Articles | Volume 24, issue 13
https://doi.org/10.5194/acp-24-8049-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-8049-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Jul 2024
Research article |
| 16 Jul 2024
| 16 Jul 2024
Diverging trends in aerosol sulfate and nitrate measured in the remote North Atlantic in Barbados are attributed to clean air policies, African smoke, and anthropogenic emissions
Rosenstiel School of Marine, Atmospheric, and Earth Science, University of Miami, Miami, FL 33149, USA
Joseph M. Prospero
Rosenstiel School of Marine, Atmospheric, and Earth Science, University of Miami, Miami, FL 33149, USA
Kristen Foley
Office of Research and Development, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina, USA
Havala O. T. Pye
Office of Research and Development, U.S. Environmental Protection Agency, Research Triangle Park, North Carolina, USA
Lillian Custals
Rosenstiel School of Marine, Atmospheric, and Earth Science, University of Miami, Miami, FL 33149, USA
Edmund Blades
Rosenstiel School of Marine, Atmospheric, and Earth Science, University of Miami, Miami, FL 33149, USA
Peter Sealy
Rosenstiel School of Marine, Atmospheric, and Earth Science, University of Miami, Miami, FL 33149, USA
James A. Christie
Rosenstiel School of Marine, Atmospheric, and Earth Science, University of Miami, Miami, FL 33149, USA
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EGUsphere, https://doi.org/10.5194/egusphere-2024-3288, https://doi.org/10.5194/egusphere-2024-3288, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Saharan dust transported across the Atlantic to the Caribbean, South America, and North America is hypothesized to undergo chemical processing by inorganic and organic acids that enhances cloud droplet formation, nutrient availability, and reflectivity of. In this study, chemical analysis performed on African dust deposited over Barbados shows that acid tracers are found mostly on sea salt and smoke particles, rather than dust, indicating that dust particles undergo minimal chemical processing.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankarararman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Hannele Hakola, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbiginiw Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-1, https://doi.org/10.5194/essd-2024-1, 2024
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Aerosol particles can interact with incoming solar radiation and outgoing long wave radiation, change cloud properties, affect photochemistry, impact surface air quality, and when deposited impact surface albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. Here we present a new compilation of aerosol observations including composition, a methodology for comparing the datasets to model output, and show the implications of these results using one model.
Haley M. Royer, Mira L. Pöhlker, Ovid Krüger, Edmund Blades, Peter Sealy, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Andrew P. Ault, Patricia K. Quinn, Paquita Zuidema, Christopher Pöhlker, Ulrich Pöschl, Meinrat Andreae, and Cassandra J. Gaston
Atmos. Chem. Phys., 23, 981–998, https://doi.org/10.5194/acp-23-981-2023, https://doi.org/10.5194/acp-23-981-2023, 2023
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Bjorn Stevens, Sandrine Bony, David Farrell, Felix Ament, Alan Blyth, Christopher Fairall, Johannes Karstensen, Patricia K. Quinn, Sabrina Speich, Claudia Acquistapace, Franziska Aemisegger, Anna Lea Albright, Hugo Bellenger, Eberhard Bodenschatz, Kathy-Ann Caesar, Rebecca Chewitt-Lucas, Gijs de Boer, Julien Delanoë, Leif Denby, Florian Ewald, Benjamin Fildier, Marvin Forde, Geet George, Silke Gross, Martin Hagen, Andrea Hausold, Karen J. Heywood, Lutz Hirsch, Marek Jacob, Friedhelm Jansen, Stefan Kinne, Daniel Klocke, Tobias Kölling, Heike Konow, Marie Lothon, Wiebke Mohr, Ann Kristin Naumann, Louise Nuijens, Léa Olivier, Robert Pincus, Mira Pöhlker, Gilles Reverdin, Gregory Roberts, Sabrina Schnitt, Hauke Schulz, A. Pier Siebesma, Claudia Christine Stephan, Peter Sullivan, Ludovic Touzé-Peiffer, Jessica Vial, Raphaela Vogel, Paquita Zuidema, Nicola Alexander, Lyndon Alves, Sophian Arixi, Hamish Asmath, Gholamhossein Bagheri, Katharina Baier, Adriana Bailey, Dariusz Baranowski, Alexandre Baron, Sébastien Barrau, Paul A. Barrett, Frédéric Batier, Andreas Behrendt, Arne Bendinger, Florent Beucher, Sebastien Bigorre, Edmund Blades, Peter Blossey, Olivier Bock, Steven Böing, Pierre Bosser, Denis Bourras, Pascale Bouruet-Aubertot, Keith Bower, Pierre Branellec, Hubert Branger, Michal Brennek, Alan Brewer, Pierre-Etienne Brilouet, Björn Brügmann, Stefan A. Buehler, Elmo Burke, Ralph Burton, Radiance Calmer, Jean-Christophe Canonici, Xavier Carton, Gregory Cato Jr., Jude Andre Charles, Patrick Chazette, Yanxu Chen, Michal T. Chilinski, Thomas Choularton, Patrick Chuang, Shamal Clarke, Hugh Coe, Céline Cornet, Pierre Coutris, Fleur Couvreux, Susanne Crewell, Timothy Cronin, Zhiqiang Cui, Yannis Cuypers, Alton Daley, Gillian M. Damerell, Thibaut Dauhut, Hartwig Deneke, Jean-Philippe Desbios, Steffen Dörner, Sebastian Donner, Vincent Douet, Kyla Drushka, Marina Dütsch, André Ehrlich, Kerry Emanuel, Alexandros Emmanouilidis, Jean-Claude Etienne, Sheryl Etienne-Leblanc, Ghislain Faure, Graham Feingold, Luca Ferrero, Andreas Fix, Cyrille Flamant, Piotr Jacek Flatau, Gregory R. Foltz, Linda Forster, Iulian Furtuna, Alan Gadian, Joseph Galewsky, Martin Gallagher, Peter Gallimore, Cassandra Gaston, Chelle Gentemann, Nicolas Geyskens, Andreas Giez, John Gollop, Isabelle Gouirand, Christophe Gourbeyre, Dörte de Graaf, Geiske E. de Groot, Robert Grosz, Johannes Güttler, Manuel Gutleben, Kashawn Hall, George Harris, Kevin C. Helfer, Dean Henze, Calvert Herbert, Bruna Holanda, Antonio Ibanez-Landeta, Janet Intrieri, Suneil Iyer, Fabrice Julien, Heike Kalesse, Jan Kazil, Alexander Kellman, Abiel T. Kidane, Ulrike Kirchner, Marcus Klingebiel, Mareike Körner, Leslie Ann Kremper, Jan Kretzschmar, Ovid Krüger, Wojciech Kumala, Armin Kurz, Pierre L'Hégaret, Matthieu Labaste, Tom Lachlan-Cope, Arlene Laing, Peter Landschützer, Theresa Lang, Diego Lange, Ingo Lange, Clément Laplace, Gauke Lavik, Rémi Laxenaire, Caroline Le Bihan, Mason Leandro, Nathalie Lefevre, Marius Lena, Donald Lenschow, Qiang Li, Gary Lloyd, Sebastian Los, Niccolò Losi, Oscar Lovell, Christopher Luneau, Przemyslaw Makuch, Szymon Malinowski, Gaston Manta, Eleni Marinou, Nicholas Marsden, Sebastien Masson, Nicolas Maury, Bernhard Mayer, Margarette Mayers-Als, Christophe Mazel, Wayne McGeary, James C. McWilliams, Mario Mech, Melina Mehlmann, Agostino Niyonkuru Meroni, Theresa Mieslinger, Andreas Minikin, Peter Minnett, Gregor Möller, Yanmichel Morfa Avalos, Caroline Muller, Ionela Musat, Anna Napoli, Almuth Neuberger, Christophe Noisel, David Noone, Freja Nordsiek, Jakub L. Nowak, Lothar Oswald, Douglas J. Parker, Carolyn Peck, Renaud Person, Miriam Philippi, Albert Plueddemann, Christopher Pöhlker, Veronika Pörtge, Ulrich Pöschl, Lawrence Pologne, Michał Posyniak, Marc Prange, Estefanía Quiñones Meléndez, Jule Radtke, Karim Ramage, Jens Reimann, Lionel Renault, Klaus Reus, Ashford Reyes, Joachim Ribbe, Maximilian Ringel, Markus Ritschel, Cesar B. Rocha, Nicolas Rochetin, Johannes Röttenbacher, Callum Rollo, Haley Royer, Pauline Sadoulet, Leo Saffin, Sanola Sandiford, Irina Sandu, Michael Schäfer, Vera Schemann, Imke Schirmacher, Oliver Schlenczek, Jerome Schmidt, Marcel Schröder, Alfons Schwarzenboeck, Andrea Sealy, Christoph J. Senff, Ilya Serikov, Samkeyat Shohan, Elizabeth Siddle, Alexander Smirnov, Florian Späth, Branden Spooner, M. Katharina Stolla, Wojciech Szkółka, Simon P. de Szoeke, Stéphane Tarot, Eleni Tetoni, Elizabeth Thompson, Jim Thomson, Lorenzo Tomassini, Julien Totems, Alma Anna Ubele, Leonie Villiger, Jan von Arx, Thomas Wagner, Andi Walther, Ben Webber, Manfred Wendisch, Shanice Whitehall, Anton Wiltshire, Allison A. Wing, Martin Wirth, Jonathan Wiskandt, Kevin Wolf, Ludwig Worbes, Ethan Wright, Volker Wulfmeyer, Shanea Young, Chidong Zhang, Dongxiao Zhang, Florian Ziemen, Tobias Zinner, and Martin Zöger
Earth Syst. Sci. Data, 13, 4067–4119, https://doi.org/10.5194/essd-13-4067-2021, https://doi.org/10.5194/essd-13-4067-2021, 2021
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The EUREC4A field campaign, designed to test hypothesized mechanisms by which clouds respond to warming and benchmark next-generation Earth-system models, is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. It was the first campaign that attempted to characterize the full range of processes and scales influencing trade wind clouds.
