Articles | Volume 18, issue 19
https://doi.org/10.5194/acp-18-13813-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-13813-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
01 Oct 2018
Research article |
| 01 Oct 2018
| 01 Oct 2018
Modeling the formation and composition of secondary organic aerosol from diesel exhaust using parameterized and semi-explicit chemistry and thermodynamic models
Sailaja Eluri
Department of Mechanical Engineering, Colorado State University, Fort Collins, CO, 80523, USA
Christopher D. Cappa
Department of Civil and Environmental Engineering, University of California Davis, Davis, CA, 95616, USA
Beth Friedman
Department of Chemistry, Colorado State University, Fort Collins, CO, 80523, USA
Delphine K. Farmer
Department of Chemistry, Colorado State University, Fort Collins, CO, 80523, USA
Shantanu H. Jathar
CORRESPONDING AUTHOR
Department of Mechanical Engineering, Colorado State University, Fort Collins, CO, 80523, USA
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Atmos. Chem. Phys., 24, 12881–12901, https://doi.org/10.5194/acp-24-12881-2024, https://doi.org/10.5194/acp-24-12881-2024, 2024
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The magnitude and evolution of brown carbon (BrC) absorption remain unclear, with uncertainty in climate models. Data from the WE-CAN airborne experiment show that model parameterizations overestimate the mass absorption cross section (MAC) of BrC. Observed decreases in BrC absorption with chemical markers are due to decreasing organic aerosol (OA) mass rather than a decreasing BrC MAC, which is currently implemented in models. Water-soluble BrC contributes 23 % of total absorption at 660 nm.
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
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Kathryn A. Moore, Thomas C. J. Hill, Samantha Greeney, Chamika K. Madawala, Raymond J. Leibensperger III, Christopher D. Cappa, M. Dale Stokes, Grant B. Deane, Christopher Lee, Alexei V. Tivanski, Kimberly A. Prather, and Paul J. DeMott
EGUsphere, https://doi.org/10.5194/egusphere-2024-2159, https://doi.org/10.5194/egusphere-2024-2159, 2024
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This article presents results from the first study in a new wind-wave channel at the Scripps Institution of Oceanography. The experiment tested how wind speed over the ocean surface influences production of sea spray particles, which are important for radiative forcing and cloud formation in the atmosphere. We found that particle concentration and chemical composition varied with winds speed, and the changes were driven by changes in wind and wave-breaking rather seawater biology or chemistry.
Ryan N. Farley, James E. Lee, Laura-Hélèna Rivellini, Alex K. Y. Lee, Rachael Dal Porto, Christopher D. Cappa, Kyle Gorkowski, Abu Sayeed Md Shawon, Katherine B. Benedict, Allison C. Aiken, Manvendra K. Dubey, and Qi Zhang
Atmos. Chem. Phys., 24, 3953–3971, https://doi.org/10.5194/acp-24-3953-2024, https://doi.org/10.5194/acp-24-3953-2024, 2024
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The black carbon aerosol composition and mixing state were characterized using a soot particle aerosol mass spectrometer. Single-particle measurements revealed the major role of atmospheric processing in modulating the black carbon mixing state. A significant fraction of soot particles were internally mixed with oxidized organic aerosol and sulfate, with implications for activation as cloud nuclei.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
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Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
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
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
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
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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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.
Erin K. Boedicker, Holly M. DeBolt, Ryan Fulgam, Ethan W. Emerson, and Delphine K. Farmer
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-431, https://doi.org/10.5194/acp-2022-431, 2022
Preprint withdrawn
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We present particle flux and size-resolved dry deposition measurements from a pine forest for all four major seasons. Dry deposition of particles was highest in the winter and was significantly elevated compared to the summer data. Several mechanisms were investigated to determine what effects were driving the enhanced deposition in the winter. We show that the wintertime changes are likely caused by changes in plant physiology and needle structure that increase the influence of interception.
Delaney B. Kilgour, Gordon A. Novak, Jon S. Sauer, Alexia N. Moore, Julie Dinasquet, Sarah Amiri, Emily B. Franklin, Kathryn Mayer, Margaux Winter, Clare K. Morris, Tyler Price, Francesca Malfatti, Daniel R. Crocker, Christopher Lee, Christopher D. Cappa, Allen H. Goldstein, Kimberly A. Prather, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 1601–1613, https://doi.org/10.5194/acp-22-1601-2022, https://doi.org/10.5194/acp-22-1601-2022, 2022
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We report measurements of gas-phase volatile organosulfur molecules made during a mesocosm phytoplankton bloom experiment. Dimethyl sulfide (DMS), methanethiol (MeSH), and benzothiazole accounted for on average over 90 % of total gas-phase sulfur emissions. This work focuses on factors controlling the production and emission of DMS and MeSH and the role of non-DMS molecules (such as MeSH and benzothiazole) in secondary sulfate formation in coastal marine environments.
