Articles | Volume 17, issue 1
https://doi.org/10.5194/acp-17-343-2017
© 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-17-343-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
06 Jan 2017
Research article |
| 06 Jan 2017
On the implications of aerosol liquid water and phase separation for organic aerosol mass
National Exposure Research Laboratory, US Environmental Protection Agency, Research Triangle Park, NC, USA
Benjamin N. Murphy
National Exposure Research Laboratory, US Environmental Protection Agency, Research Triangle Park, NC, USA
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
Nga L. 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
Annmarie G. Carlton
Department of Environmental Sciences, Rutgers University, New Brunswick, NJ, USA
now at: Department of Chemistry, University of California, Irvine, CA, USA
Hongyu Guo
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
Rodney Weber
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
Petros Vasilakos
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
K. Wyat Appel
National Exposure Research Laboratory, US Environmental Protection Agency, Research Triangle Park, NC, USA
Sri Hapsari Budisulistiorini
Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, NC, USA
Jason D. Surratt
Gillings School of Global Public Health, The University of North Carolina at Chapel Hill, Chapel Hill, NC, USA
Athanasios Nenes
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
Institute of Environmental Research and Sustainable Development, National Observatory of Athens, Palea Penteli, 15236, Greece
Institute for Chemical Engineering Sciences, Foundation for Research and Technology Hellas, Patras, Greece
Weiwei Hu
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA
Jose L. Jimenez
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO, USA
Gabriel Isaacman-VanWertz
Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA USA
Pawel K. Misztal
Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA USA
Allen H. Goldstein
Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA USA
Department of Civil and Environmental Engineering, University of California, Berkeley, CA USA
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Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
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K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
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Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
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Preprint withdrawn
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Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Quanyang Lu, Benjamin N. Murphy, Momei Qin, Peter J. Adams, Yunliang Zhao, Havala O. T. Pye, Christos Efstathiou, Chris Allen, and Allen L. Robinson
Atmos. Chem. Phys., 20, 4313–4332, https://doi.org/10.5194/acp-20-4313-2020, https://doi.org/10.5194/acp-20-4313-2020, 2020
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This research work investigates organic aerosol formation in California during the CalNex study. We update the chemical transport model with the most recent mobile-source emission data and introduce a simple parameterization for secondary organic aerosol formed from intermediate-volatility organic compounds. Our results highlight the important contribution of IVOCs to SOA production in the Los Angeles region but underscore that other uncertainties must be addressed to close the SOA mass balance.
Lu Xu, Havala O. T. Pye, Jia He, Yunle Chen, Benjamin N. Murphy, and Nga Lee Ng
Atmos. Chem. Phys., 18, 12613–12637, https://doi.org/10.5194/acp-18-12613-2018, https://doi.org/10.5194/acp-18-12613-2018, 2018
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In this study, we integrate lab-in-the-field experiments, extensive ambient ground measurements, and state-of-the-art modeling to constrain the concentration of organic aerosol from biogenic monoterpenes and sesquiterpenes. Further, we show that the organic aerosol from the investigated sources accounts for roughly 20 % of the World Health Organization PM2.5 standard in the southeastern US.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Kathleen M. Fahey, Annmarie G. Carlton, Havala O. T. Pye, Jaemeen Baek, William T. Hutzell, Charles O. Stanier, Kirk R. Baker, K. Wyat Appel, Mohammed Jaoui, and John H. Offenberg
Geosci. Model Dev., 10, 1587–1605, https://doi.org/10.5194/gmd-10-1587-2017, https://doi.org/10.5194/gmd-10-1587-2017, 2017
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Chemical transport models (CTMs) are a crucial tool in understanding links between emissions, air quality, and climate. Only a simple description of cloud chemistry has been implemented in many of these; however, clouds play a major role in the physicochemical processing of atmospheric species. In CMAQ, EPA’s widely used CTM, the cloud code is limited to the treatment of simple chemistry. We update CMAQ clouds to consider additional chemistry and then examine regional impacts of these updates.
Shantanu H. Jathar, Matthew Woody, Havala O. T. Pye, Kirk R. Baker, and Allen L. Robinson
Atmos. Chem. Phys., 17, 4305–4318, https://doi.org/10.5194/acp-17-4305-2017, https://doi.org/10.5194/acp-17-4305-2017, 2017
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Mobile sources such as cars and trucks are large sources of pollution in cities, but it is unclear what their relative contribution to organic particle pollution is. We used a numerical model along with recent data gathered from tests performed on cars and trucks to calculate organic particle levels in southern California. We found that model calculations agreed better with measurements and gasoline cars and trucks dominated the organic particle pollution.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Matthew C. Woody, Kirk R. Baker, Patrick L. Hayes, Jose L. Jimenez, Bonyoung Koo, and Havala O. T. Pye
Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, https://doi.org/10.5194/acp-16-4081-2016, 2016
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In this work, organic aerosol (OA) predictions from the volatility basis set (VBS) module in the CMAQ photochemical transport model were evaluated against routine monitoring data and measurements collected during the 2010 CalNex field study. We found that the VBS module more accurately reproduced the observed primary/secondary OA split and secondary OA (SOA) mass at the CalNex Pasadena ground site compared to the traditional CMAQ OA module but still underpredicted observed SOA by ~ 5.2 ×.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
B. H. Henderson, F. Akhtar, H. O. T. Pye, S. L. Napelenok, and W. T. Hutzell
Geosci. Model Dev., 7, 339–360, https://doi.org/10.5194/gmd-7-339-2014, https://doi.org/10.5194/gmd-7-339-2014, 2014
K. W. Appel, G. A. Pouliot, H. Simon, G. Sarwar, H. O. T. Pye, S. L. Napelenok, F. Akhtar, and S. J. Roselle
Geosci. Model Dev., 6, 883–899, https://doi.org/10.5194/gmd-6-883-2013, https://doi.org/10.5194/gmd-6-883-2013, 2013
Wenhui Zhao, Weiwei Hu, Zhaoce Liu, Tianle Pan, Tingting Feng, Jun Wang, Yiyu Cai, Lin Liang, Shan Huang, Bin Yuan, Nan Ma, Min Shao, Guohua Zhang, Xinhui Bi, Xinming Wang, and Pengfei Yu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2974, https://doi.org/10.5194/egusphere-2025-2974, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Our study examined brown carbon—organic aerosols that absorb light—at the remote Tibet and urban Guangzhou. Field data showed Tibet’s brown carbon absorbs about 10 times less than Guangzhou’s, due to cleaner air. Yet, over 75 % of its light absorption still comes from primary emission, which causes over 98 % of its climate-warming effect in both places. This study advances understanding of BrC dynamics and its sources in diverse environments for global climate effects.
Sara L. Farrell, Quazi Z. Rasool, Havala O. T. Pye, Yue Zhang, Ying Li, Yuzhi Chen, Chi-Tsan Wang, Haofei Zhang, Ryan Schmedding, Manabu Shiraiwa, Jaime Greene, Sri H. Budisulistiorini, Jose L. Jimenez, Weiwei Hu, Jason D. Surratt, and William Vizuete
EGUsphere, https://doi.org/10.5194/egusphere-2025-2253, https://doi.org/10.5194/egusphere-2025-2253, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Fine particulate matter (PM2.5) has become increasingly important to regulate and model. In this study, we parameterize non-ideal aerosol mixing and phase state into the Community Multiscale Air Quality (CMAQ) model and analyze its impact on the formation of a globally important source of PM2.5, isoprene epoxydiol (IEPOX)-derived PM2.5. Incorporating these features furthers model bias in IEPOX-derived PM2.5, however, this work provides potential phase state bounds for future PM2.5 modeling work.
Yu Li, Momei Qin, Weiwei Hu, Bin Zhao, Ying Li, Havala O. T. Pye, Jingyi Li, Linghan Zeng, Song Guo, Min Hu, and Jianlin Hu
EGUsphere, https://doi.org/10.5194/egusphere-2025-2879, https://doi.org/10.5194/egusphere-2025-2879, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We evaluated how well a widely used air quality model simulates key properties of organic particles in the atmosphere, such as volatility and oxygen content, which influence how particles age, spread, and affect both air quality and climate. Using observations from eastern China, we found the model underestimated particle mass and misrepresented their chemical makeup. Our results highlight the need for improved emissions and chemical treatments to better predict air quality and climate impacts.
Anna Maria Neroladaki, Maria Tsagkaraki, Kyriaki Papoutsidaki, Kalliopi Tavernaraki, Filothei Boufidou, Pavlos Zarmpas, Irini Tsiodra, Eleni Liakakou, Aikaterini Bougiatioti, Giorgos Kouvarakis, Nikos Kalivitis, Christos Kaltsonoudis, Athanasios Karagioras, Dimitrios Balis, Konstantinos Mihailidis, Konstantinos Kourtidis, Stelios Myriokefalitakis, Nikos Hatzianastassiou, Spyros N. Pandis, Athanasios Nenes, Nikolaos Mihalopoulos, and Maria Kanakidou
EGUsphere, https://doi.org/10.5194/egusphere-2025-3223, https://doi.org/10.5194/egusphere-2025-3223, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Aerosol acidity affects aerosol composition and properties, and therefore climate, human health and ecosystems. We use summer and winter fine aerosol observations at 6 sites across Greece, and a thermodynamic model to calculate the spatial and seasonal variability of aerosol acidity. Aerosols were acidic to moderately acidic and more acidic during summer than winter. The importance of organics for aerosol acidity was small. Depending on location different factors controlled aerosol acidity.
Marilena Gidarakou, Alexandros Papayannis, Kunfeng Gao, Panagiotis Gidarakos, Benoit Crouzy, Romanos Foskinis, Sophie Erb, Cuiqi Zhang, Gian Lieberherr, Martine Collaud Coen, Branko Sikoparija, Zamin A. Kanji, Bernard Clot, Bertrand Calpini, Eugenia Giagka, and Athanasios Nenes
EGUsphere, https://doi.org/10.5194/egusphere-2025-2978, https://doi.org/10.5194/egusphere-2025-2978, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Vertical profiles of pollen and biomass burning particles were obtained at a semi-rural site at the MeteoSwiss station near Payerne (Switzerland) using a novel multi-channel elastic-fluorescence lidar system combined with in situ measurements during the spring 2023 wildfires and pollination season during the PERICLES (PayernE lidaR and Insitu detection of fluorescent bioaerosol and dust partiCLES and their cloud impacts) campaign.
Dongwook Kim, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Da Yang, Suresh Dhaniyala, Leah Williams, Philip Croteau, John Jayne, Douglas Worsnop, Rainer Volkamer, and Jose L. Jimenez
Aerosol Research, 3, 371–404, https://doi.org/10.5194/ar-3-371-2025, https://doi.org/10.5194/ar-3-371-2025, 2025
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Quantitative real-time aerosol sampling on board aircraft platforms is challenging, especially at higher altitudes. Herein, we present comprehensive analyses of a new aircraft inlet system and tools for aerosol beam diagnostics for aerosol mass spectrometers (AMSs). The beam focusing of aerodynamic lenses and the thermal decomposition on the vaporizer were investigated. The new inlet system can be operated at higher altitudes while sampling aerosols over a broader size range than previous versions.
Erin F. Katz, Caleb M. Arata, Eva Y. Pfannerstill, Robert J. Weber, Darian Ng, Michael J. Milazzo, Haley Byrne, Hui Wang, Alex B. Guenther, Camilo Rey-Sanchez, Joshua Apte, Dennis D. Baldocchi, and Allen H. Goldstein
EGUsphere, https://doi.org/10.5194/egusphere-2025-2682, https://doi.org/10.5194/egusphere-2025-2682, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Terpenoids are organic gases that can originate from natural and human-caused sources, and their fast reactions in the atmosphere can cause air pollution. Emissions of organic gases in an urban environment were measured. For some terpenoids, human-caused sources were responsible for about a quarter of the emissions, while others were likely to be entirely from vegetation. The terpenoids contributed substantially to the potential to form secondary pollutants.
Maria P. Georgopoulou, Kalliopi Florou, Angeliki Matrali, Georgia Starida, Christos Kaltsonoudis, Athanasios Nenes, and Spyros N. Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2025-2728, https://doi.org/10.5194/egusphere-2025-2728, 2025
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Residential biomass burning is an important wintertime source of aerosols. This study examined the complex diurnal aging cycles on biomass burning aerosol composition and oxidative potential, a key toxicity metric. Additional organic aerosol (OA) mass was produced after the two (day/night and night/day) cycles, varying from 35 to 90 % of the initial OA. The aging of the emissions led to a final oxidative potential increase of 60 % for both cycles.
Yusuf Bhatti, Duncan Watson-Parris, Leighton Regayre, Hailing Jia, David Neubauer, Ulas Im, Carl Svenhag, Nick Schutgens, Athanasios Tsikerdekis, Athanasios Nenes, Irfan Muhammed, Bastiaan van Diedenhoven, Ardit Arifi, Guangliang Fu, and Otto Hasekamp
EGUsphere, https://doi.org/10.5194/egusphere-2025-2848, https://doi.org/10.5194/egusphere-2025-2848, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Aerosols (small airborne particles) impact Earth's climate, but their extent is unknown. By running climate model simulations and emulating millions of additional variants with different settings, we found that natural emissions like sea spray and sulfur are key sources of uncertainty in climate predictions. Our work shows that understanding these natural processes better can help improve climate models and make future climate projections more accurate.
Nahin Ferdousi-Rokib, Stephanie Jacoby, N. Cazimir Armstrong, Alana Dodero, Martin Changman Ahn, Ergine Zephira Remy, Zhenfa Zhang, Avram Gold, Joseph L. Woo, Yue Zhang, Jason D. Surratt, and Akua A. Asa-Awuku
EGUsphere, https://doi.org/10.5194/egusphere-2025-1935, https://doi.org/10.5194/egusphere-2025-1935, 2025
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This study looks at how natural compounds when mixed with salts in the air affect how clouds form. These compounds come from plants and are found all over the world. They are sticky, and this changes how water droplets and clouds form. Sometimes the compound spreads more easily when mixed with salt, while the other compound does not change. Depending on the condition, these mixtures can behave differently, which affects how we predict cloud formation.
James D. A. Butler, Afsara Tasnia, Deep Sengupta, Nathan Kreisberg, Kelley C. Barsanti, Allen H. Goldstein, Chelsea V. Preble, Rebecca A. Sugrue, and Thomas W. Kirchstetter
EGUsphere, https://doi.org/10.5194/egusphere-2025-2295, https://doi.org/10.5194/egusphere-2025-2295, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Prescribed burns are controlled fires used to prevent wildfires. Smoke emissions were measured to characterize emission factors and optical properties of black and brown soot particles. Brown particles were emitted at 7–14 times that of black particles and contributed 82 % of atmospheric absorption by particles for ultraviolet light and 23 % for total solar radiation. These findings will improve inventories and climate models for prescribed burns.
Christopher N. Rapp, Sining Niu, N. Cazimir Armstrong, Xiaoli Shen, Thomas Berkemeier, Jason D. Surratt, Yue Zhang, and Daniel J. Cziczo
Atmos. Chem. Phys., 25, 5519–5536, https://doi.org/10.5194/acp-25-5519-2025, https://doi.org/10.5194/acp-25-5519-2025, 2025
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Atmospheric ice formation is initiated by particulate matter suspended in air and has profound impacts on Earth's climate. This study focuses on examining the effectiveness of ice formation by a subset of particles composed of organic matter and sulfate. We used experiments and computer modeling to obtain the result that these particles are not effective ice-nucleating particles, suggesting that molecular structure is important for ice formation on these types of particles.
Yuchen Wang, Xiang Zhang, Yuanlong Huang, Yutong Liang, and Nga L. Ng
Atmos. Chem. Phys., 25, 5215–5231, https://doi.org/10.5194/acp-25-5215-2025, https://doi.org/10.5194/acp-25-5215-2025, 2025
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This work provides the first fundamental laboratory data to evaluate SOA (secondary organic aerosol) production from styrene and NO3 chemistry. Additionally, the formation mechanisms of aromatic organic nitrates (ONs) are reported, highlighting that previously identified nitroaromatics in ambient field campaigns can be aromatic ONs. Finally, the hydrolysis lifetimes observed for ONs generated from styrene and NO3 oxidation can serve as experimentally constrained parameters for modeling hydrolysis of aromatic ONs in general.
Benjamin C. Sapper, Sean Youn, Daven K. Henze, Manjula Canagaratna, Harald Stark, and Jose L. Jimenez
Geosci. Model Dev., 18, 2891–2919, https://doi.org/10.5194/gmd-18-2891-2025, https://doi.org/10.5194/gmd-18-2891-2025, 2025
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Positive matrix factorization (PMF) has been used by atmospheric scientists to extract underlying factors present in large datasets. This paper presents a new technique for error-weighted PMF that drastically reduces the computational costs of previously developed algorithms. We use this technique to deliver interpretable factors and solution diagnostics from an atmospheric chemistry dataset.
Joseph O. Palmo, Colette L. Heald, Donald R. Blake, Ilann Bourgeois, Matthew Coggon, Jeff Collett, Frank Flocke, Alan Fried, Georgios Gkatzelis, Samuel Hall, Lu Hu, Jose L. Jimenez, Pedro Campuzano-Jost, I-Ting Ku, Benjamin Nault, Brett Palm, Jeff Peischl, Ilana Pollack, Amy Sullivan, Joel Thornton, Carsten Warneke, Armin Wisthaler, and Lu Xu
EGUsphere, https://doi.org/10.5194/egusphere-2025-1969, https://doi.org/10.5194/egusphere-2025-1969, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study investigates ozone production within wildfire smoke plumes as they age, using both aircraft observations and models. We find that the chemical environment and resulting ozone production within smoke changes as plumes evolve, with implications for climate and public health.
Daniel L. Goldberg, M. Omar Nawaz, Congmeng Lyu, Jian He, Annmarie G. Carlton, Shobha Kondragunta, and Susan C. Anenberg
EGUsphere, https://doi.org/10.5194/egusphere-2025-1350, https://doi.org/10.5194/egusphere-2025-1350, 2025
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This research investigates how air quality, specifically NO2 concentrations, is different under clear and cloudy skies. We find that in situ surface NO2 is, on average, +36 % larger during cloudy days versus clear sky days, with a wide distribution based on geographic region and roadway proximity: largest in the Northeast U.S. and smallest in the Southwest U.S. and near major roadways. This has implications for satellite data applications, which only use measurements in the absence of clouds.
Ye Kuang, Biao Luo, Shan Huang, Junwen Liu, Weiwei Hu, Yuwen Peng, Duohong Chen, Dingli Yue, Wanyun Xu, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 25, 3737–3752, https://doi.org/10.5194/acp-25-3737-2025, https://doi.org/10.5194/acp-25-3737-2025, 2025
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This research reveals the potential importance of nighttime NO3 radical chemistry and aerosol water in the rapid formation of secondary brown carbon from diluted biomass burning emissions. The findings enhance our understanding of nighttime biomass burning evolution and its implications for climate and regional air quality, especially regarding interactions with background aerosol water and water-rich fogs and clouds.
Jing Li, Jiaoshi Zhang, Xianda Gong, Steven Spielman, Chongai Kuang, Ashish Singh, Maria A. Zawadowicz, Lu Xu, and Jian Wang
EGUsphere, https://doi.org/10.5194/egusphere-2025-726, https://doi.org/10.5194/egusphere-2025-726, 2025
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Using measurements at a rural coastal site, we quantified aerosols in representative air masses and identified major source of organics in Houston area. Our results show cooking aerosol is likely overestimated by earlier studies. Additionally, diurnal variation of highly oxidized organics is mostly driven by air mass changes instead of photochemistry. This study highlights the impacts of emissions, atmospheric chemistry, and meteorology on aerosol properties in the coastal-rural environment.
Sara L. Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, and Kathleen Fahey
Atmos. Chem. Phys., 25, 3287–3312, https://doi.org/10.5194/acp-25-3287-2025, https://doi.org/10.5194/acp-25-3287-2025, 2025
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters is improved.
Matthew James Rowlinson, Lucy J. Carpenter, Mat J. Evans, James D. Lee, Simone Andersen, Tomas Sherwen, Anna B. Callaghan, Roberto Sommariva, William Bloss, Siqi Hou, Leigh R. Crilley, Klaus Pfeilsticker, Benjamin Weyland, Thomas B. Ryerson, Patrick R. Veres, Pedro Campuzano-Jost, Hongyu Guo, Benjamin A. Nault, Jose L. Jimenez, and Khanneh Wadinga Fomba
EGUsphere, https://doi.org/10.5194/egusphere-2025-830, https://doi.org/10.5194/egusphere-2025-830, 2025
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HONO is key to tropospheric chemistry. Observations show high HONO concentrations in remote air, possibly explained by nitrate aerosol photolysis. We use observational data to parameterize nitrate photolysis, evaluating simulated HONO against observations from multiple sources. We show improved agreement with observed HONO, but large overestimates in NOx and O3, beyond observational constraints. This implies a large uncertainty in the NOx budget and our understanding of atmospheric chemistry.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 18, 881–895, https://doi.org/10.5194/amt-18-881-2025, https://doi.org/10.5194/amt-18-881-2025, 2025
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Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Jan-Lukas Tirpitz, Santo Fedele Colosimo, Nathaniel Brockway, Robert Spurr, Matt Christi, Samuel Hall, Kirk Ullmann, Johnathan Hair, Taylor Shingler, Rodney Weber, Jack Dibb, Richard Moore, Elizabeth Wiggins, Vijay Natraj, Nicolas Theys, and Jochen Stutz
Atmos. Chem. Phys., 25, 1989–2015, https://doi.org/10.5194/acp-25-1989-2025, https://doi.org/10.5194/acp-25-1989-2025, 2025
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We combine plume composition data from the 2019 NASA FIREX-AQ campaign with state-of-the-art radiative transfer modeling techniques to calculate distributions of actinic flux and photolysis frequencies in a wildfire plume. Excellent agreement of the model and observations demonstrates the applicability of this approach to constrain photochemistry in such plumes. We identify limiting factors for the modeling accuracy and discuss spatial and spectral features of the distributions.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, 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
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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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).
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Katerina Seitanidi, Pourya Shahpoury, Eduardo J. d. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech., 18, 177–195, https://doi.org/10.5194/amt-18-177-2025, https://doi.org/10.5194/amt-18-177-2025, 2025
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In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP dithiothreitol assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardisation in OP procedures.
Wendell W. Walters, Masayuki Takeuchi, Danielle E. Blum, Gamze Eris, David Tanner, Weiqi Xu, Jean Rivera-Rios, Fobang Liu, Tianchang Xu, Greg Huey, Justin B. Min, Rodney Weber, Nga L. Ng, and Meredith G. Hastings
EGUsphere, https://doi.org/10.5194/egusphere-2024-3860, https://doi.org/10.5194/egusphere-2024-3860, 2024
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We studied how chemicals released from plants and pollution interact in the atmosphere, affecting air quality and climate. By combining laboratory experiments and chemistry models, we tracked unique chemical fingerprints to understand how nitrogen compounds transform to form particles in the air. Our findings help explain the role of these reactions in pollution and provide tools to improve predictions for cleaner air and better climate policies.
Amna Ijaz, Brice Temime-Roussel, Benjamin Chazeau, Sarah Albertin, Stephen R. Arnold, Brice Barrett, Slimane Bekki, Natalie Brett, Meeta Cesler-Maloney, Elsa Dieudonne, Kayane K. Dingilian, Javier G. Fochesatto, Jingqiu Mao, Allison Moon, Joel Savarino, William Simpson, Rodney J. Weber, Kathy S. Law, and Barbara D'Anna
EGUsphere, https://doi.org/10.5194/egusphere-2024-3789, https://doi.org/10.5194/egusphere-2024-3789, 2024
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Fairbanks is among the most polluted cities with the highest particulate matter (PM) levels in the US during winters. Highly time-resolved measurements of the sub-micron PM elucidated residential heating with wood and oil and hydrocarbon-like organics from traffic, as well as sulphur-containing organic aerosol, to be the key pollution sources. Remarkable differences existed between complementary instruments, warranting the deployment of multiple tools at sites with wide-ranging influences.
Mingfu Cai, Chenshuo Ye, Bin Yuan, Shan Huang, E Zheng, Suxia Yang, Zelong Wang, Yi Lin, Tiange Li, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Baoling Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
Atmos. Chem. Phys., 24, 13065–13079, https://doi.org/10.5194/acp-24-13065-2024, https://doi.org/10.5194/acp-24-13065-2024, 2024
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This study investigated the daytime secondary organic aerosol (SOA) formation in urban plumes. We observed a significant daytime SOA formation through gas–particle partitioning when the site was affected by urban plumes. A box model simulation indicated that urban pollutants (nitrogen oxide and volatile organic compounds) could enhance the oxidizing capacity, while the elevated volatile organic compounds were mainly responsible for promoting daytime SOA formation.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O'Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
Atmos. Chem. Phys., 24, 12749–12773, https://doi.org/10.5194/acp-24-12749-2024, https://doi.org/10.5194/acp-24-12749-2024, 2024
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Prescribed burning is an important method for managing ecosystems and preventing wildfires. However, smoke from prescribed fires can have a significant impact on air quality. Here, using a network of fixed sites and sampling throughout an extended prescribed burning period in 2 different years, we characterize emissions and evolutions of up to 8 h of PM2.5 mass, black carbon (BC), and brown carbon (BrC) in smoke from burning of forested lands in the southeastern USA.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
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
Atmos. Chem. Phys., 24, 10985–11004, https://doi.org/10.5194/acp-24-10985-2024, https://doi.org/10.5194/acp-24-10985-2024, 2024
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We examined aerosol particles from wildfires and identified tarballs (TBs) from the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. This study reveals the compositions, abundance, sizes, and mixing states of TBs and shows that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass-burning events and ages, enhancing our knowledge of TB emissions and our understanding of their climate impact.
Jiemei Liu, Jesper H. Christensen, Zhuyun Ye, Shikui Dong, Camilla Geels, Jørgen Brandt, Athanasios Nenes, Yuan Yuan, and Ulas Im
Atmos. Chem. Phys., 24, 10849–10867, https://doi.org/10.5194/acp-24-10849-2024, https://doi.org/10.5194/acp-24-10849-2024, 2024
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China was chosen as an example to conduct a quantitative analysis using the Danish Eulerian Hemispheric Model (DEHM) system with meteorological input from the Weather Research and Forecasting (WRF) model. Meteorological conditions and emission inventories contributed 46 % (65 %) and 54 % (35 %) to the variations in PM2.5 concentrations (oxidative potential – OP), respectively, highlighting secondary aerosol formation and biomass burning as the primary contributors to PM2.5 and OP levels.
