Articles | Volume 21, issue 13
https://doi.org/10.5194/acp-21-10199-2021
© Author(s) 2021. 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-21-10199-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
07 Jul 2021
Research article |
| 07 Jul 2021
| 07 Jul 2021
Estimation of secondary organic aerosol viscosity from explicit modeling of gas-phase oxidation of isoprene and α-pinene
Tommaso Galeazzo
Department of Chemistry, University of California Irvine, Irvine, CA 92625, USA
Richard Valorso
Univ Paris Est Creteil and Université de Paris, CNRS, LISA, 94010 Créteil, France
Department of Chemistry, University of California Irvine, Irvine, CA 92625, USA
Marie Camredon
Univ Paris Est Creteil and Université de Paris, CNRS, LISA, 94010 Créteil, France
Bernard Aumont
Univ Paris Est Creteil and Université de Paris, CNRS, LISA, 94010 Créteil, France
Department of Chemistry, University of California Irvine, Irvine, CA 92625, USA
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Tenglong Shi, Jiayao Wang, Daizhou Zhang, Jiecan Cui, Zihang Wang, Yue Zhou, Wei Pu, Yang Bai, Zhigang Han, Meng Liu, Yanbiao Liu, Hongbin Xie, Minghui Yang, Ying Li, Meng Gao, and Xin Wang
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This study examines the properties of dust in snow in Changchun, China, using advanced technology to analyze its size, shape, and light absorption. We found that dust composition affects how much heat is absorbed by snow, with certain minerals, like hematite, making snow melt faster. Our research highlights the importance of creating clear standards for classifying dust, which could improve climate models and field observations. This work helps better understand dust's role in climate change.
Mega Octaviani, Benjamin A. Musa Bandowe, Qing Mu, Jake Wilson, Holger Tost, Hang Su, Yafang Cheng, Manabu Shiraiwa, Ulrich Pöschl, Thomas Berkemeier, and Gerhard Lammel
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This research explores the atmospheric concentration of benzo(a)pyrene (BaP), a harmful air pollutant linked to lung cancer. Using advanced Earth system modeling, the study examines how BaP's degradation varies with temperature and humidity, affecting its global distribution and associated lung cancer risks. The findings reveal that BaP persists longer in colder, less humid regions, leading to higher lung cancer risks in parts of Europe and Asia.
Zichen Wu, Xueshun Chen, Zifa Wang, Huansheng Chen, Zhe Wang, Qing Mu, Lin Wu, Wending Wang, Xiao Tang, Jie Li, Ying Li, Qizhong Wu, Yang Wang, Zhiyin Zou, and Zijian Jiang
Geosci. Model Dev., 17, 8885–8907, https://doi.org/10.5194/gmd-17-8885-2024, https://doi.org/10.5194/gmd-17-8885-2024, 2024
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Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2024-3272, https://doi.org/10.5194/egusphere-2024-3272, 2024
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
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.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
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.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
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Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
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.
Emily B. Franklin, Lindsay D. Yee, Bernard Aumont, Robert J. Weber, Paul Grigas, and Allen H. Goldstein
Atmos. Meas. Tech., 15, 3779–3803, https://doi.org/10.5194/amt-15-3779-2022, https://doi.org/10.5194/amt-15-3779-2022, 2022
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The composition of atmospheric aerosols are extremely complex, containing hundreds of thousands of estimated individual compounds. The majority of these compounds have never been catalogued in widely used databases, making them extremely difficult for atmospheric chemists to identify and analyze. In this work, we present Ch3MS-RF, a machine-learning-based model to enable characterization of complex mixtures and prediction of structure-specific properties of unidentifiable organic compounds.
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.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys., 21, 11467–11487, https://doi.org/10.5194/acp-21-11467-2021, https://doi.org/10.5194/acp-21-11467-2021, 2021
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This is the first mechanistic modeling study of secondary organic aerosol (SOA) from the understudied monoterpene, camphene. The semi-explicit chemical model GECKO-A predicted camphene SOA yields that were ~2 times α-pinene. Using 50/50 α-pinene + limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA when camphene is a dominant monoterpene.
