Articles | Volume 22, issue 21
https://doi.org/10.5194/acp-22-14037-2022
© Author(s) 2022. 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-22-14037-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmospheric biogenic volatile organic compounds in the Alaskan Arctic tundra: constraints from measurements at Toolik Field Station
Vanessa Selimovic
CORRESPONDING AUTHOR
Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA
Damien Ketcherside
Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA
Sreelekha Chaliyakunnel
Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA
Catherine Wielgasz
Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA
Wade Permar
Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA
Hélène Angot
Institute of Arctic and Alpine Research, University of Colorado Boulder, Boulder, CO, USA
now at: Ecole Polytechnique Fédérale de Lausanne (EPFL), Extreme
Environments Research Laboratory, Sion, Switzerland
Dylan B. Millet
Department of Soil, Water, and Climate,
University of Minnesota Twin Cities, St Paul, MN, USA
Alan Fried
Institute of Arctic and Alpine Research, University of Colorado Boulder, Boulder, CO, USA
Detlev Helmig
Boulder A.I.R LLC, Boulder, CO, USA
Department of Chemistry and Biochemistry, University of Montana, Missoula, MT, USA
Related authors
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
Short summary
Short summary
Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
Short summary
Short summary
This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
Short summary
Short summary
Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
Short summary
Short summary
Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
Short summary
Short summary
Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
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
Short summary
Short summary
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.
Wade Permar, Mercedes Tucker, and Lu Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2937, https://doi.org/10.5194/egusphere-2025-2937, 2025
Short summary
Short summary
Furanoids are VOCs that act as major OH sinks and ozone precursors in the atmosphere. We evaluate PTR-ToF-MS measurements of five furanoids under lab conditions. Sensitivities were stable across humidity and electric field changes, though a few compounds fragmented or formed hydrated ions. Long-term gas standard concentrations were also very stable. Consequently, PTR-ToF-MS accurately measures furanoids with calibration, though is likely affected by interferences from unknown ions and fragments.
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
Short summary
Short summary
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.
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
Short summary
Short summary
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.
Yugo Kanaya, Roberto Sommariva, Alfonso Saiz-Lopez, Andrea Mazzeo, Theodore K. Koenig, Kaori Kawana, James E. Johnson, Aurélie Colomb, Pierre Tulet, Suzie Molloy, Ian E. Galbally, Rainer Volkamer, Anoop Mahajan, John W. Halfacre, Paul B. Shepson, Julia Schmale, Hélène Angot, Byron Blomquist, Matthew D. Shupe, Detlev Helmig, Junsu Gil, Meehye Lee, Sean C. Coburn, Ivan Ortega, Gao Chen, James Lee, Kenneth C. Aikin, David D. Parrish, John S. Holloway, Thomas B. Ryerson, Ilana B. Pollack, Eric J. Williams, Brian M. Lerner, Andrew J. Weinheimer, Teresa Campos, Frank M. Flocke, J. Ryan Spackman, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Ralf M. Staebler, Amir A. Aliabadi, Wanmin Gong, Roeland Van Malderen, Anne M. Thompson, Ryan M. Stauffer, Debra E. Kollonige, Juan Carlos Gómez Martin, Masatomo Fujiwara, Katie Read, Matthew Rowlinson, Keiichi Sato, Junichi Kurokawa, Yoko Iwamoto, Fumikazu Taketani, Hisahiro Takashima, Monica Navarro Comas, Marios Panagi, and Martin G. Schultz
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-566, https://doi.org/10.5194/essd-2024-566, 2025
Revised manuscript accepted for ESSD
Short summary
Short summary
The first comprehensive dataset of tropospheric ozone over oceans/polar regions is presented, including 77 ship/buoy and 48 aircraft campaign observations (1977–2022, 0–5000 m altitude), supplemented by ozonesonde and surface data. Air masses isolated from land for 72+ hours are systematically selected as essentially oceanic. Among the 11 global regions, they show daytime decreases of 10–16% in the tropics, while near-zero depletions are rare, unlike in the Arctic, implying different mechanisms.
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
Short summary
Short summary
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.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
Short summary
Short summary
Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
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
Short summary
Short summary
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.
Yingjie Shen, Rudra P. Pokhrel, Amy P. Sullivan, Ezra J. T. Levin, Lauren A. Garofalo, Delphine K. Farmer, Wade Permar, Lu Hu, Darin W. Toohey, Teresa Campos, Emily V. Fischer, and Shane M. Murphy
Atmos. Chem. Phys., 24, 12881–12901, https://doi.org/10.5194/acp-24-12881-2024, https://doi.org/10.5194/acp-24-12881-2024, 2024
Short summary
Short summary
The magnitude and evolution of brown carbon (BrC) absorption remain unclear, with uncertainty in climate models. Data from the WE-CAN airborne experiment show that model parameterizations overestimate the mass absorption cross section (MAC) of BrC. Observed decreases in BrC absorption with chemical markers are due to decreasing organic aerosol (OA) mass rather than a decreasing BrC MAC, which is currently implemented in models. Water-soluble BrC contributes 23 % of total absorption at 660 nm.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
Short summary
Short summary
We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
Preprint withdrawn
Short summary
Short summary
High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
Short summary
Short summary
Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
Short summary
Short summary
Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
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
Short summary
Short summary
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.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
Short summary
Short summary
In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Kyoung-Min Kim, Si-Wan Kim, Seunghwan Seo, Donald R. Blake, Seogju Cho, James H. Crawford, Louisa K. Emmons, Alan Fried, Jay R. Herman, Jinkyu Hong, Jinsang Jung, Gabriele G. Pfister, Andrew J. Weinheimer, Jung-Hun Woo, and Qiang Zhang
Geosci. Model Dev., 17, 1931–1955, https://doi.org/10.5194/gmd-17-1931-2024, https://doi.org/10.5194/gmd-17-1931-2024, 2024
Short summary
Short summary
Three emission inventories were evaluated for East Asia using data acquired during a field campaign in 2016. The inventories successfully reproduced the daily variations of ozone and nitrogen dioxide. However, the spatial distributions of model ozone did not fully agree with the observations. Additionally, all simulations underestimated carbon monoxide and volatile organic compound (VOC) levels. Increasing VOC emissions over South Korea resulted in improved ozone simulations.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
Short summary
Short summary
Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
Short summary
Short summary
This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
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
Short summary
Short summary
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.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
Short summary
Short summary
Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
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
Short summary
Short summary
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.
