Articles | Volume 21, issue 22
https://doi.org/10.5194/acp-21-17031-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-17031-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Transport-driven aerosol differences above and below the canopy of a mixed deciduous forest
Alexander A. T. Bui
Department of Civil and Environmental Engineering, Rice University,
Houston, TX 77005, USA
Henry W. Wallace
Department of Civil and Environmental Engineering, Rice University,
Houston, TX 77005, USA
now at: Washington State Department of Ecology, Lacey, WA 98503,
USA
Sarah Kavassalis
Department of Chemistry, University of Toronto, Toronto, ON, M5S 3H6,
Canada
Hariprasad D. Alwe
Department of Soil, Water, and Climate, University of Minnesota, St
Paul, MN 55108, USA
James H. Flynn
Department of Earth and Atmospheric Sciences, University of
Houston, Houston, TX 77204, USA
Matt H. Erickson
Department of Earth and Atmospheric Sciences, University of
Houston, Houston, TX 77204, USA
now at: TerraGraphics Environmental Engineering, Pasco, WA 99301,
USA
Sergio Alvarez
Department of Earth and Atmospheric Sciences, University of
Houston, Houston, TX 77204, USA
Dylan B. Millet
Department of Soil, Water, and Climate, University of Minnesota, St
Paul, MN 55108, USA
Allison L. Steiner
Department of Climate and Space Sciences and Engineering,
University of Michigan, Ann Arbor, MI 48109, USA
Robert J. Griffin
CORRESPONDING AUTHOR
Department of Civil and Environmental Engineering, Rice University,
Houston, TX 77005, USA
Department of Chemical and Biomolecular Engineering, Rice
University, Houston, TX 77005, USA
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Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
Candice L. Sirmollo, Don R. Collins, Jordan M. McCormick, Cassandra F. Milan, Matthew H. Erickson, James H. Flynn, Rebecca J. Sheesley, Sascha Usenko, Henry W. Wallace, Alexander A. T. Bui, Robert J. Griffin, Matthew Tezak, Sean M. Kinahan, and Joshua L. Santarpia
Atmos. Meas. Tech., 14, 3351–3370, https://doi.org/10.5194/amt-14-3351-2021, https://doi.org/10.5194/amt-14-3351-2021, 2021
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The newly developed portable 1 m3 CAGE chamber systems were characterized using data acquired during a 2-month field study in 2016 in a forested area north of Houston, TX, USA. Concentrations of several oxidant and organic compounds measured in the chamber were found to closely agree with those calculated with a zero-dimensional model. By tracking the modes of injected monodisperse particles, a pattern change was observed for hourly averaged growth rates between late summer and early fall.
Laura M. D. Heinlein, Junwei He, Michael Oluwatoyin Sunday, Fangzhou Guo, James Campbell, Allison Moon, Sukriti Kapur, Ting Fang, Kasey Edwards, Meeta Cesler-Maloney, Alyssa J. Burns, Jack Dibb, William Simpson, Manabu Shiraiwa, Becky Alexander, Jingqiu Mao, James H. Flynn III, Jochen Stutz, and Cort Anastasio
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High-latitude cities like Fairbanks, Alaska, experience severe wintertime pollution episodes. While conventional wisdom holds that oxidation is slow under these conditions, field measurements find oxidized products in particles. To explore this, we measured oxidants in aqueous extracts of winter particles from Fairbanks. We find high concentrations of oxidants during illumination experiments, indicating that particle photochemistry can be significant even in high latitudes during winter.
Hui Li, Philippe Ciais, Pramod Kumar, Didier A. Hauglustaine, Frédéric Chevallier, Grégoire Broquet, Dylan B. Millet, Kelley C. Wells, Jinghui Lian, and Bo Zheng
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-424, https://doi.org/10.5194/essd-2025-424, 2025
Preprint under review for ESSD
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We present the first global, multi-year maps of monthly isoprene emissions (2013–2020) derived from satellite isoprene observations, averaging 456 TgC yr-1. The dataset reveals two emission peaks linked to 2015–2016 El Niño and 2019–2020 extreme heat events, driven mainly by tropical regions such as the Amazon. It highlights the region-specific sensitivity of biogenic isoprene emissions to temperature anomalies, providing new insights into their roles in air quality and climate feedbacks.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
Atmos. Chem. Phys., 25, 5087–5100, https://doi.org/10.5194/acp-25-5087-2025, https://doi.org/10.5194/acp-25-5087-2025, 2025
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that the illumination of brown carbon can rapidly form HOOH within particles, even under the low-sunlight conditions of Fairbanks, Alaska, during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Meghan Guagenti, Darielle Dexheimer, Alexandra Ulinksi, Paul Walter, James H. Flynn III, and Sascha Usenko
Atmos. Meas. Tech., 18, 2125–2136, https://doi.org/10.5194/amt-18-2125-2025, https://doi.org/10.5194/amt-18-2125-2025, 2025
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A robust, automatic volatile organic compound (VOC) collection system was developed for vertical VOC sampling associated with the 2022 DOE ARM-program-led TRACER in Houston, Texas. This modular sampler has been developed to measure vertical profiles of VOCs to improve near-surface characterization. This article helps fill the current lack of commercially available options for aerial VOC sampling and serves to support and encourage researchers to build and develop custom samplers.
Joshua P. DiGangi, Glenn S. Diskin, Subin Yoon, Sergio L. Alvarez, James H. Flynn, Claire E. Robinson, Michael A. Shook, K. Lee Thornhill, Edward L. Winstead, Luke D. Ziemba, Maria Obiminda L. Cambaliza, James B. Simpas, Miguel Ricardo A. Hilario, and Armin Sorooshian
EGUsphere, https://doi.org/10.5194/egusphere-2025-1454, https://doi.org/10.5194/egusphere-2025-1454, 2025
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Both fire and urban emissions are major contributors to air pollution in Southeast Asia. Relative increases in measurements of methane and carbon monoxide gases during an aircraft campaign near the Philippines in 2019 were used to isolate pollution emissions from fires vs urban sources. Results were compared to atmospheric transport models to determine the sources' regional origins, and relationships between pollution indicators relevant to poor air quality were investigated for each source.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Kelley C. Wells, Dylan B. Millet, Jared F. Brewer, Vivienne H. Payne, Karen E. Cady-Pereira, Rick Pernak, Susan Kulawik, Corinne Vigouroux, Nicholas Jones, Emmanuel Mahieu, Maria Makarova, Tomoo Nagahama, Ivan Ortega, Mathias Palm, Kimberly Strong, Matthias Schneider, Dan Smale, Ralf Sussmann, and Minqiang Zhou
Atmos. Meas. Tech., 18, 695–716, https://doi.org/10.5194/amt-18-695-2025, https://doi.org/10.5194/amt-18-695-2025, 2025
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Atmospheric volatile organic compounds (VOCs) affect both air quality and climate. Satellite measurements can help us to assess and predict their global impacts. We present new decadal (2012–2023) measurements of four key VOCs – methanol, ethene, ethyne, and hydrogen cyanide (HCN) – from the Cross-track Infrared Sounder. The measurements reflect emissions from major forests, wildfires, and industry and provide new information to advance understanding of these sources and their changes over time.
