–405, https://doi.org/10.5194/acp-19-379-2019, https://doi.org/10.5194/acp-19-379-2019, 2019
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Model estimates of the mean European wet deposition of nitrogen and sulfur for 1990 to 2010 were within 40 % of the observed values. As a result of systematic biases, the models were better at estimating relative trends for the periods 1990–2000 and 2000–2010 than the absolute trends. Although the predominantly decreasing trends were mostly due to emission reductions, they were partially offset by other factors (e.g. changes in precipitation) during the first period, but not the second.
Mounir Chrit, Karine Sartelet, Jean Sciare, Marwa Majdi, José Nicolas, Jean-Eudes Petit, and François Dulac
Atmos. Chem. Phys., 18, 18079–18100, https://doi.org/10.5194/acp-18-18079-2018, https://doi.org/10.5194/acp-18-18079-2018, 2018
Cristina Carnerero, Noemí Pérez, Cristina Reche, Marina Ealo, Gloria Titos, Hong-Ku Lee, Hee-Ram Eun, Yong-Hee Park, Lubna Dada, Pauli Paasonen, Veli-Matti Kerminen, Enrique Mantilla, Miguel Escudero, Francisco J. Gómez-Moreno, Elisabeth Alonso-Blanco, Esther Coz, Alfonso Saiz-Lopez, Brice Temime-Roussel, Nicolas Marchand, David C. S. Beddows, Roy M. Harrison, Tuukka Petäjä, Markku Kulmala, Kang-Ho Ahn, Andrés Alastuey, and Xavier Querol
Atmos. Chem. Phys., 18, 16601–16618, https://doi.org/10.5194/acp-18-16601-2018, https://doi.org/10.5194/acp-18-16601-2018, 2018
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The vertical distribution of new particle formation events was studied using tethered balloons carrying miniaturized instrumentation. Results show that new particle formation and growth occurs only in the lower layer of the atmosphere, where aerosols are mixed due to convection, especially when the atmosphere is clean. A comparison of urban and suburban surface stations was also made, suggesting that such events may have a significant impact on ultrafine particle concentrations in a wide area.
Barbara Ervens, Armin Sorooshian, Abdulmonam M. Aldhaif, Taylor Shingler, Ewan Crosbie, Luke Ziemba, Pedro Campuzano-Jost, Jose L. Jimenez, and Armin Wisthaler
Atmos. Chem. Phys., 18, 16099–16119, https://doi.org/10.5194/acp-18-16099-2018, https://doi.org/10.5194/acp-18-16099-2018, 2018
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The paper presents a new framework that can be used to identify emission scenarios in which aerosol populations are most likely modified by chemical processes in clouds. We show that in neither very polluted nor in very clean air masses is this the case. Only if the ratio of possible aerosol mass precursors (sulfur dioxide, some organics) and preexisting aerosol mass is sufficiently high will aerosol particles show substantially modified physicochemical properties upon cloud processing.
Florian Couvidat, Marta G. Vivanco, and Bertrand Bessagnet
Atmos. Chem. Phys., 18, 15743–15766, https://doi.org/10.5194/acp-18-15743-2018, https://doi.org/10.5194/acp-18-15743-2018, 2018
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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.
Victor Lannuque, Marie Camredon, Florian Couvidat, Alma Hodzic, Richard Valorso, Sasha Madronich, Bertrand Bessagnet, and Bernard Aumont
Atmos. Chem. Phys., 18, 13411–13428, https://doi.org/10.5194/acp-18-13411-2018, https://doi.org/10.5194/acp-18-13411-2018, 2018
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Large uncertainties remain in understanding the influence of atmospheric environmental conditions on secondary organic aerosol (SOA) formation, evolution and properties. In this article, the GECKO-A modelling tool has been used in a box model under various environmental conditions to (i) explore the sensitivity of SOA formation and properties to changes on physical and chemical conditions and (ii) develop a volatility-basis-set-type parameterization for air quality models.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Noelia Otero, Jana Sillmann, Kathleen A. Mar, Henning W. Rust, Sverre Solberg, Camilla Andersson, Magnuz Engardt, Robert Bergström, Bertrand Bessagnet, Augustin Colette, Florian Couvidat, Cournelius Cuvelier, Svetlana Tsyro, Hilde Fagerli, Martijn Schaap, Astrid Manders, Mihaela Mircea, Gino Briganti, Andrea Cappelletti, Mario Adani, Massimo D'Isidoro, María-Teresa Pay, Mark Theobald, Marta G. Vivanco, Peter Wind, Narendra Ojha, Valentin Raffort, and Tim Butler
Atmos. Chem. Phys., 18, 12269–12288, https://doi.org/10.5194/acp-18-12269-2018, https://doi.org/10.5194/acp-18-12269-2018, 2018
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This paper evaluates the capability of air-quality models to capture the observed relationship between surface ozone concentrations and meteorology over Europe. The air-quality models tended to overestimate the influence of maximum temperature and surface solar radiation. None of the air-quality models captured the strength of the observed relationship between ozone and relative humidity appropriately, underestimating the effect of relative humidity, a key factor in the ozone removal processes.
