Articles | Volume 20, issue 13
https://doi.org/10.5194/acp-20-7753-2020
© Author(s) 2020. 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-20-7753-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
03 Jul 2020
Research article |
| 03 Jul 2020
Constraining remote oxidation capacity with ATom observations
Katherine R. Travis
CORRESPONDING AUTHOR
Department of Civil and Environmental Engineering, Massachusetts
Institute of Technology, Cambridge, MA, USA
now at: NASA
Langley Research Center, Hampton, VA, USA
Department of Civil and Environmental Engineering, Massachusetts
Institute of Technology, Cambridge, MA, USA
Department of Earth,
Atmospheric and Planetary Sciences, Massachusetts Institute of Technology,
Cambridge, MA, USA
Hannah M. Allen
Division of Chemistry and Chemical Engineering,
California Institute of Technology, Pasadena, CA, USA
Eric C. Apel
Atmospheric
Chemistry Observations & Modeling Laboratory, National Center for
Atmospheric Research, Boulder, CO, USA
Stephen R. Arnold
Institute for
Climate and Atmospheric Science, School of Earth and Environment, University
of Leeds, Leeds, UK
Donald R. Blake
Department of Chemistry, University of
California Irvine, Irvine, CA, USA
William H. Brune
Department of Meteorology,
Pennsylvania State University, University Park, PA, USA
University
of Minnesota, Department of Soil, Water and Climate, St. Paul, MN, USA
Róisín Commane
Dept. of Earth & Environmental Sciences of Lamont-Doherty Earth
Observatory and Columbia University, Palisades, NY, USA
John D. Crounse
Division of Geological and Planetary Sciences, California
Institute of Technology, Pasadena, CA, USA
Bruce C. Daube
Harvard John A.
Paulson School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA, USA
Glenn S. Diskin
NASA Langley Research Center, Hampton, VA,
USA
James W. Elkins
Global Monitoring Division, NOAA Earth System Research
Laboratory, Boulder, CO, USA
Mathew J. Evans
Wolfson Atmospheric Chemistry
Laboratories (WACL), Department of Chemistry, University of York, York, UK
National Centre for Atmospheric Science (NCAS), University of
York, York, UK
Samuel R. Hall
Atmospheric
Chemistry Observations & Modeling Laboratory, National Center for
Atmospheric Research, Boulder, CO, USA
Eric J. Hintsa
Global Monitoring Division, NOAA Earth System Research
Laboratory, Boulder, CO, USA
Cooperative Institute for Research in
Environmental Science, University of Colorado, CO, USA
Rebecca S. Hornbrook
Atmospheric
Chemistry Observations & Modeling Laboratory, National Center for
Atmospheric Research, Boulder, CO, USA
Prasad S. Kasibhatla
Nicholas
School of the Environment, Duke University, Durham, NC, USA
Michelle J. Kim
Division of Geological and Planetary Sciences, California
Institute of Technology, Pasadena, CA, USA
Division of Engineering and Applied Science, California Institute
of Technology, Pasadena, CA, USA
Atmospheric Sciences Research
Center, University of Albany, Albany, NY, USA
Kathryn McKain
Global Monitoring Division, NOAA Earth System Research
Laboratory, Boulder, CO, USA
Cooperative Institute for Research in
Environmental Science, University of Colorado, CO, USA
Dylan B. Millet
University
of Minnesota, Department of Soil, Water and Climate, St. Paul, MN, USA
Fred L. Moore
Global Monitoring Division, NOAA Earth System Research
Laboratory, Boulder, CO, USA
Cooperative Institute for Research in
Environmental Science, University of Colorado, CO, USA
Jeffrey Peischl
Cooperative Institute for Research in
Environmental Science, University of Colorado, CO, USA
Chemical Sciences
Division, NOAA Earth System Research Laboratory, Boulder, CO, USA
Thomas B. Ryerson
Chemical Sciences
Division, NOAA Earth System Research Laboratory, Boulder, CO, USA
Tomás Sherwen
Wolfson Atmospheric Chemistry
Laboratories (WACL), Department of Chemistry, University of York, York, UK
National Centre for Atmospheric Science (NCAS), University of
York, York, UK
Alexander B. Thames
Department of Meteorology,
Pennsylvania State University, University Park, PA, USA
Kirk Ullmann
Atmospheric
Chemistry Observations & Modeling Laboratory, National Center for
Atmospheric Research, Boulder, CO, USA
Xuan Wang
Harvard John A.
Paulson School of Engineering and Applied Sciences, Harvard University,
Cambridge, MA, USA
School of Energy and Environment, City University of Hong Kong,
Hong Kong, China
Paul O. Wennberg
Division of Chemistry and Chemical Engineering,
California Institute of Technology, Pasadena, CA, USA
Division of Engineering and Applied Science, California Institute
of Technology, Pasadena, CA, USA
Glenn M. Wolfe
Atmospheric Chemistry and Dynamics Laboratory,
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Fangqun Yu
Atmospheric Sciences Research
Center, University of Albany, Albany, NY, USA
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P. Zoogman, D. J. Jacob, K. Chance, X. Liu, M. Lin, A. Fiore, and K. Travis
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J. Mao, S. Fan, D. J. Jacob, and K. R. Travis
Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, https://doi.org/10.5194/acp-13-509-2013, 2013
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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Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
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Qian Xiao, Jiaoshi Zhang, Yang Wang, Luke D. Ziemba, Ewan Crosbie, Edward L. Winstead, Claire E. Robinson, Joshua P. DiGangi, Glenn S. Diskin, Jeffrey S. Reid, K. Sebastian Schmidt, Armin Sorooshian, Miguel Ricardo A. Hilario, Sarah Woods, Paul Lawson, Snorre A. Stamnes, and Jian Wang
Atmos. Chem. Phys., 23, 9853–9871, https://doi.org/10.5194/acp-23-9853-2023, https://doi.org/10.5194/acp-23-9853-2023, 2023
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Kyoung-Min Kim, Si-Wan Kim, Seunghwan Seo, Donald R. Blake, Seogju Cho, James H. Crawford, Louisa Emmons, Alan Fried, Jay R. Herman, Jinkyu Hong, Jinsang Jung, Gabriele Pfister, Andrew J. Weinheimer, Jung-Hun Woo, and Qiang Zhang
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Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
EGUsphere, https://doi.org/10.5194/egusphere-2023-1824, https://doi.org/10.5194/egusphere-2023-1824, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the northern hemisphere, therefore mixing ratios in the southern hemisphere lag behind. Comparing the observations to results from a box model, the model predicts air in the southern hemisphere to be older. For a better agreement, the emissions used as model input need to be increased, their spatial pattern changed, and we need to modify north-south transport.
Joshua L. Laughner, Geoffrey C. Toon, Joseph Mendonca, Christof Petri, Sébastien Roche, Debra Wunch, Jean-Francois Blavier, David W. T. Griffith, Pauli Heikkinen, Ralph F. Keeling, Matthäus Kiel, Rigel Kivi, Coleen M. Roehl, Britton B. Stephens, Bianca C. Baier, Huilin Chen, Yonghoon Choi, Nicholas M. Deutscher, Joshua P. DiGangi, Jochen Gross, Benedikt Herkommer, Pascal Jeseck, Thomas Laemmel, Xin Lan, Erin McGee, Kathryn McKain, John Miller, Isamu Morino, Justus Notholt, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Haris Riris, Constantina Rousogenous, Mahesh Kumar Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Steven C. Wofsy, Minquiang Zhou, and Paul O. Wennberg
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-331, https://doi.org/10.5194/essd-2023-331, 2023
Preprint under review for ESSD
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This paper describes a new version, called GGG2020, of a dataset containing column-integrated observations of greenhouse and related gases (including CO2, CH4, CO, and N2O) made by ground stations located around the world. Compared to the previous version (GGG2014), improvements have been made towards site-to-site consistency. This dataset plays a key role in validating space-based greenhouse gas observations and in understanding the carbon cycle.
Adedayo R. Adedeji, Stephen J. Andrews, Matthew J. Rowlinson, Mathew J. Evans, Alastair C. Lewis, Shigeru Hashimoto, Hitoshi Mukai, Hiroshi Tanimoto, Yasunori Tohjima, and Takuya Saito
Atmos. Chem. Phys., 23, 9229–9244, https://doi.org/10.5194/acp-23-9229-2023, https://doi.org/10.5194/acp-23-9229-2023, 2023
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We use the GEOS-Chem model to interpret observations of CO, C2H6, C3H8, NOx, NOy and O3 made from Hateruma Island in 2018. The model captures many synoptic-scale events and the seasonality of most pollutants at the site but underestimates C2H6 and C3H8 during the winter. These underestimates are unlikely to be reconciled by increases in biomass burning emissions but could be reconciled by increasing the Asian anthropogenic source of C2H6 and C3H8 by factors of around 2 and 3, respectively.
Sarah M. Ludwig, Luke Schiferl, Jacqueline Hung, Susan M. Natali, and Roisin Commane
Biogeosciences Discuss., https://doi.org/10.5194/bg-2023-119, https://doi.org/10.5194/bg-2023-119, 2023
Preprint under review for BG
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Landscapes are often assumed to be homogeneous when using eddy covariance fluxes, which can lead to biases when calculating carbon budgets. In this study we report eddy covariance carbon fluxes from heterogeneous tundra. We used the footprints of each flux observation to un-mix the fluxes coming from components of the landscape. We identified and quantified hot spots of carbon emissions in the landscape. Accurately scaling with landscape heterogeneity yielded half as much regional carbon uptake.
