Articles | Volume 17, issue 19
https://doi.org/10.5194/acp-17-11779-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-11779-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
05 Oct 2017
Research article |
| 05 Oct 2017
CCN activity and organic hygroscopicity of aerosols downwind of an urban region in central Amazonia: seasonal and diel variations and impact of anthropogenic emissions
Ryan Thalman
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
now at: Department of Chemistry, Snow College, Richfield, UT,
USA
Suzane S. de Sá
School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA, USA
Brett B. Palm
Department of Chemistry and Biochemistry and Cooperative
Institute for Research in Environmental Sciences (CIRES), University
of Colorado Boulder, Boulder, CO, USA
Henrique M. J. Barbosa
Physics Institute, University of São Paulo, São
Paulo, Brazil
Mira L. Pöhlker
Biogeochemistry and Multiphase Chemistry
Departments, Max Planck Institute for Chemistry, Mainz, Germany
M. Lizabeth Alexander
Pacific Northwest National Laboratory, Richland, WA, USA
Joel Brito
Physics Institute, University of São Paulo, São
Paulo, Brazil
now at: Laboratory for Meteorological Physics, Université
Clermont Auvergne, Clermont-Ferrand, France
Samara Carbone
Physics Institute, University of São Paulo, São
Paulo, Brazil
Paulo Castillo
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
Douglas A. Day
Department of Chemistry and Biochemistry and Cooperative
Institute for Research in Environmental Sciences (CIRES), University
of Colorado Boulder, Boulder, CO, USA
Chongai Kuang
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
Antonio Manzi
National Institute of Amazonian Research, Manaus, Amazonas,
Brazil
Nga Lee Ng
School of Chemical and Biomolecular Engineering, Georgia
Institute of Technology, Atlanta, GA, USA
School of Earth and Atmospheric Sciences, Georgia Institute
of Technology, Atlanta, GA, USA
Arthur J. Sedlacek III
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
Rodrigo Souza
Amazonas State University, Manaus, Amazonas, Brazil
Stephen Springston
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
Thomas Watson
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
Christopher Pöhlker
Biogeochemistry and Multiphase Chemistry
Departments, Max Planck Institute for Chemistry, Mainz, Germany
Ulrich Pöschl
Biogeochemistry and Multiphase Chemistry
Departments, Max Planck Institute for Chemistry, Mainz, Germany
Meinrat O. Andreae
Biogeochemistry and Multiphase Chemistry
Departments, Max Planck Institute for Chemistry, Mainz, Germany
Scripps Institution of Oceanography, University of
California San Diego, La Jolla, CA, USA
Paulo Artaxo
Physics Institute, University of São Paulo, São
Paulo, Brazil
Jose L. Jimenez
Department of Chemistry and Biochemistry and Cooperative
Institute for Research in Environmental Sciences (CIRES), University
of Colorado Boulder, Boulder, CO, USA
Scot T. Martin
School of Engineering and Applied Sciences, Harvard
University, Cambridge, MA, USA
Department of Earth and Planetary Sciences, Harvard
University, Cambridge, MA, USA
Environmental and Climate Sciences Department, Brookhaven
National Laboratory, Upton, NY, USA
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Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
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Tianle Pan, Andrew T. Lambe, Weiwei Hu, Yicong He, Minghao Hu, Huaishan Zhou, Xinming Wang, Qingqing Hu, Hui Chen, Yue Zhao, Yuanlong Huang, Doug R. Worsnop, Zhe Peng, Melissa A. Morris, Douglas A. Day, Pedro Campuzano-Jost, Jose-Luis Jimenez, and Shantanu H. Jathar
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Ludovico Di Antonio, Claudia Di Biagio, Paola Formenti, Aline Gratien, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Patrice Coll, Barbara D'Anna, Joel F. de Brito, David O. De Haan, Juliette R. Dignum, Shravan Deshmukh, Olivier Favez, Pierre-Marie Flaud, Cecile Gaimoz, Lelia N. Hawkins, Julien Kammer, Brigitte Language, Franck Maisonneuve, Griša Močnik, Emilie Perraudin, Jean-Eudes Petit, Prodip Acharja, Laurent Poulain, Pauline Pouyes, Eva Drew Pronovost, Véronique Riffault, Kanuri I. Roundtree, Marwa Shahin, Guillaume Siour, Eric Villenave, Pascal Zapf, Gilles Foret, Jean-François Doussin, and Matthias Beekmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2299, https://doi.org/10.5194/egusphere-2024-2299, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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The spectral complex refractive index (CRI) and single scattering albedo were retrieved from submicron aerosol measurements at three sites within the greater Paris area during the ACROSS field campaign (June–July 2022). Measurements revealed the urban emission impact on the surrounding areas. The CRI full period averages at 520 nm were 1.41–0.037i (urban), 1.52–0.038i (peri-urban), 1.50−0.025i (rural). Organic aerosols dominated the aerosol mass and contributed up to 22% of absorption at 370 nm.
Luiz A. T. Machado, Jürgen Kesselmeier, Santiago Botía, Hella van Asperen, Meinrat O. Andreae, Alessandro C. de Araújo, Paulo Artaxo, Achim Edtbauer, Rosaria R. Ferreira, Marco A. Franco, Hartwig Harder, Sam P. Jones, Cléo Q. Dias-Júnior, Guido G. Haytzmann, Carlos A. Quesada, Shujiro Komiya, Jost Lavric, Jos Lelieveld, Ingeborg Levin, Anke Nölscher, Eva Pfannerstill, Mira L. Pöhlker, Ulrich Pöschl, Akima Ringsdorf, Luciana Rizzo, Ana M. Yáñez-Serrano, Susan Trumbore, Wanda I. D. Valenti, Jordi Vila-Guerau de Arellano, David Walter, Jonathan Williams, Stefan Wolff, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 8893–8910, https://doi.org/10.5194/acp-24-8893-2024, https://doi.org/10.5194/acp-24-8893-2024, 2024
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Manfred Wendisch, Susanne Crewell, André Ehrlich, Andreas Herber, Benjamin Kirbus, Christof Lüpkes, Mario Mech, Steven J. Abel, Elisa F. Akansu, Felix Ament, Clémantyne Aubry, Sebastian Becker, Stephan Borrmann, Heiko Bozem, Marlen Brückner, Hans-Christian Clemen, Sandro Dahlke, Georgios Dekoutsidis, Julien Delanoë, Elena De La Torre Castro, Henning Dorff, Regis Dupuy, Oliver Eppers, Florian Ewald, Geet George, Irina V. Gorodetskaya, Sarah Grawe, Silke Groß, Jörg Hartmann, Silvia Henning, Lutz Hirsch, Evelyn Jäkel, Philipp Joppe, Olivier Jourdan, Zsofia Jurányi, Michail Karalis, Mona Kellermann, Marcus Klingebiel, Michael Lonardi, Johannes Lucke, Anna E. Luebke, Maximilian Maahn, Nina Maherndl, Marion Maturilli, Bernhard Mayer, Johanna Mayer, Stephan Mertes, Janosch Michaelis, Michel Michalkov, Guillaume Mioche, Manuel Moser, Hanno Müller, Roel Neggers, Davide Ori, Daria Paul, Fiona M. Paulus, Christian Pilz, Felix Pithan, Mira Pöhlker, Veronika Pörtge, Maximilian Ringel, Nils Risse, Gregory C. Roberts, Sophie Rosenburg, Johannes Röttenbacher, Janna Rückert, Michael Schäfer, Jonas Schaefer, Vera Schemann, Imke Schirmacher, Jörg Schmidt, Sebastian Schmidt, Johannes Schneider, Sabrina Schnitt, Anja Schwarz, Holger Siebert, Harald Sodemann, Tim Sperzel, Gunnar Spreen, Bjorn Stevens, Frank Stratmann, Gunilla Svensson, Christian Tatzelt, Thomas Tuch, Timo Vihma, Christiane Voigt, Lea Volkmer, Andreas Walbröl, Anna Weber, Birgit Wehner, Bruno Wetzel, Martin Wirth, and Tobias Zinner
Atmos. Chem. Phys., 24, 8865–8892, https://doi.org/10.5194/acp-24-8865-2024, https://doi.org/10.5194/acp-24-8865-2024, 2024
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Atmos. Chem. Phys., 24, 8821–8846, https://doi.org/10.5194/acp-24-8821-2024, https://doi.org/10.5194/acp-24-8821-2024, 2024
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Through the use of our machine-learning-based optical model, realistic BC morphologies can be incorporated into atmospheric science applications that require highly accurate results with minimal computational resources. The results of the study demonstrate that the predictions of single-scattering albedo (ω) and mass absorption cross-section (MAC) were improved over the conventional Mie-based predictions when using the machine learning method.
Olivia G. Norman, Colette L. Heald, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
EGUsphere, https://doi.org/10.5194/egusphere-2024-2296, https://doi.org/10.5194/egusphere-2024-2296, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Marco A. Franco, Rafael Valiati, Bruna A. Holanda, Bruno B. Meller, Leslie A. Kremper, Luciana V. Rizzo, Samara Carbone, Fernando G. Morais, Janaína P. Nascimento, Meinrat O. Andreae, Micael A. Cecchini, Luiz A. T. Machado, Milena Ponczek, Ulrich Pöschl, David Walter, Christopher Pöhlker, and Paulo Artaxo
Atmos. Chem. Phys., 24, 8751–8770, https://doi.org/10.5194/acp-24-8751-2024, https://doi.org/10.5194/acp-24-8751-2024, 2024
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The Amazon wet-season atmosphere was studied at the Amazon Tall Tower Observatory site, revealing vertical variations (between 60 and 325 m) in natural aerosols. Daytime mixing contrasted with nighttime stratification, with distinct rain-induced changes in aerosol populations. Notably, optical property recovery at higher levels was faster, while near-canopy aerosols showed higher scattering efficiency. These findings enhance our understanding of aerosol impacts on climate dynamics.
McKenna Stanford, Ann Fridlind, Andrew Ackerman, Bastiaan van Diedenhoven, Qian Xiao, Jian Wang, Toshihisa Matsui, Daniel Hernandez-Deckers, and Paul Lawson
EGUsphere, https://doi.org/10.5194/egusphere-2024-2413, https://doi.org/10.5194/egusphere-2024-2413, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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The evolution of cloud droplets, from the point they are activated by atmospheric aerosol to the formation of precipitation, is an important process relevant to understanding cloud-climate feedbacks. This study demonstrates a benchmark framework for using novel airborne measurements and retrievals to constrain high-resolution simulations of moderately deep cumulus clouds and pathways for scaling results to large-scale models and space-based observational platforms.
Leandro Alex Moreira Viscardi, Giuseppe Torri, David K. Adams, and Henrique de Melo Jorge Barbosa
Atmos. Chem. Phys., 24, 8529–8548, https://doi.org/10.5194/acp-24-8529-2024, https://doi.org/10.5194/acp-24-8529-2024, 2024
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We evaluate the environmental conditions that control how clouds grow from fair weather cumulus into severe thunderstorms during the Amazonian wet season. Days with rain clouds begin with more moisture in the air and have strong convergence in the afternoon, while precipitation intensity increases with large-scale vertical velocity, moisture, and low-level wind. These results contribute to understanding how clouds form over the rainforest.
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
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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.
Delaney B. Kilgour, Christopher M. Jernigan, Olga Garmash, Sneha Aggarwal, Claudia Mohr, Matt E. Salter, Joel A. Thornton, Jian Wang, Paul Zieger, and Timothy H. Bertram
EGUsphere, https://doi.org/10.5194/egusphere-2024-1975, https://doi.org/10.5194/egusphere-2024-1975, 2024
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We report simultaneous measurements of dimethyl sulfide (DMS) and hydroperoxymethyl thioformate (HPMTF) in the Eastern North Atlantic. We use an observationally constrained box model to show cloud loss is the dominant sink of HPMTF in this region over six weeks, resulting in large reductions in DMS-derived products that contribute to aerosol formation and growth. Our findings indicate that fast cloud processing of HPMTF must be included in global models to accurately capture the sulfur cycle.
Fan Mei, Jennifer M. Comstock, Mikhail S. Pekour, Jerome D. Fast, Beat Schmid, Krista L. Gaustad, Shuaiqi Tang, Damao Zhang, John E. Shilling, Jason Tomlinson, Adam C. Varble, Jian Wang, L. Ruby Leung, Lawrence Kleinman, Scot Martin, Sebastien C. Biraud, Brian D. Ermold, and Kenneth W. Burk
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-97, https://doi.org/10.5194/essd-2024-97, 2024
Preprint under review for ESSD
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Our study explores a rich dataset from the final decade of the U.S. DOE's Gulfstream-1 (G-1) aircraft operations (2013-2018). The 236 flights cover diverse regions, including the Arctic, U.S. Southern Great Plains, U.S. West Coast, Eastern North Atlantic, Amazon Basin in Brazil, and Sierras de Córdoba range in Argentina. This airborne dataset offers unprecedented insights into atmospheric dynamics, aerosols, and clouds with a more accessible data format.
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.