Anne-Cyrielle Genard-Zielinski, Christophe Boissard, Elena Ormeño, Juliette Lathière, Ilja M. Reiter, Henri Wortham, Jean-Philippe Orts, Brice Temime-Roussel, Bertrand Guenet, Svenja Bartsch, Thierry Gauquelin, and Catherine Fernandez
Biogeosciences, 15, 4711–4730, https://doi.org/10.5194/bg-15-4711-2018, https://doi.org/10.5194/bg-15-4711-2018, 2018
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From seasonal in situ observations on how a Mediterranean ecosystem responds to drought, a specific isoprene emission (ER, emission rates) algorithm was developed, upon which 2100 projections (IPCC RCP2.6 and RCP8.5 scenarios) were made. Emission rates were found to be mainly sensitive to future temperature changes and poorly represented by current empirical emission models. Drought was found to aggravate thermal stress on emission rates.
Amelie Bertrand, Giulia Stefenelli, Simone M. Pieber, Emily A. Bruns, Brice Temime-Roussel, Jay G. Slowik, Henri Wortham, André S. H. Prévôt, Imad El Haddad, and Nicolas Marchand
Atmos. Chem. Phys., 18, 10915–10930, https://doi.org/10.5194/acp-18-10915-2018, https://doi.org/10.5194/acp-18-10915-2018, 2018
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We model the evolution of several BBOA markers including levoglucosan during aging experiments conducted in an atmospheric Teflon chamber, in order to evaluate the influence of vapor wall loss on the determination of the rate constants of the compounds with hydroxyl radicals (OH).
Marta G. Vivanco, Mark R. Theobald, Héctor García-Gómez, Juan Luis Garrido, Marje Prank, Wenche Aas, Mario Adani, Ummugulsum Alyuz, Camilla Andersson, Roberto Bellasio, Bertrand Bessagnet, Roberto Bianconi, Johannes Bieser, Jørgen Brandt, Gino Briganti, Andrea Cappelletti, Gabriele Curci, Jesper H. Christensen, Augustin Colette, Florian Couvidat, Cornelis Cuvelier, Massimo D'Isidoro, Johannes Flemming, Andrea Fraser, Camilla Geels, Kaj M. Hansen, Christian Hogrefe, Ulas Im, Oriol Jorba, Nutthida Kitwiroon, Astrid Manders, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Luca Pozzoli, Efisio Solazzo, Svetlana Tsyro, Alper Unal, Peter Wind, and Stefano Galmarini
Atmos. Chem. Phys., 18, 10199–10218, https://doi.org/10.5194/acp-18-10199-2018, https://doi.org/10.5194/acp-18-10199-2018, 2018
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European wet and dry atmospheric deposition of N and S estimated by 14 air quality models was found to vary substantially. An ensemble of models meeting acceptability criteria was used to estimate the exceedances of the critical loads for N in habitats within the Natura 2000 network, as well as their lower and upper limits. Scenarios with 20 % emission reductions in different regions of the world showed that European emissions are responsible for most of the N and S deposition in Europe.
Mounir Chrit, Karine Sartelet, Jean Sciare, Jorge Pey, José B. Nicolas, Nicolas Marchand, Evelyn Freney, Karine Sellegri, Matthias Beekmann, and François Dulac
Atmos. Chem. Phys., 18, 9631–9659, https://doi.org/10.5194/acp-18-9631-2018, https://doi.org/10.5194/acp-18-9631-2018, 2018
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Fine particulate matter (PM) in the atmosphere is of concern due to its effects on health, climate, ecosystems and biological cycles, and visibility.
These effects are especially important in the Mediterranean region. In this study, the air quality model Polyphemus is used to understand the
sources of inorganic and organic particles in the western Mediterranean and evaluate the uncertainties linked to the model parameters and hypotheses related to condensation/evaporation in the model.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Andrew R. Rickard, and Timothy J. Wallington
Atmos. Chem. Phys., 18, 9297–9328, https://doi.org/10.5194/acp-18-9297-2018, https://doi.org/10.5194/acp-18-9297-2018, 2018
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Organic compounds are emitted in large quantities from natural and human-influenced sources. Removal from the atmosphere occurs mainly by reaction with hydroxyl (OH) radicals, and initiates reaction sequences forming pollutants such as ozone and organic particles. Due to their very large number, it is impossible to measure the removal rate for all compounds, and most have to be estimated. An updated and extended estimation method is reported for use in atmospheric models and impact assessments.
Michael E. Jenkin, Richard Valorso, Bernard Aumont, Andrew R. Rickard, and Timothy J. Wallington
Atmos. Chem. Phys., 18, 9329–9349, https://doi.org/10.5194/acp-18-9329-2018, https://doi.org/10.5194/acp-18-9329-2018, 2018
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Organic compounds are emitted in large quantities from natural and human-influenced sources. Removal from the atmosphere occurs mainly by reaction with hydroxyl (OH) radicals, and initiates reaction sequences forming pollutants such as ozone and organic particles. Due to their very large number, it is impossible to measure the removal rate for all compounds, and most have to be estimated. An updated and extended estimation method is reported for use in atmospheric models and impact assessments.
