Articles | Volume 18, issue 19
https://doi.org/10.5194/acp-18-14585-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-14585-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Oct 2018
Research article |
| 11 Oct 2018
| 11 Oct 2018
Influence of relative humidity on the heterogeneous oxidation of secondary organic aerosol
Atmospheric Sciences Graduate Group, University of California, Davis,
USA
Katherine A. Smith
Dept. of Civil and Environmental Engineering, University of
California, Davis, USA
Dept. of Civil and Environmental Engineering, University of
California, Davis, USA
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Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
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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.
Jianlin Hu, Shantanu Jathar, Hongliang Zhang, Qi Ying, Shu-Hua Chen, Christopher D. Cappa, and Michael J. Kleeman
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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.
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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.
Sara D. Forestieri, Gavin C. Cornwell, Taylor M. Helgestad, Kathryn A. Moore, Christopher Lee, Gordon A. Novak, Camille M. Sultana, Xiaofei Wang, Timothy H. Bertram, Kimberly A. Prather, and Christopher D. Cappa
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Alma Hodzic, Prasad S. Kasibhatla, Duseong S. Jo, Christopher D. Cappa, Jose L. Jimenez, Sasha Madronich, and Rokjin J. Park
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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.
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.
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.
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
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)
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
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
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
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
Photoenhanced sulfates formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
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
Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime
Formation of highly oxygenated organic molecules from the oxidation of limonene by OH radical: significant contribution of H-abstraction pathway
Measurement report: Atmospheric aging of combustion-derived particles – impact on stable free radical concentration and its ability to produce reactive oxygen species in aqueous media
Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants
An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles
Simultaneous formation of sulfate and nitrate via co-uptake of SO2 and NO2 by aqueous NaCl droplets: combined effect of nitrate photolysis and chlorine chemistry
Photo-induced shrinking of aqueous glycine aerosol droplets
Sulfate formation via aerosol-phase SO2 oxidation by model biomass burning photosensitizers: 3,4-dimethoxybenzaldehyde, vanillin and syringaldehyde using single-particle mixing-state analysis
Yields and molecular composition of gas-phase and secondary organic aerosol from the photooxidation of the volatile consumer product benzyl alcohol: formation of highly oxygenated and hydroxy nitro-aromatic compounds
A combined gas- and particle-phase analysis of highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis
Comparison of aqueous secondary organic aerosol (aqSOA) product distributions from guaiacol oxidation by non-phenolic and phenolic methoxybenzaldehydes as photosensitizers in the absence and presence of ammonium nitrate
Technical note: Chemical composition and source identification of fluorescent components in atmospheric water-soluble brown carbon by excitation–emission matrix spectroscopy with parallel factor analysis – potential limitations and applications
Insoluble lipid film mediates transfer of soluble saccharides from the sea to the atmosphere: the role of hydrogen bonding
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.
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.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
EGUsphere, https://doi.org/10.5194/egusphere-2023-2657, https://doi.org/10.5194/egusphere-2023-2657, 2023
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Cooking is one of the major particle sources in urban areas. Previous laboratory studies demonstrated the chemical lifetimes of cooking organic aerosols 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.
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.
Chong Han, Jiawei Ma, Wangjin Yang, and Hongxing Yang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1273, https://doi.org/10.5194/egusphere-2023-1273, 2023
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We provide direct evidences that light prominently enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where 3SO2 can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. It is suggested that the SO2 photochemistry on non-photoactive mineral dust significantly contributes to sulfates, highlighting previously unknown pathway to better explain the missing sources of atmospheric sulfates.
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.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Hao Luo, Luc Vereecken, Hongru Shen, Sungah Kang, Iida Pullinen, Mattias Hallquist, Hendrik Fuchs, Andreas Wahner, Astrid Kiendler-Scharr, Thomas F. Mentel, and Defeng Zhao
Atmos. Chem. Phys., 23, 7297–7319, https://doi.org/10.5194/acp-23-7297-2023, https://doi.org/10.5194/acp-23-7297-2023, 2023
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Oxidation of limonene, an element emitted by trees and chemical products, by OH, a daytime oxidant, forms many highly oxygenated organic molecules (HOMs), including C10-20 compounds. HOMs play an important role in new particle formation and growth. HOM formation can be explained by the chemistry of peroxy radicals. We found that a minor branching ratio initial pathway plays an unexpected, significant role. Considering this pathway enables accurate simulations of HOMs and other concentrations.
