Articles | Volume 17, issue 6
https://doi.org/10.5194/acp-17-4305-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-4305-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
30 Mar 2017
Research article |
| 30 Mar 2017
Chemical transport model simulations of organic aerosol in southern California: model evaluation and gasoline and diesel source contributions
Shantanu H. Jathar
CORRESPONDING AUTHOR
Mechanical Engineering, Colorado State University, Fort Collins, CO 80525, USA
Matthew Woody
US Environmental Protection Agency, Research Triangle Park, NC 27711, USA
Havala O. T. Pye
US Environmental Protection Agency, Research Triangle Park, NC 27711, USA
Kirk R. Baker
US Environmental Protection Agency, Research Triangle Park, NC 27711, USA
Mechanical Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, USA
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T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
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Christopher A. Emery, Kirk R. Baker, Gary M. Wilson, and Greg Yarwood
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Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
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Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
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Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Forwood Wiser, Bryan K. Place, Siddhartha Sen, Havala O. T. Pye, Benjamin Yang, Daniel M. Westervelt, Daven K. Henze, Arlene M. Fiore, and V. Faye McNeill
Geosci. Model Dev., 16, 1801–1821, https://doi.org/10.5194/gmd-16-1801-2023, https://doi.org/10.5194/gmd-16-1801-2023, 2023
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We developed a reduced model of atmospheric isoprene oxidation, AMORE-Isoprene 1.0. It was created using a new Automated Model Reduction (AMORE) method designed to simplify complex chemical mechanisms with minimal manual adjustments to the output. AMORE-Isoprene 1.0 has improved accuracy and similar size to other reduced isoprene mechanisms. When included in the CRACMM mechanism, it improved the accuracy of EPA’s CMAQ model predictions for the northeastern USA compared to observations.
Peeyush Khare, Jordan E. Krechmer, Jo E. Machesky, Tori Hass-Mitchell, Cong Cao, Junqi Wang, Francesca Majluf, Felipe Lopez-Hilfiker, Sonja Malek, Will Wang, Karl Seltzer, Havala O. T. Pye, Roisin Commane, Brian C. McDonald, Ricardo Toledo-Crow, John E. Mak, and Drew R. Gentner
Atmos. Chem. Phys., 22, 14377–14399, https://doi.org/10.5194/acp-22-14377-2022, https://doi.org/10.5194/acp-22-14377-2022, 2022
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Ammonium adduct chemical ionization is used to examine the atmospheric abundances of oxygenated volatile organic compounds associated with emissions from volatile chemical products, which are now key contributors of reactive precursors to ozone and secondary organic aerosols in urban areas. The application of this valuable measurement approach in densely populated New York City enables the evaluation of emissions inventories and thus the role these oxygenated compounds play in urban air quality.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Michael Cheeseman, Bonne Ford, Zoey Rosen, Eric Wendt, Alex DesRosiers, Aaron J. Hill, Christian L'Orange, Casey Quinn, Marilee Long, Shantanu H. Jathar, John Volckens, and Jeffrey R. Pierce
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-751, https://doi.org/10.5194/acp-2021-751, 2021
Revised manuscript not accepted
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This article predicts concentrations of airborne particulate matter over wintertime Denver, CO, USA, using meteorological and geographic information, as well as low-cost aerosol optical depth (AOD) measurements captured by citizen scientists. Machine learning methods revealed that low boundary layer heights and stagnant air were the best predictors of poor air quality, while AOD provided little skill in predicting particulate matter for this location and time period.