Wendell W. Walters, Masayuki Takeuchi, Nga L. Ng, and Meredith G. Hastings
Geosci. Model Dev., 17, 4673–4687, https://doi.org/10.5194/gmd-17-4673-2024, https://doi.org/10.5194/gmd-17-4673-2024, 2024
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The study introduces a novel chemical mechanism for explicitly tracking oxygen isotope transfer in oxidized reactive nitrogen and odd oxygen using the Regional Atmospheric Chemistry Mechanism, version 2. This model enhances our ability to simulate and compare oxygen isotope compositions of reactive nitrogen, revealing insights into oxidation chemistry. The approach shows promise for improving atmospheric chemistry models and tropospheric oxidation capacity predictions.
Amie Dobracki, Ernie Lewis, Arthur Sedlacek III, Tyler Tatro, Maria Zawadowicz, and Paquita Zuidema
EGUsphere, https://doi.org/10.5194/egusphere-2024-1347, https://doi.org/10.5194/egusphere-2024-1347, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Biomass-burning aerosol is commonly present in the marine boundary layer of the southeast Atlantic Ocean between June and October. Our research indicates that burning conditions, aerosol transport pathways, and prolonged oxidation processes, both heterogeneous and aqueous-phase determine the chemical, microphysical, and optical properties of the boundary layer aerosol. Notably, we find that the aerosol optical properties can be estimated from the chemical properties alone.
Diego Aliaga, Victoria A. Sinclair, Radovan Krejci, Marcos Andrade, Paulo Artaxo, Luis Blacutt, Runlong Cai, Samara Carbone, Yvette Gramlich, Liine Heikkinen, Dominic Heslin-Rees, Wei Huang, Veli-Matti Kerminen, Alkuin Maximilian Koenig, Markku Kulmala, Paolo Laj, Valeria Mardoñez-Balderrama, Claudia Mohr, Isabel Moreno, Pauli Paasonen, Wiebke Scholz, Karine Sellegri, Laura Ticona, Gaëlle Uzu, Fernando Velarde, Alfred Wiedensohler, Doug Worsnop, Cheng Wu, Chen Xuemeng, Qiaozhi Zha, and Federico Bianchi
Aerosol Research Discuss., https://doi.org/10.5194/ar-2024-15, https://doi.org/10.5194/ar-2024-15, 2024
Preprint under review for AR
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This study examines new particle formation (NPF) in the Bolivian Andes at Chacaltaya mountain (CHC) and the urban El Alto-La Paz area (EAC). Days are clustered into four categories based on NPF intensity. Differences in particle size, precursor gases, and pollution levels are found. High NPF intensities increased Aitken mode particle concentrations at both sites, while volcanic influence selectively diminished NPF intensity at CHC but not EAC. This study highlights NPF dynamics in the Andes.
Alejandra Velazquez-Garcia, Joel F. de Brito, Suzanne Crumeyrolle, Isabelle Chiapello, and Véronique Riffault
Aerosol Research, 2, 107–122, https://doi.org/10.5194/ar-2-107-2024, https://doi.org/10.5194/ar-2-107-2024, 2024
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Multi-annual in situ observations were combined with back trajectory and emissions inventories to study black and brown carbon (BC, BrC) sources in the north of France. Results show BC to be mainly originated from vehicular traffic (31 %), shipping (25 %), and residential heating (21 %). Also, a significant decrease of the BrC component from residential heating is observed after 24 h of atmospheric aging. These results should lead to better climate and air pollution mitigation strategies.
Jerome D. Fast, Adam C. Varble, Fan Mei, Mikhail Pekour, Jason Tomlinson, Alla Zelenyuk, Art J. Sedlacek III, Maria Zawadowicz, and Louisa K. Emmons
EGUsphere, https://doi.org/10.5194/egusphere-2024-1349, https://doi.org/10.5194/egusphere-2024-1349, 2024
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Aerosol property measurements recently collected at the ground and by a research aircraft in central Argentina during the CACTI campaign exhibit large spatial and temporal variability. These measurements coupled with coincident meteorological information provide a valuable dataset needed to evaluate and improve model predictions of aerosols in a traditionally data sparse region of South America.
Melinda K. Schueneman, Douglas A. Day, Dongwook Kim, Pedro Campuzano-Jost, Seonsik Yun, Marla P. DeVault, Anna C. Ziola, Paul J. Ziemann, and Jose L. Jimenez
Aerosol Research, 2, 59–76, https://doi.org/10.5194/ar-2-59-2024, https://doi.org/10.5194/ar-2-59-2024, 2024
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Our study presents a novel method for quantifying mass spectrometer responses to molecular species in organic aerosols. Traditional calibrations often fail for complex mixtures like secondary organic aerosol. We combined chromatography with statistical component analysis to improve separation and quantification, achieving promising agreement with direct calibration. Our findings offer a new approach to assess aerosol composition, especially beneficial for complex mixtures.
Hasna Chebaicheb, Joel F. de Brito, Tanguy Amodeo, Florian Couvidat, Jean-Eudes Petit, Emmanuel Tison, Gregory Abbou, Alexia Baudic, Mélodie Chatain, Benjamin Chazeau, Nicolas Marchand, Raphaele Falhun, Florie Francony, Cyril Ratier, Didier Grenier, Romain Vidaud, Shouwen Zhang, Gregory Gille, Laurent Meunier, Caroline Marchand, Véronique Riffault, and Olivier Favez
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-80, https://doi.org/10.5194/essd-2024-80, 2024
Revised manuscript accepted for ESSD
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Long-term (2015–2021) quasi-continuous measurements have been obtained at 13 French urban sites using online mass spectrometry, to acquire comprehensive chemical composition of submicron particulate matter. The results show their spatial and temporal differences and confirm the predominance of organics in France (40–60 %). These measurements can be used for many future studies such as trend and epidemiological analyses, or comparisons with chemical transport models.
Florian Wieland, Nadine Bothen, Ralph Schwidetzky, Teresa M. Seifried, Paul Bieber, Ulrich Pöschl, Konrad Meister, Mischa Bonn, Janine Fröhlich-Nowoisky, and Hinrich Grothe
EGUsphere, https://doi.org/10.5194/egusphere-2024-752, https://doi.org/10.5194/egusphere-2024-752, 2024
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Betula pendula is a widespread birch tree species containing ice nucleation agents that can trigger the freezing of cloud droplets, and thereby alter the evolution of clouds. Our study identifies three distinct ice-nucleating macromolecules (INMs) and aggregates of varying size that can nucleate ice at temperatures of up to -5.4 °C. Our findings suggest that these vegetation-derived particles may influence atmospheric processes, weather, and climate stronger than previously thought.
Kouji Adachi, Jack E. Dibb, Joseph M. Katich, Joshua P. Schwarz, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Jeff Peischl, Christopher D. Holmes, and James Crawford
EGUsphere, https://doi.org/10.5194/egusphere-2024-880, https://doi.org/10.5194/egusphere-2024-880, 2024
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We examined aerosol particles from wildfires and identified tarballs (TBs) during the FIREX-AQ campaign. This study revealed the compositions, abundance, sizes, and mixing states of TBs and showed that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass burning and ages and enhances the knowledge of TB emissions and our understanding of their climate impact.
Gabriela R. Unfer, Luiz A. T. Machado, Paulo Artaxo, Marco A. Franco, Leslie A. Kremper, Mira L. Pöhlker, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 24, 3869–3882, https://doi.org/10.5194/acp-24-3869-2024, https://doi.org/10.5194/acp-24-3869-2024, 2024
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Amazonian aerosols and their interactions with precipitation were studied by understanding them in a 3D space based on three parameters that characterize the concentration and size distribution of aerosols. The results showed characteristic arrangements regarding seasonal and diurnal cycles, as well as when interacting with precipitation. The use of this 3D space appears to be a promising tool for aerosol population analysis and for model validation and parameterization.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Andrea Cuesta-Mosquera, Kristina Glojek, Griša Močnik, Luka Drinovec, Asta Gregorič, Martin Rigler, Matej Ogrin, Baseerat Romshoo, Kay Weinhold, Maik Merkel, Dominik van Pinxteren, Hartmut Herrmann, Alfred Wiedensohler, Mira Pöhlker, and Thomas Müller
Atmos. Chem. Phys., 24, 2583–2605, https://doi.org/10.5194/acp-24-2583-2024, https://doi.org/10.5194/acp-24-2583-2024, 2024
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This study evaluated the air pollution and climate impacts of residential-wood-burning particle emissions from a rural European site. The authors investigate the optical and physical properties that connect the aerosol emissions with climate by evaluating atmospheric radiative impacts via simple-forcing calculations. The study contributes to reducing the lack of information on the understanding of the optical properties of air pollution from anthropogenic sources.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen Arnold, Leighton Regayre, Meinrat Andreae, Mira Pöhlker, Duseong Jo, Man Yue, and Ken Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-401, https://doi.org/10.5194/egusphere-2024-401, 2024
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Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model. The updated model shows better agreement with measurements of nucleation rate, growth rate, NPF event frequency. Our results reveal that HOMs-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
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This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
EGUsphere, https://doi.org/10.5194/egusphere-2023-2937, https://doi.org/10.5194/egusphere-2023-2937, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to assess ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the behaviour of ozone in the tropics, except in Southeast Asia. Results demonstrate that UKESM1 can be used for health assessments and highlights areas that would benefit from further observations.
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.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Yang Wang, Chanakya Bagya Ramesh, Scott E. Giangrande, Jerome Fast, Xianda Gong, Jiaoshi Zhang, Ahmet Tolga Odabasi, Marcus Vinicius Batista Oliveira, Alyssa Matthews, Fan Mei, John E. Shilling, Jason Tomlinson, Die Wang, and Jian Wang
Atmos. Chem. Phys., 23, 15671–15691, https://doi.org/10.5194/acp-23-15671-2023, https://doi.org/10.5194/acp-23-15671-2023, 2023
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We report the vertical profiles of aerosol properties over the Southern Great Plains (SGP), a region influenced by shallow convective clouds, land–atmosphere interactions, boundary layer turbulence, and the aerosol life cycle. We examined the processes that drive the aerosol population and distribution in the lower troposphere over the SGP. This study helps improve our understanding of aerosol–cloud interactions and the model representation of aerosol processes.
Sohyeon Jeon, Michael J. Walker, Donna T. Sueper, Douglas A. Day, Anne V. Handschy, Jose L. Jimenez, and Brent J. Williams
Atmos. Meas. Tech., 16, 6075–6095, https://doi.org/10.5194/amt-16-6075-2023, https://doi.org/10.5194/amt-16-6075-2023, 2023
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A searchable database tool for the Aerosol Mass Spectrometer (AMS) and Aerosol Chemical Speciation Monitor (ACSM) mass spectral datasets was built to improve the efficiency of data analysis using Igor Pro. The tool incorporates the published mass spectra (MS) and sample information uploaded on the website. The tool allows users to compare their own mass spectrum with the reference MS in the database.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023, https://doi.org/10.5194/acp-23-13911-2023, 2023
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To better understand smoke properties and its interactions with clouds, we compare the WRF-CAM5 model with observations from ORACLES, CLARIFY, and LASIC field campaigns in the southeastern Atlantic in August 2017. The model transports and mixes smoke well but does not fully capture some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, sulfate particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Yutong Liang, Rebecca A. Wernis, Kasper Kristensen, Nathan M. Kreisberg, Philip L. Croteau, Scott C. Herndon, Arthur W. H. Chan, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12441–12454, https://doi.org/10.5194/acp-23-12441-2023, https://doi.org/10.5194/acp-23-12441-2023, 2023
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We measured the gas–particle partitioning behaviors of biomass burning markers and examined the effect of wildfire organic aerosol on the partitioning of semivolatile organic compounds. Most compounds measured are less volatile than model predictions. Wildfire aerosol enhanced the condensation of polar compounds and caused some nonpolar (e.g., polycyclic aromatic hydrocarbons) compounds to partition into the gas phase, thus affecting their lifetimes in the atmosphere and the mode of exposure.
Jean-Philippe Putaud, Enrico Pisoni, Alexander Mangold, Christoph Hueglin, Jean Sciare, Michael Pikridas, Chrysanthos Savvides, Jakub Ondracek, Saliou Mbengue, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Laurent Poulain, Dominik van Pinxteren, Hartmut Herrmann, Andreas Massling, Claus Nordstroem, Andrés Alastuey, Cristina Reche, Noemí Pérez, Sonia Castillo, Mar Sorribas, Jose Antonio Adame, Tuukka Petaja, Katrianne Lehtipalo, Jarkko Niemi, Véronique Riffault, Joel F. de Brito, Augustin Colette, Olivier Favez, Jean-Eudes Petit, Valérie Gros, Maria I. Gini, Stergios Vratolis, Konstantinos Eleftheriadis, Evangelia Diapouli, Hugo Denier van der Gon, Karl Espen Yttri, and Wenche Aas
Atmos. Chem. Phys., 23, 10145–10161, https://doi.org/10.5194/acp-23-10145-2023, https://doi.org/10.5194/acp-23-10145-2023, 2023
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Many European people are still exposed to levels of air pollution that can affect their health. COVID-19 lockdowns in 2020 were used to assess the impact of the reduction in human mobility on air pollution across Europe by comparing measurement data with values that would be expected if no lockdown had occurred. We show that lockdown measures did not lead to consistent decreases in the concentrations of fine particulate matter suspended in the air, and we investigate why.
