Articles | Volume 24, issue 10
https://doi.org/10.5194/acp-24-6153-2024
© Author(s) 2024. 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-24-6153-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere
Chuanyang Shen
Department of Chemistry, University of California, Riverside, CA 92507, USA
Xiaoyan Yang
Department of Environmental Sciences, University of California, Riverside, CA 92507, USA
Joel Thornton
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
John Shilling
Atmospheric, Climate, and Earth Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA
Chenyang Bi
Center for Aerosol and Cloud Chemistry, Aerodyne Research Inc., Billerica, MA 01821, USA
Gabriel Isaacman-VanWertz
Department of Civil and Environmental Engineering, Virginia Tech, Blacksburg, VA 24061, USA
Department of Chemistry, University of California, Riverside, CA 92507, USA
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Qinghao Guo, Haofei Zhang, Bo Long, Lehui Cui, Yiyang Sun, Hao Liu, Yaxin Liu, Yunting Xiao, Pingqing Fu, and Jialei Zhu
Atmos. Chem. Phys., 25, 9249–9262, https://doi.org/10.5194/acp-25-9249-2025, https://doi.org/10.5194/acp-25-9249-2025, 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 enhances predictions of pollution and climate impacts while deepening our understanding of how natural and human-made emissions interact in the atmosphere.
Phil Rund, Ben H. Lee, Siddharth Iyer, Gordon A. Novak, Jake T. Vallow, and Joel A. Thornton
EGUsphere, https://doi.org/10.5194/egusphere-2025-3709, https://doi.org/10.5194/egusphere-2025-3709, 2025
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We introduce a custom-built chamber (known as an IMR) for use with a Chemical Ionization Mass Spectrometry (CIMS) gas measurement instrument. The IMR shows large improvements compared to previous designs in reducing non-real signal in the instrument, reducing uncertainties for trace gas studies in the laboratory and the field. We characterize this new IMR and demonstrate its use in analyzing air masses of unknown composition during a field campaign, reporting concentrations of important gases.
Carley D. Fredrickson, Scott J. Janz, Lok N. Lamsal, Ursula A. Jongebloed, Joshua L. Laughner, and Joel A. Thornton
Atmos. Meas. Tech., 18, 3669–3689, https://doi.org/10.5194/amt-18-3669-2025, https://doi.org/10.5194/amt-18-3669-2025, 2025
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We present an analysis of high-resolution remote sensing measurements of nitrogen-containing trace gases emitted by wildfires. The measurements were made using an instrument on the NASA ER-2 aircraft in the summer of 2019. We find that time-resolved fire intensity is critical to quantify trace gas emissions over a fire's entire lifespan. These findings have implications for improving air pollution forecasts downwind of wildfires using computer models of atmospheric chemistry and meteorology.
Sara L. Farrell, Quazi Z. Rasool, Havala O. T. Pye, Yue Zhang, Ying Li, Yuzhi Chen, Chi-Tsan Wang, Haofei Zhang, Ryan Schmedding, Manabu Shiraiwa, Jaime Greene, Sri H. Budisulistiorini, Jose L. Jimenez, Weiwei Hu, Jason D. Surratt, and William Vizuete
EGUsphere, https://doi.org/10.5194/egusphere-2025-2253, https://doi.org/10.5194/egusphere-2025-2253, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Fine particulate matter (PM2.5) has become increasingly important to regulate and model. In this study, we parameterize non-ideal aerosol mixing and phase state into the Community Multiscale Air Quality (CMAQ) model and analyze its impact on the formation of a globally important source of PM2.5, isoprene epoxydiol (IEPOX)-derived PM2.5. Incorporating these features furthers model bias in IEPOX-derived PM2.5, however, this work provides potential phase state bounds for future PM2.5 modeling work.