Eric A. Wendt, Casey Quinn, Christian L'Orange, Daniel D. Miller-Lionberg, Bonne Ford, Jeffrey R. Pierce, John Mehaffy, Michael Cheeseman, Shantanu H. Jathar, David H. Hagan, Zoey Rosen, Marilee Long, and John Volckens
Atmos. Meas. Tech., 14, 6023–6038, https://doi.org/10.5194/amt-14-6023-2021, https://doi.org/10.5194/amt-14-6023-2021, 2021
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Fine particulate matter air pollution is one of the leading contributors to adverse health outcomes on the planet. Here, we describe the design and validation of a low-cost, compact, and autonomous instrument capable of measuring particulate matter levels directly, via mass sampling, and optically, via mass and sunlight extinction measurements. We demonstrate the instrument's accuracy relative to reference measurements and its potential for community-level sampling.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Xiaoyang Chen, Yang Zhang, Kai Wang, Daniel Tong, Pius Lee, Youhua Tang, Jianping Huang, Patrick C. Campbell, Jeff Mcqueen, Havala O. T. Pye, Benjamin N. Murphy, and Daiwen Kang
Geosci. Model Dev., 14, 3969–3993, https://doi.org/10.5194/gmd-14-3969-2021, https://doi.org/10.5194/gmd-14-3969-2021, 2021
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The continuously updated National Air Quality Forecast Capability (NAQFC) provides air quality forecasts. To support the development of the next-generation NAQFC, we evaluate a prototype of GFSv15-CMAQv5.0.2. The performance and the potential improvements for the system are discussed. This study can provide a scientific basis for further development of NAQFC and help it to provide more accurate air quality forecasts to the public over the contiguous United States.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
Preprint withdrawn
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
Anna L. Hodshire, Emily Ramnarine, Ali Akherati, Matthew L. Alvarado, Delphine K. Farmer, Shantanu H. Jathar, Sonia M. Kreidenweis, Chantelle R. Lonsdale, Timothy B. Onasch, Stephen R. Springston, Jian Wang, Yang Wang, Lawrence I. Kleinman, Arthur J. Sedlacek III, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 6839–6855, https://doi.org/10.5194/acp-21-6839-2021, https://doi.org/10.5194/acp-21-6839-2021, 2021
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Biomass burning emits particles and vapors that can impact both health and climate. Here, we investigate the role of dilution in the evolution of aerosol size and composition in observed US wildfire smoke plumes. Centers of plumes dilute more slowly than edges. We see differences in concentrations and composition between the centers and edges both in the first measurement and in subsequent measurements. Our findings support the hypothesis that plume dilution influences smoke aging.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Rongzhi Tang, Quanyang Lu, Song Guo, Hui Wang, Kai Song, Ying Yu, Rui Tan, Kefan Liu, Ruizhe Shen, Shiyi Chen, Limin Zeng, Spiro D. Jorga, Zhou Zhang, Wenbin Zhang, Shijin Shuai, and Allen L. Robinson
Atmos. Chem. Phys., 21, 2569–2583, https://doi.org/10.5194/acp-21-2569-2021, https://doi.org/10.5194/acp-21-2569-2021, 2021
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We performed chassis dynamometer experiments to investigate the emissions and secondary organic aerosol (SOA) formation potential of intermediate volatility organic compounds (IVOCs) from an on-road Chinese gasoline vehicle. High IVOC emission factors (EFs) and distinct volatility distribution were recognized. Our results indicate that vehicular IVOCs contribute significantly to SOA, implying the importance of reducing IVOCs when making air pollution control policies in urban areas of China.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Quanyang Lu, Benjamin N. Murphy, Momei Qin, Peter J. Adams, Yunliang Zhao, Havala O. T. Pye, Christos Efstathiou, Chris Allen, and Allen L. Robinson
Atmos. Chem. Phys., 20, 4313–4332, https://doi.org/10.5194/acp-20-4313-2020, https://doi.org/10.5194/acp-20-4313-2020, 2020
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This research work investigates organic aerosol formation in California during the CalNex study. We update the chemical transport model with the most recent mobile-source emission data and introduce a simple parameterization for secondary organic aerosol formed from intermediate-volatility organic compounds. Our results highlight the important contribution of IVOCs to SOA production in the Los Angeles region but underscore that other uncertainties must be addressed to close the SOA mass balance.
Joseph R. Salazar, Benton T. Cartledge, John P. Haynes, Rachel York-Marini, Allen L. Robinson, Greg T. Drozd, Allen H. Goldstein, Sirine C. Fakra, and Brian J. Majestic
Atmos. Chem. Phys., 20, 1849–1860, https://doi.org/10.5194/acp-20-1849-2020, https://doi.org/10.5194/acp-20-1849-2020, 2020
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The solubility of atmospheric iron is important in human health and environmental chemistry. To understand the origin of water-soluble iron in urban areas, tailpipe emissions were collected from 32 low-emitting vehicles, from which iron solubility averaged 30 % (0–82 %), more than 10 times the average in the Earth's crust. Water-soluble iron was independent of almost all exhaust components and of the iron phase in the particles but was correlated with specific exhaust-derived organic compounds.
Bonne Ford, Jeffrey R. Pierce, Eric Wendt, Marilee Long, Shantanu Jathar, John Mehaffy, Jessica Tryner, Casey Quinn, Lizette van Zyl, Christian L'Orange, Daniel Miller-Lionberg, and John Volckens
Atmos. Meas. Tech., 12, 6385–6399, https://doi.org/10.5194/amt-12-6385-2019, https://doi.org/10.5194/amt-12-6385-2019, 2019
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This study demonstrates the use of a low-cost sensor in a citizen-science network, Citizen-Enabled Aerosol Measurements for Satellites (CEAMS), to measure air quality in participants’ backyards. The pilot network was conducted in the fall and winter of 2017 in northern Colorado. Measurements of aerosols taken by the citizens are also compared to standard air quality instruments.