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Arineh Cholakian, Matthias Beekmann, Augustin Colette, Isabelle Coll, Guillaume Siour, Jean Sciare, Nicolas Marchand, Florian Couvidat, Jorge Pey, Valerie Gros, Stéphane Sauvage, Vincent Michoud, Karine Sellegri, Aurélie Colomb, Karine Sartelet, Helen Langley DeWitt, Miriam Elser, André S. H. Prévot, Sonke Szidat, and François Dulac
Atmos. Chem. Phys., 18, 7287–7312, https://doi.org/10.5194/acp-18-7287-2018, https://doi.org/10.5194/acp-18-7287-2018, 2018
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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
Evelyn Freney, Karine Sellegri, Mounir Chrit, Kouji Adachi, Joel Brito, Antoine Waked, Agnès Borbon, Aurélie Colomb, Régis Dupuy, Jean-Marc Pichon, Laetitia Bouvier, Claire Delon, Corinne Jambert, Pierre Durand, Thierry Bourianne, Cécile Gaimoz, Sylvain Triquet, Anaïs Féron, Matthias Beekmann, François Dulac, and Karine Sartelet
Atmos. Chem. Phys., 18, 7041–7056, https://doi.org/10.5194/acp-18-7041-2018, https://doi.org/10.5194/acp-18-7041-2018, 2018
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The focus of these experiments, within the ChArMEx project, were to better understand the chemical properties of ambient aerosols over the Mediterranean region. A series of airborne measurements were performed aboard the French research aircraft, the ATR42, during the summer period. Aerosol and gas-phase chemical mass spectrometry allowed us to understand the sources and formation of organic aerosols. Numerical models were incorporated into this study to help interpret our observations.
Xavier Querol, Andrés Alastuey, Gotzon Gangoiti, Noemí Perez, Hong K. Lee, Heeram R. Eun, Yonghee Park, Enrique Mantilla, Miguel Escudero, Gloria Titos, Lucio Alonso, Brice Temime-Roussel, Nicolas Marchand, Juan R. Moreta, M. Arantxa Revuelta, Pedro Salvador, Begoña Artíñano, Saúl García dos Santos, Mónica Anguas, Alberto Notario, Alfonso Saiz-Lopez, Roy M. Harrison, Millán Millán, and Kang-Ho Ahn
Atmos. Chem. Phys., 18, 6511–6533, https://doi.org/10.5194/acp-18-6511-2018, https://doi.org/10.5194/acp-18-6511-2018, 2018
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We show the main drivers of high O3 episodes in and around Madrid. High levels of ultrafine particles (UFPs) are evidenced, but we demonstrate that most O3 arises from the fumigation of high atmospheric layers, whereas UFPs are generated inside the PBL. O3 contributions from the fumigation of the vertical recirculation of regional air masses, hemispheric transport, and horizontally from direct urban plume transport are shown. Complexity arises from the need to quantify them to abate surface O3.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Ningxin Wang, Evangelia Kostenidou, Neil M. Donahue, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 3589–3601, https://doi.org/10.5194/acp-18-3589-2018, https://doi.org/10.5194/acp-18-3589-2018, 2018
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This study investigates aging in the α-pinene ozonolysis system with hydroxyl radicals (OH) through smog chamber experiments. After an equivalent of 2–4 days of typical atmospheric oxidation conditions, homogeneous OH oxidation of the α-pinene ozonolysis products resulted in a 20–40 % net increase in the organic aerosol concentration and an increase in aerosol O : C by up to 0.04. The relative humidity in the 5–50 % range had a minimum effect on aging.
Florian Couvidat, Bertrand Bessagnet, Marta Garcia-Vivanco, Elsa Real, Laurent Menut, and Augustin Colette
Geosci. Model Dev., 11, 165–194, https://doi.org/10.5194/gmd-11-165-2018, https://doi.org/10.5194/gmd-11-165-2018, 2018
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This paper includes the development of a new aerosol module in the air quality model CHIMERE to improve particulate matter (PM) simulation. The results of the model are compared to numerous measurements over Europe to evaluate the strengths and weaknesses of the model.
Allison N. Schwier, Karine Sellegri, Sébastien Mas, Bruno Charrière, Jorge Pey, Clémence Rose, Brice Temime-Roussel, Jean-Luc Jaffrezo, David Parin, David Picard, Mickael Ribeiro, Greg Roberts, Richard Sempéré, Nicolas Marchand, and Barbara D'Anna
Atmos. Chem. Phys., 17, 14645–14660, https://doi.org/10.5194/acp-17-14645-2017, https://doi.org/10.5194/acp-17-14645-2017, 2017
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In the present paper, we quantify sea-to-air emission fluxes of aerosol to the atmosphere and characterize their physical and chemical properties as a function of the seawater biochemical and physical properties. Fluxes are evaluated with an original approach, a "lab in the field" experiment that preserves the seawater and atmospheric complexity while isolating air-to-sea exchanges from their surroundings. We show different features of the aerosol emission fluxes compared to previous findings.
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
Evangelos E. Louvaris, Eleni Karnezi, Evangelia Kostenidou, Christos Kaltsonoudis, and Spyros N. Pandis
Atmos. Meas. Tech., 10, 3909–3918, https://doi.org/10.5194/amt-10-3909-2017, https://doi.org/10.5194/amt-10-3909-2017, 2017
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A method for the determination of the organic aerosol volatility distribution combining thermodenuder and isothermal dilution measurements is developed. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol produced during meat charbroiling. Addition of the dilution measurements to the thermodenuder data results in a lower uncertainty of the estimated vaporization enthalpy as well as the semivolatile content of the aerosol.
