Articles | Volume 16, issue 8
https://doi.org/10.5194/acp-16-4897-2016
© Author(s) 2016. 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-16-4897-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
21 Apr 2016
Research article |
| 21 Apr 2016
Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study
Weruka Rattanavaraha
CORRESPONDING AUTHOR
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
Kevin Chu
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
Sri Hapsari Budisulistiorini
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
now at: Earth Observatory of Singapore, Nanyang Technological
University, Singapore
Matthieu Riva
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
Ying-Hsuan Lin
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
now at: Michigan Society of Fellows, Department of Chemistry,
University of Michigan, Ann Arbor, MI, USA
Eric S. Edgerton
Atmospheric Research & Analysis, Inc., Cary, NC, USA
Karsten Baumann
Atmospheric Research & Analysis, Inc., Cary, NC, USA
Stephanie L. Shaw
Electric Power Research Institute, Palo Alto, CA, USA
Hongyu Guo
Earth and Atmospheric Science, Georgia Institute of Technology,
Atlanta, GA, USA
Laura King
Earth and Atmospheric Science, Georgia Institute of Technology,
Atlanta, GA, USA
Rodney J. Weber
Earth and Atmospheric Science, Georgia Institute of Technology,
Atlanta, GA, USA
Miranda E. Neff
Department of Chemistry, University of Iowa, Iowa City, IA, USA
Elizabeth A. Stone
Department of Chemistry, University of Iowa, Iowa City, IA, USA
John H. Offenberg
Human Exposure and Atmospheric Sciences Division, United States
Environmental Protection Agency, Research Triangle Park, NC, USA
Zhenfa Zhang
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
Avram Gold
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
Jason D. Surratt
Department of Environmental Sciences and Engineering, Gillings
School of Global Public Health, The University of North Carolina at Chapel
Hill, Chapel Hill, NC, USA
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EGUsphere, https://doi.org/10.5194/egusphere-2024-1485, https://doi.org/10.5194/egusphere-2024-1485, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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 two different years, we characterize the emissions and evolution up to 8 hours of PM2.5 mass, BC, and BrC in smoke from burning of forested lands in the southeastern US.
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.
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.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
Biogeosciences, 20, 971–995, https://doi.org/10.5194/bg-20-971-2023, https://doi.org/10.5194/bg-20-971-2023, 2023
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Better estimates of atmospheric nitrogen (N) deposition are needed to accurately assess ecosystem risk and impacts from deposition of nutrients and acidity. Using measurements and modeling, we estimate total N deposition of 6.7 kg N ha−1 yr−1 at a forest site in the southern Appalachian Mountains, a region sensitive to atmospheric deposition. Reductions in deposition of reduced forms of N (ammonia and ammonium) will be needed to meet the lowest estimates of N critical loads for the region.
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.
Robert J. Yokelson, Bambang H. Saharjo, Chelsea E. Stockwell, Erianto I. Putra, Thilina Jayarathne, Acep Akbar, Israr Albar, Donald R. Blake, Laura L. B. Graham, Agus Kurniawan, Simone Meinardi, Diah Ningrum, Ati D. Nurhayati, Asmadi Saad, Niken Sakuntaladewi, Eko Setianto, Isobel J. Simpson, Elizabeth A. Stone, Sigit Sutikno, Andri Thomas, Kevin C. Ryan, and Mark A. Cochrane
Atmos. Chem. Phys., 22, 10173–10194, https://doi.org/10.5194/acp-22-10173-2022, https://doi.org/10.5194/acp-22-10173-2022, 2022
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Fire plus non-fire GHG emissions associated with draining peatlands are the largest per area of any land use change considered by the IPCC. To characterize average and variability for tropical peat fire emissions, highly mobile smoke sampling teams were deployed across four Indonesian provinces to explore an extended interannual, climatic, and spatial range. Large adjustments to IPCC-recommended emissions are suggested. Lab data bolster an extensive emissions database for tropical peat fires.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
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.
Paul A. Solomon, Dena Vallano, Melissa Lunden, Brian LaFranchi, Charles L. Blanchard, and Stephanie L. Shaw
Atmos. Meas. Tech., 13, 3277–3301, https://doi.org/10.5194/amt-13-3277-2020, https://doi.org/10.5194/amt-13-3277-2020, 2020
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Analyzing street-level air pollutants (2016–2017), this assessment indicates that mobile measurement is precise and accurate (5 % to 25 % bias) relative to regulatory sites, with higher spatial resolution. Collocated sensor measurements in California showed differences less than 20 %, suggesting that greater differences represent spatial variability. Mobile data confirm regulatory-site spatial representation and that pollutant levels can also be 6 to 8 times higher just blocks apart.
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.
Charlotte Bürki, Matteo Reggente, Ann M. Dillner, Jenny L. Hand, Stephanie L. Shaw, and Satoshi Takahama
Atmos. Meas. Tech., 13, 1517–1538, https://doi.org/10.5194/amt-13-1517-2020, https://doi.org/10.5194/amt-13-1517-2020, 2020
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Infrared spectroscopy is a chemically informative method for particulate matter characterization. However, recent work has demonstrated that predictions depend heavily on the choice of calibration model parameters. We propose a means for managing parameter uncertainties by combining available data from laboratory standards, molecular databases, and collocated ambient measurements to provide useful characterization of atmospheric organic matter on a large scale.
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.
Md. Robiul Islam, Thilina Jayarathne, Isobel J. Simpson, Benjamin Werden, John Maben, Ashley Gilbert, Puppala S. Praveen, Sagar Adhikari, Arnico K. Panday, Maheswar Rupakheti, Donald R. Blake, Robert J. Yokelson, Peter F. DeCarlo, William C. Keene, and Elizabeth A. Stone
Atmos. Chem. Phys., 20, 2927–2951, https://doi.org/10.5194/acp-20-2927-2020, https://doi.org/10.5194/acp-20-2927-2020, 2020
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The Kathmandu Valley experiences high levels of air pollution. In this study, atmospheric gases and particulate matter were characterized by online and off-line measurements, with an emphasis on understanding their sources. The major sources of particulate matter and trace gases were identified as garbage burning, biomass burning, and vehicles. The majority of secondary organic aerosol was attributed to anthropogenic precursors, while a minority was attributed to biogenic gases.
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.
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 %.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Carley D. Fredrickson, Martin Esparza-Sanchez, Charlotte Burki, Matteo Reggente, Stephanie L. Shaw, Eric S. Edgerton, and Ann M. Dillner
Atmos. Meas. Tech., 12, 5391–5415, https://doi.org/10.5194/amt-12-5391-2019, https://doi.org/10.5194/amt-12-5391-2019, 2019
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Organic species are abundant in atmospheric particle-phase (aerosol) pollution and originate from a variety of biogenic and anthropogenic sources. Infrared spectrometry of filter-based atmospheric particle samples can afford a direct measurement of the particulate organic matter concentration and a characterization of its composition. This work discusses recent method improvements and compositions measured in samples from the SouthEastern Aerosol Research and Characterization (SEARCH) network.
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.
Min Zhong, Eri Saikawa, Alexander Avramov, Chen Chen, Boya Sun, Wenlu Ye, William C. Keene, Robert J. Yokelson, Thilina Jayarathne, Elizabeth A. Stone, Maheswar Rupakheti, and Arnico K. Panday
Atmos. Chem. Phys., 19, 8209–8228, https://doi.org/10.5194/acp-19-8209-2019, https://doi.org/10.5194/acp-19-8209-2019, 2019
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Air pollution is one of the most pressing environmental issues in the Kathmandu Valley, the capital city of Nepal. We estimated emissions from two of the major source types in the valley (vehicles and brick kilns) and found that they have significant impacts on air quality surrounding the valley. Our results highlight the importance of improving local emissions estimates for air quality modeling.
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.
Hansol D. Lee, Chathuri P. Kaluarachchi, Elias S. Hasenecz, Jonic Z. Zhu, Eduard Popa, Elizabeth A. Stone, and Alexei V. Tivanski
Atmos. Meas. Tech., 12, 2033–2042, https://doi.org/10.5194/amt-12-2033-2019, https://doi.org/10.5194/amt-12-2033-2019, 2019
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Dry and wet aerosol deposition modes are commonly used to collect particles on a solid substrate for experiments. We demonstrate, using single-particle microscopy and bulk methods, how the substrate-deposited particles with two components can yield the same core–shell morphology but different shell thicknesses depending on the deposition method. Thus we strongly advise future works to use wet deposition when possible to obtain accurate assessment of the single-particle organic volume fraction.