Armin Sorooshian, Mikhail D. Alexandrov, Adam D. Bell, Ryan Bennett, Grace Betito, Sharon P. Burton, Megan E. Buzanowicz, Brian Cairns, Eduard V. Chemyakin, Gao Chen, Yonghoon Choi, Brian L. Collister, Anthony L. Cook, Andrea F. Corral, Ewan C. Crosbie, Bastiaan van Diedenhoven, Joshua P. DiGangi, Glenn S. Diskin, Sanja Dmitrovic, Eva-Lou Edwards, Marta A. Fenn, Richard A. Ferrare, David van Gilst, Johnathan W. Hair, David B. Harper, Miguel Ricardo A. Hilario, Chris A. Hostetler, Nathan Jester, Michael Jones, Simon Kirschler, Mary M. Kleb, John M. Kusterer, Sean Leavor, Joseph W. Lee, Hongyu Liu, Kayla McCauley, Richard H. Moore, Joseph Nied, Anthony Notari, John B. Nowak, David Painemal, Kasey E. Phillips, Claire E. Robinson, Amy Jo Scarino, Joseph S. Schlosser, Shane T. Seaman, Chellappan Seethala, Taylor J. Shingler, Michael A. Shook, Kenneth A. Sinclair, William L. Smith Jr., Douglas A. Spangenberg, Snorre A. Stamnes, Kenneth L. Thornhill, Christiane Voigt, Holger Vömel, Andrzej P. Wasilewski, Hailong Wang, Edward L. Winstead, Kira Zeider, Xubin Zeng, Bo Zhang, Luke D. Ziemba, and Paquita Zuidema
Earth Syst. Sci. Data, 15, 3419–3472, https://doi.org/10.5194/essd-15-3419-2023, https://doi.org/10.5194/essd-15-3419-2023, 2023
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The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol–cloud–meteorology interactions. HU-25 Falcon and King Air aircraft conducted systematic and spatially coordinated flights over the northwest Atlantic Ocean. This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Katherine Ball, 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 DiGangi, Glenn Diskin, Alan Fried, Jessica Gilman, Hongyu Guo, Johnathan W. Hair, Hannah A. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, 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, James A. 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 Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn Wolfe, Caroline Womack, Lu Xu, Robert Yokelson, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2023-1439, https://doi.org/10.5194/egusphere-2023-1439, 2023
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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.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
EGUsphere, https://doi.org/10.5194/egusphere-2023-1161, https://doi.org/10.5194/egusphere-2023-1161, 2023
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models are generally underpredicting the concentrations of these gases in the Arctic troposphere.
Thomas E. Taylor, Christopher W. O'Dell, David Baker, Carol Bruegge, Albert Chang, Lars Chapsky, Abhishek Chatterjee, Cecilia Cheng, Frédéric Chevallier, David Crisp, Lan Dang, Brian Drouin, Annmarie Eldering, Liang Feng, Brendan Fisher, Dejian Fu, Michael Gunson, Vance Haemmerle, Graziela R. Keller, Matthäus Kiel, Le Kuai, Thomas Kurosu, Alyn Lambert, Joshua Laughner, Richard Lee, Junjie Liu, Lucas Mandrake, Yuliya Marchetti, Gregory McGarragh, Aronne Merrelli, Robert R. Nelson, Greg Osterman, Fabiano Oyafuso, Paul I. Palmer, Vivienne H. Payne, Robert Rosenberg, Peter Somkuti, Gary Spiers, Cathy To, Brad Weir, Paul O. Wennberg, Shanshan Yu, and Jia Zong
Atmos. Meas. Tech., 16, 3173–3209, https://doi.org/10.5194/amt-16-3173-2023, https://doi.org/10.5194/amt-16-3173-2023, 2023
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NASA's Orbiting Carbon Observatory 2 and 3 (OCO-2 and OCO-3, respectively) provide complementary spatiotemporal coverage from a sun-synchronous and precession orbit, respectively. Estimates of total column carbon dioxide (XCO2) derived from the two sensors using the same retrieval algorithm show broad consistency over a 2.5-year overlapping time record. This suggests that data from the two satellites may be used together for scientific analysis.
Jianghanyang Li, Bianca C. Baier, Fred Moore, Tim Newberger, Sonja Wolter, Jack Higgs, Geoff Dutton, Eric Hintsa, Bradley Hall, and Colm Sweeney
Atmos. Meas. Tech., 16, 2851–2863, https://doi.org/10.5194/amt-16-2851-2023, https://doi.org/10.5194/amt-16-2851-2023, 2023
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Monitoring a suite of trace gases in the stratosphere will help us better understand the stratospheric circulation and its impact on the earth's radiation balance. However, such measurements are rare and usually expensive. We developed an instrument that can measure stratospheric trace gases using a low-cost sampling platform (AirCore). The results showed expected agreement with aircraft measurements, demonstrating this technique provides a low-cost and robust way to observe the stratosphere.
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
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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.
Harrison A. Parker, Joshua L. Laughner, Geoffrey C. Toon, Debra Wunch, Coleen M. Roehl, Laura T. Iraci, James R. Podolske, Kathryn McKain, Bianca C. Baier, and Paul O. Wennberg
Atmos. Meas. Tech., 16, 2601–2625, https://doi.org/10.5194/amt-16-2601-2023, https://doi.org/10.5194/amt-16-2601-2023, 2023
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We describe a retrieval algorithm for determining limited information about the vertical distribution of carbon monoxide (CO) and carbon dioxide (CO2) from total column observations from ground-based observations. Our retrieved partial column values compare well with integrated in situ data. The average error for our retrieval is 1.51 ppb (~ 2 %) for CO and 5.09 ppm (~ 1.25 %) for CO2. We anticipate that this approach will find broad application for use in carbon cycle science.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
EGUsphere, https://doi.org/10.5194/egusphere-2023-860, https://doi.org/10.5194/egusphere-2023-860, 2023
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We measured cyanogen bromide (BrCN) in the troposphere for the first time as part of a series of survey flights around the globe. BrCN is found to be a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments, and so is a previously unrecognized participant in this chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Miguel Ricardo A. Hilario, Avelino F. Arellano, Ali Behrangi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Michael A. Shook, Luke D. Ziemba, and Armin Sorooshian
EGUsphere, https://doi.org/10.5194/egusphere-2023-726, https://doi.org/10.5194/egusphere-2023-726, 2023
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Wet scavenging strongly influences aerosol lifetime and interactions but is a large uncertainty in global models. We present a flexible and repeatable method to identify meteorological variables relevant for estimating wet scavenging. For the tropical West Pacific, we show frequencies of precipitation or high humidity are better scavenging indicators than accumulated precipitation. This method applicable to different regions and may be used to inform scavenging parametrization schemes in models.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-50, https://doi.org/10.5194/gmd-2023-50, 2023
Revised manuscript accepted for GMD
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations, and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model-satellite discrepancies, we find that future field campaigns in an East African region (30° E – 45° E, 5° S – 5° N) could substantially improve the predictive skill of air quality models.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
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Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
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From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
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.
Róisín Commane, Andrew Hallward-Driemeier, and Lee T. Murray
Atmos. Meas. Tech., 16, 1431–1441, https://doi.org/10.5194/amt-16-1431-2023, https://doi.org/10.5194/amt-16-1431-2023, 2023
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Methane / ethane ratios can be used to identify and partition the different sources of methane, especially in areas with natural gas mixed with biogenic methane emissions, such as cities. We tested three commercially available laser-based analyzers for sensitivity, precision, size, power requirement, ease of use on mobile platforms, and expertise needed to operate the instrument, and we make recommendations for use in various situations.
Joshua L. Laughner, Sébastien Roche, Matthäus Kiel, Geoffrey C. Toon, Debra Wunch, Bianca C. Baier, Sébastien Biraud, Huilin Chen, Rigel Kivi, Thomas Laemmel, Kathryn McKain, Pierre-Yves Quéhé, Constantina Rousogenous, Britton B. Stephens, Kaley Walker, and Paul O. Wennberg
Atmos. Meas. Tech., 16, 1121–1146, https://doi.org/10.5194/amt-16-1121-2023, https://doi.org/10.5194/amt-16-1121-2023, 2023
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Observations using sunlight to measure surface-to-space total column of greenhouse gases in the atmosphere need an initial guess of the vertical distribution of those gases to start from. We have developed an approach to provide those initial guess profiles that uses readily available meteorological data as input. This lets us make these guesses without simulating them with a global model. The profiles generated this way match independent observations well.