Patricia K. Quinn, Elizabeth J. Thompson, Derek J. Coffman, Sunil Baidar, Ludovic Bariteau, Timothy S. Bates, Sebastien Bigorre, Alan Brewer, Gijs de Boer, Simon P. de Szoeke, Kyla Drushka, Gregory R. Foltz, Janet Intrieri, Suneil Iyer, Chris W. Fairall, Cassandra J. Gaston, Friedhelm Jansen, James E. Johnson, Ovid O. Krüger, Richard D. Marchbanks, Kenneth P. Moran, David Noone, Sergio Pezoa, Robert Pincus, Albert J. Plueddemann, Mira L. Pöhlker, Ulrich Pöschl, Estefania Quinones Melendez, Haley M. Royer, Malgorzata Szczodrak, Jim Thomson, Lucia M. Upchurch, Chidong Zhang, Dongxiao Zhang, and Paquita Zuidema
Earth Syst. Sci. Data, 13, 1759–1790, https://doi.org/10.5194/essd-13-1759-2021, https://doi.org/10.5194/essd-13-1759-2021, 2021
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ATOMIC took place in the northwestern tropical Atlantic during January and February of 2020 to gather information on shallow atmospheric convection, the effects of aerosols and clouds on the ocean surface energy budget, and mesoscale oceanic processes. Measurements made from the NOAA RV Ronald H. Brown and assets it deployed (instrumented mooring and uncrewed seagoing vehicles) are described herein to advance widespread use of the data by the ATOMIC and broader research communities.
Samantha J. Kramer, Claudia Alvarez, Anne E. Barkley, Peter R. Colarco, Lillian Custals, Rodrigo Delgadillo, Cassandra J. Gaston, Ravi Govindaraju, and Paquita Zuidema
Atmos. Chem. Phys., 20, 10047–10062, https://doi.org/10.5194/acp-20-10047-2020, https://doi.org/10.5194/acp-20-10047-2020, 2020
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Comparisons of sea salt and size-resolved dust mass concentration measurements over southeast Florida to those from the MERRA-2/GEOS-5 FP aerosol reanalysis show the reanalysis depicts excessive sea salt and puts too much dust in larger intermediate sizes than do the measurements. The vertical distribution of the dust mass is approximately correct. The incorrect reanalysis aerosol speciation and dust sizes have implications for the modeling of their transport, deposition, and radiative impact.
Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
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Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Haley M. Royer, Michael T. Sheridan, Hope E. Elliott, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Zihua Zhu, Andrew P. Ault, and Cassandra J. Gaston
EGUsphere, https://doi.org/10.5194/egusphere-2024-3288, https://doi.org/10.5194/egusphere-2024-3288, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Saharan dust transported across the Atlantic to the Caribbean, South America, and North America is hypothesized to undergo chemical processing by inorganic and organic acids that enhances cloud droplet formation, nutrient availability, and reflectivity of. In this study, chemical analysis performed on African dust deposited over Barbados shows that acid tracers are found mostly on sea salt and smoke particles, rather than dust, indicating that dust particles undergo minimal chemical processing.
Christos I. Efstathiou, Elizabeth Adams, Carlie J. Coats, Robert Zelt, Mark Reed, John McGee, Kristen M. Foley, Fahim I. Sidi, David C. Wong, Steven Fine, and Saravanan Arunachalam
Geosci. Model Dev., 17, 7001–7027, https://doi.org/10.5194/gmd-17-7001-2024, https://doi.org/10.5194/gmd-17-7001-2024, 2024
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We present a summary of enabling high-performance computing of the Community Multiscale Air Quality Model (CMAQ) – a state-of-the-science community multiscale air quality model – on two cloud computing platforms through documenting the technologies, model performance, scaling and relative merits. This may be a new paradigm for computationally intense future model applications. We initiated this work due to a need to leverage cloud computing advances and to ease the learning curve for new users.
Sara Louise Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, and Kathleen Fahey
EGUsphere, https://doi.org/10.5194/egusphere-2024-1550, https://doi.org/10.5194/egusphere-2024-1550, 2024
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters, is improved.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter G. Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
EGUsphere, https://doi.org/10.5194/egusphere-2024-1617, https://doi.org/10.5194/egusphere-2024-1617, 2024
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as variable in size and composition. Here we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the datasets to model output.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
EGUsphere, https://doi.org/10.5194/egusphere-2024-554, https://doi.org/10.5194/egusphere-2024-554, 2024
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Chemical transport model simulations are combined with ozone observations to estimate the bias in ozone attributable to US anthropogenic sources as well as several individual sources of US background ozone: natural sources, non-US anthropogenic sources, and stratospheric ozone. Results indicate a positive bias correlated with US anthropogenic emissions during summer in the eastern US and a negative bias correlated with stratospheric ozone during spring.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankarararman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Hannele Hakola, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbiginiw Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-1, https://doi.org/10.5194/essd-2024-1, 2024
Preprint withdrawn
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Aerosol particles can interact with incoming solar radiation and outgoing long wave radiation, change cloud properties, affect photochemistry, impact surface air quality, and when deposited impact surface albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. Here we present a new compilation of aerosol observations including composition, a methodology for comparing the datasets to model output, and show the implications of these results using one model.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Monica Crippa, Diego Guizzardi, Tim Butler, Terry Keating, Rosa Wu, Jacek Kaminski, Jeroen Kuenen, Junichi Kurokawa, Satoru Chatani, Tazuko Morikawa, George Pouliot, Jacinthe Racine, Michael D. Moran, Zbigniew Klimont, Patrick M. Manseau, Rabab Mashayekhi, Barron H. Henderson, Steven J. Smith, Harrison Suchyta, Marilena Muntean, Efisio Solazzo, Manjola Banja, Edwin Schaaf, Federico Pagani, Jung-Hun Woo, Jinseok Kim, Fabio Monforti-Ferrario, Enrico Pisoni, Junhua Zhang, David Niemi, Mourad Sassi, Tabish Ansari, and Kristen Foley
Earth Syst. Sci. Data, 15, 2667–2694, https://doi.org/10.5194/essd-15-2667-2023, https://doi.org/10.5194/essd-15-2667-2023, 2023
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This study responds to the global and regional atmospheric modelling community's need for a mosaic of air pollutant emissions with global coverage, long time series, spatially distributed data at a high time resolution, and a high sectoral resolution in order to enhance the understanding of transboundary air pollution. The mosaic approach to integrating official regional emission inventories with a global inventory based on a consistent methodology ensures policy-relevant results.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Forwood Wiser, Bryan K. Place, Siddhartha Sen, Havala O. T. Pye, Benjamin Yang, Daniel M. Westervelt, Daven K. Henze, Arlene M. Fiore, and V. Faye McNeill
Geosci. Model Dev., 16, 1801–1821, https://doi.org/10.5194/gmd-16-1801-2023, https://doi.org/10.5194/gmd-16-1801-2023, 2023
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We developed a reduced model of atmospheric isoprene oxidation, AMORE-Isoprene 1.0. It was created using a new Automated Model Reduction (AMORE) method designed to simplify complex chemical mechanisms with minimal manual adjustments to the output. AMORE-Isoprene 1.0 has improved accuracy and similar size to other reduced isoprene mechanisms. When included in the CRACMM mechanism, it improved the accuracy of EPA’s CMAQ model predictions for the northeastern USA compared to observations.
Haley M. Royer, Mira L. Pöhlker, Ovid Krüger, Edmund Blades, Peter Sealy, Nurun Nahar Lata, Zezhen Cheng, Swarup China, Andrew P. Ault, Patricia K. Quinn, Paquita Zuidema, Christopher Pöhlker, Ulrich Pöschl, Meinrat Andreae, and Cassandra J. Gaston
Atmos. Chem. Phys., 23, 981–998, https://doi.org/10.5194/acp-23-981-2023, https://doi.org/10.5194/acp-23-981-2023, 2023
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This paper presents atmospheric particle chemical composition and measurements of aerosol water uptake properties collected at Ragged Point, Barbados, during the winter of 2020. The result of this study indicates the importance of small African smoke particles for cloud droplet formation in the tropical North Atlantic and highlights the large spatial and temporal pervasiveness of smoke over the Atlantic Ocean.