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.
Anusha Priyadarshani Silva Hettiyadura, Ibrahim M. Al-Naiema, Dagen D. Hughes, Ting Fang, and Elizabeth A. Stone
Atmos. Chem. Phys., 19, 3191–3206, https://doi.org/10.5194/acp-19-3191-2019, https://doi.org/10.5194/acp-19-3191-2019, 2019
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This study examines anthropogenic influences on secondary organic aerosol at an urban site in Atlanta, Georgia. Organosulfates accounted for 16.5 % of PM2.5 organic carbon and were mostly derived from isoprene. In contrast to a rural forested site, Atlanta's isoprene-derived organosulfate concentrations were 2–6 times higher and accounted for twice as much organic carbon. Insights are provided as to which organosulfates should be measured in future studies and targeted for standard development.
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.
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.
Ibrahim M. Al-Naiema, Anusha P. S. Hettiyadura, Henry W. Wallace, Nancy P. Sanchez, Carter J. Madler, Basak Karakurt Cevik, Alexander A. T. Bui, Josh Kettler, Robert J. Griffin, and Elizabeth A. Stone
Atmos. Chem. Phys., 18, 15601–15622, https://doi.org/10.5194/acp-18-15601-2018, https://doi.org/10.5194/acp-18-15601-2018, 2018
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By integrating newly developed tracers for anthropogenic secondary organic aerosol in source apportionment for the first time, we estimate that this source contributes 28 % of fine particle organic carbon in the Houston Ship Channel. Our approach can be used to evaluate anthropogenic, biogenic, and biomass burning contributions to secondary organic aerosols elsewhere in the world. Because anthropogenic emissions are potentially controllable, they provide an opportunity to improve air quality.
J. Douglas Goetz, Michael R. Giordano, Chelsea E. Stockwell, Ted J. Christian, Rashmi Maharjan, Sagar Adhikari, Prakash V. Bhave, Puppala S. Praveen, Arnico K. Panday, Thilina Jayarathne, Elizabeth A. Stone, Robert J. Yokelson, and Peter F. DeCarlo
Atmos. Chem. Phys., 18, 14653–14679, https://doi.org/10.5194/acp-18-14653-2018, https://doi.org/10.5194/acp-18-14653-2018, 2018
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Size distributions and emission factors of submicron aerosol were quantified using online techniques for a variety of common but under-sampled combustion sources in South Asia: wood and dung cooking fires, groundwater pumps, brick kilns, trash burning, and open burning of crop residues. Optical properties (brown carbon light absorption and the absorption Ångström exponent, AAE) of the emissions were also investigated. Contextual comparisons to the literature and other NAMaSTE results were made.
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.
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.
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.
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.
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.
Xi Chen, Mingjie Xie, Michael D. Hays, Eric Edgerton, Donna Schwede, and John T. Walker
Atmos. Chem. Phys., 18, 6829–6846, https://doi.org/10.5194/acp-18-6829-2018, https://doi.org/10.5194/acp-18-6829-2018, 2018
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.
Thilina Jayarathne, Chelsea E. Stockwell, Ashley A. Gilbert, Kaitlyn Daugherty, Mark A. Cochrane, Kevin C. Ryan, Erianto I. Putra, Bambang H. Saharjo, Ati D. Nurhayati, Israr Albar, Robert J. Yokelson, and Elizabeth A. Stone
Atmos. Chem. Phys., 18, 2585–2600, https://doi.org/10.5194/acp-18-2585-2018, https://doi.org/10.5194/acp-18-2585-2018, 2018
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Fine particulate matter (PM2.5) emissions from Indonesian peat burning were measured in situ. Fuel-based emission factors from 6.0–29.6 gPM kg-1. Detailed chemical analysis revealed high levels of organic carbon that was primarily water insoluble, little to no detectable elemental carbon, and alkane contributions to organic carbon in the range of 6 %. These data were used to estimate that 3.2–11 Tg of PM2.5 were emitted by the 2015 peat burning episodes in Indonesia.
Thilina Jayarathne, Chelsea E. Stockwell, Prakash V. Bhave, Puppala S. Praveen, Chathurika M. Rathnayake, Md. Robiul Islam, Arnico K. Panday, Sagar Adhikari, Rashmi Maharjan, J. Douglas Goetz, Peter F. DeCarlo, Eri Saikawa, Robert J. Yokelson, and Elizabeth A. Stone
Atmos. Chem. Phys., 18, 2259–2286, https://doi.org/10.5194/acp-18-2259-2018, https://doi.org/10.5194/acp-18-2259-2018, 2018
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Emissions of fine particulate matter and its constituents were quantified for a variety of under-sampled combustion sources in South Asia: wood and dung cooking fires, generators, groundwater pumps, brick kilns, trash burning, and open burning of biomasses. Garbage burning and three-stone cooking fires were among the highest emitters, while servicing of motor vehicles significantly reduced PM. These data may be used in source apportionment and to update regional and global emission inventories.
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.
Ryan D. Cook, Ying-Hsuan Lin, Zhuoyu Peng, Eric Boone, Rosalie K. Chu, James E. Dukett, Matthew J. Gunsch, Wuliang Zhang, Nikola Tolic, Alexander Laskin, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 15167–15180, https://doi.org/10.5194/acp-17-15167-2017, https://doi.org/10.5194/acp-17-15167-2017, 2017
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Reactions occur within water in both atmospheric particles and cloud droplets, yet little is known about the organic compounds in cloud water. In this work, cloud water samples were collected at Whiteface Mountain, New York, and analyzed using ultra-high-resolution mass spectrometry to investigate the molecular composition of the dissolved organic compounds. The results focus on changes in cloud water composition with air mass origin – influences of forest, urban, and wildfire emissions.
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.
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.
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
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.
Rudra P. Pokhrel, Eric R. Beamesderfer, Nick L. Wagner, Justin M. Langridge, Daniel A. Lack, Thilina Jayarathne, Elizabeth A. Stone, Chelsea E. Stockwell, Robert J. Yokelson, and Shane M. Murphy
Atmos. Chem. Phys., 17, 5063–5078, https://doi.org/10.5194/acp-17-5063-2017, https://doi.org/10.5194/acp-17-5063-2017, 2017
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This study investigates enhancement of black carbon (BC) absorption in biomass burning emissions due to absorbing and non-absorbing coatings. The fraction of absorption due to BC, brown carbon (BrC), and lensing is estimated using different approaches. The similarities and differences between the results from these approaches are discussed. Absorption by BrC is shown to have good correlation with the elemental to organic carbon ratio (EC / OC) and AAE.
Chathurika M. Rathnayake, Nervana Metwali, Thilina Jayarathne, Josh Kettler, Yuefan Huang, Peter S. Thorne, Patrick T. O'Shaughnessy, and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 2459–2475, https://doi.org/10.5194/acp-17-2459-2017, https://doi.org/10.5194/acp-17-2459-2017, 2017
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Exposures to bioaerosols depend on their type, particle size, and concentration. While typically found in coarse particles (2.5–10 microns), pollens, fungal spores, and bacterial endotoxins decrease to less than 2.5 microns and simultaneously increase in concentration during rain events. These observations contrast the assumption that rain washes bioaerosols from the air and reduces allergen levels. Instead, population exposures to bioaerosols are expected to be enhanced during rain events.
Ibrahim M. Al-Naiema and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 2053–2065, https://doi.org/10.5194/acp-17-2053-2017, https://doi.org/10.5194/acp-17-2053-2017, 2017
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Molecular tracers have proven useful in estimating contributions of primary and biogenic secondary sources to atmospheric particulate matter but have lagged behind for anthropogenic secondary sources. This study takes a field-based approach to evaluate the detectability, specificity, and gas–particle partitioning of prospective anthropogenic SOA tracers. We conclude that a subset of species are likely useful tracers and are recommended for use in future source apportionment studies.
