Articles | Volume 16, issue 14
https://doi.org/10.5194/acp-16-9003-2016
© 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-16-9003-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
22 Jul 2016
Research article |
| 22 Jul 2016
Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments
Sara D. Forestieri
Department of Civil and Environmental Engineering, University of
California, Davis, CA 95616, USA
Gavin C. Cornwell
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Taylor M. Helgestad
Department of Civil and Environmental Engineering, University of
California, Davis, CA 95616, USA
Kathryn A. Moore
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Christopher Lee
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Gordon A. Novak
Department of Chemistry, University of Wisconsin, Madison, WI 53706, USA
Camille M. Sultana
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Xiaofei Wang
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Timothy H. Bertram
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Department of Chemistry, University of Wisconsin, Madison, WI 53706, USA
Kimberly A. Prather
Department of Chemistry and Biochemistry, University of California,
San Diego, La Jolla, CA 92093, USA
Scripps Institution of Oceanography, 9500 Gilman Drive, La Jolla, CA
92093, USA
Department of Civil and Environmental Engineering, University of
California, Davis, CA 95616, USA
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Charlotte M. Beall, Jennifer M. Michaud, Meredith A. Fish, Julie Dinasquet, Gavin C. Cornwell, M. Dale Stokes, Michael D. Burkart, Thomas C. Hill, Paul J. DeMott, and Kimberly A. Prather
Atmos. Chem. Phys., 21, 9031–9045, https://doi.org/10.5194/acp-21-9031-2021, https://doi.org/10.5194/acp-21-9031-2021, 2021
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Ice-nucleating particles (INPs) can influence multiple climate-relevant cloud properties by triggering droplet freezing at relative humidities below or temperatures above the freezing point of water. The ocean is a significant INP source; however, the specific identities of marine INPs remain largely unknown. Here, we identify 14 ice-nucleating microbes from aerosol and precipitation samples collected at a coastal site in southern California, two or more of which are likely marine.
Charlotte M. Beall, Dolan Lucero, Thomas C. Hill, Paul J. DeMott, M. Dale Stokes, and Kimberly A. Prather
Atmos. Meas. Tech., 13, 6473–6486, https://doi.org/10.5194/amt-13-6473-2020, https://doi.org/10.5194/amt-13-6473-2020, 2020
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Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Gordon A. Novak, Michael P. Vermeuel, and Timothy H. Bertram
Atmos. Meas. Tech., 13, 1887–1907, https://doi.org/10.5194/amt-13-1887-2020, https://doi.org/10.5194/amt-13-1887-2020, 2020
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Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
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We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
Crystal D. McClure, Christopher Y. Lim, David H. Hagan, Jesse H. Kroll, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 1531–1547, https://doi.org/10.5194/acp-20-1531-2020, https://doi.org/10.5194/acp-20-1531-2020, 2020
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We characterized various optical, chemical, and physical properties of particles produced from combustion of a variety of different biomass fuels, many representative of those found in the western US. We find that many properties scale with the ratio between bulk average organic aerosol and black carbon mass concentrations, although there are some properties that do not.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
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.
Ingeborg E. Nielsen, Henrik Skov, Andreas Massling, Axel C. Eriksson, Manuel Dall'Osto, Heikki Junninen, Nina Sarnela, Robert Lange, Sonya Collier, Qi Zhang, Christopher D. Cappa, and Jacob K. Nøjgaard
Atmos. Chem. Phys., 19, 10239–10256, https://doi.org/10.5194/acp-19-10239-2019, https://doi.org/10.5194/acp-19-10239-2019, 2019
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Measurements of the chemical composition of sub-micrometer aerosols were carried out in northern Greenland during the Arctic haze (February–May) where concentrations are high due to favorable conditions for long-range transport. Sulfate was the dominant aerosol (66 %), followed by organic matter (24 %). The highest black carbon concentrations where observed in February. Source apportionment yielded three factors: a primary factor (12 %), an Arctic haze factor (64 %) and a marine factor (22 %).