Xurong Wang, Qiaoqiao Wang, Maria Prass, Christopher Pöhlker, Daniel Moran-Zuloaga, Paulo Artaxo, Jianwei Gu, Ning Yang, Xiajie Yang, Jiangchuan Tao, Juan Hong, Nan Ma, Yafang Cheng, Hang Su, and Meinrat O. Andreae
Atmos. Chem. Phys., 23, 9993–10014, https://doi.org/10.5194/acp-23-9993-2023, https://doi.org/10.5194/acp-23-9993-2023, 2023
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In this work, with an optimized particle mass size distribution, we captured observed aerosol optical depth (AOD) and coarse aerosol concentrations over source and/or receptor regions well, demonstrating good performance in simulating export of African dust toward the Amazon Basin. In addition to factors controlling the transatlantic transport of African dust, the study investigated the impact of African dust over the Amazon Basin, including the nutrient inputs associated with dust deposition.
Qian Xiao, Jiaoshi Zhang, Yang Wang, Luke D. Ziemba, Ewan Crosbie, Edward L. Winstead, Claire E. Robinson, Joshua P. DiGangi, Glenn S. Diskin, Jeffrey S. Reid, K. Sebastian Schmidt, Armin Sorooshian, Miguel Ricardo A. Hilario, Sarah Woods, Paul Lawson, Snorre A. Stamnes, and Jian Wang
Atmos. Chem. Phys., 23, 9853–9871, https://doi.org/10.5194/acp-23-9853-2023, https://doi.org/10.5194/acp-23-9853-2023, 2023
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Using recent airborne measurements, we show that the influences of anthropogenic emissions, transport, convective clouds, and meteorology lead to new particle formation (NPF) under a variety of conditions and at different altitudes in tropical marine environments. NPF is enhanced by fresh urban emissions in convective outflow but is suppressed in air masses influenced by aged urban emissions where reactive precursors are mostly consumed while particle surface area remains relatively high.
Juan Vicente Pallotta, Silvânia Alves de Carvalho, Fabio Juliano da Silva Lopes, Alexandre Cacheffo, Eduardo Landulfo, and Henrique Melo Jorge Barbosa
Geosci. Instrum. Method. Data Syst., 12, 171–185, https://doi.org/10.5194/gi-12-171-2023, https://doi.org/10.5194/gi-12-171-2023, 2023
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Lidar networks coordinate efforts of different groups, providing guidelines to homogenize retrievals from different instruments. We describe an ongoing effort to develop the Lidar Processing Pipeline (LPP) collaboratively, a collection of tools developed in C/C++ to handle all the steps of a typical lidar analysis. Analysis of simulations and real lidar data showcases the LPP’s features. From this exercise, we draw a roadmap to guide future development, accommodating the needs of our community.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Eliane Gomes Alves, Raoni Aquino Santana, Cléo Quaresma Dias-Júnior, Santiago Botía, Tyeen Taylor, Ana Maria Yáñez-Serrano, Jürgen Kesselmeier, Efstratios Bourtsoukidis, Jonathan Williams, Pedro Ivo Lembo Silveira de Assis, Giordane Martins, Rodrigo de Souza, Sérgio Duvoisin Júnior, Alex Guenther, Dasa Gu, Anywhere Tsokankunku, Matthias Sörgel, Bruce Nelson, Davieliton Pinto, Shujiro Komiya, Diogo Martins Rosa, Bettina Weber, Cybelli Barbosa, Michelle Robin, Kenneth J. Feeley, Alvaro Duque, Viviana Londoño Lemos, Maria Paula Contreras, Alvaro Idarraga, Norberto López, Chad Husby, Brett Jestrow, and Iván Mauricio Cely Toro
Atmos. Chem. Phys., 23, 8149–8168, https://doi.org/10.5194/acp-23-8149-2023, https://doi.org/10.5194/acp-23-8149-2023, 2023
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Isoprene is emitted mainly by plants and can influence atmospheric chemistry and air quality. But, there are uncertainties in model emission estimates and follow-up atmospheric processes. In our study, with long-term observational datasets of isoprene and biological and environmental factors from central Amazonia, we show that isoprene emission estimates could be improved when biological processes were mechanistically incorporated into the model.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Samira Atabakhsh, Laurent Poulain, Gang Chen, Francesco Canonaco, André S. H. Prévôt, Mira Pöhlker, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6963–6988, https://doi.org/10.5194/acp-23-6963-2023, https://doi.org/10.5194/acp-23-6963-2023, 2023
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The study focuses on the aerosol chemical variations found in the rural-background station of Melpitz based on ACSM and MAAP measurements. Source apportionment on both organic aerosol (OA) and black carbon (eBC) was performed, and source seasonality was also linked to air mass trajectories. Overall, three anthropogenic sources were identified in OA and eBC plus two additional aged OA. Our results demonstrate the influence of transported coal-combustion-related OA even during summer time.
Najin Kim, Hang Su, Nan Ma, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 16, 2771–2780, https://doi.org/10.5194/amt-16-2771-2023, https://doi.org/10.5194/amt-16-2771-2023, 2023
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We propose a multiple-charging correction algorithm for a broad-supersaturation scanning cloud condensation nuclei (BS2-CCN) system which can obtain high time-resolution aerosol hygroscopicity and CCN activity. The correction algorithm aims at deriving the activation fraction's true value for each particle size. The meaningful differences between corrected and original κ values (single hygroscopicity parameter) emphasize the correction algorithm's importance for ambient aerosol measurement.
Brent A. McBride, J. Vanderlei Martins, J. Dominik Cieslak, Roberto Fernandez-Borda, Anin Puthukuddy, Xiaoguang Xu, Noah Sienkiewicz, Brian Cairns, and Henrique M. J. Barbosa
EGUsphere, https://doi.org/10.5194/egusphere-2023-865, https://doi.org/10.5194/egusphere-2023-865, 2023
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The Airborne Hyper-Angular Rainbow Polarimeter (AirHARP) is a new Earth-observing instrument that can provide highly accurate measurements of the atmosphere and surface. Using a physics-based calibration technique, we show that AirHARP can achieve high measurement accuracy in lab and field environments and exceed a benchmark accuracy requirement for modern aerosol and cloud climate observations. Our calibration technique makes the HARP design highly attractive for upcoming NASA climate missions.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Amie Dobracki, Paquita Zuidema, Steven G. Howell, Pablo Saide, Steffen Freitag, Allison C. Aiken, Sharon P. Burton, Arthur J. Sedlacek III, Jens Redemann, and Robert Wood
Atmos. Chem. Phys., 23, 4775–4799, https://doi.org/10.5194/acp-23-4775-2023, https://doi.org/10.5194/acp-23-4775-2023, 2023
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Southern Africa produces approximately one-third of the world’s carbon from fires. The thick smoke layer can flow westward, interacting with the southeastern Atlantic cloud deck. The net radiative impact can alter regional circulation patterns, impacting rainfall over Africa. We find that the smoke is highly absorbing of sunlight, mostly because it contains more black carbon than smoke over the Northern Hemisphere.
Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774, https://doi.org/10.5194/acp-23-4763-2023, https://doi.org/10.5194/acp-23-4763-2023, 2023
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We investigate the hygroscopic behavior of levoglucosan and D-glucose nanoparticles using a nano-HTDMA. There is a weak size dependence of the hygroscopic growth factor of levoglucosan and D-glucose with diameters down to 20 nm, while a strong size dependence of the hygroscopic growth factor of D-glucose has been clearly observed in the size range 6 to 20 nm. The use of the DKA method leads to good agreement with the hygroscopic growth factor of glucose nanoparticles with diameters down to 6 nm.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Thomas Berkemeier, Matteo Krüger, Aryeh Feinberg, Marcel Müller, Ulrich Pöschl, and Ulrich K. Krieger
Geosci. Model Dev., 16, 2037–2054, https://doi.org/10.5194/gmd-16-2037-2023, https://doi.org/10.5194/gmd-16-2037-2023, 2023
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Kinetic multi-layer models (KMs) successfully describe heterogeneous and multiphase atmospheric chemistry. In applications requiring repeated execution, however, these models can be too expensive. We trained machine learning surrogate models on output of the model KM-SUB and achieved high correlations. The surrogate models run orders of magnitude faster, which suggests potential applicability in global optimization tasks and as sub-modules in large-scale atmospheric models.
Francesca Gallo, Janek Uin, Kevin J. Sanchez, Richard H. Moore, Jian Wang, Robert Wood, Fan Mei, Connor Flynn, Stephen Springston, Eduardo B. Azevedo, Chongai Kuang, and Allison C. Aiken
Atmos. Chem. Phys., 23, 4221–4246, https://doi.org/10.5194/acp-23-4221-2023, https://doi.org/10.5194/acp-23-4221-2023, 2023
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This study provides a summary statistic of multiday aerosol plume transport event influences on aerosol physical properties and the cloud condensation nuclei budget at the U.S. Department of Energy Atmospheric Radiation Measurement Facility in the eastern North Atlantic (ENA). An algorithm that integrates aerosol properties is developed and applied to identify multiday aerosol transport events. The influence of the aerosol plumes on aerosol populations at the ENA is successively assessed.
Elion Daniel Hack, Theotonio Pauliquevis, Henrique Melo Jorge Barbosa, Marcia Akemi Yamasoe, Dimitri Klebe, and Alexandre Lima Correia
Atmos. Meas. Tech., 16, 1263–1278, https://doi.org/10.5194/amt-16-1263-2023, https://doi.org/10.5194/amt-16-1263-2023, 2023
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Water vapor is a key factor when seeking to understand fast-changing processes when clouds and storms form and develop. We show here how images from a calibrated infrared camera can be used to derive how much water vapor there is in the atmosphere at a given time. Comparing our results to an established technique, for a case of stable atmospheric conditions, we found an agreement within 2.8 %. Water vapor sky maps can be retrieved every few minutes, day or night, under partly cloudy skies.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
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During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
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.
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Suzanne Crumeyrolle, Jenni S. S. Kontkanen, Clémence Rose, Alejandra Velazquez Garcia, Eric Bourrianne, Maxime Catalfamo, Véronique Riffault, Emmanuel Tison, Joel Ferreira de Brito, Nicolas Visez, Nicolas Ferlay, Frédérique Auriol, and Isabelle Chiapello
Atmos. Chem. Phys., 23, 183–201, https://doi.org/10.5194/acp-23-183-2023, https://doi.org/10.5194/acp-23-183-2023, 2023
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Ultrafine particles (UFPs) are particles with an aerodynamic diameter of 100 nm or less and negligible mass concentration but are the dominant contributor to the total particle number concentration. The present study aims to better understand the environmental factors favoring or inhibiting atmospheric new particle formation (NPF) over Lille, a large city in the north of France, and to analyze the impact of such an event on urban air quality using a long-term dataset (3 years).
Yuan Wang, Silvia Henning, Laurent Poulain, Chunsong Lu, Frank Stratmann, Yuying Wang, Shengjie Niu, Mira L. Pöhlker, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 15943–15962, https://doi.org/10.5194/acp-22-15943-2022, https://doi.org/10.5194/acp-22-15943-2022, 2022
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Aerosol particle activation affects cloud, precipitation, radiation, and thus the global climate. Its long-term measurements are important but still scarce. In this study, more than 4 years of measurements at a central European station were analyzed. The overall characteristics and seasonal changes of aerosol particle activation are summarized. The power-law fit between particle hygroscopicity factor and diameter was recommended for predicting cloud
condensation nuclei number concentration.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Baseerat Romshoo, Mira Pöhlker, Alfred Wiedensohler, Sascha Pfeifer, Jorge Saturno, Andreas Nowak, Krzysztof Ciupek, Paul Quincey, Konstantina Vasilatou, Michaela N. Ess, Maria Gini, Konstantinos Eleftheriadis, Chris Robins, François Gaie-Levrel, and Thomas Müller
Atmos. Meas. Tech., 15, 6965–6989, https://doi.org/10.5194/amt-15-6965-2022, https://doi.org/10.5194/amt-15-6965-2022, 2022
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Black carbon (BC) is often assumed to be spherically shaped, causing uncertainties in its optical properties when modelled. This study investigates different modelling techniques for the optical properties of BC by comparing them to laboratory measurements. We provide experimental support for emphasizing the use of appropriate size representation (polydisperse size method) and morphological representation (aggregate morphology) for optical modelling and parameterization scheme development of BC.