Qiaorong Xie, Sihui Su, Jing Chen, Yuqing Dai, Siyao Yue, Hang Su, Haijie Tong, Wanyu Zhao, Lujie Ren, Yisheng Xu, Dong Cao, Ying Li, Yele Sun, Zifa Wang, Cong-Qiang Liu, Kimitaka Kawamura, Guibin Jiang, Yafang Cheng, and Pingqing Fu
Atmos. Chem. Phys., 21, 11453–11465, https://doi.org/10.5194/acp-21-11453-2021, https://doi.org/10.5194/acp-21-11453-2021, 2021
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This study investigated the role of nighttime chemistry during Chinese New Year's Eve that enhances the formation of nitrooxy organosulfates in the aerosol phase. Results show that anthropogenic precursors, together with biogenic ones, considerably contribute to the formation of low-volatility nitrooxy OSs. Our study provides detailed molecular composition of firework-related aerosols, which gives new insights into the physicochemical properties and potential health effects of urban aerosols.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys., 21, 6175–6198, https://doi.org/10.5194/acp-21-6175-2021, https://doi.org/10.5194/acp-21-6175-2021, 2021
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This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
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Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
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Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
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.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
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.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
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We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Peter Bräuer, Camille Mouchel-Vallon, Andreas Tilgner, Anke Mutzel, Olaf Böge, Maria Rodigast, Laurent Poulain, Dominik van Pinxteren, Ralf Wolke, Bernard Aumont, and Hartmut Herrmann
Atmos. Chem. Phys., 19, 9209–9239, https://doi.org/10.5194/acp-19-9209-2019, https://doi.org/10.5194/acp-19-9209-2019, 2019
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The article presents a new protocol for computer-assisted automated aqueous-phase chemistry mechanism generation, which has been validated against chamber experiments. Together with a large kinetics database and improved prediction methods for kinetic data, the novel protocol provides an unmatched tool for detailed studies of tropospheric aqueous-phase chemistry in complex model studies and for the design and analysis of chamber experiments.
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
Ying Li and Manabu Shiraiwa
Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, https://doi.org/10.5194/acp-19-5959-2019, 2019
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Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under various temperatures and relative humidities. Equilibration timescales in free troposphere can be longer than hours or days, even at moderate or relatively high relative humidities. These results provide critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in chemical transport models.
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.
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.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
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The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
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We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
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In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
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Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
David O. Topping, James Allan, M. Rami Alfarra, and Bernard Aumont
Geosci. Model Dev., 10, 2365–2377, https://doi.org/10.5194/gmd-10-2365-2017, https://doi.org/10.5194/gmd-10-2365-2017, 2017
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Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. In this proof of concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated to facilitate improved model evaluation. The study demonstrates the use of a methodology that would be improved with more training data and data from simple mixed systems.
Camille Mouchel-Vallon, Laurent Deguillaume, Anne Monod, Hélène Perroux, Clémence Rose, Giovanni Ghigo, Yoann Long, Maud Leriche, Bernard Aumont, Luc Patryl, Patrick Armand, and Nadine Chaumerliac
Geosci. Model Dev., 10, 1339–1362, https://doi.org/10.5194/gmd-10-1339-2017, https://doi.org/10.5194/gmd-10-1339-2017, 2017
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The Cloud Explicit Physico-chemical Scheme (CLEPS 1.0) describes oxidation of water-soluble organic compounds resulting from isoprene oxidation. It is based on structure activity relationships (SARs) (global rate constants and branching ratios for HO• abstraction and addition) and GROMHE SAR (Henry's law constants for undocumented species). It is coupled to the MCM gas phase mechanism and is included in a model using the DSMACC model and KPP to analyze experimental and field data.
Andrea M. Arangio, Haijie Tong, Joanna Socorro, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, https://doi.org/10.5194/acp-16-13105-2016, 2016
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We have quantified environmentally persistent free radicals and reactive oxygen species (ROS) in size-segregated atmospheric aerosol particles. We suggest that ROS were formed by decomposition of secondary organic aerosols interacting with transition metal ions and quinones contained in humic-like substances. The results have significant implications for aqueous-phase and cloud processing of organic aerosols as well as adverse health effects upon respiratory deposition of aerosol particles.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
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Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
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.
David Topping, Mark Barley, Michael K. Bane, Nicholas Higham, Bernard Aumont, Nicholas Dingle, and Gordon McFiggans
Geosci. Model Dev., 9, 899–914, https://doi.org/10.5194/gmd-9-899-2016, https://doi.org/10.5194/gmd-9-899-2016, 2016
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In this paper we describe the development and application of a new web-based and open-source facility, UManSysProp (http://umansysprop .seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include pure component vapour pressures, critical properties, and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic-organic liquid systems; hygroscopic growth factors and CCN activation potential.
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
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We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
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.