Amir H. Souri, Matthew S. Johnson, Glenn M. Wolfe, James H. Crawford, Alan Fried, Armin Wisthaler, William H. Brune, Donald R. Blake, Andrew J. Weinheimer, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Corinne Vigouroux, Bavo Langerock, Sungyeon Choi, Lok Lamsal, Lei Zhu, Shuai Sun, Ronald C. Cohen, Kyung-Eun Min, Changmin Cho, Sajeev Philip, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 23, 1963–1986, https://doi.org/10.5194/acp-23-1963-2023, https://doi.org/10.5194/acp-23-1963-2023, 2023
Short summary
Short summary
We have rigorously characterized different sources of error in satellite-based HCHO / NO2 tropospheric columns, a widely used metric for diagnosing near-surface ozone sensitivity. Specifically, the errors were categorized/quantified into (i) an inherent chemistry error, (ii) the decoupled relationship between columns and the near-surface concentration, (iii) the spatial representativeness error of ground satellite pixels, and (iv) the satellite retrieval errors.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
Short summary
Short summary
The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities to but also distinct differences from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
Amy Christiansen, Loretta J. Mickley, Junhua Liu, Luke D. Oman, and Lu Hu
Atmos. Chem. Phys., 22, 14751–14782, https://doi.org/10.5194/acp-22-14751-2022, https://doi.org/10.5194/acp-22-14751-2022, 2022
Short summary
Short summary
Understanding tropospheric ozone trends is crucial for accurate predictions of future air quality and climate, but drivers of trends are not well understood. We analyze global tropospheric ozone trends since 1980 using ozonesonde and surface measurements, and we evaluate two models for their ability to reproduce trends. We find observational evidence of increasing tropospheric ozone, but models underestimate these increases. This hinders our ability to estimate ozone radiative forcing.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
Short summary
Short summary
This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
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
Short summary
Short summary
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.
Albane Barbero, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, Nicolas Caillon, and Joël Savarino
Atmos. Chem. Phys., 22, 12025–12054, https://doi.org/10.5194/acp-22-12025-2022, https://doi.org/10.5194/acp-22-12025-2022, 2022
Short summary
Short summary
The high reactivity of the summer Antarctic boundary layer results in part from the emissions of nitrogen oxides produced during photo-denitrification of the snowpack, but its underlying mechanisms are not yet fully understood. The results of this study suggest that more NO2 is produced from the snowpack early in the photolytic season, possibly due to stronger UV irradiance caused by a smaller solar zenith angle near the solstice.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
Short summary
Short summary
Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
Short summary
Short summary
California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
Short summary
Short summary
We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
Short summary
Short summary
Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
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
Short summary
Short summary
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.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
Short summary
Short summary
CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
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
Short summary
Short summary
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.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
Short summary
Short summary
Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Alexander A. T. Bui, Henry W. Wallace, Sarah Kavassalis, Hariprasad D. Alwe, James H. Flynn, Matt H. Erickson, Sergio Alvarez, Dylan B. Millet, Allison L. Steiner, and Robert J. Griffin
Atmos. Chem. Phys., 21, 17031–17050, https://doi.org/10.5194/acp-21-17031-2021, https://doi.org/10.5194/acp-21-17031-2021, 2021
Short summary
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.
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
Short summary
Short summary
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.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170, https://doi.org/10.5194/acp-21-15153-2021, https://doi.org/10.5194/acp-21-15153-2021, 2021
Short summary
Short summary
After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
Short summary
Short summary
Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
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
Short summary
Short summary
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.
Petter Weibring, Dirk Richter, James G. Walega, Alan Fried, Joshua DiGangi, Hannah Halliday, Yonghoon Choi, Bianca Baier, Colm Sweeney, Ben Miller, Kenneth J. Davis, Zachary Barkley, and Michael D. Obland
Atmos. Meas. Tech., 13, 6095–6112, https://doi.org/10.5194/amt-13-6095-2020, https://doi.org/10.5194/amt-13-6095-2020, 2020
Short summary
Short summary
The present study describes an autonomously operated instrument for high-precision (20–40 parts per trillion in 1 s) measurements of ethane during actual airborne operations on a small aircraft platform (NASA's King Air B200). This paper discusses the dynamic nature of airborne performance due to various aircraft-induced perturbations, methods devised to identify such events, and solutions we have enacted to circumvent these perturbations.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
Short summary
Short summary
We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304, https://doi.org/10.5194/acp-20-11287-2020, https://doi.org/10.5194/acp-20-11287-2020, 2020
Short summary
Short summary
Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
Johannes Bieser, Hélène Angot, Franz Slemr, and Lynwill Martin
Atmos. Chem. Phys., 20, 10427–10439, https://doi.org/10.5194/acp-20-10427-2020, https://doi.org/10.5194/acp-20-10427-2020, 2020
Short summary
Short summary
We use numerical models to determine the origin of air masses measured for elemental gaseous mercury (GEM) at Cape Point (CPT), South Africa. Our analysis is based on 10 years of hourly GEM measurements at CPT from 2007 to 2016. Based on GEM concentration and the origin of the air mass, we identify source and sink regions at CPT. We find, that the warm Agulhas Current to the south-east is the major Hg source and the continent the major sink.
Xiao Lu, Lin Zhang, Tongwen Wu, Michael S. Long, Jun Wang, Daniel J. Jacob, Fang Zhang, Jie Zhang, Sebastian D. Eastham, Lu Hu, Lei Zhu, Xiong Liu, and Min Wei
Geosci. Model Dev., 13, 3817–3838, https://doi.org/10.5194/gmd-13-3817-2020, https://doi.org/10.5194/gmd-13-3817-2020, 2020
Short summary
Short summary
This study presents the development and evaluation of a new climate chemistry model, BCC-GEOS-Chem v1.0, which couples the GEOS-Chem chemical transport model as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model. A 3-year (2012–2014) simulation of BCC-GEOS-Chem v1.0 shows that the model captures well the spatiotemporal distributions of tropospheric ozone, other gaseous pollutants, and aerosols.