Eric A. Wendt, Casey W. Quinn, Daniel D. Miller-Lionberg, Jessica Tryner, Christian L'Orange, Bonne Ford, Azer P. Yalin, Jeffrey R. Pierce, Shantanu Jathar, and John Volckens
Atmos. Meas. Tech., 12, 5431–5441, https://doi.org/10.5194/amt-12-5431-2019, https://doi.org/10.5194/amt-12-5431-2019, 2019
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We introduce a low-cost, compact device (aerosol mass and optical depth (AMOD) sampler) that can be used by citizen scientists to measure air quality. Our paper discusses the development and different components for measuring aerosols. It also shows that measurements made by the AMOD next to reference-grade monitors agreed within 10 %. Coupled with the cost of these instruments, this agreement demonstrates that the AMOD can be widely deployed to monitor air quality by citizen scientists.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
Quanyang Lu, Yunliang Zhao, and Allen L. Robinson
Atmos. Chem. Phys., 18, 17637–17654, https://doi.org/10.5194/acp-18-17637-2018, https://doi.org/10.5194/acp-18-17637-2018, 2018
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This work combines previously published data to illustrate the mechanics of emission from internal combustion engine sources. Engine exhaust can be decomposed into combustion "by-product", "unburned fuel" and "oil" modes. Intermediate and semi-volatile organic compounds are included to create comprehensive model-ready organic emission profiles. Gasoline and gas-turbine engine emissions are enriched in intermediate volatile organic compounds relative to unburned fuel.
Rishabh U. Shah, Ellis S. Robinson, Peishi Gu, Allen L. Robinson, Joshua S. Apte, and Albert A. Presto
Atmos. Chem. Phys., 18, 16325–16344, https://doi.org/10.5194/acp-18-16325-2018, https://doi.org/10.5194/acp-18-16325-2018, 2018
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We measured spatial differences in airborne particulate matter (PM) in Oakland, CA, with repeated mobile measurements on all city streets. In addition to primary, we also find higher secondary organic PM downtown, which suggests stronger photochemical PM production in areas of high emissions and poor air ventilation (i.e., urban street canyons). This finding is original because while other modeling studies have predicted higher photochemistry in street canyons, we confirm this observationally.
Sailaja Eluri, Christopher D. Cappa, Beth Friedman, Delphine K. Farmer, and Shantanu H. Jathar
Atmos. Chem. Phys., 18, 13813–13838, https://doi.org/10.5194/acp-18-13813-2018, https://doi.org/10.5194/acp-18-13813-2018, 2018
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As oxidation flow reactors (OFRs) are increasingly used to study aerosol formation and evolution in laboratory and field environments, there is a need to develop models that can be used to interpret OFR data. In this work, we evaluate two coupled chemistry and thermodynamic models to simulate secondary organic aerosol formation (SOA) from diluted diesel exhaust and explore the sources, pathways, and processes important to SOA formation.
Lu Xu, Havala O. T. Pye, Jia He, Yunle Chen, Benjamin N. Murphy, and Nga Lee Ng
Atmos. Chem. Phys., 18, 12613–12637, https://doi.org/10.5194/acp-18-12613-2018, https://doi.org/10.5194/acp-18-12613-2018, 2018
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In this study, we integrate lab-in-the-field experiments, extensive ambient ground measurements, and state-of-the-art modeling to constrain the concentration of organic aerosol from biogenic monoterpenes and sesquiterpenes. Further, we show that the organic aerosol from the investigated sources accounts for roughly 20 % of the World Health Organization PM2.5 standard in the southeastern US.