Y. Tang, J. An, F. Wang, Y. Li, Y. Qu, Y. Chen, and J. Lin
Atmos. Chem. Phys., 15, 9381–9398, https://doi.org/10.5194/acp-15-9381-2015, https://doi.org/10.5194/acp-15-9381-2015, 2015
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High daytime HONO mixing ratios in experiments suggest that an unknown daytime HONO source (P unknown) could exist. P unknown≈19.60×NO2×J(NO2) was obtained using observed data from 13 field experiments across the globe, then coupled into the WRF-Chem model. Simulations indicated that elevated P unknown was found in the coastal regions of China; the additional HONO sources, especially the P unknown produced significant increases of radicals in the major cities, and accelerated the radical cycles.
A. Hodzic, S. Madronich, P. S. Kasibhatla, G. Tyndall, B. Aumont, J. L. Jimenez, J. Lee-Taylor, and J. Orlando
Atmos. Chem. Phys., 15, 9253–9269, https://doi.org/10.5194/acp-15-9253-2015, https://doi.org/10.5194/acp-15-9253-2015, 2015
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Our study combines process and global chemistry modeling to investigate the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Photolysis of the oxidation intermediates that partition between gas and particle phases to form SOA is not included in 3D models. Our results suggest that exposure to UV light can suppress the formation of SOA or even lead to its substantial loss (comparable to wet deposition).
E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae
Atmos. Chem. Phys., 15, 8847–8869, https://doi.org/10.5194/acp-15-8847-2015, https://doi.org/10.5194/acp-15-8847-2015, 2015
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Our manuscript describes the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the ZOTTO in central Siberia (61º N, 89º E). The hygroscopic growth measurements were supplemented with chemical analyses of the samples. In addition, the microstructure and chemical composition of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM).
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
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
J. Lee-Taylor, A. Hodzic, S. Madronich, B. Aumont, M. Camredon, and R. Valorso
Atmos. Chem. Phys., 15, 595–615, https://doi.org/10.5194/acp-15-595-2015, https://doi.org/10.5194/acp-15-595-2015, 2015
T. Berkemeier, M. Shiraiwa, U. Pöschl, and T. Koop
Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, https://doi.org/10.5194/acp-14-12513-2014, 2014
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Glassy organic particles can serve as ice nuclei at low temperatures. We provide a rationale for these findings using a numerical aerosol diffusion model that describes particle phase state and its kinetics during simulated atmospheric updrafts dependent upon composition, size, updraft velocity, temperature and humidity. Our simulations suggest that aerosols from anthropogenic aromatic organics can be particularly relevant for ice cloud formation.
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
V. Michoud, A. Colomb, A. Borbon, K. Miet, M. Beekmann, M. Camredon, B. Aumont, S. Perrier, P. Zapf, G. Siour, W. Ait-Helal, C. Afif, A. Kukui, M. Furger, J. C. Dupont, M. Haeffelin, and J. F. Doussin
Atmos. Chem. Phys., 14, 2805–2822, https://doi.org/10.5194/acp-14-2805-2014, https://doi.org/10.5194/acp-14-2805-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
C. Mouchel-Vallon, P. Bräuer, M. Camredon, R. Valorso, S. Madronich, H. Herrmann, and B. Aumont
Atmos. Chem. Phys., 13, 1023–1037, https://doi.org/10.5194/acp-13-1023-2013, https://doi.org/10.5194/acp-13-1023-2013, 2013
V. Michoud, A. Kukui, M. Camredon, A. Colomb, A. Borbon, K. Miet, B. Aumont, M. Beekmann, R. Durand-Jolibois, S. Perrier, P. Zapf, G. Siour, W. Ait-Helal, N. Locoge, S. Sauvage, C. Afif, V. Gros, M. Furger, G. Ancellet, and J. F. Doussin
Atmos. Chem. Phys., 12, 11951–11974, https://doi.org/10.5194/acp-12-11951-2012, https://doi.org/10.5194/acp-12-11951-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Population exposure to outdoor NO2, black carbon, and ultrafine and fine particles over Paris with multi-scale modelling down to the street scale
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States
Critical load exceedances for North America and Europe using an ensemble of models and an investigation of causes of environmental impact estimate variability: an AQMEII4 study