Manu Anna Thomas, Klaus Wyser, Shiyu Wang, Marios Chatziparaschos, Paraskevi Georgakaki, Montserrat Costa-Surós, Maria Gonçalves Ageitos, Maria Kanakidou, Carlos Pérez García-Pando, Athanasios Nenes, Twan van Noije, Philippe Le Sager, and Abhay Devasthale
Geosci. Model Dev., 17, 6903–6927, https://doi.org/10.5194/gmd-17-6903-2024, https://doi.org/10.5194/gmd-17-6903-2024, 2024
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Aerosol–cloud interactions occur at a range of spatio-temporal scales. While evaluating recent developments in EC-Earth3-AerChem, this study aims to understand the extent to which the Twomey effect manifests itself at larger scales. We find a reduction in the warm bias over the Southern Ocean due to model improvements. While we see footprints of the Twomey effect at larger scales, the negative relationship between cloud droplet number and liquid water drives the shortwave radiative effect.
Kunfeng Gao, Franziska Vogel, Romanos Foskinis, Stergios Vratolis, Maria I. Gini, Konstantinos Granakis, Anne-Claire Billault-Roux, Paraskevi Georgakaki, Olga Zografou, Prodromos Fetfatzis, Alexis Berne, Alexandros Papayannis, Konstantinos Eleftheridadis, Ottmar Möhler, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9939–9974, https://doi.org/10.5194/acp-24-9939-2024, https://doi.org/10.5194/acp-24-9939-2024, 2024
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Ice nucleating particle (INP) concentrations are required for correct predictions of clouds and precipitation in a changing climate, but they are poorly constrained in climate models. We unravel source contributions to INPs in the eastern Mediterranean and find that biological particles are important, regardless of their origin. The parameterizations developed exhibit superior performance and enable models to consider biological-particle effects on INPs.
Romanos Foskinis, Ghislain Motos, Maria I. Gini, Olga Zografou, Kunfeng Gao, Stergios Vratolis, Konstantinos Granakis, Ville Vakkari, Kalliopi Violaki, Andreas Aktypis, Christos Kaltsonoudis, Zongbo Shi, Mika Komppula, Spyros N. Pandis, Konstantinos Eleftheriadis, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9827–9842, https://doi.org/10.5194/acp-24-9827-2024, https://doi.org/10.5194/acp-24-9827-2024, 2024
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Analysis of modeling, in situ, and remote sensing measurements reveals the microphysical state of orographic clouds and their response to aerosol from the boundary layer and free troposphere. We show that cloud response to aerosol is robust, as predicted supersaturation and cloud droplet number levels agree with those determined from in-cloud measurements. The ability to determine if clouds are velocity- or aerosol-limited allows for novel model constraints and remote sensing products.
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
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
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
Atmos. Meas. Tech., 17, 4915–4939, https://doi.org/10.5194/amt-17-4915-2024, https://doi.org/10.5194/amt-17-4915-2024, 2024
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This study systematically characterizes the temperature enhancement in the lamp-enclosed oxidation flow reactor (OFR). The enhancement varied multiple dimensional factors, emphasizing the complexity of temperature inside of OFR. The effects of temperature on the flow field and gas- or particle-phase reaction inside OFR were also evaluated with experiments and model simulations. Finally, multiple mitigation strategies were demonstrated to minimize this temperature increase.
Edward J. Strobach, Sunil Baidar, Brian J. Carroll, Steven S. Brown, Kristen Zuraski, Matthew Coggon, Chelsea E. Stockwell, Lu Xu, Yelena L. Pichugina, W. Alan Brewer, Carsten Warneke, Jeff Peischl, Jessica Gilman, Brandi McCarty, Maxwell Holloway, and Richard Marchbanks
Atmos. Chem. Phys., 24, 9277–9307, https://doi.org/10.5194/acp-24-9277-2024, https://doi.org/10.5194/acp-24-9277-2024, 2024
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Large-scale weather patterns are isolated from local patterns to study the impact that different weather scales have on air quality measurements. While impacts from large-scale meteorology were evaluated by separating ozone (O3) exceedance (>70 ppb) and non-exceedance (<70 ppb) days, we developed a technique that allows direct comparisons of small temporal variations between chemical and dynamics measurements under rapid dynamical transitions.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Cassandra J. Gaston, Joseph M. Prospero, Kristen Foley, Havala O. T. Pye, Lillian Custals, Edmund Blades, Peter Sealy, and James A. Christie
Atmos. Chem. Phys., 24, 8049–8066, https://doi.org/10.5194/acp-24-8049-2024, https://doi.org/10.5194/acp-24-8049-2024, 2024
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To understand how changing emissions have impacted aerosols in remote regions, we measured nitrate and sulfate in Barbados and compared them to model predictions from EPA’s Air QUAlity TimE Series (EQUATES). Nitrate was stable, except for spikes in 2008 and 2010 due to transported smoke. Sulfate decreased in the 1990s due to reductions in sulfur dioxide (SO2) in the US and Europe; then it increased in the 2000s, likely due to anthropogenic emissions from Africa.
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.
Chuanyang Shen, Xiaoyan Yang, Joel Thornton, John Shilling, Chenyang Bi, Gabriel Isaacman-VanWertz, and Haofei Zhang
Atmos. Chem. Phys., 24, 6153–6175, https://doi.org/10.5194/acp-24-6153-2024, https://doi.org/10.5194/acp-24-6153-2024, 2024
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In this work, a condensed multiphase isoprene oxidation mechanism was developed to simulate isoprene SOA formation from chamber and field studies. Our results show that the measured isoprene SOA mass concentrations can be reasonably reproduced. The simulation results indicate that multifunctional low-volatility products contribute significantly to total isoprene SOA. Our findings emphasize that the pathways to produce these low-volatility species should be considered in models.
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.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Marios Chatziparaschos, Stelios Myriokefalitakis, Nikos Kalivitis, Nikos Daskalakis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Mihalis Vrekoussis, and Maria Kanakidou
EGUsphere, https://doi.org/10.5194/egusphere-2024-952, https://doi.org/10.5194/egusphere-2024-952, 2024
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We show distinct seasonal and geographical patterns in the contributions of mineral dust, marine and terrestrial biological particles to ice-nucleating particles (INP) concentrations that lead to atmospheric ice formation, a major source of uncertainty in climate predictions. Bioaerosols are the major source of INP at high temperatures, while mineral dust influences the global INP population at lower temperatures. These particles can satisfactorily reproduce INP in a climate model.
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Qian Li, Maor Gabay, Chen Dayan, Pawel Misztal, Alex Guenther, Erick Fredj, and Eran Tas
EGUsphere, https://doi.org/10.5194/egusphere-2024-717, https://doi.org/10.5194/egusphere-2024-717, 2024
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Biogenic volatile organic compounds (BVOCs) affect the climate and air quality, while their emission from terrestrial vegetation is affected by drought in a way that is not well characterized. Our study reveals that the instantaneous intraday changes in meteorological conditions serve as a better proxy for drought-related variations in BVOCs emission rate than the absolute values of the meteorological parameters, advancing our understanding of BVOCs emission effects under climate change.
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.
Karl Espen Yttri, Are Bäcklund, Franz Conen, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Anne Kasper-Giebl, Avram Gold, Hans Gundersen, Cathrine Lund Myhre, Stephen Matthew Platt, David Simpson, Jason D. Surratt, Sönke Szidat, Martin Rauber, Kjetil Tørseth, Martin Album Ytre-Eide, Zhenfa Zhang, and Wenche Aas
Atmos. Chem. Phys., 24, 2731–2758, https://doi.org/10.5194/acp-24-2731-2024, https://doi.org/10.5194/acp-24-2731-2024, 2024
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We discuss carbonaceous aerosol (CA) observed at the high Arctic Zeppelin Observatory (2017 to 2020). We find that organic aerosol is a significant fraction of the Arctic aerosol, though less than sea salt aerosol and mineral dust, as well as non-sea-salt sulfate, originating mainly from anthropogenic sources in winter and from natural sources in summer, emphasizing the importance of wildfires for biogenic secondary organic aerosol and primary biological aerosol particles observed in the Arctic.
Elyse A. Pennington, Yuan Wang, Benjamin C. Schulze, Karl M. Seltzer, Jiani Yang, Bin Zhao, Zhe Jiang, Hongru Shi, Melissa Venecek, Daniel Chau, Benjamin N. Murphy, Christopher M. Kenseth, Ryan X. Ward, Havala O. T. Pye, and John H. Seinfeld
Atmos. Chem. Phys., 24, 2345–2363, https://doi.org/10.5194/acp-24-2345-2024, https://doi.org/10.5194/acp-24-2345-2024, 2024
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To assess the air quality in Los Angeles (LA), we improved the CMAQ model by using dynamic traffic emissions and new secondary organic aerosol schemes to represent volatile chemical products. Source apportionment demonstrates that the urban areas of the LA Basin and vicinity are NOx-saturated, with the largest sensitivity of O3 to changes in volatile organic compounds in the urban core. The improvement and remaining issues shed light on the future direction of the model development.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
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This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
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.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
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.
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.
Ghislain Motos, Gabriel Freitas, Paraskevi Georgakaki, Jörg Wieder, Guangyu Li, Wenche Aas, Chris Lunder, Radovan Krejci, Julie Thérèse Pasquier, Jan Henneberger, Robert Oscar David, Christoph Ritter, Claudia Mohr, Paul Zieger, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13941–13956, https://doi.org/10.5194/acp-23-13941-2023, https://doi.org/10.5194/acp-23-13941-2023, 2023
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Low-altitude clouds play a key role in regulating the climate of the Arctic, a region that suffers from climate change more than any other on the planet. We gathered meteorological and aerosol physical and chemical data over a year and utilized them for a parameterization that help us unravel the factors driving and limiting the efficiency of cloud droplet formation. We then linked this information to the sources of aerosol found during each season and to processes of cloud glaciation.
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.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu Jathar, Li Li, Andrew A. May, and Allen L. Robinson
Atmos. Chem. Phys., 23, 13469–13483, https://doi.org/10.5194/acp-23-13469-2023, https://doi.org/10.5194/acp-23-13469-2023, 2023
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We update methods for calculating organic particle and vapor emissions from mobile sources in the USA. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
James F. Hurley, Alejandra Caceres, Deborah F. McGlynn, Mary E. Tovillo, Suzanne Pinar, Roger Schürch, Ksenia Onufrieva, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4681–4692, https://doi.org/10.5194/amt-16-4681-2023, https://doi.org/10.5194/amt-16-4681-2023, 2023
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Volatile organic compounds (VOCs) have a wide range of sources and impacts on environments and human health that make them spatially, temporally, and chemically varied. Current methods lack the ability to collect samples in ways that provide spatial and chemical resolution without complex, costly instrumentation. We describe and validate a low-cost, portable VOC sampler and demonstrate its utility in collecting distributed coordinated samples.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
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.
Namrata Shanmukh Panji and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4319–4330, https://doi.org/10.5194/amt-16-4319-2023, https://doi.org/10.5194/amt-16-4319-2023, 2023
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Measuring volatile organic compounds (VOCs) in the atmosphere is crucial for understanding air quality and environmental impact. Since these compounds are present in low concentrations, preconcentration of samples is often necessary for accurate detection. To address this issue, we have developed a novel inlet that uses selective permeation to concentrate organic gases in small sample flows. This device offers a promising approach for accurately detecting low levels of VOCs in the atmosphere.
Guangyu Li, Elise K. Wilbourn, Zezhen Cheng, Jörg Wieder, Allison Fagerson, Jan Henneberger, Ghislain Motos, Rita Traversi, Sarah D. Brooks, Mauro Mazzola, Swarup China, Athanasios Nenes, Ulrike Lohmann, Naruki Hiranuma, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 10489–10516, https://doi.org/10.5194/acp-23-10489-2023, https://doi.org/10.5194/acp-23-10489-2023, 2023
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In this work, we present results from an Arctic field campaign (NASCENT) in Ny-Ålesund, Svalbard, on the abundance, variability, physicochemical properties, and potential sources of ice-nucleating particles (INPs) relevant for mixed-phase cloud formation. This work improves the data coverage of Arctic INPs and aerosol properties, allowing for the validation of models predicting cloud microphysical and radiative properties of mixed-phase clouds in the rapidly warming Arctic.
Anne-Claire Billault-Roux, Paraskevi Georgakaki, Josué Gehring, Louis Jaffeux, Alfons Schwarzenboeck, Pierre Coutris, Athanasios Nenes, and Alexis Berne
Atmos. Chem. Phys., 23, 10207–10234, https://doi.org/10.5194/acp-23-10207-2023, https://doi.org/10.5194/acp-23-10207-2023, 2023
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Secondary ice production plays a key role in clouds and precipitation. In this study, we analyze radar measurements from a snowfall event in the Jura Mountains. Complex signatures are observed, which reveal that ice crystals were formed through various processes. An analysis of multi-sensor data suggests that distinct ice multiplication processes were taking place. Both the methods used and the insights gained through this case study contribute to a better understanding of snowfall microphysics.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, https://doi.org/10.5194/acp-23-10057-2023, 2023
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Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Bryan K. Place, William T. Hutzell, K. Wyat Appel, Sara Farrell, Lukas Valin, Benjamin N. Murphy, Karl M. Seltzer, Golam Sarwar, Christine Allen, Ivan R. Piletic, Emma L. D'Ambro, Emily Saunders, Heather Simon, Ana Torres-Vasquez, Jonathan Pleim, Rebecca H. Schwantes, Matthew M. Coggon, Lu Xu, William R. Stockwell, and Havala O. T. Pye
Atmos. Chem. Phys., 23, 9173–9190, https://doi.org/10.5194/acp-23-9173-2023, https://doi.org/10.5194/acp-23-9173-2023, 2023
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Ground-level ozone is a pollutant with adverse human health and ecosystem effects. Air quality models allow scientists to understand the chemical production of ozone and demonstrate impacts of air quality management plans. In this work, the role of multiple systems in ozone production was investigated for the northeastern US in summer. Model updates to chemical reaction rates and monoterpene chemistry were most influential in decreasing predicted ozone and improving agreement with observations.
Yiyu Cai, Chenshuo Ye, Wei Chen, Weiwei Hu, Wei Song, Yuwen Peng, Shan Huang, Jipeng Qi, Sihang Wang, Chaomin Wang, Caihong Wu, Zelong Wang, Baolin Wang, Xiaofeng Huang, Lingyan He, Sasho Gligorovski, Bin Yuan, Min Shao, and Xinming Wang
Atmos. Chem. Phys., 23, 8855–8877, https://doi.org/10.5194/acp-23-8855-2023, https://doi.org/10.5194/acp-23-8855-2023, 2023
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We studied the variability and molecular composition of ambient oxidized organic nitrogen (OON) in both gas and particle phases using a state-of-the-art online mass spectrometer in urban air. Biomass burning and secondary formation were found to be the two major sources of OON. Daytime nitrate radical chemistry for OON formation was more important than previously thought. Our results improved the understanding of the sources and molecular composition of OON in the polluted urban atmosphere.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
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.
Molly Frauenheim, Jason D. Surratt, Zhenfa Zhang, and Avram Gold
Atmos. Chem. Phys., 23, 7859–7866, https://doi.org/10.5194/acp-23-7859-2023, https://doi.org/10.5194/acp-23-7859-2023, 2023
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We report synthesis of the isoprene-derived photochemical oxidation products trans- and cis-β-epoxydiols in high overall yields from inexpensive, readily available starting compounds. Protection/deprotection steps or time-consuming purification is not required, and the reactions can be scaled up to gram quantities. The procedures provide accessibility of these important compounds to atmospheric chemistry laboratories with only basic capabilities in organic synthesis.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
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The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
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.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Emily D. Lenhardt, Lan Gao, Jens Redemann, Feng Xu, Sharon P. Burton, Brian Cairns, Ian Chang, Richard A. Ferrare, Chris A. Hostetler, Pablo E. Saide, Calvin Howes, Yohei Shinozuka, Snorre Stamnes, Mary Kacarab, Amie Dobracki, Jenny Wong, Steffen Freitag, and Athanasios Nenes
Atmos. Meas. Tech., 16, 2037–2054, https://doi.org/10.5194/amt-16-2037-2023, https://doi.org/10.5194/amt-16-2037-2023, 2023
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Small atmospheric particles, such as smoke from wildfires or pollutants from human activities, impact cloud properties, and clouds have a strong influence on climate. To better understand the distributions of these particles, we develop relationships to derive their concentrations from remote sensing measurements from an instrument called a lidar. Our method is reliable for smoke particles, and similar steps can be taken to develop relationships for other particle types.
Forwood Wiser, Bryan K. Place, Siddhartha Sen, Havala O. T. Pye, Benjamin Yang, Daniel M. Westervelt, Daven K. Henze, Arlene M. Fiore, and V. Faye McNeill
Geosci. Model Dev., 16, 1801–1821, https://doi.org/10.5194/gmd-16-1801-2023, https://doi.org/10.5194/gmd-16-1801-2023, 2023
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We developed a reduced model of atmospheric isoprene oxidation, AMORE-Isoprene 1.0. It was created using a new Automated Model Reduction (AMORE) method designed to simplify complex chemical mechanisms with minimal manual adjustments to the output. AMORE-Isoprene 1.0 has improved accuracy and similar size to other reduced isoprene mechanisms. When included in the CRACMM mechanism, it improved the accuracy of EPA’s CMAQ model predictions for the northeastern USA compared to observations.
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+.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys., 23, 1785–1801, https://doi.org/10.5194/acp-23-1785-2023, https://doi.org/10.5194/acp-23-1785-2023, 2023
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Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
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.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Deborah F. McGlynn, Graham Frazier, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Biogeosciences, 20, 45–55, https://doi.org/10.5194/bg-20-45-2023, https://doi.org/10.5194/bg-20-45-2023, 2023
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Using a custom-made gas chromatography flame ionization detector, 2 years of speciated hourly biogenic volatile organic compound data were collected in a forest in central Virginia. We identify diurnal and seasonal variability in the data, which is shown to impact atmospheric oxidant budgets. A comparison with emission models identified discrepancies with implications for model outcomes. We suggest increased monitoring of speciated biogenic volatile organic compounds to improve modeled results.
Daniel J. Bryant, Beth S. Nelson, Stefan J. Swift, Sri Hapsari Budisulistiorini, Will S. Drysdale, Adam R. Vaughan, Mike J. Newland, James R. Hopkins, James M. Cash, Ben Langford, Eiko Nemitz, W. Joe F. Acton, C. Nicholas Hewitt, Tuhin Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 23, 61–83, https://doi.org/10.5194/acp-23-61-2023, https://doi.org/10.5194/acp-23-61-2023, 2023
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This paper investigates the sources of isoprene and monoterpene compounds and their particulate-phase oxidation products in Delhi, India. This was done to improve our understanding of the sources, concentrations, and fate of volatile emissions in megacities. By studying the chemical composition of offline filter samples, we report that a significant share of the oxidised organic aerosol in Delhi is from isoprene and monoterpenes. This has implications for human health and policy development.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Ziqi Gao, Yifeng Wang, Petros Vasilakos, Cesunica E. Ivey, Khanh Do, and Armistead G. Russell
Geosci. Model Dev., 15, 9015–9029, https://doi.org/10.5194/gmd-15-9015-2022, https://doi.org/10.5194/gmd-15-9015-2022, 2022
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While the national ambient air quality standard of ozone is based on the 3-year average of the fourth highest 8 h maximum (MDA8) ozone concentrations, these predicted extreme values using numerical methods are always biased low. We built four computational models (GAM, MARS, random forest and SVR) to predict the fourth highest MDA8 ozone in Southern California using precursor emissions, meteorology and climatological patterns. All models presented acceptable performance, with GAM being the best.
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.
Rebecca A. Wernis, Nathan M. Kreisberg, Robert J. Weber, Greg T. Drozd, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 14987–15019, https://doi.org/10.5194/acp-22-14987-2022, https://doi.org/10.5194/acp-22-14987-2022, 2022
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We measured volatile and intermediate-volatility gases and semivolatile gas- and particle-phase compounds in the atmosphere during an 11 d period in a Bay Area suburb. We separated compounds based on variability in time to arrive at 13 distinct sources. Some compounds emitted from plants are found in greater quantities as fragrance compounds in consumer products. The wide volatility range of these measurements enables the construction of more complete source profiles.
Haichao Wang, Bin Yuan, E Zheng, Xiaoxiao Zhang, Jie Wang, Keding Lu, Chenshuo Ye, Lei Yang, Shan Huang, Weiwei Hu, Suxia Yang, Yuwen Peng, Jipeng Qi, Sihang Wang, Xianjun He, Yubin Chen, Tiange Li, Wenjie Wang, Yibo Huangfu, Xiaobing Li, Mingfu Cai, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 22, 14837–14858, https://doi.org/10.5194/acp-22-14837-2022, https://doi.org/10.5194/acp-22-14837-2022, 2022
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We present intensive field measurement of ClNO2 in the Pearl River Delta in 2019. Large variation in the level, formation, and atmospheric impacts of ClNO2 was found in different air masses. ClNO2 formation was limited by the particulate chloride (Cl−) and aerosol surface area. Our results reveal that Cl− originated from various anthropogenic emissions rather than sea sources and show minor contribution to the O3 pollution and photochemistry.
Peeyush Khare, Jordan E. Krechmer, Jo E. Machesky, Tori Hass-Mitchell, Cong Cao, Junqi Wang, Francesca Majluf, Felipe Lopez-Hilfiker, Sonja Malek, Will Wang, Karl Seltzer, Havala O. T. Pye, Roisin Commane, Brian C. McDonald, Ricardo Toledo-Crow, John E. Mak, and Drew R. Gentner
Atmos. Chem. Phys., 22, 14377–14399, https://doi.org/10.5194/acp-22-14377-2022, https://doi.org/10.5194/acp-22-14377-2022, 2022
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Ammonium adduct chemical ionization is used to examine the atmospheric abundances of oxygenated volatile organic compounds associated with emissions from volatile chemical products, which are now key contributors of reactive precursors to ozone and secondary organic aerosols in urban areas. The application of this valuable measurement approach in densely populated New York City enables the evaluation of emissions inventories and thus the role these oxygenated compounds play in urban air quality.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
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.
Biao Luo, Ye Kuang, Shan Huang, Qicong Song, Weiwei Hu, Wei Li, Yuwen Peng, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 22, 12401–12415, https://doi.org/10.5194/acp-22-12401-2022, https://doi.org/10.5194/acp-22-12401-2022, 2022
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We performed comprehensive analysis on biomass burning organic aerosol (BBOA) size distributions, as well as mass scattering and absorption efficiencies, with an improved method of on-line quantification of brown carbon absorptions. Both BBOA volume size distribution and retrieved refractive index depend highly on combustion conditions represented by the black carbon content, which has significant implications for BBOA climate effect simulations.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Sungwoo Kim, Brian M. Lerner, Donna T. Sueper, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 15, 5061–5075, https://doi.org/10.5194/amt-15-5061-2022, https://doi.org/10.5194/amt-15-5061-2022, 2022
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Atmospheric samples can be complex, and current analysis methods often require substantial human interaction and discard potentially important information. To improve analysis accuracy and computational cost of these large datasets, we developed an automated analysis algorithm that utilizes a factor analysis approach coupled with a decision tree. We demonstrate that this algorithm cataloged approximately 10 times more analytes compared to a manual analysis and in a quarter of the analysis time.
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.
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.
Yutong Liang, Christos Stamatis, Edward C. Fortner, Rebecca A. Wernis, Paul Van Rooy, Francesca Majluf, Tara I. Yacovitch, Conner Daube, Scott C. Herndon, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 9877–9893, https://doi.org/10.5194/acp-22-9877-2022, https://doi.org/10.5194/acp-22-9877-2022, 2022
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This article reports the measurements of organic compounds emitted from western US wildfires. We identified and quantified 240 particle-phase compounds and 72 gas-phase compounds emitted in wildfire and related the emissions to the modified combustion efficiency. Higher emissions of diterpenoids and monoterpenes were observed, likely due to distillation from unburned heated vegetation. Our results can benefit future source apportionment and modeling studies as well as exposure assessments.
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.
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.
Yihang Yu, Peng Cheng, Huirong Li, Wenda Yang, Baobin Han, Wei Song, Weiwei Hu, Xinming Wang, Bin Yuan, Min Shao, Zhijiong Huang, Zhen Li, Junyu Zheng, Haichao Wang, and Xiaofang Yu
Atmos. Chem. Phys., 22, 8951–8971, https://doi.org/10.5194/acp-22-8951-2022, https://doi.org/10.5194/acp-22-8951-2022, 2022
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We have investigated the budget of HONO at an urban site in Guangzhou. Budget and comprehensive uncertainty analysis suggest that at such locations as ours, HONO direct emissions and NO + OH can become comparable or even surpass other HONO sources that typically receive greater attention and interest, such as the NO2 heterogeneous source and the unknown daytime photolytic source. Our findings emphasize the need to reduce the uncertainties of both conventional and novel HONO sources and sinks.
Emily B. Franklin, Lindsay D. Yee, Bernard Aumont, Robert J. Weber, Paul Grigas, and Allen H. Goldstein
Atmos. Meas. Tech., 15, 3779–3803, https://doi.org/10.5194/amt-15-3779-2022, https://doi.org/10.5194/amt-15-3779-2022, 2022
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The composition of atmospheric aerosols are extremely complex, containing hundreds of thousands of estimated individual compounds. The majority of these compounds have never been catalogued in widely used databases, making them extremely difficult for atmospheric chemists to identify and analyze. In this work, we present Ch3MS-RF, a machine-learning-based model to enable characterization of complex mixtures and prediction of structure-specific properties of unidentifiable organic compounds.
Mingfu Cai, Shan Huang, Baoling Liang, Qibin Sun, Li Liu, Bin Yuan, Min Shao, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Zelong Wang, Duohong Chen, Haobo Tan, Hanbin Xu, Fei Li, Xuejiao Deng, Tao Deng, Jiaren Sun, and Jun Zhao
Atmos. Chem. Phys., 22, 8117–8136, https://doi.org/10.5194/acp-22-8117-2022, https://doi.org/10.5194/acp-22-8117-2022, 2022
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This study investigated the size dependence and diurnal variation in organic aerosol hygroscopicity, volatility, and cloud condensation nuclei (CCN) activity. We found that the physical properties of OA could vary in a large range at different particle sizes and affected the number concentration of CCN (NCCN) at all supersaturations. Our results highlight the importance of evaluating the atmospheric evolution processes of OA at different size ranges and their impact on climate effects.
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.
Andrew J. Lindsay, Daniel C. Anderson, Rebecca A. Wernis, Yutong Liang, Allen H. Goldstein, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Ed C. Fortner, Philip L. Croteau, Francesca Majluf, Jordan E. Krechmer, Tara I. Yacovitch, Walter B. Knighton, and Ezra C. Wood
Atmos. Chem. Phys., 22, 4909–4928, https://doi.org/10.5194/acp-22-4909-2022, https://doi.org/10.5194/acp-22-4909-2022, 2022
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Wildfire smoke dramatically impacts air quality and often has elevated concentrations of ozone. We present measurements of ozone and its precursors at a rural site periodically impacted by wildfire smoke. Measurements of total peroxy radicals, key ozone precursors that have been studied little within wildfires, compare well with chemical box model predictions. Our results indicate no serious issues with using current chemistry mechanisms to model chemistry in aged wildfire plumes.