Cited articles
Akagi, S. K., Yokelson, R. J., Wiedinmyer, C., Alvarado, M. J., Reid, J. S., Karl, T., Crounse, J. D., and Wennberg, P. O.: Emission factors for open and domestic biomass burning for use in atmospheric models, Atmos. Chem. Phys., 11, 4039–4072, https://doi.org/10.5194/acp-11-4039-2011, 2011.
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.
AMAP: Arctic Climate Change Update 2021: Key Trends and Impacts. Summary for Policy-makers. Arctic Monitoring and Assessment Programme (AMAP), Tromsø, Norway, 16 pp.,
https://www.amap.no/documents/doc/arctic-climate-change-update-2021-key-trends-and-impacts.-summary-for-policy-makers/3508
(last access: May 2022), 2021.
Angot, H., McErlean, K., Hu, L., Millet, D. B., Hueber, J., Cui, K., Moss, J., Wielgasz, C., Milligan, T., Ketcherside, D., Bret-Harte, M. S., and Helmig, D.: Biogenic volatile organic compound ambient mixing ratios and emission rates in the Alaskan Arctic tundra, Biogeosciences, 17, 6219–6236, https://doi.org/10.5194/bg-17-6219-2020, 2020.
Apel, E. C.: Measurement and interpretation of isoprene fluxes and isoprene,
methacrolein, and methyl vinyl ketone mixing ratios at the PROPHET site
during the 1998 Intensive, J. Geophys. Res., 107, 4034,
https://doi.org/10.1029/2000JD000225, 2002.
Atkinson, R. and Arey, J.: Atmospheric Degradation of Volatile Organic Compounds, Chem. Rev., 103, 4605–4638, https://doi.org/10.1021/cr0206420, 2003.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I – gas phase reactions of Ox, HOx, NOx and SOx species, Atmos. Chem. Phys., 4, 1461–1738, https://doi.org/10.5194/acp-4-1461-2004, 2004.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055, https://doi.org/10.5194/acp-6-3625-2006, 2006.
Bates, K. H., Jacob, D. J., Wang, S., Hornbrook, R. S., Apel, E. C., Kim, M.
J., Millet, D. B., Wells, K. C., Chen, X., Brewer, J. F., Ray, E. A.,
Commane, R., Diskin, G. S., and Wofsy, S. C.: The Global Budget of
Atmospheric Methanol: New Constraints on Secondary, Oceanic, and Terrestrial
Sources, 126, e2020JD033439,
https://doi.org/10.1029/2020JD033439, 2021.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation, J. Geophys. Res., 106, 23073–23095, https://doi.org/10.1029/2001JD000807, 2001.
Brasseur, G. P., Schultz, M., Granier, C., Saunois, M., Diehl, T., Botzet,
M., Roeckner, E., and Walters, S.: Impact of Climate Change on the Future
Chemical Composition of the Global Troposphere, J. Climate, 19,
3932–3951, https://doi.org/10.1175/JCLI3832.1, 2006.
Chen, X., Millet, D. B., Neuman, J. A., Veres, P. R., Ray, E. A., Commane,
R., Daube, B. C., McKain, K., Schwarz, J. P., Katich, J. M., Froyd, K. D.,
Schill, G. P., Kim, M. J., Crounse, J. D., Allen, H. M., Apel, E. C.,
Hornbrook, R. S., Blake, D. R., Nault, B. A., Campuzano-Jost, P., Jimenez,
J. L., and Dibb, J. E: HCOOH in the remote atmosphere: Constraints from
Atmospheric Tomography (ATom) airborne observations, ACS Earth Space Chem.,
5, 1436–1454, https://doi.org/10.1021/acsearthspacechem.1c00049, 2021.
Coggon, M. M., Lim, C. Y., Koss, A. R., Sekimoto, K., Yuan, B., Gilman, J. B., Hagan, D. H., Selimovic, V., Zarzana, K. J., Brown, S. S., Roberts, J. M., Müller, M., Yokelson, R., Wisthaler, A., Krechmer, J. E., Jimenez, J. L., Cappa, C., Kroll, J. H., de Gouw, J., and Warneke, C.: OH chemistry of non-methane organic gases (NMOGs) emitted from laboratory and ambient biomass burning smoke: evaluating the influence of furans and oxygenated aromatics on ozone and secondary NMOG formation, Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, 2019.
Elmendorf, S. C., Henry, G. H. R., Hollister, R. D., Björk, R. G.,
Boulanger-Lapointe, N., Cooper, E. J., Cornelissen, J. H. C., Day, T. A.,
Dorrepaal, E., Elumeeva, T. G., Gill, M., Gould, W. A., Harte, J., Hik, D.
S., Hofgaard, A., Johnson, D. R., Johnstone, J. F., Jónsdóttir, I.
S., Jorgenson, J. C., Klanderud, K., Klein, J. A., Koh, S., Kudo, G., Lara,
M., Lévesque, E., Magnússon, B., May, J. L., Mercado-Díaz, J.
A., Michelsen, A., Molau, U., Myers-Smith, I. H., Oberbauer, S. F.,
Onipchenko, V. G., Rixen, C., Schmidt, N. M., Shaver, G. R., Spasojevic, M.
J., Þórhallsdóttir, Þ. E., Tolvanen, A., Troxler, T.,
Tweedie, C. E., Villareal, S., Wahren, C.-H., Walker, X., Webber, P. J.,
Welker, J. M., and Wipf, S.: Plot-scale evidence of tundra vegetation change
and links to recent summer warming, Nat. Clim. Change, 2,
453–457, https://doi.org/10.1038/nclimate1465, 2012.