Samuel A. Atwood, Sonia M. Kreidenweis, Paul J. DeMott, Markus D. Petters, Gavin C. Cornwell, Andrew C. Martin, and Kathryn A. Moore
Atmos. Chem. Phys., 19, 6931–6947, https://doi.org/10.5194/acp-19-6931-2019, https://doi.org/10.5194/acp-19-6931-2019, 2019
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This paper presents measurements of aerosol particles at a coastal location. The particles were classified into distinct aerosol types using both microphysical measurements and meteorological information, allowing rapid changes between the aerosol types to be reliably identified. These particles can alter cloud and precipitation processes, and inclusion of the differences between types can improve atmospheric models and remote sensing retrievals in littoral zones.
Ali Akherati, Christopher D. Cappa, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, Stephen M. Griffith, Sebastien Dusanter, Philip S. Stevens, and Shantanu H. Jathar
Atmos. Chem. Phys., 19, 4561–4594, https://doi.org/10.5194/acp-19-4561-2019, https://doi.org/10.5194/acp-19-4561-2019, 2019
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Unburned and partially burned organic compounds emitted from fossil fuel and biomass combustion can react in the atmosphere in the presence of sunlight to form particles. In this work, we use an air pollution model to examine the influence of these organic compounds released by motor vehicles and fires on fine particle pollution in southern California.
Andrew C. Martin, Gavin Cornwell, Charlotte M. Beall, Forest Cannon, Sean Reilly, Bas Schaap, Dolan Lucero, Jessie Creamean, F. Martin Ralph, Hari T. Mix, and Kimberly Prather
Atmos. Chem. Phys., 19, 4193–4210, https://doi.org/10.5194/acp-19-4193-2019, https://doi.org/10.5194/acp-19-4193-2019, 2019
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Aerosols that promote ice formation in clouds were investigated during an atmospheric river that caused significant rain in northern California. We found that biological particles produced by local terrestrial ecosystems greatly enhanced cloud ice when meteorology allowed for their injection to the storm. The local terrestrial particles had greater impact on clouds than particles transported from across the Pacific Ocean, lending additional insight to which aerosols are important for cloud ice.
Ziyue Li, Katherine A. Smith, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 14585–14608, https://doi.org/10.5194/acp-18-14585-2018, https://doi.org/10.5194/acp-18-14585-2018, 2018
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We investigated the influence of relative humidity (RH) on the heterogeneous oxidation of secondary organic aerosol (SOA) particles by OH radicals. We observed significantly faster volume loss and compositional change of SOA at high RH, showing that viscosity differences determine compositional changes, but variability in either the uptake coefficient or the fragmentation probability are required to explain the difference in volume loss between low and high RH.
Sailaja Eluri, Christopher D. Cappa, Beth Friedman, Delphine K. Farmer, and Shantanu H. Jathar
Atmos. Chem. Phys., 18, 13813–13838, https://doi.org/10.5194/acp-18-13813-2018, https://doi.org/10.5194/acp-18-13813-2018, 2018
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As oxidation flow reactors (OFRs) are increasingly used to study aerosol formation and evolution in laboratory and field environments, there is a need to develop models that can be used to interpret OFR data. In this work, we evaluate two coupled chemistry and thermodynamic models to simulate secondary organic aerosol formation (SOA) from diluted diesel exhaust and explore the sources, pathways, and processes important to SOA formation.