Bryan N. Duncan, Daniel C. Anderson, Arlene M. Fiore, Joanna Joiner, Nickolay A. Krotkov, Can Li, Dylan B. Millet, Julie M. Nicely, Luke D. Oman, Jason M. St. Clair, Joshua D. Shutter, Amir H. Souri, Sarah A. Strode, Brad Weir, Glenn M. Wolfe, Helen M. Worden, and Qindan Zhu
Atmos. Chem. Phys., 24, 13001–13023, https://doi.org/10.5194/acp-24-13001-2024, https://doi.org/10.5194/acp-24-13001-2024, 2024
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Trace gases emitted to or formed within the atmosphere may be chemically or physically removed from the atmosphere. One trace gas, the hydroxyl radical (OH), is responsible for initiating the chemical removal of many trace gases, including some greenhouse gases. Despite its importance, scientists have not been able to adequately measure OH. In this opinion piece, we discuss promising new methods to indirectly constrain OH using satellite data of trace gases that control the abundance of OH.
Lee Tiszenkel, James H. Flynn, and Shan-Hu Lee
Atmos. Chem. Phys., 24, 11351–11363, https://doi.org/10.5194/acp-24-11351-2024, https://doi.org/10.5194/acp-24-11351-2024, 2024
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Ammonia and amines are important ingredients for aerosol formation in urban environments, but the measurements of these compounds are extremely challenging. Our observations show that urban ammonia and amines in Houston are emitted from urban sources, and diurnal variations in their concentrations are likely governed by gas-to-particle conversion and emissions.
Akinleye Folorunsho, Jimy Dudhia, John Sullivan, Paul Walter, James Flynn, Travis Griggs, Rebecca Sheesley, Sascha Usenko, Guillaume Gronoff, Mark Estes, and Yang Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-1190, https://doi.org/10.5194/egusphere-2024-1190, 2024
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Our study investigates the factors driving high ozone levels over the Houston urban area. Using advanced modeling techniques and real-world measurements, we found vehicle and industrial emissions especially of highly reactive organic compounds play a key role in ozone formation. Our study highlights spatial and temporal changes in ozone sensitivity and variability of atmosphere's self-cleaning capacity to emissions, signifying effective ways of controlling emissions to mitigate urban ozone.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
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Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
Wei Li, Yuxuan Wang, Xueying Liu, Ehsan Soleimanian, Travis Griggs, James Flynn, and Paul Walter
Atmos. Chem. Phys., 23, 13685–13699, https://doi.org/10.5194/acp-23-13685-2023, https://doi.org/10.5194/acp-23-13685-2023, 2023
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This study examined high offshore ozone events in Galveston Bay and the Gulf of Mexico, using boat data and WRF–CAMx modeling during the TRACER-AQ 2021 field campaign. On average, high ozone is caused by chemistry due to the regional transport of volatile organic compounds and downwind advection of NOx from the ship channel. Two case studies show advection of ozone can be another process leading to high ozone, and accurate wind prediction is crucial for air quality forecasting in coastal areas.
Sujan Shrestha, Shan Zhou, Manisha Mehra, Meghan Guagenti, Subin Yoon, Sergio L. Alvarez, Fangzhou Guo, Chun-Ying Chao, James H. Flynn III, Yuxuan Wang, Robert J. Griffin, Sascha Usenko, and Rebecca J. Sheesley
Atmos. Chem. Phys., 23, 10845–10867, https://doi.org/10.5194/acp-23-10845-2023, https://doi.org/10.5194/acp-23-10845-2023, 2023
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We evaluated different methods for assessing the influence of long-range transport of biomass burning (BB) plumes at a coastal site in Texas, USA. We show that the aerosol composition and optical properties exhibited good agreement, while CO and acetonitrile trends were less specific for assessing BB source influence. Our results demonstrate that the network of aerosol optical measurements can be useful for identifying the influence of aged BB plumes in anthropogenically influenced areas.
Xueying Liu, Yuxuan Wang, Shailaja Wasti, Wei Li, Ehsan Soleimanian, James Flynn, Travis Griggs, Sergio Alvarez, John T. Sullivan, Maurice Roots, Laurence Twigg, Guillaume Gronoff, Timothy Berkoff, Paul Walter, Mark Estes, Johnathan W. Hair, Taylor Shingler, Amy Jo Scarino, Marta Fenn, and Laura Judd
Geosci. Model Dev., 16, 5493–5514, https://doi.org/10.5194/gmd-16-5493-2023, https://doi.org/10.5194/gmd-16-5493-2023, 2023
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With a comprehensive suite of ground-based and airborne remote sensing measurements during the 2021 TRacking Aerosol Convection ExpeRiment – Air Quality (TRACER-AQ) campaign in Houston, this study evaluates the simulation of the planetary boundary layer (PBL) height and the ozone vertical profile by a high-resolution (1.33 km) 3-D photochemical model Weather Research and Forecasting-driven GEOS-Chem (WRF-GC).