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.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Bjorn Stevens, Sandrine Bony, David Farrell, Felix Ament, Alan Blyth, Christopher Fairall, Johannes Karstensen, Patricia K. Quinn, Sabrina Speich, Claudia Acquistapace, Franziska Aemisegger, Anna Lea Albright, Hugo Bellenger, Eberhard Bodenschatz, Kathy-Ann Caesar, Rebecca Chewitt-Lucas, Gijs de Boer, Julien Delanoë, Leif Denby, Florian Ewald, Benjamin Fildier, Marvin Forde, Geet George, Silke Gross, Martin Hagen, Andrea Hausold, Karen J. Heywood, Lutz Hirsch, Marek Jacob, Friedhelm Jansen, Stefan Kinne, Daniel Klocke, Tobias Kölling, Heike Konow, Marie Lothon, Wiebke Mohr, Ann Kristin Naumann, Louise Nuijens, Léa Olivier, Robert Pincus, Mira Pöhlker, Gilles Reverdin, Gregory Roberts, Sabrina Schnitt, Hauke Schulz, A. Pier Siebesma, Claudia Christine Stephan, Peter Sullivan, Ludovic Touzé-Peiffer, Jessica Vial, Raphaela Vogel, Paquita Zuidema, Nicola Alexander, Lyndon Alves, Sophian Arixi, Hamish Asmath, Gholamhossein Bagheri, Katharina Baier, Adriana Bailey, Dariusz Baranowski, Alexandre Baron, Sébastien Barrau, Paul A. Barrett, Frédéric Batier, Andreas Behrendt, Arne Bendinger, Florent Beucher, Sebastien Bigorre, Edmund Blades, Peter Blossey, Olivier Bock, Steven Böing, Pierre Bosser, Denis Bourras, Pascale Bouruet-Aubertot, Keith Bower, Pierre Branellec, Hubert Branger, Michal Brennek, Alan Brewer, Pierre-Etienne Brilouet, Björn Brügmann, Stefan A. Buehler, Elmo Burke, Ralph Burton, Radiance Calmer, Jean-Christophe Canonici, Xavier Carton, Gregory Cato Jr., Jude Andre Charles, Patrick Chazette, Yanxu Chen, Michal T. Chilinski, Thomas Choularton, Patrick Chuang, Shamal Clarke, Hugh Coe, Céline Cornet, Pierre Coutris, Fleur Couvreux, Susanne Crewell, Timothy Cronin, Zhiqiang Cui, Yannis Cuypers, Alton Daley, Gillian M. Damerell, Thibaut Dauhut, Hartwig Deneke, Jean-Philippe Desbios, Steffen Dörner, Sebastian Donner, Vincent Douet, Kyla Drushka, Marina Dütsch, André Ehrlich, Kerry Emanuel, Alexandros Emmanouilidis, Jean-Claude Etienne, Sheryl Etienne-Leblanc, Ghislain Faure, Graham Feingold, Luca Ferrero, Andreas Fix, Cyrille Flamant, Piotr Jacek Flatau, Gregory R. Foltz, Linda Forster, Iulian Furtuna, Alan Gadian, Joseph Galewsky, Martin Gallagher, Peter Gallimore, Cassandra Gaston, Chelle Gentemann, Nicolas Geyskens, Andreas Giez, John Gollop, Isabelle Gouirand, Christophe Gourbeyre, Dörte de Graaf, Geiske E. de Groot, Robert Grosz, Johannes Güttler, Manuel Gutleben, Kashawn Hall, George Harris, Kevin C. Helfer, Dean Henze, Calvert Herbert, Bruna Holanda, Antonio Ibanez-Landeta, Janet Intrieri, Suneil Iyer, Fabrice Julien, Heike Kalesse, Jan Kazil, Alexander Kellman, Abiel T. Kidane, Ulrike Kirchner, Marcus Klingebiel, Mareike Körner, Leslie Ann Kremper, Jan Kretzschmar, Ovid Krüger, Wojciech Kumala, Armin Kurz, Pierre L'Hégaret, Matthieu Labaste, Tom Lachlan-Cope, Arlene Laing, Peter Landschützer, Theresa Lang, Diego Lange, Ingo Lange, Clément Laplace, Gauke Lavik, Rémi Laxenaire, Caroline Le Bihan, Mason Leandro, Nathalie Lefevre, Marius Lena, Donald Lenschow, Qiang Li, Gary Lloyd, Sebastian Los, Niccolò Losi, Oscar Lovell, Christopher Luneau, Przemyslaw Makuch, Szymon Malinowski, Gaston Manta, Eleni Marinou, Nicholas Marsden, Sebastien Masson, Nicolas Maury, Bernhard Mayer, Margarette Mayers-Als, Christophe Mazel, Wayne McGeary, James C. McWilliams, Mario Mech, Melina Mehlmann, Agostino Niyonkuru Meroni, Theresa Mieslinger, Andreas Minikin, Peter Minnett, Gregor Möller, Yanmichel Morfa Avalos, Caroline Muller, Ionela Musat, Anna Napoli, Almuth Neuberger, Christophe Noisel, David Noone, Freja Nordsiek, Jakub L. Nowak, Lothar Oswald, Douglas J. Parker, Carolyn Peck, Renaud Person, Miriam Philippi, Albert Plueddemann, Christopher Pöhlker, Veronika Pörtge, Ulrich Pöschl, Lawrence Pologne, Michał Posyniak, Marc Prange, Estefanía Quiñones Meléndez, Jule Radtke, Karim Ramage, Jens Reimann, Lionel Renault, Klaus Reus, Ashford Reyes, Joachim Ribbe, Maximilian Ringel, Markus Ritschel, Cesar B. Rocha, Nicolas Rochetin, Johannes Röttenbacher, Callum Rollo, Haley Royer, Pauline Sadoulet, Leo Saffin, Sanola Sandiford, Irina Sandu, Michael Schäfer, Vera Schemann, Imke Schirmacher, Oliver Schlenczek, Jerome Schmidt, Marcel Schröder, Alfons Schwarzenboeck, Andrea Sealy, Christoph J. Senff, Ilya Serikov, Samkeyat Shohan, Elizabeth Siddle, Alexander Smirnov, Florian Späth, Branden Spooner, M. Katharina Stolla, Wojciech Szkółka, Simon P. de Szoeke, Stéphane Tarot, Eleni Tetoni, Elizabeth Thompson, Jim Thomson, Lorenzo Tomassini, Julien Totems, Alma Anna Ubele, Leonie Villiger, Jan von Arx, Thomas Wagner, Andi Walther, Ben Webber, Manfred Wendisch, Shanice Whitehall, Anton Wiltshire, Allison A. Wing, Martin Wirth, Jonathan Wiskandt, Kevin Wolf, Ludwig Worbes, Ethan Wright, Volker Wulfmeyer, Shanea Young, Chidong Zhang, Dongxiao Zhang, Florian Ziemen, Tobias Zinner, and Martin Zöger
Earth Syst. Sci. Data, 13, 4067–4119, https://doi.org/10.5194/essd-13-4067-2021, https://doi.org/10.5194/essd-13-4067-2021, 2021
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The EUREC4A field campaign, designed to test hypothesized mechanisms by which clouds respond to warming and benchmark next-generation Earth-system models, is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. It was the first campaign that attempted to characterize the full range of processes and scales influencing trade wind clouds.