Suxia Yang, Bin Yuan, Yuwen Peng, Shan Huang, Wei Chen, Weiwei Hu, Chenglei Pei, Jun Zhou, David D. Parrish, Wenjie Wang, Xianjun He, Chunlei Cheng, Xiao-Bing Li, Xiaoyun Yang, Yu Song, Haichao Wang, Jipeng Qi, Baolin Wang, Chen Wang, Chaomin Wang, Zelong Wang, Tiange Li, E Zheng, Sihang Wang, Caihong Wu, Mingfu Cai, Chenshuo Ye, Wei Song, Peng Cheng, Duohong Chen, Xinming Wang, Zhanyi Zhang, Xuemei Wang, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4539–4556, https://doi.org/10.5194/acp-22-4539-2022, https://doi.org/10.5194/acp-22-4539-2022, 2022
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We use a model constrained using observations to study the formation of nitrate aerosol in and downwind of a representative megacity. We found different contributions of various chemical reactions to ground-level nitrate concentrations between urban and suburban regions. We also show that controlling VOC emissions are effective for decreasing nitrate formation in both urban and regional environments, although VOCs are not direct precursors of nitrate aerosol.
Stelios Myriokefalitakis, Elisa Bergas-Massó, María Gonçalves-Ageitos, Carlos Pérez García-Pando, Twan van Noije, Philippe Le Sager, Akinori Ito, Eleni Athanasopoulou, Athanasios Nenes, Maria Kanakidou, Maarten C. Krol, and Evangelos Gerasopoulos
Geosci. Model Dev., 15, 3079–3120, https://doi.org/10.5194/gmd-15-3079-2022, https://doi.org/10.5194/gmd-15-3079-2022, 2022
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We here describe the implementation of atmospheric multiphase processes in the EC-Earth Earth system model. We provide global budgets of oxalate, sulfate, and iron-containing aerosols, along with an analysis of the links among atmospheric composition, aqueous-phase processes, and aerosol dissolution, supported by comparison to observations. This work is a first step towards an interactive calculation of the deposition of bioavailable atmospheric iron coupled to the model’s ocean component.
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.
Wenjie Wang, Bin Yuan, Yuwen Peng, Hang Su, Yafang Cheng, Suxia Yang, Caihong Wu, Jipeng Qi, Fengxia Bao, Yibo Huangfu, Chaomin Wang, Chenshuo Ye, Zelong Wang, Baolin Wang, Xinming Wang, Wei Song, Weiwei Hu, Peng Cheng, Manni Zhu, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4117–4128, https://doi.org/10.5194/acp-22-4117-2022, https://doi.org/10.5194/acp-22-4117-2022, 2022
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From thorough measurements of numerous oxygenated volatile organic compounds, we show that their photodissociation can be important for radical production and ozone formation in the atmosphere. This effect was underestimated in previous studies, as measurements of them were lacking.
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.
Xiajie Yang, Qiaoqiao Wang, Nan Ma, Weiwei Hu, Yang Gao, Zhijiong Huang, Junyu Zheng, Bin Yuan, Ning Yang, Jiangchuan Tao, Juan Hong, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3743–3762, https://doi.org/10.5194/acp-22-3743-2022, https://doi.org/10.5194/acp-22-3743-2022, 2022
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We use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for N2O5 ＋ Cl chemistry to investigate the impacts of chlorine chemistry on air quality in China. Our study not only significantly improves the model's performance but also demonstrates the importance of non-sea-salt chlorine sources as well as an appropriate parameterization for N2O5 ＋ Cl chemistry to the impact of chlorine chemistry in China.
Paraskevi Georgakaki, Georgia Sotiropoulou, Étienne Vignon, Anne-Claire Billault-Roux, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 22, 1965–1988, https://doi.org/10.5194/acp-22-1965-2022, https://doi.org/10.5194/acp-22-1965-2022, 2022
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The modelling study focuses on the importance of ice multiplication processes in orographic mixed-phase clouds, which is one of the least understood cloud types in the climate system. We show that the consideration of ice seeding and secondary ice production through ice–ice collisional breakup is essential for correct predictions of precipitation in mountainous terrain, with important implications for radiation processes.
Delaney B. Kilgour, Gordon A. Novak, Jon S. Sauer, Alexia N. Moore, Julie Dinasquet, Sarah Amiri, Emily B. Franklin, Kathryn Mayer, Margaux Winter, Clare K. Morris, Tyler Price, Francesca Malfatti, Daniel R. Crocker, Christopher Lee, Christopher D. Cappa, Allen H. Goldstein, Kimberly A. Prather, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 1601–1613, https://doi.org/10.5194/acp-22-1601-2022, https://doi.org/10.5194/acp-22-1601-2022, 2022
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We report measurements of gas-phase volatile organosulfur molecules made during a mesocosm phytoplankton bloom experiment. Dimethyl sulfide (DMS), methanethiol (MeSH), and benzothiazole accounted for on average over 90 % of total gas-phase sulfur emissions. This work focuses on factors controlling the production and emission of DMS and MeSH and the role of non-DMS molecules (such as MeSH and benzothiazole) in secondary sulfate formation in coastal marine environments.
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.
Michael A. Battaglia Jr., Nicholas Balasus, Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 18271–18281, https://doi.org/10.5194/acp-21-18271-2021, https://doi.org/10.5194/acp-21-18271-2021, 2021
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This study characterizes aerosol liquid water content and aerosol pH at a land–water transition site near Baltimore, Maryland. We characterize the effects of unique meteorology associated with the close proximity to the Chesapeake Bay and episodic NH3 events derived from industrial and agricultural sources on aerosol chemistry during the summer. We also examine two events where primary Bay emissions underwent aging in the polluted urban atmosphere.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 21, 17865–17883, https://doi.org/10.5194/acp-21-17865-2021, https://doi.org/10.5194/acp-21-17865-2021, 2021
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We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are 4 times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with the high PM levels that develop.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714, https://doi.org/10.5194/acp-21-17687-2021, https://doi.org/10.5194/acp-21-17687-2021, 2021
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Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
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.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Deborah F. McGlynn, Laura E. R. Barry, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 21, 15755–15770, https://doi.org/10.5194/acp-21-15755-2021, https://doi.org/10.5194/acp-21-15755-2021, 2021
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We present 1 year of hourly measurements of chemically resolved Biogenic volatile organic compound (BVOCs) between 15 September 2019 and 15 September 2020, collected at a research tower in central Virginia. Concentrations of a range of BVOCs are described and examined for their impact on atmospheric reactivity. The majority of reactivity comes from α-pinene and limonene, highlighting the importance of both concentration and structure in assessing atmospheric impacts of emissions.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Chenyang Bi, Jordan E. Krechmer, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6551–6560, https://doi.org/10.5194/amt-14-6551-2021, https://doi.org/10.5194/amt-14-6551-2021, 2021
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Calibration techniques have been recently developed to log-linearly correlate analyte sensitivity with CIMS operating conditions particularly for compounds without authentic standards. In this work, we examine the previously ignored bias in the log-linear-based calibration method and estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A step-by-step guide was provided to reduce and even remove the bias.
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.
Rebecca A. Wernis, Nathan M. Kreisberg, Robert J. Weber, Yutong Liang, John Jayne, Susanne Hering, and Allen H. Goldstein
Atmos. Meas. Tech., 14, 6533–6550, https://doi.org/10.5194/amt-14-6533-2021, https://doi.org/10.5194/amt-14-6533-2021, 2021
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cTAG is a new scientific instrument that measures concentrations of organic chemicals in the atmosphere. cTAG is the first instrument capable of measuring small, light chemicals as well as heavier chemicals and everything in between on a single detector, every hour. In this work we explain how cTAG works and some of the tests we performed to verify that it works properly and reliably. We also present measurements of alkanes that suggest they have three dominant sources in a Bay Area suburb.
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.
Linghan Zeng, Amy P. Sullivan, Rebecca A. Washenfelder, Jack Dibb, Eric Scheuer, Teresa L. Campos, Joseph M. Katich, Ezra Levin, Michael A. Robinson, and Rodney J. Weber
Atmos. Meas. Tech., 14, 6357–6378, https://doi.org/10.5194/amt-14-6357-2021, https://doi.org/10.5194/amt-14-6357-2021, 2021
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Three online systems for measuring water-soluble brown carbon are compared. A mist chamber and two different particle-into-liquid samplers were deployed on separate research aircraft targeting wildfires and followed a similar detection method using a long-path liquid waveguide with a spectrometer to measure the light absorption from 300 to 700 nm. Detection limits, signal hysteresis and other sampling issues are compared, and further improvements of these liquid-based systems are provided.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, https://doi.org/10.5194/acp-21-13051-2021, 2021
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Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
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.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Ye Kuang, Shan Huang, Biao Xue, Biao Luo, Qicong Song, Wei Chen, Weiwei Hu, Wei Li, Pusheng Zhao, Mingfu Cai, Yuwen Peng, Jipeng Qi, Tiange Li, Sihang Wang, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 21, 10375–10391, https://doi.org/10.5194/acp-21-10375-2021, https://doi.org/10.5194/acp-21-10375-2021, 2021
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We found that organic aerosol factors with identified sources perform much better than oxidation level parameters in characterizing variations in organic aerosol hygroscopicity, and secondary aerosol formations associated with different sources have distinct effects on organic aerosol hygroscopicity. It reveals that source-oriented organic aerosol hygroscopicity investigations might result in more appropriate parameterization approaches in chemical and climate models.
James M. Cash, Ben Langford, Chiara Di Marco, Neil J. Mullinger, James Allan, Ernesto Reyes-Villegas, Ruthambara Joshi, Mathew R. Heal, W. Joe F. Acton, C. Nicholas Hewitt, Pawel K. Misztal, Will Drysdale, Tuhin K. Mandal, Shivani, Ranu Gadi, Bhola Ram Gurjar, and Eiko Nemitz
Atmos. Chem. Phys., 21, 10133–10158, https://doi.org/10.5194/acp-21-10133-2021, https://doi.org/10.5194/acp-21-10133-2021, 2021
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We present the first real-time composition of submicron particulate matter (PM1) in Old Delhi using high-resolution aerosol mass spectrometry. Seasonal analysis shows peak concentrations occur during the post-monsoon, and novel-tracers reveal the largest sources are a combination of local open and regional crop residue burning. Strong links between increased chloride aerosol concentrations and burning sources of PM1 suggest burning sources are responsible for the post-monsoon chloride peak.
Hua Fang, Xiaoqing Huang, Yanli Zhang, Chenglei Pei, Zuzhao Huang, Yujun Wang, Yanning Chen, Jianhong Yan, Jianqiang Zeng, Shaoxuan Xiao, Shilu Luo, Sheng Li, Jun Wang, Ming Zhu, Xuewei Fu, Zhenfeng Wu, Runqi Zhang, Wei Song, Guohua Zhang, Weiwei Hu, Mingjin Tang, Xiang Ding, Xinhui Bi, and Xinming Wang
Atmos. Chem. Phys., 21, 10005–10013, https://doi.org/10.5194/acp-21-10005-2021, https://doi.org/10.5194/acp-21-10005-2021, 2021
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A tunnel test was initiated to measure the vehicular IVOC emissions under real-world driving conditions. Higher SOA formation estimated from vehicular IVOCs compared to those from traditional VOCs emphasized the greater importance of IVOCs in modulating urban SOA. The results also revealed that non-road diesel-fueled engines greatly contributed to IVOCs in China.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760, https://doi.org/10.5194/acp-21-9741-2021, https://doi.org/10.5194/acp-21-9741-2021, 2021
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Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud ice formation processes. Implementing a parameterization for ice multiplication due to mechanical breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
Xiaoyang Chen, Yang Zhang, Kai Wang, Daniel Tong, Pius Lee, Youhua Tang, Jianping Huang, Patrick C. Campbell, Jeff Mcqueen, Havala O. T. Pye, Benjamin N. Murphy, and Daiwen Kang
Geosci. Model Dev., 14, 3969–3993, https://doi.org/10.5194/gmd-14-3969-2021, https://doi.org/10.5194/gmd-14-3969-2021, 2021
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The continuously updated National Air Quality Forecast Capability (NAQFC) provides air quality forecasts. To support the development of the next-generation NAQFC, we evaluate a prototype of GFSv15-CMAQv5.0.2. The performance and the potential improvements for the system are discussed. This study can provide a scientific basis for further development of NAQFC and help it to provide more accurate air quality forecasts to the public over the contiguous United States.
Yuhan Yang, Dong Gao, and Rodney J. Weber
Atmos. Meas. Tech., 14, 4707–4719, https://doi.org/10.5194/amt-14-4707-2021, https://doi.org/10.5194/amt-14-4707-2021, 2021
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Iron and copper are commonly found in ambient aerosols and have been linked to adverse health effects. We describe a relatively simple benchtop instrument that can be used to quantify these metals in aqueous solutions and verify the method by comparison with inductively coupled plasma mass spectrometry. The approach is based on forming light-absorbing metal–ligand complexes that can be measured with high sensitivity utilizing a long-path liquid waveguide capillary cell.
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.
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.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
Chenshuo Ye, Bin Yuan, Yi Lin, Zelong Wang, Weiwei Hu, Tiange Li, Wei Chen, Caihong Wu, Chaomin Wang, Shan Huang, Jipeng Qi, Baolin Wang, Chen Wang, Wei Song, Xinming Wang, E Zheng, Jordan E. Krechmer, Penglin Ye, Zhanyi Zhang, Xuemei Wang, Douglas R. Worsnop, and Min Shao
Atmos. Chem. Phys., 21, 8455–8478, https://doi.org/10.5194/acp-21-8455-2021, https://doi.org/10.5194/acp-21-8455-2021, 2021
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We performed measurements of gaseous and particulate organic compounds using a state-of-the-art online mass spectrometer in urban air. Using the dataset, we provide a holistic chemical characterization of oxygenated organic compounds in the polluted urban atmosphere, which can serve as a reference for the future field measurements of organic compounds in cities.
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, T. Nash Skipper, and Armistead G. Russell
Atmos. Chem. Phys., 21, 8341–8356, https://doi.org/10.5194/acp-21-8341-2021, https://doi.org/10.5194/acp-21-8341-2021, 2021
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Extended ground-level measurements are coupled with model simulations to comprehensively compare the aerosol acidity in China and the United States. Aerosols in China are significantly less acidic than those in the United States, with pH values 1–2 units higher. Higher aerosol mass concentrations and the abundance of ammonia and ammonium in China, compared to the United States, are leading causes of the pH difference between these two countries.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
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.
K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Qian Shu, Benjamin Murphy, Jonathan E. Pleim, Donna Schwede, Barron H. Henderson, Havala O.T. Pye, Keith Wyat Appel, Tanvir R. Khan, and Judith A. Perlinger
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2021-129, https://doi.org/10.5194/gmd-2021-129, 2021
Preprint withdrawn
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We have bridged the gap between dry deposition measurement and modeling by rigorous use of box and regional transport models and field measurements, but more efforts are needed. This study highlights that deviation among deposition schemes is most pronounced for small and large particles. This study better links model predictions to available real-world observations and incrementally reduces uncertainties in the magnitude of loss processes important for the lifecycle of air pollutants.
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys., 21, 6541–6563, https://doi.org/10.5194/acp-21-6541-2021, https://doi.org/10.5194/acp-21-6541-2021, 2021
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There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Yutong Liang, Coty N. Jen, Robert J. Weber, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 21, 5719–5737, https://doi.org/10.5194/acp-21-5719-2021, https://doi.org/10.5194/acp-21-5719-2021, 2021
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This article reports the molecular composition of smoke particles people in SF Bay Area were exposed to during northern California wildfires in Oct. 2017. Major components are sugars, acids, aromatics, and terpenoids. These observations can be used to better understand health impacts of smoke exposure. Tracer compounds indicate which fuels burned, including diterpenoids for softwood and syringyls for hardwood. A statistical analysis reveals a group of secondary compounds formed in daytime aging.
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.
Karl M. Seltzer, Elyse Pennington, Venkatesh Rao, Benjamin N. Murphy, Madeleine Strum, Kristin K. Isaacs, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 5079–5100, https://doi.org/10.5194/acp-21-5079-2021, https://doi.org/10.5194/acp-21-5079-2021, 2021
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Volatile chemical products (VCPs) are an increasingly important source of anthropogenic reactive organic carbon emissions. Here, we develop VCPy, a new framework to model organic emissions from VCPs throughout the United States. At the national-level, VCPy emissions are broadly consistent with the US EPA’s 2017 National Emission Inventory, however county-level and categorical estimates can differ substantially. An observational evaluation indicates high fidelity in the methods employed here.
Pamela S. Rickly, Lu Xu, John D. Crounse, Paul O. Wennberg, and Andrew W. Rollins
Atmos. Meas. Tech., 14, 2429–2439, https://doi.org/10.5194/amt-14-2429-2021, https://doi.org/10.5194/amt-14-2429-2021, 2021
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Key improvements have been made to an in situ laser-induced fluorescence instrument for measuring SO2 in polluted and pristine environments. Laser linewidth is reduced, rapid laser tuning is implemented, and fluorescence bandpass filters are optimized. These improvements have led to a 50 % reduction in instrument detection limit. The influence of aromatic compounds was also investigated and determined to not bias SO2 measurements.
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.
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.
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.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
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.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771, https://doi.org/10.5194/acp-21-755-2021, https://doi.org/10.5194/acp-21-755-2021, 2021
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Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
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.
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.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Caihong Wu, Chaomin Wang, Sihang Wang, Wenjie Wang, Bin Yuan, Jipeng Qi, Baolin Wang, Hongli Wang, Chen Wang, Wei Song, Xinming Wang, Weiwei Hu, Shengrong Lou, Chenshuo Ye, Yuwen Peng, Zelong Wang, Yibo Huangfu, Yan Xie, Manni Zhu, Junyu Zheng, Xuemei Wang, Bin Jiang, Zhanyi Zhang, and Min Shao
Atmos. Chem. Phys., 20, 14769–14785, https://doi.org/10.5194/acp-20-14769-2020, https://doi.org/10.5194/acp-20-14769-2020, 2020
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Based on measurements from an online mass spectrometer, we quantify volatile organic compound (VOC) concentrations from numerous ions of the mass spectrometer, using information from laboratory-obtained calibration results. We find that most VOC concentrations are from oxygenated VOCs (OVOCs). We further show that these OVOCs also contribute significantly to OH reactivity. Our results suggest the important role of OVOCs in VOC emissions and chemistry in urban air.
Chaomin Wang, Bin Yuan, Caihong Wu, Sihang Wang, Jipeng Qi, Baolin Wang, Zelong Wang, Weiwei Hu, Wei Chen, Chenshuo Ye, Wenjie Wang, Yele Sun, Chen Wang, Shan Huang, Wei Song, Xinming Wang, Suxia Yang, Shenyang Zhang, Wanyun Xu, Nan Ma, Zhanyi Zhang, Bin Jiang, Hang Su, Yafang Cheng, Xuemei Wang, and Min Shao
Atmos. Chem. Phys., 20, 14123–14138, https://doi.org/10.5194/acp-20-14123-2020, https://doi.org/10.5194/acp-20-14123-2020, 2020
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We utilized a novel online mass spectrometry method to measure the total concentration of higher alkanes at each carbon number at two different sites in China, allowing us to take into account SOA contributions from all isomers for higher alkanes. We found that higher alkanes account for significant fractions of SOA formation at the two sites. The contributions are comparable to or even higher than single-ring aromatics, the most-recognized SOA precursors in urban air.
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.
Chao Peng, Yu Wang, Zhijun Wu, Lanxiadi Chen, Ru-Jin Huang, Weigang Wang, Zhe Wang, Weiwei Hu, Guohua Zhang, Maofa Ge, Min Hu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13877–13903, https://doi.org/10.5194/acp-20-13877-2020, https://doi.org/10.5194/acp-20-13877-2020, 2020
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
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.
Chen Dayan, Erick Fredj, Pawel K. Misztal, Maor Gabay, Alex B. Guenther, and Eran Tas
Atmos. Chem. Phys., 20, 12741–12759, https://doi.org/10.5194/acp-20-12741-2020, https://doi.org/10.5194/acp-20-12741-2020, 2020
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We studied the emission of biogenic volatile organic compounds from both marine and terrestrial ecosystems in the Eastern Mediterranean Basin, a global warming hot spot. We focused on isoprene and dimethyl sulfide (DMS), which are well recognized for their effect on climate and strong impact on photochemical pollution by the former. We found high emissions of isoprene and a strong decadal decrease in the emission of DMS which can both be attributed to the strong increase in seawater temperature.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Amy E. Christiansen, Annmarie G. Carlton, and Barron H. Henderson
Atmos. Chem. Phys., 20, 11607–11624, https://doi.org/10.5194/acp-20-11607-2020, https://doi.org/10.5194/acp-20-11607-2020, 2020
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We quantify differences in surface-level fine particle mass (PM2.5) chemical composition in relation to satellite-derived cloud flags and find significant differences between clear-sky and cloud days. The work suggests that future analysis in this area is warranted.
James F. Hurley, Nathan M. Kreisberg, Braden Stump, Chenyang Bi, Purushottam Kumar, Susanne V. Hering, Pat Keady, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 13, 4911–4925, https://doi.org/10.5194/amt-13-4911-2020, https://doi.org/10.5194/amt-13-4911-2020, 2020
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The chemical composition of aerosols has implications for human and ecosystem health. Current methods for determining chemical composition are expensive and require highly trained personnel. Our method is promising for moderate-cost, low-maintenance measurements of oxygen / carbon ratios, a key chemical parameter, and other elements may also be studied. In this work, we coupled two commonly used detectors to assess O / C ratios in a variety of compounds and mixtures within an acceptable error.
Damon M. Smith, Tianqu Cui, Marc N. Fiddler, Rudra P. Pokhrel, Jason D. Surratt, and Solomon Bililign
Atmos. Chem. Phys., 20, 10169–10191, https://doi.org/10.5194/acp-20-10169-2020, https://doi.org/10.5194/acp-20-10169-2020, 2020
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Biomass fuels used for domestic purposes in east Africa produce a significant atmospheric burden of aerosols and volatile organic compounds. The chemical properties and composition of these aerosols have not been investigated in the laboratory. In this work methanol extracts from filter samples of aerosol collected from an indoor smog chamber were analyzed to determine the chemical composition and identify the light absorption properties of organic aerosol constituents.
Ru-Jin Huang, Yao He, Jing Duan, Yongjie Li, Qi Chen, Yan Zheng, Yang Chen, Weiwei Hu, Chunshui Lin, Haiyan Ni, Wenting Dai, Junji Cao, Yunfei Wu, Renjian Zhang, Wei Xu, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin D. O'Dowd
Atmos. Chem. Phys., 20, 9101–9114, https://doi.org/10.5194/acp-20-9101-2020, https://doi.org/10.5194/acp-20-9101-2020, 2020
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We systematically compared the submicron particle (PM1) processes in haze days with low and high relative humidity (RH) in wintertime Beijing. Nitrate had similar daytime growth rates in low-RH and high-RH pollution. OOA had a higher growth rate in low-RH pollution than in high-RH pollution. Sulfate had a decreasing trend in low-RH pollution, while it increased significantly in high-RH pollution. This distinction may be explained by the different processes affected by meteorological conditions.
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.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
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.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Junchen Guo, Shengzhen Zhou, Mingfu Cai, Jun Zhao, Wei Song, Weixiong Zhao, Weiwei Hu, Yele Sun, Yao He, Chengqiang Yang, Xuezhe Xu, Zhisheng Zhang, Peng Cheng, Qi Fan, Jian Hang, Shaojia Fan, Xinming Wang, and Xuemei Wang
Atmos. Chem. Phys., 20, 7595–7615, https://doi.org/10.5194/acp-20-7595-2020, https://doi.org/10.5194/acp-20-7595-2020, 2020
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We characterized non-refractory submicron particulate matter (PM1.0) during winter in Guangzhou, south China. Chemical composition and key sources of ambient PM1.0 are revealed, highlighting the significant role of SOA. The relationship with SOA and peroxy radicals indicated gas-phase oxidation contributed predominantly to SOA formation during non-pollution periods, while heterogeneous/multiphase reactions played more important roles in SOA formation during pollution periods.
Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di Liu, Zongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 20, 7531–7552, https://doi.org/10.5194/acp-20-7531-2020, https://doi.org/10.5194/acp-20-7531-2020, 2020
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Using the chemical composition of offline filter samples, we report that a large share of oxidized organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates showed a strong correlation with the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate in heterogeneous reactions and further demonstrates that iSOA formation is controlled by anthropogenic emissions.
Jian Xu, Jia Chen, Na Zhao, Guochen Wang, Guangyuan Yu, Hao Li, Juntao Huo, Yanfen Lin, Qingyan Fu, Hongyu Guo, Congrui Deng, Shan-Hu Lee, Jianmin Chen, and Kan Huang
Atmos. Chem. Phys., 20, 7259–7269, https://doi.org/10.5194/acp-20-7259-2020, https://doi.org/10.5194/acp-20-7259-2020, 2020
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This study provided evidence that gas-particle partitioning of ammonia, as opposed to ammonia concentration, plays a critical role in the haze formation. A reduction in ammonia emissions alone may not reduce air pollution effectively, at least at rural agricultural sites in China.
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.
Sungyeon Choi, Lok N. Lamsal, Melanie Follette-Cook, Joanna Joiner, Nickolay A. Krotkov, William H. Swartz, Kenneth E. Pickering, Christopher P. Loughner, Wyat Appel, Gabriele Pfister, Pablo E. Saide, Ronald C. Cohen, Andrew J. Weinheimer, and Jay R. Herman
Atmos. Meas. Tech., 13, 2523–2546, https://doi.org/10.5194/amt-13-2523-2020, https://doi.org/10.5194/amt-13-2523-2020, 2020
Yan Zheng, Xi Cheng, Keren Liao, Yaowei Li, Yong Jie Li, Ru-Jin Huang, Weiwei Hu, Ying Liu, Tong Zhu, Shiyi Chen, Limin Zeng, Douglas R. Worsnop, and Qi Chen
Atmos. Meas. Tech., 13, 2457–2472, https://doi.org/10.5194/amt-13-2457-2020, https://doi.org/10.5194/amt-13-2457-2020, 2020
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This paper provides important information to help researchers to understand the mass quantification and source apportionment by Aerodyne aerosol mass spectrometers.
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.