Heather L. Runberg and Brian J. Majestic
Atmos. Chem. Phys., 23, 7213–7223, https://doi.org/10.5194/acp-23-7213-2023, https://doi.org/10.5194/acp-23-7213-2023, 2023
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Environmentally persistent free radicals (EPFRs) are an emerging pollutant found in soot particles. Understanding how these change as they move through the atmosphere is important to human health. Here, soot was generated in the laboratory and exposed to simulated sunlight. The concentrations and characteristics of EPFRs in the soot were measured and found to be unchanged. However, it was also found that the ability of soot to form hydroxyl radicals was stronger for fresh soot.
Wenqing Jiang, Christopher Niedek, Cort Anastasio, and Qi Zhang
Atmos. Chem. Phys., 23, 7103–7120, https://doi.org/10.5194/acp-23-7103-2023, https://doi.org/10.5194/acp-23-7103-2023, 2023
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We studied how aqueous-phase secondary organic aerosol (aqSOA) form and evolve from a phenolic carbonyl commonly present in biomass burning smoke. The composition and optical properties of the aqSOA are significantly affected by photochemical reactions and are dependent on the oxidants' concentration and identity in water. During photoaging, the aqSOA initially becomes darker, but prolonged aging leads to the formation of volatile products, resulting in significant mass loss and photobleaching.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Ruifeng Zhang and Chak Keung Chan
Atmos. Chem. Phys., 23, 6113–6126, https://doi.org/10.5194/acp-23-6113-2023, https://doi.org/10.5194/acp-23-6113-2023, 2023
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Research into sulfate and nitrate formation from co-uptake of NO2 and SO2, especially under irradiation, is rare. We studied the co-uptake of NO2 and SO2 by NaCl droplets under various conditions, including irradiation and dark, and RHs, using Raman spectroscopy flow cell and kinetic model simulation. Significant nitrate formation from NO2 hydrolysis can be photolyzed to generate OH radicals that can further react with chloride to produce reactive chlorine species and promote sulfate formation.
Shinnosuke Ishizuka, Oliver Reich, Grégory David, and Ruth Signorell
Atmos. Chem. Phys., 23, 5393–5402, https://doi.org/10.5194/acp-23-5393-2023, https://doi.org/10.5194/acp-23-5393-2023, 2023
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Photosensitizers play an important role in the photochemistry of atmospheric aerosols. Our study provides evidence that mesoscopic glycine clusters forming in aqueous droplets act as unconventional photosensitizers in the visible light spectrum. We observed the influence of these photoactive molecular aggregates in single optically trapped aqueous droplets. Such mesoscopic photosensitizers might be more important for aerosol photochemistry than previously anticipated.
Liyuan Zhou, Zhancong Liang, Beatrix Rosette Go Mabato, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, and Chak K. Chan
Atmos. Chem. Phys., 23, 5251–5261, https://doi.org/10.5194/acp-23-5251-2023, https://doi.org/10.5194/acp-23-5251-2023, 2023
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This study reveals the sulfate formation in photosensitized particles from biomass burning under UV and SO2, of which the relative atmospheric importance in sulfate production was qualitatively compared to nitrate photolysis. On the basis of single-particle aerosol mass spectrometry measurements, the number percentage of sulfate-containing particles and relative peak area of sulfate in single-particle spectra exhibited a descending order of 3,4-dimethoxybenzaldehyde > vanillin > syringaldehyde.