Jiaoyan Huang, Matthieu B. Miller, Eric Edgerton, and Mae Sexauer Gustin
Atmos. Chem. Phys., 17, 1689–1698, https://doi.org/10.5194/acp-17-1689-2017, https://doi.org/10.5194/acp-17-1689-2017, 2017
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The highest mercury (Hg) wet deposition in USA occurs along the Gulf of Mexico. Gaseous oxidized Hg (GOM) is a major contributor due to high water solubility and reactivity. Concentration and dry deposition of GOM were determined for OLF, Florida. Results indicated at least 5 GOM compounds in this area including HgBr2, HgO, and Hg–nitrogen and –sulfur forms. GOM chemistry indicates reactions with local mobile source pollutants and long-range transport from outside of the USA.
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.
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.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Marie Ila Gosselin, Chathurika M. Rathnayake, Ian Crawford, Christopher Pöhlker, Janine Fröhlich-Nowoisky, Beatrice Schmer, Viviane R. Després, Guenter Engling, Martin Gallagher, Elizabeth Stone, Ulrich Pöschl, and J. Alex Huffman
Atmos. Chem. Phys., 16, 15165–15184, https://doi.org/10.5194/acp-16-15165-2016, https://doi.org/10.5194/acp-16-15165-2016, 2016
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We present an analysis of bioaerosol measurements using two real-time fluorescence instruments in combination with molecular tracer techniques for quantifying airborne fungal spores in a semi-arid forest. Both techniques provide fungal spore concentrations of the order of 104 m−3 and up to 30 % of particle mass. Rainy periods exhibited higher concentrations and stronger correlations between fluorescent bioparticle and molecular tracer measurements. Fungal culture results are also presented.
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.
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.
Chelsea E. Stockwell, Thilina Jayarathne, Mark A. Cochrane, Kevin C. Ryan, Erianto I. Putra, Bambang H. Saharjo, Ati D. Nurhayati, Israr Albar, Donald R. Blake, Isobel J. Simpson, Elizabeth A. Stone, and Robert J. Yokelson
Atmos. Chem. Phys., 16, 11711–11732, https://doi.org/10.5194/acp-16-11711-2016, https://doi.org/10.5194/acp-16-11711-2016, 2016
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We present the first or rare field measurements of emission factors for Indonesian peat fires made in Borneo during the 2015 El Niño. The data include up to 90 gases, aerosol mass, and aerosol optical properties at two wavelengths (405 and 870 nm). Brown carbon dominates aerosol absorption, revisions to previous values for greenhouse gas emissions are supported and air toxics are assessed.
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.
Chelsea E. Stockwell, Ted J. Christian, J. Douglas Goetz, Thilina Jayarathne, Prakash V. Bhave, Puppala S. Praveen, Sagar Adhikari, Rashmi Maharjan, Peter F. DeCarlo, Elizabeth A. Stone, Eri Saikawa, Donald R. Blake, Isobel J. Simpson, Robert J. Yokelson, and Arnico K. Panday
Atmos. Chem. Phys., 16, 11043–11081, https://doi.org/10.5194/acp-16-11043-2016, https://doi.org/10.5194/acp-16-11043-2016, 2016
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We present the first, or rare, field measurements in South Asia of emission factors for up to 80 gases (pollutants, greenhouse gases, and precursors) and black carbon and aerosol optical properties at 405 and 870 nm for many previously under-sampled sources that are important in developing countries such as cooking with dung and wood, garbage and crop residue burning, brick kilns, motorcycles, generators and pumps, etc. Brown carbon contributes significantly to total aerosol absorption.
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.
Rudra P. Pokhrel, Nick L. Wagner, Justin M. Langridge, Daniel A. Lack, Thilina Jayarathne, Elizabeth A. Stone, Chelsea E. Stockwell, Robert J. Yokelson, and Shane M. Murphy
Atmos. Chem. Phys., 16, 9549–9561, https://doi.org/10.5194/acp-16-9549-2016, https://doi.org/10.5194/acp-16-9549-2016, 2016
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This paper gives first multi-wavelength estimates of SSA and AAE of emissions from combustion of Indonesian peat. In addition, it demonstrates that SSA of biomass burning emissions can be parameterized with EC / (EC+OC) and that this parameterization is quantitatively superior to previously published parameterizations based on MCE. It also shows that EC / (EC+OC) parameterization accurately predicts SSA during the first few hours of aging of a biomass burning plume.
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.
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
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
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.
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.
Min Zhong, Eri Saikawa, Yang Liu, Vaishali Naik, Larry W. Horowitz, Masayuki Takigawa, Yu Zhao, Neng-Huei Lin, and Elizabeth A. Stone
Geosci. Model Dev., 9, 1201–1218, https://doi.org/10.5194/gmd-9-1201-2016, https://doi.org/10.5194/gmd-9-1201-2016, 2016
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Large discrepancies exist among emission inventories (e.g., REAS and EDGAR) at the provincial level in China. We use WRF-Chem to evaluate the impact of the difference in existing emission inventories and find that emissions inputs significantly affect our air pollutant simulation results. Our study highlights the importance of constraining emissions at the provincial level for regional air quality modeling over East Asia.
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.
Sean Coburn, Barbara Dix, Eric Edgerton, Christopher D. Holmes, Douglas Kinnison, Qing Liang, Arnout ter Schure, Siyuan Wang, and Rainer Volkamer
Atmos. Chem. Phys., 16, 3743–3760, https://doi.org/10.5194/acp-16-3743-2016, https://doi.org/10.5194/acp-16-3743-2016, 2016
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Here we present a day of case study measurements of the vertical distribution of bromine monoxide over the coastal region of the Gulf of Mexico. These measurements are used to assess the contribution of bromine radicals to the oxidation of elemental mercury in the troposphere. We find that the measured levels of bromine in the troposphere are sufficient to quickly oxidize mercury, which has significant implications for our understanding of atmospheric mercury processes.
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.
E. W. Butt, A. Rap, A. Schmidt, C. E. Scott, K. J. Pringle, C. L. Reddington, N. A. D. Richards, M. T. Woodhouse, J. Ramirez-Villegas, H. Yang, V. Vakkari, E. A. Stone, M. Rupakheti, P. S. Praveen, P. G. van Zyl, J. P. Beukes, M. Josipovic, E. J. S. Mitchell, S. M. Sallu, P. M. Forster, and D. V. Spracklen
Atmos. Chem. Phys., 16, 873–905, https://doi.org/10.5194/acp-16-873-2016, https://doi.org/10.5194/acp-16-873-2016, 2016
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We estimate the impact of residential emissions (cooking and heating) on atmospheric aerosol, human health, and climate. We find large contributions to annual mean ambient PM2.5 in residential sources regions resulting in significant but uncertain global premature mortality when key uncertainties in emission flux are considered. We show that residential emissions exert an uncertain global radiative effect and suggest more work is needed to characterise residential emissions climate importance.
C. L. Blanchard, G. M. Hidy, S. Shaw, K. Baumann, and E. S. Edgerton
Atmos. Chem. Phys., 16, 215–238, https://doi.org/10.5194/acp-16-215-2016, https://doi.org/10.5194/acp-16-215-2016, 2016
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Fifteen years of gas and particle measurements at eight monitoring sites comprising the Southeastern Aerosol Research and Characterization (SEARCH) network offer insights into the sources of organic aerosol in the southeastern United States. Between 1999 and 2013, mean organic aerosol concentrations declined due to decreasing particle emissions from motor vehicles and to less secondary organic aerosol with declining emissions of sulfur dioxide, nitrogen oxides, and volatile organic compounds.
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.
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.
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.
H. M. Allen, D. C. Draper, B. R. Ayres, A. Ault, A. Bondy, S. Takahama, R. L. Modini, K. Baumann, E. Edgerton, C. Knote, A. Laskin, B. Wang, and J. L. Fry
Atmos. Chem. Phys., 15, 10669–10685, https://doi.org/10.5194/acp-15-10669-2015, https://doi.org/10.5194/acp-15-10669-2015, 2015
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We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
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.
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.
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.