Penglin Ye, Yunliang Zhao, Wayne K. Chuang, Allen L. Robinson, and Neil M. Donahue
Atmos. Chem. Phys., 18, 6171–6186, https://doi.org/10.5194/acp-18-6171-2018, https://doi.org/10.5194/acp-18-6171-2018, 2018
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This work describes experiments to constrain the production of secondary organic aerosol from pinanediol, a semi-volatile oxidation product of α-pinene. Our results and the implications for SOA aging are directly relevant to the atmospheric chemistry community because they connect new-particle formation experiments and SOA formation experiments. The oxidation conditions are typically different and experiments are also influenced in different ways by wall losses of condensible vapors.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Naomi Zimmerman, Albert A. Presto, Sriniwasa P. N. Kumar, Jason Gu, Aliaksei Hauryliuk, Ellis S. Robinson, Allen L. Robinson, and R. Subramanian
Atmos. Meas. Tech., 11, 291–313, https://doi.org/10.5194/amt-11-291-2018, https://doi.org/10.5194/amt-11-291-2018, 2018
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Low-cost sensors promise neighborhood-scale air quality monitoring but have been plagued by inconsistent performance for precision, accuracy, and drift. CMU and SenSevere collaborated to develop the RAMP, which uses electrochemical sensors. We present a machine learning algorithm that overcomes previous performance issues and meets US EPA's data quality recommendations for personal exposure for NO2 and tougher "supplemental monitoring" standards for CO & ozone across 19 RAMPs for several months.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
Prettiny K. Ma, Yunliang Zhao, Allen L. Robinson, David R. Worton, Allen H. Goldstein, Amber M. Ortega, Jose L. Jimenez, Peter Zotter, André S. H. Prévôt, Sönke Szidat, and Patrick L. Hayes
Atmos. Chem. Phys., 17, 9237–9259, https://doi.org/10.5194/acp-17-9237-2017, https://doi.org/10.5194/acp-17-9237-2017, 2017
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Airborne particulate matter (PM) negatively impacts air quality in cities throughout the world. An important fraction of PM is organic aerosol. We have evaluated and developed several new models for secondary organic aerosol (SOA), which is formed from the chemical processing of gaseous precursors. Using our model results, we have quantified important SOA sources and precursors and also identified possible model parameterizations that could be used for air quality predictions.
Shantanu H. Jathar, Christopher Heppding, Michael F. Link, Delphine K. Farmer, Ali Akherati, Michael J. Kleeman, Joost A. de Gouw, Patrick R. Veres, and James M. Roberts
Atmos. Chem. Phys., 17, 8959–8970, https://doi.org/10.5194/acp-17-8959-2017, https://doi.org/10.5194/acp-17-8959-2017, 2017
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Our work makes novel emissions measurements of isocyanic acid, a toxic gas, from a modern-day diesel engine and finds that diesel engines emit isocyanic acid but the emissions control devices do not enhance or destroy the isocyanic acid. Air quality model calculations suggest that diesel engines are possibly important sources of isocyanic acid in urban environments although the isocyanic acid levels are ten times lower than levels linked to adverse human health effects.
Qijing Bian, Shantanu H. Jathar, John K. Kodros, Kelley C. Barsanti, Lindsay E. Hatch, Andrew A. May, Sonia M. Kreidenweis, and Jeffrey R. Pierce
Atmos. Chem. Phys., 17, 5459–5475, https://doi.org/10.5194/acp-17-5459-2017, https://doi.org/10.5194/acp-17-5459-2017, 2017
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In this paper, we perform simulations of the evolution of biomass-burning organic aerosol in laboratory smog-chamber experiments and ambient plumes. We find that in smog-chamber experiments, vapor wall losses lead to a large reduction in the apparent secondary organic aerosol formation. In ambient plumes, fire size and meteorology regulate the plume dilution rate, primary organic aerosol evaporation rate, and secondary organic aerosol formation rate.
Jianlin Hu, Shantanu Jathar, Hongliang Zhang, Qi Ying, Shu-Hua Chen, Christopher D. Cappa, and Michael J. Kleeman
Atmos. Chem. Phys., 17, 5379–5391, https://doi.org/10.5194/acp-17-5379-2017, https://doi.org/10.5194/acp-17-5379-2017, 2017
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Organic aerosol is a major constituent of ultrafine particulate matter (PM0.1). In this study, a source-oriented air quality model was used to simulate the concentrations and sources of primary and secondary organic aerosols in PM0.1 in California for a 9-year modeling period to provide useful information for epidemiological studies to further investigate the associations with health outcomes.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Kathleen M. Fahey, Annmarie G. Carlton, Havala O. T. Pye, Jaemeen Baek, William T. Hutzell, Charles O. Stanier, Kirk R. Baker, K. Wyat Appel, Mohammed Jaoui, and John H. Offenberg
Geosci. Model Dev., 10, 1587–1605, https://doi.org/10.5194/gmd-10-1587-2017, https://doi.org/10.5194/gmd-10-1587-2017, 2017
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Chemical transport models (CTMs) are a crucial tool in understanding links between emissions, air quality, and climate. Only a simple description of cloud chemistry has been implemented in many of these; however, clouds play a major role in the physicochemical processing of atmospheric species. In CMAQ, EPA’s widely used CTM, the cloud code is limited to the treatment of simple chemistry. We update CMAQ clouds to consider additional chemistry and then examine regional impacts of these updates.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Jesse O. Bash, Kirk R. Baker, and Melinda R. Beaver
Geosci. Model Dev., 9, 2191–2207, https://doi.org/10.5194/gmd-9-2191-2016, https://doi.org/10.5194/gmd-9-2191-2016, 2016
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Biogenic volatile organic compounds (BVOCs) participate in reactions that can lead to secondarily formed ozone and particulate matter impacting air quality and climate and are important inputs for atmospheric models. BVOC emissions are sensitive to the vegetation species and leaf temperature. Here, we have improved the vegetation data and modeled leaf temperature of the Biogenic Emission Inventory System model. Updated algorithms improved model evaluation against observations in California.