Guo Li, Hang Su, Meng Li, Uwe Kuhn, Guangjie Zheng, Lei Han, Fengxia Bao, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 15, 6433–6446, https://doi.org/10.5194/amt-15-6433-2022, https://doi.org/10.5194/amt-15-6433-2022, 2022
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A large fraction of previous work using dynamic flow chambers was to quantify gas exchange in terms of flux or deposition/emission rate. Here, we extended the usage of this technique to examine uptake kinetics on sample surfaces. The good performance of the chamber system was validated. This technique can be further used for liquid samples and real atmospheric aerosol samples without complicated coating procedures, which complements the existing techniques in atmospheric kinetic studies.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
Paul A. Barrett, Steven J. Abel, Hugh Coe, Ian Crawford, Amie Dobracki, James Haywood, Steve Howell, Anthony Jones, Justin Langridge, Greg M. McFarquhar, Graeme J. Nott, Hannah Price, Jens Redemann, Yohei Shinozuka, Kate Szpek, Jonathan W. Taylor, Robert Wood, Huihui Wu, Paquita Zuidema, Stéphane Bauguitte, Ryan Bennett, Keith Bower, Hong Chen, Sabrina Cochrane, Michael Cotterell, Nicholas Davies, David Delene, Connor Flynn, Andrew Freedman, Steffen Freitag, Siddhant Gupta, David Noone, Timothy B. Onasch, James Podolske, Michael R. Poellot, Sebastian Schmidt, Stephen Springston, Arthur J. Sedlacek III, Jamie Trembath, Alan Vance, Maria A. Zawadowicz, and Jianhao Zhang
Atmos. Meas. Tech., 15, 6329–6371, https://doi.org/10.5194/amt-15-6329-2022, https://doi.org/10.5194/amt-15-6329-2022, 2022
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To better understand weather and climate, it is vital to go into the field and collect observations. Often measurements take place in isolation, but here we compared data from two aircraft and one ground-based site. This was done in order to understand how well measurements made on one platform compared to those made on another. Whilst this is easy to do in a controlled laboratory setting, it is more challenging in the real world, and so these comparisons are as valuable as they are rare.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys., 22, 13783–13796, https://doi.org/10.5194/acp-22-13783-2022, https://doi.org/10.5194/acp-22-13783-2022, 2022
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The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types that are internally mixed within individual particles.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Charlotte M. Beall, Thomas C. J. Hill, Paul J. DeMott, Tobias Köneman, Michael Pikridas, Frank Drewnick, Hartwig Harder, Christopher Pöhlker, Jos Lelieveld, Bettina Weber, Minas Iakovides, Roman Prokeš, Jean Sciare, Meinrat O. Andreae, M. Dale Stokes, and Kimberly A. Prather
Atmos. Chem. Phys., 22, 12607–12627, https://doi.org/10.5194/acp-22-12607-2022, https://doi.org/10.5194/acp-22-12607-2022, 2022
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Ice-nucleating particles (INPs) are rare aerosols that can trigger ice formation in clouds and affect climate-relevant cloud properties such as phase, reflectivity and lifetime. Dust is the dominant INP source, yet few measurements have been reported near major dust sources. We report INP observations within hundreds of kilometers of the biggest dust source regions globally: the Sahara and the Arabian Peninsula. Results show that at temperatures > −15 °C, INPs are dominated by organics.
Micael Amore Cecchini, Marco de Bruine, Jordi Vilà-Guerau de Arellano, and Paulo Artaxo
Atmos. Chem. Phys., 22, 11867–11888, https://doi.org/10.5194/acp-22-11867-2022, https://doi.org/10.5194/acp-22-11867-2022, 2022
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Shallow clouds (vertical extent up to 3 km height) are ubiquitous throughout the Amazon and are responsible for redistributing the solar heat and moisture vertically and horizontally. They are a key component of the water cycle because they can grow past the shallow phase to contribute significantly to the precipitation formation. However, they need favourable environmental conditions to grow. In this study, we analyse how changing wind patterns affect the development of such shallow clouds.
Jerome D. Fast, David M. Bell, Gourihar Kulkarni, Jiumeng Liu, Fan Mei, Georges Saliba, John E. Shilling, Kaitlyn Suski, Jason Tomlinson, Jian Wang, Rahul Zaveri, and Alla Zelenyuk
Atmos. Chem. Phys., 22, 11217–11238, https://doi.org/10.5194/acp-22-11217-2022, https://doi.org/10.5194/acp-22-11217-2022, 2022
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Recent aircraft measurements from the HI-SCALE campaign conducted over the Southern Great Plains (SGP) site in Oklahoma are used to quantify spatial variability of aerosol properties in terms of grid spacings typically used by weather and climate models. Surprisingly large horizontal gradients in aerosol properties were frequently observed in this rural area. This spatial variability can be used as an uncertainty range when comparing surface point measurements with model predictions.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219, https://doi.org/10.5194/acp-22-10195-2022, https://doi.org/10.5194/acp-22-10195-2022, 2022
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We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
Deanna C. Myers, Saewung Kim, Steven Sjostedt, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
Atmos. Chem. Phys., 22, 10061–10076, https://doi.org/10.5194/acp-22-10061-2022, https://doi.org/10.5194/acp-22-10061-2022, 2022
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We present the first measurements of gas-phase sulfuric acid from the Amazon basin and evaluate the efficacy of existing sulfuric acid parameterizations in this understudied region. Sulfuric acid is produced during the daytime and nighttime, though current proxies underestimate nighttime production. These results illustrate the need for better parameterizations of sulfuric acid and its precursors that are informed by measurements across a broad range of locations.
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.
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanasios Nenes, Arthur Sedlacek III, Hugh Coe, Jens Redemann, Paquita Zuidema, Steven Howell, and James Haywood
Atmos. Chem. Phys., 22, 9389–9412, https://doi.org/10.5194/acp-22-9389-2022, https://doi.org/10.5194/acp-22-9389-2022, 2022
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Transmission electron microscopy was used to analyze aged African smoke particles and how the smoke interacts with the marine atmosphere. We found that the volatility of organic aerosol increases with biomass burning plume age, that black carbon is often mixed with potassium salts and that the marine atmosphere can incorporate Na and Cl into smoke particles. Marine salts are more processed when mixed with smoke plumes, and there are interesting Cl-rich yet Na-absent marine particles.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Arthur J. Sedlacek III, Ernie R. Lewis, Amie Dobracki, Jenny P. S. Wong, Paola Formenti, Steven G. Howell, and Athanasios Nenes
Atmos. Chem. Phys., 22, 9199–9213, https://doi.org/10.5194/acp-22-9199-2022, https://doi.org/10.5194/acp-22-9199-2022, 2022
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Widespread biomass burning (BB) events occur annually in Africa and contribute ~ 1 / 3 of global BB emissions, which contain a large family of light-absorbing organics, known as brown carbon (BrC), whose absorption of incident radiation is difficult to estimate, leading to large uncertainties in the global radiative forcing estimation. This study quantifies the BrC absorption of aged BB particles and highlights the potential presence of absorbing iron oxides in this climatically important region.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys., 22, 8739–8766, https://doi.org/10.5194/acp-22-8739-2022, https://doi.org/10.5194/acp-22-8739-2022, 2022
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A unique dataset of concentrations and sources of polycyclic aromatic hydrocarbons (PAHs) and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range-transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Haochi Che, Michal Segal-Rozenhaimer, Lu Zhang, Caroline Dang, Paquita Zuidema, Arthur J. Sedlacek III, Xiaoye Zhang, and Connor Flynn
Atmos. Chem. Phys., 22, 8767–8785, https://doi.org/10.5194/acp-22-8767-2022, https://doi.org/10.5194/acp-22-8767-2022, 2022
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A 17-month in situ study on Ascension Island found low single-scattering albedo and strong absorption enhancement of the marine boundary layer aerosols during biomass burnings on the African continent, along with apparent patterns of regular monthly variability. We further discuss the characteristics and drivers behind these changes and find that biomass burning conditions in Africa may be the main factor influencing the optical properties of marine boundary aerosols.
Ovid O. Krüger, Bruna A. Holanda, Sourangsu Chowdhury, Andrea Pozzer, David Walter, Christopher Pöhlker, Maria Dolores Andrés Hernández, John P. Burrows, Christiane Voigt, Jos Lelieveld, Johannes Quaas, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 22, 8683–8699, https://doi.org/10.5194/acp-22-8683-2022, https://doi.org/10.5194/acp-22-8683-2022, 2022
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The abrupt reduction in human activities during the first COVID-19 lockdown created unprecedented atmospheric conditions. We took the opportunity to quantify changes in black carbon (BC) as a major anthropogenic air pollutant. Therefore, we measured BC on board a research aircraft over Europe during the lockdown and compared the results to measurements from 2017. With model simulations we account for different weather conditions and find a lockdown-related decrease in BC of 41 %.
Simon Kirschler, Christiane Voigt, Bruce Anderson, Ramon Campos Braga, Gao Chen, Andrea F. Corral, Ewan Crosbie, Hossein Dadashazar, Richard A. Ferrare, Valerian Hahn, Johannes Hendricks, Stefan Kaufmann, Richard Moore, Mira L. Pöhlker, Claire Robinson, Amy J. Scarino, Dominik Schollmayer, Michael A. Shook, K. Lee Thornhill, Edward Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 22, 8299–8319, https://doi.org/10.5194/acp-22-8299-2022, https://doi.org/10.5194/acp-22-8299-2022, 2022
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In this study we show that the vertical velocity dominantly impacts the cloud droplet number concentration (NC) of low-level clouds over the western North Atlantic in the winter and summer season, while the cloud condensation nuclei concentration, aerosol size distribution and chemical composition impact NC within a season. The observational data presented in this study can evaluate and improve the representation of aerosol–cloud interactions for a wide range of conditions.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Jiaoshi Zhang, Yang Wang, Steven Spielman, Susanne Hering, and Jian Wang
Atmos. Meas. Tech., 15, 2579–2590, https://doi.org/10.5194/amt-15-2579-2022, https://doi.org/10.5194/amt-15-2579-2022, 2022
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New nonparametric, regularized methods are developed to invert the growth factor probability density function (GF-PDF) from humidity-controlled fast integrated mobility spectrometer measurements. These algorithms are computationally efficient, require no prior assumptions of the GF-PDF distribution, and reduce the error in inverted GF-PDF. They can be applied to humidified tandem differential mobility analyzer data. Among all algorithms, Twomey’s method retrieves GF-PDF with the smallest error.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
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Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
Marco A. Franco, Florian Ditas, Leslie A. Kremper, Luiz A. T. Machado, Meinrat O. Andreae, Alessandro Araújo, Henrique M. J. Barbosa, Joel F. de Brito, Samara Carbone, Bruna A. Holanda, Fernando G. Morais, Janaína P. Nascimento, Mira L. Pöhlker, Luciana V. Rizzo, Marta Sá, Jorge Saturno, David Walter, Stefan Wolff, Ulrich Pöschl, Paulo Artaxo, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 3469–3492, https://doi.org/10.5194/acp-22-3469-2022, https://doi.org/10.5194/acp-22-3469-2022, 2022
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In Central Amazonia, new particle formation in the planetary boundary layer is rare. Instead, there is the appearance of sub-50 nm aerosols with diameters larger than about 20 nm that eventually grow to cloud condensation nuclei size range. Here, 254 growth events were characterized which have higher predominance in the wet season. About 70 % of them showed direct relation to convective downdrafts, while 30 % occurred partly under clear-sky conditions, evidencing still unknown particle sources.
Adrien Deroubaix, Laurent Menut, Cyrille Flamant, Peter Knippertz, Andreas H. Fink, Anneke Batenburg, Joel Brito, Cyrielle Denjean, Cheikh Dione, Régis Dupuy, Valerian Hahn, Norbert Kalthoff, Fabienne Lohou, Alfons Schwarzenboeck, Guillaume Siour, Paolo Tuccella, and Christiane Voigt
Atmos. Chem. Phys., 22, 3251–3273, https://doi.org/10.5194/acp-22-3251-2022, https://doi.org/10.5194/acp-22-3251-2022, 2022
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During the summer monsoon in West Africa, pollutants emitted in urbanized areas modify cloud cover and precipitation patterns. We analyze these patterns with the WRF-CHIMERE model, integrating the effects of aerosols on meteorology, based on the numerous observations provided by the Dynamics-Aerosol-Climate-Interactions campaign. This study adds evidence to recent findings that increased pollution levels in West Africa delay the breakup time of low-level clouds and reduce precipitation.