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
The surface tension and cloud condensation nuclei (CCN) activation of sea spray aerosol particles
Exploring the processes controlling secondary inorganic aerosol: evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Driving factors of aerosol acidity: a new hierarchical quantitative analysis framework and its application in Changzhou, China
Understanding the Long-term Trend of Organic Aerosol and the Influences from Anthropogenic Emission and Regional Climate Change in China
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Trends and Drivers of Soluble Iron Deposition from East Asian Dust to the Northwest Pacific: A Springtime Analysis (2001–2017)
Impacts of Sea Ice Leads on Sea Salt Aerosols and Atmospheric Chemistry in the Arctic
Implications of Reduced-Complexity Aerosol Thermodynamics on Organic Aerosol Mass Concentration and Composition over North America
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
A Comprehensive Global Modelling Assessment of Nitrate Heterogeneous Formation on Desert Dust
Modelling of atmospheric variability of gas and aerosols during the ACROSS campaign 2022 in the greater Paris area: evaluation of the meteorology, dynamics and chemistry
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Long-term trends in aerosol properties derived from AERONET measurements
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Unveiling the optimal regression model for source apportionment of the oxidative potential of PM10
AERO-MAP: A data compilation and modelling approach to understand spatial variability in fine and coarse mode aerosol composition
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 2: Modeling chemical drivers and 3-D new particle formation occurrence
Technical note: Influence of different averaging metrics and temporal resolutions on the aerosol pH calculated by thermodynamic modeling
Dual roles of the inorganic aqueous phase on secondary organic aerosol growth from benzene and phenol
Global source apportionment of aerosols into major emission regions and sectors over 1850–2017
Modeling atmospheric brown carbon in the GISS ModelE Earth system model
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Spatial-temporal patterns of anthropogenic and biomass burning contributions on air pollution and mortality burden changes in India from 1995 to 2014
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
Soo-Jin Park, Lya Lugon, Oscar Jacquot, Youngseob Kim, Alexia Baudic, Barbara D'Anna, Ludovico Di Antonio, Claudia Di Biagio, Fabrice Dugay, Olivier Favez, Véronique Ghersi, Aline Gratien, Julien Kammer, Jean-Eudes Petit, Olivier Sanchez, Myrto Valari, Jérémy Vigneron, and Karine Sartelet
Atmos. Chem. Phys., 25, 3363–3387, https://doi.org/10.5194/acp-25-3363-2025, https://doi.org/10.5194/acp-25-3363-2025, 2025
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To accurately represent the population exposure to outdoor concentrations of pollutants of interest to health (NO2, PM2.5, black carbon, and ultrafine particles), multi-scale modelling down to the street scale is set up and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing regional-scale simulations to be corrected to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon, and ultrafine particles but less strongly PM2.5.
Sara L. Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, and Kathleen Fahey
Atmos. Chem. Phys., 25, 3287–3312, https://doi.org/10.5194/acp-25-3287-2025, https://doi.org/10.5194/acp-25-3287-2025, 2025
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters is improved.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark W. Shephard, Ranjeet S. Sokhi, and Stefano Galmarini
Atmos. Chem. Phys., 25, 3049–3107, https://doi.org/10.5194/acp-25-3049-2025, https://doi.org/10.5194/acp-25-3049-2025, 2025
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The large range of sulfur and nitrogen deposition estimates from air quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulfur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by hydrometeors, aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, gas deposition via plant cuticles and soil, and land use data.