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.
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.
Mj Riches, Daniel Lee, and Delphine K. Farmer
Atmos. Meas. Tech., 13, 4123–4139, https://doi.org/10.5194/amt-13-4123-2020, https://doi.org/10.5194/amt-13-4123-2020, 2020
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This paper presents a thorough characterization of a leaf emission sampling technique coupling a portable photosynthesis system with different trace gas analyzers. We provide several case studies using both online and offline gas analyzers to measure different types of leaf emissions. We further highlight both the capabilities and pitfalls of this method.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
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We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
Crystal D. McClure, Christopher Y. Lim, David H. Hagan, Jesse H. Kroll, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 1531–1547, https://doi.org/10.5194/acp-20-1531-2020, https://doi.org/10.5194/acp-20-1531-2020, 2020
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We characterized various optical, chemical, and physical properties of particles produced from combustion of a variety of different biomass fuels, many representative of those found in the western US. We find that many properties scale with the ratio between bulk average organic aerosol and black carbon mass concentrations, although there are some properties that do not.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
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.
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
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.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Ingeborg E. Nielsen, Henrik Skov, Andreas Massling, Axel C. Eriksson, Manuel Dall'Osto, Heikki Junninen, Nina Sarnela, Robert Lange, Sonya Collier, Qi Zhang, Christopher D. Cappa, and Jacob K. Nøjgaard
Atmos. Chem. Phys., 19, 10239–10256, https://doi.org/10.5194/acp-19-10239-2019, https://doi.org/10.5194/acp-19-10239-2019, 2019
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Measurements of the chemical composition of sub-micrometer aerosols were carried out in northern Greenland during the Arctic haze (February–May) where concentrations are high due to favorable conditions for long-range transport. Sulfate was the dominant aerosol (66 %), followed by organic matter (24 %). The highest black carbon concentrations where observed in February. Source apportionment yielded three factors: a primary factor (12 %), an Arctic haze factor (64 %) and a marine factor (22 %).
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.
Ziyue Li, Katherine A. Smith, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 14585–14608, https://doi.org/10.5194/acp-18-14585-2018, https://doi.org/10.5194/acp-18-14585-2018, 2018
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We investigated the influence of relative humidity (RH) on the heterogeneous oxidation of secondary organic aerosol (SOA) particles by OH radicals. We observed significantly faster volume loss and compositional change of SOA at high RH, showing that viscosity differences determine compositional changes, but variability in either the uptake coefficient or the fragmentation probability are required to explain the difference in volume loss between low and high RH.
James M. Mattila, Patrick Brophy, Jeffrey Kirkland, Samuel Hall, Kirk Ullmann, Emily V. Fischer, Steve Brown, Erin McDuffie, Alex Tevlin, and Delphine K. Farmer
Atmos. Chem. Phys., 18, 12315–12327, https://doi.org/10.5194/acp-18-12315-2018, https://doi.org/10.5194/acp-18-12315-2018, 2018
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Molecular acids in the atmosphere have implications for human health and air quality. Measurements of various acidic molecules were performed in the Colorado Front Range. Atmospheric concentrations of many acids increased during the day, indicative of sunlight-related production sources. A surface-level source of many acids persisting throughout day and night was observed. Traffic and agricultural activity were important anthropogenic sources of several acids near the measurement site.
Sara D. Forestieri, Taylor M. Helgestad, Andrew T. Lambe, Lindsay Renbaum-Wolff, Daniel A. Lack, Paola Massoli, Eben S. Cross, Manvendra K. Dubey, Claudio Mazzoleni, Jason S. Olfert, Arthur J. Sedlacek III, Andrew Freedman, Paul Davidovits, Timothy B. Onasch, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 12141–12159, https://doi.org/10.5194/acp-18-12141-2018, https://doi.org/10.5194/acp-18-12141-2018, 2018
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We characterized optical properties of flame-derived black carbon particles and interpret our observations through the use of Mie theory and Rayleigh–Debye–Gans theory. We determined that the mass absorption coefficient is independent of particle collapse and use this to derive theory- and wavelength-specific refractive indices for black carbon (BC). We demonstrate the inadequacy of Mie theory and suggest an alternative approach for atmospheric models to better represent light absorption by BC.