Sara D. Forestieri, Taylor M. Helgestad, Andrew T. Lambe, Lindsay Renbaum-Wolff, Daniel A. Lack, Paola Massoli, Eben S. Cross, Manvendra K. Dubey, Claudio Mazzoleni, Jason S. Olfert, Arthur J. Sedlacek III, Andrew Freedman, Paul Davidovits, Timothy B. Onasch, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 12141–12159, https://doi.org/10.5194/acp-18-12141-2018, https://doi.org/10.5194/acp-18-12141-2018, 2018
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We characterized optical properties of flame-derived black carbon particles and interpret our observations through the use of Mie theory and Rayleigh–Debye–Gans theory. We determined that the mass absorption coefficient is independent of particle collapse and use this to derive theory- and wavelength-specific refractive indices for black carbon (BC). We demonstrate the inadequacy of Mie theory and suggest an alternative approach for atmospheric models to better represent light absorption by BC.
Sara D. Forestieri, Sean M. Staudt, Thomas M. Kuborn, Katharine Faber, Christopher R. Ruehl, Timothy H. Bertram, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, https://doi.org/10.5194/acp-18-10985-2018, 2018
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Our work establishes how surface tension reduction influences droplet growth and activation of simple sea spray mimics (NaCl coated with fatty acids). Fatty acids can substantially reduce droplet surface tension near activation but have limited impact on activation. Coating of NaCl by palmitic acid (a wax) impedes water uptake, but this impedance is removed if oleic acid (a liquid) is mixed in. The properties that surface-active compounds need to impact activation are theoretically examined.
Avi Lavi, Michael P. Vermeuel, Gordon A. Novak, and Timothy H. Bertram
Atmos. Meas. Tech., 11, 3251–3262, https://doi.org/10.5194/amt-11-3251-2018, https://doi.org/10.5194/amt-11-3251-2018, 2018
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Chemical ionization mass spectrometry has emerged as a versatile tool for the study of reactive gases. Robust calibration is required to assess the sensitivity of these instruments and their dependence on external factors such as specific humidity. Here, we report the sensitivity of benzene cluster cation chemical ionization for an array of terpene compounds. This work permits a more universal understanding of the sensitivity of this technique to a host of isobaric compounds.
Dean B. Atkinson, Mikhail Pekour, Duli Chand, James G. Radney, Katheryn R. Kolesar, Qi Zhang, Ari Setyan, Norman T. O'Neill, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 5499–5514, https://doi.org/10.5194/acp-18-5499-2018, https://doi.org/10.5194/acp-18-5499-2018, 2018
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We use in situ measurements of particle light extinction to assess the performance of a typical aerosol remote retrieval method. The retrieved fine-mode fraction of extinction, a property commonly used to characterize the anthropogenic influence on the aerosol optical depth, compares well with the in situ measurements as does the retrieved effective fine-mode radius, which characterizes the average size of the particles that contribute most to scattering.
Alex K. Y. Lee, Chia-Li Chen, Jun Liu, Derek J. Price, Raghu Betha, Lynn M. Russell, Xiaolu Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 15055–15067, https://doi.org/10.5194/acp-17-15055-2017, https://doi.org/10.5194/acp-17-15055-2017, 2017
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Understanding the mixing state of ambient black carbon (BC) and the chemical characteristics of its associated coatings is important to evaluate BC fate and environmental impacts. This study reports fresh secondary organic aerosol (SOA) formation near traffic emissions during daytime. Our observations suggest that BC was unlikely the major condensation sink of SOA, and a portion of SOA condensed on BC surface was chemically different from other SOA particles that were externally mixed with BC.
Gouri Prabhakar, Caroline L. Parworth, Xiaolu Zhang, Hwajin Kim, Dominique E. Young, Andreas J. Beyersdorf, Luke D. Ziemba, John B. Nowak, Timothy H. Bertram, Ian C. Faloona, Qi Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 14747–14770, https://doi.org/10.5194/acp-17-14747-2017, https://doi.org/10.5194/acp-17-14747-2017, 2017
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This work assesses the processes that control the ambient concentrations of particulate nitrate in the the wintertime San Joaquin Valley of California through a combination of aircraft and surface measurements made during the DISCOVER-AQ study. We provide an observational demonstration of how nocturnal production and advection in aloft layers combines with daytime production and loss from entrainment and deposition to give rise to a distinct diurnal profile in surface nitrate concentrations.