Mohammed Jaoui, Kenneth S. Docherty, Michael Lewandowski, and Tadeusz E. Kleindienst
Atmos. Chem. Phys., 23, 4637–4661, https://doi.org/10.5194/acp-23-4637-2023, https://doi.org/10.5194/acp-23-4637-2023, 2023
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VCPs are a class of chemicals widely used in industrial and consumer products (e.g., coatings, adhesives, inks, personal care products) and are an important component of total VOCs in urban atmospheres. This study provides SOA yields and detailed chemical analysis of the gas- and aerosol-phase products of the photooxidation of one of these VCPs, benzyl alcohol. These results will allow better links between characterized sources and their resulting criteria for pollutant formation.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Beatrix Rosette Go Mabato, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak K. Chan
Atmos. Chem. Phys., 23, 2859–2875, https://doi.org/10.5194/acp-23-2859-2023, https://doi.org/10.5194/acp-23-2859-2023, 2023
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We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud and fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings are useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA predictive models.
Tao Cao, Meiju Li, Cuncun Xu, Jianzhong Song, Xingjun Fan, Jun Li, Wanglu Jia, and Ping'an Peng
Atmos. Chem. Phys., 23, 2613–2625, https://doi.org/10.5194/acp-23-2613-2023, https://doi.org/10.5194/acp-23-2613-2023, 2023
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This work comprehensively investigated the fluorescence data of light-absorbing organic compounds, water-soluble organic matter in different types of aerosol samples, soil dust, and fulvic and humic acids using an excitation–emission matrix (EEM) method and parallel factor modeling. The results revealed which light-absorbing species can be detected by EEM and also provided important information for identifying the chemical composition and possible sources of these species in atmospheric samples.
Minglan Xu, Narcisse Tsona Tchinda, Jianlong Li, and Lin Du
Atmos. Chem. Phys., 23, 2235–2249, https://doi.org/10.5194/acp-23-2235-2023, https://doi.org/10.5194/acp-23-2235-2023, 2023
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The promotion of soluble saccharides on sea spray aerosol (SSA) generation and the changes in particle morphology were observed. On the contrary, the coexistence of surface insoluble fatty acid film and soluble saccharides significantly inhibited the production of SSA. This is the first demonstration that hydrogen bonding mediated by surface-insoluble fatty acids contributes to saccharide transfer in seawater, providing a new mechanism for saccharide enrichment in SSA.
Cited articles
Arangio, A. M., Slade, J. H., Berkemeier, T., Pöschl, U., Knopf, D. A., and
Shiraiwa, M.: Multiphase chemical kinetics of OH radical uptake by molecular
organic markers of biomass burning aerosols: humidity and temperature
dependence, surface reaction, and bulk diffusion, J. Phys. Chem. A, 119,
4533–4544, https://doi.org/10.1021/jp510489z, 2015.
Bateman, A. P., Bertram, A. K., and Martin, S. T.: Hygroscopic Influence on
the Semisolid-to-Liquid Transition of Secondary Organic Materials, J.
Phys. Chem. A, 119, 4386–4395,
https://doi.org/10.1021/jp508521c, 2015.
Camredon, M., Hamilton, J. F., Alam, M. S., Wyche, K. P., Carr, T., White, I.
R., Monks, P. S., Rickard, A. R., and Bloss, W. J.: Distribution of gaseous
and particulate organic composition during dark a-pinene ozonolysis, Atmos.
Chem. Phys., 10, 2893–2917, https://doi.org/10.5194/acp-10-2893-2010, 2010.
Cappa, C. D. and Wilson, K. R.: Evolution of organic aerosol mass spectra
upon heating: implications for OA phase and partitioning behavior, Atmos.
Chem. Phys., 11, 1895–1911, https://doi.org/10.5194/acp-11-1895-2011, 2011.
Cappa, C. D., Che, D. L., Kessler, S. H., Kroll, J. H., and Wilson, K. R.:
Variations in organic aerosol optical and hygroscopic properties upon
heterogeneous OH oxidation, J. Geophys. Res., 116, D15204,
https://doi.org/10.1029/2011jd015918, 2011.
Cappa, C. D., Li, Z., and Smith, K.: Influence of Relative Humidity on the
Heterogeneous Oxidation of Secondary Organic Aerosol, UC Davis Dash,
https://doi.org/10.25338/B8ZK5X, 8 October 2018.
Chan, M. N., Zhang, H., Goldstein, A. H., and Wilson, K. R.: Role of Water
and Phase in the Heterogeneous Oxidation of Solid and Aqueous Succinic Acid
Aerosol by Hydroxyl Radicals, J. Phys. Chem. C, 118, 28978–28992,
https://doi.org/10.1021/jp5012022, 2014.