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
EGUsphere, https://doi.org/10.5194/egusphere-2024-3584, https://doi.org/10.5194/egusphere-2024-3584, 2024
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Aerosol acidity is an important parameter in atmospheric chemistry, while its driving factors, especially chemical profiles versus meteorological conditions, are not yet fully understood. Here, we established a hierarchical quantitative analysis framework to understand the driving factors of aerosol acidity on different time scales. Its application in Changzhou, China revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residues.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3420, https://doi.org/10.5194/egusphere-2024-3420, 2024
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Understanding long-term organic aerosols (OA) trends and their driving factors is important for air quality management. Our modeling revealed that OA in China increased by 5.6% from 1990 to 2019, primarily due to a 32.3% increase in secondary organic aerosols (SOA) and an 8.1% decrease in primary organic aerosols (POA), both largely driven by changes in anthropogenic emissions. Biogenic SOA increased due to warming but showed little response to changes in anthropogenic nitrogen oxide emissions.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Sijia Lou, Manish Shrivastava, Alexandre Albinet, Sophie Tomaz, Deepchandra Srivastava, Olivier Favez, Huizhong Shen, and Aijun Ding
EGUsphere, https://doi.org/10.5194/egusphere-2024-3269, https://doi.org/10.5194/egusphere-2024-3269, 2024
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PAHs, emitted from incomplete combustion, pose serious health risks due to their carcinogenic properties. This research demonstrates that viscous organic aerosol coatings significantly hinder PAH oxidation, with spatial distributions sensitive to the degradation modelling approach. Our findings underscore the importance of accurately modelling these processes for risk assessments, highlighting the need to consider both fresh and oxidized PAHs in evaluating human exposure and health risks.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2293, https://doi.org/10.5194/egusphere-2024-2293, 2024
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Dust soluble iron deposition from East Asia plays an important role in the marine ecology of the Northwest Pacific. Using the developed model, our findings highlight a dual trend: a decrease in the overall deposition of soluble iron from dust, but an increase in the solubility of the iron itself due to the enhanced atmospheric processing. It underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
Erin Emme and Hannah Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-3147, https://doi.org/10.5194/egusphere-2024-3147, 2024
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There is uncertainty in the sources of Arctic cold season (November-April) sea salt aerosols. Using a chemical transport model and satellite observations, we quantify Arctic-wide sea salt aerosol emissions from fractures in sea ice, called open sea ice leads, and their atmospheric chemistry impacts for the cold season. We show sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-2712, https://doi.org/10.5194/egusphere-2024-2712, 2024
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Organic aerosol water content impacts the gas–particle partitioning of semivolatile organics. We used an aerosol thermodynamic model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake and nonideal mixing. This led to a substantial enhancement in mean organic aerosol mass concentration with respect to GEOS-Chem's most advanced scheme. The water-sensitive scheme could be a valuable tool for reconciling model estimations and field measurements.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winksi, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2024-3026, https://doi.org/10.5194/egusphere-2024-3026, 2024
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a models to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Rubén Soussé-Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
EGUsphere, https://doi.org/10.5194/egusphere-2024-2310, https://doi.org/10.5194/egusphere-2024-2310, 2024
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Desert dust forms nitrate coatings as it travels through the atmosphere. However, current models that predict this process vary greatly due to different methods and inaccuracies. We examined how nitrate forms in a global model, focusing on how gases condense on dust, the lifespan of different particles, and the impact of alkalinity. Our findings show that models work best when they consider reversible gas condensation with alkalinity. This should lead to better estimates of climate impacts.
Ludovico Di Antonio, Matthias Beekmann, Guillaume Siour, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Joel F. de Brito, Paola Formenti, Cecile Gaimoz, Olivier Garret, Aline Gratien, Valérie Gros, Martial Haeffelin, Lelia N. Hawkins, Simone Kotthaus, Gael Noyalet, Diana Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
EGUsphere, https://doi.org/10.5194/egusphere-2024-2175, https://doi.org/10.5194/egusphere-2024-2175, 2024
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Summer 2022 has been considered a proxy for future climate scenarios, given the registered hot and dry conditions. In this paper, we used the measurements from the ACROSS campaign, occurred over the Paris area in June–July 2022, in addition to observations from existing networks, to evaluate the WRF–CHIMERE model simulation over France and the Ile-de-France regions. Results over the Ile–de–France show to be satisfactory, allowing to explain the gas and aerosol variability at the ACROSS sites.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Zhenyu Zhang, Jing Li, Huizheng Che, Yueming Dong, Oleg Dubovik, Thomas Eck, Pawan Gupta, Brent Holben, Jhoon Kim, Elena Lind, Trailokya Saud, Sachchida Nand Tripathi, and Tong Ying
EGUsphere, https://doi.org/10.5194/egusphere-2024-2533, https://doi.org/10.5194/egusphere-2024-2533, 2024
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We used ground-based remote sensing data from the Aerosol Robotic Network to examine long-term trends in aerosol characteristics. We found aerosol loadings generally decreased globally, and aerosols became more scattering. These changes are closely related to variations in aerosol compositions, such as decreased anthropogenic emissions over East Asia, Europe, and North America, increased anthropogenic source over North India, increased dust activities over the Arabian Peninsula, etc.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Vy Dinh Ngoc Thuy, Jean-Luc Jaffrezo, Ian Hough, Pamela A. Dominutti, Guillaume Salque Moreton, Grégory Gille, Florie Francony, Arabelle Patron-Anquez, Olivier Favez, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 7261–7282, https://doi.org/10.5194/acp-24-7261-2024, https://doi.org/10.5194/acp-24-7261-2024, 2024
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The capacity of particulate matter (PM) to generate reactive oxygen species in vivo is represented by oxidative potential (OP). This study focuses on finding the appropriate model to evaluate the oxidative character of PM sources in six sites using the PM sources and OP. Eight regression techniques are introduced to assess the OP of PM. The study highlights the importance of selecting a model according to the input data characteristics and establishes some recommendations for the procedure.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-1617, https://doi.org/10.5194/egusphere-2024-1617, 2024
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output.