Charlotte M. Beall, M. Dale Stokes, Thomas C. Hill, Paul J. DeMott, Jesse T. DeWald, and Kimberly A. Prather
Atmos. Meas. Tech., 10, 2613–2626, https://doi.org/10.5194/amt-10-2613-2017, https://doi.org/10.5194/amt-10-2613-2017, 2017
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Ice nucleating particles (INPs) influence cloud properties and can affect the overall precipitation efficiency. An existing technique for measuring INP
concentrations is modified and automated, and heat transfer properties of the INP measurement technique are characterized for the first time using
a finite-element-analysis-based heat transfer simulation to improve accuracy of INP freezing temperature measurement.
Jianlin Hu, Shantanu Jathar, Hongliang Zhang, Qi Ying, Shu-Hua Chen, Christopher D. Cappa, and Michael J. Kleeman
Atmos. Chem. Phys., 17, 5379–5391, https://doi.org/10.5194/acp-17-5379-2017, https://doi.org/10.5194/acp-17-5379-2017, 2017
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Organic aerosol is a major constituent of ultrafine particulate matter (PM0.1). In this study, a source-oriented air quality model was used to simulate the concentrations and sources of primary and secondary organic aerosols in PM0.1 in California for a 9-year modeling period to provide useful information for epidemiological studies to further investigate the associations with health outcomes.
Camille M. Sultana, Gavin C. Cornwell, Paul Rodriguez, and Kimberly A. Prather
Atmos. Meas. Tech., 10, 1323–1334, https://doi.org/10.5194/amt-10-1323-2017, https://doi.org/10.5194/amt-10-1323-2017, 2017
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Single-particle mass spectrometers (SPMSs) can determine the size and chemical composition of single particles in real time. We developed the first open-source SPMS toolkit to allow creative script-based data mining along with GUI-based visual data exploration and calibration all within a single programming environment. We believe that this software will be adopted by many in the SPMS community and improve the efficiency of knowledge discovery from these atmospherically critical data sets.
Andrew C. Martin, Gavin C. Cornwell, Samuel A. Atwood, Kathryn A. Moore, Nicholas E. Rothfuss, Hans Taylor, Paul J. DeMott, Sonia M. Kreidenweis, Markus D. Petters, and Kimberly A. Prather
Atmos. Chem. Phys., 17, 1491–1509, https://doi.org/10.5194/acp-17-1491-2017, https://doi.org/10.5194/acp-17-1491-2017, 2017
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Anthropogenic influence on air quality, aerosol properties, and cloud activity was observed at Bodega Bay, CA, during periods when air from California's interior was transported to the coast. The sudden change in aerosol properties can impact atmospheric radiative balance and cloud formation in ways that must be accounted for in regional climate simulations.
M. Dale Stokes, Grant Deane, Douglas B. Collins, Christopher Cappa, Timothy Bertram, Abigail Dommer, Steven Schill, Sara Forestieri, and Mathew Survilo
Atmos. Meas. Tech., 9, 4257–4267, https://doi.org/10.5194/amt-9-4257-2016, https://doi.org/10.5194/amt-9-4257-2016, 2016
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A small breaking wave and foam simulator has been fabricated that allows the continuous analysis of the produced marine aerosols. Based on the original Marine Aerosol Reference Tank (MART) the miniature version allows the culturing of delicate planktonic organisms because it operates without a large, sheer-inducing pump. This allows the study of marine aerosol production and the effects of biologically controlled seawater chemistry under controlled and repeatable experimental conditions.
Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
Atmos. Chem. Phys., 16, 7917–7941, https://doi.org/10.5194/acp-16-7917-2016, https://doi.org/10.5194/acp-16-7917-2016, 2016
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The global budget and spatial distribution of secondary organic aerosol (SOA) are highly uncertain in chemistry-climate models, which reflects our inability to characterize all phases of the OA lifecycle. We have performed global model simulations with the newly proposed formation and removal processes (photolysis and heterogeneous chemistry) and shown that SOA is a far more dynamic system, with 4 times stronger production rates and more efficient removal mechanisms, than assumed in models.
Christopher D. Cappa, Katheryn R. Kolesar, Xiaolu Zhang, Dean B. Atkinson, Mikhail S. Pekour, Rahul A. Zaveri, Alla Zelenyuk, and Qi Zhang
Atmos. Chem. Phys., 16, 6511–6535, https://doi.org/10.5194/acp-16-6511-2016, https://doi.org/10.5194/acp-16-6511-2016, 2016
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Measurements of size-dependent aerosol optical properties at visible wavelengths made during the 2010 CARES study are reported on, with a special focus on the characterization of supermicron particles. The relationships with and dependence upon particle composition, particle size, photochemical aging, water uptake and heating are discussed, along with broader implications of these in situ measurements for the interpretation of remote sensing products.
Dominique E. Young, Hwajin Kim, Caroline Parworth, Shan Zhou, Xiaolu Zhang, Christopher D. Cappa, Roger Seco, Saewung Kim, and Qi Zhang
Atmos. Chem. Phys., 16, 5427–5451, https://doi.org/10.5194/acp-16-5427-2016, https://doi.org/10.5194/acp-16-5427-2016, 2016
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Aerosol chemistry and the sources and processes driving the observed temporal and diurnal variations of PM were studied in a polluted urban environment during winter 2013. These results were compared to a similar campaign from winter 2010. Meteorology strongly influenced PM composition, both directly and indirectly. Nighttime reactions played a more important role in 2013 and the influence from a nighttime formed residual layer that mixed down in the morning was also much more intense in 2013.
Michelle J. Kim, Matthew C. Zoerb, Nicole R. Campbell, Kathryn J. Zimmermann, Byron W. Blomquist, Barry J. Huebert, and Timothy H. Bertram
Atmos. Meas. Tech., 9, 1473–1484, https://doi.org/10.5194/amt-9-1473-2016, https://doi.org/10.5194/amt-9-1473-2016, 2016
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Benzene cluster cations were revisited as a sensitive and selective reagent ion for the chemical ionization of dimethyl sulfide (DMS) and a select group of volatile organic compounds (VOCs). Laboratory and field measurements were used to assess the sensitivity of the ionization scheme under a wide array of operating condition. Underway measurements of DMS in the North Atlantic were validated against an atmospheric pressure ionization mass spectrometer.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Atmos. Chem. Phys., 16, 2309–2322, https://doi.org/10.5194/acp-16-2309-2016, https://doi.org/10.5194/acp-16-2309-2016, 2016
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Multi-generational chemistry schemes applied in regional models do not increase secondary organic aerosol (SOA) mass production relative to traditional "two-product" schemes when both models are fitted to the same chamber data. The multi-generational chemistry schemes do change the predicted composition of SOA and the source attribution of SOA.
K. R. Kolesar, C. Chen, D. Johnson, and C. D. Cappa
Atmos. Chem. Phys., 15, 9327–9343, https://doi.org/10.5194/acp-15-9327-2015, https://doi.org/10.5194/acp-15-9327-2015, 2015
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Secondary organic aerosol from the dark ozonolysis of α‑pinene was formed at a range of mass loadings from 1 to 800μg m-3. The amount of mass loss during evaporation in a thermodenuder was found to be independent of mass loading. A kinetic model of evaporation was fit to the observations and good agreement was obtained when the particle was either composed of dimers that decompose into semi-volatile monomers or when it was composed of low-volatility compounds that evaporate directly.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, https://doi.org/10.5194/gmd-8-2553-2015, 2015
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Multi-generational oxidation of organic vapors can significantly alter the mass, chemical composition and properties of secondary organic aerosol (SOA). Here, we implement a semi-explicit, constrained multi-generational oxidation model of Cappa and Wilson (2012) in a 3-D air quality model. When compared with results from a current-generation SOA model, we predict similar mass concentrations of SOA but a different chemical composition. O:C ratios of SOA are in line with those measured globally.