Dong Gao, Krystal J. Godri Pollitt, James A. Mulholland, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 20, 5197–5210, https://doi.org/10.5194/acp-20-5197-2020, https://doi.org/10.5194/acp-20-5197-2020, 2020
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This study provides a direct intercomparison between two assays for quantifying oxidative potential (OP) of ambient particles: the synthetic respiratory-tract-lining fluid (RTLF) assay and the dithiothreitol (DTT) assay. The results suggest that the DTT assay and the ascorbic acid depletion in RTLF are associated with organic species, transition metal ions, and antagonistic interactions between species. The glutathione depletion in RTLF is strongly dependent on water-soluble copper.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
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.
Quanyang Lu, Benjamin N. Murphy, Momei Qin, Peter J. Adams, Yunliang Zhao, Havala O. T. Pye, Christos Efstathiou, Chris Allen, and Allen L. Robinson
Atmos. Chem. Phys., 20, 4313–4332, https://doi.org/10.5194/acp-20-4313-2020, https://doi.org/10.5194/acp-20-4313-2020, 2020
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This research work investigates organic aerosol formation in California during the CalNex study. We update the chemical transport model with the most recent mobile-source emission data and introduce a simple parameterization for secondary organic aerosol formed from intermediate-volatility organic compounds. Our results highlight the important contribution of IVOCs to SOA production in the Los Angeles region but underscore that other uncertainties must be addressed to close the SOA mass balance.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040, https://doi.org/10.5194/acp-20-3029-2020, https://doi.org/10.5194/acp-20-3029-2020, 2020
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We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
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.
Aoxing Zhang, Yuhang Wang, Yuzhong Zhang, Rodney J. Weber, Yongjia Song, Ziming Ke, and Yufei Zou
Atmos. Chem. Phys., 20, 1901–1920, https://doi.org/10.5194/acp-20-1901-2020, https://doi.org/10.5194/acp-20-1901-2020, 2020
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Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosols. We developed a module to simulate the emissions, atmospheric processing and direct radiative effect of BrC in the Community Earth System Model (CESM). We found that globally BrC is a significant absorber and is more centered in the tropical free troposphere compared to BC. The contribution of BrC heating to the Hadley circulation and latitudinal expansion of the tropics is comparable to BC heating.
Joseph R. Salazar, Benton T. Cartledge, John P. Haynes, Rachel York-Marini, Allen L. Robinson, Greg T. Drozd, Allen H. Goldstein, Sirine C. Fakra, and Brian J. Majestic
Atmos. Chem. Phys., 20, 1849–1860, https://doi.org/10.5194/acp-20-1849-2020, https://doi.org/10.5194/acp-20-1849-2020, 2020
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The solubility of atmospheric iron is important in human health and environmental chemistry. To understand the origin of water-soluble iron in urban areas, tailpipe emissions were collected from 32 low-emitting vehicles, from which iron solubility averaged 30 % (0–82 %), more than 10 times the average in the Earth's crust. Water-soluble iron was independent of almost all exhaust components and of the iron phase in the particles but was correlated with specific exhaust-derived organic compounds.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838, https://doi.org/10.5194/acp-20-1817-2020, https://doi.org/10.5194/acp-20-1817-2020, 2020
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Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316, https://doi.org/10.5194/acp-20-1301-2020, https://doi.org/10.5194/acp-20-1301-2020, 2020
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Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
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.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
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.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342, https://doi.org/10.5194/acp-19-11315-2019, https://doi.org/10.5194/acp-19-11315-2019, 2019
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We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
Laura Kiely, Dominick V. Spracklen, Christine Wiedinmyer, Luke Conibear, Carly L. Reddington, Scott Archer-Nicholls, Douglas Lowe, Stephen R. Arnold, Christoph Knote, Md Firoz Khan, Mohd Talib Latif, Mikinori Kuwata, Sri Hapsari Budisulistiorini, and Lailan Syaufina
Atmos. Chem. Phys., 19, 11105–11121, https://doi.org/10.5194/acp-19-11105-2019, https://doi.org/10.5194/acp-19-11105-2019, 2019
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In 2015, a large fire episode occurred in Indonesia, reducing air quality. Fires occurred predominantly on peatland, where large uncertainties are associated with emissions. Current fire emissions datasets underestimate peat fire emissions. We created new fire emissions data, with data specific to Indonesian peat fires. Using these emissions in simulations of particulate matter and aerosol optical depth shows an improvement over simulations using current data, when compared with observations.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Eloise A. Marais, Zhe Peng, Benjamin A. Nault, Weiwei Hu, Pedro Campuzano-Jost, and Jose L. Jimenez
Geosci. Model Dev., 12, 2983–3000, https://doi.org/10.5194/gmd-12-2983-2019, https://doi.org/10.5194/gmd-12-2983-2019, 2019
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We developed a parameterization method for IEPOX-SOA based on the detailed chemical mechanism. Our parameterizations were tested using a box model and 3-D chemical transport model, which accurately captured the spatiotemporal distribution and response to changes in emissions compared to the explicit full chemistry, while being more computationally efficient. The method developed in this study can be applied to global climate models for long-term studies with a lower computational cost.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Benjamin L. Deming, Demetrios Pagonis, Xiaoxi Liu, Douglas A. Day, Ranajit Talukdar, Jordan E. Krechmer, Joost A. de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 12, 3453–3461, https://doi.org/10.5194/amt-12-3453-2019, https://doi.org/10.5194/amt-12-3453-2019, 2019
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Losses or measurement delays of gas-phase compounds sampled through tubing are important to atmospheric science. Here we characterize 14 tubing materials by measuring the effects on step changes in organic compound concentration. We find that polymeric tubings exhibit absorptive partitioning behaviour while glass and metal tubings show adsorptive partitioning. Adsorptive materials impart complex humidity, concentration, and VOC–VOC interaction dependencies that absorptive tubings do not.
Suzane S. de Sá, Luciana V. Rizzo, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Joel Brito, Samara Carbone, Yingjun J. Liu, Arthur Sedlacek, Stephen Springston, Allen H. Goldstein, Henrique M. J. Barbosa, M. Lizabeth Alexander, Paulo Artaxo, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 19, 7973–8001, https://doi.org/10.5194/acp-19-7973-2019, https://doi.org/10.5194/acp-19-7973-2019, 2019
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This study investigates the impacts of urban and fire emissions on the concentration, composition, and optical properties of submicron particulate matter (PM1) in central Amazonia during the dry season. Biomass-burning and urban emissions appeared to contribute at least 80 % of brown carbon absorption while accounting for 30 % to 40 % of the organic PM1 mass concentration. Only a fraction of the 9-fold increase in mass concentration relative to the wet season was due to biomass burning.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Charles A. Brock, Christina Williamson, Agnieszka Kupc, Karl D. Froyd, Frank Erdesz, Nicholas Wagner, Matthews Richardson, Joshua P. Schwarz, Ru-Shan Gao, Joseph M. Katich, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, Bernadett Weinzierl, Maximilian Dollner, ThaoPaul Bui, and Daniel M. Murphy
Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, https://doi.org/10.5194/amt-12-3081-2019, 2019
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From 2016 to 2018 a NASA aircraft profiled the atmosphere from 180 m to ~12 km from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, ATom, sought to sample atmospheric chemical composition to compare with global climate models. We describe the how measurements of particulate matter were made during ATom, and show that the instrument performance was excellent. Data from this project can be used with confidence to evaluate models and compare with satellites.
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, https://doi.org/10.5194/acp-19-7319-2019, 2019
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Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Anna L. Hodshire, Pedro Campuzano-Jost, John K. Kodros, Betty Croft, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 3137–3160, https://doi.org/10.5194/acp-19-3137-2019, https://doi.org/10.5194/acp-19-3137-2019, 2019
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A global chemical-transport model is used to determine the impact of methanesulfonic acid (MSA) on the aerosol size distribution and associated radiative effects, testing varying assumptions of MSA’s effective volatility and nucleating ability. We find that MSA mass best matches the ATom airborne measurements when volatility varies as a function of temperature, relative humidity, and available gas-phase bases, and the MSA radiative forcing is on the order of -50 mW m-2 over the Southern Ocean.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Hoi Ki Lam, Kai Chung Kwong, Hon Yin Poon, James F. Davies, Zhenfa Zhang, Avram Gold, Jason D. Surratt, and Man Nin Chan
Atmos. Chem. Phys., 19, 2433–2440, https://doi.org/10.5194/acp-19-2433-2019, https://doi.org/10.5194/acp-19-2433-2019, 2019
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Organosulfates are ubiquitous in the atmosphere. We find that chemical transformation of IEPOX-derived organosulfates, one of the most abundant organosulfates, can generate inorganic sulfate through heterogeneous OH oxidation. The findings of this work provide new reaction pathways for recycling of inorganic and organic sulfur and may suggest that organosulfates could be reservoirs of inorganic sulfates in the atmosphere.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
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We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Coty N. Jen, Lindsay E. Hatch, Vanessa Selimovic, Robert J. Yokelson, Robert Weber, Arantza E. Fernandez, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 19, 1013–1026, https://doi.org/10.5194/acp-19-1013-2019, https://doi.org/10.5194/acp-19-1013-2019, 2019
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Wildfires in the western US are occurring more frequently and burning larger land areas. Smoke from these fires will play a greater role in regional air quality and atmospheric chemistry than in the past. To help fire and climate modelers and atmospheric experimentalists better understand how smoke impacts the environment, we have separated, identified, classified, and quantified the thousands of organic compounds found in smoke and related their amounts emitted to fire conditions.
Zhe Peng, Julia Lee-Taylor, John J. Orlando, Geoffrey S. Tyndall, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 813–834, https://doi.org/10.5194/acp-19-813-2019, https://doi.org/10.5194/acp-19-813-2019, 2019
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The use of oxidation flow reactors (OFRs) has been rapidly increasing. We investigate organic peroxy radical (RO2) chemistry in OFRs by kinetic modeling. It is found that, at low NO, UV intensity should be limited to avoid high radical levels leading to significant reaction of RO2 with OH and negligible RO2 isomerization, both of which are atmospherically irrelevant. We also develop two RO2 fate estimators (for general use and for OFRs) to aid experiment design and interpretation.
Juhi Nagori, Ruud H. H. Janssen, Juliane L. Fry, Maarten Krol, Jose L. Jimenez, Weiwei Hu, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 19, 701–729, https://doi.org/10.5194/acp-19-701-2019, https://doi.org/10.5194/acp-19-701-2019, 2019
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Secondary organic aerosol (SOA) is produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions, and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry above the southeastern US with data collected during the SOAS campaign to constrain the model.
Andrew T. Lambe, Jordan E. Krechmer, Zhe Peng, Jason R. Casar, Anthony J. Carrasquillo, Jonathan D. Raff, Jose L. Jimenez, and Douglas R. Worsnop
Atmos. Meas. Tech., 12, 299–311, https://doi.org/10.5194/amt-12-299-2019, https://doi.org/10.5194/amt-12-299-2019, 2019
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This paper is an evaluation of methods used to generate OH radicals under conditions with high concentrations of NO and NO2 to simulate oxidation chemistry in polluted urban atmospheres over equivalent atmospheric timescales of ~ 1 day.
Krystal T. Vasquez, Hannah M. Allen, John D. Crounse, Eric Praske, Lu Xu, Anke C. Noelscher, and Paul O. Wennberg
Atmos. Meas. Tech., 11, 6815–6832, https://doi.org/10.5194/amt-11-6815-2018, https://doi.org/10.5194/amt-11-6815-2018, 2018
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Oxygenated volatile organic compounds (OVOCs) are difficult to measure in the atmosphere due to their high reactivity and low concentrations. This hinders our understanding of their impact on air quality and climate. Therefore, we have developed a field-deployable instrument capable of providing isomer-resolved measurements of OVOCs in the ambient air. Its performance is assessed through data collected both in the laboratory and during two field studies.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Lindsay E. Hatch, Albert Rivas-Ubach, Coty N. Jen, Mary Lipton, Allen H. Goldstein, and Kelley C. Barsanti
Atmos. Chem. Phys., 18, 17801–17817, https://doi.org/10.5194/acp-18-17801-2018, https://doi.org/10.5194/acp-18-17801-2018, 2018
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We demonstrate the use of solid-phase extraction (SPE) disks for the untargeted analysis of gas-phase intermediate volatility and semi-volatile organic compounds emitted from biomass burning. SPE and Teflon filter samples collected from laboratory fires were analyzed by two-dimensional gas chromatography, with distinct differences in the observed chromatographic profiles as a function of
fuel type. Fuel-dependent emissions and volatility differences among benzenediol isomers were captured.
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, https://doi.org/10.5194/acp-18-17307-2018, 2018
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Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Sri Hapsari Budisulistiorini, Matthieu Riva, Michael Williams, Takuma Miyakawa, Jing Chen, Masayuki Itoh, Jason D. Surratt, and Mikinori Kuwata
Atmos. Chem. Phys., 18, 16481–16498, https://doi.org/10.5194/acp-18-16481-2018, https://doi.org/10.5194/acp-18-16481-2018, 2018
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Wildfire emits a large number of haze particles. During transport in the atmosphere, the organic aerosol in the haze particles can undergo atmospheric processes and become highly oxidized. We show that the haze particles transported from wildfires in Indonesia are dominated by oxygenated organic aerosols. This study highlights the impact of atmospheric processes on the transboundary haze particles.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480, https://doi.org/10.5194/acp-18-16461-2018, https://doi.org/10.5194/acp-18-16461-2018, 2018
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Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Barbara Ervens, Armin Sorooshian, Abdulmonam M. Aldhaif, Taylor Shingler, Ewan Crosbie, Luke Ziemba, Pedro Campuzano-Jost, Jose L. Jimenez, and Armin Wisthaler
Atmos. Chem. Phys., 18, 16099–16119, https://doi.org/10.5194/acp-18-16099-2018, https://doi.org/10.5194/acp-18-16099-2018, 2018
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The paper presents a new framework that can be used to identify emission scenarios in which aerosol populations are most likely modified by chemical processes in clouds. We show that in neither very polluted nor in very clean air masses is this the case. Only if the ratio of possible aerosol mass precursors (sulfur dioxide, some organics) and preexisting aerosol mass is sufficiently high will aerosol particles show substantially modified physicochemical properties upon cloud processing.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Mariel D. Friberg, Ralph A. Kahn, James A. Limbacher, K. Wyat Appel, and James A. Mulholland
Atmos. Chem. Phys., 18, 12891–12913, https://doi.org/10.5194/acp-18-12891-2018, https://doi.org/10.5194/acp-18-12891-2018, 2018
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Advances in satellite retrieval of aerosol type can improve ambient air quality concentration estimates by providing regional context where surface monitors are scarce or absent. This work focuses on the degree to which regional-scale satellite and model data can be combined to improve surface estimates of fine particles and their major speciated components. The physically based method applies satellite-derived column observations directly to total and speciated surface particle concentrations.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Jason A. Ducker, Christopher D. Holmes, Trevor F. Keenan, Silvano Fares, Allen H. Goldstein, Ivan Mammarella, J. William Munger, and Jordan Schnell
Biogeosciences, 15, 5395–5413, https://doi.org/10.5194/bg-15-5395-2018, https://doi.org/10.5194/bg-15-5395-2018, 2018
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We have developed an accurate method (SynFlux) to estimate ozone deposition and stomatal uptake across 103 flux tower sites (43 US, 60 Europe), where ozone concentrations and fluxes have not been measured. In all, the SynFlux public dataset provides monthly values of ozone dry deposition for 926 site years across a wide array of ecosystems. The SynFlux dataset will promote further applications to ecosystem, air quality, or climate modeling across the geoscience community.
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, https://doi.org/10.5194/acp-18-12765-2018, 2018
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In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Lu Xu, Havala O. T. Pye, Jia He, Yunle Chen, Benjamin N. Murphy, and Nga Lee Ng
Atmos. Chem. Phys., 18, 12613–12637, https://doi.org/10.5194/acp-18-12613-2018, https://doi.org/10.5194/acp-18-12613-2018, 2018
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In this study, we integrate lab-in-the-field experiments, extensive ambient ground measurements, and state-of-the-art modeling to constrain the concentration of organic aerosol from biogenic monoterpenes and sesquiterpenes. Further, we show that the organic aerosol from the investigated sources accounts for roughly 20 % of the World Health Organization PM2.5 standard in the southeastern US.
Anna L. Hodshire, Brett B. Palm, M. Lizabeth Alexander, Qijing Bian, Pedro Campuzano-Jost, Eben S. Cross, Douglas A. Day, Suzane S. de Sá, Alex B. Guenther, Armin Hansel, James F. Hunter, Werner Jud, Thomas Karl, Saewung Kim, Jesse H. Kroll, Jeong-Hoo Park, Zhe Peng, Roger Seco, James N. Smith, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 18, 12433–12460, https://doi.org/10.5194/acp-18-12433-2018, https://doi.org/10.5194/acp-18-12433-2018, 2018
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We investigate the nucleation and growth processes that shape the aerosol size distribution inside oxidation flow reactors (OFRs) that sampled ambient air from Colorado and the Amazon rainforest. Results indicate that organics are important for both nucleation and growth, vapor uptake was limited to accumulation-mode particles, fragmentation reactions were important to limit particle growth at higher OH exposures, and an H2SO4-organics nucleation mechanism captured new particle formation well.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206, https://doi.org/10.5194/acp-18-12185-2018, https://doi.org/10.5194/acp-18-12185-2018, 2018
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This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Jing Chen, Sri Hapsari Budisulistiorini, Takuma Miyakawa, Yuichi Komazaki, and Mikinori Kuwata
Atmos. Chem. Phys., 18, 7781–7798, https://doi.org/10.5194/acp-18-7781-2018, https://doi.org/10.5194/acp-18-7781-2018, 2018
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We present water uptake properties of haze particles originating from Indonesian peatland fires and further link the water uptake to particle chemical characteristics. Organic-rich wildfire haze particles are highly hygroscopic, governed by sulfate and promoted by secondary organic aerosol formation. Water-soluble organic fraction plays a minor role in determining particle hygroscopicity. This deepens our understanding, and reported results can be further applied into climate models.
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Haiyan Li, Qiang Zhang, Bo Zheng, Chunrong Chen, Nana Wu, Hongyu Guo, Yuxuan Zhang, Yixuan Zheng, Xin Li, and Kebin He
Atmos. Chem. Phys., 18, 5293–5306, https://doi.org/10.5194/acp-18-5293-2018, https://doi.org/10.5194/acp-18-5293-2018, 2018
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This study revealed the driving role of nitrate in urban haze development in the North China Plain (NCP) during summertime. Several factors favoring the rapid nitrate formation were investigated in detail. The higher concentration and, in particular, the higher contribution of nitrate in PM1 suggest an urgent need to initiate ammonia emission control measures and further reduce NOx emissions over the NCP region.
Riinu Ots, Mathew R. Heal, Dominique E. Young, Leah R. Williams, James D. Allan, Eiko Nemitz, Chiara Di Marco, Anais Detournay, Lu Xu, Nga L. Ng, Hugh Coe, Scott C. Herndon, Ian A. Mackenzie, David C. Green, Jeroen J. P. Kuenen, Stefan Reis, and Massimo Vieno
Atmos. Chem. Phys., 18, 4497–4518, https://doi.org/10.5194/acp-18-4497-2018, https://doi.org/10.5194/acp-18-4497-2018, 2018
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The main hypothesis of this paper is that people who live in large cities in the UK disobey the
smoke control lawas it has not been actively enforced for decades now. However, the use of wood in residential heating has increased, partly due to renewable energy targets, but also for discretionary (i.e. pleasant fireplaces) reasons. Our study is based mainly in London, but similar struggles with urban air quality due to residential wood and coal burning are seen in other major European cities.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Brett B. Palm, Suzane S. de Sá, Douglas A. Day, Pedro Campuzano-Jost, Weiwei Hu, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Joel Brito, Florian Wurm, Paulo Artaxo, Ryan Thalman, Jian Wang, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Allen H. Goldstein, Yingjun Liu, Stephen R. Springston, Rodrigo Souza, Matt K. Newburn, M. Lizabeth Alexander, Scot T. Martin, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 467–493, https://doi.org/10.5194/acp-18-467-2018, https://doi.org/10.5194/acp-18-467-2018, 2018
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Ambient air was oxidized by OH or O3 in an oxidation flow reactor during both wet and dry seasons in the GoAmazon2014/5 campaign to study secondary organic aerosol (SOA) formation. We investigated how much biogenic, urban, and biomass burning sources contributed to the ambient concentrations of SOA precursor gases and how their contributions changed diurnally and seasonally. SOA yields and hygroscopicity of organic aerosol in the oxidation flow reactor were also studied.
David H. Hagan, Gabriel Isaacman-VanWertz, Jonathan P. Franklin, Lisa M. M. Wallace, Benjamin D. Kocar, Colette L. Heald, and Jesse H. Kroll
Atmos. Meas. Tech., 11, 315–328, https://doi.org/10.5194/amt-11-315-2018, https://doi.org/10.5194/amt-11-315-2018, 2018
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The use of low-cost sensors for air pollution research has outpaced our understanding of their capabilities and limitations under real-world conditions. Here we describe the deployment, calibration and evaluation of electrochemical sensors on the Island of Hawai‘i. We obtain excellent performance (RMSE < 7 ppb, r2 = 0.997) across a wide dynamic range (1 ppb–2 ppm). We introduce a hybrid regression algorithm which works across a large dynamic range and shows little decay in sensitivity over time.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Haihan Chen, Anna L. Hodshire, John Ortega, James Greenberg, Peter H. McMurry, Annmarie G. Carlton, Jeffrey R. Pierce, Dave R. Hanson, and James N. Smith
Atmos. Chem. Phys., 18, 311–326, https://doi.org/10.5194/acp-18-311-2018, https://doi.org/10.5194/acp-18-311-2018, 2018
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Much of what we know about atmospheric new particle formation (NPF) is based on ground-level measurements. We used tethered balloon measurements and remote sensing to study the location in the boundary layer in which NPF events are initiated, the degree to which the boundary layer is well-mixed during NPF, and the potential role that water may play in aerosol particle chemical evolution. This information will improve the representativeness of process level models and laboratory experiments.
Demetrios Pagonis, Jordan E. Krechmer, Joost de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 10, 4687–4696, https://doi.org/10.5194/amt-10-4687-2017, https://doi.org/10.5194/amt-10-4687-2017, 2017
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Laboratory studies were conducted to investigate gas-wall partitioning of atmospheric organic compounds in Teflon tubing and inside an instrument used to monitor concentrations. Rapid partitioning caused time delays in instrument response that vary with tubing length and diameter, flow rate, and compound volatility. Tubing delay times of seconds to hours were described using a model that also included effects of instrument surfaces. The results can enable better design of air sampling systems.
Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, and Allan K. Bertram
Atmos. Chem. Phys., 17, 13037–13048, https://doi.org/10.5194/acp-17-13037-2017, https://doi.org/10.5194/acp-17-13037-2017, 2017
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Using laboratory data, meteorological fields and a chemical transport model, we investigated how often mixing times are < 1 h within SOA in the planetary boundary layer (PBL). Based on viscosity data for alpha-pinene SOA generated using mass concentrations of ~1000 µg m −3, mixing times in biogenic SOA are < 1h most of the time.
Zhe Peng and Jose L. Jimenez
Atmos. Chem. Phys., 17, 11991–12010, https://doi.org/10.5194/acp-17-11991-2017, https://doi.org/10.5194/acp-17-11991-2017, 2017
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Oxidation flow reactors (OFRs) have been increasingly used to study atmospheric chemistry at high NO. We show that it is very difficult to obtain high-NO chemistry (in terms of RO2 fate) in OFRs by initial NO injection. Past OFR studies with combustion sources generally had too-high precursor and NOx concentrations that caused several types of experimental artifacts. A strong dilution (× 100 or larger) may be needed for such experiments to avoid undesired chemistry.
Ryan Thalman, Suzane S. de Sá, Brett B. Palm, Henrique M. J. Barbosa, Mira L. Pöhlker, M. Lizabeth Alexander, Joel Brito, Samara Carbone, Paulo Castillo, Douglas A. Day, Chongai Kuang, Antonio Manzi, Nga Lee Ng, Arthur J. Sedlacek III, Rodrigo Souza, Stephen Springston, Thomas Watson, Christopher Pöhlker, Ulrich Pöschl, Meinrat O. Andreae, Paulo Artaxo, Jose L. Jimenez, Scot T. Martin, and Jian Wang
Atmos. Chem. Phys., 17, 11779–11801, https://doi.org/10.5194/acp-17-11779-2017, https://doi.org/10.5194/acp-17-11779-2017, 2017
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Particle hygroscopicity, mixing state, and the hygroscopicity of organic components were characterized in central Amazonia for 1 year; their seasonal and diel variations were driven by a combination of primary emissions, photochemical oxidation, and boundary layer development. The relationship between the hygroscopicity of organic components and their oxidation level was examined, and the results help to reconcile the differences among the relationships observed in previous studies.
Jing Chen, Sri Hapsari Budisulistiorini, Masayuki Itoh, Wen-Chien Lee, Takuma Miyakawa, Yuichi Komazaki, Liu Dong Qing Yang, and Mikinori Kuwata
Atmos. Chem. Phys., 17, 11591–11604, https://doi.org/10.5194/acp-17-11591-2017, https://doi.org/10.5194/acp-17-11591-2017, 2017
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We report size-dependent water uptake by fresh Indonesian peat burning particles and discuss relationship between water uptake and chemical characteristics. Fresh peat burning particles are almost non-hygroscopic, as determined by both the water-soluble organic fraction and the difference in κ of slightly and highly water-soluble fractions. This work experimentally validates the reference for κ of OA-dominated particles, thus contributing to more accurate estimation of aerosol climate impacts.
Wing Y. Tuet, Yunle Chen, Shierly Fok, Julie A. Champion, and Nga L. Ng
Atmos. Chem. Phys., 17, 11423–11440, https://doi.org/10.5194/acp-17-11423-2017, https://doi.org/10.5194/acp-17-11423-2017, 2017
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Exposure to secondary organic aerosols (SOAs) may have cardiopulmonary health implications. Alveolar macrophages were exposed to various SOA systems and reactive oxygen and nitrogen species production and cytokine secretion was measured post-exposure. Results from this study show that the chemical structure of SOA products may be important for determining cellular responses and demonstrate that the health effects of SOA are important to consider for the health implications of ambient aerosols.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
Wei Hu, Min Hu, Wei-Wei Hu, Jing Zheng, Chen Chen, Yusheng Wu, and Song Guo
Atmos. Chem. Phys., 17, 9979–10000, https://doi.org/10.5194/acp-17-9979-2017, https://doi.org/10.5194/acp-17-9979-2017, 2017
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Seasonal changes in chemical compositions, sources, and evolution for submicron aerosols in the megacity Beijing were investigated based on high-resolution AMS measurements. Carbonaceous fraction (OA+BC) constituted over 50 % of PM1 in autumn due to primary emissions, while SNA contributed 60 % to PM1 in other seasons. Secondary components (OOA+SNA) contributed ~ 60–80 % to PM1, suggesting that secondary formation played an important role in PM pollution. OA was in a relatively high oxidation state.
Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Philip Croteau, Manjula R. Canagaratna, John T. Jayne, Douglas R. Worsnop, and Jose L. Jimenez
Atmos. Meas. Tech., 10, 2897–2921, https://doi.org/10.5194/amt-10-2897-2017, https://doi.org/10.5194/amt-10-2897-2017, 2017
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Aerosol mass spectrometers (AMS) from ARI are used widely to measure the non-refractory species in PM1. Recently, a new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction in the commonly used standard vapourizer (SV) installed in AMS. To test the CV, the fragments, CE and size distributions of four pure inorganic species in the CV-AMS are investigated in various laboratory experiments. Results from the co-located SV-AMS are also shown as a comparison.
Dong Gao, Ting Fang, Vishal Verma, Linghan Zeng, and Rodney J. Weber
Atmos. Meas. Tech., 10, 2821–2835, https://doi.org/10.5194/amt-10-2821-2017, https://doi.org/10.5194/amt-10-2821-2017, 2017
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This work compares three methods to determine the optimal approach for quantifying the total oxidative potential (OP) of fine particles collected with filters using the dithiothreitol (DTT) assay. An automated system has been developed to facilitate the total OP measurements for use in generation of large data sets needed for epidemiology studies. The results from this study show that the water-insoluble components contribute to PM2.5 OP and the related DTT-active species are largely secondary.
Prettiny K. Ma, Yunliang Zhao, Allen L. Robinson, David R. Worton, Allen H. Goldstein, Amber M. Ortega, Jose L. Jimenez, Peter Zotter, André S. H. Prévôt, Sönke Szidat, and Patrick L. Hayes
Atmos. Chem. Phys., 17, 9237–9259, https://doi.org/10.5194/acp-17-9237-2017, https://doi.org/10.5194/acp-17-9237-2017, 2017
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Airborne particulate matter (PM) negatively impacts air quality in cities throughout the world. An important fraction of PM is organic aerosol. We have evaluated and developed several new models for secondary organic aerosol (SOA), which is formed from the chemical processing of gaseous precursors. Using our model results, we have quantified important SOA sources and precursors and also identified possible model parameterizations that could be used for air quality predictions.
Khairunnisa Yahya, Timothy Glotfelty, Kai Wang, Yang Zhang, and Athanasios Nenes
Geosci. Model Dev., 10, 2333–2363, https://doi.org/10.5194/gmd-10-2333-2017, https://doi.org/10.5194/gmd-10-2333-2017, 2017
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629, https://doi.org/10.5194/acp-17-6611-2017, https://doi.org/10.5194/acp-17-6611-2017, 2017
Petros Vasilakos, Yong-Ηa Kim, Jeffrey R. Pierce, Sotira Yiacoumi, Costas Tsouris, and Athanasios Nenes
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-96, https://doi.org/10.5194/gmd-2017-96, 2017
Revised manuscript not accepted
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Radioactive charging can significantly impact the way radioactive aerosols behave, and as a result their lifetime, but such effects are neglected in predictive model studies of radioactive plumes. We extend a well-established model that simulates the evolution of atmospheric particulate matter to account for radioactive charging effects in an accurate and computationally efficient way. It is shown that radioactivity can strongly impact the deposition patterns of aerosol.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Amber M. Ortega, Juliane L. Fry, Steven S. Brown, Kyle J. Zarzana, William Dube, Nicholas L. Wagner, Danielle C. Draper, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5331–5354, https://doi.org/10.5194/acp-17-5331-2017, https://doi.org/10.5194/acp-17-5331-2017, 2017
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Ambient forest air was oxidized by OH, O3, or NO3 inside an oxidation flow reactor, leading to formation of particulate matter from any gaseous precursors found in the air. Closure was achieved between the amount of particulate mass formed from O3 and NO3 oxidation and the amount predicted from speciated gaseous precursors, which was in contrast to previous results for OH oxidation (Palm et al., 2016). Elemental analysis of the particulate mass formed in the reactor is presented.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Rachel F. Silvern, Daniel J. Jacob, Patrick S. Kim, Eloise A. Marais, Jay R. Turner, Pedro Campuzano-Jost, and Jose L. Jimenez
Atmos. Chem. Phys., 17, 5107–5118, https://doi.org/10.5194/acp-17-5107-2017, https://doi.org/10.5194/acp-17-5107-2017, 2017
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We identify a fundamental discrepancy between thermodynamic equilibrium theory and observations of inorganic aerosol composition in the eastern US in summer that shows low ammonium sulfate aerosol ratios. In addition, from 2003 to 2013, while SO2 emissions have declined due to US emission controls, aerosols have become more acidic in the southeastern US. To explain these observations, we suggest that the large and increasing source of organic aerosol may be affecting thermodynamic equilibrium.
Kathleen M. Fahey, Annmarie G. Carlton, Havala O. T. Pye, Jaemeen Baek, William T. Hutzell, Charles O. Stanier, Kirk R. Baker, K. Wyat Appel, Mohammed Jaoui, and John H. Offenberg
Geosci. Model Dev., 10, 1587–1605, https://doi.org/10.5194/gmd-10-1587-2017, https://doi.org/10.5194/gmd-10-1587-2017, 2017
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Chemical transport models (CTMs) are a crucial tool in understanding links between emissions, air quality, and climate. Only a simple description of cloud chemistry has been implemented in many of these; however, clouds play a major role in the physicochemical processing of atmospheric species. In CMAQ, EPA’s widely used CTM, the cloud code is limited to the treatment of simple chemistry. We update CMAQ clouds to consider additional chemistry and then examine regional impacts of these updates.
Shantanu H. Jathar, Matthew Woody, Havala O. T. Pye, Kirk R. Baker, and Allen L. Robinson
Atmos. Chem. Phys., 17, 4305–4318, https://doi.org/10.5194/acp-17-4305-2017, https://doi.org/10.5194/acp-17-4305-2017, 2017
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Mobile sources such as cars and trucks are large sources of pollution in cities, but it is unclear what their relative contribution to organic particle pollution is. We used a numerical model along with recent data gathered from tests performed on cars and trucks to calculate organic particle levels in southern California. We found that model calculations agreed better with measurements and gasoline cars and trucks dominated the organic particle pollution.
Theodora Nah, Renee C. McVay, Jeffrey R. Pierce, John H. Seinfeld, and Nga L. Ng
Atmos. Chem. Phys., 17, 2297–2310, https://doi.org/10.5194/acp-17-2297-2017, https://doi.org/10.5194/acp-17-2297-2017, 2017
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We present a model framework that accounts for coagulation in chamber studies where high seed aerosol surface area concentrations are used. The uncertainties in the calculated SOA mass concentrations and yields between four different particle-wall loss correction methods over the series of α-pinene ozonolysis experiments are also assessed. We show that SOA mass yields calculated by the four methods can deviate significantly in studies where high seed aerosol surface area concentrations are used.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Adam P. Bateman, Zhaoheng Gong, Tristan H. Harder, Suzane S. de Sá, Bingbing Wang, Paulo Castillo, Swarup China, Yingjun Liu, Rachel E. O'Brien, Brett B. Palm, Hung-Wei Shiu, Glauber G. Cirino, Ryan Thalman, Kouji Adachi, M. Lizabeth Alexander, Paulo Artaxo, Allan K. Bertram, Peter R. Buseck, Mary K. Gilles, Jose L. Jimenez, Alexander Laskin, Antonio O. Manzi, Arthur Sedlacek, Rodrigo A. F. Souza, Jian Wang, Rahul Zaveri, and Scot T. Martin
Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, https://doi.org/10.5194/acp-17-1759-2017, 2017
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The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Air masses representing background conditions, urban pollution, and regional- and continental-scale biomass were measured. Anthropogenic influences contributed to the presence of nonliquid PM in the atmospheric particle population, while liquid PM dominated during periods of biogenic influence.
Anusha P. S. Hettiyadura, Thilina Jayarathne, Karsten Baumann, Allen H. Goldstein, Joost A. de Gouw, Abigail Koss, Frank N. Keutsch, Kate Skog, and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, https://doi.org/10.5194/acp-17-1343-2017, 2017
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Organosulfates are components of secondary organic aerosol (SOA) formed in the presence of sulfate. Herein, their abundance, identity, and potential to form as sampling artifacts were studied in Centreville, AL, USA. The 10 most abundant signals accounted for 58–78 % of the total, with at least 20–200 other species accounting for the remainder. These major species were largely associated with biogenic gases, like isoprene and monoterpenes, and are proposed targets for future standard development.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313, https://doi.org/10.5194/amt-10-291-2017, https://doi.org/10.5194/amt-10-291-2017, 2017
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Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Wing Y. Tuet, Yunle Chen, Lu Xu, Shierly Fok, Dong Gao, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 17, 839–853, https://doi.org/10.5194/acp-17-839-2017, https://doi.org/10.5194/acp-17-839-2017, 2017
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Secondary organic aerosols (SOA) comprise a significant fraction of particulate matter (PM) and may have health implications. The water-soluble oxidative potentials of various SOA systems were determined using dithiothreitol consumption. Results from this study demonstrate that precursor identity was more influential than reaction condition in determining SOA oxidative potential and highlight a need to consider SOA contributions from anthropogenic hydrocarbons to PM-induced health effects.
Provat K. Saha, Andrey Khlystov, Khairunnisa Yahya, Yang Zhang, Lu Xu, Nga L. Ng, and Andrew P. Grieshop
Atmos. Chem. Phys., 17, 501–520, https://doi.org/10.5194/acp-17-501-2017, https://doi.org/10.5194/acp-17-501-2017, 2017
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192, https://doi.org/10.5194/acp-17-175-2017, https://doi.org/10.5194/acp-17-175-2017, 2017
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Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Stelios Myriokefalitakis, Athanasios Nenes, Alex R. Baker, Nikolaos Mihalopoulos, and Maria Kanakidou
Biogeosciences, 13, 6519–6543, https://doi.org/10.5194/bg-13-6519-2016, https://doi.org/10.5194/bg-13-6519-2016, 2016
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The global atmospheric cycle of P is simulated accounting for natural and anthropogenic sources, acid dissolution of dust aerosol and changes in atmospheric acidity. Simulations show that P-containing dust dissolution flux may have increased in the last 150 years but is expected to decrease in the future, and biological particles are important carriers of bioavailable P to the ocean. These insights to the P cycle have important implications for marine ecosystem responses to climate change.
Yaping Zhang, Brent J. Williams, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 5637–5653, https://doi.org/10.5194/amt-9-5637-2016, https://doi.org/10.5194/amt-9-5637-2016, 2016
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The binning method provides an alternate way to process GC–MS data in a very fast manner. It only takes a very small portion of time (days versus years) compared to the traditional GC–MS data analysis method (peak identification and integration). Furthermore, the binning method can also be applied to any data set from a measurement (mass spectrometry, spectroscopy, etc.) with additional separations (volatility, polarity, size, etc.).
Neha Sareen, Annmarie G. Carlton, Jason D. Surratt, Avram Gold, Ben Lee, Felipe D. Lopez-Hilfiker, Claudia Mohr, Joel A. Thornton, Zhenfa Zhang, Yong B. Lim, and Barbara J. Turpin
Atmos. Chem. Phys., 16, 14409–14420, https://doi.org/10.5194/acp-16-14409-2016, https://doi.org/10.5194/acp-16-14409-2016, 2016
Maiko Arashiro, Ying-Hsuan Lin, Kenneth G. Sexton, Zhenfa Zhang, Ilona Jaspers, Rebecca C. Fry, William G. Vizuete, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 14079–14090, https://doi.org/10.5194/acp-16-14079-2016, https://doi.org/10.5194/acp-16-14079-2016, 2016
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Atmospheric oxidation of isoprene in the presence of acidic sulfate aerosol yields substantial SOA. Potential adverse health effects resulting from exposure to this aerosol type are largely unknown. Measurements of gene expression of known inflammatory biomarkers interleukin 8 (IL-8) and cyclooxygenase 2 (COX-2) in exposed human lung cells at the air–liquid interface showed that a dose of 0.067 μg cm−2 of isoprene SOA leads to statistically significant increases in IL-8 and COX-2 mRNA levels.
Omar Amador-Muñoz, Pawel K. Misztal, Robin Weber, David R. Worton, Haofei Zhang, Greg Drozd, and Allen H. Goldstein
Atmos. Meas. Tech., 9, 5315–5329, https://doi.org/10.5194/amt-9-5315-2016, https://doi.org/10.5194/amt-9-5315-2016, 2016
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Proton transfer reaction mass spectrometry (PTR-MS) was used to detect n-alkanes that generally have a lower proton affinity than water and therefore proton transfer (PT) by reaction with H3O+ is not an effective mechanism for their detection. In this study, we developed a method using a conventional PTR-MS to detect n-alkanes by optimizing ion source and drift tube conditions to vary the relative amounts of different primary ions (H3O+, O2+, NO+) in the reaction chamber (drift tube).
Amelia F. Longo, David J. Vine, Laura E. King, Michelle Oakes, Rodney J. Weber, Lewis Gregory Huey, Armistead G. Russell, and Ellery D. Ingall
Atmos. Chem. Phys., 16, 13389–13398, https://doi.org/10.5194/acp-16-13389-2016, https://doi.org/10.5194/acp-16-13389-2016, 2016
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New synchrotron-based techniques were applied to characterize the oxidation state and composition of sulfur in ambient aerosol and emission sources. Individual particles were found to contain surprisingly high levels of elemental sulfur, a form of sulfur found in only one of the emission sources analyzed. We also show metal sulfates as a key component of urban aerosols. These metal sulfate phases are highly soluble and are indicative of acidic processes transforming metals in the environment.
Wei Hu, Min Hu, Wei-Wei Hu, Hongya Niu, Jing Zheng, Yusheng Wu, Wentai Chen, Chen Chen, Lingyu Li, Min Shao, Shaodong Xie, and Yuanhang Zhang
Atmos. Chem. Phys., 16, 13213–13230, https://doi.org/10.5194/acp-16-13213-2016, https://doi.org/10.5194/acp-16-13213-2016, 2016
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An Aerodyne high-resolution time-of-flight AMS was deployed at a suburban site in the Sichuan Basin, southwestern China, under high emission intensity, and unique geographical and adverse meteorological conditions. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. The contributions of BBOA and BC to PM1 were high in primary emission episodes, highlighting the critical influence of biomass burning.
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Aki Pajunoja, Weiwei Hu, Yu J. Leong, Nathan F. Taylor, Pasi Miettinen, Brett B. Palm, Santtu Mikkonen, Don R. Collins, Jose L. Jimenez, and Annele Virtanen
Atmos. Chem. Phys., 16, 11163–11176, https://doi.org/10.5194/acp-16-11163-2016, https://doi.org/10.5194/acp-16-11163-2016, 2016
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The phase state of ambient particles was inferred from bounce measurements conducted at a rural site in central Alabama during the SOAS campaign. The organic-dominated ambient particles are mostly in the liquid phase at summertime conditions but they turn semisolid when dried in the measurement setup. Bounce humidograms reveal that the hygroscopicity and oxidation of the particles decreases the liquefying RH. The effect of oxidation is emphasized by oxidation flow reactor measurements.
Matthieu Riva, Thais Da Silva Barbosa, Ying-Hsuan Lin, Elizabeth A. Stone, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 11001–11018, https://doi.org/10.5194/acp-16-11001-2016, https://doi.org/10.5194/acp-16-11001-2016, 2016
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Formation of organosulfates (OSs) in secondary organic aerosol from the photooxidation of alkanes is reported from smog chamber experiments. Effects of acidity and relative humidity on OS formation were examined. Most of the OSs identified could be explained by formation of gaseous epoxide and/or hydroperoxide precursors with subsequent acid-catalyzed multiphase chemistry onto sulfate aerosol. The OSs identified here were also observed and quantified in aerosols collected in two urban areas.
Javier Sanchez, David J. Tanner, Dexian Chen, L. Gregory Huey, and Nga L. Ng
Atmos. Meas. Tech., 9, 3851–3861, https://doi.org/10.5194/amt-9-3851-2016, https://doi.org/10.5194/amt-9-3851-2016, 2016
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HO2 radicals play an important role in tropospheric chemistry. Here we propose a new direct method for measuring HO2 radicals in the atmosphere using bromide anion chemical ionization mass spectrometry. Ambient measurements in Atlanta are presented. Instrument performance parameters: sensitivity, lower detection limit, and time resolution are discussed. We demonstrate that the technique provides excellent selectivity and is suitable for in situ ground-based HO2 measurements.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Monica Crippa, Jose-Luis Jimenez, Eriko Nemitz, Karine Sellegri, Mikko Äijälä, Samara Carbone, Claudia Mohr, Colin O'Dowd, Laurent Poulain, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 10313–10332, https://doi.org/10.5194/acp-16-10313-2016, https://doi.org/10.5194/acp-16-10313-2016, 2016
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Recent studies based on aerosol mass spectrometer measurements revealed that the organic fraction dominates the non-refractory PM1 composition. However its representation in chemical transport models is still very challenging due to uncertainties in emission sources and formation pathways. In this study, a novel organic aerosol scheme was tested in the regional air quality model CAMx and results were compared with ambient measurements at 11 different sites in Europe.
Pawel K. Misztal, Jeremy C. Avise, Thomas Karl, Klaus Scott, Haflidi H. Jonsson, Alex B. Guenther, and Allen H. Goldstein
Atmos. Chem. Phys., 16, 9611–9628, https://doi.org/10.5194/acp-16-9611-2016, https://doi.org/10.5194/acp-16-9611-2016, 2016
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In this study, for the first time regional BVOC models are compared with direct regional measurements of fluxes from aircraft, allowing assessment of model accuracy at scales relevant to air quality modeling. We directly assess modeled isoprene emission inventories which are important for regional air quality simulations of ozone and secondary particle concentrations.
Matthew J. Alvarado, Chantelle R. Lonsdale, Helen L. Macintyre, Huisheng Bian, Mian Chin, David A. Ridley, Colette L. Heald, Kenneth L. Thornhill, Bruce E. Anderson, Michael J. Cubison, Jose L. Jimenez, Yutaka Kondo, Lokesh K. Sahu, Jack E. Dibb, and Chien Wang
Atmos. Chem. Phys., 16, 9435–9455, https://doi.org/10.5194/acp-16-9435-2016, https://doi.org/10.5194/acp-16-9435-2016, 2016
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Understanding the scattering and absorption of light by aerosols is necessary for understanding air quality and climate change. We used data from the 2008 ARCTAS campaign to evaluate aerosol optical property models using a closure methodology that separates errors in these models from other errors in aerosol emissions, chemistry, or transport. We find that the models on average perform reasonably well, and make suggestions for how remaining biases could be reduced.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Theodora Nah, Renee C. McVay, Xuan Zhang, Christopher M. Boyd, John H. Seinfeld, and Nga L. Ng
Atmos. Chem. Phys., 16, 9361–9379, https://doi.org/10.5194/acp-16-9361-2016, https://doi.org/10.5194/acp-16-9361-2016, 2016
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The influence of seed aerosol surface area and oxidation rate on SOA formation in α-pinene ozonolysis is studied. SOA growth rate and mass yields are independent of seed surface area, consistent with the condensation of SOA-forming vapors being dominated by quasi-equilibrium growth. Faster α-pinene oxidation rates and higher SOA mass yields are observed at increasing O3 concentrations, indicating that a faster α-pinene oxidation rate leads to rapidly produced SOA-forming oxidation products.
Jordan E. Krechmer, Michael Groessl, Xuan Zhang, Heikki Junninen, Paola Massoli, Andrew T. Lambe, Joel R. Kimmel, Michael J. Cubison, Stephan Graf, Ying-Hsuan Lin, Sri H. Budisulistiorini, Haofei Zhang, Jason D. Surratt, Richard Knochenmuss, John T. Jayne, Douglas R. Worsnop, Jose-Luis Jimenez, and Manjula R. Canagaratna
Atmos. Meas. Tech., 9, 3245–3262, https://doi.org/10.5194/amt-9-3245-2016, https://doi.org/10.5194/amt-9-3245-2016, 2016
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Luping Su, Edward G. Patton, Jordi Vilà-Guerau de Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong-Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, and John E. Mak
Atmos. Chem. Phys., 16, 7725–7741, https://doi.org/10.5194/acp-16-7725-2016, https://doi.org/10.5194/acp-16-7725-2016, 2016
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Hannah M. Allen, Benjamin R. Ayres, Steven S. Brown, William H. Brune, John D. Crounse, Joost de Gouw, Danielle C. Draper, Philip A. Feiner, Juliane L. Fry, Allen H. Goldstein, Abigail Koss, Pawel K. Misztal, Tran B. Nguyen, Kevin Olson, Alex P. Teng, Paul O. Wennberg, Robert J. Wild, Li Zhang, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 7623–7637, https://doi.org/10.5194/acp-16-7623-2016, https://doi.org/10.5194/acp-16-7623-2016, 2016
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The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the southeastern United States. At warm temperatures in the daytime boundary layer, NOx interconverts rapidly with both PAN and alkyl and multifunctional nitrates (RONO2), and the relevant lifetime is the combined lifetime of these three classes. We find that the production of RONO2, followed by hydrolysis to produce nitric acid, is the dominant pathway for NOx removal in an isoprene dominated forest.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409, https://doi.org/10.5194/acp-16-7389-2016, https://doi.org/10.5194/acp-16-7389-2016, 2016
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BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Riinu Ots, Dominique E. Young, Massimo Vieno, Lu Xu, Rachel E. Dunmore, James D. Allan, Hugh Coe, Leah R. Williams, Scott C. Herndon, Nga L. Ng, Jacqueline F. Hamilton, Robert Bergström, Chiara Di Marco, Eiko Nemitz, Ian A. Mackenzie, Jeroen J. P. Kuenen, David C. Green, Stefan Reis, and Mathew R. Heal
Atmos. Chem. Phys., 16, 6453–6473, https://doi.org/10.5194/acp-16-6453-2016, https://doi.org/10.5194/acp-16-6453-2016, 2016
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This study investigates the contribution of diesel vehicle emissions to organic aerosol formation and particulate matter concentrations in London. Comparisons of simulated pollutant concentrations with observations show good agreement and give confidence in the skill of the model applied. The contribution of diesel vehicle emissions, which are currently not included in official emissions inventories, is demonstrated to be substantial, indicating that more research on this topic is required.
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Sri Hapsari Budisulistiorini, Karsten Baumann, Eric S. Edgerton, Solomon T. Bairai, Stephen Mueller, Stephanie L. Shaw, Eladio M. Knipping, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 5171–5189, https://doi.org/10.5194/acp-16-5171-2016, https://doi.org/10.5194/acp-16-5171-2016, 2016
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A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor, collocated with established air-monitoring network measurements, to identify sources of organic aerosol (OA). Further, high-volume filter samples were collected for measurements of OA tracers by offline mass spectrometry tools.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Alexis R. Attwood, Andreas Beyersdorf, Pedro Campuzano-Jost, Annmarie G. Carlton, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Nga L. Ng, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Rebecca A. Washenfelder, Andre Welti, Lu Xu, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 4987–5007, https://doi.org/10.5194/acp-16-4987-2016, https://doi.org/10.5194/acp-16-4987-2016, 2016
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Microscopic pollution particles make the atmosphere look hazy and also cool the earth by sending sunlight back to space. When the air is moist, these particles swell with water and scatter even more sunlight. We showed that particles formed from organic material – which dominates particulate pollution in the southeastern U.S. – does not take up water very effectively, toward the low end of most previous studies. We also found a better way to mathematically describe this swelling process.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Andreas Beyersdorf, Pedro Campuzano-Jost, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Andre Welti, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 5009–5019, https://doi.org/10.5194/acp-16-5009-2016, https://doi.org/10.5194/acp-16-5009-2016, 2016
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Two research aircraft made dozens of vertical profiles over rural areas in the southeastern US in summer 2013. These measurements show that, in addition to how much pollution was present and how moist the atmosphere was, the size of the pollutant particles affected how much sunlight was reflected back to space. These measurements will help climate modelers determine which characteristics of pollution are important to predict with accuracy.
Weruka Rattanavaraha, Kevin Chu, Sri Hapsari Budisulistiorini, Matthieu Riva, Ying-Hsuan Lin, Eric S. Edgerton, Karsten Baumann, Stephanie L. Shaw, Hongyu Guo, Laura King, Rodney J. Weber, Miranda E. Neff, Elizabeth A. Stone, John H. Offenberg, Zhenfa Zhang, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 4897–4914, https://doi.org/10.5194/acp-16-4897-2016, https://doi.org/10.5194/acp-16-4897-2016, 2016
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The mechanisms by which specific anthropogenic pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected from Birmingham, AL, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Isoprene SOA tracers were measured from these samples and compared to gas and aerosol data collected from the SEARCH network.
S. T. Martin, P. Artaxo, L. A. T. Machado, A. O. Manzi, R. A. F. Souza, C. Schumacher, J. Wang, M. O. Andreae, H. M. J. Barbosa, J. Fan, G. Fisch, A. H. Goldstein, A. Guenther, J. L. Jimenez, U. Pöschl, M. A. Silva Dias, J. N. Smith, and M. Wendisch
Atmos. Chem. Phys., 16, 4785–4797, https://doi.org/10.5194/acp-16-4785-2016, https://doi.org/10.5194/acp-16-4785-2016, 2016
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The Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Experiment took place in central Amazonia throughout 2014 and 2015. The experiment focused on the complex links among vegetation, atmospheric chemistry, and aerosol production on the one hand and their connections to aerosols, clouds, and precipitation on the other, especially when altered by urban pollution. This article serves as an introduction to the special issue of publications presenting findings of this experiment.
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, https://doi.org/10.5194/acp-16-4579-2016, 2016
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Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
Brent J. Williams, Yaping Zhang, Xiaochen Zuo, Raul E. Martinez, Michael J. Walker, Nathan M. Kreisberg, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 1569–1586, https://doi.org/10.5194/amt-9-1569-2016, https://doi.org/10.5194/amt-9-1569-2016, 2016
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The thermal desorption aerosol gas chromatograph (TAG) has been used for in situ measurements of organic marker compounds to identify atmospheric particle sources and transformation processes. Here we identify that inorganic aerosol components (e.g., nitrate and sulfate) and highly oxygenated organic components experience thermal decomposition upon sample heating. This thermal decomposition signal in the TAG system is investigated through laboratory and field data.