Laura Hyesung Yang, Daniel J. Jacob, Nadia K. Colombi, Shixian Zhai, Kelvin H. Bates, Viral Shah, Ellie Beaudry, Robert M. Yantosca, Haipeng Lin, Jared F. Brewer, Heesung Chong, Katherine R. Travis, James H. Crawford, Lok N. Lamsal, Ja-Ho Koo, and Jhoon Kim
Atmos. Chem. Phys., 23, 2465–2481, https://doi.org/10.5194/acp-23-2465-2023, https://doi.org/10.5194/acp-23-2465-2023, 2023
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A geostationary satellite can now provide hourly NO2 vertical columns, and obtaining the NO2 vertical columns from space relies on NO2 vertical distribution from the chemical transport model (CTM). In this work, we update the CTM to better represent the chemistry environment so that the CTM can accurately provide NO2 vertical distribution. We also find that the changes in NO2 vertical distribution driven by a change in mixing depth play an important role in the NO2 column's diurnal variation.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
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
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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.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys., 23, 1863–1877, https://doi.org/10.5194/acp-23-1863-2023, https://doi.org/10.5194/acp-23-1863-2023, 2023
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies overpredicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-827, https://doi.org/10.5194/acp-2022-827, 2023
Revised manuscript accepted for ACP
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Luke D. Schiferl, Jennifer D. Watts, Erik J. L. Larson, Kyle A. Arndt, Sébastien C. Biraud, Eugénie S. Euskirchen, Jordan P. Goodrich, John M. Henderson, Aram Kalhori, Kathryn McKain, Marikate E. Mountain, J. William Munger, Walter C. Oechel, Colm Sweeney, Yonghong Yi, Donatella Zona, and Róisín Commane
Biogeosciences, 19, 5953–5972, https://doi.org/10.5194/bg-19-5953-2022, https://doi.org/10.5194/bg-19-5953-2022, 2022
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As the Arctic rapidly warms, vast stores of thawing permafrost could release carbon dioxide (CO2) into the atmosphere. We combined observations of atmospheric CO2 concentrations from aircraft and a tower with observed CO2 fluxes from tundra ecosystems and found that the Alaskan North Slope in not a consistent source nor sink of CO2. Our study shows the importance of using both site-level and atmospheric measurements to constrain regional net CO2 fluxes and improve biogenic processes in models.
Noah S. Hirshorn, Lauren M. Zuromski, Christopher Rapp, Ian McCubbin, Gerardo Carrillo-Cardenas, Fangqun Yu, and A. Gannet Hallar
Atmos. Chem. Phys., 22, 15909–15924, https://doi.org/10.5194/acp-22-15909-2022, https://doi.org/10.5194/acp-22-15909-2022, 2022
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New particle formation (NPF) is a source of atmospheric aerosol number concentration that can impact climate by growing to larger sizes and under proper conditions form cloud condensation nuclei (CCN). Using novel methods, we find that at Storm Peak Laboratory, a remote, mountaintop site in Colorado, NPF is observed to enhance CCN concentrations in the spring by a factor of 1.54 and in the winter by a factor of 1.36 which can occur on a regional scale having important climate implications.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Dien Wu, Junjie Liu, Paul O. Wennberg, Paul I. Palmer, Robert R. Nelson, Matthäus Kiel, and Annmarie Eldering
Atmos. Chem. Phys., 22, 14547–14570, https://doi.org/10.5194/acp-22-14547-2022, https://doi.org/10.5194/acp-22-14547-2022, 2022
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Prior studies have derived the combustion efficiency for a region/city using observed CO2 and CO. We further zoomed into the urban domain and accounted for factors affecting the calculation of spatially resolved combustion efficiency from two satellites. The intra-city variability in combustion efficiency was linked to heavy industry within Shanghai and LA without relying on emission inventories. Such an approach can be applied when analyzing data from future geostationary satellites.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Peeyush Khare, Jordan E. Krechmer, Jo E. Machesky, Tori Hass-Mitchell, Cong Cao, Junqi Wang, Francesca Majluf, Felipe Lopez-Hilfiker, Sonja Malek, Will Wang, Karl Seltzer, Havala O. T. Pye, Roisin Commane, Brian C. McDonald, Ricardo Toledo-Crow, John E. Mak, and Drew R. Gentner
Atmos. Chem. Phys., 22, 14377–14399, https://doi.org/10.5194/acp-22-14377-2022, https://doi.org/10.5194/acp-22-14377-2022, 2022
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Ammonium adduct chemical ionization is used to examine the atmospheric abundances of oxygenated volatile organic compounds associated with emissions from volatile chemical products, which are now key contributors of reactive precursors to ozone and secondary organic aerosols in urban areas. The application of this valuable measurement approach in densely populated New York City enables the evaluation of emissions inventories and thus the role these oxygenated compounds play in urban air quality.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
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.
Xiao He, Xuan Zheng, Shaojun Zhang, Xuan Wang, Ting Chen, Xiao Zhang, Guanghan Huang, Yihuan Cao, Liqiang He, Xubing Cao, Yuan Cheng, Shuxiao Wang, and Ye Wu
Atmos. Chem. Phys., 22, 13935–13947, https://doi.org/10.5194/acp-22-13935-2022, https://doi.org/10.5194/acp-22-13935-2022, 2022
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With the use of two-dimensional gas chromatography time-of-flight mass spectrometry (GC × GC ToF-MS), we successfully give a comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emitted from heavy-duty diesel vehicles. I/SVOCs are speciated, identified, and quantified based on the patterns of the mass spectrum, and the gas–particle partitioning is fully addressed.
Ewan Crosbie, Luke D. Ziemba, Michael A. Shook, Claire E. Robinson, Edward L. Winstead, K. Lee Thornhill, Rachel A. Braun, Alexander B. MacDonald, Connor Stahl, Armin Sorooshian, Susan C. van den Heever, Joshua P. DiGangi, Glenn S. Diskin, Sarah Woods, Paola Bañaga, Matthew D. Brown, Francesca Gallo, Miguel Ricardo A. Hilario, Carolyn E. Jordan, Gabrielle R. Leung, Richard H. Moore, Kevin J. Sanchez, Taylor J. Shingler, and Elizabeth B. Wiggins
Atmos. Chem. Phys., 22, 13269–13302, https://doi.org/10.5194/acp-22-13269-2022, https://doi.org/10.5194/acp-22-13269-2022, 2022
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The linkage between cloud droplet and aerosol particle chemical composition was analyzed using samples collected in a polluted tropical marine environment. Variations in the droplet composition were related to physical and dynamical processes in clouds to assess their relative significance across three cases that spanned a range of rainfall amounts. In spite of the pollution, sea salt still remained a major contributor to the droplet composition and was preferentially enhanced in rainwater.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Helen M. Worden, Gene L. Francis, Susan S. Kulawik, Kevin W. Bowman, Karen Cady-Pereira, Dejian Fu, Jennifer D. Hegarty, Valentin Kantchev, Ming Luo, Vivienne H. Payne, John R. Worden, Róisín Commane, and Kathryn McKain
Atmos. Meas. Tech., 15, 5383–5398, https://doi.org/10.5194/amt-15-5383-2022, https://doi.org/10.5194/amt-15-5383-2022, 2022
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Satellite observations of global carbon monoxide (CO) are essential for understanding atmospheric chemistry and pollution sources. This paper describes a new data product using radiance measurements from the Cross-track Infrared Sounder (CrIS) instrument on the Suomi National Polar-orbiting Partnership (SNPP) satellite that provides vertical profiles of CO from single-field-of-view observations. We show how these satellite CO profiles compare to aircraft observations and evaluate their biases.
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.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
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
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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
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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.
Sara Martínez-Alonso, Merritt N. Deeter, Bianca C. Baier, Kathryn McKain, Helen Worden, Tobias Borsdorff, Colm Sweeney, and Ilse Aben
Atmos. Meas. Tech., 15, 4751–4765, https://doi.org/10.5194/amt-15-4751-2022, https://doi.org/10.5194/amt-15-4751-2022, 2022
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AirCore is a novel balloon sampling system that can measure, among others, vertical profiles of carbon monoxide (CO) from 25–30 km of altitude to near the surface. Our analyses of AirCore and satellite CO data show that AirCore profiles are suited for satellite data validation, the use of shorter aircraft vertical profiles in satellite validation results in small errors (1–3 percent points) mostly at 300 hPa and above, and the error introduced by clouds in TROPOMI land data is small (1–2 %).
Robert J. Yokelson, Bambang H. Saharjo, Chelsea E. Stockwell, Erianto I. Putra, Thilina Jayarathne, Acep Akbar, Israr Albar, Donald R. Blake, Laura L. B. Graham, Agus Kurniawan, Simone Meinardi, Diah Ningrum, Ati D. Nurhayati, Asmadi Saad, Niken Sakuntaladewi, Eko Setianto, Isobel J. Simpson, Elizabeth A. Stone, Sigit Sutikno, Andri Thomas, Kevin C. Ryan, and Mark A. Cochrane
Atmos. Chem. Phys., 22, 10173–10194, https://doi.org/10.5194/acp-22-10173-2022, https://doi.org/10.5194/acp-22-10173-2022, 2022
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Fire plus non-fire GHG emissions associated with draining peatlands are the largest per area of any land use change considered by the IPCC. To characterize average and variability for tropical peat fire emissions, highly mobile smoke sampling teams were deployed across four Indonesian provinces to explore an extended interannual, climatic, and spatial range. Large adjustments to IPCC-recommended emissions are suggested. Lab data bolster an extensive emissions database for tropical peat fires.