Matthew C. Woody, Kirk R. Baker, Patrick L. Hayes, Jose L. Jimenez, Bonyoung Koo, and Havala O. T. Pye
Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, https://doi.org/10.5194/acp-16-4081-2016, 2016
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In this work, organic aerosol (OA) predictions from the volatility basis set (VBS) module in the CMAQ photochemical transport model were evaluated against routine monitoring data and measurements collected during the 2010 CalNex field study. We found that the VBS module more accurately reproduced the observed primary/secondary OA split and secondary OA (SOA) mass at the CalNex Pasadena ground site compared to the traditional CMAQ OA module but still underpredicted observed SOA by ~ 5.2 ×.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Atmos. Chem. Phys., 16, 2309–2322, https://doi.org/10.5194/acp-16-2309-2016, https://doi.org/10.5194/acp-16-2309-2016, 2016
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Multi-generational chemistry schemes applied in regional models do not increase secondary organic aerosol (SOA) mass production relative to traditional "two-product" schemes when both models are fitted to the same chamber data. The multi-generational chemistry schemes do change the predicted composition of SOA and the source attribution of SOA.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, https://doi.org/10.5194/gmd-8-2553-2015, 2015
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Multi-generational oxidation of organic vapors can significantly alter the mass, chemical composition and properties of secondary organic aerosol (SOA). Here, we implement a semi-explicit, constrained multi-generational oxidation model of Cappa and Wilson (2012) in a 3-D air quality model. When compared with results from a current-generation SOA model, we predict similar mass concentrations of SOA but a different chemical composition. O:C ratios of SOA are in line with those measured globally.
M. C. Woody, J. J. West, S. H. Jathar, A. L. Robinson, and S. Arunachalam
Atmos. Chem. Phys., 15, 6929–6942, https://doi.org/10.5194/acp-15-6929-2015, https://doi.org/10.5194/acp-15-6929-2015, 2015
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Utilizing an aircraft-specific parameterization based on smog chamber data in a regional AQM, contributions of non-traditional secondary organic aerosols (NTSOA) from aircraft emissions of semi-volatile and intermediate volatility organic compounds were assessed. NTSOA, a previously unaccounted component of PM2.5 in most AQMs, contributed up to 7.4% of aviation-attributable PM2.5 at the airport and rose to 17.9% downwind, suggesting its significance in aviation-attributed PM2.5 at all scales.
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
J. R. Roscioli, T. I. Yacovitch, C. Floerchinger, A. L. Mitchell, D. S. Tkacik, R. Subramanian, D. M. Martinez, T. L. Vaughn, L. Williams, D. Zimmerle, A. L. Robinson, S. C. Herndon, and A. J. Marchese
Atmos. Meas. Tech., 8, 2017–2035, https://doi.org/10.5194/amt-8-2017-2015, https://doi.org/10.5194/amt-8-2017-2015, 2015
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This report presents an overview and detailed description of the measurement methods, analysis approach, and example data from a 10-week EDF-sponsored field campaign measuring methane emissions from natural gas gathering and processing facilities across the US. The dual-tracer ratio method was employed to quantify methane release rates and identify emission sources at a wide variety of facilities, using downwind measurements of CH4, C2H6, CO2, and CO with N2O and C2H2 as tracers.
R. H. F. Kwok, K. R. Baker, S. L. Napelenok, and G. S. Tonnesen
Geosci. Model Dev., 8, 99–114, https://doi.org/10.5194/gmd-8-99-2015, https://doi.org/10.5194/gmd-8-99-2015, 2015
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The implementation and application of the Integrated Source Apportionment Method (ISAM) for O3 and its precursors for the Community Multiscale Air Quality (CMAQ) model are described. CMAQ-ISAM is a hybrid of source apportionment and source sensitivity in that O3 production is attributed to precursor sources based on the O3 formation regime. CMAQ-ISAM offers a source attribution tool for the purposes of quantifying and understanding sources and impacts of regional air pollution.