Joseph O. Palmo, Colette L. Heald, Donald R. Blake, Ilann Bourgeois, Matthew Coggon, Jeff Collett, Frank Flocke, Alan Fried, Georgios Gkatzelis, Samuel Hall, Lu Hu, Jose L. Jimenez, Pedro Campuzano-Jost, I-Ting Ku, Benjamin Nault, Brett Palm, Jeff Peischl, Ilana Pollack, Amy Sullivan, Joel Thornton, Carsten Warneke, Armin Wisthaler, and Lu Xu
EGUsphere, https://doi.org/10.5194/egusphere-2025-1969, https://doi.org/10.5194/egusphere-2025-1969, 2025
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This study investigates ozone production within wildfire smoke plumes as they age, using both aircraft observations and models. We find that the chemical environment and resulting ozone production within smoke changes as plumes evolve, with implications for climate and public health.
Xinyue Shao, Yaman Liu, Xinyi Dong, Minghuai Wang, Ruochong Xu, Joel A. Thornton, Duseong S. Jo, Man Yue, Wenxiang Shen, Manish Shrivastava, Stephen R. Arnold, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2025-1526, https://doi.org/10.5194/egusphere-2025-1526, 2025
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Highly Oxygenated Organic Molecules (HOMs) are key precursors of secondary organic aerosols (SOA). Incorporating the HOMs chemical mechanism into a global climate model allows for a reasonable reproduction of observed HOM characteristics. HOM-SOA constitutes a significant fraction of global SOA, and its distribution and formation pathways exhibit strong sensitivity to uncertainties in autoxidation processes and peroxy radical branching ratios.
Alfred W. Mayhew, Lauri Franzon, Kelvin H. Bates, Theo Kurtén, Felipe D. Lopez-Hilfiker, Claudia Mohr, Andrew R. Rickard, Joel A. Thornton, and Jessica D. Haskins
EGUsphere, https://doi.org/10.5194/egusphere-2025-1922, https://doi.org/10.5194/egusphere-2025-1922, 2025
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This work outlines an investigation into an understudied atmospheric chemical reaction pathway with the potential to form particulate pollution that has important impacts on air quality and climate. We suggest that this chemical pathway is responsible for a large fraction of the atmospheric particulate matter observed in tropical forested regions, but we also highlight the need for further ambient and lab investigations to inform an accurate representation of this process in atmospheric models.
Chris J. Wright, Joel A. Thornton, Lyatt Jaeglé, Yang Cao, Yannian Zhu, Jihu Liu, Randall Jones II, Robert Holzworth, Daniel Rosenfeld, Robert Wood, Peter Blossey, and Daehyun Kim
Atmos. Chem. Phys., 25, 2937–2946, https://doi.org/10.5194/acp-25-2937-2025, https://doi.org/10.5194/acp-25-2937-2025, 2025
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Aerosol particles influence clouds, which exert a large forcing on solar radiation and freshwater. To better understand the mechanisms by which aerosol influences thunderstorms, we look at the two busiest shipping lanes in the world, where recent regulations have reduced sulfur emissions by nearly an order of magnitude. We find that the reduction in emissions has been accompanied by a dramatic decrease in both lightning and the number of droplets in clouds over the shipping lanes.
Delaney B. Kilgour, Christopher M. Jernigan, Olga Garmash, Sneha Aggarwal, Shengqian Zhou, Claudia Mohr, Matt E. Salter, Joel A. Thornton, Jian Wang, Paul Zieger, and Timothy H. Bertram
Atmos. Chem. Phys., 25, 1931–1947, https://doi.org/10.5194/acp-25-1931-2025, https://doi.org/10.5194/acp-25-1931-2025, 2025
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We report simultaneous measurements of dimethyl sulfide (DMS) and hydroperoxymethyl thioformate (HPMTF) in the eastern North Atlantic. We use an observationally constrained box model to show that cloud loss is the dominant sink of HPMTF in this region over 6 weeks, resulting in large reductions in DMS-derived products that contribute to aerosol formation and growth. Our findings indicate that fast cloud processing of HPMTF must be included in global models to accurately capture the sulfur cycle.