Matthias Schneider, Benjamin Ertl, Qiansi Tu, Christopher J. Diekmann, Farahnaz Khosrawi, Amelie N. Röhling, Frank Hase, Darko Dubravica, Omaira E. García, Eliezer Sepúlveda, Tobias Borsdorff, Jochen Landgraf, Alba Lorente, André Butz, Huilin Chen, Rigel Kivi, Thomas Laemmel, Michel Ramonet, Cyril Crevoisier, Jérome Pernin, Martin Steinbacher, Frank Meinhardt, Kimberly Strong, Debra Wunch, Thorsten Warneke, Coleen Roehl, Paul O. Wennberg, Isamu Morino, Laura T. Iraci, Kei Shiomi, Nicholas M. Deutscher, David W. T. Griffith, Voltaire A. Velazco, and David F. Pollard
Atmos. Meas. Tech., 15, 4339–4371, https://doi.org/10.5194/amt-15-4339-2022, https://doi.org/10.5194/amt-15-4339-2022, 2022
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We present a computationally very efficient method for the synergetic use of level 2 remote-sensing data products. We apply the method to IASI vertical profile and TROPOMI total column space-borne methane observations and thus gain sensitivity for the tropospheric methane partial columns, which is not achievable by the individual use of TROPOMI and IASI. These synergetic effects are evaluated theoretically and empirically by inter-comparisons to independent references of TCCON, AirCore, and GAW.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Vivienne H. Payne, Susan S. Kulawik, Emily V. Fischer, Jared F. Brewer, L. Gregory Huey, Kazuyuki Miyazaki, John R. Worden, Kevin W. Bowman, Eric J. Hintsa, Fred Moore, James W. Elkins, and Julieta Juncosa Calahorrano
Atmos. Meas. Tech., 15, 3497–3511, https://doi.org/10.5194/amt-15-3497-2022, https://doi.org/10.5194/amt-15-3497-2022, 2022
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We compare new satellite measurements of peroxyacetyl nitrate (PAN) with reference aircraft measurements from two different instruments flown on the same platform. While there is a systematic difference between the two aircraft datasets, both show the same large-scale distribution of PAN and the discrepancy between aircraft datasets is small compared to the satellite uncertainties. The satellite measurements show skill in capturing large-scale variations in PAN.
Joseph S. Schlosser, Connor Stahl, Armin Sorooshian, Yen Thi-Hoang Le, Ki-Joon Jeon, Peng Xian, Carolyn E. Jordan, Katherine R. Travis, James H. Crawford, Sung Yong Gong, Hye-Jung Shin, In-Ho Song, and Jong-sang Youn
Atmos. Chem. Phys., 22, 7505–7522, https://doi.org/10.5194/acp-22-7505-2022, https://doi.org/10.5194/acp-22-7505-2022, 2022
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During a major haze pollution episode in March 2019, anthropogenic emissions were dominant in the boundary layer over Incheon and Seoul, South Korea. Using supermicrometer and submicrometer size- and chemistry-resolved aerosol particle measurements taken during this haze pollution period, this work shows that local emissions and a shallow boundary layer, enhanced humidity, and low temperature promoted local heterogeneous formation of secondary inorganic and organic aerosol species.
Tianlang Zhao, Jingqiu Mao, William R. Simpson, Isabelle De Smedt, Lei Zhu, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Gonzalo González Abad, Caroline R. Nowlan, Barbara Barletta, Simone Meinardi, Donald R. Blake, Eric C. Apel, and Rebecca S. Hornbrook
Atmos. Chem. Phys., 22, 7163–7178, https://doi.org/10.5194/acp-22-7163-2022, https://doi.org/10.5194/acp-22-7163-2022, 2022
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Monitoring formaldehyde (HCHO) can help us understand Arctic vegetation change. Here, we compare satellite data and model and show that Alaska summertime HCHO is largely dominated by a background from methane oxidation during mild wildfire years and is dominated by wildfire (largely from direct emission of fire) during strong fire years. Consequently, it is challenging to use satellite HCHO to study vegetation change in the Arctic region.
Colm Sweeney, Abhishek Chatterjee, Sonja Wolter, Kathryn McKain, Robert Bogue, Stephen Conley, Tim Newberger, Lei Hu, Lesley Ott, Benjamin Poulter, Luke Schiferl, Brad Weir, Zhen Zhang, and Charles E. Miller
Atmos. Chem. Phys., 22, 6347–6364, https://doi.org/10.5194/acp-22-6347-2022, https://doi.org/10.5194/acp-22-6347-2022, 2022
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The Arctic Carbon Atmospheric Profiles (Arctic-CAP) project demonstrates the utility of aircraft profiles for independent evaluation of model-derived emissions and uptake of atmospheric CO2, CH4, and CO from land and ocean. Comparison with the Goddard Earth Observing System (GEOS) modeling system suggests that fluxes of CO2 are very consistent with observations, while those of CH4 have some regional and seasonal biases, and that CO comparison is complicated by transport errors.
Sparkle L. Malone, Youmi Oh, Kyle A. Arndt, George Burba, Roisin Commane, Alexandra R. Contosta, Jordan P. Goodrich, Henry W. Loescher, Gregory Starr, and Ruth K. Varner
Biogeosciences, 19, 2507–2522, https://doi.org/10.5194/bg-19-2507-2022, https://doi.org/10.5194/bg-19-2507-2022, 2022
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To understand the CH4 flux potential of natural ecosystems and agricultural lands in the United States of America, a multi-scale CH4 observation network focused on CH4 flux rates, processes, and scaling methods is required. This can be achieved with a network of ground-based observations that are distributed based on climatic regions and land cover.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Merritt Deeter, Gene Francis, John Gille, Debbie Mao, Sara Martínez-Alonso, Helen Worden, Dan Ziskin, James Drummond, Róisín Commane, Glenn Diskin, and Kathryn McKain
Atmos. Meas. Tech., 15, 2325–2344, https://doi.org/10.5194/amt-15-2325-2022, https://doi.org/10.5194/amt-15-2325-2022, 2022
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The MOPITT (Measurements of Pollution in the Troposphere) satellite instrument uses remote sensing to obtain retrievals (measurements) of carbon monoxide (CO) in the atmosphere. This paper describes the latest MOPITT data product, Version 9. Globally, the number of daytime MOPITT retrievals over land has increased by 30 %–40 % compared to the previous product. The reported improvements in the MOPITT product should benefit a wide variety of applications including studies of pollution sources.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
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
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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.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Maria Tzortziou, Charlotte F. Kwong, Daniel Goldberg, Luke Schiferl, Róisín Commane, Nader Abuhassan, James J. Szykman, and Lukas C. Valin
Atmos. Chem. Phys., 22, 2399–2417, https://doi.org/10.5194/acp-22-2399-2022, https://doi.org/10.5194/acp-22-2399-2022, 2022
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The COVID-19 pandemic created an extreme natural experiment in which sudden changes in human behavior significantly impacted urban air quality. Using a combination of model, satellite, and ground-based data, we examine the impact of multiple waves and phases of the pandemic on atmospheric nitrogen pollution in the New York metropolitan area, and address the role of weather as a key driver of high pollution episodes observed even during – and despite – the stringent early lockdowns.
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.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Andrew O. Langford, Christoph J. Senff, Raul J. Alvarez II, Ken C. Aikin, Sunil Baidar, Timothy A. Bonin, W. Alan Brewer, Jerome Brioude, Steven S. Brown, Joel D. Burley, Dani J. Caputi, Stephen A. Conley, Patrick D. Cullis, Zachary C. J. Decker, Stéphanie Evan, Guillaume Kirgis, Meiyun Lin, Mariusz Pagowski, Jeff Peischl, Irina Petropavlovskikh, R. Bradley Pierce, Thomas B. Ryerson, Scott P. Sandberg, Chance W. Sterling, Ann M. Weickmann, and Li Zhang
Atmos. Chem. Phys., 22, 1707–1737, https://doi.org/10.5194/acp-22-1707-2022, https://doi.org/10.5194/acp-22-1707-2022, 2022
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The Fires, Asian, and Stratospheric Transport–Las Vegas Ozone Study (FAST-LVOS) combined lidar, aircraft, and in situ measurements with global models to investigate the contributions of stratospheric intrusions, regional and Asian pollution, and wildfires to background ozone in the southwestern US during May and June 2017 and demonstrated that these processes contributed to background ozone levels that exceeded 70 % of the US National Ambient Air Quality Standard during the 6-week campaign.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Thomas E. Taylor, Christopher W. O'Dell, David Crisp, Akhiko Kuze, Hannakaisa Lindqvist, Paul O. Wennberg, Abhishek Chatterjee, Michael Gunson, Annmarie Eldering, Brendan Fisher, Matthäus Kiel, Robert R. Nelson, Aronne Merrelli, Greg Osterman, Frédéric Chevallier, Paul I. Palmer, Liang Feng, Nicholas M. Deutscher, Manvendra K. Dubey, Dietrich G. Feist, Omaira E. García, David W. T. Griffith, Frank Hase, Laura T. Iraci, Rigel Kivi, Cheng Liu, Martine De Mazière, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Matthias Schneider, Coleen M. Roehl, Mahesh Kumar Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, and Debra Wunch
Earth Syst. Sci. Data, 14, 325–360, https://doi.org/10.5194/essd-14-325-2022, https://doi.org/10.5194/essd-14-325-2022, 2022
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We provide an analysis of an 11-year record of atmospheric carbon dioxide (CO2) concentrations derived using an optimal estimation retrieval algorithm on measurements made by the GOSAT satellite. The new product (version 9) shows improvement over the previous version (v7.3) as evaluated against independent estimates of CO2 from ground-based sensors and atmospheric inversion systems. We also compare the new GOSAT CO2 values to collocated estimates from NASA's Orbiting Carbon Observatory-2.