Mounir Chrit, Karine Sartelet, Jean Sciare, Jorge Pey, Nicolas Marchand, Florian Couvidat, Karine Sellegri, and Matthias Beekmann
Atmos. Chem. Phys., 17, 12509–12531, https://doi.org/10.5194/acp-17-12509-2017, https://doi.org/10.5194/acp-17-12509-2017, 2017
Augustin Colette, Camilla Andersson, Astrid Manders, Kathleen Mar, Mihaela Mircea, Maria-Teresa Pay, Valentin Raffort, Svetlana Tsyro, Cornelius Cuvelier, Mario Adani, Bertrand Bessagnet, Robert Bergström, Gino Briganti, Tim Butler, Andrea Cappelletti, Florian Couvidat, Massimo D'Isidoro, Thierno Doumbia, Hilde Fagerli, Claire Granier, Chris Heyes, Zig Klimont, Narendra Ojha, Noelia Otero, Martijn Schaap, Katarina Sindelarova, Annemiek I. Stegehuis, Yelva Roustan, Robert Vautard, Erik van Meijgaard, Marta Garcia Vivanco, and Peter Wind
Geosci. Model Dev., 10, 3255–3276, https://doi.org/10.5194/gmd-10-3255-2017, https://doi.org/10.5194/gmd-10-3255-2017, 2017
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The EURODELTA-Trends numerical experiment has been designed to assess the capability of chemistry-transport models to capture the evolution of surface air quality over the 1990–2010 period in Europe. It also includes sensitivity experiments in order to analyse the relative contribution of (i) emission changes, (ii) meteorological variability, and (iii) boundary conditions to air quality trends. The article is a detailed presentation of the experiment design and participating models.
Kevin Berland, Clémence Rose, Jorge Pey, Anais Culot, Evelyn Freney, Nikolaos Kalivitis, Giorgios Kouvarakis, José Carlos Cerro, Marc Mallet, Karine Sartelet, Matthias Beckmann, Thierry Bourriane, Greg Roberts, Nicolas Marchand, Nikolaos Mihalopoulos, and Karine Sellegri
Atmos. Chem. Phys., 17, 9567–9583, https://doi.org/10.5194/acp-17-9567-2017, https://doi.org/10.5194/acp-17-9567-2017, 2017
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New particle formation (NPF) from gas-phase precursors is a process that is expected to drive the total number concentration of particles in the atmosphere. Here we use measurements performed simultaneously in Corsica, Crete and Mallorca to show that the spatial extent of the NPF events are several hundreds of kilometers large. Airborne measurements additionally show that nanoparticles in the marine atmosphere can either be of marine origin or from higher altitudes above the continent.
Sylvain Mailler, Laurent Menut, Dmitry Khvorostyanov, Myrto Valari, Florian Couvidat, Guillaume Siour, Solène Turquety, Régis Briant, Paolo Tuccella, Bertrand Bessagnet, Augustin Colette, Laurent Létinois, Kostantinos Markakis, and Frédérik Meleux
Geosci. Model Dev., 10, 2397–2423, https://doi.org/10.5194/gmd-10-2397-2017, https://doi.org/10.5194/gmd-10-2397-2017, 2017
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CHIMERE is a chemistry-transport model initially designed for box-modelling of the regional atmospheric composition. In the recent years, CHIMERE has been extended to be able to model atmospheric composition at all scales from urban to hemispheric scale, which implied major changes on the coordinate systems as well as on physical processes. This study describes how and why these changes have been brought to the model, largely increasing the range of its possible use.
Amélie Saunier, Elena Ormeño, Christophe Boissard, Henri Wortham, Brice Temime-Roussel, Caroline Lecareux, Alexandre Armengaud, and Catherine Fernandez
Atmos. Chem. Phys., 17, 7555–7566, https://doi.org/10.5194/acp-17-7555-2017, https://doi.org/10.5194/acp-17-7555-2017, 2017
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We investigated the BVOC emissions variations of Quercus Pubescens, under natural and amplified drought, in situ, in order to determine the dependency to light and/or temperature of these emissions. Our results showed that all BVOC emissions were reduced with amplified drought.
Moreover, we highlighted two dependences: (i) light and temperature and (ii) light and temperature during the day and to temperature during the night. These results can be useful to enhance emission models.
Christos Kaltsonoudis, Evangelia Kostenidou, Evangelos Louvaris, Magda Psichoudaki, Epameinondas Tsiligiannis, Kalliopi Florou, Aikaterini Liangou, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 7143–7155, https://doi.org/10.5194/acp-17-7143-2017, https://doi.org/10.5194/acp-17-7143-2017, 2017
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Cooking emissions can be a significant source of particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. More than 99% of the aerosol emitted was composed of organic compounds. The fresh particles were similar to the cooking organic aerosol over Greek cities during the winter, while the reacted particles were similar to those found in the atmosphere during the summer.