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
Atmos. Chem. Phys., 23, 3325–3346, https://doi.org/10.5194/acp-23-3325-2023, https://doi.org/10.5194/acp-23-3325-2023, 2023
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We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
Vanessa Selimovic, Damien Ketcherside, Sreelekha Chaliyakunnel, Catherine Wielgasz, Wade Permar, Hélène Angot, Dylan B. Millet, Alan Fried, Detlev Helmig, and Lu Hu
Atmos. Chem. Phys., 22, 14037–14058, https://doi.org/10.5194/acp-22-14037-2022, https://doi.org/10.5194/acp-22-14037-2022, 2022
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Arctic warming has led to an increase in plants that emit gases in response to stress, but how these gases affect regional chemistry is largely unknown due to lack of observational data. Here we present the most comprehensive gas-phase measurements for this area to date and compare them to predictions from a global transport model. We report 78 gas-phase species and investigate their importance to atmospheric chemistry in the area, with broader implications for similar plant types.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386, https://doi.org/10.5194/acp-22-12367-2022, https://doi.org/10.5194/acp-22-12367-2022, 2022
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We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
Subin Yoon, Alexander Kotsakis, Sergio L. Alvarez, Mark G. Spychala, Elizabeth Klovenski, Paul Walter, Gary Morris, Ernesto Corrales, Alfredo Alan, Jorge A. Diaz, and James H. Flynn
Atmos. Meas. Tech., 15, 4373–4384, https://doi.org/10.5194/amt-15-4373-2022, https://doi.org/10.5194/amt-15-4373-2022, 2022
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SO2 is adverse to human health and the environment. A single SO2 sonde was developed to provide direct SO2 measurement with a greater vertical extent, a lower limit of detection, and less uncertainty relative to the previous dual-sonde method. The single sonde was tested in the field near volcanoes and anthropogenic sources where the sonde measured SO2 ranging from 0.5 to 940 ppb. This lighter-weight payload can be a great candidate to attach to small drones and unmanned aerial vehicles.
Rupert Holzinger, Oliver Eppers, Kouji Adachi, Heiko Bozem, Markus Hartmann, Andreas Herber, Makoto Koike, Dylan B. Millet, Nobuhiro Moteki, Sho Ohata, Frank Stratmann, and Atsushi Yoshida
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-95, https://doi.org/10.5194/acp-2022-95, 2022
Revised manuscript not accepted
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In spring 2018 the research aircraft Polar 5 conducted flights in the Arctic atmosphere. The flight operation was from Station Nord in Greenland, 1700 km north of the Arctic Circle (81°43'N, 17°47'W). Using a mass spectrometer we measured more than 100 organic compounds in the air. We found a clear signature of natural organic compounds that are transported from forests to the high Arctic. These compounds have the potential to change the cloud cover and energy budget of the Arctic region.
Xueying Yu, Dylan B. Millet, and Daven K. Henze
Geosci. Model Dev., 14, 7775–7793, https://doi.org/10.5194/gmd-14-7775-2021, https://doi.org/10.5194/gmd-14-7775-2021, 2021
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We conduct observing system simulation experiments to test how well inverse analyses of high-resolution satellite data from sensors such as TROPOMI can quantify methane emissions. Inversions can improve monthly flux estimates at 25 km even with a spatially biased prior or model transport errors, but results are strongly degraded when both are present. We further evaluate a set of alternate formalisms to overcome limitations of the widely used scale factor approach that arise for missing sources.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
Blake Actkinson, Katherine Ensor, and Robert J. Griffin
Atmos. Meas. Tech., 14, 5809–5821, https://doi.org/10.5194/amt-14-5809-2021, https://doi.org/10.5194/amt-14-5809-2021, 2021
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This paper describes the development of a new method used to estimate background from mobile monitoring time series. The method is tested on a previously published dataset, applied to an extensive mobile dataset, and compared with other previously published techniques used to estimate background. The results suggest that the method is a promising framework for background estimation.
Candice L. Sirmollo, Don R. Collins, Jordan M. McCormick, Cassandra F. Milan, Matthew H. Erickson, James H. Flynn, Rebecca J. Sheesley, Sascha Usenko, Henry W. Wallace, Alexander A. T. Bui, Robert J. Griffin, Matthew Tezak, Sean M. Kinahan, and Joshua L. Santarpia
Atmos. Meas. Tech., 14, 3351–3370, https://doi.org/10.5194/amt-14-3351-2021, https://doi.org/10.5194/amt-14-3351-2021, 2021
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The newly developed portable 1 m3 CAGE chamber systems were characterized using data acquired during a 2-month field study in 2016 in a forested area north of Houston, TX, USA. Concentrations of several oxidant and organic compounds measured in the chamber were found to closely agree with those calculated with a zero-dimensional model. By tracking the modes of injected monodisperse particles, a pattern change was observed for hourly averaged growth rates between late summer and early fall.
Ruud H. H. Janssen, Colette L. Heald, Allison L. Steiner, Anne E. Perring, J. Alex Huffman, Ellis S. Robinson, Cynthia H. Twohy, and Luke D. Ziemba
Atmos. Chem. Phys., 21, 4381–4401, https://doi.org/10.5194/acp-21-4381-2021, https://doi.org/10.5194/acp-21-4381-2021, 2021
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Bioaerosols are ubiquitous in the atmosphere and have the potential to affect cloud formation, as well as human and ecosystem health. However, their emissions are not well quantified, which hinders the assessment of their role in atmospheric processes. Here, we develop two new emission schemes for fungal spores based on multi-annual datasets of spore counts. We find that our modeled global emissions and burden are an order of magnitude lower than previous estimates.
Miguel Ricardo A. Hilario, Ewan Crosbie, Michael Shook, Jeffrey S. Reid, Maria Obiminda L. Cambaliza, James Bernard B. Simpas, Luke Ziemba, Joshua P. DiGangi, Glenn S. Diskin, Phu Nguyen, F. Joseph Turk, Edward Winstead, Claire E. Robinson, Jian Wang, Jiaoshi Zhang, Yang Wang, Subin Yoon, James Flynn, Sergio L. Alvarez, Ali Behrangi, and Armin Sorooshian
Atmos. Chem. Phys., 21, 3777–3802, https://doi.org/10.5194/acp-21-3777-2021, https://doi.org/10.5194/acp-21-3777-2021, 2021
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This study characterizes long-range transport from major Asian pollution sources into the tropical northwest Pacific and the impact of scavenging on these air masses. We combined aircraft observations, HYSPLIT trajectories, reanalysis, and satellite retrievals to reveal distinct composition and size distribution profiles associated with specific emission sources and wet scavenging. The results of this work have implications for international policymaking related to climate and health.