Zhe Peng, Douglas A. Day, Amber M. Ortega, Brett B. Palm, Weiwei Hu, Harald Stark, Rui Li, Kostas Tsigaridis, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 4283–4305, https://doi.org/10.5194/acp-16-4283-2016, https://doi.org/10.5194/acp-16-4283-2016, 2016
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Oxidation flow reactors (OFRs) are promising tools of studying atmospheric oxidation processes. Elevated concentrations of both OH and non-OH oxidants in OFRs leave room for speculation that non-OH chemistry can play a major role. Through systematic modeling, we find conditions where non-OH VOC fate is significant and show that, in most field studies of SOA using OFRs, non-OH VOC fate in OFRs was insignificant. We also provide guidelines helping OFR users avoid significant non-OH VOC oxidation.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061, https://doi.org/10.5194/acp-16-4043-2016, https://doi.org/10.5194/acp-16-4043-2016, 2016
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A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Matthew C. Woody, Kirk R. Baker, Patrick L. Hayes, Jose L. Jimenez, Bonyoung Koo, and Havala O. T. Pye
Atmos. Chem. Phys., 16, 4081–4100, https://doi.org/10.5194/acp-16-4081-2016, https://doi.org/10.5194/acp-16-4081-2016, 2016
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In this work, organic aerosol (OA) predictions from the volatility basis set (VBS) module in the CMAQ photochemical transport model were evaluated against routine monitoring data and measurements collected during the 2010 CalNex field study. We found that the VBS module more accurately reproduced the observed primary/secondary OA split and secondary OA (SOA) mass at the CalNex Pasadena ground site compared to the traditional CMAQ OA module but still underpredicted observed SOA by ~ 5.2 ×.
Ting Fang, Vishal Verma, Josephine T. Bates, Joseph Abrams, Mitchel Klein, Matthew J. Strickland, Stefanie E. Sarnat, Howard H. Chang, James A. Mulholland, Paige E. Tolbert, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 16, 3865–3879, https://doi.org/10.5194/acp-16-3865-2016, https://doi.org/10.5194/acp-16-3865-2016, 2016
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Ascorbic acid (AA) and Dithiothreitol (DTT) assay measures of water-soluble PM2.5 oxidative potential (OP) are compared in terms of spatiotemporal trends, chemical selectivity, sources, and health impacts based on an epidemiological study with backcast estimated OP. Both assays point to metals from brake/tire wear, but only the DTT assay also identifies organics from combustion. DTT is associated with emergency department visits for asthma/wheeze and congestive heart failure, whereas AA is not.
Yong-ha Kim, Sotira Yiacoumi, Athanasios Nenes, and Costas Tsouris
Atmos. Chem. Phys., 16, 3449–3462, https://doi.org/10.5194/acp-16-3449-2016, https://doi.org/10.5194/acp-16-3449-2016, 2016
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Three microphysical approaches are proposed to incorporate mutual effects of particle charging and coagulation in predictions of transient charge and size distributions of atmospheric particles, including radioactive aerosols. The three approaches have different levels of complexities and are applicable to various laboratory and field atmospheric studies. Also, these approaches can be easily incorporated into aerosol transport models at different scales to account for particle charging effects.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
Brett B. Palm, Pedro Campuzano-Jost, Amber M. Ortega, Douglas A. Day, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, James F. Hunter, Eben S. Cross, Jesse H. Kroll, Zhe Peng, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 2943–2970, https://doi.org/10.5194/acp-16-2943-2016, https://doi.org/10.5194/acp-16-2943-2016, 2016
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Ambient pine forest air was oxidized by OH radicals in a PAM oxidation flow reactor during the BEACHON-RoMBAS campaign to study secondary organic aerosol formation. Approximately 4.4 times more secondary organic aerosol was formed in the reactor than could be explained by the volatile organic gases (VOCs) measured in ambient air. The organic aerosol formation can be explained by including an SOA yield from typically unmeasured semivolatile and intermediate-volatility organic gases (S/IVOCs).
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
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We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
E. A. Marais, D. J. Jacob, J. L. Jimenez, P. Campuzano-Jost, D. A. Day, W. Hu, J. Krechmer, L. Zhu, P. S. Kim, C. C. Miller, J. A. Fisher, K. Travis, K. Yu, T. F. Hanisco, G. M. Wolfe, H. L. Arkinson, H. O. T. Pye, K. D. Froyd, J. Liao, and V. F. McNeill
Atmos. Chem. Phys., 16, 1603–1618, https://doi.org/10.5194/acp-16-1603-2016, https://doi.org/10.5194/acp-16-1603-2016, 2016
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Isoprene secondary organic aerosol (SOA) is a dominant aerosol component in the southeast US, but models routinely underestimate isoprene SOA with traditional schemes based on chamber studies operated under conditions not representative of isoprene-emitting forests. We develop a new irreversible uptake mechanism to reproduce isoprene SOA yields (3.3 %) and composition, and find a factor of 2 co-benefit of SO2 emission controls on reducing sulfate and organic aerosol in the southeast US.
T. P. Riedel, Y.-H. Lin, Z. Zhang, K. Chu, J. A. Thornton, W. Vizuete, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 16, 1245–1254, https://doi.org/10.5194/acp-16-1245-2016, https://doi.org/10.5194/acp-16-1245-2016, 2016
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IEPOX, a photooxidation product of isoprene, contributes to ambient secondary organic aerosol concentrations. Controlled atmospheric chamber experiments and modeling are used to extract formation rate information of chemical species that contribute to IEPOX-derived secondary organic aerosol.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
A. W. H. Chan, N. M. Kreisberg, T. Hohaus, P. Campuzano-Jost, Y. Zhao, D. A. Day, L. Kaser, T. Karl, A. Hansel, A. P. Teng, C. R. Ruehl, D. T. Sueper, J. T. Jayne, D. R. Worsnop, J. L. Jimenez, S. V. Hering, and A. H. Goldstein
Atmos. Chem. Phys., 16, 1187–1205, https://doi.org/10.5194/acp-16-1187-2016, https://doi.org/10.5194/acp-16-1187-2016, 2016
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Using a novel instrument, we have made measurements of organic compounds that can exist as a gas or particle in the rural atmosphere. Through hourly measurements, we have identified the sources and atmospheric processes of these compounds, which are important for modeling the climate and health impact of these emissions.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
J. Timkovsky, A. W. H. Chan, T. Dorst, A. H. Goldstein, B. Oyama, and R. Holzinger
Atmos. Meas. Tech., 8, 5177–5187, https://doi.org/10.5194/amt-8-5177-2015, https://doi.org/10.5194/amt-8-5177-2015, 2015
S. J. Lawson, M. D. Keywood, I. E. Galbally, J. L. Gras, J. M. Cainey, M. E. Cope, P. B. Krummel, P. J. Fraser, L. P. Steele, S. T. Bentley, C. P. Meyer, Z. Ristovski, and A. H. Goldstein
Atmos. Chem. Phys., 15, 13393–13411, https://doi.org/10.5194/acp-15-13393-2015, https://doi.org/10.5194/acp-15-13393-2015, 2015
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Biomass burning (BB) plumes were opportunistically measured at the Cape Grim Baseline Station in Tasmania, Australia. We provide a unique set of trace gas and particle emission factors for temperate Australian coastal heathland fires, and attribute a major short-lived enhancement in emission ratios to a minor rainfall event. The ability of BB particles to act as cloud condensation nuclei, and the contribution of BB emissions to observed particle growth and ozone enhancements are discussed.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
Z. Peng, D. A. Day, H. Stark, R. Li, J. Lee-Taylor, B. B. Palm, W. H. Brune, and J. L. Jimenez
Atmos. Meas. Tech., 8, 4863–4890, https://doi.org/10.5194/amt-8-4863-2015, https://doi.org/10.5194/amt-8-4863-2015, 2015
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
A. Guha, D. R. Gentner, R. J. Weber, R. Provencal, and A. H. Goldstein
Atmos. Chem. Phys., 15, 12043–12063, https://doi.org/10.5194/acp-15-12043-2015, https://doi.org/10.5194/acp-15-12043-2015, 2015
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We perform a positive matrix factorization (PMF)-based source apportionment by combining GHG measurements with coincident VOC measurements in the San Joaquin Valley of California. Using VOCs as source tracers, we identify dairies and livestock as major sources of CH4 and N2O in the region. Agriculture is a significant source of N2O enhancements too, while vehicle emissions are found to be a negligible source of N2O. The findings are relevant to the state’s GHG inventory verification process.
W. W. Hu, P. Campuzano-Jost, B. B. Palm, D. A. Day, A. M. Ortega, P. L. Hayes, J. E. Krechmer, Q. Chen, M. Kuwata, Y. J. Liu, S. S. de Sá, K. McKinney, S. T. Martin, M. Hu, S. H. Budisulistiorini, M. Riva, J. D. Surratt, J. M. St. Clair, G. Isaacman-Van Wertz, L. D. Yee, A. H. Goldstein, S. Carbone, J. Brito, P. Artaxo, J. A. de Gouw, A. Koss, A. Wisthaler, T. Mikoviny, T. Karl, L. Kaser, W. Jud, A. Hansel, K. S. Docherty, M. L. Alexander, N. H. Robinson, H. Coe, J. D. Allan, M. R. Canagaratna, F. Paulot, and J. L. Jimenez
Atmos. Chem. Phys., 15, 11807–11833, https://doi.org/10.5194/acp-15-11807-2015, https://doi.org/10.5194/acp-15-11807-2015, 2015
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This work summarized all the studies reporting isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) measured globally by aerosol mass spectrometer and compare them with modeled gas-phase IEPOX, with results suggestive of the importance of IEPOX-SOA for regional and global OA budgets. A real-time tracer of IEPOX-SOA is thoroughly evaluated for the first time by combing multiple field and chamber studies. A quick and easy empirical method on IEPOX-SOA estimation is also presented.
T. Fang, H. Guo, V. Verma, R. E. Peltier, and R. J. Weber
Atmos. Chem. Phys., 15, 11667–11682, https://doi.org/10.5194/acp-15-11667-2015, https://doi.org/10.5194/acp-15-11667-2015, 2015
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This work presented a new method of quantifying water-soluble elements in PM2.5 aqueous extracts (N~500) with an X-ray fluorescence analyzer. The results indicate that water-soluble elements had marked spatial and temporal patterns. Four sources were resolved: brake/tire wear, biomass burning, secondary formation, and mineral dust. The findings have informed studies on aerosol oxidative potential and provided insights into the health effects of water-soluble metals, especially Cu, Fe, Mn and Zn.
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, F. Canonaco, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, H. Coe, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, E. Nemitz, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11291–11309, https://doi.org/10.5194/acp-15-11291-2015, https://doi.org/10.5194/acp-15-11291-2015, 2015
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Trace element measurements in three particle size ranges (PM10-2.5, PM2.5-1.0 and PM1.0-0.3) were performed with 2h time resolution at kerbside, urban background and rural sites during the ClearfLo winter 2012 campaign in London. The environment-dependent variability of emissions was characterized using the Multilinear Engine implementation of the positive matrix factorization model. A total of nine different factors were resolved from local, regional and natural origin.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
C. G. Nolte, K. W. Appel, J. T. Kelly, P. V. Bhave, K. M. Fahey, J. L. Collett Jr., L. Zhang, and J. O. Young
Geosci. Model Dev., 8, 2877–2892, https://doi.org/10.5194/gmd-8-2877-2015, https://doi.org/10.5194/gmd-8-2877-2015, 2015
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This study is the most comprehensive evaluation of CMAQ inorganic
aerosol size-composition distributions conducted to date. We compare two
methods of inferring PM2.5 concentrations from the model: (1) based on
the sum of the masses in the fine aerosol modes, as is most commonly
done in CMAQ model evaluation; and (2) computed using the simulated size
distributions. Differences are generally less than 1 microgram/m3, and
are largest over the eastern USA during the summer.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215, https://doi.org/10.5194/acp-15-9203-2015, https://doi.org/10.5194/acp-15-9203-2015, 2015
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Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
A. Hodzic, S. Madronich, P. S. Kasibhatla, G. Tyndall, B. Aumont, J. L. Jimenez, J. Lee-Taylor, and J. Orlando
Atmos. Chem. Phys., 15, 9253–9269, https://doi.org/10.5194/acp-15-9253-2015, https://doi.org/10.5194/acp-15-9253-2015, 2015
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Our study combines process and global chemistry modeling to investigate the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Photolysis of the oxidation intermediates that partition between gas and particle phases to form SOA is not included in 3D models. Our results suggest that exposure to UV light can suppress the formation of SOA or even lead to its substantial loss (comparable to wet deposition).
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, https://doi.org/10.5194/acp-15-8679-2015, 2015
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The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder.
The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents.
No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio.
The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
J. Liu, E. Scheuer, J. Dibb, G. S. Diskin, L. D. Ziemba, K. L. Thornhill, B. E. Anderson, A. Wisthaler, T. Mikoviny, J. J. Devi, M. Bergin, A. E. Perring, M. Z. Markovic, J. P. Schwarz, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, and R. J. Weber
Atmos. Chem. Phys., 15, 7841–7858, https://doi.org/10.5194/acp-15-7841-2015, https://doi.org/10.5194/acp-15-7841-2015, 2015
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Brown carbon (BrC) is found throughout the US continental troposphere during a summer of extensive biomass burning and its prevalence relative to black carbon (BC) increases with altitude. A radiative transfer model based on direct measurements of aerosol scattering and absorption by BC and BrC shows BrC reduces top-of-atmosphere forcing by 20%. A method to estimate BrC radiative forcing efficiencies from surface-based measurements is provided.
Y. Shinozuka, A. D. Clarke, A. Nenes, A. Jefferson, R. Wood, C. S. McNaughton, J. Ström, P. Tunved, J. Redemann, K. L. Thornhill, R. H. Moore, T. L. Lathem, J. J. Lin, and Y. J. Yoon
Atmos. Chem. Phys., 15, 7585–7604, https://doi.org/10.5194/acp-15-7585-2015, https://doi.org/10.5194/acp-15-7585-2015, 2015
C. M. Boyd, J. Sanchez, L. Xu, A. J. Eugene, T. Nah, W. Y. Tuet, M. I. Guzman, and N. L. Ng
Atmos. Chem. Phys., 15, 7497–7522, https://doi.org/10.5194/acp-15-7497-2015, https://doi.org/10.5194/acp-15-7497-2015, 2015
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Laboratory chamber studies were conducted to investigate the formation of secondary organic aerosol from β-pinene oxidation by nitrate radicals. These experiments probed the effects of peroxy radical fate and relative humidity on the mass and chemical composition of secondary organic aerosol formed from nighttime chemistry. Results from this study were used to evaluate the contributions of NO3+monoterpene reaction to ambient organic aerosol recently measured in the southeastern United States.
G. Wohlfahrt, C. Amelynck, C. Ammann, A. Arneth, I. Bamberger, A. H. Goldstein, L. Gu, A. Guenther, A. Hansel, B. Heinesch, T. Holst, L. Hörtnagl, T. Karl, Q. Laffineur, A. Neftel, K. McKinney, J. W. Munger, S. G. Pallardy, G. W. Schade, R. Seco, and N. Schoon
Atmos. Chem. Phys., 15, 7413–7427, https://doi.org/10.5194/acp-15-7413-2015, https://doi.org/10.5194/acp-15-7413-2015, 2015
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Methanol is the second most abundant volatile organic compound in the troposphere and plays a significant role in atmospheric chemistry. While there is consensus about the dominant role of plants as the major source and the reaction with OH as the major sink, global methanol budgets diverge considerably in terms of source/sink estimates. Here we present micrometeorological methanol flux data from eight sites in order to provide a first cross-site synthesis of the terrestrial methanol exchange.
L. Xu, S. Suresh, H. Guo, R. J. Weber, and N. L. Ng
Atmos. Chem. Phys., 15, 7307–7336, https://doi.org/10.5194/acp-15-7307-2015, https://doi.org/10.5194/acp-15-7307-2015, 2015
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Year-long comprehensive characterization of ambient aerosol was performed in both rural and urban sites in the southeastern US as part of Southeastern Center of Air Pollution and Epidemiology (SCAPE) study and Southeastern Oxidant and Aerosol Study (SOAS). Three independent methods were applied to estimate the concentration of particle-phase organic nitrates. The spatial distribution of organic aerosol is investigated by comparing simultaneous HR-ToF-AMS and ACSM measurements at different sites.
S. Myriokefalitakis, N. Daskalakis, N. Mihalopoulos, A. R. Baker, A. Nenes, and M. Kanakidou
Biogeosciences, 12, 3973–3992, https://doi.org/10.5194/bg-12-3973-2015, https://doi.org/10.5194/bg-12-3973-2015, 2015
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The global atmospheric cycle of Fe is simulated accounting for natural and combustion sources, proton- and organic ligand-promoted Fe dissolution from dust aerosol and changes in anthropogenic emissions, and thus in atmospheric acidity. Simulations show that Fe dissolution may have increased in the last 150 years and is expected to decrease due to air pollution regulations. Reductions in dissolved-Fe deposition can further limit the primary productivity over high-nutrient-low-chlorophyll water.
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
M. J. Cubison and J. L. Jimenez
Atmos. Meas. Tech., 8, 2333–2345, https://doi.org/10.5194/amt-8-2333-2015, https://doi.org/10.5194/amt-8-2333-2015, 2015
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
J. W. Taylor, J. D. Allan, D. Liu, M. Flynn, R. Weber, X. Zhang, B. L. Lefer, N. Grossberg, J. Flynn, and H. Coe
Atmos. Meas. Tech., 8, 1701–1718, https://doi.org/10.5194/amt-8-1701-2015, https://doi.org/10.5194/amt-8-1701-2015, 2015
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When using the SP2 to report black carbon core/shell coating thickness, the core density and refractive index must be estimated from literature values. We systematically vary the assumed parameters and the instrument calibration, and quantify the effects in the derived coatings. The technique is highly sensitive to the core refractive index but has only a minor sensitivity to the core density and coating refractive index. We identify the most appropriate values to use in future analysis.
Q. Chen, D. K. Farmer, L. V. Rizzo, T. Pauliquevis, M. Kuwata, T. G. Karl, A. Guenther, J. D. Allan, H. Coe, M. O. Andreae, U. Pöschl, J. L. Jimenez, P. Artaxo, and S. T. Martin
Atmos. Chem. Phys., 15, 3687–3701, https://doi.org/10.5194/acp-15-3687-2015, https://doi.org/10.5194/acp-15-3687-2015, 2015
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Submicron particle mass concentration in the Amazon during the wet season of 2008 was dominated by organic material. The PMF analysis finds a comparable importance of gas-phase (gas-to-particle condensation) and particle-phase (reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets) production of secondary organic material during the study period, together accounting for >70% of the organic-particle mass concentration.
A. Ripoll, M. C. Minguillón, J. Pey, J. L. Jimenez, D. A. Day, Y. Sosedova, F. Canonaco, A. S. H. Prévôt, X. Querol, and A. Alastuey
Atmos. Chem. Phys., 15, 2935–2951, https://doi.org/10.5194/acp-15-2935-2015, https://doi.org/10.5194/acp-15-2935-2015, 2015
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Real-time measurements of inorganic (sulfate, nitrate, ammonium, chloride and black carbon (BC)) and organic submicron aerosols from a continental background site (Montsec, MSC, 1570m a.s.l.) in the western Mediterranean Basin (WMB) were conducted for 10 months (July 2011 - April 2012) with an aerosol chemical speciation monitor (ACSM). The ACSM was co-located with other online and offline PM1 measurements. Analyses of the hourly, diurnal, and seasonal variations are presented here.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, R. Dressler, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, S. C. Herndon, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, A. Detournay, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 2367–2386, https://doi.org/10.5194/acp-15-2367-2015, https://doi.org/10.5194/acp-15-2367-2015, 2015
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Ambient concentrations of trace elements with 2h time resolution were measured in three size ranges (PM10–2.5, PM2.5–1.0, PM1.0–0.3) at kerbside, urban background and rural sites in London during the ClearfLo (Clean Air for London) field campaign. Quantification of kerb and urban increments, and assessment of diurnal and weekly variability provided insight into sources governing urban air quality and the effects of urban micro-environments on human exposure.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
T. Fang, V. Verma, H. Guo, L. E. King, E. S. Edgerton, and R. J. Weber
Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, https://doi.org/10.5194/amt-8-471-2015, 2015
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This work summarizes a newly developed semi-automated system for quantifying the oxidative potential of aerosol aqueous extracts using the dithiothreitol (DTT) assay. 500 sample analyses indicate that DTT activity in the southeast US is likely not dominated by a unique local source, and sources change with season. The unique large data set generated with the technique described in this paper allows new studies on DTT sources and investigating linkages between reactive oxygen species and health.
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
C. Knote, A. Hodzic, and J. L. Jimenez
Atmos. Chem. Phys., 15, 1–18, https://doi.org/10.5194/acp-15-1-2015, https://doi.org/10.5194/acp-15-1-2015, 2015
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Organic material found in ambient aerosol is mostly formed through the oxidation of gaseous precursors. It is semi-volatile under atmospheric conditions, and it continuously partitions between the gas and particle phases. At the same time, it is also highly water soluble. We show that wet and especially dry deposition of semi-volatile organic compounds in the gas phase are major indirect removal pathways for the particle phase, and hence need to be accurately accounted for in modeling studies.
G. Isaacman, N. M. Kreisberg, L. D. Yee, D. R. Worton, A. W. H. Chan, J. A. Moss, S. V. Hering, and A. H. Goldstein
Atmos. Meas. Tech., 7, 4417–4429, https://doi.org/10.5194/amt-7-4417-2014, https://doi.org/10.5194/amt-7-4417-2014, 2014
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We present here a new in situ instrument for ambient measurements of highly polar organic semi-volatile and low-volatility compounds in both the gas and particle phase by gas chromatography. Compounds previously measured only through filter collection and offline analysis can now be measured hourly with, in most cases, less than 20% uncertainty. This instrument provides unprecedented time resolution and the first ever observations of gas-particle partitioning for most of these compounds.