Jovanna Arndt, Jean Sciare, Marc Mallet, Greg C. Roberts, Nicolas Marchand, Karine Sartelet, Karine Sellegri, François Dulac, Robert M. Healy, and John C. Wenger
Atmos. Chem. Phys., 17, 6975–7001, https://doi.org/10.5194/acp-17-6975-2017, https://doi.org/10.5194/acp-17-6975-2017, 2017
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The chemical composition of individual PM2.5 particles was measured at a background site on Corsica in the Mediterranean to determine the contribution of different sources to background aerosol in the region. Most of the particles were from fossil fuel combustion and biomass burning, transported to the site from France, Italy and eastern Europe, and also accumulated other species en route. This work shows that largest impact on air quality in the Mediterranean is from anthropogenic emissions.
Laurent Menut, Sylvain Mailler, Bertrand Bessagnet, Guillaume Siour, Augustin Colette, Florian Couvidat, and Frédérik Meleux
Geosci. Model Dev., 10, 1199–1208, https://doi.org/10.5194/gmd-10-1199-2017, https://doi.org/10.5194/gmd-10-1199-2017, 2017
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A simple and complementary model evaluation technique for regional chemistry transport is discussed. The methodology is based on the concept that we can learn about model performance by comparing the simulation results with observational data available for time periods other than the period originally targeted.
Emily A. Bruns, Jay G. Slowik, Imad El Haddad, Dogushan Kilic, Felix Klein, Josef Dommen, Brice Temime-Roussel, Nicolas Marchand, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 705–720, https://doi.org/10.5194/acp-17-705-2017, https://doi.org/10.5194/acp-17-705-2017, 2017
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We characterize primary and aged gaseous emissions from residential wood combustion using proton transfer reaction time-of-flight mass spectrometry. This approach allows for improved characterization, particularly of oxygenated gases, which are a considerable fraction of the total gaseous mass emitted during residential wood combustion. This study is the first thorough characterization of organic gases from this source and provides a benchmark for future studies.
Christos Kaltsonoudis, Evangelia Kostenidou, Kalliopi Florou, Magda Psichoudaki, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 14825–14842, https://doi.org/10.5194/acp-16-14825-2016, https://doi.org/10.5194/acp-16-14825-2016, 2016
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Volatile organic compounds (VOCs) were monitored in urban backgrounds sites, in Athens and Patras in Greece. In summer most of the measured VOCs were due to biogenic and traffic emissions. Winter measurements in Athens revealed that biomass burning used for residential heating was the dominant VOC source. The biomass burning VOC emission ratios and emission factors were estimated.
Laurent Menut, Guillaume Siour, Sylvain Mailler, Florian Couvidat, and Bertrand Bessagnet
Atmos. Chem. Phys., 16, 12961–12982, https://doi.org/10.5194/acp-16-12961-2016, https://doi.org/10.5194/acp-16-12961-2016, 2016
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The aerosol is modelled during the summer 2013 with the WRF and CHIMERE models and over a large area encompassing Africa, Mediterranean sea and west Europe. The modelled aerosol is compared to available measurements such as the AERONET and EMEP networks. The model ability to estimate the aerosol speciation and size distribution is quantified.
Bertrand Bessagnet, Guido Pirovano, Mihaela Mircea, Cornelius Cuvelier, Armin Aulinger, Giuseppe Calori, Giancarlo Ciarelli, Astrid Manders, Rainer Stern, Svetlana Tsyro, Marta García Vivanco, Philippe Thunis, Maria-Teresa Pay, Augustin Colette, Florian Couvidat, Frédérik Meleux, Laurence Rouïl, Anthony Ung, Sebnem Aksoyoglu, José María Baldasano, Johannes Bieser, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Sandro Finardi, Richard Kranenburg, Camillo Silibello, Claudio Carnevale, Wenche Aas, Jean-Charles Dupont, Hilde Fagerli, Lucia Gonzalez, Laurent Menut, André S. H. Prévôt, Pete Roberts, and Les White
Atmos. Chem. Phys., 16, 12667–12701, https://doi.org/10.5194/acp-16-12667-2016, https://doi.org/10.5194/acp-16-12667-2016, 2016
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The EURODELTA III exercise allows a very comprehensive intercomparison and evaluation of air quality models' performance. On average, the models provide a rather good picture of the particulate matter (PM) concentrations over Europe even if the highest concentrations are underestimated. The meteorology is responsible for model discrepancies, while the lack of emissions, particularly in winter, is mentioned as the main reason for the underestimations of PM.
Rachel Gemayel, Stig Hellebust, Brice Temime-Roussel, Nathalie Hayeck, Johannes T. Van Elteren, Henri Wortham, and Sasho Gligorovski
Atmos. Meas. Tech., 9, 1947–1959, https://doi.org/10.5194/amt-9-1947-2016, https://doi.org/10.5194/amt-9-1947-2016, 2016
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LAAP-ToF-MS has been optimized for particle size and number concentration evolution and characterization of the chemical composition of ambient particles by following specific ions.
The advantage of this instrument is that it can analyze the ambient particles online and continuously. It is capable of analyzing inorganic material in ambient particles; in particular the presence of metals can be analyzed. Last but not least, it is a compact and easily transportable tool for field measurements.
Vincent Lemaire, Isabelle Coll, Florian Couvidat, Camille Mouchel-Vallon, Christian Seigneur, and Guillaume Siour
Geosci. Model Dev., 9, 1361–1382, https://doi.org/10.5194/gmd-9-1361-2016, https://doi.org/10.5194/gmd-9-1361-2016, 2016
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Oligomerization is one of the most important identified processes of secondary organic aerosol evolution. We have simulated the formation of oligomers from biogenic precursors, using two different parameterizations implemented in the air quality model CHIMERE. This study shows that oligomer concentration fields are quite sensitive to the way the competition between local formation, evaporation and transport is restituted. The benefits and disadvantages of each approach are discussed in details.