J. M. Creamean, A. P. Ault, A. B. White, P. J. Neiman, F. M. Ralph, P. Minnis, and K. A. Prather
Atmos. Chem. Phys., 15, 6535–6548, https://doi.org/10.5194/acp-15-6535-2015, https://doi.org/10.5194/acp-15-6535-2015, 2015
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Aerosols impact how clouds and precipitation form. In the California Sierra Nevada, we found that the formation and resulting amount of rain and snow were impacted by mineral dust, bioparticles such as bacteria, and biomass burning and pollution particles during three winter seasons. Dust and bioparticles from distant sources impacted high-altitude clouds by forming ice, leading to more precipitation, whereas local biomass burning and pollution entered the base of clouds, leading to less rain.
D. B. Atkinson, J. G. Radney, J. Lum, K. R. Kolesar, D. J. Cziczo, M. S. Pekour, Q. Zhang, A. Setyan, A. Zelenyuk, and C. D. Cappa
Atmos. Chem. Phys., 15, 4045–4061, https://doi.org/10.5194/acp-15-4045-2015, https://doi.org/10.5194/acp-15-4045-2015, 2015
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This work describes an analysis of measurements of the influence of water uptake on the light-scattering properties of sub- and supermicron-sized particles as observed in the Sacramento, CA, USA region during the 2010 CARES field campaign. The observations are used to derive campaign-average effective hygroscopicity parameters for submicron oxygenated organic aerosol and for supermicron particles, and the influence of chloride displacement reactions on particle hygroscopicity is examined.
D. B. Collins, D. F. Zhao, M. J. Ruppel, O. Laskina, J. R. Grandquist, R. L. Modini, M. D. Stokes, L. M. Russell, T. H. Bertram, V. H. Grassian, G. B. Deane, and K. A. Prather
Atmos. Meas. Tech., 7, 3667–3683, https://doi.org/10.5194/amt-7-3667-2014, https://doi.org/10.5194/amt-7-3667-2014, 2014
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Sea spray aerosol particles represent a system of relatively high chemical complexity. The chemical composition of sea spray aerosol particles was shown in this study to be directly determined by the method used to produce bubbles, which produce aerosol upon bursting at the sea surface. Using methods which deviate from natural breaking waves directly translated into differences in the measured particle sizes and the chemical mixing state of laboratory-generated sea spray aerosol particles.
G. M. Buffaloe, D. A. Lack, E. J. Williams, D. Coffman, K. L. Hayden, B. M. Lerner, S.-M. Li, I. Nuaaman, P. Massoli, T. B. Onasch, P. K. Quinn, and C. D. Cappa
Atmos. Chem. Phys., 14, 1881–1896, https://doi.org/10.5194/acp-14-1881-2014, https://doi.org/10.5194/acp-14-1881-2014, 2014
C. D. Cappa, E. J. Williams, D. A. Lack, G. M. Buffaloe, D. Coffman, K. L. Hayden, S. C. Herndon, B. M. Lerner, S.-M. Li, P. Massoli, R. McLaren, I. Nuaaman, T. B. Onasch, and P. K. Quinn
Atmos. Chem. Phys., 14, 1337–1352, https://doi.org/10.5194/acp-14-1337-2014, https://doi.org/10.5194/acp-14-1337-2014, 2014
J. Fan, L. R. Leung, P. J. DeMott, J. M. Comstock, B. Singh, D. Rosenfeld, J. M. Tomlinson, A. White, K. A. Prather, P. Minnis, J. K. Ayers, and Q. Min
Atmos. Chem. Phys., 14, 81–101, https://doi.org/10.5194/acp-14-81-2014, https://doi.org/10.5194/acp-14-81-2014, 2014
A. Cazorla, R. Bahadur, K. J. Suski, J. F. Cahill, D. Chand, B. Schmid, V. Ramanathan, and K. A. Prather
Atmos. Chem. Phys., 13, 9337–9350, https://doi.org/10.5194/acp-13-9337-2013, https://doi.org/10.5194/acp-13-9337-2013, 2013
T. H. Bertram, A. E. Perring, P. J. Wooldridge, J. Dibb, M. A. Avery, and R. C. Cohen
Atmos. Chem. Phys., 13, 4617–4630, https://doi.org/10.5194/acp-13-4617-2013, https://doi.org/10.5194/acp-13-4617-2013, 2013
M. D. Stokes, G. B. Deane, K. Prather, T. H. Bertram, M. J. Ruppel, O. S. Ryder, J. M. Brady, and D. Zhao
Atmos. Meas. Tech., 6, 1085–1094, https://doi.org/10.5194/amt-6-1085-2013, https://doi.org/10.5194/amt-6-1085-2013, 2013