Meinrat O. Andreae, Tracey W. Andreae, Florian Ditas, and Christopher Pöhlker
Atmos. Chem. Phys., 22, 2487–2505, https://doi.org/10.5194/acp-22-2487-2022, https://doi.org/10.5194/acp-22-2487-2022, 2022
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Atmospheric aerosol particles are key players in the Earth’s climate system, but there is still considerable uncertainty about where and how these particles are initially formed. We present the first study of new particle formation (NPF) at a pristine site in a subboreal forest region of North America. Our data suggest that, in this environment, there is frequent NPF from biogenic organic precursor compounds, which was likely the predominant source of particles in the preindustrial environment.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Douglas A. Day, Pedro Campuzano-Jost, Benjamin A. Nault, Brett B. Palm, Weiwei Hu, Hongyu Guo, Paul J. Wooldridge, Ronald C. Cohen, Kenneth S. Docherty, J. Alex Huffman, Suzane S. de Sá, Scot T. Martin, and Jose L. Jimenez
Atmos. Meas. Tech., 15, 459–483, https://doi.org/10.5194/amt-15-459-2022, https://doi.org/10.5194/amt-15-459-2022, 2022
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Particle-phase nitrates are an important component of atmospheric aerosols and chemistry. In this paper, we systematically explore the application of aerosol mass spectrometry (AMS) to quantify the organic and inorganic nitrate fractions of aerosols in the atmosphere. While AMS has been used for a decade to quantify nitrates, methods are not standardized. We make recommendations for a more universal approach based on this analysis of a large range of field and laboratory observations.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Kai Tang, Beatriz Sánchez-Parra, Petya Yordanova, Jörn Wehking, Anna T. Backes, Daniel A. Pickersgill, Stefanie Maier, Jean Sciare, Ulrich Pöschl, Bettina Weber, and Janine Fröhlich-Nowoisky
Biogeosciences, 19, 71–91, https://doi.org/10.5194/bg-19-71-2022, https://doi.org/10.5194/bg-19-71-2022, 2022
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Metagenomic sequencing and freezing experiments of aerosol samples collected on Cyprus revealed rain-related short-term changes of bioaerosol and ice nuclei composition. Filtration experiments showed a rain-related enhancement of biological ice nuclei > 5 µm and < 0.1 µm. The observed effects of rainfall on the composition of atmospheric bioaerosols and ice nuclei may influence the hydrological cycle as well as the health effects of air particulate matter (pathogens, allergens).
Amie Dobracki, Paquita Zuidema, Steve Howell, Pablo Saide, Steffen Freitag, Allison C. Aiken, Sharon P. Burton, Arthur J. Sedlacek III, Jens Redemann, and Robert Wood
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1081, https://doi.org/10.5194/acp-2021-1081, 2022
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The global maximum of shortwave-absorbing aerosol above cloud occurs above the southeast Atlantic, where the biomass-burning aerosol provides a distinct aerosol radiative warming of regional climate. The smoke aerosols are unusually highly absorbing of sunlight. This study seeks to understand the cause. We conclude the aerosol is already strongly absorbing at the fire emission source, but that chemical aging, through encouraging a net loss of organic aerosol, also contributes.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Luiz A. T. Machado, Marco A. Franco, Leslie A. Kremper, Florian Ditas, Meinrat O. Andreae, Paulo Artaxo, Micael A. Cecchini, Bruna A. Holanda, Mira L. Pöhlker, Ivan Saraiva, Stefan Wolff, Ulrich Pöschl, and Christopher Pöhlker
Atmos. Chem. Phys., 21, 18065–18086, https://doi.org/10.5194/acp-21-18065-2021, https://doi.org/10.5194/acp-21-18065-2021, 2021
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Several studies evaluate aerosol–cloud interactions, but only a few attempted to describe how clouds modify aerosol properties. This study evaluates the effect of weather events on the particle size distribution at the ATTO, combining remote sensing and in situ data. Ultrafine, Aitken and accumulation particles modes have different behaviors for the diurnal cycle and for rainfall events. This study opens up new scientific questions that need to be pursued in detail in new field campaigns.
Ramon Campos Braga, Barbara Ervens, Daniel Rosenfeld, Meinrat O. Andreae, Jan-David Förster, Daniel Fütterer, Lianet Hernández Pardo, Bruna A. Holanda, Tina Jurkat-Witschas, Ovid O. Krüger, Oliver Lauer, Luiz A. T. Machado, Christopher Pöhlker, Daniel Sauer, Christiane Voigt, Adrian Walser, Manfred Wendisch, Ulrich Pöschl, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 17513–17528, https://doi.org/10.5194/acp-21-17513-2021, https://doi.org/10.5194/acp-21-17513-2021, 2021
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Interactions of aerosol particles with clouds represent a large uncertainty in estimates of climate change. Properties of aerosol particles control their ability to act as cloud condensation nuclei. Using aerosol measurements in the Amazon, we performed model studies to compare predicted and measured cloud droplet number concentrations at cloud bases. Our results confirm previous estimates of particle hygroscopicity in this region.
Steven G. Howell, Steffen Freitag, Amie Dobracki, Nikolai Smirnow, and Arthur J. Sedlacek III
Atmos. Meas. Tech., 14, 7381–7404, https://doi.org/10.5194/amt-14-7381-2021, https://doi.org/10.5194/amt-14-7381-2021, 2021
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Small particles in the air have important effects on visibility, clouds, and human health. For the ORACLES project we got a new particle sizing instrument that is fast, works over the most important particle sizes, and avoids some of the issues that plague other optical particle sizers. Unfortunately it sees some particles much smaller than they really are, likely because they heat up and evaporate. We show a crude correction and speculate why these particles heat up much more than expected.
Fan Mei, Steven Spielman, Susanne Hering, Jian Wang, Mikhail S. Pekour, Gregory Lewis, Beat Schmid, Jason Tomlinson, and Maynard Havlicek
Atmos. Meas. Tech., 14, 7329–7340, https://doi.org/10.5194/amt-14-7329-2021, https://doi.org/10.5194/amt-14-7329-2021, 2021
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This study focuses on understanding a versatile water-based condensation particle counter (vWCPC 3789) performance under various ambient pressure conditions (500–1000 hPa). A vWCPC has the advantage of avoiding health and safety concerns. However, its performance characterization under low pressure is rare but crucial for ensuring successful airborne deployment. This paper provides advanced knowledge of operating a vWCPC 3789 to capture the spatial variations of atmospheric aerosols.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Diego Aliaga, Victoria A. Sinclair, Marcos Andrade, Paulo Artaxo, Samara Carbone, Evgeny Kadantsev, Paolo Laj, Alfred Wiedensohler, Radovan Krejci, and Federico Bianchi
Atmos. Chem. Phys., 21, 16453–16477, https://doi.org/10.5194/acp-21-16453-2021, https://doi.org/10.5194/acp-21-16453-2021, 2021
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We investigate the origin of air masses sampled at Mount Chacaltaya, Bolivia. Three-quarters of the measured air has not been influenced by the surface in the previous 4 d. However, it is rare that, at any given time, the sampled air has not been influenced at all by the surface, and often the sampled air has multiple origins. The influence of the surface is more prevalent during day than night. Furthermore, during the 6-month study, one-third of the air masses originated from Amazonia.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Najin Kim, Yafang Cheng, Nan Ma, Mira L. Pöhlker, Thomas Klimach, Thomas F. Mentel, Ovid O. Krüger, Ulrich Pöschl, and Hang Su
Atmos. Meas. Tech., 14, 6991–7005, https://doi.org/10.5194/amt-14-6991-2021, https://doi.org/10.5194/amt-14-6991-2021, 2021
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A broad supersaturation scanning CCN (BS2-CCN) system, in which particles are exposed to a range of supersaturation simultaneously, can measure a broad range of CCN activity distribution with a high time resolution. We describe how the BS2-CCN system can be effectively calibrated and which factors can affect the calibration curve. Intercomparison experiments between typical DMA-CCN and BS2-CCN measurements to evaluate the BS2-CCN system showed high correlation and good agreement.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, Mikhail V. Panchenko, and Meinrat O. Andreae
Atmos. Meas. Tech., 14, 6647–6673, https://doi.org/10.5194/amt-14-6647-2021, https://doi.org/10.5194/amt-14-6647-2021, 2021
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The absorption of solar light by organic matter, known as brown carbon (BrC), contributes significantly to the radiative budget of the Earth’s atmosphere, but its representation in atmospheric models is uncertain. This paper advances a methodology to constrain model parameters characterizing BrC absorption of atmospheric aerosol originating from biomass burning with the available remote ground-based observations of atmospheric aerosol.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Rose M. Miller, Greg M. McFarquhar, Robert M. Rauber, Joseph R. O'Brien, Siddhant Gupta, Michal Segal-Rozenhaimer, Amie N. Dobracki, Arthur J. Sedlacek, Sharon P. Burton, Steven G. Howell, Steffen Freitag, and Caroline Dang
Atmos. Chem. Phys., 21, 14815–14831, https://doi.org/10.5194/acp-21-14815-2021, https://doi.org/10.5194/acp-21-14815-2021, 2021
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A large stratocumulus cloud deck resides off the west coast of central Africa. Biomass burning in Africa produces a large plume of aerosol that is carried by the wind over this stratocumulus cloud deck. This paper shows that particles with sizes from 0.01 to 1 mm reside within this plume. Past studies have shown that biomass burning produces such particles, but this is the first study to show that they can be transported westward, over long distances, to the Atlantic stratocumulus cloud deck.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
Ramon Campos Braga, Daniel Rosenfeld, Ovid O. Krüger, Barbara Ervens, Bruna A. Holanda, Manfred Wendisch, Trismono Krisna, Ulrich Pöschl, Meinrat O. Andreae, Christiane Voigt, and Mira L. Pöhlker
Atmos. Chem. Phys., 21, 14079–14088, https://doi.org/10.5194/acp-21-14079-2021, https://doi.org/10.5194/acp-21-14079-2021, 2021
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Quantifying the precipitation within clouds is crucial for our understanding of the Earth's hydrological cycle. Using in situ measurements of cloud and rain properties over the Amazon Basin and Atlantic Ocean, we show here a linear relationship between the effective radius (re) and precipitation water content near the tops of convective clouds for different pollution states and temperature levels. Our results emphasize the role of re to determine both initiation and amount of precipitation.
Maria Prass, Meinrat O. Andreae, Alessandro C. de Araùjo, Paulo Artaxo, Florian Ditas, Wolfgang Elbert, Jan-David Förster, Marco Aurélio Franco, Isabella Hrabe de Angelis, Jürgen Kesselmeier, Thomas Klimach, Leslie Ann Kremper, Eckhard Thines, David Walter, Jens Weber, Bettina Weber, Bernhard M. Fuchs, Ulrich Pöschl, and Christopher Pöhlker
Biogeosciences, 18, 4873–4887, https://doi.org/10.5194/bg-18-4873-2021, https://doi.org/10.5194/bg-18-4873-2021, 2021
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Bioaerosols in the atmosphere over the Amazon rain forest were analyzed by molecular biological staining and microscopy. Eukaryotic, bacterial, and archaeal aerosols were quantified in time series and altitude profiles which exhibited clear differences in number concentrations and vertical distributions. Our results provide insights into the sources and dispersion of different Amazonian bioaerosol types as a basis for a better understanding of biosphere–atmosphere interactions.
Fan Mei, Jian Wang, Shan Zhou, Qi Zhang, Sonya Collier, and Jianzhong Xu
Atmos. Chem. Phys., 21, 13019–13029, https://doi.org/10.5194/acp-21-13019-2021, https://doi.org/10.5194/acp-21-13019-2021, 2021
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This work focuses on understanding aerosol's ability to act as cloud condensation nuclei (CCN) and its variations with organic oxidation level and volatility using measurements at a rural site. Aerosol properties were examined from four air mass sources. The results help improve the accurate representation of aerosol from different ambient aerosol emissions, transformation pathways, and atmospheric processes in a climate model.
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.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
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The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
Jiaoshi Zhang, Steven Spielman, Yang Wang, Guangjie Zheng, Xianda Gong, Susanne Hering, and Jian Wang
Atmos. Meas. Tech., 14, 5625–5635, https://doi.org/10.5194/amt-14-5625-2021, https://doi.org/10.5194/amt-14-5625-2021, 2021
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In this study, we present a newly developed instrument, the humidity-controlled fast integrated mobility spectrometer (HFIMS), for fast measurements of aerosol hygroscopic growth. The HFIMS can measure the distributions of particle hygroscopic growth factors at six diameters from 35 to 265 nm under five RH levels from 20 to 85 % within 25 min. The HFIMS significantly advances our capability of characterizing the hygroscopic growth of atmospheric aerosols over a wide range of relative humidities.
Mira L. Pöhlker, Minghui Zhang, Ramon Campos Braga, Ovid O. Krüger, Ulrich Pöschl, and Barbara Ervens
Atmos. Chem. Phys., 21, 11723–11740, https://doi.org/10.5194/acp-21-11723-2021, https://doi.org/10.5194/acp-21-11723-2021, 2021
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Clouds cool our atmosphere. The role of small aerosol particles in affecting them represents one of the largest uncertainties in current estimates of climate change. Traditionally it is assumed that cloud droplets only form particles of diameters ~ 100 nm (
accumulation mode). Previous studies suggest that this can also occur in smaller particles (
Aitken mode). Our study provides a general framework to estimate under which aerosol and cloud conditions Aitken mode particles affect clouds.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Ryan Thalman and Jaron C. Hansen
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-172, https://doi.org/10.5194/amt-2021-172, 2021
Revised manuscript not accepted
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Sulfur dioxide (SO2) is an important gas precursor for formation of atmospheric sulfate aerosol and acid rain. SO2 has direct human health effects through the respiratory system. A new instrument using Broad Band Cavity Enhanced Absorption Spectroscopy (BBCEAS) for the measurement of SO2 with a minimum limit of detection of 0.6 ppbv has been fabricated. The instrument provides a new technique for the measurement of SO2 over a wide range of atmospherically relevant concentrations.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Stephanie L. Shaw, Eric S. Edgerton, Taekyu Joo, Nga L. Ng, and Ann M. Dillner
Atmos. Meas. Tech., 14, 4355–4374, https://doi.org/10.5194/amt-14-4355-2021, https://doi.org/10.5194/amt-14-4355-2021, 2021
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Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give comprehensive characterization of the organic material by bond rather than species. Using this technique, the concentrations of particle organic material were found to decrease 2011–2016 in the southeastern US, driven by a decline in highly aged material, concurrent with declining anthropogenic emissions. However, an increase was observed in the fraction of more moderately aged organic matter.