Anna-Maria Virkkala, Susan M. Natali, Brendan M. Rogers, Jennifer D. Watts, Kathleen Savage, Sara June Connon, Marguerite Mauritz, Edward A. G. Schuur, Darcy Peter, Christina Minions, Julia Nojeim, Roisin Commane, Craig A. Emmerton, Mathias Goeckede, Manuel Helbig, David Holl, Hiroki Iwata, Hideki Kobayashi, Pasi Kolari, Efrén López-Blanco, Maija E. Marushchak, Mikhail Mastepanov, Lutz Merbold, Frans-Jan W. Parmentier, Matthias Peichl, Torsten Sachs, Oliver Sonnentag, Masahito Ueyama, Carolina Voigt, Mika Aurela, Julia Boike, Gerardo Celis, Namyi Chae, Torben R. Christensen, M. Syndonia Bret-Harte, Sigrid Dengel, Han Dolman, Colin W. Edgar, Bo Elberling, Eugenie Euskirchen, Achim Grelle, Juha Hatakka, Elyn Humphreys, Järvi Järveoja, Ayumi Kotani, Lars Kutzbach, Tuomas Laurila, Annalea Lohila, Ivan Mammarella, Yojiro Matsuura, Gesa Meyer, Mats B. Nilsson, Steven F. Oberbauer, Sang-Jong Park, Roman Petrov, Anatoly S. Prokushkin, Christopher Schulze, Vincent L. St. Louis, Eeva-Stiina Tuittila, Juha-Pekka Tuovinen, William Quinton, Andrej Varlagin, Donatella Zona, and Viacheslav I. Zyryanov
Earth Syst. Sci. Data, 14, 179–208, https://doi.org/10.5194/essd-14-179-2022, https://doi.org/10.5194/essd-14-179-2022, 2022
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The effects of climate warming on carbon cycling across the Arctic–boreal zone (ABZ) remain poorly understood due to the relatively limited distribution of ABZ flux sites. Fortunately, this flux network is constantly increasing, but new measurements are published in various platforms, making it challenging to understand the ABZ carbon cycle as a whole. Here, we compiled a new database of Arctic–boreal CO2 fluxes to help facilitate large-scale assessments of the ABZ carbon cycle.
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
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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.
Jennifer D. Hegarty, Karen E. Cady-Pereira, Vivienne H. Payne, Susan S. Kulawik, John R. Worden, Valentin Kantchev, Helen M. Worden, Kathryn McKain, Jasna V. Pittman, Róisín Commane, Bruce C. Daube Jr., and Eric A. Kort
Atmos. Meas. Tech., 15, 205–223, https://doi.org/10.5194/amt-15-205-2022, https://doi.org/10.5194/amt-15-205-2022, 2022
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Carbon monoxide (CO) is produced by combustion of substances such as fossil fuels and plays an important role in atmospheric pollution and climate. We evaluated estimates of atmospheric CO derived from outgoing radiation measurements of the Atmospheric Infrared Sounder (AIRS) on a satellite orbiting the Earth against CO measurements from aircraft to show that these satellite measurements are reliable for continuous global monitoring of atmospheric CO concentrations.
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.
Linda M. J. Kooijmans, Ara Cho, Jin Ma, Aleya Kaushik, Katherine D. Haynes, Ian Baker, Ingrid T. Luijkx, Mathijs Groenink, Wouter Peters, John B. Miller, Joseph A. Berry, Jerome Ogée, Laura K. Meredith, Wu Sun, Kukka-Maaria Kohonen, Timo Vesala, Ivan Mammarella, Huilin Chen, Felix M. Spielmann, Georg Wohlfahrt, Max Berkelhammer, Mary E. Whelan, Kadmiel Maseyk, Ulli Seibt, Roisin Commane, Richard Wehr, and Maarten Krol
Biogeosciences, 18, 6547–6565, https://doi.org/10.5194/bg-18-6547-2021, https://doi.org/10.5194/bg-18-6547-2021, 2021
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The gas carbonyl sulfide (COS) can be used to estimate photosynthesis. To adopt this approach on regional and global scales, we need biosphere models that can simulate COS exchange. So far, such models have not been evaluated against observations. We evaluate the COS biosphere exchange of the SiB4 model against COS flux observations. We find that the model is capable of simulating key processes in COS biosphere exchange. Still, we give recommendations for further improvement of the model.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
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
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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.
Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Simple aromatic compounds (benzene, toluene, xylene) have complex gas-phase chemistry that is inconsistently represented in atmospheric models. We compile recent experimental and theoretical insights to develop a new mechanism for gas-phase aromatic oxidation that is sufficiently compact for use in multiscale models. We compare our new mechanism to chamber experiments and other mechanisms, and implement it in a global model to quantify the impacts of aromatic oxidation on tropospheric chemistry.
Ira Leifer, Christopher Melton, and Donald R. Blake
Atmos. Chem. Phys., 21, 17607–17629, https://doi.org/10.5194/acp-21-17607-2021, https://doi.org/10.5194/acp-21-17607-2021, 2021
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We demonstrate a novel application using air quality station data to derive 3-decade-averaged emissions from the Coal Oil Point (COP) seep field, a highly spatially and temporally variable geological migration system. Emissions were 19 Gg per year, suggesting that the COP seep field contributes 0.27 % of the global marine seep budget based on a recent estimate. This provides an advance over snapshot survey values by accounting for seasonal and interannual variations.
Yanda Zhang, Fangqun Yu, Gan Luo, Jiwen Fan, and Shuai Liu
Atmos. Chem. Phys., 21, 17433–17451, https://doi.org/10.5194/acp-21-17433-2021, https://doi.org/10.5194/acp-21-17433-2021, 2021
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This paper explores the impacts of dust on summertime convective cloud and precipitation through a numerical experiment. The result indicates that the long-range-transported dust can notably affect the properties of convective cloud and precipitation by enhancing immersion freezing and invigorating convection. We also analyze the different dust effects predicted by the Morrison and SBM schemes, which are partially attributed to the saturation adjustment approach utilized in the bulk schemes.
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
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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.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
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.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Bharat Rastogi, John B. Miller, Micheal Trudeau, Arlyn E. Andrews, Lei Hu, Marikate Mountain, Thomas Nehrkorn, Bianca Baier, Kathryn McKain, John Mund, Kaiyu Guan, and Caroline B. Alden
Atmos. Chem. Phys., 21, 14385–14401, https://doi.org/10.5194/acp-21-14385-2021, https://doi.org/10.5194/acp-21-14385-2021, 2021
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Predicting Earth's climate is difficult, partly due to uncertainty in forecasting how much CO2 can be removed by oceans and plants, because we cannot measure these exchanges directly on large scales. Satellites such as NASA's OCO-2 can provide part of the needed information, but data need to be highly precise and accurate. We evaluate these data and find small biases in certain months that are similar to the signals of interest. We argue that continued improvement of these data is necessary.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Jessica L. McCarty, Juha Aalto, Ville-Veikko Paunu, Steve R. Arnold, Sabine Eckhardt, Zbigniew Klimont, Justin J. Fain, Nikolaos Evangeliou, Ari Venäläinen, Nadezhda M. Tchebakova, Elena I. Parfenova, Kaarle Kupiainen, Amber J. Soja, Lin Huang, and Simon Wilson
Biogeosciences, 18, 5053–5083, https://doi.org/10.5194/bg-18-5053-2021, https://doi.org/10.5194/bg-18-5053-2021, 2021
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Fires, including extreme fire seasons, and fire emissions are more common in the Arctic. A review and synthesis of current scientific literature find climate change and human activity in the north are fuelling an emerging Arctic fire regime, causing more black carbon and methane emissions within the Arctic. Uncertainties persist in characterizing future fire landscapes, and thus emissions, as well as policy-relevant challenges in understanding, monitoring, and managing Arctic fire regimes.
Gongda Lu, Eloise A. Marais, Tuan V. Vu, Jingsha Xu, Zongbo Shi, James D. Lee, Qiang Zhang, Lu Shen, Gan Luo, and Fangqun Yu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-428, https://doi.org/10.5194/acp-2021-428, 2021
Revised manuscript not accepted
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Emission controls were imposed in Beijing-Tianjin-Hebei in northern China in autumn-winter 2017. We find that regional PM2.5 targets (15 % decrease relative to previous year) were exceeded. Our analysis shows that decline in precursor emissions only leads to less than half (43 %) the improved air quality. Most of the change (57 %) is due to interannual variability in meteorology. Stricter emission controls may be necessary in years with unfavourable meteorology.
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
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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.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Xueshun Chen, Fangqun Yu, Wenyi Yang, Yele Sun, Huansheng Chen, Wei Du, Jian Zhao, Ying Wei, Lianfang Wei, Huiyun Du, Zhe Wang, Qizhong Wu, Jie Li, Junling An, and Zifa Wang
Atmos. Chem. Phys., 21, 9343–9366, https://doi.org/10.5194/acp-21-9343-2021, https://doi.org/10.5194/acp-21-9343-2021, 2021
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Atmospheric aerosol particles have significant climate and health effects that depend on aerosol size, composition, and mixing state. A new global-regional nested aerosol model with an advanced particle microphysics module and a volatility basis set organic aerosol module was developed to simulate aerosol microphysical processes. Simulations strongly suggest the important role of anthropogenic organic species in particle formation over the areas influenced by anthropogenic sources.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Elizabeth B. Wiggins, Arlyn Andrews, Colm Sweeney, John B. Miller, Charles E. Miller, Sander Veraverbeke, Roisin Commane, Steven Wofsy, John M. Henderson, and James T. Randerson
Atmos. Chem. Phys., 21, 8557–8574, https://doi.org/10.5194/acp-21-8557-2021, https://doi.org/10.5194/acp-21-8557-2021, 2021
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We analyzed high-resolution trace gas measurements collected from a tower in Alaska during a very active fire season to improve our understanding of trace gas emissions from boreal forest fires. Our results suggest previous studies may have underestimated emissions from smoldering combustion in boreal forest fires.