Renee C. McVay, Xuan Zhang, Bernard Aumont, Richard Valorso, Marie Camredon, Yuyi S. La, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 16, 2785–2802, https://doi.org/10.5194/acp-16-2785-2016, https://doi.org/10.5194/acp-16-2785-2016, 2016
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Secondary organic aerosol (SOA) affects climate change, human health, and cloud formation. We examine SOA formation from the biogenic hydrocarbon α-pinene and observe unexpected experimental results that run contrary to model predictions. Various processes are explored via modeling to rationalize the observations. The paper identifies the importance of further constraining via experiments various steps in the chemical mechanism in order to accurately predict SOA worldwide.
Andrea Paciga, Eleni Karnezi, Evangelia Kostenidou, Lea Hildebrandt, Magda Psichoudaki, Gabriella J. Engelhart, Byong-Hyoek Lee, Monica Crippa, André S. H. Prévôt, Urs Baltensperger, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 2013–2023, https://doi.org/10.5194/acp-16-2013-2016, https://doi.org/10.5194/acp-16-2013-2016, 2016
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We estimate the volatility distribution for the organic aerosol (OA) components during summer and winter field campaigns in Paris, France as part of the collaborative project MEGAPOLI. The OA factors (hydrocarbon like OA, cooking OA, marine OA, oxygenated OA) had a broad spectrum of volatilities with no direct link between the average volatility and average oxygen to carbon of the OA components.
L. Brégonzio-Rozier, C. Giorio, F. Siekmann, E. Pangui, S. B. Morales, B. Temime-Roussel, A. Gratien, V. Michoud, M. Cazaunau, H. L. DeWitt, A. Tapparo, A. Monod, and J.-F. Doussin
Atmos. Chem. Phys., 16, 1747–1760, https://doi.org/10.5194/acp-16-1747-2016, https://doi.org/10.5194/acp-16-1747-2016, 2016
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The impact of cloud events on isoprene secondary organic aerosol (SOA) formation has been studied from an isoprene/ NOx/light system in an atmospheric simulation chamber. aqSOA formation can be linked to water soluble volatile organic compounds' dissolution in the aqueous phase and to further aqueous phase reactions. Cloud-induced SOA formation is experimentally demonstrated in this study, thus highlighting the importance of aqueous multiphase systems in atmospheric SOA formation estimations.
Y. S. La, M. Camredon, P. J. Ziemann, R. Valorso, A. Matsunaga, V. Lannuque, J. Lee-Taylor, A. Hodzic, S. Madronich, and B. Aumont
Atmos. Chem. Phys., 16, 1417–1431, https://doi.org/10.5194/acp-16-1417-2016, https://doi.org/10.5194/acp-16-1417-2016, 2016
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The potential impact of chamber walls on the loss of gaseous organic species and secondary organic aerosol (SOA) formation has been explored using the GECKO-A modeling tool, which explicitly represents SOA formation and gas-wall partitioning. The model was compared with 41 smog chamber experiments of SOA formation under OH oxidation of alkane and alkene serie. The organic vapor loss to the chamber walls is found to affect SOA yields as well as the composition of the gas and the particle phase.
E. Kostenidou, K. Florou, C. Kaltsonoudis, M. Tsiflikiotou, S. Vratolis, K. Eleftheriadis, and S. N. Pandis
Atmos. Chem. Phys., 15, 11355–11371, https://doi.org/10.5194/acp-15-11355-2015, https://doi.org/10.5194/acp-15-11355-2015, 2015
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The concentration and chemical composition of fine particulate matter were measured during the summer of 2012 in two Greek cities, Patras and Athens. The composition of PM1 was surprisingly similar in both areas, demonstrating the importance of regional sources. Analysis of the Aerosol Mass Spectrometer data suggested that the contribution of the primary sources to organic aerosol was important (22% in Patras and 35% in Athens) but not dominant.
M. Pikridas, J. Sciare, F. Freutel, S. Crumeyrolle, S.-L. von der Weiden-Reinmüller, A. Borbon, A. Schwarzenboeck, M. Merkel, M. Crippa, E. Kostenidou, M. Psichoudaki, L. Hildebrandt, G. J. Engelhart, T. Petäjä, A. S. H. Prévôt, F. Drewnick, U. Baltensperger, A. Wiedensohler, M. Kulmala, M. Beekmann, and S. N. Pandis
Atmos. Chem. Phys., 15, 10219–10237, https://doi.org/10.5194/acp-15-10219-2015, https://doi.org/10.5194/acp-15-10219-2015, 2015
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Aerosol size distribution measurements from three ground sites, two mobile laboratories, and one airplane are combined to investigate the spatial and temporal variability of ultrafine particles in and around Paris during the summer and winter MEGAPOLI campaigns. The role of nucleation as a particle source and the influence of Paris emissions on their surroundings are examined.