D. B. Millet, M. Baasandorj, D. K. Farmer, J. A. Thornton, K. Baumann, P. Brophy, S. Chaliyakunnel, J. A. de Gouw, M. Graus, L. Hu, A. Koss, B. H. Lee, F. D. Lopez-Hilfiker, J. A. Neuman, F. Paulot, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, B. J. Williams, and J. Xu
Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, https://doi.org/10.5194/acp-15-6283-2015, 2015
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Formic acid (HCOOH) is an abundant atmospheric acid that affects precipitation chemistry and acidity. HCOOH measurements over the USA are 2-3× larger than can be explained by known sources and sinks, revealing a key gap in current understanding. Observations indicate a large biogenic source plus chemical production across a range of precursors. Model simulations cannot capture the HCOOH diurnal amplitude or nocturnal profile, implying a deposition bias and possibly even larger missing source.
A. P. S. Hettiyadura, E. A. Stone, S. Kundu, Z. Baker, E. Geddes, K. Richards, and T. Humphry
Atmos. Meas. Tech., 8, 2347–2358, https://doi.org/10.5194/amt-8-2347-2015, https://doi.org/10.5194/amt-8-2347-2015, 2015
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Organosulfates are SOA products that have proven difficult to quantify. This study addresses the need for authentic quantification standards with a straightforward approach to synthesizing highly pure organosulfate potassium salts. New standards are used to develop a new separation protocol for small, functionalized organosulfates. Upon validation, this method is used to assess sample preparation protocols and to make new measurements of organosulfates in Centreville, Alabama.
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. Huang, M. B. Miller, E. Edgerton, and M. S. Gustin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-12069-2015, https://doi.org/10.5194/acpd-15-12069-2015, 2015
Revised manuscript not accepted
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Gaseous oxidized Hg (GOM) is a major contributor to Hg in wet and dry deposition. Recent work has indicated that the concentrations of GOM as measured are too low by 3-to-12 times; and that compounds vary across space and time. Data collected in Florida indicate five potential GOM compounds, including HgBr2, HgO, Hg(NO3)2, HgSO4, and an unknown compound. Sources include local combustion (cars and power plants), the marine boundary layer, and long range transport from Asia.
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.
M. Lewandowski, M. Jaoui, J. H. Offenberg, J. D. Krug, and T. E. Kleindienst
Atmos. Chem. Phys., 15, 3773–3783, https://doi.org/10.5194/acp-15-3773-2015, https://doi.org/10.5194/acp-15-3773-2015, 2015
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This work explores the impact of acidic sulfate aerosol on the formation of SOA from isoprene and 1,3-butadiene. This study expands on previous work by extending the analysis over a broader range of humidities and aerosol liquid water contents. Extending the experiments to a wider range of hydrocarbons and across a more realistic range of humidities provides data of greater atmospheric relevance and contributes to development of acidity-influenced SOA chemistry mechanisms in air quality models.
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.
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.
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
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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
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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.
G. M. Hidy, C. L. Blanchard, K. Baumann, E. Edgerton, S. Tanenbaum, S. Shaw, E. Knipping, I. Tombach, J. Jansen, and J. Walters
Atmos. Chem. Phys., 14, 11893–11914, https://doi.org/10.5194/acp-14-11893-2014, https://doi.org/10.5194/acp-14-11893-2014, 2014
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This paper reviews aerometric measurements from Centreville, Alabama. The measurements show annual trends with air pollution emissions from 1999 to 2013. They provide a context for observations from 1 June to 15 July 2013 supporting the Southern Oxidant and Aerosol Study. An important goal of this experiment was to advance knowledge of aerosols produced in the atmosphere from precursors. The observations were in moist and warm conditions with the lowest gas and particle concentrations recorded.
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
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
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
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
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
S. Kundu, T. A. Quraishi, G. Yu, C. Suarez, F. N. Keutsch, and E. A. Stone
Atmos. Chem. Phys., 13, 4865–4875, https://doi.org/10.5194/acp-13-4865-2013, https://doi.org/10.5194/acp-13-4865-2013, 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
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
In situ measurement of organic aerosol molecular markers in urban Hong Kong during a summer period: temporal variations and source apportionment
Technical note: Determining chemical composition of atmospheric single particles by a standard-free mass calibration algorithm
Different formation pathways of nitrogen-containing organic compounds in aerosols and fog water in northern China
Impact of weather patterns and meteorological factors on PM2.5 and O3 responses to the COVID-19 lockdown in China
Daytime and nighttime aerosol soluble iron formation in clean and slightly polluted moist air in a coastal city in eastern China
Non-negligible secondary contribution to brown carbon in autumn and winter: inspiration from particulate nitrated and oxygenated aromatic compounds in urban Beijing
Simultaneous organic aerosol source apportionment at two Antarctic sites reveals large-scale and ecoregion-specific components
Measurement report: Optical characterization, seasonality, and sources of brown carbon in fine aerosols from Tianjin, North China: year-round observations
Bayesian inference-based estimation of hourly primary and secondary organic carbon in suburban Hong Kong: multi-temporal-scale variations and evolution characteristics during PM2.5 episodes
Measurement report: Characteristics of nitrogen-containing organics in PM2.5 in Ürümqi, northwestern China – differential impacts of combustion of fresh and aged biomass materials
Measurement report: Bio-physicochemistry of tropical clouds at Maïdo (Réunion, Indian Ocean): overview of results from the BIO-MAÏDO campaign
Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign
High Altitude Aerosol Chemical Characterization and Source Identification: Insights from the CALISHTO Campaign
Characterizing water solubility of fresh and aged secondary organic aerosol in PM2.5 with the stable carbon isotope technique
Measurement report: Evaluation of the TOF-ACSM-CV for PM1.0 and PM2.5 measurements during the RITA-2021 field campaign
Sea salt reactivity over the northwest Atlantic: an in-depth look using the airborne ACTIVATE dataset
Measurement report: Atmospheric ice nuclei in the Changbai Mountains (2623 m a.s.l.) in northeastern Asia
Morphological and optical properties of carbonaceous aerosol particles from ship emissions and biomass burning during a summer cruise measurement in the South China Sea
Critical contribution of chemically diverse carbonyl molecules to the oxidative potential of atmospheric aerosols
Tropical tropospheric aerosol sources and chemical composition observed at high altitude in the Bolivian Andes
Chemical composition, sources and formation mechanism of urban PM2.5 in Southwest China: a case study at the beginning of 2023
Chemical characterization of atmospheric aerosols at a high-altitude mountain site: a study of source apportionment
Composition and sources of carbonaceous aerosol in the European Arctic at Zeppelin Observatory, Svalbard (2017 to 2020)
Measurement Report: Size-resolved secondary organic aerosol formation modulated by aerosol water uptake in wintertime haze
Variation in chemical composition and volatility of oxygenated organic aerosol in different rural, urban, and mountain environments
Elucidating the mechanisms of atmospheric new particle formation in the highly polluted Po Valley, Italy
Water-insoluble organic carbon in PM2.5 over China: light-absorbing properties, potential sources, radiative forcing effects and possible light-absorbing continuum
Diverging trends in aerosol sulfate and nitrate measured in the remote North Atlantic on Barbados are attributed to clean air policies, African smoke, and anthropogenic emissions
Local ship speed reduction effect on black carbon emissions measured at remote marine station
Roles of marine biota in the formation of atmospheric bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the North Pacific Ocean, Bering Sea, and Arctic Ocean
Evolution of nucleophilic high molecular-weight organic compounds in ambient aerosols: a case study
Fractional solubility of iron in mineral dust aerosols over coastal Namibia: a link to marine biogenic emissions?