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
C. E. Stockwell, R. J. Yokelson, S. M. Kreidenweis, A. L. Robinson, P. J. DeMott, R. C. Sullivan, J. Reardon, K. C. Ryan, D. W. T. Griffith, and L. Stevens
Atmos. Chem. Phys., 14, 9727–9754, https://doi.org/10.5194/acp-14-9727-2014, https://doi.org/10.5194/acp-14-9727-2014, 2014
B. N. Murphy, N. M. Donahue, A. L. Robinson, and S. N. Pandis
Atmos. Chem. Phys., 14, 5825–5839, https://doi.org/10.5194/acp-14-5825-2014, https://doi.org/10.5194/acp-14-5825-2014, 2014
S. H. Jathar, N. M. Donahue, P. J. Adams, and A. L. Robinson
Atmos. Chem. Phys., 14, 5771–5780, https://doi.org/10.5194/acp-14-5771-2014, https://doi.org/10.5194/acp-14-5771-2014, 2014
A. A. Presto, T. D. Gordon, and A. L. Robinson
Atmos. Chem. Phys., 14, 5015–5036, https://doi.org/10.5194/acp-14-5015-2014, https://doi.org/10.5194/acp-14-5015-2014, 2014
T. D. Gordon, A. A. Presto, N. T. Nguyen, W. H. Robertson, K. Na, K. N. Sahay, M. Zhang, C. Maddox, P. Rieger, S. Chattopadhyay, H. Maldonado, M. M. Maricq, and A. L. Robinson
Atmos. Chem. Phys., 14, 4643–4659, https://doi.org/10.5194/acp-14-4643-2014, https://doi.org/10.5194/acp-14-4643-2014, 2014
T. D. Gordon, A. A. Presto, A. A. May, N. T. Nguyen, E. M. Lipsky, N. M. Donahue, A. Gutierrez, M. Zhang, C. Maddox, P. Rieger, S. Chattopadhyay, H. Maldonado, M. M. Maricq, and A. L. Robinson
Atmos. Chem. Phys., 14, 4661–4678, https://doi.org/10.5194/acp-14-4661-2014, https://doi.org/10.5194/acp-14-4661-2014, 2014
B. H. Henderson, F. Akhtar, H. O. T. Pye, S. L. Napelenok, and W. T. Hutzell
Geosci. Model Dev., 7, 339–360, https://doi.org/10.5194/gmd-7-339-2014, https://doi.org/10.5194/gmd-7-339-2014, 2014
J. Rissman, S. Arunachalam, M. Woody, J. J. West, T. BenDor, and F. S. Binkowski
Atmos. Chem. Phys., 13, 9285–9302, https://doi.org/10.5194/acp-13-9285-2013, https://doi.org/10.5194/acp-13-9285-2013, 2013
R. Saleh, C. J. Hennigan, G. R. McMeeking, W. K. Chuang, E. S. Robinson, H. Coe, N. M. Donahue, and A. L. Robinson
Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, https://doi.org/10.5194/acp-13-7683-2013, 2013
K. W. Appel, G. A. Pouliot, H. Simon, G. Sarwar, H. O. T. Pye, S. L. Napelenok, F. Akhtar, and S. J. Roselle
Geosci. Model Dev., 6, 883–899, https://doi.org/10.5194/gmd-6-883-2013, https://doi.org/10.5194/gmd-6-883-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Implications of reduced-complexity aerosol thermodynamics on organic aerosol mass concentration and composition over North America
Trends and drivers of soluble iron deposition from East Asian dust to the Northwest Pacific: a springtime analysis (2001–2017)
Modelling of atmospheric variability in gas and aerosols during the ACROSS campaign 2022 of the greater Paris area: evaluation of the meteorology, dynamics and chemistry
Spatial–temporal patterns in anthropogenic and biomass burning emission contributions to air pollution and mortality burden changes in India from 1995 to 2014
A comprehensive global modeling assessment of nitrate heterogeneous formation on desert dust
AERO-MAP: a data compilation and modeling approach to understand spatial variability in fine- and coarse-mode aerosol composition
Long-term trends in aerosol properties derived from AERONET measurements
Impacts of sea ice leads on sea salt aerosols and atmospheric chemistry in the Arctic
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
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
Competing multiple oxidation pathways shape atmospheric limonene-derived organonitrates simulated with updated explicit chemical mechanisms
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
Incorporation of multi-phase halogen chemistry into Community Multiscale Air Quality (CMAQ) model
Atmospheric fate of organosulfates through gas-phase and aqueous-phase reaction with hydroxyl radicals: implications in inorganic sulfate formation
Changes in the impacts of ship emissions on PM2.5 and its components in China under the staged fuel oil policies
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
Source-explicit estimation of brown carbon in the polluted atmosphere over North China Plain: implications for distribution, absorption and direct radiative effect
Aerosol Composition Trends during 2000–2020: In depth insights from model predictions and multiple worldwide observation datasets
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
Exploring Atmospheric Nitrate Formation Mechanisms during the Winters of 2013 and 2018 in the North China Region via Modeling and Isotopic Analysis
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
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
Opinion: The Impact of AerChemMIP on Climate and Air Quality Research
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
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
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
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
Atmos. Chem. Phys., 25, 5773–5792, https://doi.org/10.5194/acp-25-5773-2025, https://doi.org/10.5194/acp-25-5773-2025, 2025
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We implemented the BAT-VBS (Binary Activity Thermodynamics volatility basis set) aerosol thermodynamics model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake, nonideal mixing, and impacts on the gas–particle partitioning of semi-volatile organics. Compared to GEOS-Chem's complex (dry) scheme, we show that the BAT-VBS model can predict substantial enhancements in organic aerosol mass concentration at moderate-to-high relative humidity.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