Emmons, L. K., Arnold, S. R., Monks, S. A., Huijnen, V., Tilmes, S., Law, K. S., Thomas, J. L., Raut, J.-C., Bouarar, I., Turquety, S., Long, Y., Duncan, B., Steenrod, S., Strode, S., Flemming, J., Mao, J., Langner, J., Thompson, A. M., Tarasick, D., Apel, E. C., Blake, D. R., Cohen, R. C., Dibb, J., Diskin, G. S., Fried, A., Hall, S. R., Huey, L. G., Weinheimer, A. J., Wisthaler, A., Mikoviny, T., Nowak, J., Peischl, J., Roberts, J. M., Ryerson, T., Warneke, C., and Helmig, D.: The POLARCAT Model Intercomparison Project (POLMIP): overview and evaluation with observations, Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, 2015.
Eyring, V., Köhler, H. W., Lauer, A., and Lemper, B.: Emissions from
international shipping: 2. Impact of future technologies on scenarios until
2050, J. Geophys. Res., 110, D17301,
https://doi.org/10.1029/2004JD005620, 2005.
Faubert, P., Tiiva, P., Rinnan, Å., Michelsen, A., Holopainen, J. K.,
and Rinnan, R.: Doubled volatile organic compound emissions from subarctic
tundra under simulated climate warming, New Phytol., 187, 199–208,
https://doi.org/10.1111/j.1469-8137.2010.03270.x, 2010.
Fontijn, A., A. J. Sabadell, and Ronco, R. J.: Homogenous chemiluminescent
measurement of nitric oxide with ozone – implications for continuous
selective monitoring of gaseous air pollutants, Anal. Chem., 42,
575, https://doi.org/10.1021/ac60288a034, 1970.
Franco, B., Blumenstock, T., Cho, C., Clarisse, L., Clerbaux, C., Coheur,
P.-F., De Mazière, M., De Smedt, I., Dorn, H.-P., Emmerichs, T., Fuchs,
H., Gkatzelis, G., Griffith, D. W. T., Gromov, S., Hannigan, J. W., Hase,
F., Hohaus, T., Jones, N., Kerkweg, A., Kiendler-Scharr, A., Lutsch, E.,
Mahieu, E., Novelli, A., Ortega, I., Paton-Walsh, C., Pommier, M., Pozzer,
A., Reimer, D., Rosanka, S., Sander, R., Schneider, M., Strong, K.,
Tillmann, R., Van Roozendael, M., Vereecken, L., Vigouroux, C., Wahner, A.,
and Taraborrelli, D.: Ubiquitous atmospheric production of organic acids
mediated by cloud droplets, Nature, 593, 233–237,
https://doi.org/10.1038/s41586-021-03462-x, 2021.
Frost, G. V., Bhatt, U. S., Epstein, H. E., Myers-Smith, I., Phoenix, G. K.,
Berner, L. T., Bjerke, J. W., Forbes, B. C., Goetz, S. J., Kerby, J. T.,
Macander, M. J., Park, T., Raynolds, M. K., Tømmervik, H., and Walker, D.
A.: Arctic Report Card 2020: Tundra Greenness, administrative report,
https://doi.org/10.25923/46RM-0W23, 2020.
Goldstein, A. H., Goulden, M. L., Munger, J. W., Wofsy, S. C., and Geron, C.
D.: Seasonal course of isoprene emissions from a midlatitude deciduous
forest, J. Geophys. Res.-Atmos., 103, 31045–31056, https://doi.org/10.1029/98JD02708, 1998.
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.
Gong, W., Beagley, S. R., Cousineau, S., Sassi, M., Munoz-Alpizar, R., Ménard, S., Racine, J., Zhang, J., Chen, J., Morrison, H., Sharma, S., Huang, L., Bellavance, P., Ly, J., Izdebski, P., Lyons, L., and Holt, R.: Assessing the impact of shipping emissions on air pollution in the Canadian Arctic and northern regions: current and future modelled scenarios, Atmos. Chem. Phys., 18, 16653–16687, https://doi.org/10.5194/acp-18-16653-2018, 2018.
Granier, C., Niemeier, U., Jungclaus, J. H., Emmons, L., Hess, P., Lamarque,
J.-F., Walters, S., and Brasseur, G. P.: Ozone pollution from future ship
traffic in the Arctic northern passages, Geophys. Res. Lett., 33,
L13807, https://doi.org/10.1029/2006GL026180, 2006.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Hansen, J., Ruedy, R., Sato, M., and Lo, K.: Global Surface Temperature
Change, Rev. Geophys., 48, RG4004, https://doi.org/10.1029/2010RG000345, 2010.
Hansen, R. F., Griffith, S. M., Dusanter, S., Rickly, P. S., Stevens, P. S., Bertman, S. B., Carroll, M. A., Erickson, M. H., Flynn, J. H., Grossberg, N., Jobson, B. T., Lefer, B. L., and Wallace, H. W.: Measurements of total hydroxyl radical reactivity during CABINEX 2009 – Part 1: field measurements, Atmos. Chem. Phys., 14, 2923–2937, https://doi.org/10.5194/acp-14-2923-2014, 2014.
Heald, C. L. and Kroll, J. H.: The fuel of atmospheric chemistry: Toward a
complete description of reactive organic carbon, Science Advances, 6,
eaay8967, https://doi.org/10.1126/sciadv.aay8967, 2020.
Heald, C. L., Goldstein, A. H., Allan, J. D., Aiken, A. C., Apel, E., Atlas, E. L., Baker, A. K., Bates, T. S., Beyersdorf, A. J., Blake, D. R., Campos, T., Coe, H., Crounse, J. D., DeCarlo, P. F., de Gouw, J. A., Dunlea, E. J., Flocke, F. M., Fried, A., Goldan, P., Griffin, R. J., Herndon, S. C., Holloway, J. S., Holzinger, R., Jimenez, J. L., Junkermann, W., Kuster, W. C., Lewis, A. C., Meinardi, S., Millet, D. B., Onasch, T., Polidori, A., Quinn, P. K., Riemer, D. D., Roberts, J. M., Salcedo, D., Sive, B., Swanson, A. L., Talbot, R., Warneke, C., Weber, R. J., Weibring, P., Wennberg, P. O., Worsnop, D. R., Wittig, A. E., Zhang, R., Zheng, J., and Zheng, W.: Total observed organic carbon (TOOC) in the atmosphere: a synthesis of North American observations, Atmos. Chem. Phys., 8, 2007–2025, https://doi.org/10.5194/acp-8-2007-2008, 2008.