Xiaoyang Chen, Yang Zhang, Kai Wang, Daniel Tong, Pius Lee, Youhua Tang, Jianping Huang, Patrick C. Campbell, Jeff Mcqueen, Havala O. T. Pye, Benjamin N. Murphy, and Daiwen Kang
Geosci. Model Dev., 14, 3969–3993, https://doi.org/10.5194/gmd-14-3969-2021, https://doi.org/10.5194/gmd-14-3969-2021, 2021
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The continuously updated National Air Quality Forecast Capability (NAQFC) provides air quality forecasts. To support the development of the next-generation NAQFC, we evaluate a prototype of GFSv15-CMAQv5.0.2. The performance and the potential improvements for the system are discussed. This study can provide a scientific basis for further development of NAQFC and help it to provide more accurate air quality forecasts to the public over the contiguous United States.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
Patricia K. Quinn, Elizabeth J. Thompson, Derek J. Coffman, Sunil Baidar, Ludovic Bariteau, Timothy S. Bates, Sebastien Bigorre, Alan Brewer, Gijs de Boer, Simon P. de Szoeke, Kyla Drushka, Gregory R. Foltz, Janet Intrieri, Suneil Iyer, Chris W. Fairall, Cassandra J. Gaston, Friedhelm Jansen, James E. Johnson, Ovid O. Krüger, Richard D. Marchbanks, Kenneth P. Moran, David Noone, Sergio Pezoa, Robert Pincus, Albert J. Plueddemann, Mira L. Pöhlker, Ulrich Pöschl, Estefania Quinones Melendez, Haley M. Royer, Malgorzata Szczodrak, Jim Thomson, Lucia M. Upchurch, Chidong Zhang, Dongxiao Zhang, and Paquita Zuidema
Earth Syst. Sci. Data, 13, 1759–1790, https://doi.org/10.5194/essd-13-1759-2021, https://doi.org/10.5194/essd-13-1759-2021, 2021
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ATOMIC took place in the northwestern tropical Atlantic during January and February of 2020 to gather information on shallow atmospheric convection, the effects of aerosols and clouds on the ocean surface energy budget, and mesoscale oceanic processes. Measurements made from the NOAA RV Ronald H. Brown and assets it deployed (instrumented mooring and uncrewed seagoing vehicles) are described herein to advance widespread use of the data by the ATOMIC and broader research communities.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Samantha J. Kramer, Claudia Alvarez, Anne E. Barkley, Peter R. Colarco, Lillian Custals, Rodrigo Delgadillo, Cassandra J. Gaston, Ravi Govindaraju, and Paquita Zuidema
Atmos. Chem. Phys., 20, 10047–10062, https://doi.org/10.5194/acp-20-10047-2020, https://doi.org/10.5194/acp-20-10047-2020, 2020
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Comparisons of sea salt and size-resolved dust mass concentration measurements over southeast Florida to those from the MERRA-2/GEOS-5 FP aerosol reanalysis show the reanalysis depicts excessive sea salt and puts too much dust in larger intermediate sizes than do the measurements. The vertical distribution of the dust mass is approximately correct. The incorrect reanalysis aerosol speciation and dust sizes have implications for the modeling of their transport, deposition, and radiative impact.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Quanyang Lu, Benjamin N. Murphy, Momei Qin, Peter J. Adams, Yunliang Zhao, Havala O. T. Pye, Christos Efstathiou, Chris Allen, and Allen L. Robinson
Atmos. Chem. Phys., 20, 4313–4332, https://doi.org/10.5194/acp-20-4313-2020, https://doi.org/10.5194/acp-20-4313-2020, 2020
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This research work investigates organic aerosol formation in California during the CalNex study. We update the chemical transport model with the most recent mobile-source emission data and introduce a simple parameterization for secondary organic aerosol formed from intermediate-volatility organic compounds. Our results highlight the important contribution of IVOCs to SOA production in the Los Angeles region but underscore that other uncertainties must be addressed to close the SOA mass balance.
Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
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We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
Daiwen Kang, Kristen M. Foley, Rohit Mathur, Shawn J. Roselle, Kenneth E. Pickering, and Dale J. Allen
Geosci. Model Dev., 12, 4409–4424, https://doi.org/10.5194/gmd-12-4409-2019, https://doi.org/10.5194/gmd-12-4409-2019, 2019
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This paper provides a comprehensive evaluation of the lightning production schemes in CMAQ as described in https://www.geosci-model-dev.net/12/3071/2019/gmd-12-3071-2019.html on model performance. The impact of lightning NOx from different schemes is evaluated in time and space using both ground–level network measurements and aloft (ozonesonde and aircraft) observations. These results provide users the benchmark model performance when the lightning NOx production schemes are applied.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Daiwen Kang, Kenneth E. Pickering, Dale J. Allen, Kristen M. Foley, David C. Wong, Rohit Mathur, and Shawn J. Roselle
Geosci. Model Dev., 12, 3071–3083, https://doi.org/10.5194/gmd-12-3071-2019, https://doi.org/10.5194/gmd-12-3071-2019, 2019
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Lightning strikes produce significant amount of nitrogen oxides and the resulting atmospheric chemistry causes one of the primary air pollutants, ground-level ozone, to change. In this paper, we documented the evolution of scientific updates for lightning-induced nitrogen oxides schemes in the CMAQ model. The updated observation-based schemes are good for retrospective applications, while the parameterized scheme can estimate lightning nitrogen oxides for applications without observations.
Lu Xu, Havala O. T. Pye, Jia He, Yunle Chen, Benjamin N. Murphy, and Nga Lee Ng
Atmos. Chem. Phys., 18, 12613–12637, https://doi.org/10.5194/acp-18-12613-2018, https://doi.org/10.5194/acp-18-12613-2018, 2018
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In this study, we integrate lab-in-the-field experiments, extensive ambient ground measurements, and state-of-the-art modeling to constrain the concentration of organic aerosol from biogenic monoterpenes and sesquiterpenes. Further, we show that the organic aerosol from the investigated sources accounts for roughly 20 % of the World Health Organization PM2.5 standard in the southeastern US.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Kathleen M. Fahey, Annmarie G. Carlton, Havala O. T. Pye, Jaemeen Baek, William T. Hutzell, Charles O. Stanier, Kirk R. Baker, K. Wyat Appel, Mohammed Jaoui, and John H. Offenberg
Geosci. Model Dev., 10, 1587–1605, https://doi.org/10.5194/gmd-10-1587-2017, https://doi.org/10.5194/gmd-10-1587-2017, 2017
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Chemical transport models (CTMs) are a crucial tool in understanding links between emissions, air quality, and climate. Only a simple description of cloud chemistry has been implemented in many of these; however, clouds play a major role in the physicochemical processing of atmospheric species. In CMAQ, EPA’s widely used CTM, the cloud code is limited to the treatment of simple chemistry. We update CMAQ clouds to consider additional chemistry and then examine regional impacts of these updates.
Shantanu H. Jathar, Matthew Woody, Havala O. T. Pye, Kirk R. Baker, and Allen L. Robinson
Atmos. Chem. Phys., 17, 4305–4318, https://doi.org/10.5194/acp-17-4305-2017, https://doi.org/10.5194/acp-17-4305-2017, 2017
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Mobile sources such as cars and trucks are large sources of pollution in cities, but it is unclear what their relative contribution to organic particle pollution is. We used a numerical model along with recent data gathered from tests performed on cars and trucks to calculate organic particle levels in southern California. We found that model calculations agreed better with measurements and gasoline cars and trucks dominated the organic particle pollution.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Matthew C. Woody, Kirk R. Baker, Patrick L. Hayes, Jose L. Jimenez, Bonyoung Koo, and Havala O. T. Pye
Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, https://doi.org/10.5194/acp-16-4081-2016, 2016
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In this work, organic aerosol (OA) predictions from the volatility basis set (VBS) module in the CMAQ photochemical transport model were evaluated against routine monitoring data and measurements collected during the 2010 CalNex field study. We found that the VBS module more accurately reproduced the observed primary/secondary OA split and secondary OA (SOA) mass at the CalNex Pasadena ground site compared to the traditional CMAQ OA module but still underpredicted observed SOA by ~ 5.2 ×.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
B. H. Henderson, F. Akhtar, H. O. T. Pye, S. L. Napelenok, and W. T. Hutzell
Geosci. Model Dev., 7, 339–360, https://doi.org/10.5194/gmd-7-339-2014, https://doi.org/10.5194/gmd-7-339-2014, 2014
K. W. Appel, G. A. Pouliot, H. Simon, G. Sarwar, H. O. T. Pye, S. L. Napelenok, F. Akhtar, and S. J. Roselle
Geosci. Model Dev., 6, 883–899, https://doi.org/10.5194/gmd-6-883-2013, https://doi.org/10.5194/gmd-6-883-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Understanding the mechanism and importance of brown carbon bleaching across the visible spectrum in biomass burning plumes from the WE-CAN campaign
Influence of terrestrial and marine air mass on the constituents and intermixing of bioaerosols over a coastal atmosphere
A multi-site passive approach to studying the emissions and evolution of smoke from prescribed fires
The annual cycle and sources of relevant aerosol precursor vapors in the central Arctic during the MOSAiC expedition
Opinion: How will advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution?