Atmos. Chem. Phys., 25, 5175–5197, https://doi.org/10.5194/acp-25-5175-2025, https://doi.org/10.5194/acp-25-5175-2025, 2025
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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. The study underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
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 L. Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
Atmos. Chem. Phys., 25, 4803–4831, https://doi.org/10.5194/acp-25-4803-2025, https://doi.org/10.5194/acp-25-4803-2025, 2025
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The summer of 2022 has been considered a proxy for future climate scenarios due to its hot and dry conditions. In this paper, we use the measurements from the Atmospheric Chemistry of the Suburban Forest (ACROSS) campaign, conducted in the Paris area in June–July 2022, along with observations from existing networks, to evaluate a 3D chemistry transport model (WRF–CHIMERE) simulation. Results are shown to be satisfactory, allowing us to explain the gas and aerosol variability at the campaign sites.
Bin Luo, Yuqiang Zhang, Tao Tang, Hongliang Zhang, Jianlin Hu, Jiangshan Mu, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 25, 4767–4783, https://doi.org/10.5194/acp-25-4767-2025, https://doi.org/10.5194/acp-25-4767-2025, 2025
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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 underscores the urgent need for localized policies to protect public health amid escalating environmental challenges.
Rubén Soussé Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 25, 4719–4753, https://doi.org/10.5194/acp-25-4719-2025, https://doi.org/10.5194/acp-25-4719-2025, 2025
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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.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, P. Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter 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-Gómez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal L. Weagle, and Xi Zhao
Atmos. Chem. Phys., 25, 4665–4702, https://doi.org/10.5194/acp-25-4665-2025, https://doi.org/10.5194/acp-25-4665-2025, 2025
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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 being 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 data sets to model output.
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
Atmos. Chem. Phys., 25, 4617–4637, https://doi.org/10.5194/acp-25-4617-2025, https://doi.org/10.5194/acp-25-4617-2025, 2025
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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 sources over northern India; and increased dust activity over the Arabian Peninsula.
Erin J. Emme and Hannah M. Horowitz
Atmos. Chem. Phys., 25, 4531–4545, https://doi.org/10.5194/acp-25-4531-2025, https://doi.org/10.5194/acp-25-4531-2025, 2025
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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 that sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
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. Winski, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
Atmos. Chem. Phys., 25, 4083–4106, https://doi.org/10.5194/acp-25-4083-2025, https://doi.org/10.5194/acp-25-4083-2025, 2025
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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 model 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.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 25, 3919–3928, https://doi.org/10.5194/acp-25-3919-2025, https://doi.org/10.5194/acp-25-3919-2025, 2025
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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 timescales. Its application in Changzhou, China, revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residuals.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, Kan Huang, and Minghuai Wang
Atmos. Chem. Phys., 25, 3857–3872, https://doi.org/10.5194/acp-25-3857-2025, https://doi.org/10.5194/acp-25-3857-2025, 2025
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Understanding long-term organic aerosol (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 (SOAs) and an 8.1 % decrease in primary organic aerosols (POAs), 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.
Qinghao Guo, Haofei Zhang, Bo Long, Lehui Cui, Yiyang Sun, Hao Liu, Yaxin Liu, Yunting Xiao, Pingqing Fu, and Jialei Zhu
EGUsphere, https://doi.org/10.5194/egusphere-2025-1058, https://doi.org/10.5194/egusphere-2025-1058, 2025
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Limonene, a natural compound from plants, reacts with pollutants to form airborne particles that influence air quality and climate. Using advanced models with explicit chemical mechanisms, we show how different reaction pathways shape organonitrate formation, with some increasing and others decreasing particle levels. This approach enhancing predictions of pollution and climate impacts while deepening our understanding of how natural and human-made emissions interact in the atmosphere.
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).