Loredana G. Suciu, Robert J. Griffin, and Caroline A. Masiello
Geosci. Model Dev., 14, 907–921, https://doi.org/10.5194/gmd-14-907-2021, https://doi.org/10.5194/gmd-14-907-2021, 2021
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Understanding the atmospheric degradation of biomass burning tracers such as levoglucosan is essential to decreasing uncertainties in the role of biomass burning in air quality, carbon cycling and paleoclimate. Using a 0-D modeling approach and numerical chamber simulations, we found that the multiphase atmospheric degradation of levoglucosan occurs over timescales of hours to days, can form secondary organic aerosols and affects other key tropospheric gases, such as ozone.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971, https://doi.org/10.5194/acp-21-951-2021, https://doi.org/10.5194/acp-21-951-2021, 2021
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Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Hélène Angot, Katelyn McErlean, Lu Hu, Dylan B. Millet, Jacques Hueber, Kaixin Cui, Jacob Moss, Catherine Wielgasz, Tyler Milligan, Damien Ketcherside, M. Syndonia Bret-Harte, and Detlev Helmig
Biogeosciences, 17, 6219–6236, https://doi.org/10.5194/bg-17-6219-2020, https://doi.org/10.5194/bg-17-6219-2020, 2020
Short summary
Short summary
We report biogenic volatile organic compounds (BVOCs) ambient levels and emission rates from key vegetation species in the Alaskan arctic tundra, providing a new data set to further constrain isoprene chemistry under low NOx conditions in models. We add to the growing body of evidence that climate-induced changes in the vegetation composition will significantly affect the BVOC emission potential of the tundra, with implications for atmospheric oxidation processes and climate feedbacks.
Cited articles
Alwe, H. D., Millet, D. B., Chen, X., Raff, J. D., Payne, Z. C., and Fledderman, K.:
Oxidation of volatile organic compounds as the major source of formic acid
in a mixed forest canopy, Geophys. Res. Lett., 46, 2940–2948,
https://doi.org/10.1029/2018GL081526, 2019.
Ashworth, K., Chung, S. H., Griffin, R. J., Chen, J., Forkel, R., Bryan, A. M., and Steiner, A. L.: FORest Canopy Atmosphere Transfer (FORCAsT) 1.0: a 1-D model of biosphere–atmosphere chemical exchange, Geosci. Model Dev., 8, 3765–3784, https://doi.org/10.5194/gmd-8-3765-2015, 2015.
Baldocchi, D., Guenther, A. B., Harley, P., Klinger, L., Zimmerman, P., Lamb,
B., and Westberg, H.: The fluxes and air chemistry of isoprene above a deciduous
hardwood forest, Philos. T. R. Soc. A, 351, 279–296,
https://doi.org/10.1098/rsta.1995.0034, 1995.
Bergen, K. M. and Dronova, I.: Observing succession on aspen-dominated
landscapes using a remote sensing-ecosystem approach, Landscape Ecol., 22,
1395–1410, https://doi.org/10.1007/s10980-007-9119-1, 2007.
Berkowitz, C. M., Fast, J. D., Springston, S. R., Larsen, R. J., Spicer, C. W.,
Doskey, P. V., Hubbe, J. M., and Plastridge, R.: Formation mechanisms and chemical
characteristics of elevated photochemical layers over the northeast United
States, J. Geophys. Res., 103, 10631–10647,
https://doi.org/10.1029/97JD03751, 1998.
Bondy, A. L., Wang, B., Laskin, A., Craig, R. L., Nhliziyo, M. V., Bertman, S.,
Pratt, K. A., Shepson, P. B., and Ault, A. P.: Inland sea spray aerosol transport
and incomplete chloride depletion: Varying degrees of reactive processing
observed during SOAS, Environ. Sci. Technol., 51, 9533–9542,
https://doi.org/10.1021/acs.est.7b02085, 2017.
Brown, S. S., Osthoff, H. D., Stark, H., Dubé, W. P., Ryerson, T. B.,
Warneke, C., de Gouw, J. A., Wollny, A. G., Parrish, D. D., Fehsenfeld, F. C., and
Ravishankara, A. R.: Aircraft observations of daytime NO3 and
N2O5 and their implications for tropospheric chemistry, J.
Photochem. Photobiol. A, 176, 270–278,
https://doi.org/10.1016/j.jphotochem.2005.10.004, 2005.
Bryan, A. M., Bertman, S. B., Carroll, M. A., Dusanter, S., Edwards, G. D., Forkel, R., Griffith, S., Guenther, A. B., Hansen, R. F., Helmig, D., Jobson, B. T., Keutsch, F. N., Lefer, B. L., Pressley, S. N., Shepson, P. B., Stevens, P. S., and Steiner, A. L.: In-canopy gas-phase chemistry during CABINEX 2009: sensitivity of a 1-D canopy model to vertical mixing and isoprene chemistry, Atmos. Chem. Phys., 12, 8829–8849, https://doi.org/10.5194/acp-12-8829-2012, 2012.
Budisulistiorini, S. H., Nenes, A., Carlton, A. G., Surratt, J. D., McNeill,
V. F., and Pye, H. O. T.: Simulating aqueous-phase isoprene-epoxydiol (IEPOX)
secondary organic aerosol production during the 2013 Southern Oxidant and
Aerosol Study (SOAS), Environ. Sci. Technol., 51, 5026–5034,
https://doi.org/10.1021/acs.est.6b05750, 2017.
Canagaratna, M. R., Jimenez, J. L., Kroll, J. H., Chen, Q., Kessler, S. H., Massoli, P., Hildebrandt Ruiz, L., Fortner, E., Williams, L. R., Wilson, K. R., Surratt, J. D., Donahue, N. M., Jayne, J. T., and Worsnop, D. R.: Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications, Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, 2015.
Carlton, A. G. and Baker, K. R.: Photochemical modeling of the Ozark isoprene
volcano: MEGAN, BEIS, and their impacts on air quality predictions, Environ.
Sci. Technol., 45, 4438–4445, https://doi.org/10.1021/es200050x, 2011.
Carroll, M. A., Bertman, S. B., and Shepson, P. B.: Overview of the Program for
Research on Oxidants: PHotochemistry, Emissions, and Transport (PROPHET)
summer 1998 measurements intensive, J. Geophys. Res., 106, 24275–24288,
https://doi.org/10.1029/2001JD900189, 2001.