Heald, C. L., Gouw, J. de, Goldstein, A. H., Guenther, A. B., Hayes, P. L.,
Hu, W., Isaacman-VanWertz, G., Jimenez, J. L., Keutsch, F. N., Koss, A. R.,
Misztal, P. K., Rappenglück, B., Roberts, J. M., Stevens, P. S.,
Washenfelder, R. A., Warneke, C., and Young, C. J.: Contrasting Reactive
Organic Carbon Observations in the Southeast United States (SOAS) and
Southern California (CalNex), Environ. Sci. Technol., 54, 14923–14935,
https://doi.org/10.1021/acs.est.0c05027, 2020.
Hoesly, R. M., Smith, S. J., Feng, L., Klimont, Z., Janssens-Maenhout, G., Pitkanen, T., Seibert, J. J., Vu, L., Andres, R. J., Bolt, R. M., Bond, T. C., Dawidowski, L., Kholod, N., Kurokawa, J.-I., Li, M., Liu, L., Lu, Z., Moura, M. C. P., O'Rourke, P. R., and Zhang, Q.: Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS), Geosci. Model Dev., 11, 369–408, https://doi.org/10.5194/gmd-11-369-2018, 2018.
Hornbrook, R. S., Hills, A. J., Riemer, D. D., Abdelhamid, A., Flocke, F.
M., Hall, S. R., Huey, L. G., Knapp, D. J., Liao, J., Mauldin, R. L.,
Montzka, D. D., Orlando, J. J., Shepson, P. B., Sive, B., Staebler, R. M.,
Tanner, D. J., Thompson, C. R., Turnipseed, A., Ullmann, K., Weinheimer, A.
J., and Apel, E. C.: Arctic springtime observations of volatile organic
compounds during the OASIS-2009 campaign, J. Geophys. Res.-Atmos., 121, 9789–9813,
https://doi.org/10.1002/2015JD024360, 2016.
Hu, L., Millet, D. B., Mohr, M. J., Wells, K. C., Griffis, T. J., and Helmig, D.: Sources and seasonality of atmospheric methanol based on tall tower measurements in the US Upper Midwest, Atmos. Chem. Phys., 11, 11145–11156, https://doi.org/10.5194/acp-11-11145-2011, 2011.
Hu, L., Millet, D. B., Baasandorj, M., Griffis, T. J., Turner, P., Helmig,
D., Curtis, A. J., and Hueber, J.: Isoprene emissions and impacts over an
ecological transition region in the U.S. Upper Midwest inferred from tall
tower measurements: Isoprene emissions in US Upper Midwest, J. Geophys. Res.-Atmos., 120, 3553–3571, https://doi.org/10.1002/2014JD022732,
2015.
Hunter, J. F., Day, D. A., Palm, B. B., Yatavelli, R. L. N., Chan, A. W. H.,
Kaser, L., Cappellin, L., Hayes, P. L., Cross, E. S., Carrasquillo, A. J.,
Campuzano-Jost, P., Stark, H., Zhao, Y., Hohaus, T., Smith, J. N., Hansel,
A., Karl, T., Goldstein, A. H., Guenther, A., Worsnop, D. R., Thornton, J.
A., Heald, C. L., Jimenez, J. L., and Kroll, J. H.: Comprehensive
characterization of atmospheric organic carbon at a forested site, Nat.
Geosci., 10, 748–753, https://doi.org/10.1038/ngeo3018, 2017.
Kade, A., Bret-Harte, M. S., Euskirchen, E. S., Edgar, C., and Fulweber, R.
A.: Upscaling of CO2 fluxes from heterogeneous tundra plant communities
in Arctic Alaska, J. Geophys. Res.-Biogeo., 117, G04007,
https://doi.org/10.1029/2012JG002065, 2012.
Kaiser, J. W., Heil, A., Andreae, M. O., Benedetti, A., Chubarova, N., Jones, L., Morcrette, J.-J., Razinger, M., Schultz, M. G., Suttie, M., and van der Werf, G. R.: Biomass burning emissions estimated with a global fire assimilation system based on observed fire radiative power, Biogeosciences, 9, 527–554, https://doi.org/10.5194/bg-9-527-2012, 2012.
Keller, C. A., Long, M. S., Yantosca, R. M., Da Silva, A. M., Pawson, S., and Jacob, D. J.: HEMCO v1.0: a versatile, ESMF-compliant component for calculating emissions in atmospheric models, Geosci. Model Dev., 7, 1409–1417, https://doi.org/10.5194/gmd-7-1409-2014, 2014.
Koesselmeier, J. and Staudt, M.: Biogenic Volatile Organic Compounds (VOC):
An Overview on Emission, Physiology and Ecology, J. Atmos.
Chem., 33, 23–88, https://doi.org/10.1023/A:1006127516791,
1999.
Koss, A. R., Sekimoto, K., Gilman, J. B., Selimovic, V., Coggon, M. M., Zarzana, K. J., Yuan, B., Lerner, B. M., Brown, S. S., Jimenez, J. L., Krechmer, J., Roberts, J. M., Warneke, C., Yokelson, R. J., and de Gouw, J.: Non-methane organic gas emissions from biomass burning: identification, quantification, and emission factors from PTR-ToF during the FIREX 2016 laboratory experiment, Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, 2018.