Sara D. Forestieri, Sean M. Staudt, Thomas M. Kuborn, Katharine Faber, Christopher R. Ruehl, Timothy H. Bertram, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, https://doi.org/10.5194/acp-18-10985-2018, 2018
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Our work establishes how surface tension reduction influences droplet growth and activation of simple sea spray mimics (NaCl coated with fatty acids). Fatty acids can substantially reduce droplet surface tension near activation but have limited impact on activation. Coating of NaCl by palmitic acid (a wax) impedes water uptake, but this impedance is removed if oleic acid (a liquid) is mixed in. The properties that surface-active compounds need to impact activation are theoretically examined.
Dean B. Atkinson, Mikhail Pekour, Duli Chand, James G. Radney, Katheryn R. Kolesar, Qi Zhang, Ari Setyan, Norman T. O'Neill, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 5499–5514, https://doi.org/10.5194/acp-18-5499-2018, https://doi.org/10.5194/acp-18-5499-2018, 2018
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We use in situ measurements of particle light extinction to assess the performance of a typical aerosol remote retrieval method. The retrieved fine-mode fraction of extinction, a property commonly used to characterize the anthropogenic influence on the aerosol optical depth, compares well with the in situ measurements as does the retrieved effective fine-mode radius, which characterizes the average size of the particles that contribute most to scattering.
Alex K. Y. Lee, Chia-Li Chen, Jun Liu, Derek J. Price, Raghu Betha, Lynn M. Russell, Xiaolu Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 15055–15067, https://doi.org/10.5194/acp-17-15055-2017, https://doi.org/10.5194/acp-17-15055-2017, 2017
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Understanding the mixing state of ambient black carbon (BC) and the chemical characteristics of its associated coatings is important to evaluate BC fate and environmental impacts. This study reports fresh secondary organic aerosol (SOA) formation near traffic emissions during daytime. Our observations suggest that BC was unlikely the major condensation sink of SOA, and a portion of SOA condensed on BC surface was chemically different from other SOA particles that were externally mixed with BC.
Gouri Prabhakar, Caroline L. Parworth, Xiaolu Zhang, Hwajin Kim, Dominique E. Young, Andreas J. Beyersdorf, Luke D. Ziemba, John B. Nowak, Timothy H. Bertram, Ian C. Faloona, Qi Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 14747–14770, https://doi.org/10.5194/acp-17-14747-2017, https://doi.org/10.5194/acp-17-14747-2017, 2017
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This work assesses the processes that control the ambient concentrations of particulate nitrate in the the wintertime San Joaquin Valley of California through a combination of aircraft and surface measurements made during the DISCOVER-AQ study. We provide an observational demonstration of how nocturnal production and advection in aloft layers combines with daytime production and loss from entrainment and deposition to give rise to a distinct diurnal profile in surface nitrate concentrations.
Jakob Lindaas, Delphine K. Farmer, Ilana B. Pollack, Andrew Abeleira, Frank Flocke, Rob Roscioli, Scott Herndon, and Emily V. Fischer
Atmos. Chem. Phys., 17, 10691–10707, https://doi.org/10.5194/acp-17-10691-2017, https://doi.org/10.5194/acp-17-10691-2017, 2017
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Wildfire smoke is becoming increasingly important for air quality in the US. We used measurements taken during the summer 2015 near Denver, CO, to provide a case study of how wildfire smoke can impact air quality, specifically ozone, which is harmful to humans. Wildfire smoke during this time period was associated with about 15 % more ozone than we would expect under normal conditions. This smoke came from fires in the Pacific Northwest and likely impacted much of the central and western US.
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.
Trey Murschell, S. Ryan Fulgham, and Delphine K. Farmer
Atmos. Meas. Tech., 10, 2117–2127, https://doi.org/10.5194/amt-10-2117-2017, https://doi.org/10.5194/amt-10-2117-2017, 2017
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The impact of atmospheric chemistry on the fate and transport of pesticides is poorly understood. This paper describes a method for real-time measurements of four common-use pesticides in the gas phase using chemical ionization mass spectrometry. The calibration approach for atmospheric semi-volatile pesticides is described in detail.