Chang, Y., Deng, C., Cao, F., Cao, C., Zou, Z., Liu, S., Lee, X., Li, J., Zhang, G., and Zhang, Y.: Assessment of carbonaceous aerosols in Shanghai, China – Part 1: long-term evolution, seasonal variations, and meteorological effects, Atmos. Chem. Phys., 17, 9945–9964, https://doi.org/10.5194/acp-17-9945-2017, 2017.
Cooper, O. R., Moody, J. L., Thornberry, T. D., Town, M. S., and Carroll, M. A.:
PROPHET 1998 meteorological overview and air-mass classification, J.
Geophys. Res., 106, 24289–24299, https://doi.org/10.1029/2000JD900409, 2001.
Cubison, M. J., Ortega, A. M., Hayes, P. L., Farmer, D. K., Day, D., Lechner, M. J., Brune, W. H., Apel, E., Diskin, G. S., Fisher, J. A., Fuelberg, H. E., Hecobian, A., Knapp, D. J., Mikoviny, T., Riemer, D., Sachse, G. W., Sessions, W., Weber, R. J., Weinheimer, A. J., Wisthaler, A., and Jimenez, J. L.: Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies, Atmos. Chem. Phys., 11, 12049–12064, https://doi.org/10.5194/acp-11-12049-2011, 2011.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T.,
Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop,
D. R., and Jimenez, J. L.: Field-deployable, high-resolution, time-of-flight
aerosol mass spectrometer, Anal. Chem., 78, 8281–8289,
https://doi.org/10.1021/ac061249n, 2006.
Ditto, J. C., Barnes, E. B., Khare, P., Takeuchi, M., Joo, T., Bui, A. A. T.,
Lee-Taylor, J., Eris, G., Chen, Y., Aumont, B., Jimenez, J. L., Ng, N. L.,
Griffin, R. J., and Gentner, D. R.: An omnipresent diversity and variability in
the chemical composition of atmospheric functionalized organic aerosol,
Comm. Chem., 1, 75, https://doi.org/10.1038/s42004-018-0074-3, 2018.
Draxler, R. R. and Hess, G. D.: An overview of the HYSPLIT_4
modeling system for trajectories, dispersion, and deposition, Aust.
Meteorol. Mag., 47, 295–308, 1998.
El-Sayed, M. M. H., Ortiz-Montalvo, D. L., and Hennigan, C. J.: The effects of isoprene and NOx on secondary organic aerosols formed through reversible and irreversible uptake to aerosol water, Atmos. Chem. Phys., 18, 1171–1184, https://doi.org/10.5194/acp-18-1171-2018, 2018.
Farmer, D. K., Chen, Q., Kimmel, J. R., Docherty, K. S., Nemitz, E., Artaxo,
P. A., Cappa, C. D., Martin, S. T., and Jimenez, J. L.: Chemically resolved particle
fluxes over tropical and temperate forests, Aerosol Sci. Tech., 47,
818–830, https://doi.org/10.1080/02786826.2013.791022, 2013.
Finnigan, J.: Turbulence in plant canopies, Annu. Rev. Fluid Mech., 32,
519–571, https://doi.org/10.1146/annurev.fluid.32.1.519, 2000.
Foken, T.: Micrometeorology, Springer-Verlag, Berlin, 306 pp., 2008.
Foken, T., Meixner, F. X., Falge, E., Zetzsch, C., Serafimovich, A., Bargsten, A., Behrendt, T., Biermann, T., Breuninger, C., Dix, S., Gerken, T., Hunner, M., Lehmann-Pape, L., Hens, K., Jocher, G., Kesselmeier, J., Lüers, J., Mayer, J.-C., Moravek, A., Plake, D., Riederer, M., Rütz, F., Scheibe, M., Siebicke, L., Sörgel, M., Staudt, K., Trebs, I., Tsokankunku, A., Welling, M., Wolff, V., and Zhu, Z.: Coupling processes and exchange of energy and reactive and non-reactive trace gases at a forest site – results of the EGER experiment, Atmos. Chem. Phys., 12, 1923–1950, https://doi.org/10.5194/acp-12-1923-2012, 2012.
Fuentes, J. D., Wang, D., Bowling, D. R., Potosnak, M., Monson, R. K., Goliff,
W. S., and Stockwell, W. R.: Biogenic hydrocarbon chemistry within and above a
mixed deciduous forest, J. Atmos. Chem. 56, 165–185,
https://doi.org/10.1007/s10874-006-9048-4, 2007.
Gao, W., Wesely, M. L., and Doskey, P. V.: Numerical modeling of the turbulent
diffusion and chemistry of NOx, O3, isoprene, and other reactive
trace gases in and above a forest canopy, J. Geophys. Res., 98, 18339–18353,
https://doi.org/10.1029/93JD01862, 1993.
Geron, C., Rasmussen, R., Arnts, R., and Guenther, A.: A review and synthesis
of monoterpene speciation from forests in the United States, Atmos. Environ.,
34, 1761–1781, https://doi.org/10.1016/S1352-2310(99)00364-7, 2000.
Goldstein, A. H. and Galbally, I. E.: Known and unexplored organic constituents
in the Earth's atmosphere, Environ. Sci. Technol., 41, 1514–1521,
https://doi.org/10.1021/es072476p, 2007.
Gordon, M., Staebler, R. M., Liggio, J., Vlasenko, A., Li, S.-M., and Hayden, K.: Aerosol flux measurements above a mixed forest at Borden, Ontario, Atmos. Chem. Phys., 11, 6773–6786, https://doi.org/10.5194/acp-11-6773-2011, 2011.
Guenther, A., Geron, C., Pierce, T., Lamb, B., Harley, P., and Fall, R.: Natural
emissions of non-methane volatile organic compounds, carbon monoxide, and
oxides of nitrogen from North America, Atmos. Environ., 34, 2205–2230,
https://doi.org/10.1016/S1352-2310(99)00465-3, 2000.
Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T.,
Harley, P., Klinger, L., Lerdau, M., McKay, W. A., Pierce, T., Scholes, B.,
Steinbrecher, R., Tallamraju, R., Taylor, J., and Zimmerman, P.: A global model
of natural volatile organic compound emissions, J. Geophys. Res., 100,
8873–8892, https://doi.org/10.1029/94JD02950, 1995.