Fan Mei, Jennifer M. Comstock, Mikhail S. Pekour, Jerome D. Fast, Krista L. Gaustad, Beat Schmid, Shuaiqi Tang, Damao Zhang, John E. Shilling, Jason M. Tomlinson, Adam C. Varble, Jian Wang, L. Ruby Leung, Lawrence Kleinman, Scot Martin, Sebastien C. Biraud, Brian D. Ermold, and Kenneth W. Burk
Earth Syst. Sci. Data, 16, 5429–5448, https://doi.org/10.5194/essd-16-5429-2024, https://doi.org/10.5194/essd-16-5429-2024, 2024
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Our study explores a comprehensive dataset from airborne field studies (2013–2018) conducted using the US Department of Energy's Gulfstream 1 (G-1). The 236 flights span diverse regions, including the Arctic, US Southern Great Plains, US West Coast, eastern North Atlantic, Amazon Basin in Brazil, and Sierras de Córdoba range in Argentina. This dataset provides unique insights into atmospheric dynamics, aerosols, and clouds and makes data available in a more accessible format.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Matthieu Riva, Veronika Pospisilova, Carla Frege, Sebastien Perrier, Priyanka Bansal, Spiro Jorga, Patrick Sturm, Joel A. Thornton, Urs Rohner, and Felipe Lopez-Hilfiker
Atmos. Meas. Tech., 17, 5887–5901, https://doi.org/10.5194/amt-17-5887-2024, https://doi.org/10.5194/amt-17-5887-2024, 2024
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We present a newly designed reduced-pressure chemical ionization reactor for detection of gas-phase organic and inorganic species. The system operates through the combined use of vacuum ultraviolet ionization and photosensitizers to generate numerous adduct ionization schemes. As a result, it offers the ability to simultaneously measure a wide variety of organic and inorganic species in terms of compound volatility and functionality, while being largely independent of changes in sample humidity.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Yang Wang, Chanakya Bagya Ramesh, Scott E. Giangrande, Jerome Fast, Xianda Gong, Jiaoshi Zhang, Ahmet Tolga Odabasi, Marcus Vinicius Batista Oliveira, Alyssa Matthews, Fan Mei, John E. Shilling, Jason Tomlinson, Die Wang, and Jian Wang
Atmos. Chem. Phys., 23, 15671–15691, https://doi.org/10.5194/acp-23-15671-2023, https://doi.org/10.5194/acp-23-15671-2023, 2023
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We report the vertical profiles of aerosol properties over the Southern Great Plains (SGP), a region influenced by shallow convective clouds, land–atmosphere interactions, boundary layer turbulence, and the aerosol life cycle. We examined the processes that drive the aerosol population and distribution in the lower troposphere over the SGP. This study helps improve our understanding of aerosol–cloud interactions and the model representation of aerosol processes.
James F. Hurley, Alejandra Caceres, Deborah F. McGlynn, Mary E. Tovillo, Suzanne Pinar, Roger Schürch, Ksenia Onufrieva, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4681–4692, https://doi.org/10.5194/amt-16-4681-2023, https://doi.org/10.5194/amt-16-4681-2023, 2023
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Volatile organic compounds (VOCs) have a wide range of sources and impacts on environments and human health that make them spatially, temporally, and chemically varied. Current methods lack the ability to collect samples in ways that provide spatial and chemical resolution without complex, costly instrumentation. We describe and validate a low-cost, portable VOC sampler and demonstrate its utility in collecting distributed coordinated samples.