Andrew J. Abeleira and Delphine K. Farmer
Atmos. Chem. Phys., 17, 6517–6529, https://doi.org/10.5194/acp-17-6517-2017, https://doi.org/10.5194/acp-17-6517-2017, 2017
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.
Shantanu H. Jathar, Matthew Woody, Havala O. T. Pye, Kirk R. Baker, and Allen L. Robinson
Atmos. Chem. Phys., 17, 4305–4318, https://doi.org/10.5194/acp-17-4305-2017, https://doi.org/10.5194/acp-17-4305-2017, 2017
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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.
M. Dale Stokes, Grant Deane, Douglas B. Collins, Christopher Cappa, Timothy Bertram, Abigail Dommer, Steven Schill, Sara Forestieri, and Mathew Survilo
Atmos. Meas. Tech., 9, 4257–4267, https://doi.org/10.5194/amt-9-4257-2016, https://doi.org/10.5194/amt-9-4257-2016, 2016
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A small breaking wave and foam simulator has been fabricated that allows the continuous analysis of the produced marine aerosols. Based on the original Marine Aerosol Reference Tank (MART) the miniature version allows the culturing of delicate planktonic organisms because it operates without a large, sheer-inducing pump. This allows the study of marine aerosol production and the effects of biologically controlled seawater chemistry under controlled and repeatable experimental conditions.
Patrick Brophy and Delphine K. Farmer
Atmos. Meas. Tech., 9, 3969–3986, https://doi.org/10.5194/amt-9-3969-2016, https://doi.org/10.5194/amt-9-3969-2016, 2016
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We describe voltage scanning methodologies using a high-resolution time-of-flight chemical ionization mass spectrometer (HR-TOF-CIMS) with acetate reagent ions to control for clustering observed in the mass spectrum. Operational considerations related to atmospheric measurements of carboxylic acids using acetate chemical ionization are discussed.
Sara D. Forestieri, Gavin C. Cornwell, Taylor M. Helgestad, Kathryn A. Moore, Christopher Lee, Gordon A. Novak, Camille M. Sultana, Xiaofei Wang, Timothy H. Bertram, Kimberly A. Prather, and Christopher D. Cappa
Atmos. Chem. Phys., 16, 9003–9018, https://doi.org/10.5194/acp-16-9003-2016, https://doi.org/10.5194/acp-16-9003-2016, 2016
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Hygroscopic growth factors at 85 % relative humidity (GF(85 %)) were quantified along with particle composition for primary sea spray aerosol (SSA) particles generated in marine aerosol reference tanks (MARTs) from seawater in which two independent phytoplankton blooms were induced. The observed 5 to 15 % depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Christopher D. Cappa, Katheryn R. Kolesar, Xiaolu Zhang, Dean B. Atkinson, Mikhail S. Pekour, Rahul A. Zaveri, Alla Zelenyuk, and Qi Zhang
Atmos. Chem. Phys., 16, 6511–6535, https://doi.org/10.5194/acp-16-6511-2016, https://doi.org/10.5194/acp-16-6511-2016, 2016
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Measurements of size-dependent aerosol optical properties at visible wavelengths made during the 2010 CARES study are reported on, with a special focus on the characterization of supermicron particles. The relationships with and dependence upon particle composition, particle size, photochemical aging, water uptake and heating are discussed, along with broader implications of these in situ measurements for the interpretation of remote sensing products.
Dominique E. Young, Hwajin Kim, Caroline Parworth, Shan Zhou, Xiaolu Zhang, Christopher D. Cappa, Roger Seco, Saewung Kim, and Qi Zhang
Atmos. Chem. Phys., 16, 5427–5451, https://doi.org/10.5194/acp-16-5427-2016, https://doi.org/10.5194/acp-16-5427-2016, 2016
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Aerosol chemistry and the sources and processes driving the observed temporal and diurnal variations of PM were studied in a polluted urban environment during winter 2013. These results were compared to a similar campaign from winter 2010. Meteorology strongly influenced PM composition, both directly and indirectly. Nighttime reactions played a more important role in 2013 and the influence from a nighttime formed residual layer that mixed down in the morning was also much more intense in 2013.
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.