Real-world observations of reduced nitrogen and ultrafine particles in commercial cooking organic aerosol emissions
Source apportionment of PM2.5 in Montréal, Canada, and health risk assessment for potentially toxic elements
Physicochemical and temporal characteristics of individual atmospheric aerosol particles in urban Seoul during KORUS-AQ campaign: insights from single-particle analysis
Mass spectrometric analysis of unprecedented high levels of carbonaceous aerosol particles long-range transported from wildfires in the Siberian Arctic
Short-term source apportionment of fine particulate matter with time-dependent profiles using SoFi Pro: exploring the reliability of rolling positive matrix factorization (PMF) applied to bihourly molecular and elemental tracer data
Particulate-bound alkyl nitrate pollution and formation mechanisms in Beijing, China
Measurement report: Impact of emission control measures on environmental persistent free radicals and reactive oxygen species – A short-term case study in Beijing
Characterization of water-soluble brown carbon chromophores from wildfire plumes in the western USA using size-exclusion chromatography
Marine carbohydrates in Arctic aerosol particles and fog – diversity of oceanic sources and atmospheric transformations
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 1: Observational data analysis
Measurement report: Brown carbon aerosol in polluted urban air of the North China Plain – day–night differences in the chromophores and optical properties
Measurement report: Secondary organic aerosols at a forested mountain site in southeastern China
Source apportionment of soot particles and aqueous-phase processing of black carbon coatings in an urban environment
Seasonal variations in composition and sources of atmospheric ultrafine particles in urban Beijing based on near-continuous measurements
Summertime response of ozone and fine particulate matter to mixing layer meteorology over the North China Plain
Trace elements in PM2.5 aerosols in East Asian outflow in the spring of 2018: emission, transport, and source apportionment
Measurement Report: Investigation on the sources and formation processes of dicarboxylic acids and related species in urban aerosols before and during the COVID-19 lockdown in Jinan, East China
pH dependence of brown-carbon optical properties in cloud water
Hongyong Li, Xiaopu Lyu, Likun Xue, Yunxi Huo, Dawen Yao, Haoxian Lu, and Hai Guo
Atmos. Chem. Phys., 24, 7085–7100, https://doi.org/10.5194/acp-24-7085-2024, https://doi.org/10.5194/acp-24-7085-2024, 2024
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Organic aerosol is ubiquitous in the atmosphere and largely explains the gap between current levels of fine particulate matter in many cities and the World Health Organization guideline values. This study highlights the dominant contributions of cooking emissions to organic aerosol when marine air prevailed in Hong Kong, which were occasionally overwhelmed by aromatics-derived secondary organic aerosol in continental ouflows.
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Atmos. Chem. Phys., 24, 7001–7012, https://doi.org/10.5194/acp-24-7001-2024, https://doi.org/10.5194/acp-24-7001-2024, 2024
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The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~ 0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.
Wei Sun, Xiaodong Hu, Yuzhen Fu, Guohua Zhang, Yujiao Zhu, Xinfeng Wang, Caiqing Yan, Likun Xue, He Meng, Bin Jiang, Yuhong Liao, Xinming Wang, Ping'an Peng, and Xinhui Bi
Atmos. Chem. Phys., 24, 6987–6999, https://doi.org/10.5194/acp-24-6987-2024, https://doi.org/10.5194/acp-24-6987-2024, 2024
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The formation pathways of nitrogen-containing compounds (NOCs) in the atmosphere remain unclear. We investigated the composition of aerosols and fog water by state-of-the-art mass spectrometry and compared the formation pathways of NOCs. We found that NOCs in aerosols were mainly formed through nitration reaction, while ammonia addition played a more important role in fog water. The results deepen our understanding of the processes of organic particulate pollution.
Fuzhen Shen, Michaela I. Hegglin, and Yue Yuan
Atmos. Chem. Phys., 24, 6539–6553, https://doi.org/10.5194/acp-24-6539-2024, https://doi.org/10.5194/acp-24-6539-2024, 2024
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We attempt to use a novel structural self-organising map and machine learning models to identify a weather system and quantify the importance of each meteorological factor in driving the unexpected PM2.5 and O3 changes under the specific weather system during the COVID-19 lockdown in China. The result highlights that temperature under the double-centre high-pressure system plays the most crucial role in abnormal events.
Wenshuai Li, Yuxuan Qi, Yingchen Liu, Guanru Wu, Yanjing Zhang, Jinhui Shi, Wenjun Qu, Lifang Sheng, Wencai Wang, Daizhou Zhang, and Yang Zhou
Atmos. Chem. Phys., 24, 6495–6508, https://doi.org/10.5194/acp-24-6495-2024, https://doi.org/10.5194/acp-24-6495-2024, 2024
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Aerosol particles from mainland can transport to oceans and deposit, providing soluble Fe and affecting phytoplankton growth. Thus, we studied the dissolution process of aerosol Fe and found that photochemistry played a key role in promoting Fe dissolution in clean conditions. RH-dependent reactions were more influential in slightly polluted conditions. These results highlight the distinct roles of two weather-related parameters (radiation and RH) in influencing geochemical cycles related to Fe.
Yanqin Ren, Zhenhai Wu, Yuanyuan Ji, Fang Bi, Junling Li, Haijie Zhang, Hao Zhang, Hong Li, and Gehui Wang
Atmos. Chem. Phys., 24, 6525–6538, https://doi.org/10.5194/acp-24-6525-2024, https://doi.org/10.5194/acp-24-6525-2024, 2024
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Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) in PM2.5 were examined from an urban area in Beijing during the autumn and winter. The OPAH and NAC concentrations were much higher during heating than before heating. They majorly originated from the combustion of biomass and automobile emissions, and the secondary generation was the major contributor throughout the whole sampling period.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
Atmos. Chem. Phys., 24, 6305–6322, https://doi.org/10.5194/acp-24-6305-2024, https://doi.org/10.5194/acp-24-6305-2024, 2024
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Applying factor analysis techniques to H-NMR spectra, we present the organic aerosol (OA) source apportionment of PM1 samples collected in parallel at two Antarctic stations, namely Signy and Halley, allowing investigation of aerosol–climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open-ocean) and sympagic (sea-ice-influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Zhichao Dong, Chandra Mouli Pavuluri, Peisen Li, Zhanjie Xu, Junjun Deng, Xueyan Zhao, Xiaomai Zhao, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 5887–5905, https://doi.org/10.5194/acp-24-5887-2024, https://doi.org/10.5194/acp-24-5887-2024, 2024
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Comprehensive study of optical properties of brown carbon (BrC) in fine aerosols from Tianjin, China, implied that biological emissions are major sources of BrC in summer, whereas fossil fuel combustion and biomass burning emissions are in cold periods. The direct radiation absorption caused by BrC in short wavelengths contributed about 40 % to that caused by BrC in 300–700 nm. Water-insoluble but methanol-soluble BrC contains more protein-like chromophores (PLOM) than that of water-soluble BrC.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 5803–5821, https://doi.org/10.5194/acp-24-5803-2024, https://doi.org/10.5194/acp-24-5803-2024, 2024
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In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal-scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Yi-Jia Ma, Yu Xu, Ting Yang, Hong-Wei Xiao, and Hua-Yun Xiao
Atmos. Chem. Phys., 24, 4331–4346, https://doi.org/10.5194/acp-24-4331-2024, https://doi.org/10.5194/acp-24-4331-2024, 2024
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This study provides field-based evidence about the differential impacts of combustion of fresh and aged biomass materials on aerosol nitrogen-containing organic compounds (NOCs) in different seasons in Ürümqi, bridging the linkages between the observations and previous laboratory studies showing the formation mechanisms of NOCs.
Maud Leriche, Pierre Tulet, Laurent Deguillaume, Frédéric Burnet, Aurélie Colomb, Agnès Borbon, Corinne Jambert, Valentin Duflot, Stéphan Houdier, Jean-Luc Jaffrezo, Mickaël Vaïtilingom, Pamela Dominutti, Manon Rocco, Camille Mouchel-Vallon, Samira El Gdachi, Maxence Brissy, Maroua Fathalli, Nicolas Maury, Bert Verreyken, Crist Amelynck, Niels Schoon, Valérie Gros, Jean-Marc Pichon, Mickael Ribeiro, Eric Pique, Emmanuel Leclerc, Thierry Bourrianne, Axel Roy, Eric Moulin, Joël Barrie, Jean-Marc Metzger, Guillaume Péris, Christian Guadagno, Chatrapatty Bhugwant, Jean-Mathieu Tibere, Arnaud Tournigand, Evelyn Freney, Karine Sellegri, Anne-Marie Delort, Pierre Amato, Muriel Joly, Jean-Luc Baray, Pascal Renard, Angelica Bianco, Anne Réchou, and Guillaume Payen
Atmos. Chem. Phys., 24, 4129–4155, https://doi.org/10.5194/acp-24-4129-2024, https://doi.org/10.5194/acp-24-4129-2024, 2024
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Aerosol particles in the atmosphere play a key role in climate change and air pollution. A large number of aerosol particles are formed from the oxidation of volatile organic compounds (VOCs and secondary organic aerosols – SOA). An important field campaign was organized on Réunion in March–April 2019 to understand the formation of SOA in a tropical atmosphere mostly influenced by VOCs emitted by forest and in the presence of clouds. This work synthesizes the results of this campaign.