Djacinto Monteiro dos Santos, Luciana Varanda Rizzo, Samara Carbone, Patrick Schlag, and Paulo Artaxo
Atmos. Chem. Phys., 21, 8761–8773, https://doi.org/10.5194/acp-21-8761-2021, https://doi.org/10.5194/acp-21-8761-2021, 2021
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The metropolitan area of São Paulo (MASP), with very extensive biofuel use, has unique atmospheric chemistry among world megacities. In this study, we examine the complex relationships between aerosol chemical composition and particle size distribution. Our findings provide a better understanding of the dynamics of the physicochemical properties of submicron particles and highlight the key role of secondary organic aerosol formation in the pollution levels in São Paulo.
Maria A. Zawadowicz, Kaitlyn Suski, Jiumeng Liu, Mikhail Pekour, Jerome Fast, Fan Mei, Arthur J. Sedlacek, Stephen Springston, Yang Wang, Rahul A. Zaveri, Robert Wood, Jian Wang, and John E. Shilling
Atmos. Chem. Phys., 21, 7983–8002, https://doi.org/10.5194/acp-21-7983-2021, https://doi.org/10.5194/acp-21-7983-2021, 2021
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This paper describes the results of a recent field campaign in the eastern North Atlantic, where two mass spectrometers were deployed aboard a research aircraft to measure the chemistry of aerosols and trace gases. Very clean conditions were found, dominated by local sulfate-rich acidic aerosol and very aged organics. Evidence of
long-range transport of aerosols from the continents was also identified.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Dongwook Kim, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 3631–3655, https://doi.org/10.5194/amt-14-3631-2021, https://doi.org/10.5194/amt-14-3631-2021, 2021
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We utilize a set of high-quality datasets collected during the NASA Atmospheric Tomography Mission to investigate the impact of differences in observable particle sizes across aerosol instruments in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of an Aerodyne aerosol mass spectrometer (AMS) when sampling remote aerosols across the globe.
Eugene F. Mikhailov, Mira L. Pöhlker, Kathrin Reinmuth-Selzle, Sergey S. Vlasenko, Ovid O. Krüger, Janine Fröhlich-Nowoisky, Christopher Pöhlker, Olga A. Ivanova, Alexey A. Kiselev, Leslie A. Kremper, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 6999–7022, https://doi.org/10.5194/acp-21-6999-2021, https://doi.org/10.5194/acp-21-6999-2021, 2021
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Subpollen particles are a relatively new subset of atmospheric aerosol particles. When pollen grains rupture, they release cytoplasmic fragments known as subpollen particles (SPPs). We found that SPPs, containing a broad spectrum of biopolymers and hydrocarbons, exhibit abnormally high water uptake. This effect may influence the life cycle of SPPs and the related direct and indirect impacts on radiation budget as well as reinforce their allergic potential.
Robbie Ramsay, Chiara F. Di Marco, Mathew R. Heal, Matthias Sörgel, Paulo Artaxo, Meinrat O. Andreae, and Eiko Nemitz
Biogeosciences, 18, 2809–2825, https://doi.org/10.5194/bg-18-2809-2021, https://doi.org/10.5194/bg-18-2809-2021, 2021
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The exchange of the gas ammonia between the atmosphere and the surface is an important biogeochemical process, but little is known of this exchange for certain ecosystems, such as the Amazon rainforest. This study took measurements of ammonia exchange over an Amazon rainforest site and subsequently modelled the observed deposition and emission patterns. We observed emissions of ammonia from the rainforest, which can be simulated accurately by using a canopy resistance modelling approach.
Anna L. Hodshire, Emily Ramnarine, Ali Akherati, Matthew L. Alvarado, Delphine K. Farmer, Shantanu H. Jathar, Sonia M. Kreidenweis, Chantelle R. Lonsdale, Timothy B. Onasch, Stephen R. Springston, Jian Wang, Yang Wang, Lawrence I. Kleinman, Arthur J. Sedlacek III, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 6839–6855, https://doi.org/10.5194/acp-21-6839-2021, https://doi.org/10.5194/acp-21-6839-2021, 2021
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Biomass burning emits particles and vapors that can impact both health and climate. Here, we investigate the role of dilution in the evolution of aerosol size and composition in observed US wildfire smoke plumes. Centers of plumes dilute more slowly than edges. We see differences in concentrations and composition between the centers and edges both in the first measurement and in subsequent measurements. Our findings support the hypothesis that plume dilution influences smoke aging.
Janaína P. Nascimento, Megan M. Bela, Bruno B. Meller, Alessandro L. Banducci, Luciana V. Rizzo, Angel Liduvino Vara-Vela, Henrique M. J. Barbosa, Helber Gomes, Sameh A. A. Rafee, Marco A. Franco, Samara Carbone, Glauber G. Cirino, Rodrigo A. F. Souza, Stuart A. McKeen, and Paulo Artaxo
Atmos. Chem. Phys., 21, 6755–6779, https://doi.org/10.5194/acp-21-6755-2021, https://doi.org/10.5194/acp-21-6755-2021, 2021
Andrea Cuesta-Mosquera, Griša Močnik, Luka Drinovec, Thomas Müller, Sascha Pfeifer, María Cruz Minguillón, Björn Briel, Paul Buckley, Vadimas Dudoitis, Javier Fernández-García, María Fernández-Amado, Joel Ferreira De Brito, Veronique Riffault, Harald Flentje, Eimear Heffernan, Nikolaos Kalivitis, Athina-Cerise Kalogridis, Hannes Keernik, Luminita Marmureanu, Krista Luoma, Angela Marinoni, Michael Pikridas, Gerhard Schauer, Norbert Serfozo, Henri Servomaa, Gloria Titos, Jesús Yus-Díez, Natalia Zioła, and Alfred Wiedensohler
Atmos. Meas. Tech., 14, 3195–3216, https://doi.org/10.5194/amt-14-3195-2021, https://doi.org/10.5194/amt-14-3195-2021, 2021
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Measurements of black carbon must be conducted with instruments operating in quality-checked and assured conditions to generate reliable and comparable data. Here, 23 Aethalometers monitoring black carbon mass concentrations in European networks were characterized and intercompared. The influence of different aerosol sources, maintenance activities, and the filter material on the instrumental variabilities were investigated. Good agreement and in general low deviations were seen.
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.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys., 21, 6175–6198, https://doi.org/10.5194/acp-21-6175-2021, https://doi.org/10.5194/acp-21-6175-2021, 2021
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This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Miguel Ricardo A. Hilario, Ewan Crosbie, Michael Shook, Jeffrey S. Reid, Maria Obiminda L. Cambaliza, James Bernard B. Simpas, Luke Ziemba, Joshua P. DiGangi, Glenn S. Diskin, Phu Nguyen, F. Joseph Turk, Edward Winstead, Claire E. Robinson, Jian Wang, Jiaoshi Zhang, Yang Wang, Subin Yoon, James Flynn, Sergio L. Alvarez, Ali Behrangi, and Armin Sorooshian
Atmos. Chem. Phys., 21, 3777–3802, https://doi.org/10.5194/acp-21-3777-2021, https://doi.org/10.5194/acp-21-3777-2021, 2021
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This study characterizes long-range transport from major Asian pollution sources into the tropical northwest Pacific and the impact of scavenging on these air masses. We combined aircraft observations, HYSPLIT trajectories, reanalysis, and satellite retrievals to reveal distinct composition and size distribution profiles associated with specific emission sources and wet scavenging. The results of this work have implications for international policymaking related to climate and health.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Zhibo Zhang, Qianqian Song, David B. Mechem, Vincent E. Larson, Jian Wang, Yangang Liu, Mikael K. Witte, Xiquan Dong, and Peng Wu
Atmos. Chem. Phys., 21, 3103–3121, https://doi.org/10.5194/acp-21-3103-2021, https://doi.org/10.5194/acp-21-3103-2021, 2021
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This study investigates the small-scale variations and covariations of cloud microphysical properties, namely, cloud liquid water content and cloud droplet number concentration, in marine boundary layer clouds based on in situ observation from the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We discuss the dependence of cloud variations on vertical location in cloud and the implications for warm-rain simulations in the global climate models.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
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Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Chuchu Chen, Xiaoxiang Wang, Kurt Binder, Mohammad Mehdi Ghahremanpour, David van der Spoel, Ulrich Pöschl, Hang Su, and Yafang Cheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1329, https://doi.org/10.5194/acp-2020-1329, 2021
Publication in ACP not foreseen
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Size dependence of succinic acid solvation in the nanoparticles is investigated based on the molecular dynamics (MD) simulation and energetic analysis. The results show a stronger surface preference and a weaker internal bulk volume solvation of succinic acid in the smaller droplets, which may explain the previously observed size-dependent phase-state of aerosol nanoparticles containing organic molecules, fundamentally promoting a better understanding of atmospheric aerosols.
Guilherme F. Camarinha-Neto, Julia C. P. Cohen, Cléo Q. Dias-Júnior, Matthias Sörgel, José Henrique Cattanio, Alessandro Araújo, Stefan Wolff, Paulo A. F. Kuhn, Rodrigo A. F. Souza, Luciana V. Rizzo, and Paulo Artaxo
Atmos. Chem. Phys., 21, 339–356, https://doi.org/10.5194/acp-21-339-2021, https://doi.org/10.5194/acp-21-339-2021, 2021
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It was observed that friagem phenomena (incursion of cold waves from the high latitudes of the Southern Hemisphere to the Amazon region), very common in the dry season of the Amazon region, produced significant changes in microclimate and atmospheric chemistry. Moreover, the effects of the friagem change the surface O3 and CO2 mixing ratios and therefore interfere deeply in the microclimatic conditions and the chemical composition of the atmosphere above the rainforest.
Igor B. Konovalov, Nikolai A. Golovushkin, Matthias Beekmann, and Meinrat O. Andreae
Atmos. Chem. Phys., 21, 357–392, https://doi.org/10.5194/acp-21-357-2021, https://doi.org/10.5194/acp-21-357-2021, 2021
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A lack of consistent observational constraints on the atmospheric evolution of the optical properties of biomass burning (BB) aerosol limits the accuracy of assessments of the aerosol radiative and climate effects. We show that useful insights into the evolution of the BB aerosol optical properties can be inferred from a combination of satellite observations and 3D modeling. We report major changes that occurred in the optical properties of Siberian BB aerosol during its long-range transport.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
Robert B. Chatfield, Meinrat O. Andreae, ARCTAS Science Team, and SEAC4RS Science Team
Atmos. Meas. Tech., 13, 7069–7096, https://doi.org/10.5194/amt-13-7069-2020, https://doi.org/10.5194/amt-13-7069-2020, 2020
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Forest burning affects air pollution and global climate. A NASA aircraft studied fire emissions including the Rim Fire near Yosemite. We found frequent confusions between the actual fire emission factors and other effects on the air samples. Effects on CO2 and CO can originate far upwind; the gases can mix variably into a smoke plume. We devised a theory of constant features in plumes. A statistical mixed-effects analysis of a co-emitted tracers model disentangles such mixing from fire effects.
Jann Schrod, Erik S. Thomson, Daniel Weber, Jens Kossmann, Christopher Pöhlker, Jorge Saturno, Florian Ditas, Paulo Artaxo, Valérie Clouard, Jean-Marie Saurel, Martin Ebert, Joachim Curtius, and Heinz G. Bingemer
Atmos. Chem. Phys., 20, 15983–16006, https://doi.org/10.5194/acp-20-15983-2020, https://doi.org/10.5194/acp-20-15983-2020, 2020
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Long-term ice-nucleating particle (INP) data are presented from four semi-pristine sites located in the Amazon, the Caribbean, Germany and the Arctic. Average INP concentrations did not differ by orders of magnitude between the sites. For all sites short-term variability dominated the time series, which lacked clear trends and seasonalities. Common drivers to explain the INP levels and their variations could not be identified, illustrating the complex nature of heterogeneous ice nucleation.