N. M. Kreisberg, D. R. Worton, Y. Zhao, G. Isaacman, A. H. Goldstein, and S. V. Hering
Atmos. Meas. Tech., 7, 4431–4444, https://doi.org/10.5194/amt-7-4431-2014, https://doi.org/10.5194/amt-7-4431-2014, 2014
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
Short summary
Short summary
The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
Short summary
Short summary
Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
T. K. V. Nguyen, M. D. Petters, S. R. Suda, H. Guo, R. J. Weber, and A. G. Carlton
Atmos. Chem. Phys., 14, 10911–10930, https://doi.org/10.5194/acp-14-10911-2014, https://doi.org/10.5194/acp-14-10911-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
R. Morales Betancourt and A. Nenes
Geosci. Model Dev., 7, 2345–2357, https://doi.org/10.5194/gmd-7-2345-2014, https://doi.org/10.5194/gmd-7-2345-2014, 2014
P. K. Misztal, T. Karl, R. Weber, H. H. Jonsson, A. B. Guenther, and A. H. Goldstein
Atmos. Chem. Phys., 14, 10631–10647, https://doi.org/10.5194/acp-14-10631-2014, https://doi.org/10.5194/acp-14-10631-2014, 2014
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
T. R. Dallmann, T. B. Onasch, T. W. Kirchstetter, D. R. Worton, E. C. Fortner, S. C. Herndon, E. C. Wood, J. P. Franklin, D. R. Worsnop, A. H. Goldstein, and R. A. Harley
Atmos. Chem. Phys., 14, 7585–7599, https://doi.org/10.5194/acp-14-7585-2014, https://doi.org/10.5194/acp-14-7585-2014, 2014
B. Gantt, J. He, X. Zhang, Y. Zhang, and A. Nenes
Atmos. Chem. Phys., 14, 7485–7497, https://doi.org/10.5194/acp-14-7485-2014, https://doi.org/10.5194/acp-14-7485-2014, 2014
S. Saarikoski, S. Carbone, M. J. Cubison, R. Hillamo, P. Keronen, C. Sioutas, D. R. Worsnop, and J. L. Jimenez
Atmos. Meas. Tech., 7, 2121–2135, https://doi.org/10.5194/amt-7-2121-2014, https://doi.org/10.5194/amt-7-2121-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
C. J. Gaston, J. A. Thornton, and N. L. Ng
Atmos. Chem. Phys., 14, 5693–5707, https://doi.org/10.5194/acp-14-5693-2014, https://doi.org/10.5194/acp-14-5693-2014, 2014
D. R. Gentner, E. Ormeño, S. Fares, T. B. Ford, R. Weber, J.-H. Park, J. Brioude, W. M. Angevine, J. F. Karlik, and A. H. Goldstein
Atmos. Chem. Phys., 14, 5393–5413, https://doi.org/10.5194/acp-14-5393-2014, https://doi.org/10.5194/acp-14-5393-2014, 2014
G. Drozd, J. Woo, S. A. K. Häkkinen, A. Nenes, and V. F. McNeill
Atmos. Chem. Phys., 14, 5205–5215, https://doi.org/10.5194/acp-14-5205-2014, https://doi.org/10.5194/acp-14-5205-2014, 2014
S. G. Howell, A. D. Clarke, S. Freitag, C. S. McNaughton, V. Kapustin, V. Brekovskikh, J.-L. Jimenez, and M. J. Cubison
Atmos. Chem. Phys., 14, 5073–5087, https://doi.org/10.5194/acp-14-5073-2014, https://doi.org/10.5194/acp-14-5073-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384, https://doi.org/10.5194/amt-7-1377-2014, https://doi.org/10.5194/amt-7-1377-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
R. Morales Betancourt and A. Nenes
Atmos. Chem. Phys., 14, 4809–4826, https://doi.org/10.5194/acp-14-4809-2014, https://doi.org/10.5194/acp-14-4809-2014, 2014
K. Kristensen, T. Cui, H. Zhang, A. Gold, M. Glasius, and J. D. Surratt
Atmos. Chem. Phys., 14, 4201–4218, https://doi.org/10.5194/acp-14-4201-2014, https://doi.org/10.5194/acp-14-4201-2014, 2014
S. E. Pusede, D. R. Gentner, P. J. Wooldridge, E. C. Browne, A. W. Rollins, K.-E. Min, A. R. Russell, J. Thomas, L. Zhang, W. H. Brune, S. B. Henry, J. P. DiGangi, F. N. Keutsch, S. A. Harrold, J. A. Thornton, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, J. Sanders, X. Ren, T. C. VandenBoer, M. Z. Markovic, A. Guha, R. Weber, A. H. Goldstein, and R. C. Cohen
Atmos. Chem. Phys., 14, 3373–3395, https://doi.org/10.5194/acp-14-3373-2014, https://doi.org/10.5194/acp-14-3373-2014, 2014
E. J. T. Levin, A. J. Prenni, B. B. Palm, D. A. Day, P. Campuzano-Jost, P. M. Winkler, S. M. Kreidenweis, P. J. DeMott, J. L. Jimenez, and J. N. Smith
Atmos. Chem. Phys., 14, 2657–2667, https://doi.org/10.5194/acp-14-2657-2014, https://doi.org/10.5194/acp-14-2657-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 2014
K. Skyllakou, B. N. Murphy, A. G. Megaritis, C. Fountoukis, and S. N. Pandis
Atmos. Chem. Phys., 14, 2343–2352, https://doi.org/10.5194/acp-14-2343-2014, https://doi.org/10.5194/acp-14-2343-2014, 2014
P. Tiitta, V. Vakkari, P. Croteau, J. P. Beukes, P. G. van Zyl, M. Josipovic, A. D. Venter, K. Jaars, J. J. Pienaar, N. L. Ng, M. R. Canagaratna, J. T. Jayne, V.-M. Kerminen, H. Kokkola, M. Kulmala, A. Laaksonen, D. R. Worsnop, and L. Laakso
Atmos. Chem. Phys., 14, 1909–1927, https://doi.org/10.5194/acp-14-1909-2014, https://doi.org/10.5194/acp-14-1909-2014, 2014
B. H. Henderson, F. Akhtar, H. O. T. Pye, S. L. Napelenok, and W. T. Hutzell
Geosci. Model Dev., 7, 339–360, https://doi.org/10.5194/gmd-7-339-2014, https://doi.org/10.5194/gmd-7-339-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
J.-H. Park, S. Fares, R. Weber, and A. H. Goldstein
Atmos. Chem. Phys., 14, 231–244, https://doi.org/10.5194/acp-14-231-2014, https://doi.org/10.5194/acp-14-231-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
K. C. Barsanti, A. G. Carlton, and S. H. Chung
Atmos. Chem. Phys., 13, 12073–12088, https://doi.org/10.5194/acp-13-12073-2013, https://doi.org/10.5194/acp-13-12073-2013, 2013
A. M. Ortega, D. A. Day, M. J. Cubison, W. H. Brune, D. Bon, J. A. de Gouw, and J. L. Jimenez
Atmos. Chem. Phys., 13, 11551–11571, https://doi.org/10.5194/acp-13-11551-2013, https://doi.org/10.5194/acp-13-11551-2013, 2013
L. D. Yee, J. S. Craven, C. L. Loza, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 11121–11140, https://doi.org/10.5194/acp-13-11121-2013, https://doi.org/10.5194/acp-13-11121-2013, 2013
N. Unger, K. Harper, Y. Zheng, N. Y. Kiang, I. Aleinov, A. Arneth, G. Schurgers, C. Amelynck, A. Goldstein, A. Guenther, B. Heinesch, C. N. Hewitt, T. Karl, Q. Laffineur, B. Langford, K. A. McKinney, P. Misztal, M. Potosnak, J. Rinne, S. Pressley, N. Schoon, and D. Serça
Atmos. Chem. Phys., 13, 10243–10269, https://doi.org/10.5194/acp-13-10243-2013, https://doi.org/10.5194/acp-13-10243-2013, 2013
A. G. Carlton and B. J. Turpin
Atmos. Chem. Phys., 13, 10203–10214, https://doi.org/10.5194/acp-13-10203-2013, https://doi.org/10.5194/acp-13-10203-2013, 2013
R. Holzinger, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, and J. Timkovsky
Atmos. Chem. Phys., 13, 10125–10141, https://doi.org/10.5194/acp-13-10125-2013, https://doi.org/10.5194/acp-13-10125-2013, 2013
N. J. Warwick, A. T. Archibald, K. Ashworth, J. Dorsey, P. M. Edwards, D. E. Heard, B. Langford, J. Lee, P. K. Misztal, L. K. Whalley, and J. A. Pyle
Atmos. Chem. Phys., 13, 9183–9194, https://doi.org/10.5194/acp-13-9183-2013, https://doi.org/10.5194/acp-13-9183-2013, 2013
M. Dall'Osto, X. Querol, A. Alastuey, M. C. Minguillon, M. Alier, F. Amato, M. Brines, M. Cusack, J. O. Grimalt, A. Karanasiou, T. Moreno, M. Pandolfi, J. Pey, C. Reche, A. Ripoll, R. Tauler, B. L. Van Drooge, M. Viana, R. M. Harrison, J. Gietl, D. Beddows, W. Bloss, C. O'Dowd, D. Ceburnis, G. Martucci, N. L. Ng, D. Worsnop, J. Wenger, E. Mc Gillicuddy, J. Sodeau, R. Healy, F. Lucarelli, S. Nava, J. L. Jimenez, F. Gomez Moreno, B. Artinano, A. S. H. Prévôt, L. Pfaffenberger, S. Frey, F. Wilsenack, D. Casabona, P. Jiménez-Guerrero, D. Gross, and N. Cots
Atmos. Chem. Phys., 13, 8991–9019, https://doi.org/10.5194/acp-13-8991-2013, https://doi.org/10.5194/acp-13-8991-2013, 2013
M. Trail, A. P. Tsimpidi, P. Liu, K. Tsigaridis, Y. Hu, A. Nenes, and A. G. Russell
Geosci. Model Dev., 6, 1429–1445, https://doi.org/10.5194/gmd-6-1429-2013, https://doi.org/10.5194/gmd-6-1429-2013, 2013
Y. J. Li, B. Y. L. Lee, J. Z. Yu, N. L. Ng, and C. K. Chan
Atmos. Chem. Phys., 13, 8739–8753, https://doi.org/10.5194/acp-13-8739-2013, https://doi.org/10.5194/acp-13-8739-2013, 2013
J. L. Fry, D. C. Draper, K. J. Zarzana, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, S. S. Brown, R. C. Cohen, L. Kaser, A. Hansel, L. Cappellin, T. Karl, A. Hodzic Roux, A. Turnipseed, C. Cantrell, B. L. Lefer, and N. Grossberg
Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, https://doi.org/10.5194/acp-13-8585-2013, 2013
Y.-H. Lin, E. M. Knipping, E. S. Edgerton, S. L. Shaw, and J. D. Surratt
Atmos. Chem. Phys., 13, 8457–8470, https://doi.org/10.5194/acp-13-8457-2013, https://doi.org/10.5194/acp-13-8457-2013, 2013
Y. Cheng, G. Engling, K.-B. He, F.-K. Duan, Y.-L. Ma, Z.-Y. Du, J.-M. Liu, M. Zheng, and R. J. Weber
Atmos. Chem. Phys., 13, 7765–7781, https://doi.org/10.5194/acp-13-7765-2013, https://doi.org/10.5194/acp-13-7765-2013, 2013
L. E. King and R. J. Weber
Atmos. Meas. Tech., 6, 1647–1658, https://doi.org/10.5194/amt-6-1647-2013, https://doi.org/10.5194/amt-6-1647-2013, 2013
K. W. Appel, G. A. Pouliot, H. Simon, G. Sarwar, H. O. T. Pye, S. L. Napelenok, F. Akhtar, and S. J. Roselle
Geosci. Model Dev., 6, 883–899, https://doi.org/10.5194/gmd-6-883-2013, https://doi.org/10.5194/gmd-6-883-2013, 2013
J. A. Huffman, A. J. Prenni, P. J. DeMott, C. Pöhlker, R. H. Mason, N. H. Robinson, J. Fröhlich-Nowoisky, Y. Tobo, V. R. Després, E. Garcia, D. J. Gochis, E. Harris, I. Müller-Germann, C. Ruzene, B. Schmer, B. Sinha, D. A. Day, M. O. Andreae, J. L. Jimenez, M. Gallagher, S. M. Kreidenweis, A. K. Bertram, and U. Pöschl
Atmos. Chem. Phys., 13, 6151–6164, https://doi.org/10.5194/acp-13-6151-2013, https://doi.org/10.5194/acp-13-6151-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
E. C. Browne, K.-E. Min, P. J. Wooldridge, E. Apel, D. R. Blake, W. H. Brune, C. A. Cantrell, M. J. Cubison, G. S. Diskin, J. L. Jimenez, A. J. Weinheimer, P. O. Wennberg, A. Wisthaler, and R. C. Cohen
Atmos. Chem. Phys., 13, 4543–4562, https://doi.org/10.5194/acp-13-4543-2013, https://doi.org/10.5194/acp-13-4543-2013, 2013
R. H. Moore, V. A. Karydis, S. L. Capps, T. L. Lathem, and A. Nenes
Atmos. Chem. Phys., 13, 4235–4251, https://doi.org/10.5194/acp-13-4235-2013, https://doi.org/10.5194/acp-13-4235-2013, 2013
K. Kristensen, K. L. Enggrob, S. M. King, D. R. Worton, S. M. Platt, R. Mortensen, T. Rosenoern, J. D. Surratt, M. Bilde, A. H. Goldstein, and M. Glasius
Atmos. Chem. Phys., 13, 3763–3776, https://doi.org/10.5194/acp-13-3763-2013, https://doi.org/10.5194/acp-13-3763-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297, https://doi.org/10.5194/acp-13-2283-2013, https://doi.org/10.5194/acp-13-2283-2013, 2013
C. He, J. Liu, A. G. Carlton, S. Fan, L. W. Horowitz, H. Levy II, and S. Tao
Atmos. Chem. Phys., 13, 1913–1926, https://doi.org/10.5194/acp-13-1913-2013, https://doi.org/10.5194/acp-13-1913-2013, 2013
J.-H. Park, A. H. Goldstein, J. Timkovsky, S. Fares, R. Weber, J. Karlik, and R. Holzinger
Atmos. Chem. Phys., 13, 1439–1456, https://doi.org/10.5194/acp-13-1439-2013, https://doi.org/10.5194/acp-13-1439-2013, 2013
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
J. S. Craven, L. D. Yee, N. L. Ng, M. R. Canagaratna, C. L. Loza, K. A. Schilling, R. L. N. Yatavelli, J. A. Thornton, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 12, 11795–11817, https://doi.org/10.5194/acp-12-11795-2012, https://doi.org/10.5194/acp-12-11795-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Enhanced atmospheric oxidation and particle reductions driving changes to nitrate formation mechanisms across coastal and inland regions of north China
Atmospheric fate of organosulfates through gas-phase and aqueous-phase reactions with hydroxyl radicals: implications for inorganic sulfate formation
Opinion: The role of AerChemMIP in advancing climate and air quality research
Uncertainties in the effects of organic aerosol coatings on polycyclic aromatic hydrocarbon concentrations and their estimated health effects
Source-explicit estimation of brown carbon in the polluted atmosphere over the North China Plain: implications for distribution, absorption, and the direct radiative effect
Implications of reduced-complexity aerosol thermodynamics on organic aerosol mass concentration and composition over North America
Global modeling of brown carbon: impact of temperature- and humidity-dependent bleaching
Trends and drivers of soluble iron deposition from East Asian dust to the Northwest Pacific: a springtime analysis (2001–2017)
Modelling of atmospheric variability in gas and aerosols during the ACROSS campaign 2022 of the greater Paris area: evaluation of the meteorology, dynamics and chemistry
Spatial–temporal patterns in anthropogenic and biomass burning emission contributions to air pollution and mortality burden changes in India from 1995 to 2014
A comprehensive global modeling assessment of nitrate heterogeneous formation on desert dust
AERO-MAP: a data compilation and modeling approach to understand spatial variability in fine- and coarse-mode aerosol composition
Long-term trends in aerosol properties derived from AERONET measurements
Acid-catalyzed hydrolysis kinetics of organic hydroperoxides: Computational strategy and structure-activity relationship
Impacts of sea ice leads on sea salt aerosols and atmospheric chemistry in the Arctic
Dimethyl sulfide chemistry over the industrial era: comparison of key oxidation mechanisms and long-term observations
Driving factors of aerosol acidity: a new hierarchical quantitative analysis framework and its application in Changzhou, China
Understanding the long-term trend of organic aerosol and the influences from anthropogenic emission and regional climate change in China
Competing multiple oxidation pathways shape atmospheric limonene-derived organonitrates simulated with updated explicit chemical mechanisms
Population exposure to outdoor NO2, black carbon, and ultrafine and fine particles over Paris with multi-scale modelling down to the street scale
Predicted impacts of heterogeneous chemical pathways on particulate sulfur over Fairbanks (Alaska), the Northern Hemisphere, and the Contiguous United States
Critical load exceedances for North America and Europe using an ensemble of models and an investigation of causes of environmental impact estimate variability: an AQMEII4 study
The influence of ammonia emissions on the size-resolved global atmospheric aerosol composition and acidity
Toxic Dust Emission from Drought-Exposed Lakebeds – A New Air Pollution Threat from Dried Lakes
Observationally Constrained Analysis on the Distribution of Fine and Coarse Mode Nitrate in Global Climate Models
Dust pollution substantially weakens the impact of ammonia emission reduction on particulate nitrate formation
Impacts of meteorology and emission reductions on haze pollution during the lockdown in the North China Plain
Impact of mineral dust on the global nitrate aerosol direct and indirect radiative effect
Aerosol impacts on regional climate: chaotic or physical effect?
The surface tension and cloud condensation nuclei (CCN) activation of sea spray aerosol particles
Exploring the processes controlling secondary inorganic aerosol: evaluating the global GEOS-Chem simulation using a suite of aircraft campaigns
Incorporation of multi-phase halogen chemistry into Community Multiscale Air Quality (CMAQ) model
Changes in the impacts of ship emissions on PM2.5 and its components in China under the staged fuel oil policies
Influence of land cover change on atmospheric organic gases, aerosols, and radiative effects
Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions
Quantifying the impact of global nitrate aerosol on tropospheric composition fields and its production from lightning NOx
Aerosol Composition Trends during 2000–2020: In depth insights from model predictions and multiple worldwide observation datasets
Rapid oxidation of phenolic compounds by O3 and HO●: effects of the air–water interface and mineral dust in tropospheric chemical processes
Modeling the contribution of leads to sea spray aerosol in the high Arctic
Importance of aerosol composition and aerosol vertical profiles in global spatial variation in the relationship between PM2.5 and aerosol optical depth
The co-benefits of a low-carbon future for PM2.5 and O3 air pollution in Europe
Assessing the effectiveness of SO2, NOx, and NH3 emission reductions in mitigating winter PM2.5 in Taiwan using CMAQ
Modelling of atmospheric concentrations of fungal spores: a 2-year simulation over France using CHIMERE
Cluster-dynamics-based parameterization for sulfuric acid–dimethylamine nucleation: comparison and selection through box and three-dimensional modeling
Observed and CMIP6-model-simulated organic aerosol response to drought in the contiguous United States during summertime
Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation
Source-resolved atmospheric metal emissions, concentrations, and deposition fluxes into the East Asian seas
Analysis of secondary inorganic aerosols over the greater Athens area using the EPISODE–CityChem source dispersion and photochemistry model
Global estimates of ambient reactive nitrogen components during 2000–2100 based on the multi-stage model
The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China
Zhenze Liu, Jianhua Qi, Yuanzhe Ni, Likun Xue, and Xiaohuan Liu
Atmos. Chem. Phys., 25, 8719–8742, https://doi.org/10.5194/acp-25-8719-2025, https://doi.org/10.5194/acp-25-8719-2025, 2025
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Our research investigated nitrate formation in air pollution across inland and coastal cities in northern China during the winters of 2013 and 2018. Using air quality models and isotopic analysis, we identified regional differences, with coastal cities showing more contribution from the dinitrogen pentoxide (N2O5) heterogeneous reaction. Reducing nitrogen oxides (NOx), volatile organic compounds (VOCs), and ammonia (NH3) was crucial for lowering nitrate levels and improving air quality.
Narcisse Tsona Tchinda, Xiaofan Lv, Stanley Numbonui Tasheh, Julius Numbonui Ghogomu, and Lin Du
Atmos. Chem. Phys., 25, 8575–8590, https://doi.org/10.5194/acp-25-8575-2025, https://doi.org/10.5194/acp-25-8575-2025, 2025
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This study examines the transformation of organosulfates through reaction with HO• radicals. The results show that the nature of substituents on the carbon chain can effectively affect the decomposition rate of organosulfates, and ozone is unveiled as a complementary oxidant in the intermediate steps of this decomposition. The primary products from these reactions include carbonyl compounds and inorganic sulfate, which highlights the role of organosulfates in altering aerosol chemical composition.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael Prather, Alex Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Bjørn H. Samset, Chris Smith, Steven Turnock, Duncan Watson-Parris, and Paul J. Young
Atmos. Chem. Phys., 25, 8289–8328, https://doi.org/10.5194/acp-25-8289-2025, https://doi.org/10.5194/acp-25-8289-2025, 2025
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The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. We review its contribution to AR6 (Sixth Assessment Report of the Intergovernmental Panel on Climate Change) and the wider understanding of the role of these species in climate and climate change. We identify challenges and provide recommendations to improve the utility and uptake of climate model data, detailed summary tables of CMIP6 models, experiments, and emergent diagnostics.
Sijia Lou, Manish Shrivastava, Alexandre Albinet, Sophie Tomaz, Deepchandra Srivastava, Olivier Favez, Huizhong Shen, and Aijun Ding
Atmos. Chem. Phys., 25, 8163–8183, https://doi.org/10.5194/acp-25-8163-2025, https://doi.org/10.5194/acp-25-8163-2025, 2025
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Polycyclic aromatic hydrocarbons (PAHs), emitted from incomplete combustion, pose serious health risks due to their carcinogenic properties. This research demonstrates that viscous organic aerosol coatings significantly hinder PAH oxidation, with spatial distributions sensitive to the degradation modeling approach. Our findings emphasize the need for accurate modeling of PAH oxidation processes in risk assessments, considering both fresh and oxidized PAHs in evaluating human health risks.
Jiamao Zhou, Jiarui Wu, Xiaoli Su, Ruonan Wang, Imad EI Haddad, Xia Li, Qian Jiang, Ting Zhang, Wenting Dai, Junji Cao, Andre S. H. Prevot, Xuexi Tie, and Guohui Li
Atmos. Chem. Phys., 25, 7563–7580, https://doi.org/10.5194/acp-25-7563-2025, https://doi.org/10.5194/acp-25-7563-2025, 2025
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Brown carbon (BrC) is a type of airborne particle produced from various combustion sources which is light absorption. Historically, climate models have categorizing organic particles as either non-absorbing or purely reflective. Our study shows that BrC can reduce the usual cooling effect of organic particles. While BrC is often linked to biomass burning, however, BrC from fossil fuels contributes significantly to atmospheric heating.
Camilo Serrano Damha, Kyle Gorkowski, and Andreas Zuend
Atmos. Chem. Phys., 25, 5773–5792, https://doi.org/10.5194/acp-25-5773-2025, https://doi.org/10.5194/acp-25-5773-2025, 2025
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We implemented the BAT-VBS (Binary Activity Thermodynamics volatility basis set) aerosol thermodynamics model in the GEOS-Chem chemical transport model to efficiently account for organic aerosol water uptake, nonideal mixing, and impacts on the gas–particle partitioning of semi-volatile organics. Compared to GEOS-Chem's complex (dry) scheme, we show that the BAT-VBS model can predict substantial enhancements in organic aerosol mass concentration at moderate-to-high relative humidity.
Xinchun Xie, Yuzhong Zhang, Ruosi Liang, and Xuan Wang
EGUsphere, https://doi.org/10.5194/egusphere-2025-2305, https://doi.org/10.5194/egusphere-2025-2305, 2025
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Brown carbon (BrC), mainly from biomass burning, absorbs short wavelength sunlight and affects climate and atmospheric chemistry. This study implemented an improved parameterization of BrC bleaching in a model with which BrC can survive much longer in cold, dry air, especially when lofted into the upper atmosphere by wildfires. The results reveal stronger warming effects and impacts on atmospheric oxidation, highlighting the need to consider BrC in climate and pollution control strategies.
Hanzheng Zhu, Yaman Liu, Man Yue, Shihui Feng, Pingqing Fu, Kan Huang, Xinyi Dong, and Minghuai Wang
Atmos. Chem. Phys., 25, 5175–5197, https://doi.org/10.5194/acp-25-5175-2025, https://doi.org/10.5194/acp-25-5175-2025, 2025
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Dust-soluble iron deposition from East Asia plays an important role in the marine ecology of the Northwest Pacific. Using the developed model, our findings highlight a dual trend: a decrease in the overall deposition of soluble iron from dust but an increase in the solubility of the iron itself due to the enhanced atmospheric processing. The study underscores the critical roles of both dust emission and atmospheric processing in soluble iron deposition and marine ecology.
Ludovico Di Antonio, Matthias Beekmann, Guillaume Siour, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Joel F. de Brito, Paola Formenti, Cecile Gaimoz, Olivier Garret, Aline Gratien, Valérie Gros, Martial Haeffelin, Lelia N. Hawkins, Simone Kotthaus, Gael Noyalet, Diana L. Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
Atmos. Chem. Phys., 25, 4803–4831, https://doi.org/10.5194/acp-25-4803-2025, https://doi.org/10.5194/acp-25-4803-2025, 2025
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The summer of 2022 has been considered a proxy for future climate scenarios due to its hot and dry conditions. In this paper, we use the measurements from the Atmospheric Chemistry of the Suburban Forest (ACROSS) campaign, conducted in the Paris area in June–July 2022, along with observations from existing networks, to evaluate a 3D chemistry transport model (WRF–CHIMERE) simulation. Results are shown to be satisfactory, allowing us to explain the gas and aerosol variability at the campaign sites.
Bin Luo, Yuqiang Zhang, Tao Tang, Hongliang Zhang, Jianlin Hu, Jiangshan Mu, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 25, 4767–4783, https://doi.org/10.5194/acp-25-4767-2025, https://doi.org/10.5194/acp-25-4767-2025, 2025
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India is facing a severe air pollution crisis that poses significant health risks, particularly from PM2.5 and O3. Our study reveals rising levels of both pollutants from 1995 to 2014, leading to increased premature mortality. While anthropogenic emissions play a significant role, biomass burning also impacts air quality, in particular seasons and regions in India. This study underscores the urgent need for localized policies to protect public health amid escalating environmental challenges.
Rubén Soussé Villa, Oriol Jorba, María Gonçalves Ageitos, Dene Bowdalo, Marc Guevara, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 25, 4719–4753, https://doi.org/10.5194/acp-25-4719-2025, https://doi.org/10.5194/acp-25-4719-2025, 2025
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Desert dust forms nitrate coatings as it travels through the atmosphere. However, current models that predict this process vary greatly due to different methods and inaccuracies. We examined how nitrate forms in a global model, focusing on how gases condense on dust, the lifespan of different particles, and the impact of alkalinity. Our findings show that models work best when they consider reversible gas condensation with alkalinity. This should lead to better estimates of climate impacts.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, P. 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, 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-Gómez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal L. Weagle, and Xi Zhao
Atmos. Chem. Phys., 25, 4665–4702, https://doi.org/10.5194/acp-25-4665-2025, https://doi.org/10.5194/acp-25-4665-2025, 2025
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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 being 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 data sets to model output.
Zhenyu Zhang, Jing Li, Huizheng Che, Yueming Dong, Oleg Dubovik, Thomas Eck, Pawan Gupta, Brent Holben, Jhoon Kim, Elena Lind, Trailokya Saud, Sachchida Nand Tripathi, and Tong Ying
Atmos. Chem. Phys., 25, 4617–4637, https://doi.org/10.5194/acp-25-4617-2025, https://doi.org/10.5194/acp-25-4617-2025, 2025
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We used ground-based remote sensing data from the Aerosol Robotic Network to examine long-term trends in aerosol characteristics. We found aerosol loadings generally decreased globally, and aerosols became more scattering. These changes are closely related to variations in aerosol compositions, such as decreased anthropogenic emissions over East Asia, Europe, and North America; increased anthropogenic sources over northern India; and increased dust activity over the Arabian Peninsula.
Qiaojing Zhao, Fangfang Ma, Hui Zhao, Qian Xu, Rujing Yin, Hong-Bin Xie, Xin Wang, and Jingwen Chen
EGUsphere, https://doi.org/10.5194/egusphere-2025-1662, https://doi.org/10.5194/egusphere-2025-1662, 2025
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The scarcity of kinetic data for key aerosol aqueous-phase reactions contributes to large uncertainties in atmospheric models. We establish a computational strategy to rapidly predict acid-catalyzed hydrolysis kinetics of organic hydroperoxides, an aerosol constituent with high abundance. The kinetic parameters can be integrated into atmospheric models to improve simulations of the global hydrogen peroxide budget and secondary organic aerosol production.
Erin J. Emme and Hannah M. Horowitz
Atmos. Chem. Phys., 25, 4531–4545, https://doi.org/10.5194/acp-25-4531-2025, https://doi.org/10.5194/acp-25-4531-2025, 2025
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There is uncertainty in the sources of Arctic cold-season (November–April) sea salt aerosols. Using a chemical transport model and satellite observations, we quantify Arctic-wide sea salt aerosol emissions from fractures in sea ice, called open sea ice leads, and their atmospheric chemistry impacts for the cold season. We show that sea ice leads contribute to Arctic sea salt aerosols and bromine, especially in under-observed regions.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winski, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
Atmos. Chem. Phys., 25, 4083–4106, https://doi.org/10.5194/acp-25-4083-2025, https://doi.org/10.5194/acp-25-4083-2025, 2025
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a model to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Xiaolin Duan, Guangjie Zheng, Chuchu Chen, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 25, 3919–3928, https://doi.org/10.5194/acp-25-3919-2025, https://doi.org/10.5194/acp-25-3919-2025, 2025
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Aerosol acidity is an important parameter in atmospheric chemistry, while its driving factors, especially chemical profiles versus meteorological conditions, are not yet fully understood. Here, we established a hierarchical quantitative analysis framework to understand the driving factors of aerosol acidity on different timescales. Its application in Changzhou, China, revealed distinct driving factors and corresponding mechanisms of aerosol acidity from annual trends to random residuals.
Wenxin Zhang, Yaman Liu, Man Yue, Xinyi Dong, Kan Huang, and Minghuai Wang
Atmos. Chem. Phys., 25, 3857–3872, https://doi.org/10.5194/acp-25-3857-2025, https://doi.org/10.5194/acp-25-3857-2025, 2025
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Understanding long-term organic aerosol (OA) trends and their driving factors is important for air quality management. Our modeling revealed that OA in China increased by 5.6 % from 1990 to 2019, primarily due to a 32.3 % increase in secondary organic aerosols (SOAs) and an 8.1 % decrease in primary organic aerosols (POAs), both largely driven by changes in anthropogenic emissions. Biogenic SOA increased due to warming but showed little response to changes in anthropogenic nitrogen oxide emissions.
Qinghao Guo, Haofei Zhang, Bo Long, Lehui Cui, Yiyang Sun, Hao Liu, Yaxin Liu, Yunting Xiao, Pingqing Fu, and Jialei Zhu
EGUsphere, https://doi.org/10.5194/egusphere-2025-1058, https://doi.org/10.5194/egusphere-2025-1058, 2025
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Limonene, a natural compound from plants, reacts with pollutants to form airborne particles that influence air quality and climate. Using advanced models with explicit chemical mechanisms, we show how different reaction pathways shape organonitrate formation, with some increasing and others decreasing particle levels. This approach enhancing predictions of pollution and climate impacts while deepening our understanding of how natural and human-made emissions interact in the atmosphere.