Gunsch, M. J., May, N. W., Wen, M., Bottenus, C. L. H., Gardner, D. J., VanReken, T. M., Bertman, S. B., Hopke, P. K., Ault, A. P., and Pratt, K. A.: Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region, Atmos. Chem. Phys., 18, 3701–3715, https://doi.org/10.5194/acp-18-3701-2018, 2018.
Holzinger, R., Lee, A., Paw, K. T., and Goldstein, U. A. H.: Observations of oxidation products above a forest imply biogenic emissions of very reactive compounds, Atmos. Chem. Phys., 5, 67–75, https://doi.org/10.5194/acp-5-67-2005, 2005.
Hu, W. W., Campuzano-Jost, P., Palm, B. B., Day, D. A., Ortega, A. M., Hayes, P. L., Krechmer, J. E., Chen, Q., Kuwata, M., Liu, Y. J., de Sá, S. S., McKinney, K., Martin, S. T., Hu, M., Budisulistiorini, S. H., Riva, M., Surratt, J. D., St. Clair, J. M., Isaacman-Van Wertz, G., Yee, L. D., Goldstein, A. H., Carbone, S., Brito, J., Artaxo, P., de Gouw, J. A., Koss, A., Wisthaler, A., Mikoviny, T., Karl, T., Kaser, L., Jud, W., Hansel, A., Docherty, K. S., Alexander, M. L., Robinson, N. H., Coe, H., Allan, J. D., Canagaratna, M. R., Paulot, F., and Jimenez, J. L.: Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements, Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, 2015.
IPCC: Climate change 2007: The physical science basis: Contribution of
Working Group I to the Fourth Assessment Report of the Intergovernmental
Panel on Climate Change, Cambridge University Press, Cambridge, New York,
2007.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q.,
Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C.,
Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J.,
Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J.,
Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M.,
Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E.,
Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K.,
Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian,
K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T.,
Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel,
J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams,
L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop,
D. R.: Evolution of organic aerosols in the atmosphere, Science, 326,
1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Jokinen, T., Berndt, T., Makkonen, R., Kerminen, V.-M., Junninen, H.,
Paasonen, P., Stratmann, F., Herrmann, H., Guenther, A. B., Worsnop, D. R.,
Kulmala, M., Ehn, M., and Sipilä, M.: Production of extremely low volatile
organic compounds from biogenic emissions: Measured yields and atmospheric
implications, P. Natl. Acad. Sci. USA, 112, 7123–7128,
https://doi.org/10.1073/pnas.1423977112, 2015.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
Kroll, J. H., Donahue, N. M., Jimenez, J. L., Kessler, S. H., Canagaratna, M. R.,
Wilson, K. R., Altieri, K. E., Mazzoleni, L. R., Wozniak, A. S., Bluhm, H.,
Mysak, E. R., Smith, J. D., Kolb, C. E., and Worsnop, D. R.: Carbon oxidation state
as a metric for describing the chemistry of atmospheric organic aerosol,
Nat. Chem., 3, 133–139, https://doi.org/10.1038/nchem.948, 2011.
Kruijt, B., Malhi, Y., Lloyd, J., Norbre, A. D., Miranda, A. C., Pereira,
M. G. P., Culf, A., and Grace, J.: Turbulence statistics above and within two
Amazon rainforest canopies, Bound.-Lay. Meteorol., 94, 297–331,
https://doi.org/10.1023/A:1002401829007, 2000.
Leong, Y. J., Sanchez, N. P., Wallace, H. W., Cevik, B. K., Hernandez, C. S.,
Han, Y., Flynn, J. H., Massoli, P., Floerchinger, C., Fortner, E. C., Herndon,
S., Bean, J. K., Ruiz, L. H., Jeon, W., Choi, Y., Lefer, B., and Griffin, R. J.:
Overview of surface measurements and spatial characterization of
submicrometer particulate matter during the DISCOVER-AQ 2013 campaign in
Houston, TX, J. Air Waste Manage., 67, 854–872,
https://doi.org/10.1080/10962247.2017.1296502, 2017.
Makar, P. A., Staebler, R. M., Akingunola, A., Zhang, J., McLinden, C.,
Kharol, S. K., Pabla, B., Cheung, P., and Zheng, Q.: The effects of forest canopy
shading and turbulence on boundary layer ozone, Nat. Commun., 8, 15243,
https://doi.org/10.1038/ncomms15243, 2017.
Marais, E. A., Jacob, D. J., Jimenez, J. L., Campuzano-Jost, P., Day, D. A., Hu, W., Krechmer, J., Zhu, L., Kim, P. S., Miller, C. C., Fisher, J. A., Travis, K., Yu, K., Hanisco, T. F., Wolfe, G. M., Arkinson, H. L., Pye, H. O. T., Froyd, K. D., Liao, J., and McNeill, V. F.: Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls, Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, 2016.
Middlebrook, A. M., Bahreini, R., Jimenez, J. L., and Canagaratna, M. R.:
Evaluation of composition-dependent collection efficiencies for the Aerodyne
aerosol mass spectrometer using field data, Aerosol Sci. Tech., 46,
258–271, https://doi.org/10.1080/02786826.2011.620041, 2012.
Millet, D. B., Alwe, H. D., Chen, X., Deventer, M. J., Griffis, T. J.,
Holzinger, R., Bertman, S. B., Rickly, P. S., Stevens, P. S., Léonardis,
T., Locoge, N., Dusanter, S., Tyndall, G. S., Alvarez, S. L., Erickson, M. H., and
Flynn, J. H.: Bidirectional ecosystem–atmosphere fluxes of volatile organic
compounds across the mass spectrum: How many matter?, ACS Earth Space Chem.,
2, 764–777, https://doi.org/10.1021/acsearthspacechem.8b00061, 2018.
Miyazaki, Y., Fu, P., Ono, K., Tachibana, E., and Kawamura, K.: Seasonal cycles
of water-soluble organic nitrogen aerosols in a deciduous broadleaf forest
in northern Japan, J. Geophys. Res., 119, 1440–1454,
https://doi.org/10.1002/2013JD020713, 2014.
Mohr, C., DeCarlo, P. F., Heringa, M. F., Chirico, R., Slowik, J. G., Richter, R., Reche, C., Alastuey, A., Querol, X., Seco, R., Peñuelas, J., Jiménez, J. L., Crippa, M., Zimmermann, R., Baltensperger, U., and Prévôt, A. S. H.: Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data, Atmos. Chem. Phys., 12, 1649–1665, https://doi.org/10.5194/acp-12-1649-2012, 2012.