K. R. Kolesar, C. Chen, D. Johnson, and C. D. Cappa
Atmos. Chem. Phys., 15, 9327–9343, https://doi.org/10.5194/acp-15-9327-2015, https://doi.org/10.5194/acp-15-9327-2015, 2015
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Secondary organic aerosol from the dark ozonolysis of α‑pinene was formed at a range of mass loadings from 1 to 800μg m-3. The amount of mass loss during evaporation in a thermodenuder was found to be independent of mass loading. A kinetic model of evaporation was fit to the observations and good agreement was obtained when the particle was either composed of dimers that decompose into semi-volatile monomers or when it was composed of low-volatility compounds that evaporate directly.
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.
D. B. Atkinson, J. G. Radney, J. Lum, K. R. Kolesar, D. J. Cziczo, M. S. Pekour, Q. Zhang, A. Setyan, A. Zelenyuk, and C. D. Cappa
Atmos. Chem. Phys., 15, 4045–4061, https://doi.org/10.5194/acp-15-4045-2015, https://doi.org/10.5194/acp-15-4045-2015, 2015
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This work describes an analysis of measurements of the influence of water uptake on the light-scattering properties of sub- and supermicron-sized particles as observed in the Sacramento, CA, USA region during the 2010 CARES field campaign. The observations are used to derive campaign-average effective hygroscopicity parameters for submicron oxygenated organic aerosol and for supermicron particles, and the influence of chloride displacement reactions on particle hygroscopicity is examined.
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
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
G. M. Buffaloe, D. A. Lack, E. J. Williams, D. Coffman, K. L. Hayden, B. M. Lerner, S.-M. Li, I. Nuaaman, P. Massoli, T. B. Onasch, P. K. Quinn, and C. D. Cappa
Atmos. Chem. Phys., 14, 1881–1896, https://doi.org/10.5194/acp-14-1881-2014, https://doi.org/10.5194/acp-14-1881-2014, 2014
C. D. Cappa, E. J. Williams, D. A. Lack, G. M. Buffaloe, D. Coffman, K. L. Hayden, S. C. Herndon, B. M. Lerner, S.-M. Li, P. Massoli, R. McLaren, I. Nuaaman, T. B. Onasch, and P. K. Quinn
Atmos. Chem. Phys., 14, 1337–1352, https://doi.org/10.5194/acp-14-1337-2014, https://doi.org/10.5194/acp-14-1337-2014, 2014
J. R. Pierce, M. J. Evans, C. E. Scott, S. D. D'Andrea, D. K. Farmer, E. Swietlicki, and D. V. Spracklen
Atmos. Chem. Phys., 13, 3163–3176, https://doi.org/10.5194/acp-13-3163-2013, https://doi.org/10.5194/acp-13-3163-2013, 2013
C. D. Cappa, X. Zhang, C. L. Loza, J. S. Craven, L. D. Yee, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 1591–1606, https://doi.org/10.5194/acp-13-1591-2013, https://doi.org/10.5194/acp-13-1591-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
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
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
Exploring the processes controlling secondary inorganic aerosol: Evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks, Alaska, the N. Hemisphere, and the Contiguous United States
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Land use change influence on atmospheric organic gases, aerosols, and radiative effects
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
Quantifying the Impacts of Marine Aerosols over the Southeast Atlantic Ocean using a chemical transport model: Implications for aerosol-cloud interactions
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
Significant impact of urban tree biogenic emissions on air quality estimated by a bottom-up inventory and chemistry transport modeling
Secondary organic aerosols derived from intermediate-volatility n-alkanes adopt low-viscous phase state
Modeling the drivers of fine PM pollution over Central Europe: impacts and contributions of emissions from different sources
Reaction of SO3 with H2SO4 and its implications for aerosol particle formation in the gas phase and at the air–water interface
Weakened aerosol–radiation interaction exacerbating ozone pollution in eastern China since China's clean air actions
Uncertainties from biomass burning aerosols in air quality models obscure public health impacts in Southeast Asia
Oxidative potential apportionment of atmospheric PM1: a new approach combining high-sensitive online analysers for chemical composition and offline OP measurement technique
Aqueous-phase chemistry of glyoxal with multifunctional reduced nitrogen compounds: a potential missing route for secondary brown carbon
An updated modeling framework to simulate Los Angeles air quality – Part 1: Model development, evaluation, and source apportionment
Frequent haze events associated with transport and stagnation over the corridor between the North China Plain and Yangtze River Delta
Evaluation of WRF-Chem-simulated meteorology and aerosols over northern India during the severe pollution episode of 2016
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
pH regulates the formation of organosulfates and inorganic sulfate from organic peroxide reaction with dissolved SO2 in aquatic media
Technical note: Accurate, reliable, and high-resolution air quality predictions by improving the Copernicus Atmosphere Monitoring Service using a novel statistical post-processing method
Contribution of intermediate-volatility organic compounds from on-road transport to secondary organic aerosol levels in Europe
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities
CAMx–UNIPAR simulation of secondary organic aerosol mass formed from multiphase reactions of hydrocarbons under the Central Valley urban atmospheres of California
Impact of urbanization on fine particulate matter concentrations over central Europe
Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US
Reactive organic carbon air emissions from mobile sources in the United States
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
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.