Ming Chu, Xing Wei, Shangfei Hai, Yang Gao, Huiwang Gao, Yujiao Zhu, Biwu Chu, Nan Ma, Juan Hong, Yele Sun, and Xiaohong Yao
Atmos. Chem. Phys., 24, 6769–6786, https://doi.org/10.5194/acp-24-6769-2024, https://doi.org/10.5194/acp-24-6769-2024, 2024
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We used a 20-bin WRF-Chem model to simulate NPF events in the NCP during a three-week observational period in the summer of 2019. The model was able to reproduce the observations during June 29–July 6, which was characterized by a high frequency of NPF occurrence.
Haoqi Wang, Xiao Tian, Wanting Zhao, Jiacheng Li, Haoyu Yu, Yinchang Feng, and Shaojie Song
Atmos. Chem. Phys., 24, 6583–6592, https://doi.org/10.5194/acp-24-6583-2024, https://doi.org/10.5194/acp-24-6583-2024, 2024
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pH is a key property of ambient aerosols, which affect many atmospheric processes. As aerosol pH is a non-conservative parameter, diverse averaging metrics and temporal resolutions may influence the pH values calculated by thermodynamic models. This technical note seeks to quantitatively evaluate the average pH using varied metrics and resolutions. The ultimate goal is to establish standardized reporting practices in future research endeavors.
Jiwon Choi, Myoseon Jang, and Spencer Blau
Atmos. Chem. Phys., 24, 6567–6582, https://doi.org/10.5194/acp-24-6567-2024, https://doi.org/10.5194/acp-24-6567-2024, 2024
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Persistent phenoxy radical (PPR), formed by phenol gas oxidation and its aqueous reaction, catalytically destroys O3 and retards secondary organic aerosol (SOA) growth. Explicit gas mechanisms including the formation of PPR and low-volatility products from the oxidation of phenol or benzene are applied to the UNIPAR model to predict SOA mass via multiphase reactions of precursors. Aqueous reactions of reactive organics increase SOA mass but retard SOA growth via heterogeneously formed PPR.
Yang Yang, Shaoxuan Mou, Hailong Wang, Pinya Wang, Baojie Li, and Hong Liao
Atmos. Chem. Phys., 24, 6509–6523, https://doi.org/10.5194/acp-24-6509-2024, https://doi.org/10.5194/acp-24-6509-2024, 2024
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The variations in anthropogenic aerosol concentrations and source contributions and their subsequent radiative impact in major emission regions during historical periods are quantified based on an aerosol-tagging system in E3SMv1. Due to the industrial development and implementation of economic policies, sources of anthropogenic aerosols show different variations, which has important implications for pollution prevention and control measures and decision-making for global collaboration.
Maegan A. DeLessio, Kostas Tsigaridis, Susanne E. Bauer, Jacek Chowdhary, and Gregory L. Schuster
Atmos. Chem. Phys., 24, 6275–6304, https://doi.org/10.5194/acp-24-6275-2024, https://doi.org/10.5194/acp-24-6275-2024, 2024
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This study presents the first explicit representation of brown carbon aerosols in the GISS ModelE Earth system model (ESM). Model sensitivity to a range of brown carbon parameters and model performance compared to AERONET and MODIS retrievals of total aerosol properties were assessed. A summary of best practices for incorporating brown carbon into ModelE is also included.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
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.
Bin Luo, Yuqiang Zhang, Tao Tang, Hongliang Zhang, Jianlin Hu, Jiangshan Mu, Wenxing Wang, and Likun Xue
EGUsphere, https://doi.org/10.5194/egusphere-2024-974, https://doi.org/10.5194/egusphere-2024-974, 2024
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India is facing a severe air pollution crisis that poses significant health risks, particularly from PM2.5 and O3. Our study reveals rising levels of both pollutants from 1995 to 2014, leading to increased premature mortality. While anthropogenic emissions play a significant role, biomass burning also impacts air quality, in particular seasons and regions in India. This study highlights the urgent need for localized policies to protect public health amid escalating environmental challenges.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
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Short summary
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.
We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and...
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