Kim, P. S., Jacob, D. J., Fisher, J. A., Travis, K., Yu, K., Zhu, L., Yantosca, R. M., Sulprizio, M. P., Jimenez, J. L., Campuzano-Jost, P., Froyd, K. D., Liao, J., Hair, J. W., Fenn, M. A., Butler, C. F., Wagner, N. L., Gordon, T. D., Welti, A., Wennberg, P. O., Crounse, J. D., St. Clair, J. M., Teng, A. P., Millet, D. B., Schwarz, J. P., Markovic, M. Z., and Perring, A. E.: Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model, Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, 2015.
Kirchner, F., Jeanneret, F., Clappier, A., Krüger, B., van den Bergh,
H., and Calpini, B.: Total VOC reactivity in the planetary boundary layer:
2. A new indicator for determining the sensitivity of the ozone production
to VOC and NOx, J. Geophys. Res., 106, 3095–3110,
https://doi.org/10.1029/2000JD900603, 2001.
Kramshøj, M., Vedel-Petersen, I., Schollert, M., Rinnan, Å., Nymand, J., Ro-Poulsen, H., and Rinnan, R.: Large increases in
Arctic biogenic volatile emissions are a direct effect of warming, Nat. Geosci., 9, 349–352, https://doi.org/10.1038/ngeo2692,
2016.
Lawrence, D. M., Oleson, K. W., Flanner, M. G., Thornton, P. E., Swenson, S.
C., Lawrence, P. J., Zeng, X., Yang, Z.-L., Levis, S., Sakaguchi, K., Bonan,
G. B., and Slater, A. G.: Parameterization improvements and functional and
structural advances in Version 4 of the Community Land Model, J.
Adv. Model. Earth Sy., 3, M03001,
https://doi.org/10.1029/2011MS00045, 2011.
Lindwall, F., Schollert, M., Michelsen, A., Blok, D., and Rinnan, R.:
Fourfold higher tundra volatile emissions due to arctic summer warming, J. Geophys. Res.-Atmos., 121,
895–902, https://doi.org/10.1002/2015JG003295, 2016.
Mao, J., Ren, X., Zhang, L., Van Duin, D. M., Cohen, R. C., Park, J.-H., Goldstein, A. H., Paulot, F., Beaver, M. R., Crounse, J. D., Wennberg, P. O., DiGangi, J. P., Henry, S. B., Keutsch, F. N., Park, C., Schade, G. W., Wolfe, G. M., Thornton, J. A., and Brune, W. H.: Insights into hydroxyl measurements and atmospheric oxidation in a California forest, Atmos. Chem. Phys., 12, 8009–8020, https://doi.org/10.5194/acp-12-8009-2012, 2012.
McDuffie, E. E., Smith, S. J., O'Rourke, P., Tibrewal, K., Venkataraman, C., Marais, E. A., Zheng, B., Crippa, M., Brauer, M., and Martin, R. V.: A global anthropogenic emission inventory of atmospheric pollutants from sector- and fuel-specific sources (1970–2017): an application of the Community Emissions Data System (CEDS), Earth Syst. Sci. Data, 12, 3413–3442, https://doi.org/10.5194/essd-12-3413-2020, 2020.
McGlynn, D. F., Barry, L. E. R., Lerdau, M. T., Pusede, S. E., and Isaacman-VanWertz, G.: Measurement report: Variability in the composition of biogenic volatile organic compounds in a Southeastern US forest and their role in atmospheric reactivity, Atmos. Chem. Phys., 21, 15755–15770, https://doi.org/10.5194/acp-21-15755-2021, 2021.
Millet, D. B., Guenther, A., Siegel, D. A., Nelson, N. B., Singh, H. B., de Gouw, J. A., Warneke, C., Williams, J., Eerdekens, G., Sinha, V., Karl, T., Flocke, F., Apel, E., Riemer, D. D., Palmer, P. I., and Barkley, M.: Global atmospheric budget of acetaldehyde: 3-D model analysis and constraints from in-situ and satellite observations, Atmos. Chem. Phys., 10, 3405–3425, https://doi.org/10.5194/acp-10-3405-2010, 2010.
Millet, D. B., Baasandorj, M., Farmer, D. K., Thornton, J. A., Baumann, K., Brophy, P., Chaliyakunnel, S., de Gouw, J. A., Graus, M., Hu, L., Koss, A., Lee, B. H., Lopez-Hilfiker, F. D., Neuman, J. A., Paulot, F., Peischl, J., Pollack, I. B., Ryerson, T. B., Warneke, C., Williams, B. J., and Xu, J.: A large and ubiquitous source of atmospheric formic acid, Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, 2015.
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.
Mungall, E. L., Abbatt, J. P. D., Wentzell, J. J. B., Wentworth, G. R., Murphy, J. G., Kunkel, D., Gute, E., Tarasick, D. W., Sharma, S., Cox, C. J., Uttal, T., and Liggio, J.: High gas-phase mixing ratios of formic and acetic acid in the High Arctic, Atmos. Chem. Phys., 18, 10237–10254, https://doi.org/10.5194/acp-18-10237-2018, 2018.
Nölscher, A. C., Williams, J., Sinha, V., Custer, T., Song, W., Johnson, A. M., Axinte, R., Bozem, H., Fischer, H., Pouvesle, N., Phillips, G., Crowley, J. N., Rantala, P., Rinne, J., Kulmala, M., Gonzales, D., Valverde-Canossa, J., Vogel, A., Hoffmann, T., Ouwersloot, H. G., Vilà-Guerau de Arellano, J., and Lelieveld, J.: Summertime total OH reactivity measurements from boreal forest during HUMPPA-COPEC 2010, Atmos. Chem. Phys., 12, 8257–8270, https://doi.org/10.5194/acp-12-8257-2012, 2012.
Pagonis, D., Sekimoto, K., and de Gouw, J.: A Library of Proton-Transfer
Reactions of H3O+ Ions Used for Trace Gas Detection, J. Am. Soc. Mass.
Spectrom., 30, 1330–1335,
https://doi.org/10.1007/s13361-019-02209-3, 2019.