C. Di Biagio, L. Doppler, C. Gaimoz, N. Grand, G. Ancellet, J.-C. Raut, M. Beekmann, A. Borbon, K. Sartelet, J.-L. Attié, F. Ravetta, and P. Formenti
Atmos. Chem. Phys., 15, 9611–9630, https://doi.org/10.5194/acp-15-9611-2015, https://doi.org/10.5194/acp-15-9611-2015, 2015
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Observations from this study indicate that continental pollution largely affects the atmospheric composition and structure of the western Mediterranean basin. Pollution plumes reach 3000-4000 m in altitude and present a very complex and highly stratified structure, characterized by fresh and aged layers both in the boundary layer and in the free troposphere. Also we report the observations of high levels of ultrafine particles over the basin, possibly linked to new particle formation events.
S. Zhu, K. N. Sartelet, and C. Seigneur
Geosci. Model Dev., 8, 1595–1612, https://doi.org/10.5194/gmd-8-1595-2015, https://doi.org/10.5194/gmd-8-1595-2015, 2015
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This article presents the Size-Composition Resolved Aerosol Model (SCRAM) for simulating the dynamics of externally mixed atmospheric particles. The model is first validated by comparison with a reference solution and with results of simulations using internally mixed particles. Then, the importance of representing the mixing state when modelling atmospheric aerosol concentrations is investigated in a box model simulation using data representative of air pollution in Greater Paris.
H. L. DeWitt, S. Hellebust, B. Temime-Roussel, S. Ravier, L. Polo, V. Jacob, C. Buisson, A. Charron, M. André, A. Pasquier, J. L. Besombes, J. L. Jaffrezo, H. Wortham, and N. Marchand
Atmos. Chem. Phys., 15, 4373–4387, https://doi.org/10.5194/acp-15-4373-2015, https://doi.org/10.5194/acp-15-4373-2015, 2015
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By performing source-apportionment modeling, the amount of primary and secondary organic emissions was resolved from a bulk aerosol data set measured adjacent to a major highway in France. Over 70% of vehicles on this highway were diesel, and a high concentration of BC and NOx were measured. Even close to a major highway, the bulk of the aerosol mass was secondary in nature. Radiocarbon data revealed that most of the fossil organic carbon was from primary vehicular emissions and not from SOA.
F. Couvidat and K. Sartelet
Geosci. Model Dev., 8, 1111–1138, https://doi.org/10.5194/gmd-8-1111-2015, https://doi.org/10.5194/gmd-8-1111-2015, 2015
C. Denjean, P. Formenti, B. Picquet-Varrault, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, A. Monod, B. Temime-Roussel, P. Decorse, C. Mangeney, and J. F. Doussin
Atmos. Chem. Phys., 15, 3339–3358, https://doi.org/10.5194/acp-15-3339-2015, https://doi.org/10.5194/acp-15-3339-2015, 2015
L. Brégonzio-Rozier, F. Siekmann, C. Giorio, E. Pangui, S. B. Morales, B. Temime-Roussel, A. Gratien, V. Michoud, S. Ravier, M. Cazaunau, A. Tapparo, A. Monod, and J.-F. Doussin
Atmos. Chem. Phys., 15, 2953–2968, https://doi.org/10.5194/acp-15-2953-2015, https://doi.org/10.5194/acp-15-2953-2015, 2015
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First- and higher order -generation products formed from the oxidation of isoprene and methacrolein with OH radicals in the presence of NOx have been studied in a simulation chamber. Differences in light source are proposed to partially explain the discrepancies observed between different studies in the literature for both isoprene- and methacrolein-SOA mass yields. According to our results, these SOA yields in the atmosphere could be lower than suggested by most of the current chamber studies.
C. Denjean, P. Formenti, B. Picquet-Varrault, M. Camredon, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, B. Temime-Roussel, A. Monod, B. Aumont, and J. F. Doussin
Atmos. Chem. Phys., 15, 883–897, https://doi.org/10.5194/acp-15-883-2015, https://doi.org/10.5194/acp-15-883-2015, 2015
P. Renard, F. Siekmann, G. Salque, C. Demelas, B. Coulomb, L. Vassalo, S. Ravier, B. Temime-Roussel, D. Voisin, and A. Monod
Atmos. Chem. Phys., 15, 21–35, https://doi.org/10.5194/acp-15-21-2015, https://doi.org/10.5194/acp-15-21-2015, 2015
Y. Wang, K. N. Sartelet, M. Bocquet, P. Chazette, M. Sicard, G. D'Amico, J. F. Léon, L. Alados-Arboledas, A. Amodeo, P. Augustin, J. Bach, L. Belegante, I. Binietoglou, X. Bush, A. Comerón, H. Delbarre, D. García-Vízcaino, J. L. Guerrero-Rascado, M. Hervo, M. Iarlori, P. Kokkalis, D. Lange, F. Molero, N. Montoux, A. Muñoz, C. Muñoz, D. Nicolae, A. Papayannis, G. Pappalardo, J. Preissler, V. Rizi, F. Rocadenbosch, K. Sellegri, F. Wagner, and F. Dulac
Atmos. Chem. Phys., 14, 12031–12053, https://doi.org/10.5194/acp-14-12031-2014, https://doi.org/10.5194/acp-14-12031-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
Y. Wang, K. N. Sartelet, M. Bocquet, and P. Chazette
Atmos. Chem. Phys., 14, 3511–3532, https://doi.org/10.5194/acp-14-3511-2014, https://doi.org/10.5194/acp-14-3511-2014, 2014
P. Kupiszewski, C. Leck, M. Tjernström, S. Sjogren, J. Sedlar, M. Graus, M. Müller, B. Brooks, E. Swietlicki, S. Norris, and A. Hansel
Atmos. Chem. Phys., 13, 12405–12431, https://doi.org/10.5194/acp-13-12405-2013, https://doi.org/10.5194/acp-13-12405-2013, 2013
E. Kostenidou, C. Kaltsonoudis, M. Tsiflikiotou, E. Louvaris, L. M. Russell, and S. N. Pandis