Robbie Ramsay, Chiara F. Di Marco, Matthias Sörgel, Mathew R. Heal, Samara Carbone, Paulo Artaxo, Alessandro C. de Araùjo, Marta Sá, Christopher Pöhlker, Jost Lavric, Meinrat O. Andreae, and Eiko Nemitz
Atmos. Chem. Phys., 20, 15551–15584, https://doi.org/10.5194/acp-20-15551-2020, https://doi.org/10.5194/acp-20-15551-2020, 2020
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The Amazon rainforest is a unique
laboratoryto study the processes which govern the exchange of gases and aerosols to and from the atmosphere. This study investigated these processes by measuring the atmospheric concentrations of trace gases and particles at the Amazon Tall Tower Observatory. We found that the long-range transport of pollutants can affect the atmospheric composition above the Amazon rainforest and that the gases ammonia and nitrous acid can be emitted from the rainforest.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, https://doi.org/10.5194/acp-20-15513-2020, 2020
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This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Zhuang Wang, Cheng Liu, Zhouqing Xie, Qihou Hu, Meinrat O. Andreae, Yunsheng Dong, Chun Zhao, Ting Liu, Yizhi Zhu, Haoran Liu, Chengzhi Xing, Wei Tan, Xiangguang Ji, Jinan Lin, and Jianguo Liu
Atmos. Chem. Phys., 20, 14917–14932, https://doi.org/10.5194/acp-20-14917-2020, https://doi.org/10.5194/acp-20-14917-2020, 2020
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Significant stratification of aerosols was observed in North China. Polluted dust dominated above the PBL, and anthropogenic aerosols prevailed within the PBL, which is mainly driven by meteorological conditions. The key role of the elevated dust is to alter atmospheric thermodynamics and stability, causing the suppression of turbulence exchange and a decrease in PBL height, especially during the dissipation stage, thereby inhibiting dissipation of persistent heavy surface haze pollution.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Guo Li, Hang Su, Nan Ma, Guangjie Zheng, Uwe Kuhn, Meng Li, Thomas Klimach, Ulrich Pöschl, and Yafang Cheng
Atmos. Meas. Tech., 13, 6053–6065, https://doi.org/10.5194/amt-13-6053-2020, https://doi.org/10.5194/amt-13-6053-2020, 2020
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Aerosol acidity plays an important role in regulating the chemistry, health, and ecological effect of aerosol particles. However, a direct measurement of aerosol pH is very challenging because of its fast transition and equilibrium with adjacent environments. Therefore, most early studies have to use modeled pH, resulting in intensive debates about model uncertainties. Here we developed an optimized approach to measure aerosol pH by using pH-indicator papers combined with RGB-based colorimetry.
Nina Löbs, David Walter, Cybelli G. G. Barbosa, Sebastian Brill, Rodrigo P. Alves, Gabriela R. Cerqueira, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Florian Ditas, Daniel Moran-Zuloaga, Ana Paula Pires Florentino, Stefan Wolff, Ricardo H. M. Godoi, Jürgen Kesselmeier, Sylvia Mota de Oliveira, Meinrat O. Andreae, Christopher Pöhlker, and Bettina Weber
Biogeosciences, 17, 5399–5416, https://doi.org/10.5194/bg-17-5399-2020, https://doi.org/10.5194/bg-17-5399-2020, 2020
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Cryptogamic organisms, such as bryophytes, lichens, and algae, cover major parts of vegetation in the Amazonian rain forest, but their relevance in biosphere–atmosphere exchange, climate processes, and nutrient cycling is largely unknown.
Over the duration of 2 years we measured their water content, temperature, and light conditions to get better insights into their physiological activity patterns and thus their potential impact on local, regional, and even global biogeochemical processes.
Lawrence I. Kleinman, Arthur J. Sedlacek III, Kouji Adachi, Peter R. Buseck, Sonya Collier, Manvendra K. Dubey, Anna L. Hodshire, Ernie Lewis, Timothy B. Onasch, Jeffery R. Pierce, John Shilling, Stephen R. Springston, Jian Wang, Qi Zhang, Shan Zhou, and Robert J. Yokelson
Atmos. Chem. Phys., 20, 13319–13341, https://doi.org/10.5194/acp-20-13319-2020, https://doi.org/10.5194/acp-20-13319-2020, 2020
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Aerosols from wildfires affect the Earth's temperature by absorbing light or reflecting it back into space. This study investigates time-dependent chemical, microphysical, and optical properties of aerosols generated by wildfires in the Pacific Northwest, USA. Wildfire smoke plumes were traversed by an instrumented aircraft at locations near the fire and up to 3.5 h travel time downwind. Although there was no net aerosol production, aerosol particles grew and became more efficient scatters.
Lixia Liu, Yafang Cheng, Siwen Wang, Chao Wei, Mira L. Pöhlker, Christopher Pöhlker, Paulo Artaxo, Manish Shrivastava, Meinrat O. Andreae, Ulrich Pöschl, and Hang Su
Atmos. Chem. Phys., 20, 13283–13301, https://doi.org/10.5194/acp-20-13283-2020, https://doi.org/10.5194/acp-20-13283-2020, 2020
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This modeling paper reveals how aerosol–cloud interactions (ACIs) and aerosol–radiation interactions (ARIs) induced by biomass burning (BB) aerosols act oppositely on radiation, cloud, and precipitation in the Amazon during the dry season. The varying relative significance of ACIs and ARIs with BB aerosol concentration leads to a nonlinear dependence of the total climate response on BB aerosol loading and features the growing importance of ARIs at high aerosol loading.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Guangjie Zheng, Chongai Kuang, Janek Uin, Thomas Watson, and Jian Wang
Atmos. Chem. Phys., 20, 12515–12525, https://doi.org/10.5194/acp-20-12515-2020, https://doi.org/10.5194/acp-20-12515-2020, 2020
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Condensational growth of Aitken-mode particles is a major source of cloud condensation nuclei in the remote marine boundary layer. It has been long thought that over remote oceans, condensation growth is dominated by sulfate that derives from ocean-emitted dimethyl sulfide. In this study, we present the first long-term observational evidence that, contrary to conventional thinking, organics play an even more important role than sulfate in particle growth over remote oceans throughout the year.
Kouji Adachi, Naga Oshima, Zhaoheng Gong, Suzane de Sá, Adam P. Bateman, Scot T. Martin, Joel F. de Brito, Paulo Artaxo, Glauber G. Cirino, Arthur J. Sedlacek III, and Peter R. Buseck
Atmos. Chem. Phys., 20, 11923–11939, https://doi.org/10.5194/acp-20-11923-2020, https://doi.org/10.5194/acp-20-11923-2020, 2020
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Occurrences, size distributions, and number fractions of individual aerosol particles from the Amazon basin during the GoAmazon2014/5 campaign were analyzed using transmission electron microscopy. Aerosol particles from natural sources (e.g., mineral dust, primary biological aerosols, and sea salts) during the wet season originated from the Amazon forest and long-range transports (the Saharan desert and the Atlantic Ocean). They commonly mix at an individual particle scale during transport.
Ting Lei, Nan Ma, Juan Hong, Thomas Tuch, Xin Wang, Zhibin Wang, Mira Pöhlker, Maofa Ge, Weigang Wang, Eugene Mikhailov, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Alfred Wiedensohler, and Yafang Cheng
Atmos. Meas. Tech., 13, 5551–5567, https://doi.org/10.5194/amt-13-5551-2020, https://doi.org/10.5194/amt-13-5551-2020, 2020
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We present the design of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. We further introduce comprehensive methods for system calibration and validation of the performance of the system. We then study the size dependence of the deliquescence and the efflorescence of aerosol nanoparticles for sizes down to 6 nm.
Wei Tao, Hang Su, Guangjie Zheng, Jiandong Wang, Chao Wei, Lixia Liu, Nan Ma, Meng Li, Qiang Zhang, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 20, 11729–11746, https://doi.org/10.5194/acp-20-11729-2020, https://doi.org/10.5194/acp-20-11729-2020, 2020
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We simulated the thermodynamic and multiphase reactions in aerosol water during a wintertime haze event over the North China Plain. It was found that aerosol pH exhibited a strong spatiotemporal variability, and multiple oxidation pathways were predominant for particulate sulfate formation in different locations. Sensitivity tests further showed that ammonia, crustal particles, and dissolved transition metal ions were important factors for multiphase chemistry during haze episodes.
Anin Puthukkudy, J. Vanderlei Martins, Lorraine A. Remer, Xiaoguang Xu, Oleg Dubovik, Pavel Litvinov, Brent McBride, Sharon Burton, and Henrique M. J. Barbosa
Atmos. Meas. Tech., 13, 5207–5236, https://doi.org/10.5194/amt-13-5207-2020, https://doi.org/10.5194/amt-13-5207-2020, 2020
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In this work, we report the demonstration and validation of the aerosol properties retrieved using AirHARP and GRASP for data from the NASA ACEPOL campaign 2017. These results serve as a proxy for the scale and detail of aerosol retrievals that are anticipated from future space mission data, as HARP CubeSat (mission begins 2020) and HARP2 (aboard the NASA PACE mission with the launch in 2023) are near duplicates of AirHARP and are expected to provide the same level of aerosol characterization.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
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We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Kirk Knobelspiesse, Henrique M. J. Barbosa, Christine Bradley, Carol Bruegge, Brian Cairns, Gao Chen, Jacek Chowdhary, Anthony Cook, Antonio Di Noia, Bastiaan van Diedenhoven, David J. Diner, Richard Ferrare, Guangliang Fu, Meng Gao, Michael Garay, Johnathan Hair, David Harper, Gerard van Harten, Otto Hasekamp, Mark Helmlinger, Chris Hostetler, Olga Kalashnikova, Andrew Kupchock, Karla Longo De Freitas, Hal Maring, J. Vanderlei Martins, Brent McBride, Matthew McGill, Ken Norlin, Anin Puthukkudy, Brian Rheingans, Jeroen Rietjens, Felix C. Seidel, Arlindo da Silva, Martijn Smit, Snorre Stamnes, Qian Tan, Sebastian Val, Andrzej Wasilewski, Feng Xu, Xiaoguang Xu, and John Yorks
Earth Syst. Sci. Data, 12, 2183–2208, https://doi.org/10.5194/essd-12-2183-2020, https://doi.org/10.5194/essd-12-2183-2020, 2020
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The Aerosol Characterization from Polarimeter and Lidar (ACEPOL) field campaign is a resource for the next generation of spaceborne multi-angle polarimeter (MAP) and lidar missions. Conducted in the fall of 2017 from the Armstrong Flight Research Center in Palmdale, California, four MAP instruments and two lidars were flown on the high-altitude ER-2 aircraft over a variety of scene types and ground assets. Data are freely available to the public and useful for algorithm development and testing.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Jan-David Förster, Christian Gurk, Mark Lamneck, Haijie Tong, Florian Ditas, Sarah S. Steimer, Peter A. Alpert, Markus Ammann, Jörg Raabe, Markus Weigand, Benjamin Watts, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Meas. Tech., 13, 3717–3729, https://doi.org/10.5194/amt-13-3717-2020, https://doi.org/10.5194/amt-13-3717-2020, 2020
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A gas flow system coupled with a microreactor for X-ray microspectroscopy is presented. Its core objective is to mimic the atmospheric processing of aerosol particles under laboratory conditions in a controlled gas-phase environment and allow in situ observations with high spatial and chemical resolution. We here emphasize its analytical capabilities and show initial results from hydration–dehydration experiments and the observation of water ice at low temperature and high relative humidity.
Francesca Gallo, Janek Uin, Stephen Springston, Jian Wang, Guangjie Zheng, Chongai Kuang, Robert Wood, Eduardo B. Azevedo, Allison McComiskey, Fan Mei, Adam Theisen, Jenni Kyrouac, and Allison C. Aiken
Atmos. Chem. Phys., 20, 7553–7573, https://doi.org/10.5194/acp-20-7553-2020, https://doi.org/10.5194/acp-20-7553-2020, 2020
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Continuous high-time-resolution ambient data can include periods when aerosol properties do not represent regional aerosol processes due to high-concentration local events. We develop a novel aerosol mask at the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) facility in the eastern North Atlantic (ENA). We use two ground sites to validate the mask, include a comparison with aircraft overflights, and provide guidance to increase data quality at ENA and other locations.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Andrew T. Lambe, Ezra C. Wood, Jordan E. Krechmer, Francesca Majluf, Leah R. Williams, Philip L. Croteau, Manuela Cirtog, Anaïs Féron, Jean-Eudes Petit, Alexandre Albinet, Jose L. Jimenez, and Zhe Peng
Atmos. Meas. Tech., 13, 2397–2411, https://doi.org/10.5194/amt-13-2397-2020, https://doi.org/10.5194/amt-13-2397-2020, 2020
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We present a new method to continuously generate N2O5 in the gas phase that is injected into a reactor where it decomposes to generate nitrate radicals (NO3). To assess the applicability of the method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure and other metrics as a function of operating conditions. We demonstrate the method by characterizing secondary organic aerosol particles generated from the β-pinene + NO3 reaction.