Ryan N. Farley, James E. Lee, Laura-Hélèna Rivellini, Alex K. Y. Lee, Rachael Dal Porto, Christopher D. Cappa, Kyle Gorkowski, Abu Sayeed Md Shawon, Katherine B. Benedict, Allison C. Aiken, Manvendra K. Dubey, and Qi Zhang
Atmos. Chem. Phys., 24, 3953–3971, https://doi.org/10.5194/acp-24-3953-2024, https://doi.org/10.5194/acp-24-3953-2024, 2024
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The black carbon aerosol composition and mixing state were characterized using a soot particle aerosol mass spectrometer. Single-particle measurements revealed the major role of atmospheric processing in modulating the black carbon mixing state. A significant fraction of soot particles were internally mixed with oxidized organic aerosol and sulfate, with implications for activation as cloud nuclei.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-737, https://doi.org/10.5194/egusphere-2024-737, 2024
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PM1 chemical characterization and PMF source apportionment on the combined organic and inorganic fraction took place at the high-altitude (HAC)2 station. Cloud presence was found to reduce PM1 concentrations, affecting sulphate more than organics. Interstitial aerosol was richer in low hygroscopic organics and acidic inorganics, compared to activated. Higher relative abundance of eBC compared to the other components was revealed for FT conditions compared to PBL.
Fenghua Wei, Xing Peng, Liming Cao, Mengxue Tang, Ning Feng, Xiaofeng Huang, and Lingyan He
EGUsphere, https://doi.org/10.5194/egusphere-2024-736, https://doi.org/10.5194/egusphere-2024-736, 2024
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The water solubility of secondary organic aerosols (SOA) is a crucial factor in determining their hygroscopicity and climatic impact. Stable carbon isotope and mass spectrometry techniques were combined to assess the water solubility of SOA with different aging degrees in a coastal megacity in China. This work revealed a much higher water-soluble fraction of aged SOA compared to fresh SOA, indicating that the aging degree of SOA has considerable impacts on its water solubility.
Xinya Liu, Bas Henzing, Arjan Hensen, Jan Mulder, Peng Yao, Danielle van Dinther, Jerry van Bronckhorst, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 3405–3420, https://doi.org/10.5194/acp-24-3405-2024, https://doi.org/10.5194/acp-24-3405-2024, 2024
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We evaluated the time-of-flight aerosol chemical speciation monitor (TOF-ACSM) following the implementation of the PM2.5 aerodynamic lens and a capture vaporizer (CV). The results showed that it significantly improved the accuracy and precision of ACSM in the field observations. The paper elucidates the measurement outcomes of various instruments and provides an analysis of their biases. This comprehensive evaluation is expected to benefit the ACSM community and other aerosol field measurements.
Eva-Lou Edwards, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Claire E. Robinson, Michael A. Shook, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 3349–3378, https://doi.org/10.5194/acp-24-3349-2024, https://doi.org/10.5194/acp-24-3349-2024, 2024
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We investigate Cl− depletion in sea salt particles over the northwest Atlantic from December 2021 to June 2022 using an airborne dataset. Losses of Cl− are greatest in May and least in December–February and March. Inorganic acidic species can account for all depletion observed for December–February, March, and June near Bermuda but none in May. Quantifying Cl− depletion as a percentage captures seasonal trends in depletion but fails to convey the effects it may have on atmospheric oxidation.
Yue Sun, Yujiao Zhu, Yanbin Qi, Lanxiadi Chen, Jiangshan Mu, Ye Shan, Yu Yang, Yanqiu Nie, Ping Liu, Can Cui, Ji Zhang, Mingxuan Liu, Lingli Zhang, Yufei Wang, Xinfeng Wang, Mingjin Tang, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 24, 3241–3256, https://doi.org/10.5194/acp-24-3241-2024, https://doi.org/10.5194/acp-24-3241-2024, 2024
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Field observations were conducted at the summit of Changbai Mountain in northeast Asia. The cumulative number concentration of ice-nucleating particles (INPs) varied from 1.6 × 10−3 to 78.3 L−1 over the temperature range of −5.5 to −29.0 ℃. Biological INPs (bio-INPs) accounted for the majority of INPs, and the proportion exceeded 90% above −13.0 ℃. Planetary boundary layer height, valley breezes, and long-distance transport of air mass influence the abundance of bio-INPs.
Cuizhi Sun, Yongyun Zhang, Baoling Liang, Min Gao, Xi Sun, Fei Li, Xue Ni, Qibin Sun, Hengjia Ou, Dexian Chen, Shengzhen Zhou, and Jun Zhao
Atmos. Chem. Phys., 24, 3043–3063, https://doi.org/10.5194/acp-24-3043-2024, https://doi.org/10.5194/acp-24-3043-2024, 2024
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In a May–June 2021 expedition in the South China Sea, we analyzed black and brown carbon in marine aerosols, key to light absorption and climate impact. Using advanced in situ and microscope techniques, we observed particle size, structure, and tar balls mixed with various elements. Results showed biomass burning and fossil fuels majorly influence light absorption, especially during significant burning events. This research aids the understanding of carbonaceous aerosols' role in marine climate.
Feifei Li, Shanshan Tang, Jitao Lv, Shiyang Yu, Xu Sun, Dong Cao, Yawei Wang, and Guibin Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-37, https://doi.org/10.5194/egusphere-2024-37, 2024
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Targeted derivatization and non-targeted analysis with FT-ICR MS were used to reveal the molecular composition of carbonyl molecules in PM2.5, and the important role of carbonyls in increasing the oxidative potential of organic aerosol was found in the real samples.
C. Isabel Moreno, Radovan Krejci, Jean-Luc Jaffrezo, Gaëlle Uzu, Andrés Alastuey, Marcos F. Andrade, Valeria Mardóñez, Alkuin Maximilian Koenig, Diego Aliaga, Claudia Mohr, Laura Ticona, Fernando Velarde, Luis Blacutt, Ricardo Forno, David N. Whiteman, Alfred Wiedensohler, Patrick Ginot, and Paolo Laj
Atmos. Chem. Phys., 24, 2837–2860, https://doi.org/10.5194/acp-24-2837-2024, https://doi.org/10.5194/acp-24-2837-2024, 2024
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Aerosol chemical composition (ions, sugars, carbonaceous matter) from 2011 to 2020 was studied at Mt. Chacaltaya (5380 m a.s.l., Bolivian Andes). Minimum concentrations occur in the rainy season with maxima in the dry and transition seasons. The origins of the aerosol are located in a radius of hundreds of kilometers: nearby urban and rural areas, natural biogenic emissions, vegetation burning from Amazonia and Chaco, Pacific Ocean emissions, soil dust, and Peruvian volcanism.
Junke Zhang, Yunfei Su, Chunying Chen, Wenkai Guo, Qinwen Tan, Miao Feng, Danlin Song, Tao Jiang, Qiang Chen, Yuan Li, Wei Li, Yizhi Wang, Xiaojuan Huang, Lin Han, Wanqing Wu, and Gehui Wang
Atmos. Chem. Phys., 24, 2803–2820, https://doi.org/10.5194/acp-24-2803-2024, https://doi.org/10.5194/acp-24-2803-2024, 2024
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Typical haze events in Chengdu at the beginning of 2023 were investigated with bulk-chemical and single-particle analyses along with numerical model simulations. By integrating the obtained chemical composition, source, mixing state and numerical simulation results, we infer that Haze-1 was mainly caused by pollutants related to fossil fuel combustion, especially local mobile sources, while Haze-2 was triggered by the secondary pollutants, which mainly came from regional transmission.
Elena Barbaro, Matteo Feltracco, Fabrizio De Blasi, Clara Turetta, Marta Radaelli, Warren Cairns, Giulio Cozzi, Giovanna Mazzi, Marco Casula, Jacopo Gabrieli, Carlo Barbante, and Andrea Gambaro
Atmos. Chem. Phys., 24, 2821–2835, https://doi.org/10.5194/acp-24-2821-2024, https://doi.org/10.5194/acp-24-2821-2024, 2024
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The study analyzed a year of atmospheric aerosol composition at Col Margherita in the Italian Alps. Over 100 chemical markers were identified, including major ions, organic compounds, and trace elements. It revealed sources of aerosol, highlighted impacts of Saharan dust events, and showed anthropogenic pollution's influence despite the site's remoteness. Enrichment factors emphasized non-natural sources of trace elements. Source apportionment identified four key factors affecting the area.