Paulot, F., Wunch, D., Crounse, J. D., Toon, G. C., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., González Abad, G., Notholt, J., Warneke, T., Hannigan, J. W., Warneke, C., de Gouw, J. A., Dunlea, E. J., De Mazière, M., Griffith, D. W. T., Bernath, P., Jimenez, J. L., and Wennberg, P. O.: Importance of secondary sources in the atmospheric budgets of formic and acetic acids, Atmos. Chem. Phys., 11, 1989–2013, https://doi.org/10.5194/acp-11-1989-2011, 2011.
Pearson, R. G., Phillips, S. J., Loranty, M. M., Beck, P. S. A., Damoulas,
T., Knight, S. J., and Goetz, S. J.: Shifts in Arctic vegetation and
associated feedbacks under climate change, Nat. Clim. Change, 3, 673–677,
https://doi.org/10.1038/nclimate1858, 2013.
Permar, W., Wang, Q., Selimovic, V., Wielgasz, C., Yokelson, R. J.,
Hornbrook, R. S., Hills, A. J., Apel, E. C., Ku, I., Zhou, Y., Sive, B. C.,
Sullivan, A. P., Collett, J. L., Campos, T. L., Palm, B. B., Peng, Q.,
Thornton, J. A., Garofalo, L. A., Farmer, D. K., Kreidenweis, S. M., Levin,
E. J. T., DeMott, P. J., Flocke, F., Fischer, E. V., and Hu, L.: Emissions
of Trace Organic Gases From Western U.S. Wildfires Based on WE-CAN Aircraft
Measurements, J. Geophys. Res.-Atmos., 126, e2020JD033838,
https://doi.org/10.1029/2020JD033838, 2021.
Pernov, J. B., Bossi, R., Lebourgeois, T., Nøjgaard, J. K., Holzinger, R., Hjorth, J. L., and Skov, H.: Atmospheric VOC measurements at a High Arctic site: characteristics and source apportionment, Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, 2021.
Post, E., Alley, R. B., Christensen, T. R., Macias-Fauria, M., Forbes, B.
C., Gooseff, M. N., Iler, A., Kerby, J. T., Laidre, K. L., Mann, M. E.,
Olofsson, J., Stroeve, J. C., Ulmer, F., Virginia, R. A., and Wang, M.: The
polar regions in a 2 ∘C warmer world, Science Advances, 5, eaaw9883,
https://doi.org/10.1126/sciadv.aaw9883, 2019.
Potosnak, M. J., Baker, B. M., LeStourgeon, L., Disher, S. M., Griffin, K. L., Bret-Harte, M. S., and Starr, G.: Isoprene emissions from a tundra ecosystem, Biogeosciences, 10, 871–889, https://doi.org/10.5194/bg-10-871-2013, 2013.
Praplan, A. P., Tykkä, T., Chen, D., Boy, M., Taipale, D., Vakkari, V., Zhou, P., Petäjä, T., and Hellén, H.: Long-term total OH reactivity measurements in a boreal forest, Atmos. Chem. Phys., 19, 14431–14453, https://doi.org/10.5194/acp-19-14431-2019, 2019.
Rinnan, R., Rinnan, Å., Faubert, P., Tiiva, P., Holopainen, J. K., and
Michelsen, A.: Few long-term effects of simulated climate change on volatile
organic compound emissions and leaf chemistry of three subarctic dwarf
shrubs, Environ. Exp. Bot., 72, 377–386,
https://doi.org/10.1016/j.envexpbot.2010.11.006, 2011.
Rinnan, R., Steinke, M., Mcgenity, T., and Loreto, F.: Plant volatiles in
extreme terrestrial and marine environments, Plant Cell Environ., 37, 1776–1789,
https://doi.org/10.1111/pce.12320, 2014.
Safieddine, S. A., Heald, C. L., and Henderson, B. H.: The global nonmethane
reactive organic carbon budget: A modeling perspective, Geophys. Res. Lett., 44, 3897–3906, https://doi.org/10.1002/2017GL072602,
2017.
Schobesberger, S., Lopez-Hilfiker, F. D., Taipale, D., Millet, D. B.,
D'Ambro, E. L., Rantala, P., Mammarella, I., Zhou, P., Wolfe, G. M., Lee, B.
H., Boy, M., and Thornton, J. A.: High upward fluxes of formic acid from a
boreal forest canopy, Geophys. Res. Lett., 43, 9342–9351,
https://doi.org/10.1002/2016GL069599, 2016.
Seco, R., Holst, T., Matzen, M. S., Westergaard-Nielsen, A., Li, T., Simin, T., Jansen, J., Crill, P., Friborg, T., Rinne, J., and Rinnan, R.: Volatile organic compound fluxes in a subarctic peatland and lake, Atmos. Chem. Phys., 20, 13399–13416, https://doi.org/10.5194/acp-20-13399-2020, 2020.
Sekimoto, K., Li, S.-M., Yuan, B., Koss, A., Coggon, M., Warneke, C., and de
Gouw, J.: Calculation of the sensitivity of proton-transfer-reaction mass
spectrometry (PTR-MS) for organic trace gases using molecular properties,
Int. J. Mass Spectrom., 421, 71–94, https://doi.org/10.1016/j.ijms.2017.04.006, 2017.
Selimovic, V., Ketcherside, D., Chaliyakunnel, S., Wielgasz, C., Permar, W., Angot, H., Millet, D. B., Fried, A., Helmig, D., and Hu, L.: VOC Observations at Toolik Field Station (TFS), https://www.umt.edu/atmoschem/data.php, last access: 31 October 2022.
Sharkey, T. D., Wiberley, A. E., and Donohue, A. R.: Isoprene emission from
plants: why and how, Ann. Bot., 101, 5–18,
https://doi.org/10.1093/aob/mcm240, 2008.
Shaver, G. R. and Chapin, F. S.: Production: Biomass Relationships and
Element Cycling in Contrasting Arctic Vegetation Types, Ecol. Monogr., 61,
1–31, https://doi.org/10.2307/1942997, 1991.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Sinha, V., Williams, J., Lelieveld, J., Ruuskanen, T., Kajos, M., Patokoski,
J., Hellen, H., Hakola, H., Mogensen, D., Boy, M., Rinne, J., and Kulmala,
M.: OH Reactivity Measurements within a Boreal Forest: Evidence for Unknown
Reactive Emissions, Environ. Sci. Technol., 44, 6614–6620,
https://doi.org/10.1021/es101780b, 2010.