William T. Morgan, James D. Allan, Stéphane Bauguitte, Eoghan Darbyshire, Michael J. Flynn, James Lee, Dantong Liu, Ben Johnson, Jim Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 20, 5309–5326, https://doi.org/10.5194/acp-20-5309-2020, https://doi.org/10.5194/acp-20-5309-2020, 2020
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We flew a large atmospheric research aircraft across a number of different environments in the Amazon basin during the 2012 biomass burning season. Smoke from fires builds up and has a significant impact on weather, climate, health and natural ecosystems. Our goal was to quantify changes in the properties of the smoke emitted by fires as it is transported through the atmosphere. We found that the major control on the properties of the smoke was due to differences in the fires themselves.
Bruna A. Holanda, Mira L. Pöhlker, David Walter, Jorge Saturno, Matthias Sörgel, Jeannine Ditas, Florian Ditas, Christiane Schulz, Marco Aurélio Franco, Qiaoqiao Wang, Tobias Donth, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Ramon Braga, Joel Brito, Yafang Cheng, Maximilian Dollner, Johannes W. Kaiser, Thomas Klimach, Christoph Knote, Ovid O. Krüger, Daniel Fütterer, Jošt V. Lavrič, Nan Ma, Luiz A. T. Machado, Jing Ming, Fernando G. Morais, Hauke Paulsen, Daniel Sauer, Hans Schlager, Johannes Schneider, Hang Su, Bernadett Weinzierl, Adrian Walser, Manfred Wendisch, Helmut Ziereis, Martin Zöger, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
Atmos. Chem. Phys., 20, 4757–4785, https://doi.org/10.5194/acp-20-4757-2020, https://doi.org/10.5194/acp-20-4757-2020, 2020
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Biomass burning smoke from African savanna and grassland is transported across the South Atlantic Ocean in defined layers within the free troposphere. The combination of in situ aircraft and ground-based measurements aided by satellite observations showed that these layers are transported into the Amazon Basin during the early dry season. The influx of aged smoke, enriched in black carbon and cloud condensation nuclei, has important implications for the Amazonian aerosol and cloud cycling.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Brent A. McBride, J. Vanderlei Martins, Henrique M. J. Barbosa, William Birmingham, and Lorraine A. Remer
Atmos. Meas. Tech., 13, 1777–1796, https://doi.org/10.5194/amt-13-1777-2020, https://doi.org/10.5194/amt-13-1777-2020, 2020
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Clouds play a large role in the way our Earth system distributes energy. The measurement of cloud droplet size distribution (DSD) is one way to connect small-scale cloud processes to scattered radiation. Our small satellite instrument, the Airborne Hyper-Angular Rainbow Polarimeter, is the first to infer DSDs over a wide spatial cloud field using polarized light. This study improves the way we interpret cloud properties and shows that high-quality science does not require a large taxpayer cost.
Sinikka T. Lennartz, Christa A. Marandino, Marc von Hobe, Meinrat O. Andreae, Kazushi Aranami, Elliot Atlas, Max Berkelhammer, Heinz Bingemer, Dennis Booge, Gregory Cutter, Pau Cortes, Stefanie Kremser, Cliff S. Law, Andrew Marriner, Rafel Simó, Birgit Quack, Günther Uher, Huixiang Xie, and Xiaobin Xu
Earth Syst. Sci. Data, 12, 591–609, https://doi.org/10.5194/essd-12-591-2020, https://doi.org/10.5194/essd-12-591-2020, 2020
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Sulfur-containing trace gases in the atmosphere influence atmospheric chemistry and the energy budget of the Earth by forming aerosols. The ocean is an important source of the most abundant sulfur gas in the atmosphere, carbonyl sulfide (OCS) and its most important precursor carbon disulfide (CS2). In order to assess global variability of the sea surface concentrations of both gases to calculate their oceanic emissions, we have compiled a database of existing shipborne measurements.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Fan Mei, Jian Wang, Jennifer M. Comstock, Ralf Weigel, Martina Krämer, Christoph Mahnke, John E. Shilling, Johannes Schneider, Christiane Schulz, Charles N. Long, Manfred Wendisch, Luiz A. T. Machado, Beat Schmid, Trismono Krisna, Mikhail Pekour, John Hubbe, Andreas Giez, Bernadett Weinzierl, Martin Zoeger, Mira L. Pöhlker, Hans Schlager, Micael A. Cecchini, Meinrat O. Andreae, Scot T. Martin, Suzane S. de Sá, Jiwen Fan, Jason Tomlinson, Stephen Springston, Ulrich Pöschl, Paulo Artaxo, Christopher Pöhlker, Thomas Klimach, Andreas Minikin, Armin Afchine, and Stephan Borrmann
Atmos. Meas. Tech., 13, 661–684, https://doi.org/10.5194/amt-13-661-2020, https://doi.org/10.5194/amt-13-661-2020, 2020
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In 2014, the US DOE G1 aircraft and the German HALO aircraft overflew the Amazon basin to study how aerosols influence cloud cycles under a clean condition and around a tropical megacity. This paper describes how to meaningfully compare similar measurements from two research aircraft and identify the potential measurement issue. We also discuss the uncertainty range for each measurement for further usage in model evaluation and satellite data validation.
Pascal Polonik, Christoph Knote, Tobias Zinner, Florian Ewald, Tobias Kölling, Bernhard Mayer, Meinrat O. Andreae, Tina Jurkat-Witschas, Thomas Klimach, Christoph Mahnke, Sergej Molleker, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Christiane Voigt, Ralf Weigel, and Manfred Wendisch
Atmos. Chem. Phys., 20, 1591–1605, https://doi.org/10.5194/acp-20-1591-2020, https://doi.org/10.5194/acp-20-1591-2020, 2020
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A realistic representation of cloud–aerosol interactions is central to accurate climate projections. Here we combine observations collected during the ACRIDICON-CHUVA campaign with chemistry-transport simulations to evaluate the model’s ability to represent the indirect effects of biomass burning aerosol on cloud microphysics. We find an upper limit for the model sensitivity on cloud condensation nuclei concentrations well below the levels reached during the burning season in the Amazon Basin.
Nina Löbs, Cybelli G. G. Barbosa, Sebastian Brill, David Walter, Florian Ditas, Marta de Oliveira Sá, Alessandro C. de Araújo, Leonardo R. de Oliveira, Ricardo H. M. Godoi, Stefan Wolff, Meike Piepenbring, Jürgen Kesselmeier, Paulo Artaxo, Meinrat O. Andreae, Ulrich Pöschl, Christopher Pöhlker, and Bettina Weber
Atmos. Meas. Tech., 13, 153–164, https://doi.org/10.5194/amt-13-153-2020, https://doi.org/10.5194/amt-13-153-2020, 2020
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Bioaerosols are considered to play a relevant role in atmospheric processes, but their sources, properties, and spatiotemporal distribution in the atmosphere are not yet well characterized. Measurement data on the release of fungal spores under natural conditions are also sparse. Here, we present an experimental approach to analyze and quantify the spore release from fungi and other spore-producing organisms under natural and laboratory conditions.
Maurício I. Oliveira, Otávio C. Acevedo, Matthias Sörgel, Ernani L. Nascimento, Antonio O. Manzi, Pablo E. S. Oliveira, Daiane V. Brondani, Anywhere Tsokankunku, and Meinrat O. Andreae
Atmos. Chem. Phys., 20, 15–27, https://doi.org/10.5194/acp-20-15-2020, https://doi.org/10.5194/acp-20-15-2020, 2020
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In this study, data collected during four deep convection events at the 80 m tower from the Amazon Tall Tower Observatory are analyzed. It provides a unique view on how such events affect the local boundary layer and how it recovers after their passage. Quantities analyzed include mean wind speed, virtual potential temperature, turbulent kinetic energy, sensible, and latent heat fluxes. A conceptual model for boundary layer structure along the passage of deep convection events is proposed.
Claudia Di Biagio, Paola Formenti, Yves Balkanski, Lorenzo Caponi, Mathieu Cazaunau, Edouard Pangui, Emilie Journet, Sophie Nowak, Meinrat O. Andreae, Konrad Kandler, Thuraya Saeed, Stuart Piketh, David Seibert, Earle Williams, and Jean-François Doussin
Atmos. Chem. Phys., 19, 15503–15531, https://doi.org/10.5194/acp-19-15503-2019, https://doi.org/10.5194/acp-19-15503-2019, 2019
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This paper presents a new dataset of laboratory measurements of the shortwave (SW) spectral complex refractive index and single-scattering albedo (SSA) for global mineral dust aerosols of varying origin and composition. Our results show that the dust refractive index and SSA vary strongly from source to source, mostly due to particle iron content changes. We recommend that source-dependent values of the SW spectral refractive index and SSA be used in models and remote sensing applications.
Sophie L. Haslett, Jonathan W. Taylor, Mathew Evans, Eleanor Morris, Bernhard Vogel, Alima Dajuma, Joel Brito, Anneke M. Batenburg, Stephan Borrmann, Johannes Schneider, Christiane Schulz, Cyrielle Denjean, Thierry Bourrianne, Peter Knippertz, Régis Dupuy, Alfons Schwarzenböck, Daniel Sauer, Cyrille Flamant, James Dorsey, Ian Crawford, and Hugh Coe
Atmos. Chem. Phys., 19, 15217–15234, https://doi.org/10.5194/acp-19-15217-2019, https://doi.org/10.5194/acp-19-15217-2019, 2019
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Three aircraft datasets from the DACCIWA campaign in summer 2016 are used here to show there is a background mass of pollution present in the lower atmosphere in southern West Africa. We suggest that this likely comes from biomass burning in central and southern Africa, which has been carried into the region over the Atlantic Ocean. This would have a negative health impact on populations living near the coast and may alter the impact of growing city emissions on cloud formation and the monsoon.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Anna T. Kunert, Mira L. Pöhlker, Kai Tang, Carola S. Krevert, Carsten Wieder, Kai R. Speth, Linda E. Hanson, Cindy E. Morris, David G. Schmale III, Ulrich Pöschl, and Janine Fröhlich-Nowoisky
Biogeosciences, 16, 4647–4659, https://doi.org/10.5194/bg-16-4647-2019, https://doi.org/10.5194/bg-16-4647-2019, 2019
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A screening of more than 100 strains from 65 different species revealed that the ice nucleation activity within the fungal genus Fusarium is more widespread than previously assumed. Filtration experiments suggest that the single cell-free Fusarium IN is smaller than 100 kDa (~ 6 nm) and that aggregates can be formed in solution. Exposure experiments, freeze–thaw cycles, and long-term storage tests demonstrate a high stability of Fusarium IN under atmospherically relevant conditions.
Karl D. Froyd, Daniel M. Murphy, Charles A. Brock, Pedro Campuzano-Jost, Jack E. Dibb, Jose-Luis Jimenez, Agnieszka Kupc, Ann M. Middlebrook, Gregory P. Schill, Kenneth L. Thornhill, Christina J. Williamson, James C. Wilson, and Luke D. Ziemba
Atmos. Meas. Tech., 12, 6209–6239, https://doi.org/10.5194/amt-12-6209-2019, https://doi.org/10.5194/amt-12-6209-2019, 2019
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Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with a fast time response applicable to aircraft sampling.
Brett B. Palm, Xiaoxi Liu, Jose L. Jimenez, and Joel A. Thornton
Atmos. Meas. Tech., 12, 5829–5844, https://doi.org/10.5194/amt-12-5829-2019, https://doi.org/10.5194/amt-12-5829-2019, 2019
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We introduce a coaxial, low-pressure ion–molecule reaction (IMR) region for iodide-adduct chemical ionization mass spectrometry, designed to decrease the effects of IMR wall interactions with organic/inorganic gases. This IMR has 3–10 times shorter delay times than previous IMRs. We introduce a conceptual framework for understanding and subtracting the background signal due to analyte molecules interacting with IMR walls. This framework can be applied to other tubing and instrument systems.
Hayley S. Glicker, Michael J. Lawler, John Ortega, Suzane S. de Sá, Scot T. Martin, Paulo Artaxo, Oscar Vega Bustillos, Rodrigo de Souza, Julio Tota, Annmarie Carlton, and James N. Smith
Atmos. Chem. Phys., 19, 13053–13066, https://doi.org/10.5194/acp-19-13053-2019, https://doi.org/10.5194/acp-19-13053-2019, 2019
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An understanding of the chemical composition of the smallest particles in the air over the Amazon Basin provides insights into the natural and human-caused influences on particle production in this sensitive region. We present measurements of the composition of sub-100 nm diameter particles performed during the wet season and identify unique constituents that point to both natural and human-caused sources and processes.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Masayuki Takeuchi and Nga L. Ng
Atmos. Chem. Phys., 19, 12749–12766, https://doi.org/10.5194/acp-19-12749-2019, https://doi.org/10.5194/acp-19-12749-2019, 2019
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Organic nitrate is ubiquitous in the atmosphere and impacts the formation of aerosol and ozone, two leading air pollutants of concern worldwide. We conducted a comprehensive laboratory study to investigate the hydrolysis process of organic nitrate aerosol formed from monoterpenes, which are important reactive chemicals emitted by plants. Our results provide experimentally constrained parameters required to assess the role of organic nitrate in the formation of the air pollutants of our concern.