Measurement report: Intra-annual variability of black carbon and brown carbon and their interrelation with meteorological conditions over Gangtok, Sikkim
Long-range transport of air pollutants increases the concentration of hazardous components of PM2.5 in northern South America
Dominant influence of biomass combustion and cross-border transport on nitrogen-containing organic compound levels in the southeastern Tibetan Plateau
Impacts of elevated anthropogenic emissions on physicochemical characteristics of black-carbon-containing particles over the Tibetan Plateau
Online characterization of primary and secondary emissions of particulate matter and acidic molecules from a modern fleet of city buses
Atmospheric evolution of environmentally persistent free radicals in the rural North China Plain: effects on water solubility and PM2.5 oxidative potential
Two distinct ship emission profiles for organic-sulfate source apportionment of PM in sulfur emission control areas
Automated compound speciation, cluster analysis, and quantification of organic vapors and aerosols using comprehensive two-dimensional gas chromatography and mass spectrometry
Measurement report: Occurrence of aminiums in PM2.5 during winter in China – aminium outbreak during polluted episodes and potential constraints
Bridging gas and aerosol properties between the northeastern US and Bermuda: analysis of eight transit flights
The behaviour of charged particles (ions) during new particle formation events in urban Leipzig, Germany
Exploring the sources of light-absorbing carbonaceous aerosols by integrating observational and modeling results: insights from Northeast China
Measurement report: Characteristics of airborne black-carbon-containing particles during the 2021 summer COVID-19 lockdown in a typical Yangtze River Delta city, China
Aerosol optical properties within the atmospheric boundary layer predicted from ground-based observations compared to Raman lidar retrievals during RITA-2021
Hygroscopic growth and activation changed submicron aerosol composition and properties in the North China Plain
Measurement report: Formation of tropospheric brown carbon in a lifting air mass
Vertical variability of aerosol properties and trace gases over a remote marine region: a case study over Bermuda
Differences in aerosol and cloud properties along the central California coast when winds change from northerly to southerly
International airport emissions and their impact on local air quality: chemical speciation of ambient aerosols at Madrid–Barajas Airport during the AVIATOR campaign
Significant role of biomass burning in heavy haze formation in a megacity: Molecular-level insights from intensive PM2.5 sampling on winter hazy days
The local ship speed reduction effect on black carbon emissions measured at a remote marine station
High-altitude aerosol chemical characterization and source identification: insights from the CALISHTO campaign
Measurement report: Impact of emission control measures on environmental persistent free radicals and reactive oxygen species – a short-term case study in Beijing
Characterizing water solubility of fresh and aged secondary organic aerosol in PM2.5 with the stable carbon isotope technique
Measurement report: Impact of cloud processes on secondary organic aerosols at a forested mountain site in southeastern China
Critical contribution of chemically diverse carbonyl molecules to the oxidative potential of atmospheric aerosols
Seasonal Investigation of Ultrafine Particle Composition in an Eastern Amazonian Rainforest
Measurement report: Vanadium-containing ship exhaust particles detected in and above the marine boundary layer in the remote atmosphere
Technical note: Quantified organic aerosol subsaturated hygroscopicity by a simple optical scatter monitor system through field measurements
Diverse sources and aging change the mixing state and ice nucleation properties of aerosol particles over the western Pacific and Southern Ocean
The water-insoluble organic carbon in PM2.5 of typical Chinese urban areas: light-absorbing properties, potential sources, radiative forcing effects, and a possible light-absorbing continuum
Measurement report: Size-resolved secondary organic aerosol formation modulated by aerosol water uptake in wintertime haze
In situ measurement of organic aerosol molecular markers in urban Hong Kong during a summer period: temporal variations and source apportionment
Technical note: Determining chemical composition of atmospheric single particles by a standard-free mass calibration algorithm
Different formation pathways of nitrogen-containing organic compounds in aerosols and fog water in northern China
Impact of weather patterns and meteorological factors on PM2.5 and O3 responses to the COVID-19 lockdown in China
Daytime and nighttime aerosol soluble iron formation in clean and slightly polluted moist air in a coastal city in eastern China
Non-negligible secondary contribution to brown carbon in autumn and winter: inspiration from particulate nitrated and oxygenated aromatic compounds in urban Beijing
Non-sea-salt aerosols that contain trace bromine and iodine are widespread in the remote troposphere
Simultaneous organic aerosol source apportionment at two Antarctic sites reveals large-scale and ecoregion-specific components
Measurement report: Optical characterization, seasonality, and sources of brown carbon in fine aerosols from Tianjin, North China: year-round observations
High-resolution analyses of concentrations and sizes of black carbon particles deposited on northwest Greenland over the past 350 years – Part 2: Seasonal and temporal trends in black carbon originated from fossil fuel combustion and biomass burning
Bayesian inference-based estimation of hourly primary and secondary organic carbon in suburban Hong Kong: multi-temporal-scale variations and evolution characteristics during PM2.5 episodes
Formation and chemical evolution of SOA in two different environments: A dual chamber study
Enhanced daytime secondary aerosol formation driven by gas-particle partitioning in downwind urban plumes
Yingjie Shen, Rudra P. Pokhrel, Amy P. Sullivan, Ezra J. T. Levin, Lauren A. Garofalo, Delphine K. Farmer, Wade Permar, Lu Hu, Darin W. Toohey, Teresa Campos, Emily V. Fischer, and Shane M. Murphy
Atmos. Chem. Phys., 24, 12881–12901, https://doi.org/10.5194/acp-24-12881-2024, https://doi.org/10.5194/acp-24-12881-2024, 2024
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The magnitude and evolution of brown carbon (BrC) absorption remain unclear, with uncertainty in climate models. Data from the WE-CAN airborne experiment show that model parameterizations overestimate the mass absorption cross section (MAC) of BrC. Observed decreases in BrC absorption with chemical markers are due to decreasing organic aerosol (OA) mass rather than a decreasing BrC MAC, which is currently implemented in models. Water-soluble BrC contributes 23 % of total absorption at 660 nm.
Qun He, Zhaowen Wang, Houfeng Liu, Pengju Xu, Rongbao Duan, Caihong Xu, Jianmin Chen, and Min Wei
Atmos. Chem. Phys., 24, 12775–12792, https://doi.org/10.5194/acp-24-12775-2024, https://doi.org/10.5194/acp-24-12775-2024, 2024
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Coastal environments provide an ideal setting for investigating the intermixing of terrestrial and marine aerosols. Terrestrial air mass constituted a larger number of microbes from anthropogenic and soil emissions, whereas saprophytic and gut microbes were predominant in marine samples. Mixed air masses indicated a fusion of marine and terrestrial aerosols, characterized by alterations in the ratio of pathogenic and saprophytic microbes when compared to either terrestrial or marine samples.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O'Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
Atmos. Chem. Phys., 24, 12749–12773, https://doi.org/10.5194/acp-24-12749-2024, https://doi.org/10.5194/acp-24-12749-2024, 2024
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Prescribed burning is an important method for managing ecosystems and preventing wildfires. However, smoke from prescribed fires can have a significant impact on air quality. Here, using a network of fixed sites and sampling throughout an extended prescribed burning period in 2 different years, we characterize emissions and evolutions of up to 8 h of PM2.5 mass, black carbon (BC), and brown carbon (BrC) in smoke from burning of forested lands in the southeastern USA.
Matthew Boyer, Diego Aliaga, Lauriane L. J. Quéléver, Silvia Bucci, Hélène Angot, Lubna Dada, Benjamin Heutte, Lisa Beck, Marina Duetsch, Andreas Stohl, Ivo Beck, Tiia Laurila, Nina Sarnela, Roseline C. Thakur, Branka Miljevic, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 24, 12595–12621, https://doi.org/10.5194/acp-24-12595-2024, https://doi.org/10.5194/acp-24-12595-2024, 2024
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We analyze the seasonal cycle and sources of gases that are relevant for the formation of aerosol particles in the central Arctic. Since theses gases can form new particles, they can influence Arctic climate. We show that the sources of these gases are associated with changes in the Arctic environment during the year, especially with respect to sea ice. Therefore, the concentration of these gases will likely change in the future as the Arctic continues to warm.
Imad El Haddad, Danielle Vienneau, Kaspar R. Daellenbach, Robin Modini, Jay G. Slowik, Abhishek Upadhyay, Petros N. Vasilakos, David Bell, Kees de Hoogh, and Andre S. H. Prevot
Atmos. Chem. Phys., 24, 11981–12011, https://doi.org/10.5194/acp-24-11981-2024, https://doi.org/10.5194/acp-24-11981-2024, 2024
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This opinion paper explores how advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution. We advocate for a shift in the way we target PM pollution, focusing on the most harmful anthropogenic emissions. We highlight key observations, modelling developments, and emission measurements needed to achieve this shift.
Pramod Kumar, Khushboo Sharma, Ankita Malu, Rajeev Rajak, Aparna Gupta, Bidyutjyoti Baruah, Shailesh Yadav, Thupstan Angchuk, Jayant Sharma, Rakesh Kumar Ranjan, Anil Kumar Misra, and Nishchal Wanjari
Atmos. Chem. Phys., 24, 11585–11601, https://doi.org/10.5194/acp-24-11585-2024, https://doi.org/10.5194/acp-24-11585-2024, 2024
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This work monitors and assesses air pollution, especially black and brown carbon, its controlling factor, and its effect on the environment of Sikkim Himalayan region. The huge urban sprawl in recent decades has led to regional human-induced air pollution in the region. Black carbon was highest in April 2021 and March 2022, exceeding the WHO limit. The monsoon season causes huge rainfall over the region, which reduces the pollutants by scavenging (rainout and washout).