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.
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.
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.
Olivia G. Norman, Colette L. Heald, 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
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
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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).
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.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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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.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1363, https://doi.org/10.5194/egusphere-2024-1363, 2024
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Nitrate aerosol is often omitted in global chemistry-climate models due to the chemical complexity of its formation process. Using a global model, we demonstrate 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.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
EGUsphere, https://doi.org/10.5194/egusphere-2024-2014, https://doi.org/10.5194/egusphere-2024-2014, 2024
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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.
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.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1948, https://doi.org/10.5194/egusphere-2024-1948, 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.
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
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
Tommaso Galeazzo, Bernard Aumont, Marie Camredon, Richard Valorso, Yong B. Lim, Paul J. Ziemann, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 5549–5565, https://doi.org/10.5194/acp-24-5549-2024, https://doi.org/10.5194/acp-24-5549-2024, 2024
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Secondary organic aerosol (SOA) derived from n-alkanes is a major component of anthropogenic particulate matter. We provide an analysis of n-alkane SOA by chemistry modeling, machine learning, and laboratory experiments, showing that n-alkane SOA adopts low-viscous semi-solid or liquid states. Our results indicate few kinetic limitations of mass accommodation in SOA formation, supporting the application of equilibrium partitioning for simulating n-alkane SOA in large-scale atmospheric models.
Lukáš Bartík, Peter Huszár, Jan Karlický, Ondřej Vlček, and Kryštof Eben
Atmos. Chem. Phys., 24, 4347–4387, https://doi.org/10.5194/acp-24-4347-2024, https://doi.org/10.5194/acp-24-4347-2024, 2024
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The presented study deals with the attribution of fine particulate matter (PM2.5) concentrations to anthropogenic emissions over Central Europe using regional-scale models. It calculates the present-day contributions of different emissions sectors to concentrations of PM2.5 and its secondary components. Moreover, the study investigates the effect of chemical nonlinearities by using multiple source attribution methods and secondary organic aerosol calculation methods.
Rui Wang, Yang Cheng, Shasha Chen, Rongrong Li, Yue Hu, Xiaokai Guo, Tianlei Zhang, Fengmin Song, and Hao Li
Atmos. Chem. Phys., 24, 4029–4046, https://doi.org/10.5194/acp-24-4029-2024, https://doi.org/10.5194/acp-24-4029-2024, 2024
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We used quantum chemical calculations, Born–Oppenheimer molecular dynamics simulations, and the ACDC kinetic model to characterize SO3–H2SO4 interaction in the gas phase and at the air–water interface and to study the effect of H2S2O7 on H2SO4–NH3-based clusters. The work expands our understanding of new pathways for the loss of SO3 in acidic polluted areas and helps reveal some missing sources of NPF in metropolitan industrial regions and understand the atmospheric organic–sulfur cycle better.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 24, 4001–4015, https://doi.org/10.5194/acp-24-4001-2024, https://doi.org/10.5194/acp-24-4001-2024, 2024
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The present study quantifies the response of aerosol–radiation interaction (ARI) to anthropogenic emission reduction from 2013 to 2017, with the main focus on the contribution to changed O3 concentrations over eastern China both in summer and winter using the WRF-Chem model. The weakened ARI due to decreased anthropogenic emission aggravates the summer (winter) O3 pollution by +0.81 ppb (+0.63 ppb), averaged over eastern China.
Margaret R. Marvin, Paul I. Palmer, Fei Yao, Mohd Talib Latif, and Md Firoz Khan
Atmos. Chem. Phys., 24, 3699–3715, https://doi.org/10.5194/acp-24-3699-2024, https://doi.org/10.5194/acp-24-3699-2024, 2024
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We use an atmospheric chemistry model to investigate aerosols emitted from fire activity across Southeast Asia. We find that the limited nature of measurements in this region leads to large uncertainties that significantly hinder the model representation of these aerosols and their impacts on air quality. As a result, the number of monthly attributable deaths is underestimated by as many as 4500, particularly in March at the peak of the mainland burning season.