Namrata Shanmukh Panji and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4319–4330, https://doi.org/10.5194/amt-16-4319-2023, https://doi.org/10.5194/amt-16-4319-2023, 2023
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Measuring volatile organic compounds (VOCs) in the atmosphere is crucial for understanding air quality and environmental impact. Since these compounds are present in low concentrations, preconcentration of samples is often necessary for accurate detection. To address this issue, we have developed a novel inlet that uses selective permeation to concentrate organic gases in small sample flows. This device offers a promising approach for accurately detecting low levels of VOCs in the atmosphere.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
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In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
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We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
Deborah F. McGlynn, Graham Frazier, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Biogeosciences, 20, 45–55, https://doi.org/10.5194/bg-20-45-2023, https://doi.org/10.5194/bg-20-45-2023, 2023
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Using a custom-made gas chromatography flame ionization detector, 2 years of speciated hourly biogenic volatile organic compound data were collected in a forest in central Virginia. We identify diurnal and seasonal variability in the data, which is shown to impact atmospheric oxidant budgets. A comparison with emission models identified discrepancies with implications for model outcomes. We suggest increased monitoring of speciated biogenic volatile organic compounds to improve modeled results.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Sungwoo Kim, Brian M. Lerner, Donna T. Sueper, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 15, 5061–5075, https://doi.org/10.5194/amt-15-5061-2022, https://doi.org/10.5194/amt-15-5061-2022, 2022
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Atmospheric samples can be complex, and current analysis methods often require substantial human interaction and discard potentially important information. To improve analysis accuracy and computational cost of these large datasets, we developed an automated analysis algorithm that utilizes a factor analysis approach coupled with a decision tree. We demonstrate that this algorithm cataloged approximately 10 times more analytes compared to a manual analysis and in a quarter of the analysis time.
Jerome D. Fast, David M. Bell, Gourihar Kulkarni, Jiumeng Liu, Fan Mei, Georges Saliba, John E. Shilling, Kaitlyn Suski, Jason Tomlinson, Jian Wang, Rahul Zaveri, and Alla Zelenyuk
Atmos. Chem. Phys., 22, 11217–11238, https://doi.org/10.5194/acp-22-11217-2022, https://doi.org/10.5194/acp-22-11217-2022, 2022
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Recent aircraft measurements from the HI-SCALE campaign conducted over the Southern Great Plains (SGP) site in Oklahoma are used to quantify spatial variability of aerosol properties in terms of grid spacings typically used by weather and climate models. Surprisingly large horizontal gradients in aerosol properties were frequently observed in this rural area. This spatial variability can be used as an uncertainty range when comparing surface point measurements with model predictions.
Shuaiqi Tang, Jerome D. Fast, Kai Zhang, Joseph C. Hardin, Adam C. Varble, John E. Shilling, Fan Mei, Maria A. Zawadowicz, and Po-Lun Ma
Geosci. Model Dev., 15, 4055–4076, https://doi.org/10.5194/gmd-15-4055-2022, https://doi.org/10.5194/gmd-15-4055-2022, 2022
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We developed an Earth system model (ESM) diagnostics package to compare various types of aerosol properties simulated in ESMs with aircraft, ship, and surface measurements from six field campaigns across spatial scales. The diagnostics package is coded and organized to be flexible and modular for future extension to other field campaign datasets and adapted to higher-resolution model simulations. Future releases will include comprehensive cloud and aerosol–cloud interaction diagnostics.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Arto Heitto, Kari Lehtinen, Tuukka Petäjä, Felipe Lopez-Hilfiker, Joel A. Thornton, Markku Kulmala, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 155–171, https://doi.org/10.5194/acp-22-155-2022, https://doi.org/10.5194/acp-22-155-2022, 2022
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For atmospheric aerosol particles to take part in cloud formation, they need to be at least a few tens of nanometers in diameter. By using a particle condensation model, we investigated how two types of chemical reactions, oligomerization and decomposition, of organic molecules inside the particle may affect the growth of secondary aerosol particles to these sizes. We show that the effect is potentially significant, which highlights the importance of increasing understanding of these processes.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Deborah F. McGlynn, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 21, 15755–15770, https://doi.org/10.5194/acp-21-15755-2021, https://doi.org/10.5194/acp-21-15755-2021, 2021
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We present 1 year of hourly measurements of chemically resolved Biogenic volatile organic compound (BVOCs) between 15 September 2019 and 15 September 2020, collected at a research tower in central Virginia. Concentrations of a range of BVOCs are described and examined for their impact on atmospheric reactivity. The majority of reactivity comes from α-pinene and limonene, highlighting the importance of both concentration and structure in assessing atmospheric impacts of emissions.