Maria P. Velásquez-García, K. Santiago Hernández, James A. Vergara-Correa, Richard J. Pope, Miriam Gómez-Marín, and Angela M. Rendón
Atmos. Chem. Phys., 24, 11497–11520, https://doi.org/10.5194/acp-24-11497-2024, https://doi.org/10.5194/acp-24-11497-2024, 2024
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In the Aburrá Valley, northern South America, local emissions determine air quality conditions. However, we found that external sources, such as regional fires, Saharan dust, and volcanic emissions, increase particulate concentrations and worsen chemical composition by introducing elements like heavy metals. Dry winds and source variability contribute to seasonal influences on these events. This study assesses the air quality risks posed by such events, which can affect broad regions worldwide.
Meng Wang, Qiyuan Wang, Steven Sai Hang Ho, Jie Tian, Yong Zhang, Shun-cheng Lee, and Junji Cao
Atmos. Chem. Phys., 24, 11175–11189, https://doi.org/10.5194/acp-24-11175-2024, https://doi.org/10.5194/acp-24-11175-2024, 2024
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We studied nitrogen-containing organic compounds (NOCs) in particulate matter <2.5 µm particles on the southeastern Tibetan Plateau. We found that biomass burning and transboundary transport are the main sources of NOCs in the high-altitude area. Understanding these aerosol sources informs how they add to regional and potentially global climate changes. Our findings could help shape effective environmental policies to enhance air quality and address climate impacts in this sensitive region.
Jinbo Wang, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Xuguang Chi, Xin Huang, Dafeng Ge, Shiyi Lai, Caijun Zhu, Lei Wang, Qiaozhi Zha, Ximeng Qi, Wei Nie, Congbin Fu, and Aijun Ding
Atmos. Chem. Phys., 24, 11063–11080, https://doi.org/10.5194/acp-24-11063-2024, https://doi.org/10.5194/acp-24-11063-2024, 2024
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In this study, we found large spatial discrepancies in the physical and chemical properties of black carbon over the Tibetan Plateau (TP). Elevated anthropogenic emissions from low-altitude regions can significantly change the mass concentration, mixing state and chemical composition of black-carbon-containing aerosol in the TP region, further altering its light absorption ability. Our study emphasizes the vulnerability of remote plateau regions to intense anthropogenic influences.
Liyuan Zhou, Qianyun Liu, Christian M. Salvador, Michael Le Breton, Mattias Hallquist, Jian Zhen Yu, Chak K. Chan, and Åsa M. Hallquist
Atmos. Chem. Phys., 24, 11045–11061, https://doi.org/10.5194/acp-24-11045-2024, https://doi.org/10.5194/acp-24-11045-2024, 2024
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Our research on city bus emissions reveals that alternative fuels (compressed natural gas and biofuels) reduce fresh particle emissions compared to diesel. However, all fuels lead to secondary air pollution. Aiming at guiding better environmental policies, we studied 76 buses using advanced emission measurement techniques. This work sheds light on the complex effects of bus fuels on urban air quality, emphasizing the need for comprehensive evaluations of future transportation technologies.
Xu Yang, Fobang Liu, Shuqi Yang, Yuling Yang, Yanan Wang, Jingjing Li, Mingyu Zhao, Zhao Wang, Kai Wang, Chi He, and Haijie Tong
Atmos. Chem. Phys., 24, 11029–11043, https://doi.org/10.5194/acp-24-11029-2024, https://doi.org/10.5194/acp-24-11029-2024, 2024
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A study in the rural North China Plain showed environmentally persistent free radicals (EPFRs) in atmospheric particulate matter (PM), with a notable water-soluble fraction likely from atmospheric oxidation during transport. Significant positive correlations between EPFRs and the water-soluble oxidative potential of PM2.5 were found, primarily attributable to the water-soluble fractions of EPFRs. These findings emphasize understanding EPFRs' atmospheric evolution for climate and health impacts.
Kirsten N. Fossum, Chunshui Lin, Niall O'Sullivan, Lu Lei, Stig Hellebust, Darius Ceburnis, Aqeel Afzal, Anja Tremper, David Green, Srishti Jain, Steigvilė Byčenkienė, Colin O'Dowd, John Wenger, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 24, 10815–10831, https://doi.org/10.5194/acp-24-10815-2024, https://doi.org/10.5194/acp-24-10815-2024, 2024
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The chemical composition and sources of submicron aerosol in the Dublin Port area were investigated over a month-long campaign. Two distinct types of ship emissions were identified and characterised: sulfate-rich plumes from the use of heavy fuel oil with scrubbers and organic-rich plumes from the use of low-sulfur fuels. The latter were more frequent, emitting double the particle number and having a typical V / Ni ratio for ship emission.
Xiao He, Xuan Zheng, Shuwen Guo, Lewei Zeng, Ting Chen, Bohan Yang, Shupei Xiao, Qiongqiong Wang, Zhiyuan Li, Yan You, Shaojun Zhang, and Ye Wu
Atmos. Chem. Phys., 24, 10655–10666, https://doi.org/10.5194/acp-24-10655-2024, https://doi.org/10.5194/acp-24-10655-2024, 2024
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This study introduces an innovative method for identifying and quantifying complex organic vapors and aerosols. By combining advanced analytical techniques and new algorithms, we categorized thousands of compounds from heavy-duty diesel vehicles and ambient air and highlighted specific tracers for emission sources. The innovative approach enhances peak identification, reduces quantification uncertainties, and offers new insights for air quality management and atmospheric chemistry.
Yu Xu, Tang Liu, Yi-Jia Ma, Qi-Bin Sun, Hong-Wei Xiao, Hao Xiao, Hua-Yun Xiao, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 10531–10542, https://doi.org/10.5194/acp-24-10531-2024, https://doi.org/10.5194/acp-24-10531-2024, 2024
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This study investigates the characteristics of aminiums and ammonium in PM2.5 on clean and polluted winter days in 11 Chinese cities, highlighting the possibility of the competitive uptake of ammonia versus amines on acidic aerosols or the displacement of aminiums by ammonia under high-ammonia conditions. The overall results deepen the understanding of the spatiotemporal differences in aminium characteristics and formation in China.
Cassidy Soloff, Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Francesca Gallo, Johnathan W. Hair, Miguel Ricardo A. Hilario, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 10385–10408, https://doi.org/10.5194/acp-24-10385-2024, https://doi.org/10.5194/acp-24-10385-2024, 2024
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Using aircraft measurements over the northwestern Atlantic between the US East Coast and Bermuda and trajectory modeling of continental outflow, we identify trace gas and particle properties that exhibit gradients with offshore distance and quantify these changes with high-resolution measurements of concentrations and particle chemistry, size, and scattering properties. This work furthers our understanding of the complex interactions between continental and marine environments.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Avinash Kumar, Matti Rissanen, Miikka Dal Maso, Peter Mettke, Kay Weinhold, Maik Merkel, and Roy M. Harrison
Atmos. Chem. Phys., 24, 10349–10361, https://doi.org/10.5194/acp-24-10349-2024, https://doi.org/10.5194/acp-24-10349-2024, 2024
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Ions enhance the formation and growth rates of new particles, affecting the Earth's radiation budget. Despite these effects, there is little published data exploring the sources of ions in the urban environment and their role in new particle formation (NPF). Here we show that natural ion sources dominate in urban environments, while traffic is a secondary source. Ions contribute up to 12.7 % of the formation rate of particles, indicating that they are important for forming urban PM.
Yuan Cheng, Xu-bing Cao, Sheng-qiang Zhu, Zhi-qing Zhang, Jiu-meng Liu, Hong-liang Zhang, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 24, 9869–9883, https://doi.org/10.5194/acp-24-9869-2024, https://doi.org/10.5194/acp-24-9869-2024, 2024
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The agreement between observational and modeling results is essential for the development of efficient air pollution control strategies. Here we constrained the modeling results of carbonaceous aerosols by field observation in Northeast China, a historically overlooked but recently targeted region of national clean-air actions. Our study suggested that the simulation of agricultural fire emissions and secondary organic aerosols remains challenging.
Yuan Dai, Junfeng Wang, Houjun Wang, Shijie Cui, Yunjiang Zhang, Haiwei Li, Yun Wu, Ming Wang, Eleonora Aruffo, and Xinlei Ge
Atmos. Chem. Phys., 24, 9733–9748, https://doi.org/10.5194/acp-24-9733-2024, https://doi.org/10.5194/acp-24-9733-2024, 2024
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Short-term strict emission control can improve air quality, but its effectiveness needs assessment. During the 2021 summer COVID-19 lockdown in Yangzhou, we found that PM2.5 levels did not decrease despite reduced primary emissions. Aged black-carbon particles increased substantially due to higher O3 levels and transported pollutants. High humidity and low wind also played key roles. The results highlight the importance of a regionally balanced control strategy for future air quality management.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 9597–9614, https://doi.org/10.5194/acp-24-9597-2024, https://doi.org/10.5194/acp-24-9597-2024, 2024
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The vertical distribution of aerosol optical properties is important for their effect on climate. This is usually measured by lidar, which has limitations, most notably the assumption of a lidar ratio. Our study shows that routine surface-level aerosol measurements are able to predict this lidar ratio reasonably well within the lower layers of the atmosphere and thus provide a relatively simple and cost-effective method to improve lidar measurements.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
Atmos. Chem. Phys., 24, 9387–9399, https://doi.org/10.5194/acp-24-9387-2024, https://doi.org/10.5194/acp-24-9387-2024, 2024
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We deployed an advanced aerosol–fog sampling system at a rural site in the North China Plain to investigate impacts of aerosol hygroscopic growth and activation on the physicochemical properties of submicron aerosols. Observed results highlighted remarkably different aqueous processing of primary and secondary submicron aerosol components under distinct ambient relative humidity (RH) conditions and that RH levels significantly impact aerosol sampling through the aerosol swelling effect.