Julie Camman, Benjamin Chazeau, Nicolas Marchand, Amandine Durand, Grégory Gille, Ludovic Lanzi, Jean-Luc Jaffrezo, Henri Wortham, and Gaëlle Uzu
Atmos. Chem. Phys., 24, 3257–3278, https://doi.org/10.5194/acp-24-3257-2024, https://doi.org/10.5194/acp-24-3257-2024, 2024
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Fine particle (PM1) pollution is a major health issue in the city of Marseille, which is subject to numerous pollution sources. Sampling carried out during the summer enabled a fine characterization of the PM1 sources and their oxidative potential, a promising new metric as a proxy for health impact. PM1 came mainly from combustion sources, secondary ammonium sulfate, and organic nitrate, while the oxidative potential of PM1 came from these sources and from resuspended dust in the atmosphere.
Yuemeng Ji, Zhang Shi, Wenjian Li, Jiaxin Wang, Qiuju Shi, Yixin Li, Lei Gao, Ruize Ma, Weijun Lu, Lulu Xu, Yanpeng Gao, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 3079–3091, https://doi.org/10.5194/acp-24-3079-2024, https://doi.org/10.5194/acp-24-3079-2024, 2024
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The formation mechanisms for secondary brown carbon (SBrC) contributed by multifunctional reduced nitrogen compounds (RNCs) remain unclear. Hence, from combined laboratory experiments and quantum chemical calculations, we investigated the heterogeneous reactions of glyoxal (GL) with multifunctional RNCs, which are driven by four-step indirect nucleophilic addition reactions. Our results show a possible missing source for SBrC formation on urban, regional, and global scales.
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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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Feifan Yan, Hang Su, Yafang Cheng, Rujin Huang, Hong Liao, Ting Yang, Yuanyuan Zhu, Shaoqing Zhang, Lifang Sheng, Wenbin Kou, Xinran Zeng, Shengnan Xiang, Xiaohong Yao, Huiwang Gao, and Yang Gao
Atmos. Chem. Phys., 24, 2365–2376, https://doi.org/10.5194/acp-24-2365-2024, https://doi.org/10.5194/acp-24-2365-2024, 2024
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PM2.5 pollution is a major air quality issue deteriorating human health, and previous studies mostly focus on regions like the North China Plain and Yangtze River Delta. However, the characteristics of PM2.5 concentrations between these two regions are studied less often. Focusing on the transport corridor region, we identify an interesting seesaw transport phenomenon with stagnant weather conditions, conducive to PM2.5 accumulation over this region, resulting in large health effects.
Prerita Agarwal, David S. Stevenson, and Mathew R. Heal
Atmos. Chem. Phys., 24, 2239–2266, https://doi.org/10.5194/acp-24-2239-2024, https://doi.org/10.5194/acp-24-2239-2024, 2024
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Air pollution levels across northern India are amongst some of the worst in the world, with episodic and hazardous haze events. Here, the ability of the WRF-Chem model to predict air quality over northern India is assessed against several datasets. Whilst surface wind speed and particle pollution peaks are over- and underestimated, respectively, meteorology and aerosol trends are adequately captured, and we conclude it is suitable for investigating severe particle pollution events.
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024, https://doi.org/10.5194/acp-24-1939-2024, 2024
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The 2014–15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region, providing a chance to study how aerosol alters cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2, where changes to cloud properties are explored.
Lin Du, Xiaofan Lv, Makroni Lily, Kun Li, and Narcisse Tsona Tchinda
Atmos. Chem. Phys., 24, 1841–1853, https://doi.org/10.5194/acp-24-1841-2024, https://doi.org/10.5194/acp-24-1841-2024, 2024
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This study explores the pH effect on the reaction of dissolved SO2 with selected organic peroxides. Results show that the formation of organic and/or inorganic sulfate from these peroxides strongly depends on their electronic structures, and these processes are likely to alter the chemical composition of dissolved organic matter in different ways. The rate constants of these reactions exhibit positive pH and temperature dependencies within pH 1–10 and 240–340 K ranges.