Chim, M. M., Cheng, C. T., Davies, J. F., Berkemeier, T., Shiraiwa, M.,
Zuend, A., and Chan, M. N.: Compositional evolution of particle-phase
reaction products and water in the heterogeneous OH oxidation of model
aqueous organic aerosols, Atmos. Chem. Phys., 17, 14415–14431,
https://doi.org/10.5194/acp-17-14415-2017, 2017a.
Chim, M. M., Chow, C. Y., Davies, J. F., and Chan, M. N.: Effects of
Relative Humidity and Particle Phase Water on the Heterogeneous OH
Oxidation of 2-Methylglutaric Acid Aqueous Droplets, J. Phys. Chem. A, 121,
1667–1675, https://doi.org/10.1021/acs.jpca.6b11606, 2017b.
Davies, J. F. and Wilson, K. R.: Nanoscale interfacial gradients formed by
the reactive uptake of OH radicals onto viscous aerosol surfaces,
Chem. Sci., 6, 7020–7027, https://doi.org/10.1039/c5sc02326b, 2015.
Denisov, E. T. and Afanas'ev, I. B.: Oxidation and antioxidants in organic
chemistry and biology, Taylor & Francis, Boca Raton, FL, 981 pp., 2005.
Dennis-Smither, B. J., Miles, R. E. H., and Reid, J. P.: Oxidative aging of
mixed oleic acid/sodium chloride aerosol particles, J. Geophys. Res.-Atmos.,
117, D20204, https://doi.org/10.1029/2012JD018163, 2012.
Docherty, K. S., Wu, W., Lim, Y. B., and Ziemann, P. J.: Contributions of
organic peroxides to secondary aerosol formed from reactions of monoterpenes
with O3, Environ. Sci. Technol., 39, 4049–4059,
https://doi.org/10.1021/es050228s, 2005.
Donahue, N. M., Henry, K. M., Mentel, T. F., Kiendler-Scharr, A., Spindler,
C., Bohn, B., Brauers, T., Dorn, H. P., Fuchs, H., Tillmann, R., Wahner, A.,
Saathoff, H., Naumann, K. H., Mohler, O., Leisner, T., Muller, L., Reinnig,
M. C., Hoffmann, T., Salo, K., Hallquist, M., Frosch, M., Bilde, M.,
Tritscher, T., Barmet, P., Praplan, A. P., DeCarlo, P. F., Dommen, J.,
Prevot, A. S., and Baltensperger, U.: Aging of biogenic secondary organic
aerosol via gas-phase OH radical reactions, P. Natl. Acad. Sci. USA,
109, 13503–13508, https://doi.org/10.1073/pnas.1115186109, 2012.
Emanuelsson, E. U., Mentel, T. F., Watne, A. K., Spindler, C., Bohn, B.,
Brauers, T., Dorn, H. P., Hallquist, A. M., Haseler, R., Kiendler-Scharr, A.,
Muller, K. P., Pleijel, H., Rohrer, F., Rubach, F., Schlosser, E., Tillmann,
R., and Hallquist, M.: Parameterization of Thermal Properties of Aging
Secondary Organic Aerosol Produced by Photo-Oxidation of Selected Terpene
Mixtures, Environ. Sci. Technol., 48, 6168–6176,
https://doi.org/10.1021/es405412p, 2014.
Fan, H., Tinsley, M. R., and Goulay, F.: Effect of Relative Humidity on the
OH-Initiated Heterogeneous Oxidation of Monosaccharide Nanoparticles,
J. Phys. Chem. A, 119, 11182–11190,
https://doi.org/10.1021/acs.jpca.5b06364, 2015.
George, I. J., Vlasenko, A., Slowik, J. G., Broekhuizen, K., and Abbatt, J.
P. D.: Heterogeneous oxidation of saturated organic aerosols by hydroxyl
radicals: uptake kinetics, condensed-phase products, and particle size
change, Atmos. Chem. Phys., 7, 4187–4201,
https://doi.org/10.5194/acp-7-4187-2007, 2007.
George, I. J., Chang, R. Y. W., Danov, V., Vlasenko, A., and Abbatt, J. P.