Soo-Jin Park, Lya Lugon, Oscar Jacquot, Youngseob Kim, Alexia Baudic, Barbara D'Anna, Ludovico Di Antonio, Claudia Di Biagio, Fabrice Dugay, Olivier Favez, Véronique Ghersi, Aline Gratien, Julien Kammer, Jean-Eudes Petit, Olivier Sanchez, Myrto Valari, Jérémy Vigneron, and Karine Sartelet
Atmos. Chem. Phys., 25, 3363–3387, https://doi.org/10.5194/acp-25-3363-2025, https://doi.org/10.5194/acp-25-3363-2025, 2025
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To accurately represent the population exposure to outdoor concentrations of pollutants of interest to health (NO2, PM2.5, black carbon, and ultrafine particles), multi-scale modelling down to the street scale is set up and evaluated using measurements from field campaigns. An exposure scaling factor is defined, allowing regional-scale simulations to be corrected to evaluate population exposure. Urban heterogeneities strongly influence NO2, black carbon, and ultrafine particles but less strongly PM2.5.
Sara L. Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, and Kathleen Fahey
Atmos. Chem. Phys., 25, 3287–3312, https://doi.org/10.5194/acp-25-3287-2025, https://doi.org/10.5194/acp-25-3287-2025, 2025
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters is improved.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark W. Shephard, Ranjeet S. Sokhi, and Stefano Galmarini
Atmos. Chem. Phys., 25, 3049–3107, https://doi.org/10.5194/acp-25-3049-2025, https://doi.org/10.5194/acp-25-3049-2025, 2025
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The large range of sulfur and nitrogen deposition estimates from air quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulfur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by hydrometeors, aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, gas deposition via plant cuticles and soil, and land use data.
Xurong Wang, Alexandra P. Tsimpidi, Zhenqi Luo, Benedikt Steil, Andrea Pozzer, Jos Lelieveld, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2025-527, https://doi.org/10.5194/egusphere-2025-527, 2025
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Ammonia (NH3) is an abundant alkaline gas and key precursor in particulate matter formation. While SO2 and NOx emissions have decreased, global NH3 emissions are stable or rising. This study investigates NH3 emission impacts on size-resolved aerosol composition and acidity using the EMAC model, analyzing three emission schemes. Sulphate-nitrate-ammonium aerosols in fine mode sizes are most sensitive to NH3 changes. Regional responses vary. NH3 buffers aerosol acidity, mitigating pH shifts.
Qianqian Gao, Guochao Chen, Xiaohui Lu, Jianmin Chen, Hongliang Zhang, and Xiaofei Wang
EGUsphere, https://doi.org/10.5194/egusphere-2025-596, https://doi.org/10.5194/egusphere-2025-596, 2025
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Numerous lakes are shrinking due to climate change and human activities, releasing pollutants from dried lakebeds as dust aerosols. The health risks remain unclear. Recently, Poyang and Dongting Lakes faced record droughts, exposing 99 % and 88 % of their areas. We show lakebed dust can raise PM10 to 637.5 μg/m³ and exceed non-carcinogenic (HQ=4.13) and Cr carcinogenic (~2.10×10⁻⁶) risk thresholds, posing growing health threats.
Mingxuan Wu, Hailong Wang, Zheng Lu, Xiaohong Liu, Huisheng Bian, David Cohen, Yan Feng, Mian Chin, Didier A. Hauglustaine, Vlassis A. Karydis, Marianne T. Lund, Gunnar Myhre, Andrea Pozzer, Michael Schulz, Ragnhild B. Skeie, Alexandra P. Tsimpidi, Svetlana G. Tsyro, and Shaocheng Xie
EGUsphere, https://doi.org/10.5194/egusphere-2025-235, https://doi.org/10.5194/egusphere-2025-235, 2025
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A key challenge in simulating the lifecycle of nitrate aerosol in global climate models is to accurately represent mass size distribution of nitrate aerosol, which lacks sufficient observational constraints. We found that most climate models underestimate the mass fraction of fine-mode nitrate at surface in all regions. Our study highlights the importance of gas-aerosol partitioning parameterization and simulation of dust and sea salt in correctly simulating mass size distribution of nitrate.
Hanrui Lang, Yunjiang Zhang, Sheng Zhong, Yongcai Rao, Minfeng Zhou, Jian Qiu, Jingyi Li, Diwen Liu, Florian Couvidat, Olivier Favez, Didier Hauglustaine, and Xinlei Ge
EGUsphere, https://doi.org/10.5194/egusphere-2025-231, https://doi.org/10.5194/egusphere-2025-231, 2025
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This study investigates how dust pollution influences particulate nitrate formation. We found that dust pollution could reduce the effectiveness of ammonia emission controls by altering aerosol chemistry. Using field observations and modeling, we showed that dust particles affect nitrate distribution between gas and particle phases. Our findings highlight the need for pollution control strategies that consider both human emissions and dust sources for better urban air quality management.
Lang Liu, Xin Long, Yi Li, Zengliang Zang, Fengwen Wang, Yan Han, Zhier Bao, Yang Chen, Tian Feng, and Jinxin Yang
Atmos. Chem. Phys., 25, 1569–1585, https://doi.org/10.5194/acp-25-1569-2025, https://doi.org/10.5194/acp-25-1569-2025, 2025
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This study uses WRF-Chem to assess how meteorological conditions and emission reductions affected fine particulate matter (PM2.5) in the North China Plain (NCP). It highlights regional disparities: in the northern NCP, adverse weather negated emission reduction effects. In contrast, the southern NCP featured a PM2.5 decrease due to favorable weather and emission reductions. The research highlighted the interaction between emissions, meteorology, and PM2.5.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol–radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are −0.11 and +0.17 W m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
Jiawang Feng, Chun Zhao, Jun Gu, Gudongze Li, Mingyue Xu, Shengfu Lin, and Jie Feng
EGUsphere, https://doi.org/10.5194/egusphere-2024-4037, https://doi.org/10.5194/egusphere-2024-4037, 2025
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Climate models help study aerosol impacts on regional climate. However, the atmosphere's chaotic nature makes it hard to separate true aerosol impacts from chaotic effects. Our ensemble experiments show that while large-scale aerosol effects are consistent, regional aerosol impacts vary significantly among experiments. We give a formula showing the relationship between chaotic effects and ensemble sizes, emphasizing the necessity of adequate ensemble members to capture reliable aerosol impacts.
Judith Kleinheins, Nadia Shardt, Ulrike Lohmann, and Claudia Marcolli
Atmos. Chem. Phys., 25, 881–903, https://doi.org/10.5194/acp-25-881-2025, https://doi.org/10.5194/acp-25-881-2025, 2025
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We model the cloud condensation nuclei (CCN) activation of sea spray aerosol particles with classical Köhler theory and with a new model approach that takes surface tension lowering into account. We categorize organic compounds into weak, intermediate, and strong surfactants, and we outline for which composition surface tension lowering is important. The results suggest that surface tension lowering allows sea spray aerosol particles in the Aitken mode to be a source of CCN in marine updraughts.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, 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
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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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).
Kiyeon Kim, Chul Han Song, Kyung Man Han, Greg Yarwood, Ross Beardsley, and Saewung Kim
EGUsphere, https://doi.org/10.5194/egusphere-2025-23, https://doi.org/10.5194/egusphere-2025-23, 2025
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Despite the crucial role of halogen radicals in the atmosphere, the current CMAQ model does not account for multi-phase halogen processes. To address this issue, we incorporated 177 halogen reactions, together with anthropogenic and natural halogen emissions into the CMAQ model. Our findings reveal that incorporation of these halogen processes significantly improves model performances compared to ground observations. In addition, we emphasize the influence of halogen radicals on air quality.
Guangyuan Yu, Yan Zhang, Qian Wang, Zimin Han, Shenglan Jiang, Fan Yang, Xin Yang, and Cheng Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-3892, https://doi.org/10.5194/egusphere-2024-3892, 2025
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China has carried out staged low-sulfur fuel policies since 2017. This study simulated the changing spatiotemporal patterns of the impacts of ship emissions on PM2.5 from 2017 to 2021 based on the updated emission inventories and mapping of chemical species in the CMAQ. Fuel policies caused evident relative changes in inorganic and organic components of the shipping-related PM2.5 over China’s port cities. The driving factors of the interannual, seasonal, and diurnal patterns were discussed.
Ryan Vella, Matthew Forrest, Andrea Pozzer, Alexandra P. Tsimpidi, Thomas Hickler, Jos Lelieveld, and Holger Tost
Atmos. Chem. Phys., 25, 243–262, https://doi.org/10.5194/acp-25-243-2025, https://doi.org/10.5194/acp-25-243-2025, 2025
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This study examines how land cover changes influence biogenic volatile organic compound (BVOC) emissions and atmospheric states. Using a coupled chemistry–climate–vegetation model, we compare present-day land cover (deforested for crops and grazing) with natural vegetation and an extreme reforestation scenario. We find that vegetation changes significantly impact global BVOC emissions and organic aerosols but have a relatively small effect on total aerosols, clouds, and radiative effects.
Mashiat Hossain, Rebecca M. Garland, and Hannah M. Horowitz
Atmos. Chem. Phys., 24, 14123–14143, https://doi.org/10.5194/acp-24-14123-2024, https://doi.org/10.5194/acp-24-14123-2024, 2024
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Our research examines aerosol dynamics over the southeast Atlantic, a region with significant uncertainties in aerosol radiative forcings. Using the GEOS-Chem model, we find that at cloud altitudes, organic aerosols dominate during the biomass burning season, while sulfate aerosols, driven by marine emissions, prevail during peak primary production. These findings highlight the need for accurate representation of marine aerosols in models to improve climate predictions and reduce uncertainties.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
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Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Alexandra P. Tsimpidi, Susanne M. C. Scholz, Alexandros Milousis, Nikolaos Mihalopoulos, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3590, https://doi.org/10.5194/egusphere-2024-3590, 2024
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This study examines global changes in air pollution from 2000 to 2020, focusing on fine aerosols that impact climate and health. Using models and global data, it finds organic aerosols dominate in many regions, especially with wildfires or natural emissions. Pollution from sulfate and nitrate has decreased in Europe and North America due to regulations, while trends in Asia are more complex. The findings improve understanding and support policies for cleaner air and healthier environments.
Yanru Huo, Mingxue Li, Xueyu Wang, Jianfei Sun, Yuxin Zhou, Yuhui Ma, and Maoxia He
Atmos. Chem. Phys., 24, 12409–12423, https://doi.org/10.5194/acp-24-12409-2024, https://doi.org/10.5194/acp-24-12409-2024, 2024
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This work found that the air–water (A–W) interface and TiO2 clusters promote the oxidation of phenolic compounds (PhCs) to varying degrees compared with the gas phase and bulk water. Some byproducts are more harmful than their parent compounds. This work provides important evidence for the rapid oxidation observed in O3/HO• + PhC experiments at the A–W interface and in mineral dust.
Rémy Lapere, Louis Marelle, Pierre Rampal, Laurent Brodeau, Christian Melsheimer, Gunnar Spreen, and Jennie L. Thomas
Atmos. Chem. Phys., 24, 12107–12132, https://doi.org/10.5194/acp-24-12107-2024, https://doi.org/10.5194/acp-24-12107-2024, 2024
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Elongated open-water areas in sea ice, called leads, can release marine aerosols into the atmosphere. In the Arctic, this source of atmospheric particles could play an important role for climate. However, the amount, seasonality and spatial distribution of such emissions are all mostly unknown. Here, we propose a first parameterization for sea spray aerosols emitted through leads in sea ice and quantify their impact on aerosol populations in the high Arctic.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Connor J. Clayton, Daniel R. Marsh, Steven T. Turnock, Ailish M. Graham, Kirsty J. Pringle, Carly L. Reddington, Rajesh Kumar, and James B. McQuaid
Atmos. Chem. Phys., 24, 10717–10740, https://doi.org/10.5194/acp-24-10717-2024, https://doi.org/10.5194/acp-24-10717-2024, 2024
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We demonstrate that strong climate mitigation could improve air quality in Europe; however, less ambitious mitigation does not result in these co-benefits. We use a high-resolution atmospheric chemistry model. This allows us to demonstrate how this varies across European countries and analyse the underlying chemistry. This may help policy-facing researchers understand which sectors and regions need to be prioritised to achieve strong air quality co-benefits of climate mitigation.
Ping-Chieh Huang, Hui-Ming Hung, Hsin-Chih Lai, and Charles C.-K. Chou
Atmos. Chem. Phys., 24, 10759–10772, https://doi.org/10.5194/acp-24-10759-2024, https://doi.org/10.5194/acp-24-10759-2024, 2024
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Models were used to study ways to reduce particulate matter (PM) pollution in Taiwan during winter. After considering various factors, such as physical processes and chemical reactions, we found that reducing NOx or NH3 emissions is more effective at mitigating PM2.5 than reducing SO2 emissions. When considering both efficiency and cost, reducing NH3 emissions seems to be a more suitable policy for the studied environment in Taiwan.
Matthieu Vida, Gilles Foret, Guillaume Siour, Florian Couvidat, Olivier Favez, Gaelle Uzu, Arineh Cholakian, Sébastien Conil, Matthias Beekmann, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 24, 10601–10615, https://doi.org/10.5194/acp-24-10601-2024, https://doi.org/10.5194/acp-24-10601-2024, 2024
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We simulate 2 years of atmospheric fungal spores over France and use observations of polyols and primary biogenic factors from positive matrix factorisation. The representation of emissions taking into account a proxy for vegetation surface and specific humidity enables us to reproduce very accurately the seasonal cycle of fungal spores. Furthermore, we estimate that fungal spores can account for 20 % of PM10 and 40 % of the organic fraction of PM10 over vegetated areas in summer.
Jiewen Shen, Bin Zhao, Shuxiao Wang, An Ning, Yuyang Li, Runlong Cai, Da Gao, Biwu Chu, Yang Gao, Manish Shrivastava, Jingkun Jiang, Xiuhui Zhang, and Hong He
Atmos. Chem. Phys., 24, 10261–10278, https://doi.org/10.5194/acp-24-10261-2024, https://doi.org/10.5194/acp-24-10261-2024, 2024
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We extensively compare various cluster-dynamics-based parameterizations for sulfuric acid–dimethylamine nucleation and identify a newly developed parameterization derived from Atmospheric Cluster Dynamic Code (ACDC) simulations as being the most reliable one. This study offers a valuable reference for developing parameterizations of other nucleation systems and is meaningful for the accurate quantification of the environmental and climate impacts of new particle formation.
Wei Li and Yuxuan Wang
Atmos. Chem. Phys., 24, 9339–9353, https://doi.org/10.5194/acp-24-9339-2024, https://doi.org/10.5194/acp-24-9339-2024, 2024
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Droughts immensely increased organic aerosol (OA) in the contiguous United States in summer (1998–2019), notably in the Pacific Northwest (PNW) and Southeast (SEUS). The OA rise in the SEUS is driven by the enhanced formation of epoxydiol-derived secondary organic aerosol due to the increase in biogenic volatile organic compounds and sulfate, while in the PNW, it is caused by wildfires. A total of 10 climate models captured the OA increase in the PNW yet greatly underestimated it in the SEUS.
Weina Zhang, Jianhua Mai, Zhichao Fan, Yongpeng Ji, Yuemeng Ji, Guiying Li, Yanpeng Gao, and Taicheng An
Atmos. Chem. Phys., 24, 9019–9030, https://doi.org/10.5194/acp-24-9019-2024, https://doi.org/10.5194/acp-24-9019-2024, 2024
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This study reveals heterogeneous oxidation causes further radiative forcing effect (RFE) enhancement of amine–mineral mixed particles. Note that RFE increment is higher under clean conditions than that under polluted conditions, which is contributed to high-oxygen-content products. The enhanced RFE of amine–mineral particles caused by heterogenous oxidation is expected to alleviate warming effects.
Shenglan Jiang, Yan Zhang, Guangyuan Yu, Zimin Han, Junri Zhao, Tianle Zhang, and Mei Zheng
Atmos. Chem. Phys., 24, 8363–8381, https://doi.org/10.5194/acp-24-8363-2024, https://doi.org/10.5194/acp-24-8363-2024, 2024
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This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals using the modified CMAQ model. We developed a monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from terrestrial anthropogenic, ship, and dust sources in East Asia in 2017. Our results reveal the contribution of each source to the emissions, concentrations, and deposition fluxes of metals in the East Asian seas.
Stelios Myriokefalitakis, Matthias Karl, Kim A. Weiss, Dimitris Karagiannis, Eleni Athanasopoulou, Anastasia Kakouri, Aikaterini Bougiatioti, Eleni Liakakou, Iasonas Stavroulas, Georgios Papangelis, Georgios Grivas, Despina Paraskevopoulou, Orestis Speyer, Nikolaos Mihalopoulos, and Evangelos Gerasopoulos
Atmos. Chem. Phys., 24, 7815–7835, https://doi.org/10.5194/acp-24-7815-2024, https://doi.org/10.5194/acp-24-7815-2024, 2024
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A state-of-the-art thermodynamic model has been coupled with the city-scale chemistry transport model EPISODE–CityChem to investigate the equilibrium between the inorganic gas and aerosol phases over the greater Athens area, Greece. The simulations indicate that the formation of nitrates in an urban environment is significantly affected by local nitrogen oxide emissions, as well as ambient temperature, relative humidity, photochemical activity, and the presence of non-volatile cations.
Rui Li, Yining Gao, Lijia Zhang, Yubing Shen, Tianzhao Xu, Wenwen Sun, and Gehui Wang
Atmos. Chem. Phys., 24, 7623–7636, https://doi.org/10.5194/acp-24-7623-2024, https://doi.org/10.5194/acp-24-7623-2024, 2024
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A three-stage model was developed to obtain the global maps of reactive nitrogen components during 2000–2100. The results implied that cross-validation R2 values of four species showed satisfactory performance (R2 > 0.55). Most reactive nitrogen components, except NH3, in China showed increases during 2000–2013. In the future scenarios, SSP3-7.0 (traditional-energy scenario) and SSP1-2.6 (carbon neutrality scenario) showed the highest and lowest reactive nitrogen component concentrations.
Fei Ye, Jingyi Li, Yaqin Gao, Hongli Wang, Jingyu An, Cheng Huang, Song Guo, Keding Lu, Kangjia Gong, Haowen Zhang, Momei Qin, and Jianlin Hu
Atmos. Chem. Phys., 24, 7467–7479, https://doi.org/10.5194/acp-24-7467-2024, https://doi.org/10.5194/acp-24-7467-2024, 2024
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Naphthalene (Nap) and methylnaphthalene (MN) are key precursors of secondary organic aerosol (SOA), yet their sources and sinks are often inadequately represented in air quality models. In this study, we incorporated detailed emissions, gas-phase chemistry, and SOA parameterization of Nap and MN into CMAQ to address this issue. The findings revealed remarkably high SOA formation potentials for these compounds despite their low emissions in the Yangtze River Delta region during summer.
Cited articles
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Altieri, K. E., Seitzinger, S. P., Carlton, A. G., Turpin, B. J., Klein, G. C., and Marshall, A. G.: Oligomers formed through in-cloud methylglyoxal reactions: Chemical composition, properties, and mechanisms investigated by ultra-high resolution FT-ICR mass spectrometry, Atmos. Environ., 42, 1476–1490, https://doi.org/10.1016/j.atmosenv.2007.11.015, 2008.
Appel, K. W., Napelenok, S. L., Foley, K. M., Pye, H. O. T., Hogrefe, C., Luecken, D. J., Bash, J. O., Roselle, S. J., Pleim, J. E., Foroutan, H., Hutzell, W. T., Pouliot, G. A., Sarwar, G., Fahey, K. M., Gantt, B., Gilliam, R. C., Kang, D., Mathur, R., Schwede, D. B., Spero, T. L., Wong, D. C., and Young, J. O.: Overview and evaluation of the Community Multiscale Air Quality (CMAQ) model version 5.1, Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2016-226, in review, 2016.
Baker, K. R., Carlton, A. G., Kleindienst, T. E., Offenberg, J. H., Beaver, M. R., Gentner, D. R., Goldstein, A. H., Hayes, P. L., Jimenez, J. L., Gilman, J. B., de Gouw, J. A., Woody, M. C., Pye, H. O. T., Kelly, J. T., Lewandowski, M., Jaoui, M., Stevens, P. S., Brune, W. H., Lin, Y. H., Rubitschun, C. L., and Surratt, J. D.: Gas and aerosol carbon in California: comparison of measurements and model predictions in Pasadena and Bakersfield, Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, 2015.
Bash, J. O., Baker, K. R., and Beaver, M. R.: Evaluation of improved land use and canopy representation in BEIS v3.61 with biogenic VOC measurements in California, Geosci. Model Dev., 9, 2191–2207, https://doi.org/10.5194/gmd-9-2191-2016, 2016.
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Boyd, C. M., Sanchez, J., Xu, L., Eugene, A. J., Nah, T., Tuet, W. Y., Guzman, M. I., and Ng, N. L.: Secondary organic aerosol formation from the β-pinene+NO3 system: effect of humidity and peroxy radical fate, Atmos. Chem. Phys., 15, 7497–7522, https://doi.org/10.5194/acp-15-7497-2015, 2015.
Budisulistiorini, S. H., Canagaratna, M. R., Croteau, P. L., Marth, W. J., Baumann, K., Edgerton, E. S., Shaw, S. L., Knipping, E., Worsnop, D. R., Jayne, J. T., Gold, A., and Surratt, J. D.: Real-time continuous characterization of secondary organic aerosol derived from isoprene epoxydiols (IEPOX) in downtown Atlanta, Georgia, using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM), Environ. Sci. Technol., 47, 5686–5694, https://doi.org/10.1021/es400023n, 2013.
Budisulistiorini, S. H., Li, X., Bairai, S. T., Renfro, J., Liu, Y., Liu, Y. J., McKinney, K. A., Martin, S. T., McNeill, V. F., Pye, H. O. T., Nenes, A., Neff, M. E., Stone, E. A., Mueller, S., Knote, C., Shaw, S. L., Zhang, Z., Gold, A., and Surratt, J. D.: Examining the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol formation during the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee ground site, Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, 2015.
Budisulistiorini, S. H., Baumann, K., Edgerton, E. S., Bairai, S. T., Mueller, S., Shaw, S. L., Knipping, E. M., Gold, A., and Surratt, J. D.: Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee, Atmos. Chem. Phys., 16, 5171–5189, https://doi.org/10.5194/acp-16-5171-2016, 2016.
Canagaratna, M. R., Jimenez, J. L., Kroll, J. H., Chen, Q., Kessler, S. H., Massoli, P., Hildebrandt Ruiz, L., Fortner, E., Williams, L. R., Wilson, K. R., Surratt, J. D., Donahue, N. M., Jayne, J. T., and Worsnop, D. R.: Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications, Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, 2015.
Carlton, A. G. and Baker, K. R.: Photochemical modeling of the Ozark isoprene volcano: MEGAN, BEIS, and their impacts on air quality predictions, Environ. Sci. Technol., 45, 4438–4445, https://doi.org/10.1021/es200050x, 2011.
Carlton, A. G. and Turpin, B. J.: Particle partitioning potential of organic compounds is highest in the Eastern US and driven by anthropogenic water, Atmos. Chem. Phys., 13, 10203–10214, https://doi.org/10.5194/acp-13-10203-2013, 2013.
Carlton, A. G., Bhave, P. V., Napelenok, S. L., Edney, E. D., Sarwar, G., Pinder, R. W., Pouliot, G. A., and Houyoux, M.: Model representation of secondary organic aerosol in CMAQv4.7, Environ. Sci. Technol., 44, 8553–8560, https://doi.org/10.1021/es100636q, 2010.
Cerully, K. M., Bougiatioti, A., Hite Jr, J. R., Guo, H., Xu, L., Ng, N. L., Weber, R., and Nenes, A.: On the link between hygroscopicity, volatility, and oxidation state of ambient and water-soluble aerosols in the southeastern United States, Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, 2015.
Chan, A. W. H., Kautzman, K. E., Chhabra, P. S., Surratt, J. D., Chan, M. N., Crounse, J. D., Kurten, A., Wennberg, P. O., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: Implications for oxidation of intermediate volatility organic compounds (IVOCs), Atmos. Chem. Phys., 9, 3049–3060, https://doi.org/10.5194/acp-9-3049-2009, 2009.
Chang, E. I. and Pankow, J. F.: Organic particulate matter formation at varying relative humidity using surrogate secondary and primary organic compounds with activity corrections in the condensed phase obtained using a method based on the Wilson equation, Atmos. Chem. Phys., 10, 5475–5490, https://doi.org/10.5194/acp-10-5475-2010, 2010.
Chen, Q., Heald, C. L., Jimenez, J. L., Canagaratna, M. R., Zhang, Q., He, L.-Y., Huang, X.-F., Campuzano-Jost, P., Palm, B. B., Poulain, L., Kuwata, M., Martin, S. T., Abbatt, J. P. D., Lee, A. K. Y., and Liggio, J.: Elemental composition of organic aerosol: The gap between ambient and laboratory measurements, Geophys. Res. Lett., 42, 4182–4189, https://doi.org/10.1002/2015GL063693, 2015.
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Donahue, N. M., Epstein, S. A., Pandis, S. N., and Robinson, A. L.: A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics, Atmos. Chem. Phys., 11, 3303–3318, https://doi.org/10.5194/acp-11-3303-2011, 2011.
Duplissy, J., DeCarlo, P. F., Dommen, J., Alfarra, M. R., Metzger, A., Barmpadimos, I., Prevot, A. S. H., Weingartner, E., Tritscher, T., Gysel, M., Aiken, A. C., Jimenez, J. L., Canagaratna, M. R., Worsnop, D. R., Collins, D. R., Tomlinson, J., and Baltensperger, U.: Relating hygroscopicity and composition of organic aerosol particulate matter, Atmos. Chem. Phys., 11, 1155–1165, https://doi.org/10.5194/acp-11-1155-2011, 2011.
Eddingsaas, N. C., VanderVelde, D. G., and Wennberg, P. O.: Kinetics and products of the acid-catalyzed ring-opening of atmospherically relevant butyl epoxy alcohols, J. Phys. Chem. A, 114, 8106–8113, https://doi.org/10.1021/jp103907c, 2010.
Edney, E. O., Driscoll, D. J., Speer, R. E., Weathers, W. S., Kleindienst, T. E., Li, W., and Smith, D. F.: Impact of aerosol liquid water on secondary organic aerosol yields of irradiated toluene/propylene/NOx/(NH4)2SO4/air mixtures, Atmos. Environ., 34, 3907–3919, https://doi.org/10.1016/S1352-2310(00)00174-6, 2000.
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Short summary
We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
We use a chemical transport model to examine how organic compounds in the atmosphere interact...
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