Fabienne Maignan, Camille Abadie, Marine Remaud, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Róisín Commane, Richard Wehr, J. Elliott Campbell, Sauveur Belviso, Stephen A. Montzka, Nina Raoult, Ulli Seibt, Yoichi P. Shiga, Nicolas Vuichard, Mary E. Whelan, and Philippe Peylin
Biogeosciences, 18, 2917–2955, https://doi.org/10.5194/bg-18-2917-2021, https://doi.org/10.5194/bg-18-2917-2021, 2021
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The assimilation of carbonyl sulfide (COS) by continental vegetation has been proposed as a proxy for gross primary production (GPP). Using a land surface and a transport model, we compare a mechanistic representation of the plant COS uptake (Berry et al., 2013) to the classical leaf relative uptake (LRU) approach linking GPP and vegetation COS fluxes. We show that at high temporal resolutions a mechanistic approach is mandatory, but at large scales the LRU approach compares similarly.
Xiaojing Shen, Junying Sun, Fangqun Yu, Ying Wang, Junting Zhong, Yangmei Zhang, Xinyao Hu, Can Xia, Sinan Zhang, and Xiaoye Zhang
Atmos. Chem. Phys., 21, 7039–7052, https://doi.org/10.5194/acp-21-7039-2021, https://doi.org/10.5194/acp-21-7039-2021, 2021
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In this work, we revealed the changes of PNSD and NPF events during the COVID-19 lockdown period in Beijing, China, to illustrate the impact of reduced primary emission and elavated atmospheric oxidized capicity on the nucleation and growth processes. The subsequent growth of nucleated particles and their contribution to the aerosol pollution formation were also explored, to highlight the necessity of controlling the nanoparticles in the future air quality management.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Dianne Sanchez, Roger Seco, Dasa Gu, Alex Guenther, John Mak, Youngjae Lee, Danbi Kim, Joonyoung Ahn, Don Blake, Scott Herndon, Daun Jeong, John T. Sullivan, Thomas Mcgee, Rokjin Park, and Saewung Kim
Atmos. Chem. Phys., 21, 6331–6345, https://doi.org/10.5194/acp-21-6331-2021, https://doi.org/10.5194/acp-21-6331-2021, 2021
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We present observations of total reactive gases in a suburban forest observatory in the Seoul metropolitan area. The quantitative comparison with speciated trace gas observations illustrated significant underestimation in atmospheric reactivity from the speciated trace gas observational dataset. We present scientific discussion about potential causes.
Ling Liu, Fangqun Yu, Kaipeng Tu, Zhi Yang, and Xiuhui Zhang
Atmos. Chem. Phys., 21, 6221–6230, https://doi.org/10.5194/acp-21-6221-2021, https://doi.org/10.5194/acp-21-6221-2021, 2021
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Trifluoroacetic acid (TFA) was previously proved to participate in sulfuric acid (SA)–dimethylamine (DMA) nucleation in Shanghai, China. However, complex atmospheric environments can influence the nucleation of aerosol significantly. We show the influence of different atmospheric conditions on the SA-DMA-TFA nucleation and find the enhancement by TFA can be significant in cold and polluted areas, which provides the perspective of the realistic role of TFA in different atmospheric environments.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775, https://doi.org/10.5194/acp-21-5755-2021, https://doi.org/10.5194/acp-21-5755-2021, 2021
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Pamela S. Rickly, Lu Xu, John D. Crounse, Paul O. Wennberg, and Andrew W. Rollins
Atmos. Meas. Tech., 14, 2429–2439, https://doi.org/10.5194/amt-14-2429-2021, https://doi.org/10.5194/amt-14-2429-2021, 2021
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Key improvements have been made to an in situ laser-induced fluorescence instrument for measuring SO2 in polluted and pristine environments. Laser linewidth is reduced, rapid laser tuning is implemented, and fluorescence bandpass filters are optimized. These improvements have led to a 50 % reduction in instrument detection limit. The influence of aromatic compounds was also investigated and determined to not bias SO2 measurements.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
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.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Junjie Liu, Latha Baskaran, Kevin Bowman, David Schimel, A. Anthony Bloom, Nicholas C. Parazoo, Tomohiro Oda, Dustin Carroll, Dimitris Menemenlis, Joanna Joiner, Roisin Commane, Bruce Daube, Lucianna V. Gatti, Kathryn McKain, John Miller, Britton B. Stephens, Colm Sweeney, and Steven Wofsy
Earth Syst. Sci. Data, 13, 299–330, https://doi.org/10.5194/essd-13-299-2021, https://doi.org/10.5194/essd-13-299-2021, 2021
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On average, the terrestrial biosphere carbon sink is equivalent to ~ 20 % of fossil fuel emissions. Understanding where and why the terrestrial biosphere absorbs carbon from the atmosphere is pivotal to any mitigation policy. Here we present a regionally resolved satellite-constrained net biosphere exchange (NBE) dataset with corresponding uncertainties between 2010–2018: CMS-Flux NBE 2020. The dataset provides a unique perspective on monitoring regional contributions to the CO2 growth rate.
Angharad C. Stell, Luke M. Western, Tomás Sherwen, and Matthew Rigby
Atmos. Chem. Phys., 21, 1717–1736, https://doi.org/10.5194/acp-21-1717-2021, https://doi.org/10.5194/acp-21-1717-2021, 2021
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Although it is the second-most important greenhouse gas, our understanding of the atmospheric-methane budget is limited. The uncertainty highlights the need for new tools to investigate sources and sinks. Here, we use a Gaussian process emulator to efficiently approximate the response of atmospheric-methane observations to changes in the most uncertain emission or loss processes. With this new method, we rigorously quantify the sensitivity of atmospheric observations to budget uncertainties.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Alba Lorente, Tobias Borsdorff, Andre Butz, Otto Hasekamp, Joost aan de Brugh, Andreas Schneider, Lianghai Wu, Frank Hase, Rigel Kivi, Debra Wunch, David F. Pollard, Kei Shiomi, Nicholas M. Deutscher, Voltaire A. Velazco, Coleen M. Roehl, Paul O. Wennberg, Thorsten Warneke, and Jochen Landgraf
Atmos. Meas. Tech., 14, 665–684, https://doi.org/10.5194/amt-14-665-2021, https://doi.org/10.5194/amt-14-665-2021, 2021
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TROPOMI aboard Sentinel-5P satellite provides methane (CH4) measurements with exceptional temporal and spatial resolution. The study describes a series of improvements developed to retrieve CH4 from TROPOMI. The updated CH4 product features (among others) a more accurate a posteriori correction derived independently of any reference data. The validation of the improved data product shows good agreement with ground-based and satellite measurements, which highlights the quality of the TROPOMI CH4.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
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.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
Reem A. Hannun, Andrew K. Swanson, Steven A. Bailey, Thomas F. Hanisco, T. Paul Bui, Ilann Bourgeois, Jeff Peischl, and Thomas B. Ryerson
Atmos. Meas. Tech., 13, 6877–6887, https://doi.org/10.5194/amt-13-6877-2020, https://doi.org/10.5194/amt-13-6877-2020, 2020
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We have developed a cavity-enhanced absorption instrument to measure ozone in the atmosphere. The detection technique enables highly sensitive measurements in fast averaging times. The compact, robust instrument is suitable for operation in varied field environments, including aboard research aircraft. We have successfully flown the instrument and demonstrated its performance capabilities with measurements of ozone deposition rates over the coastal Pacific Ocean.
Robert J. Parker, Alex Webb, Hartmut Boesch, Peter Somkuti, Rocio Barrio Guillo, Antonio Di Noia, Nikoleta Kalaitzi, Jasdeep S. Anand, Peter Bergamaschi, Frederic Chevallier, Paul I. Palmer, Liang Feng, Nicholas M. Deutscher, Dietrich G. Feist, David W. T. Griffith, Frank Hase, Rigel Kivi, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, Christof Petri, David F. Pollard, Coleen Roehl, Mahesh K. Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Thorsten Warneke, Paul O. Wennberg, and Debra Wunch
Earth Syst. Sci. Data, 12, 3383–3412, https://doi.org/10.5194/essd-12-3383-2020, https://doi.org/10.5194/essd-12-3383-2020, 2020
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This work presents the latest release of the University of Leicester GOSAT methane data and acts as the definitive description of this dataset. We detail the processing, validation and evaluation involved in producing these data and highlight its many applications. With now over a decade of global atmospheric methane observations, this dataset has helped, and will continue to help, us better understand the global methane budget and investigate how it may respond to a future changing climate.
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
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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.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
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Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Jake P. Rowe, Andrew T. Lambe, and William H. Brune
Atmos. Chem. Phys., 20, 13417–13424, https://doi.org/10.5194/acp-20-13417-2020, https://doi.org/10.5194/acp-20-13417-2020, 2020
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We conducted a series of experiments in which the 185 to 254 nm photon flux ratio (I185 : I254) emitted by low-pressure mercury lamps installed in an oxidation flow reactor (OFR) was systematically varied using multiple novel lamp configurations. Integrated OH exposure values achieved for each lamp type were obtained as a function of OFR operating conditions. A photochemical box model was used to develop a generalized OH exposure estimation equation as a function of [H2O], [O3], and OH reactivity.
Arshad Arjunan Nair and Fangqun Yu
Atmos. Chem. Phys., 20, 12853–12869, https://doi.org/10.5194/acp-20-12853-2020, https://doi.org/10.5194/acp-20-12853-2020, 2020
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Small particles in the atmosphere can affect cloud formation and properties and thus Earth's energy budget. These cloud condensation nuclei (CCN) contribute the largest uncertainties in climate change modeling. To reduce these uncertainties, it is important to quantify CCN numbers accurately, measurements of which are sparse. We propose and evaluate a machine learning method to estimate CCN, in the absence of their direct measurements, using more common measurements of weather and air quality.
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
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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.