C. D. Cappa, X. Zhang, C. L. Loza, J. S. Craven, L. D. Yee, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 1591–1606, https://doi.org/10.5194/acp-13-1591-2013, https://doi.org/10.5194/acp-13-1591-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photooxidation: Remarkably enhancing effects of seeds and ammonia
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Technical note: High-resolution analyses of concentrations and sizes of black carbon particles deposited on northwest Greenland over the past 350 years – Part 1. Continuous flow analysis of the SIGMA-D ice core using a Wide-Range Single-Particle Soot Photometer and a high-efficiency nebulizer
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
The impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Technical note: Improved synthetic routes to cis- and trans-(2-methyloxirane-2,3-diyl)dimethanol (cis- and trans-β-isoprene epoxydiol)
Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
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This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Si Zhang, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2119, https://doi.org/10.5194/egusphere-2024-2119, 2024
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SOA from acetone photooxidation can be formed more readily on neutral aerosols than on acidic aerosols, while heterogeneous reaction of carbonyl with ammonium is only active on acidic aerosols in the presence of NH3, which produces light-absorbing N-containing compounds. Our work suggested that the heterogeneous oxidation of highly volatile VOC, for example acetone, is an importance source of SOA in the atmosphere, which should be accounted for in the future model studies.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
EGUsphere, https://doi.org/10.5194/egusphere-2024-1496, https://doi.org/10.5194/egusphere-2024-1496, 2024
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We developed a continuous flow analysis system to analyse an ice core from northwest Greenland, and coupled it with an improved BC measurement technique. This coupling allowed accurate high-resolution analyses of BC particles' size distributions and concentrations with diameters between 70 nm and 4 μm for the past 350 years. Our results provide crucial insights into BC's climatic effects. We also found that previous ice core studies substantially underestimated the BC mass concentrations.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
EGUsphere, https://doi.org/10.5194/egusphere-2024-905, https://doi.org/10.5194/egusphere-2024-905, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate & fructose) during humidity change & ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact on water uptake & chemical reactivity affecting atmospheric lifetimes, urban air quality (protecting harmful emissions from degradation and enabling their long-range transport) & climate (affecting cloud formation) with implications for human health.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
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Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
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The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
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.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
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The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
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Short summary
Hygroscopic growth factors at 85 % relative humidity (GF(85 %)) were quantified along with particle composition for primary sea spray aerosol (SSA) particles generated in marine aerosol reference tanks (MARTs) from seawater in which two independent phytoplankton blooms were induced. The observed 5 to 15 % depression in the GF(85 %) values (relative to pure sea salt) is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM) comprising the SSA.
Hygroscopic growth factors at 85 % relative humidity (GF(85 %)) were quantified along with...
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