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.
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, and Colin O’Dowd
EGUsphere, https://doi.org/10.5194/egusphere-2024-573, https://doi.org/10.5194/egusphere-2024-573, 2024
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The chemical composition of atmospheric particles showed significant changes in recent years. We investigated the potential effects of inorganics changes on aerosol water uptake and thus secondary organic aerosol formation in wintertime haze, based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, Northwest China. This study highlights the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
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By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Yangzhi Mo, Jun Li, Guangcai Zhong, Sanyuan Zhu, Shizhen Zhao, Jiao Tang, Hongxing Jiang, Zhineng Cheng, Chongguo Tian, Yingjun Chen, and Gan Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2024-130, https://doi.org/10.5194/egusphere-2024-130, 2024
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In this study, we found that biomass burning (31.0 %) and coal combustion (31.1 %), were the dominant sources of water-insoluble organic carbon in China, with coal combustion sources exhibited the strongest light-absorbing capacity. Additionally, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to have stronger light-absorbing capacity, higher aromaticity, higher molecular weights, and greater recalcitrance in the atmosphere.
Cassandra J. Gaston, Joseph M. Prospero, Kristen Foley, Havala O. T. Pye, Lillian Custals, Edmund Blades, Peter Sealy, and James A. Christie
EGUsphere, https://doi.org/10.5194/egusphere-2024-11, https://doi.org/10.5194/egusphere-2024-11, 2024
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To understand how changing emissions have impacted aerosols in remote regions, we measured nitrate and sulfate at Barbados and compared 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 of sulfur dioxide (SO2) in the U.S. and Europe, then increased in the 2000s due to anthropogenic emissions from Africa and more efficient oxidation of SO2.
Mikko Heikkilä, Krista Luoma, Timo Mäkelä, and Tiia Grönholm
EGUsphere, https://doi.org/10.5194/egusphere-2023-2823, https://doi.org/10.5194/egusphere-2023-2823, 2024
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Black carbon (BC) concentration was measured from 211 ship exhaust gas plumes at a remote marine station. Emission factors of BC were calculated in grams/kilograms fuel. Ships using exhaust gas cleaning systems (EGCS) were found to emit 80 % less BC than ships without EGCS. Emission factors were used to model BC emissions as a function of speed to define the effect of speed reduction. BC emissions increased with a decrease in speed from the ship’s service speed.
Kaori Kawana, Fumikazu Taketani, Kazuhiko Matsumoto, Yutaka Tobo, Yoko Iwamoto, Takuma Miyakawa, Akinori Ito, and Yugo Kanaya
Atmos. Chem. Phys., 24, 1777–1799, https://doi.org/10.5194/acp-24-1777-2024, https://doi.org/10.5194/acp-24-1777-2024, 2024
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Based on comprehensive shipborne observations, we found strong links between sea-surface biological materials and the formation of atmospheric fluorescent bioaerosols, cloud condensation nuclei, and ice-nucleating particles over the Arctic Ocean and Bering Sea during autumn 2019. Taking the wind-speed effect into account, we propose equations to approximate the links for this cruise, which can be used as a guide for modeling as well as for systematic comparisons with other observations.
Chen He, Hanxiong Che, Zier Bao, Yiliang Liu, Qing Li, Miao Hu, Jiawei Zhou, Shumin Zhang, Xiaojiang Yao, Quan Shi, Chunmao Chen, Yan Han, Lingshuo Meng, Xin Long, Fumo Yang, and Yang Chen
Atmos. Chem. Phys., 24, 1627–1639, https://doi.org/10.5194/acp-24-1627-2024, https://doi.org/10.5194/acp-24-1627-2024, 2024
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We examined the daily evolution of high molecular-weight organic compounds with a molecular weight of up to 1000 Da in order to comprehend their behaviors in the atmosphere under actual conditions. These compounds were proven to undergo multi-generation oxidation, carboxylation, and nitrification via both day- and nighttime chemistry.
Karine Desboeufs, Paola Formenti, Raquel Torres-Sánchez, Kerstin Schepanski, Jean-Pierre Chaboureau, Hendrik Andersen, Jan Cermak, Stefanie Feuerstein, Benoit Laurent, Danitza Klopper, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cécile Mirande-Bret, Sylvain Triquet, and Stuart J. Piketh
Atmos. Chem. Phys., 24, 1525–1541, https://doi.org/10.5194/acp-24-1525-2024, https://doi.org/10.5194/acp-24-1525-2024, 2024
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This study investigates the fractional solubility of iron (Fe) in dust particles along the coast of Namibia, a critical region for the atmospheric Fe supply of the South Atlantic Ocean. Our results suggest a possible two-way interplay whereby marine biogenic emissions from the coastal marine ecosystems into the atmosphere would increase the solubility of Fe-bearing dust by photo-reduction processes. The subsequent deposition of soluble Fe could act to further enhance marine biogenic emissions.
Sunhye Kim, Jo Machesky, Drew R. Gentner, and Albert A. Presto
Atmos. Chem. Phys., 24, 1281–1298, https://doi.org/10.5194/acp-24-1281-2024, https://doi.org/10.5194/acp-24-1281-2024, 2024
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Cooking emissions are often an overlooked source of air pollution. We used a mobile lab to measure the characteristics of particles emitted from cooking sites in two cities. Our findings showed that cooking releases a substantial number of fine particles. While most emissions were similar, a bakery site showed distinctive chemical compositions with higher nitrogen compound levels. Thus, understanding the particle emissions from different cooking activities is crucial.
Nansi Fakhri, Robin Stevens, Arnold Downey, Konstantina Oikonomou, Jean Sciare, Charbel Afif, and Patrick L. Hayes
Atmos. Chem. Phys., 24, 1193–1212, https://doi.org/10.5194/acp-24-1193-2024, https://doi.org/10.5194/acp-24-1193-2024, 2024
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We investigated the chemical composition of atmospheric fine particles, their emission sources, and the potential human health risk associated with trace elements in particles for an urban site in Montréal over a 3-month period (August–November). This study represents the first time that such extensive composition measurements were included in an urban source apportionment study in Canada, and it provides greater resolution of fine-particle sources than has been previously achieved in Canada.
Hanjin Yoo, Li Wu, Hong Geng, and Chul-Un Ro
Atmos. Chem. Phys., 24, 853–867, https://doi.org/10.5194/acp-24-853-2024, https://doi.org/10.5194/acp-24-853-2024, 2024
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We conducted an investigation of atmospheric aerosols collected in Seoul, South Korea, during the KORUS-AQ campaign on a single-particle basis. We were able to identify their sources, the atmospheric fate, and the impacts of local emissions and long-range transport on aerosol composition. Additionally, we traced potential sources of non-exhaust heavy-metal particles. This comprehensive analysis provides valuable insights into the complex dynamics of urban aerosols.
Eric Schneider, Hendryk Czech, Olga Popovicheva, Marina Chichaeva, Vasily Kobelev, Nikolay Kasimov, Tatiana Minkina, Christopher Paul Rüger, and Ralf Zimmermann
Atmos. Chem. Phys., 24, 553–576, https://doi.org/10.5194/acp-24-553-2024, https://doi.org/10.5194/acp-24-553-2024, 2024
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This study provides insights into the complex chemical composition of long-range-transported wildfire plumes from Yakutia, which underwent different levels of atmospheric processing. With complementary mass spectrometric techniques, we improve our understanding of the chemical processes and atmospheric fate of wildfire plumes. Unprecedented high levels of carbonaceous aerosols crossed the polar circle with implications for the Arctic ecosystem and consequently climate.
Qiongqiong Wang, Shuhui Zhu, Shan Wang, Cheng Huang, Yusen Duan, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 475–486, https://doi.org/10.5194/acp-24-475-2024, https://doi.org/10.5194/acp-24-475-2024, 2024
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We investigated short-term source apportionment of PM2.5 utilizing rolling positive matrix factorization (PMF) and online PM chemical speciation data, which included source-specific organic tracers collected over a period of 37 d during the winter of 2019–2020 in suburban Shanghai, China. The findings highlight that by imposing constraints on the primary source profiles, short-term PMF analysis successfully replicated both the individual primary sources and the total secondary sources.