Kiyeon Kim, Chul Han Song, Kyung Man Han, Greg Yarwood, Ross Beardsley, and Saewung Kim
EGUsphere, https://doi.org/10.5194/egusphere-2025-23, https://doi.org/10.5194/egusphere-2025-23, 2025
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Despite the crucial role of halogen radicals in the atmosphere, the current CMAQ model does not account for multi-phase halogen processes. To address this issue, we incorporated 177 halogen reactions, together with anthropogenic and natural halogen emissions into the CMAQ model. Our findings reveal that incorporation of these halogen processes significantly improves model performances compared to ground observations. In addition, we emphasize the influence of halogen radicals on air quality.
Narcisse Tsona Tchinda, Xiaofan Lv, Stanley Numboniu Tasheh, Julius Numboniu Ghogomu, and Lin Du
EGUsphere, https://doi.org/10.5194/egusphere-2025-29, https://doi.org/10.5194/egusphere-2025-29, 2025
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This study examines the chemical transformation of selected organosulfates by reactions with HO• radicals both in the gas-phase and in the aqueous-phase. Results show that the nature of the substituents on the carbon chain can effectively alter the decomposition of organosulfates and ozone is highlighted as a key oxidant in the intermediate steps of this decomposition. The primary products from these reactions include inorganic sulfate and carbonyl compounds.
Guangyuan Yu, Yan Zhang, Qian Wang, Zimin Han, Shenglan Jiang, Fan Yang, Xin Yang, and Cheng Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3892, https://doi.org/10.5194/egusphere-2024-3892, 2025
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China has carried out staged low-sulfur fuel policies since 2017. This study simulated the changing spatiotemporal patterns of the impacts of ship emissions on PM2.5 from 2017 to 2021 based on the updated emission inventories and mapping of chemical species in the CMAQ. Fuel policies caused evident relative changes in inorganic and organic components of the shipping-related PM2.5 over China’s port cities. The driving factors of the interannual, seasonal, and diurnal patterns were discussed.
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.
Jiamao Zhou, Jiarui Wu, Xiaoli Su, Ruonan Wang, Xia Li, Qian Jiang, Ting Zhang, Wenting Dai, Junji Cao, Xuexi Tie, and Guohui Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3468, https://doi.org/10.5194/egusphere-2024-3468, 2024
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Brown carbon (BrC) is a type of airborne particle produced from various combustion sources which is light absorption. Historically, climate models have categorizing organic particles as either non-absorbing or purely reflective. Our study shows that BrC can reduce the usual cooling effect of organic particles. While BrC is often linked to biomass burning, however, BrC from fossil fuels contributes significantly to atmospheric heating.
Alexandra P. Tsimpidi, Susanne M. C. Scholz, Alexandros Milousis, Nikolaos Mihalopoulos, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3590, https://doi.org/10.5194/egusphere-2024-3590, 2024
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This study examines global changes in air pollution from 2000 to 2020, focusing on fine aerosols that impact climate and health. Using models and global data, it finds organic aerosols dominate in many regions, especially with wildfires or natural emissions. Pollution from sulfate and nitrate has decreased in Europe and North America due to regulations, while trends in Asia are more complex. The findings improve understanding and support policies for cleaner air and healthier environments.
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.
Zhenze Liu, Jianhua Qi, Yuanzhe Ni, Likun Xue, and Xiaohuan Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-3044, https://doi.org/10.5194/egusphere-2024-3044, 2024
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Our study explores the formation of nitrate in the atmosphere of inland and coastal cities in China during the winters of 2013 & 2018. Through air quality modelling & isotope analysis, we found regional differences between these cities; coastal cities show another contribution from the heterogeneous reaction of dinitrogen pentoxide (N2O5). It turns out that the combined reduction of nitrogen oxides (NOx), volatile organic compounds (VOCs) and ammonia (NH3) is critical to reducing nitrate levels.
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.
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.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael J. Prather, Alexander T. Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Christopher J. Smith, Steven T. Turnock, Duncan Watson-Parris, and Paul J. Young
EGUsphere, https://doi.org/10.5194/egusphere-2024-2528, https://doi.org/10.5194/egusphere-2024-2528, 2024
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The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. In this paper, we review its contribution to AR6, and the wider understanding of the role of these species in climate and climate change. We identify remaining challenges concluding with recommendations aimed to improve the utility and uptake of climate model data to address the role of short-lived climate forcers in the Earth system.
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.
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.
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
Short summary
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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.
Cited articles
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Short summary
Mobile sources such as cars and trucks are large sources of pollution in cities, but it is unclear what their relative contribution to organic particle pollution is. We used a numerical model along with recent data gathered from tests performed on cars and trucks to calculate organic particle levels in southern California. We found that model calculations agreed better with measurements and gasoline cars and trucks dominated the organic particle pollution.
Mobile sources such as cars and trucks are large sources of pollution in cities, but it is...
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