Atmos. Chem. Phys., 13, 8797–8811, https://doi.org/10.5194/acp-13-8797-2013, https://doi.org/10.5194/acp-13-8797-2013, 2013
Y. Zhang, K. Sartelet, S.-Y. Wu, and C. Seigneur
Atmos. Chem. Phys., 13, 6807–6843, https://doi.org/10.5194/acp-13-6807-2013, https://doi.org/10.5194/acp-13-6807-2013, 2013
Y. Zhang, K. Sartelet, S. Zhu, W. Wang, S.-Y. Wu, X. Zhang, K. Wang, P. Tran, C. Seigneur, and Z.-F. Wang
Atmos. Chem. Phys., 13, 6845–6875, https://doi.org/10.5194/acp-13-6845-2013, https://doi.org/10.5194/acp-13-6845-2013, 2013
A. Waked, C. Seigneur, F. Couvidat, Y. Kim, K. Sartelet, C. Afif, A. Borbon, P. Formenti, and S. Sauvage
Atmos. Chem. Phys., 13, 5873–5886, https://doi.org/10.5194/acp-13-5873-2013, https://doi.org/10.5194/acp-13-5873-2013, 2013
E. Solazzo, R. Bianconi, G. Pirovano, M. D. Moran, R. Vautard, C. Hogrefe, K. W. Appel, V. Matthias, P. Grossi, B. Bessagnet, J. Brandt, C. Chemel, J. H. Christensen, R. Forkel, X. V. Francis, A. B. Hansen, S. McKeen, U. Nopmongcol, M. Prank, K. N. Sartelet, A. Segers, J. D. Silver, G. Yarwood, J. Werhahn, J. Zhang, S. T. Rao, and S. Galmarini
Geosci. Model Dev., 6, 791–818, https://doi.org/10.5194/gmd-6-791-2013, https://doi.org/10.5194/gmd-6-791-2013, 2013
F. Couvidat, Y. Kim, K. Sartelet, C. Seigneur, N. Marchand, and J. Sciare
Atmos. Chem. Phys., 13, 983–996, https://doi.org/10.5194/acp-13-983-2013, https://doi.org/10.5194/acp-13-983-2013, 2013
Y. Wang, K. N. Sartelet, M. Bocquet, and P. Chazette
Atmos. Chem. Phys., 13, 269–283, https://doi.org/10.5194/acp-13-269-2013, https://doi.org/10.5194/acp-13-269-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
The lifetimes and potential change in planetary albedo owing to the oxidation of organic films extracted from atmospheric aerosol by hydroyxl (OH) radical oxidation at the air-water interface of aerosol particles
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photooxidation: Remarkably enhancing effects of seeds and ammonia
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement Report: Changes of ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice core record
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
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We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
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This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Rosalie Shepherd, Martin King, Andrew Ward, Edward Stuckey, Rebecca Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2367, https://doi.org/10.5194/egusphere-2024-2367, 2024
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Thin film formation at the air-water interface from material extracted from atmospheric aerosol was demonstrated, supporting core-shell morphology. The film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 hour. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top of the atmosphere albedo for urban films.
Si Zhang, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2119, https://doi.org/10.5194/egusphere-2024-2119, 2024
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SOA from acetone photooxidation can be formed more readily on neutral aerosols than on acidic aerosols, while heterogeneous reaction of carbonyl with ammonium is only active on acidic aerosols in the presence of NH3, which produces light-absorbing N-containing compounds. Our work suggested that the heterogeneous oxidation of highly volatile VOC, for example acetone, is an importance source of SOA in the atmosphere, which should be accounted for in the future model studies.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
EGUsphere, https://doi.org/10.5194/egusphere-2024-1381, https://doi.org/10.5194/egusphere-2024-1381, 2024
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A record of ammonium covering the years 1750 to 2008 was extracted from a 182-meter-long ice core drilled in 2009 at Mt. Elbrus in the Caucasus, Russia. Changes in ammonia emissions in southeastern Europe during the pre-industrial and industrial periods were investigated. The level of ammonium in 1750 indicates a significant contribution of natural sources to the ammonia budget, contrasting with present-day conditions, where agricultural emissions outweigh those from biogenic sources in Europe.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
EGUsphere, https://doi.org/10.5194/egusphere-2024-1880, https://doi.org/10.5194/egusphere-2024-1880, 2024
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The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolite and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
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Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
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The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
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Couvidat, F., Debry, É., Sartelet, K., and Seigneur, C.: A hydrophilic/hydrophobic organic (H2O) aerosol model: Development, evaluation and sensitivity analysis, J. Geophys. Res., 117, D10304, https://doi.org/10.1029/2011JD017214, 2012.
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Short summary
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.
Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from...
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