Viral Shah, Daniel J. Jacob, Jonathan M. Moch, Xuan Wang, and Shixian Zhai
Atmos. Chem. Phys., 20, 12223–12245, https://doi.org/10.5194/acp-20-12223-2020, https://doi.org/10.5194/acp-20-12223-2020, 2020
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Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Atmos. Chem. Phys., 20, 12093–12114, https://doi.org/10.5194/acp-20-12093-2020, https://doi.org/10.5194/acp-20-12093-2020, 2020
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Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
Wayne M. Angevine, Jeff Peischl, Alice Crawford, Christopher P. Loughner, Ilana B. Pollack, and Chelsea R. Thompson
Atmos. Chem. Phys., 20, 11855–11868, https://doi.org/10.5194/acp-20-11855-2020, https://doi.org/10.5194/acp-20-11855-2020, 2020
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Emissions of air pollutants must be known for a wide variety of applications. Different methods of estimating emissions often disagree substantially. In this study, we apply standard methods to a well-known source, a power plant. We explore the uncertainty implied by the different answers that come from the different methods, different samples taken over several years, and different pollutants. We find that the overall uncertainty of emissions estimates is about 30 %.
Ben Silver, Luke Conibear, Carly L. Reddington, Christoph Knote, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 20, 11683–11695, https://doi.org/10.5194/acp-20-11683-2020, https://doi.org/10.5194/acp-20-11683-2020, 2020
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China suffers from serious air pollution, which is thought to cause millions of early deaths each year. Measurements on the ground show that overall air quality is improving. Air quality is also affected by weather conditions, which can vary from year to year. We conduct computer simulations to show it is the reduction of the amount of pollution emitted, rather than weather conditions, which caused air quality to improve during 2015–2017. We then estimate that 150 000 fewer people die early.
Hirofumi Ohyama, Isamu Morino, Voltaire A. Velazco, Theresa Klausner, Gerry Bagtasa, Matthäus Kiel, Matthias Frey, Akihiro Hori, Osamu Uchino, Tsuneo Matsunaga, Nicholas M. Deutscher, Joshua P. DiGangi, Yonghoon Choi, Glenn S. Diskin, Sally E. Pusede, Alina Fiehn, Anke Roiger, Michael Lichtenstern, Hans Schlager, Pao K. Wang, Charles C.-K. Chou, Maria Dolores Andrés-Hernández, and John P. Burrows
Atmos. Meas. Tech., 13, 5149–5163, https://doi.org/10.5194/amt-13-5149-2020, https://doi.org/10.5194/amt-13-5149-2020, 2020
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Column-averaged dry-air mole fractions of CO2 and CH4 measured by a solar viewing portable Fourier transform spectrometer (EM27/SUN) were validated with in situ profile data obtained during the transfer flights of two aircraft campaigns. Atmospheric dynamical properties based on ERA5 and WRF-Chem were used as criteria for selecting the best aircraft profiles for the validation. The resulting air-mass-independent correction factors for the EM27/SUN data were 0.9878 for CO2 and 0.9829 for CH4.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
Sara Martínez-Alonso, Merritt Deeter, Helen Worden, Tobias Borsdorff, Ilse Aben, Róisin Commane, Bruce Daube, Gene Francis, Maya George, Jochen Landgraf, Debbie Mao, Kathryn McKain, and Steven Wofsy
Atmos. Meas. Tech., 13, 4841–4864, https://doi.org/10.5194/amt-13-4841-2020, https://doi.org/10.5194/amt-13-4841-2020, 2020
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CO is of great importance in climate and air quality studies. To understand newly available TROPOMI data in the frame of the global CO record, we compared those to satellite (MOPITT) and airborne (ATom) CO datasets. The MOPITT dataset is the longest to date (2000–present) and is well-characterized. We used ATom to validate cloudy TROPOMI data over oceans and investigate TROPOMI's vertical sensitivity to CO. Our results show that TROPOMI CO data are in excellent agreement with the other datasets.
Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Kenneth C. Aikin, Teresa Campos, Hannah Clark, Róisín Commane, Bruce Daube, Glenn W. Diskin, James W. Elkins, Ru-Shan Gao, Audrey Gaudel, Eric J. Hintsa, Bryan J. Johnson, Rigel Kivi, Kathryn McKain, Fred L. Moore, David D. Parrish, Richard Querel, Eric Ray, Ricardo Sánchez, Colm Sweeney, David W. Tarasick, Anne M. Thompson, Valérie Thouret, Jacquelyn C. Witte, Steve C. Wofsy, and Thomas B. Ryerson
Atmos. Chem. Phys., 20, 10611–10635, https://doi.org/10.5194/acp-20-10611-2020, https://doi.org/10.5194/acp-20-10611-2020, 2020
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
Amir H. Souri, Caroline R. Nowlan, Gonzalo González Abad, Lei Zhu, Donald R. Blake, Alan Fried, Andrew J. Weinheimer, Armin Wisthaler, Jung-Hun Woo, Qiang Zhang, Christopher E. Chan Miller, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 20, 9837–9854, https://doi.org/10.5194/acp-20-9837-2020, https://doi.org/10.5194/acp-20-9837-2020, 2020
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For the first time, we provide a joint nonlinear optimal estimate of NOx and NMVOC emissions during the KORUS-AQ campaign by simultaneously incorporating SAO's new product of HCHO columns from OMPS and OMI tropospheric NO2 columns into a regional model. Results demonstrate a promising improvement in the performance of the model in terms of HCHO and NO2 concentrations, which in turn enables us to quantify the impact of the emission changes on different pathways of ozone formation and loss.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623, https://doi.org/10.5194/essd-12-1561-2020, https://doi.org/10.5194/essd-12-1561-2020, 2020
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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
Peter D. Ivatt and Mathew J. Evans
Atmos. Chem. Phys., 20, 8063–8082, https://doi.org/10.5194/acp-20-8063-2020, https://doi.org/10.5194/acp-20-8063-2020, 2020
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We investigate the potential of using a decision tree algorithm to identify and correct the tropospheric ozone bias in a chemical transport model. We train the algorithm on 2010–2015 ground and column observation data and test the algorithm on the 2016–2017 data using the ground data as well as independent flight data. We find the algorithm is successfully able to identify and correct the bias, improving the model performance.
Gan Luo, Fangqun Yu, and Jonathan M. Moch
Geosci. Model Dev., 13, 2879–2903, https://doi.org/10.5194/gmd-13-2879-2020, https://doi.org/10.5194/gmd-13-2879-2020, 2020
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This work improved pH calculation for cloud, rain, and wet surfaces, fraction of cloud available for aqueous-phase chemistry, rainout efficiencies for various types of cloud, empirical washout by rain and snow, and wet surface uptake in GEOS-Chem v12.6.0. We compared simulated mass concentrations of aerosol precursors and aerosols with surface monitoring networks, Arctic sites, and ATom observations, and showed that the model results with the updated wet processes agree better for most species.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
Fangqun Yu, Alexey B. Nadykto, Gan Luo, and Jason Herb
Geosci. Model Dev., 13, 2663–2670, https://doi.org/10.5194/gmd-13-2663-2020, https://doi.org/10.5194/gmd-13-2663-2020, 2020
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Secondary particles formed via nucleation have important implications for air quality and climate. Here we describe nucleation rate lookup tables for four different nucleation mechanisms that can be readily used in chemistry transport and climate models. The nucleation rates predicted have been assessed against state-of-the-art laboratory measurements. The lookup tables cover a wide range of key parameters controlling binary, ternary, and ion-mediated nucleation in the Earth's atmosphere.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Sam J. Silva, Colette L. Heald, and Alex B. Guenther
Geosci. Model Dev., 13, 2569–2585, https://doi.org/10.5194/gmd-13-2569-2020, https://doi.org/10.5194/gmd-13-2569-2020, 2020
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Simulating the influence of the biosphere on atmospheric chemistry has traditionally been computationally intensive. We describe a surrogate canopy physics model parameterized using a statistical learning technique and specifically designed for use in large-scale chemical transport models. Our surrogate model reproduces a more detailed model to within 10 % without a large computational demand, improving the process representation of biosphere–atmosphere exchange.
Lu Shen, Daniel J. Jacob, Mauricio Santillana, Xuan Wang, and Wei Chen
Geosci. Model Dev., 13, 2475–2486, https://doi.org/10.5194/gmd-13-2475-2020, https://doi.org/10.5194/gmd-13-2475-2020, 2020
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Chemical mechanisms in air quality models tend to get more complicated with time, reflecting both increasing knowledge and the need for greater scope. This objectively improves the models but increases the computational burden. In this work, we present an approach that can reduce the computational cost of chemical integration by 30–40 % while maintaining an accuracy better than 1 %. It retains the complexity of the full mechanism where it is needed and preserves full diagnostic information.
Andrew W. Rollins, Pamela S. Rickly, Ru-Shan Gao, Thomas B. Ryerson, Steven S. Brown, Jeff Peischl, and Ilann Bourgeois
Atmos. Meas. Tech., 13, 2425–2439, https://doi.org/10.5194/amt-13-2425-2020, https://doi.org/10.5194/amt-13-2425-2020, 2020
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Nitric oxide (NO) is a key atmospheric constituent controlling atmospheric oxidation chemistry and tropospheric ozone formation. Existing instrumentation capable of quantifying NO at very low mixing ratios is uncommon and typically relies on chemiluminescence. We describe and demonstrate a new laser-based technique (LIF) with significant practical and technical advantages to CL. This technique is expected to allow for advances in understanding of atmospheric radical chemistry.