Stavrakou, T., Müller, J.-F., Peeters, J., Razavi, A., Clarisse, L.,
Clerbaux, C., Coheur, P.-F., Hurtmans, D., De Mazière, M., Vigouroux,
C., Deutscher, N. M., Griffith, D. W. T., Jones, N., and Paton-Walsh, C.:
Satellite evidence for a large source of formic acid from boreal and
tropical forests, Nat. Geosci., 5, 26–30,
https://doi.org/10.1038/ngeo1354, 2012.
Stroud, C. A., Roberts, J. M., Goldan, P. D., Kuster, W. C., Murphy, P. C.,
Williams, E. J., Hereid, D., Parrish, D., Sueper, D., Trainer, M.,
Fehsenfeld, F. C., Apel, E. C., Riemer, D., Wert, B., Henry, B., Fried, A.,
Martinez-Harder, M., Harder, H., Brune, W. H., Li, G., Xie, H., and Young,
V. L.: Isoprene and its oxidation products, methacrolein and methylvinyl
ketone, at an urban forested site during the 1999 Southern Oxidants Study,
J. Geophys. Res., 106, 8035–8046,
https://doi.org/10.1029/2000JD900628, 2001.
Survey: Maps – Toolik Lake Area Vegetation,
http://www.arcticatlas.org/maps/themes/tl5k/tl5kvg (last access:
2 January 2022), 2012.
Tang, J., Schurgers, G., Valolahti, H., Faubert, P., Tiiva, P., Michelsen, A., and Rinnan, R.: Challenges in modelling isoprene and monoterpene emission dynamics of Arctic plants: a case study from a subarctic tundra heath, Biogeosciences, 13, 6651–6667, https://doi.org/10.5194/bg-13-6651-2016, 2016.
Trentmann, J., Yokelson, R. J., Hobbs, P. V., Winterrath, T., Christian, T.
J., Andreae, M. O., and Mason, S. A.: An analysis of the chemical processes
in the smoke plume from a savanna fire, J. Geophys. Res., 110, D12301,
https://doi.org/10.1029/2004JD005628, 2005.
Walker, M. D., Walker, D. A., and Auerbach, N. A.: Plant communities of a
tussock tundra landscape in the Brooks Range Foothills, Alaska, J. Veg.
Sci., 5, 843–866, https://doi.org/10.2307/3236198, 1994.
Wang, S., Apel, E. C., Schwantes, R. H., Bates, K. H., Jacob, D. J.,
Fischer, E. V., Hornbrook, R. S., Hills, A. J., Emmons, L. K., Pan, L. L.,
Honomichl, S., Tilmes, S., Lamarque, J.-F., Yang, M., Marandino, C. A.,
Saltzman, E. S., de Bruyn, W., Kameyama, S., Tanimoto, H., Omori, Y., Hall,
S. R., Ullmann, K., Ryerson, T. B., Thompson, C. R., Peischl, J., Daube, B.
C., Commane, R., McKain, K., Sweeney, C., Thames, A. B., Miller, D. O.,
Brune, W. H., Diskin, G. S., DiGangi, J. P., and Wofsy, S. C.: Global
Atmospheric Budget of Acetone: Air-Sea Exchange and the Contribution to
Hydroxyl Radicals, J. Geophys.-Res.-Atmos., 125, e2020JD032553,
https://doi.org/10.1029/2020JD032553, 2020.
Wang, Y. X., McElroy, M. B., Jacob, D. J., and Yantosca, R. M.: A nested
grid formulation for chemical transport over Asia: Applications to CO, J.
Geophys. Res., 109, D22307, https://doi.org/10.1029/2004JD005237, 2004.
Warneke, C., de Gouw, J. A., Goldan, P. D., Kuster, W. C., Williams, E. J., Lerner, B. M., Jakoubek, R., Brown, S. S., Stark, H., Aldener, M., Ravishankara, A. R., Roberts, J. M., Marchewka, M., Bertman, S., Sueper, D. T., McKeen, S. A., Meagher, J. F., and Fehsenfeld, F. C.: Comparison of daytime and nighttime oxidation of biogenic and anthropogenic VOCs along the New England coast in summer during New England Air Quality Study 2002, J. Geophys. Res.-Atmos., 109, D10309, https://doi.org/10.1029/2003JD004424, 2004.
Wells, K. C., Millet, D. B., Payne, V. H., Deventer, M. J., Bates, K. H., de
Gouw, J. A., Graus, M., Warneke, C., Wisthaler, A., and Fuentes, J. D.:
Satellite isoprene retrievals constrain emissions and atmospheric oxidation,
Nature, 585, 225–233,
https://doi.org/10.1038/s41586-020-2664-3, 2020.
Yokelson, R. J., Bertschi, I. T., Christian, T. J., Hobbs, P. V., Ward, D.
E., and Hao, W. M.: Trace gas measurements in nascent, aged, and
cloud-processed smoke from African savanna fires by airborne Fourier
transform infrared spectroscopy (AFTIR), J. Geophys. Res., 108, 8478,
https://doi.org/10.1029/2002JD002322, 2003.
Zhao, T., Mao, J., Simpson, W. R., De Smedt, I., Zhu, L., Hanisco, T. F., Wolfe, G. M., St. Clair, J. M., González Abad, G., Nowlan, C. R., Barletta, B., Meinardi, S., Blake, D. R., Apel, E. C., and Hornbrook, R. S.: Source and variability of formaldehyde (HCHO) at northern high latitudes: an integrated satellite, aircraft, and model study, Atmos. Chem. Phys., 22, 7163–7178, https://doi.org/10.5194/acp-22-7163-2022, 2022.
Short summary
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.
Arctic warming has led to an increase in plants that emit gases in response to stress, but how...
Altmetrics
Final-revised paper
Preprint