National Atmospheric Deposition Program: National Trends Network (NTN) Site
Details, available at:
https://nadp.slh.wisc.edu/sites/ntn-mi09/ (last access: 20 November 2021),
2016.
Ng, N. L., Canagaratna, M. R., Zhang, Q., Jimenez, J. L., Tian, J., Ulbrich, I. M., Kroll, J. H., Docherty, K. S., Chhabra, P. S., Bahreini, R., Murphy, S. M., Seinfeld, J. H., Hildebrandt, L., Donahue, N. M., DeCarlo, P. F., Lanz, V. A., Prévôt, A. S. H., Dinar, E., Rudich, Y., and Worsnop, D. R.: Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry, Atmos. Chem. Phys., 10, 4625–4641, https://doi.org/10.5194/acp-10-4625-2010, 2010.
Öztürk, F., Bahreini, R., Wagner, N. L., Dubé, W. P., Young, C. J.,
Brown, S. S., Brock, C. A., Ulbrich, I. M., Jimenez, J. L., Cooper, O. R., and
Middlebrook, A. M.: Vertically resolved chemical characteristics and sources
of submicron aerosols measured on a tall tower in a suburban area near
Denver, Colorado in winter, J. Geophys. Res., 118, 13591–13605,
https://doi.org/10.1002/2013JD019923, 2013.
Paatero, P.: Least squares formulation of robust non-negative factor
analysis, Chemometr. Intell. Lab., 37, 23–35,
https://doi.org/10.1016/S0169-7439(96)00044-5, 1997.
Paatero, P. and Tapper, U.: Positive matrix factorization: A non-negative
factor model with optimal utilization of error estimates of data values,
Environmetrics, 5, 111–126, https://doi.org/10.1002/env.3170050203, 1994.
Polissar, A.: The aerosol at Barrow, Alaska: Long-term trends and source
locations, Atmos. Environ., 33, 2441–2458,
https://doi.org/10.1016/S1352-2310(98)00423-3, 1999.
Polissar, A. V., Hopke, P. K., and Harris, J. M.: Source regions for atmospheric
aerosol measured at Barrow, Alaska, Environ. Sci. Technol., 35, 4214–4226,
https://doi.org/10.1021/es0107529, 2001.
Pryor, S. C., Larsen, S. E., Sørensen, L. L., Barthelmie, R. J.,
Grönholm, T., Kulmala, M., Launiainen, S., Rannik, Ü., and Vesala, T.:
Particle fluxes over forests: Analyses of flux methods and functional
dependencies, J. Geophys. Res., 112, D07205,
https://doi.org/10.1029/2006JD008066, 2007.
Pugh, T. A. M., MacKenzie, A. R., Hewitt, C. N., Langford, B., Edwards, P. M., Furneaux, K. L., Heard, D. E., Hopkins, J. R., Jones, C. E., Karunaharan, A., Lee, J., Mills, G., Misztal, P., Moller, S., Monks, P. S., and Whalley, L. K.: Simulating atmospheric composition over a South-East Asian tropical rainforest: performance of a chemistry box model, Atmos. Chem. Phys., 10, 279–298, https://doi.org/10.5194/acp-10-279-2010, 2010.
Rannik, Ü., Zhou, L., Zhou, P., Gierens, R., Mammarella, I., Sogachev, A., and Boy, M.: Aerosol dynamics within and above forest in relation to turbulent transport and dry deposition, Atmos. Chem. Phys., 16, 3145–3160, https://doi.org/10.5194/acp-16-3145-2016, 2016.
Rizzo, L. V., Artaxo, P., Karl, T., Guenther, A. B., and Greenberg, J.: Aerosol
properties, in-canopy gradients, turbulent fluxes and VOC concentrations at
a pristine forest site in Amazonia, Atmos. Environ., 44, 503–511,
https://doi.org/10.1016/j.atmosenv.2009.11.002, 2010.
Schulze, B. C., Wallace, H. W., Bui, A. T., Flynn, J. H., Erickson, M. H., Alvarez, S., Dai, Q., Usenko, S., Sheesley, R. J., and Griffin, R. J.: The impacts of regional shipping emissions on the chemical characteristics of coastal submicron aerosols near Houston, TX, Atmos. Chem. Phys., 18, 14217–14241, https://doi.org/10.5194/acp-18-14217-2018, 2018.
Schulze, B. C., Wallace, H. W., Flynn, J. H., Lefer, B. L., Erickson, M. H., Jobson, B. T., Dusanter, S., Griffith, S. M., Hansen, R. F., Stevens, P. S., VanReken, T., and Griffin, R. J.: Differences in BVOC oxidation and SOA formation above and below the forest canopy, Atmos. Chem. Phys., 17, 1805–1828, https://doi.org/10.5194/acp-17-1805-2017, 2017.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: From air
pollution to climate change, Hoboken, N.J., John Wiley, 2006.
Sheesley, R. J., Schauer, J. J., Bean, E., and Kenski, D.: Trends in secondary
organic aerosol at a remote site in Michigan's Upper Peninsula, Environ.
Sci. Technol., 38, 6491–6500, https://doi.org/10.1021/es049104q, 2004.
Sirois, A. and Bottenheim, J. W.: Use of backward trajectories to interpret the
5-year record of PAN and O3 ambient air concentrations at Kejimkujik
National Park, Nova Scotia, J. Geophys. Res., 100, 2867,
https://doi.org/10.1029/94JD02951, 1995.
Stein, A. F., Draxler, R. R., Rolph, G. D., Stunder, B. J. B., Cohen, M. D., and Ngan,
F.: NOAA's HYSPLIT atmospheric transport and dispersion modeling system,
B. Am. Meteorol. Soc., 96, 2059–2077,
https://doi.org/10.1175/BAMS-D-14-00110.1, 2015.
Steiner, A. L., Pressley, S. N., Botros, A., Jones, E., Chung, S. H., and Edburg, S. L.: Analysis of coherent structures and atmosphere-canopy coupling strength during the CABINEX field campaign, Atmos. Chem. Phys., 11, 11921–11936, https://doi.org/10.5194/acp-11-11921-2011, 2011.