Chenyang Bi, Jordan E. Krechmer, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6551–6560, https://doi.org/10.5194/amt-14-6551-2021, https://doi.org/10.5194/amt-14-6551-2021, 2021
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Calibration techniques have been recently developed to log-linearly correlate analyte sensitivity with CIMS operating conditions particularly for compounds without authentic standards. In this work, we examine the previously ignored bias in the log-linear-based calibration method and estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A step-by-step guide was provided to reduce and even remove the bias.
Huisheng Bian, Eunjee Lee, Randal D. Koster, Donifan Barahona, Mian Chin, Peter R. Colarco, Anton Darmenov, Sarith Mahanama, Michael Manyin, Peter Norris, John Shilling, Hongbin Yu, and Fanwei Zeng
Atmos. Chem. Phys., 21, 14177–14197, https://doi.org/10.5194/acp-21-14177-2021, https://doi.org/10.5194/acp-21-14177-2021, 2021
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Maria A. Zawadowicz, Kaitlyn Suski, Jiumeng Liu, Mikhail Pekour, Jerome Fast, Fan Mei, Arthur J. Sedlacek, Stephen Springston, Yang Wang, Rahul A. Zaveri, Robert Wood, Jian Wang, and John E. Shilling
Atmos. Chem. Phys., 21, 7983–8002, https://doi.org/10.5194/acp-21-7983-2021, https://doi.org/10.5194/acp-21-7983-2021, 2021
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This paper describes the results of a recent field campaign in the eastern North Atlantic, where two mass spectrometers were deployed aboard a research aircraft to measure the chemistry of aerosols and trace gases. Very clean conditions were found, dominated by local sulfate-rich acidic aerosol and very aged organics. Evidence of
long-range transport of aerosols from the continents was also identified.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Jiumeng Liu, Liz Alexander, Jerome D. Fast, Rodica Lindenmaier, and John E. Shilling
Atmos. Chem. Phys., 21, 5101–5116, https://doi.org/10.5194/acp-21-5101-2021, https://doi.org/10.5194/acp-21-5101-2021, 2021
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To bridge the gaps in modeling and observational results due to insufficient understanding of aerosol properties, co-located measurements of aerosols and trace gases were conducted at SGP during the HI-SCALE campaign. Organic aerosols at the SGP site exhibited to be highly oxidized, and biogenic emissions appear to largely control the formation of organic aerosols. Seasonal variations of sources and meteorological impacts likely resulted in the highly oxygenated feature of aerosols.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Lawrence I. Kleinman, Arthur J. Sedlacek III, Kouji Adachi, Peter R. Buseck, Sonya Collier, Manvendra K. Dubey, Anna L. Hodshire, Ernie Lewis, Timothy B. Onasch, Jeffery R. Pierce, John Shilling, Stephen R. Springston, Jian Wang, Qi Zhang, Shan Zhou, and Robert J. Yokelson
Atmos. Chem. Phys., 20, 13319–13341, https://doi.org/10.5194/acp-20-13319-2020, https://doi.org/10.5194/acp-20-13319-2020, 2020
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Aerosols from wildfires affect the Earth's temperature by absorbing light or reflecting it back into space. This study investigates time-dependent chemical, microphysical, and optical properties of aerosols generated by wildfires in the Pacific Northwest, USA. Wildfire smoke plumes were traversed by an instrumented aircraft at locations near the fire and up to 3.5 h travel time downwind. Although there was no net aerosol production, aerosol particles grew and became more efficient scatters.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
James F. Hurley, Nathan M. Kreisberg, Braden Stump, Chenyang Bi, Purushottam Kumar, Susanne V. Hering, Pat Keady, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 13, 4911–4925, https://doi.org/10.5194/amt-13-4911-2020, https://doi.org/10.5194/amt-13-4911-2020, 2020
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The chemical composition of aerosols has implications for human and ecosystem health. Current methods for determining chemical composition are expensive and require highly trained personnel. Our method is promising for moderate-cost, low-maintenance measurements of oxygen / carbon ratios, a key chemical parameter, and other elements may also be studied. In this work, we coupled two commonly used detectors to assess O / C ratios in a variety of compounds and mixtures within an acceptable error.
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Short summary
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.
In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate...
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