Sophia Brilke, Nikolaus Fölker, Thomas Müller, Konrad Kandler, Xianda Gong, Jeff Peischl, Bernadett Weinzierl, and Paul M. Winkler
Atmos. Chem. Phys., 20, 5645–5656, https://doi.org/10.5194/acp-20-5645-2020, https://doi.org/10.5194/acp-20-5645-2020, 2020
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Atmospheric particle size distributions with the focus on freshly nucleated particles were measured during the A-LIFE field experiment in Cyprus. A DMA-train was set up for the first time in an atmospheric environment and captures the sub-10 nm particle dynamics. Several new particle formation (NPF) events are studied in detail, of which some did not show particle growth beyond 10 nm indicating that NPF may occur more frequently than estimated when the sub-10 nm size range is not covered.
Anton Laakso, Peter K. Snyder, Stefan Liess, Antti-Ilari Partanen, and Dylan B. Millet
Earth Syst. Dynam., 11, 415–434, https://doi.org/10.5194/esd-11-415-2020, https://doi.org/10.5194/esd-11-415-2020, 2020
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Geoengineering techniques have been proposed to prevent climate warming in the event of insufficient greenhouse gas emission reductions. Simultaneously, these techniques have an impact on precipitation, which depends on the techniques used, geoengineering magnitude, and background circumstances. We separated the independent and dependent components of precipitation responses to temperature, which were then used to explain the precipitation changes in the studied climate model simulations.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Alexander B. Thames, William H. Brune, David O. Miller, Hannah M. Allen, Eric C. Apel, Donald R. Blake, T. Paul Bui, Roisin Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, Joshua P. DiGangi, James W. Elkins, Samuel R. Hall, Thomas F. Hanisco, Reem A. Hannun, Eric Hintsa, Rebecca S. Hornbrook, Michelle J. Kim, Kathryn McKain, Fred L. Moore, Julie M. Nicely, Jeffrey Peischl, Thomas B. Ryerson, Jason M. St. Clair, Colm Sweeney, Alex Teng, Chelsea R. Thompson, Kirk Ullmann, Paul O. Wennberg, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 4013–4029, https://doi.org/10.5194/acp-20-4013-2020, https://doi.org/10.5194/acp-20-4013-2020, 2020
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Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Wenfu Tang, Helen M. Worden, Merritt N. Deeter, David P. Edwards, Louisa K. Emmons, Sara Martínez-Alonso, Benjamin Gaubert, Rebecca R. Buchholz, Glenn S. Diskin, Russell R. Dickerson, Xinrong Ren, Hao He, and Yutaka Kondo
Atmos. Meas. Tech., 13, 1337–1356, https://doi.org/10.5194/amt-13-1337-2020, https://doi.org/10.5194/amt-13-1337-2020, 2020
Md. Robiul Islam, Thilina Jayarathne, Isobel J. Simpson, Benjamin Werden, John Maben, Ashley Gilbert, Puppala S. Praveen, Sagar Adhikari, Arnico K. Panday, Maheswar Rupakheti, Donald R. Blake, Robert J. Yokelson, Peter F. DeCarlo, William C. Keene, and Elizabeth A. Stone
Atmos. Chem. Phys., 20, 2927–2951, https://doi.org/10.5194/acp-20-2927-2020, https://doi.org/10.5194/acp-20-2927-2020, 2020
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The Kathmandu Valley experiences high levels of air pollution. In this study, atmospheric gases and particulate matter were characterized by online and off-line measurements, with an emphasis on understanding their sources. The major sources of particulate matter and trace gases were identified as garbage burning, biomass burning, and vehicles. The majority of secondary organic aerosol was attributed to anthropogenic precursors, while a minority was attributed to biogenic gases.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, James J. Schwab, James P. Sherman, and Yanda Zhang
Atmos. Chem. Phys., 20, 2591–2601, https://doi.org/10.5194/acp-20-2591-2020, https://doi.org/10.5194/acp-20-2591-2020, 2020
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Particle number concentration (PNC) is a key parameter important for the health and climate impacts of atmospheric aerosols. We show that, even during wintertime, regional nucleation occurs and contributes significantly to number concentrations of ultrafine particles and cloud condensation nuclei. Due to low biogenic emissions, wintertime regional nucleation is solely controlled by inorganic species, and ternary ion-mediated nucleation is able to capture the observed variations in PNC.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Xiaoyan Ma, Hailing Jia, Rong Tian, Fangqun Yu, and Jiagnan Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-54, https://doi.org/10.5194/acp-2020-54, 2020
Preprint withdrawn
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BC Mixing state, is one of critical microphysical properties to modulate optical properties, radiative forcing (RF), and climatic effect. However, it has been simply assumed previously as either external or internal mixing. In this study, by employing a nested GEOS-Chem-APM with predicted BC mixing state, we examined the effect of mixing state on aerosol optical properties, RF, and heating rate over East Asia. This will improve the predictions of aerosol climatic effect in the future.
Karl M. Seltzer, Drew T. Shindell, Prasad Kasibhatla, and Christopher S. Malley
Atmos. Chem. Phys., 20, 1757–1775, https://doi.org/10.5194/acp-20-1757-2020, https://doi.org/10.5194/acp-20-1757-2020, 2020
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Long-term exposure to ambient ozone is associated with a variety of impacts, including adverse human-health effects and reduced commercial crop yields. We apply machine learning to empirically model long-term O3 exposure over the continental United States from 2000 to 2015 and generate a measurement-based assessment of impacts on human health and crop yields. Notably, our results illustrate how different conclusions regarding historical impacts can be drawn through the use of varying metrics.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Joshua D. Shutter, Norton T. Allen, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 6079–6089, https://doi.org/10.5194/amt-12-6079-2019, https://doi.org/10.5194/amt-12-6079-2019, 2019
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A new mid-infrared and ultra-portable formaldehyde (HCHO) sensor from Aeris Technologies is characterized and evaluated against well-established laser-induced fluorescence (LIF) instrumentation. The Aeris sensor displays linear behavior (R squared > 0.94) and shows good agreement with LIF instruments. While the compact sensor is not currently a replacement for the most sensitive research-grade instrumentation available, its sub-ppbv precision is sufficient for indoor and outdoor HCHO monitoring.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Maria A. Zawadowicz, Karl D. Froyd, Anne E. Perring, Daniel M. Murphy, Dominick V. Spracklen, Colette L. Heald, Peter R. Buseck, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 13859–13870, https://doi.org/10.5194/acp-19-13859-2019, https://doi.org/10.5194/acp-19-13859-2019, 2019
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We report measurements of small particles of biological origin (for example, fragments of bacteria, pollen, or fungal spores) in the atmosphere over the continental United States. We use a recently developed identification technique based on airborne mass spectrometry in conjunction with an extensive aircraft dataset. We show that biological particles are present at altitudes up to 10 km and we quantify typical concentrations.
William C. Porter and Colette L. Heald
Atmos. Chem. Phys., 19, 13367–13381, https://doi.org/10.5194/acp-19-13367-2019, https://doi.org/10.5194/acp-19-13367-2019, 2019
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In this paper we explore the connection between changes in surface temperature and changes in ozone pollution. While explanations for this connection have been proposed in the past, we attempt to better quantify them using models and statistics. We find that some of the most commonly cited mechanisms, including biogenic emissions and temperature-dependent chemical processes, can explain less than half of the O3–T correlation. Meteorology is identified as the most likely driver for the remainder.
Susan S. Kulawik, Sean Crowell, David Baker, Junjie Liu, Kathryn McKain, Colm Sweeney, Sebastien C. Biraud, Steve Wofsy, Christopher W. O'Dell, Paul O. Wennberg, Debra Wunch, Coleen M. Roehl, Nicholas M. Deutscher, Matthäus Kiel, David W. T. Griffith, Voltaire A. Velazco, Justus Notholt, Thorsten Warneke, Christof Petri, Martine De Mazière, Mahesh K. Sha, Ralf Sussmann, Markus Rettinger, Dave F. Pollard, Isamu Morino, Osamu Uchino, Frank Hase, Dietrich G. Feist, Sébastien Roche, Kimberly Strong, Rigel Kivi, Laura Iraci, Kei Shiomi, Manvendra K. Dubey, Eliezer Sepulveda, Omaira Elena Garcia Rodriguez, Yao Té, Pascal Jeseck, Pauli Heikkinen, Edward J. Dlugokencky, Michael R. Gunson, Annmarie Eldering, David Crisp, Brendan Fisher, and Gregory B. Osterman
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2019-257, https://doi.org/10.5194/amt-2019-257, 2019
Publication in AMT not foreseen
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This paper provides a benchmark of OCO-2 v8 and ACOS-GOSAT v7.3 XCO2 and lowermost tropospheric (LMT) errors. The paper focuses on the systematic errors and subtracts out validation, co-location, and random errors, looks at the correlation scale-length (spatially and temporally) of systematic errors, finding that the scale lengths are similar to bias correction scale-lengths. The assimilates of the bias correction term is used to place an error on fluxes estimates.
Jacob K. Hedelius, Tai-Long He, Dylan B. A. Jones, Bianca C. Baier, Rebecca R. Buchholz, Martine De Mazière, Nicholas M. Deutscher, Manvendra K. Dubey, Dietrich G. Feist, David W. T. Griffith, Frank Hase, Laura T. Iraci, Pascal Jeseck, Matthäus Kiel, Rigel Kivi, Cheng Liu, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Sébastien Roche, Coleen M. Roehl, Matthias Schneider, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Colm Sweeney, Yao Té, Osamu Uchino, Voltaire A. Velazco, Wei Wang, Thorsten Warneke, Paul O. Wennberg, Helen M. Worden, and