Can Wu, Xiaodi Liu, Ke Zhang, Si Zhang, Cong Cao, Jianjun Li, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 9263–9275, https://doi.org/10.5194/acp-24-9263-2024, https://doi.org/10.5194/acp-24-9263-2024, 2024
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Brown carbon (BrC) is prevalent in the troposphere and can efficiently absorb solar and terrestrial radiation. Our observations show that the enhanced light absorption of BrC relative to black carbon at the tropopause can be attributed to the formation of nitrogen-containing organic compounds through the aqueous-phase reactions of carbonyls with ammonium.
Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Johnathan W. Hair, Miguel Ricardo A. Hilario, Chris A. Hostetler, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Cassidy Soloff, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9197–9218, https://doi.org/10.5194/acp-24-9197-2024, https://doi.org/10.5194/acp-24-9197-2024, 2024
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This study uses airborne data to examine vertical profiles of trace gases, aerosol particles, and meteorological variables over a remote marine area (Bermuda). Results show distinct differences based on both air mass source region (North America, Ocean, Caribbean/North Africa) and altitude for a given air mass type. This work highlights the sensitivity of remote marine areas to long-range transport and the importance of considering the vertical dependence of trace gas and aerosol properties.
Kira Zeider, Grace Betito, Anthony Bucholtz, Peng Xian, Annette Walker, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9059–9083, https://doi.org/10.5194/acp-24-9059-2024, https://doi.org/10.5194/acp-24-9059-2024, 2024
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The predominant wind direction along the California coast (northerly) reverses several times during the summer (to southerly). The effects of these wind reversals on aerosol and cloud characteristics are not well understood. Using data from multiple datasets we found that southerly flow periods had enhanced signatures of anthropogenic emissions due to shipping and continental sources, and clouds had more but smaller droplets.
Saleh Alzahrani, Doğuşhan Kılıç, Michael Flynn, Paul I. Williams, and James Allan
Atmos. Chem. Phys., 24, 9045–9058, https://doi.org/10.5194/acp-24-9045-2024, https://doi.org/10.5194/acp-24-9045-2024, 2024
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This paper investigates emissions from aviation activities at an international airport to evaluate their impact on local air quality. The study provides detailed insights into the chemical composition of aerosols and key pollutants in the airport environment. Source apportionment analysis using positive matrix factorisation (PMF) identified three significant sources: less oxidised oxygenated organic aerosol, alkane organic aerosol, and more oxidised oxygenated organic aerosol.
Mingjie Kang, Mengying Bao, Wenhuai Song, Aduburexiati Abulimiti, Fang Cao, Sönke Szidat, and Yanlin Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2098, https://doi.org/10.5194/egusphere-2024-2098, 2024
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Reports on the molecular level knowledge of high temporal resolution PM2.5 components on hazy days are still limited. This study investigated many individual PM2.5 species and sources. The results show biomass burning (BB) was the main source of organic carbon. Moreover, BB enhanced fungal spore emissions and secondary aerosol formation. The contribution of non-fossils increased with increasing haze pollution. These findings suggest BB may be an important driver of haze events in winter.
Mikko Heikkilä, Krista Luoma, Timo Mäkelä, and Tiia Grönholm
Atmos. Chem. Phys., 24, 8927–8941, https://doi.org/10.5194/acp-24-8927-2024, https://doi.org/10.5194/acp-24-8927-2024, 2024
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Black carbon (BC) concentration was measured from 211 ship exhaust gas plumes at a remote marine station. Emission factors of BC were calculated in grams per kilogram of fuel. Ships with an exhaust gas cleaning system (EGCS) were found to have median BC emissions per fuel consumed 5 times lower than ships without an EGCS. However, this might be because of non-EGCS ships running at low engine loads rather than the EGCS itself. A local speed restriction would increase BC emissions of ships.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Yuanyuan Qin, Xinghua Zhang, Wei Huang, Juanjuan Qin, Xiaoyu Hu, Yuxuan Cao, Tianyi Zhao, Yang Zhang, Jihua Tan, Ziyin Zhang, Xinming Wang, and Zhenzhen Wang
Atmos. Chem. Phys., 24, 8737–8750, https://doi.org/10.5194/acp-24-8737-2024, https://doi.org/10.5194/acp-24-8737-2024, 2024
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Environmental persistent free radicals (EPFRs) and reactive oxygen species (ROSs) play an active role in the atmosphere. Despite control measures having effectively reduced their emissions, reductions were less than in PM2.5. Emission control measures performed well in achieving Parade Blue, but reducing the impact of the atmosphere on human health remains challenging. Thus, there is a need to reassess emission control measures to better address the challenges posed by EPFRs and ROSs.
Fenghua Wei, Xing Peng, Liming Cao, Mengxue Tang, Ning Feng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 24, 8507–8518, https://doi.org/10.5194/acp-24-8507-2024, https://doi.org/10.5194/acp-24-8507-2024, 2024
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The water solubility of secondary organic aerosols (SOAs) is a crucial factor in determining their hygroscopicity and climatic impact. Stable carbon isotope and mass spectrometry techniques were combined to assess the water solubility of SOAs with different aging degrees in a coastal megacity in China. This work revealed a much higher water-soluble fraction of aged SOA compared to fresh SOA, indicating that the aging degree of SOA has considerable impacts on its water solubility.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
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We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Feifei Li, Shanshan Tang, Jitao Lv, Shiyang Yu, Xu Sun, Dong Cao, Yawei Wang, and Guibin Jiang
Atmos. Chem. Phys., 24, 8397–8411, https://doi.org/10.5194/acp-24-8397-2024, https://doi.org/10.5194/acp-24-8397-2024, 2024
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Targeted derivatization and non-targeted analysis with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) were used to reveal the molecular composition of carbonyl molecules in PM2.5, and the important role of carbonyls in increasing the oxidative potential of organic aerosol was found in real samples.
Adam E. Thomas, Hayley S. Glicker, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
EGUsphere, https://doi.org/10.5194/egusphere-2024-2230, https://doi.org/10.5194/egusphere-2024-2230, 2024
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We present measurements of the composition of ultrafine particles collected from the eastern Amazon, a relatively understudied region that is subjected to increasing human influence. We find that while isoprene chemistry is likely significant to ultrafine particle growth throughout the year, compounds related to other sources such as biological spore emissions and biomass burning exhibit striking seasonal differences, implying an extensive variation in regional ultrafine particle sources.
Maya Abou-Ghanem, Daniel M. Murphy, Gregory P. Schill, Michael J. Lawler, and Karl D. Froyd
Atmos. Chem. Phys., 24, 8263–8275, https://doi.org/10.5194/acp-24-8263-2024, https://doi.org/10.5194/acp-24-8263-2024, 2024
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Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust particles measured on NASA's DC-8 during the Atmospheric Tomography Mission (ATom). Our results reveal ship exhaust particles are sufficiently widespread in the marine atmosphere and experience atmospheric aging. Finally, we use laboratory calibrations to determine the vanadium, sulfate, and organic single-particle mass fractions of vanadium-containing ship exhaust particles.
Jie Zhang, Tianyu Zhu, Alexandra Catena, Yaowei Li, Margaret Schwab, Pengfei Liu, Akua Asa-Awuku, and James Schwab
EGUsphere, https://doi.org/10.5194/egusphere-2024-1390, https://doi.org/10.5194/egusphere-2024-1390, 2024
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This study shows the derived organic aerosol hygroscopicity under high humidity conditions based on a simple optical scatter monitor system, including two nephelometric monitors (pDR-1500), after knowing the aerosol chemical composition.
Jiao Xue, Tian Zhang, Keyhong Park, Jinpei Yan, Young Jun Yoon, Jiyeon Park, and Bingbing Wang
Atmos. Chem. Phys., 24, 7731–7754, https://doi.org/10.5194/acp-24-7731-2024, https://doi.org/10.5194/acp-24-7731-2024, 2024
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Ice formation by particles is an important way of making mixed-phase and ice clouds. We found that particles collected in the marine atmosphere exhibit diverse ice nucleation abilities and mixing states. Sea salt mixed-sulfate particles were enriched in ice-nucleating particles. Selective aging on sea salt particles made particle populations more externally mixed. Characterizations of particles and their mixing state are needed for a better understanding of aerosol–cloud interactions.