Jiyuan Yang, Guoyang Lei, Jinfeng Zhu, Yutong Wu, Chang Liu, Kai Hu, Junsong Bao, Zitong Zhang, Weili Lin, and Jun Jin
Atmos. Chem. Phys., 24, 123–136, https://doi.org/10.5194/acp-24-123-2024, https://doi.org/10.5194/acp-24-123-2024, 2024
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The atmospheric pollution and formation mechanisms of particulate-bound alkyl nitrate in Beijing were studied. C9–C16 long-chain n-alkyl nitrates negatively correlated with O3 but positively correlated with PM2.5 and NO2, so they may not be produced during gas-phase homogeneous reactions in the photochemical process but form through reactions between alkanes and nitrates on PM surfaces. Particulate-bound n-alkyl nitrates strongly affect both haze pollution and atmospheric visibility.
Yuanyuan Qin, Xinghua Zhang, Wei Huang, Juanjuan Qin, Xiaoyu Hu, Yuxuan Cao, Tianyi Zhao, Yang Zhang, Jihua Tan, Ziyin Zhang, Xinming Wang, and Zhenzhen Wang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2703, https://doi.org/10.5194/egusphere-2023-2703, 2024
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Environmental persistent free radicals (EPFRs) and reactive oxygen species (ROS) play an active role in the atmosphere. We quantified the impact of control measures on EPFRs and ROS and found that strict control measures have effectively reduced their emissions, largely linked to a significant decrease in secondary aerosols. Our findings have great implications for further understanding the formation and sources and for developing future air quality management policies targeting EPFRs and ROS.
Lisa Azzarello, Rebecca A. Washenfelder, Michael A. Robinson, Alessandro Franchin, Caroline C. Womack, Christopher D. Holmes, Steven S. Brown, Ann Middlebrook, Tim Newberger, Colm Sweeney, and Cora J. Young
Atmos. Chem. Phys., 23, 15643–15654, https://doi.org/10.5194/acp-23-15643-2023, https://doi.org/10.5194/acp-23-15643-2023, 2023
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We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Moritz Zeising, Astrid Bracher, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 15561–15587, https://doi.org/10.5194/acp-23-15561-2023, https://doi.org/10.5194/acp-23-15561-2023, 2023
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Marine carbohydrates are produced in the surface of the ocean, enter the atmophere as part of sea spray aerosol particles, and potentially contribute to the formation of fog and clouds. Here, we present the results of a sea–air transfer study of marine carbohydrates conducted in the high Arctic. Besides a chemo-selective transfer, we observed a quick atmospheric aging of carbohydrates, possibly as a result of both biotic and abiotic processes.
Xing Wei, Yanjie Shen, Xiao-Ying Yu, Yang Gao, Huiwang Gao, Ming Chu, Yujiao Zhu, and Xiaohong Yao
Atmos. Chem. Phys., 23, 15325–15350, https://doi.org/10.5194/acp-23-15325-2023, https://doi.org/10.5194/acp-23-15325-2023, 2023
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We investigate the contribution of grown new particles to Nccn at a rural mountain site in the North China Plain. The total particle number concentrations (Ncn) observed on 8 new particle formation (NPF) days were higher compared to non-NPF days. The Nccn at 0.2 % supersaturation (SS) and 0.4 % SS on the NPF days was significantly lower than on non-NPF days. Only one of eight NPF events had detectable net contributions to Nccn at 0.4 % SS and 1.0 % SS with increased κ values.
Yuquan Gong, Ru-Jin Huang, Lu Yang, Ting Wang, Wei Yuan, Wei Xu, Wenjuan Cao, Yang Wang, and Yongjie Li
Atmos. Chem. Phys., 23, 15197–15207, https://doi.org/10.5194/acp-23-15197-2023, https://doi.org/10.5194/acp-23-15197-2023, 2023
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This study reveals the large day–night differences in brown carbon (BrC) chromophore composition, which was not known previously. The results provide insights into the effects of atmospheric processes and emissions on BrC composition.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyang Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
EGUsphere, https://doi.org/10.5194/egusphere-2023-2684, https://doi.org/10.5194/egusphere-2023-2684, 2023
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We investigated aerosol composition, sources, and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more-oxidized SOA; however, cloud evaporation leads to the production of less-oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
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Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
Xiaoxiao Li, Yijing Chen, Yuyang Li, Runlong Cai, Yiran Li, Chenjuan Deng, Jin Wu, Chao Yan, Hairong Cheng, Yongchun Liu, Markku Kulmala, Jiming Hao, James N. Smith, and Jingkun Jiang
Atmos. Chem. Phys., 23, 14801–14812, https://doi.org/10.5194/acp-23-14801-2023, https://doi.org/10.5194/acp-23-14801-2023, 2023
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Near-continuous measurements show the composition, sources, and seasonal variations of ultrafine particles (UFPs) in urban Beijing. Vehicle and cooking emissions and new particle formation are the main sources of UFPs, and aqueous/heterogeneous processes increase UFP mode diameters. UFPs are the highest in winter due to the highest primary particle emission rates and new particle formation rates, and CHO fractions are the highest in summer due to the strongest photooxidation.
Jiaqi Wang, Jian Gao, Fei Che, Xin Yang, Yuanqin Yang, Lei Liu, Yan Xiang, and Haisheng Li
Atmos. Chem. Phys., 23, 14715–14733, https://doi.org/10.5194/acp-23-14715-2023, https://doi.org/10.5194/acp-23-14715-2023, 2023
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Regional-scale observations of surface O3, PM2.5 and its major chemical species, mixing layer height (MLH), and other meteorological parameters were made in the North China Plain during summer. Unlike the cold season, synchronized increases in MDA8 O3 and PM2.5 under medium MLH conditions have been witnessed. The increasing trend of PM2.5 was associated with enhanced secondary chemical formation. The correlation between MLH and secondary air pollutants should be treated with care in hot seasons.
Takuma Miyakawa, Akinori Ito, Chunmao Zhu, Atsushi Shimizu, Erika Matsumoto, Yusuke Mizuno, and Yugo Kanaya
Atmos. Chem. Phys., 23, 14609–14626, https://doi.org/10.5194/acp-23-14609-2023, https://doi.org/10.5194/acp-23-14609-2023, 2023
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This study conducted semi-continuous measurements of PM2.5 aerosols and their elemental composition in western Japan, during spring 2018. It analyzed the emissions, transport, and wet removal of elements such as Pb, Cu, Fe, and Mn. It also assessed the accuracy of modeled concentrations and found overestimations of BC and underestimations of Cu and anthropogenic Fe in East Asia. Insights into emissions, removals, and source apportionment of trace metals in the East Asian outflow were provided.
Jingjing Meng, Yachen Wang, Yuanyuan Li, Tonglin Huang, Zhifei Wang, Yiqiu Wang, Min Chen, Zhanfang Hou, Houhua Zhou, Keding Lu, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 23, 14481–14503, https://doi.org/10.5194/acp-23-14481-2023, https://doi.org/10.5194/acp-23-14481-2023, 2023
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This study investigated the effect of COVID-19 lockdown (LCD) measures on the formation and evolutionary process of diacids and related compounds from field observations. Results demonstrate that more aged organic aerosols are observed during the LCD due to the enhanced photochemical oxidation. Our study also found that the reactivity of 13C was higher than that of 12C in the gaseous photochemical oxidation, leading to higher δ13C values of C2 during the LCD than before the LCD.
Christopher J. Hennigan, Michael McKee, Vikram Pratap, Bryanna Boegner, Jasper Reno, Lucia Garcia, Madison McLaren, and Sara M. Lance
Atmos. Chem. Phys., 23, 14437–14449, https://doi.org/10.5194/acp-23-14437-2023, https://doi.org/10.5194/acp-23-14437-2023, 2023
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This study characterized the optical properties of light-absorbing organic compounds, called brown carbon (BrC), in atmospheric cloud water samples. In all samples, light absorption by BrC increased linearly with increasing pH. There was variability in the sensitivity of the absorption–pH relationship, depending on the degree of influence from fire emissions. Overall, these results show that the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.
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Short summary
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.
The mechanisms by which specific anthropogenic pollutants enhance isoprene SOA in ambient PM2.5...
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