Stroud, C., Makar, P., Karl, T., Guenther, A., Geron, C., Turnipseed, A.,
Nemitz, E., Baker, B., Potosnak, M., and Fuentes, J. D.: Role of canopy-scale
photochemistry in modifying biogenic-atmosphere exchange of reactive terpene
species: Results from the CELTIC field study, J. Geophys. Res., 110, D17303,
https://doi.org/10.1029/2005JD005775, 2005.
Thomas, C. and Foken, T.: Flux contribution of coherent structures and its
implications for the exchange of energy and matter in a tall spruce canopy,
Bound.-Lay. Meteorol., 123, 317–337,
https://doi.org/10.1007/s10546-006-9144-7, 2007.
Thornberry, T., Carroll, M. A., Keeler, G. A., Sanford, S., Bertman, S. B.,
Pippin, M. R., Ostling, K., Grossenbacher, J. W., Shepson, P. B., Cooper, O. R.,
Moody, J. L., and Stockwell, W. R.: Observations of reactive oxidized nitrogen and
speciation of NOy during the PROPHET summer 1998 intensive, J. Geophys.
Res., 106, 359–386, https://doi.org/10.1029/2000JD900760, 2001.
Toma, S. and Bertman, S.: The atmospheric potential of biogenic volatile organic compounds from needles of white pine (Pinus strobus) in Northern Michigan, Atmos. Chem. Phys., 12, 2245–2252, https://doi.org/10.5194/acp-12-2245-2012, 2012.
Ulbrich, I. M., Canagaratna, M. R., Zhang, Q., Worsnop, D. R., and Jimenez, J. L.: Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data, Atmos. Chem. Phys., 9, 2891–2918, https://doi.org/10.5194/acp-9-2891-2009, 2009.
US Census Bureau: City and Town Population Totals: 2010–2016, available at:
https://www.census.gov/data/tables/2016/demo/popest/total-cities-and-towns.html, last access: 24 January 2018.
VanReken, T. M., Mwaniki, G. R., Wallace, H. W., Pressley, S. N., Erickson,
M. H., Jobson, B. T., and Lamb, B. K.: Influence of air mass origin on aerosol
properties at a remote Michigan forest site, Atmos. Environ., 107, 35–43,
https://doi.org/10.1016/j.atmosenv.2015.02.027, 2015.
Wallace, H. W., Sanchez, N. P., Flynn, J. H., Erickson, M. H., Lefer, B. L., and
Griffin, R. J.: Source apportionment of particulate matter and trace gases
near a major refinery near the Houston Ship Channel, Atmos. Environ., 173,
16–29, https://doi.org/10.1016/j.atmosenv.2017.10.049, 2018.
Wang, Y. Q.: MeteoInfo: GIS software for meteorological data visualization
and analysis: Meteorological GIS software, Meteorol. Appl., 21,
360–368, https://doi.org/10.1002/met.1345, 2014.
Wang, Y. Q., Zhang, X. Y., and Draxler, R. R.: TrajStat: GIS-based software that
uses various trajectory statistical analysis methods to identify potential
sources from long-term air pollution measurement data, Environ. Model.
Softw., 24, 938–939, https://doi.org/10.1016/j.envsoft.2009.01.004, 2009.
Whitehead, J. D., Gallagher, M. W., Dorsey, J. R., Robinson, N., Gabey, A. M., Coe, H., McFiggans, G., Flynn, M. J., Ryder, J., Nemitz, E., and Davies, F.: Aerosol fluxes and dynamics within and above a tropical rainforest in South-East Asia, Atmos. Chem. Phys., 10, 9369–9382, https://doi.org/10.5194/acp-10-9369-2010, 2010.
Wiedinmyer, C., Greenberg, J., Guenther, A., Hopkins, B., Baker, K., Geron,
C., Palmer, P. I., Long, B. P., Turner, J. R., Pétron, G., Harley, P.,
Pierce, T. E., Lamb, B., Westberg, H., Baugh, W., Koerber, M., and Janssen, M.:
Ozarks Isoprene Experiment (OZIE): Measurements and modeling of the
“isoprene volcano”, J. Geophys. Res., 110, D18307,
https://doi.org/10.1029/2005JD005800, 2005.
Wolfe, G. M. and Thornton, J. A.: The Chemistry of Atmosphere-Forest Exchange (CAFE) Model – Part 1: Model description and characterization, Atmos. Chem. Phys., 11, 77–101, https://doi.org/10.5194/acp-11-77-2011, 2011.
Xu, L., Suresh, S., Guo, H., Weber, R. J., and Ng, N. L.: Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates, Atmos. Chem. Phys., 15, 7307–7336, https://doi.org/10.5194/acp-15-7307-2015, 2015.
Xu, L., Pye, H. O. T., He, J., Chen, Y., Murphy, B. N., and Ng, N. L.: Experimental and model estimates of the contributions from biogenic monoterpenes and sesquiterpenes to secondary organic aerosol in the southeastern United States, Atmos. Chem. Phys., 18, 12613–12637, https://doi.org/10.5194/acp-18-12613-2018, 2018.
Zhang, Q., Worsnop, D. R., Canagaratna, M. R., and Jimenez, J. L.: Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols, Atmos. Chem. Phys., 5, 3289–3311, https://doi.org/10.5194/acp-5-3289-2005, 2005.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H., Ulbrich,
I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L., Dzepina, K.,
Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch, T., Jayne,
J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N., Kondo, Y.,
Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K.,
Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J.,
Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and
dominance of oxygenated species in organic aerosols in
anthropogenically-influenced Northern Hemisphere midlatitudes: Ubiquity and
dominance of oxygenated OA, Geophys. Res. Lett., 34, L13801,
https://doi.org/10.1029/2007GL029979, 2007.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Ulbrich, I. M., Ng, N. L.,
Worsnop, D. R., and Sun, Y.: Understanding atmospheric organic aerosols via
factor analysis of aerosol mass spectrometry: A review, Anal.
Bioanal. Chem., 401, 3045–3067,
https://doi.org/10.1007/s00216-011-5355-y, 2011.
Short summary
Differences in atmospheric species above and below a forest canopy provide insight into the relative importance of local mixing, long-range transport, and chemical processes in determining vertical gradients in atmospheric particles in a forested environment. This helps in understanding the flux of climate-relevant material out of the forest to the atmosphere. We studied this in a remote forest using vertically resolved measurements of gases and particles.
Differences in atmospheric species above and below a forest canopy provide insight into the...
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