Angelo Riccio and Elena Chianese
Atmos. Chem. Phys., 24, 1673–1689, https://doi.org/10.5194/acp-24-1673-2024, https://doi.org/10.5194/acp-24-1673-2024, 2024
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Starting from the Copernicus Atmosphere Monitoring Service (CAMS), we provided a novel ensemble statistical post-processing approach to improve their air quality predictions. Our approach is able to provide reliable short-term forecasts of pollutant concentrations, which is a key challenge in supporting national authorities in their tasks related to EU Air Quality Directives, such as planning and reporting the state of air quality to the citizens.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
Atmos. Chem. Phys., 24, 649–661, https://doi.org/10.5194/acp-24-649-2024, https://doi.org/10.5194/acp-24-649-2024, 2024
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This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves as an important tool for combined exposure assessment in epidemiological studies.
Yujin Jo, Myoseon Jang, Sanghee Han, Azad Madhu, Bonyoung Koo, Yiqin Jia, Zechen Yu, Soontae Kim, and Jinsoo Park
Atmos. Chem. Phys., 24, 487–508, https://doi.org/10.5194/acp-24-487-2024, https://doi.org/10.5194/acp-24-487-2024, 2024
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The CAMx–UNIPAR model simulated the SOA budget formed via multiphase reactions of hydrocarbons and the impact of emissions and climate on SOA characteristics under California’s urban environments during winter 2018. SOA growth was dominated by daytime oxidation of long-chain alkanes and nighttime terpene oxidation with O3 and NO−3 radicals. The spatial distributions of anthropogenic SOA were affected by the northwesterly wind, whereas those of biogenic SOA were insensitive to wind directions.
Peter Huszar, Alvaro Patricio Prieto Perez, Lukáš Bartík, Jan Karlický, and Anahi Villalba-Pradas
Atmos. Chem. Phys., 24, 397–425, https://doi.org/10.5194/acp-24-397-2024, https://doi.org/10.5194/acp-24-397-2024, 2024
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Urbanization transforms rural land into artificial land, while due to human activities, it also introduces a great quantity of emissions. We quantify the impact of urbanization on the final particulate matter pollutant levels by looking not only at these emissions, but also at the way urban land cover influences meteorological conditions, how the removal of pollutants changes due to urban land cover, and how biogenic emissions from vegetation change due to less vegetation in urban areas.
Yinbao Jin, Yiming Liu, Xiao Lu, Xiaoyang Chen, Ao Shen, Haofan Wang, Yinping Cui, Yifei Xu, Siting Li, Jian Liu, Ming Zhang, Yingying Ma, and Qi Fan
Atmos. Chem. Phys., 24, 367–395, https://doi.org/10.5194/acp-24-367-2024, https://doi.org/10.5194/acp-24-367-2024, 2024
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This study aims to address these issues by evaluating eight independent biomass burning (BB) emission inventories (GFED, FINN1.5, FINN2.5 MOS, FINN2.5 MOSVIS, GFAS, FEER, QFED, and IS4FIRES) using the WRF-Chem model and analyzing their impact on aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in peninsular Southeast Asia (PSEA) that occurred in March 2019.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
Atmos. Chem. Phys., 23, 14505–14520, https://doi.org/10.5194/acp-23-14505-2023, https://doi.org/10.5194/acp-23-14505-2023, 2023
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Annual PM2.5 emissions in China consistently decreased by about 3% to 5% from 2017 to 2020 with spatial variations and seasonal dependencies. High-temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reductions in PM2.5 emissions in the North China Plain and northeast of China in 2020 were caused by COVID-19.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
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
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
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New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Cited articles
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Ahmadov, R., McKeen, S. A., Robinson, A. L., Bahreini, R., Middlebrook, A. M., de Gouw, J. A., Meagher, J., Hsie, E. Y., Edgerton, E., Shaw, S., and Trainer, M.: A volatility basis set model for summertime secondary organic aerosols over the eastern United States in 2006, J. Geophys. Res.-Atmos., 117, D06301, https://doi.org/10.1029/2011JD016831, 2012.
Anderson, J. O., Thundiyil, J. G., and Stolbach, A.: Clearing the air: a review of the effects of particulate matter air pollution on human health, J. Med. Toxicol., 8, 166–175, 2012.
Atkinson, R. and Arey, J.: Atmospheric degradation of volatile organic compounds, Chem. Rev., 103, 4605–4638, 2003.
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Short summary
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.
As oxidation flow reactors (OFRs) are increasingly used to study aerosol formation and evolution...
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