Yangzhi Mo, Jun Li, Guangcai Zhong, Sanyuan Zhu, Shizhen Zhao, Jiao Tang, Hongxing Jiang, Zhineng Cheng, Chongguo Tian, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 24, 7755–7772, https://doi.org/10.5194/acp-24-7755-2024, https://doi.org/10.5194/acp-24-7755-2024, 2024
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In this study, we found that biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of water-insoluble organic carbon in China, with coal combustion sources exhibiting the strongest light-absorbing capacity. Additionally, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to have stronger light-absorbing capacity, higher aromaticity, higher molecular weights, and greater recalcitrance in the atmosphere.
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, and Colin O'Dowd
Atmos. Chem. Phys., 24, 7687–7698, https://doi.org/10.5194/acp-24-7687-2024, https://doi.org/10.5194/acp-24-7687-2024, 2024
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The chemical composition of atmospheric particles has shown significant changes in recent years. We investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, secondary organic aerosol formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, northwestern China. We highlight the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
Hongyong Li, Xiaopu Lyu, Likun Xue, Yunxi Huo, Dawen Yao, Haoxian Lu, and Hai Guo
Atmos. Chem. Phys., 24, 7085–7100, https://doi.org/10.5194/acp-24-7085-2024, https://doi.org/10.5194/acp-24-7085-2024, 2024
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Organic aerosol is ubiquitous in the atmosphere and largely explains the gap between current levels of fine particulate matter in many cities and the World Health Organization guideline values. This study highlights the dominant contributions of cooking emissions to organic aerosol when marine air prevailed in Hong Kong, which were occasionally overwhelmed by aromatics-derived secondary organic aerosol in continental ouflows.
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Atmos. Chem. Phys., 24, 7001–7012, https://doi.org/10.5194/acp-24-7001-2024, https://doi.org/10.5194/acp-24-7001-2024, 2024
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The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~ 0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.
Wei Sun, Xiaodong Hu, Yuzhen Fu, Guohua Zhang, Yujiao Zhu, Xinfeng Wang, Caiqing Yan, Likun Xue, He Meng, Bin Jiang, Yuhong Liao, Xinming Wang, Ping'an Peng, and Xinhui Bi
Atmos. Chem. Phys., 24, 6987–6999, https://doi.org/10.5194/acp-24-6987-2024, https://doi.org/10.5194/acp-24-6987-2024, 2024
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The formation pathways of nitrogen-containing compounds (NOCs) in the atmosphere remain unclear. We investigated the composition of aerosols and fog water by state-of-the-art mass spectrometry and compared the formation pathways of NOCs. We found that NOCs in aerosols were mainly formed through nitration reaction, while ammonia addition played a more important role in fog water. The results deepen our understanding of the processes of organic particulate pollution.
Fuzhen Shen, Michaela I. Hegglin, and Yue Yuan
Atmos. Chem. Phys., 24, 6539–6553, https://doi.org/10.5194/acp-24-6539-2024, https://doi.org/10.5194/acp-24-6539-2024, 2024
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We attempt to use a novel structural self-organising map and machine learning models to identify a weather system and quantify the importance of each meteorological factor in driving the unexpected PM2.5 and O3 changes under the specific weather system during the COVID-19 lockdown in China. The result highlights that temperature under the double-centre high-pressure system plays the most crucial role in abnormal events.
Wenshuai Li, Yuxuan Qi, Yingchen Liu, Guanru Wu, Yanjing Zhang, Jinhui Shi, Wenjun Qu, Lifang Sheng, Wencai Wang, Daizhou Zhang, and Yang Zhou
Atmos. Chem. Phys., 24, 6495–6508, https://doi.org/10.5194/acp-24-6495-2024, https://doi.org/10.5194/acp-24-6495-2024, 2024
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Aerosol particles from mainland can transport to oceans and deposit, providing soluble Fe and affecting phytoplankton growth. Thus, we studied the dissolution process of aerosol Fe and found that photochemistry played a key role in promoting Fe dissolution in clean conditions. RH-dependent reactions were more influential in slightly polluted conditions. These results highlight the distinct roles of two weather-related parameters (radiation and RH) in influencing geochemical cycles related to Fe.
Yanqin Ren, Zhenhai Wu, Yuanyuan Ji, Fang Bi, Junling Li, Haijie Zhang, Hao Zhang, Hong Li, and Gehui Wang
Atmos. Chem. Phys., 24, 6525–6538, https://doi.org/10.5194/acp-24-6525-2024, https://doi.org/10.5194/acp-24-6525-2024, 2024
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Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) in PM2.5 were examined from an urban area in Beijing during the autumn and winter. The OPAH and NAC concentrations were much higher during heating than before heating. They majorly originated from the combustion of biomass and automobile emissions, and the secondary generation was the major contributor throughout the whole sampling period.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
EGUsphere, https://doi.org/10.5194/egusphere-2024-1399, https://doi.org/10.5194/egusphere-2024-1399, 2024
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol, and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
Atmos. Chem. Phys., 24, 6305–6322, https://doi.org/10.5194/acp-24-6305-2024, https://doi.org/10.5194/acp-24-6305-2024, 2024
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Applying factor analysis techniques to H-NMR spectra, we present the organic aerosol (OA) source apportionment of PM1 samples collected in parallel at two Antarctic stations, namely Signy and Halley, allowing investigation of aerosol–climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open-ocean) and sympagic (sea-ice-influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Zhichao Dong, Chandra Mouli Pavuluri, Peisen Li, Zhanjie Xu, Junjun Deng, Xueyan Zhao, Xiaomai Zhao, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 5887–5905, https://doi.org/10.5194/acp-24-5887-2024, https://doi.org/10.5194/acp-24-5887-2024, 2024
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Comprehensive study of optical properties of brown carbon (BrC) in fine aerosols from Tianjin, China, implied that biological emissions are major sources of BrC in summer, whereas fossil fuel combustion and biomass burning emissions are in cold periods. The direct radiation absorption caused by BrC in short wavelengths contributed about 40 % to that caused by BrC in 300–700 nm. Water-insoluble but methanol-soluble BrC contains more protein-like chromophores (PLOM) than that of water-soluble BrC.
Kumiko Goto-Azuma, Yoshimi Ogawa-Tsukagawa, Kaori Fukuda, Koji Fujita, Motohiro Hirabayashi, Remi Dallmayr, Jun Ogata, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Sumito Matoba, and Teruo Aoki
EGUsphere, https://doi.org/10.5194/egusphere-2024-1498, https://doi.org/10.5194/egusphere-2024-1498, 2024
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Monthly records spanning 350 years from a Greenland ice core reveal trends in black carbon (BC) concentrations and sizes. BC concentrations have risen since the late 19th century due to the inflow of anthropogenic BC, with these particles being larger than those from biomass burning (BB). High BB BC concentration peaks in summer originating from BB could reduce albedo. However, BB BC showed no upward trend until the early 2000s. Our findings are crucial for validating aerosol and climate models.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 5803–5821, https://doi.org/10.5194/acp-24-5803-2024, https://doi.org/10.5194/acp-24-5803-2024, 2024
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In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal-scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Andreas Aktypis, Dontavious Sippial, Christina Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1317, https://doi.org/10.5194/egusphere-2024-1317, 2024
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A dual chamber system was deployed in two different environments (Po Valley, Italy and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary aerosol. In the Po Valley, the system reacts rapidly forming large amounts of SOA, while in Pertouli the corresponding SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Mingfu Cai, Chenshuo Ye, Bin Yuan, Shan Huang, E Zheng, Suxia Yang, Zelong Wang, Yi Lin, Tiange Li, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Baolin Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
EGUsphere, https://doi.org/10.5194/egusphere-2024-887, https://doi.org/10.5194/egusphere-2024-887, 2024
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This study investigated the daytime secondary organic aerosol (SOA) formation in urban plumes. We observed a significant daytime SOA formation through gas-particle partitioning when the site was affected by urban plumes. Box model simulation indicated that urban pollutants (nitrogen oxide and volatile organic compounds) could enhance the oxidizing capacity, while the elevated volatile organic compounds were mainly responsible for promoting daytime SOA formation.
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Short summary
To understand how changing emissions have impacted aerosols in remote regions, we measured nitrate and sulfate in Barbados and compared them to model predictions from EPA’s Air QUAlity TimE Series (EQUATES). Nitrate was stable, except for spikes in 2008 and 2010 due to transported smoke. Sulfate decreased in the 1990s due to reductions in sulfur dioxide (SO2) in the US and Europe; then it increased in the 2000s, likely due to anthropogenic emissions from Africa.
To understand how changing emissions have impacted aerosols in remote regions, we measured...
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