D.: Modification of cloud condensation nucleus activity of organic aerosols
by hydroxyl radical heterogeneous oxidation, Atmos. Environ., 43, 5038–5045,
https://doi.org/10.1016/j.atmosenv.2009.06.043, 2009.
Gierczak, T., Gilles, M. K., Bauerle, S., and Ravishankara, A. R.: Reaction
of hydroxyl radical with acetone. 1. Kinetics of the reactions of OH,
OD, and (OH)-O-18 with acetone and acetone-d(6), J. Phys. Chem. A,
107, 5014–5020, https://doi.org/10.1021/jp027301a, 2003.
Gloaguen, E., Mysak, E. R., Leone, S. R., Ahmed, M., and Wilson, K. R.:
Investigating the chemical composition of mixed organic-inorganic particles
by “soft” vacuum ultraviolet photoionization: The reaction of ozone with
anthracene on sodium chloride particles, Int. J. Mass. Spectrom., 258,
74–85, https://doi.org/10.1016/j.ijms.2006.07.019, 2006.
Grayson, J. W., Zhang, Y., Mutzel, A., Renbaum-Wolff, L., Böge, O., Kamal,
S., Herrmann, H., Martin, S. T., and Bertram, A. K.: Effect of varying
experimental conditions on the viscosity of a-pinene derived secondary
organic material, Atmos. Chem. Phys., 16, 6027–6040,
https://doi.org/10.5194/acp-16-6027-2016, 2016.
Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T.,
Harley, P., Klinger, L., Lerdau, M., Mckay, W. A., Pierce, T., Scholes, B.,
Steinbrecher, R., Tallamraju, R., Taylor, J., and Zimmerman, P.: A
Global-Model of Natural Volatile Organic-Compound Emissions, J. Geophys.
Res.-Atmos., 100, 8873–8892, https://doi.org/10.1029/94JD02950, 1995.
Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T.,
Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols
from Nature version 2.1 (MEGAN2.1): an extended and updated framework for
modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492,
https://doi.org/10.5194/gmd-5-1471-2012, 2012.
Hall, W. A., Pennington, M. R., and Johnston, M. V.: Molecular
Transformations Accompanying the Aging of Laboratory Secondary Organic
Aerosol, Environ. Sci. Technol., 47, 2230–2237,
https://doi.org/10.1021/es303891q, 2013.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D.,
Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H.,
Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M.
E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel,
Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D.,
Szmigielski, R., and Wildt, J.: The formation, properties and impact of
secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys.,
9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Harmon, C. W., Ruehl, C. R., Cappa, C. D., and Wilson, K. R.: A statistical
description of the evolution of cloud condensation nuclei activity during the
heterogeneous oxidation of squalane and bis(2-ethylhexyl) sebacate aerosol by
hydroxyl radicals, Phys. Chem. Chem. Phys., 15, 9679–9693,
https://doi.org/10.1039/c3cp50347j, 2013.
Hennigan, C. J., Sullivan, A. P., Collett, J. L., and Robinson, A. L.:
Levoglucosan stability in biomass burning particles exposed to hydroxyl
radicals, Geophys. Res. Lett., 37, L09806,
https://doi.org/10.1029/2010gl043088, 2010.
Houle, F. A., Hinsberg, W. D., and Wilson, K. R.: Oxidation of a model
alkane aerosol by OH radical: the emergent nature of reactive uptake,
Phys. Chem. Chem. Phys., 17, 4412–4423,
https://doi.org/10.1039/c4cp05093b, 2015.
Hu, W., Palm, B. B., Day, D. A., Campuzano-Jost, P., Krechmer, J. E., Peng,
Z., de Sá, S. S., Martin, S. T., Alexander, M. L., Baumann, K., Hacker, L.,
Kiendler-Scharr, A., Koss, A. R., de Gouw, J. A., Goldstein, A. H., Seco, R.,
Sjostedt, S. J., Park, J.-H., Guenther, A. B., Kim, S., Canonaco, F.,
Prévôt, A. S. H., Brune, W. H., and Jimenez, J. L.: Volatility and
lifetime against OH heterogeneous reaction of ambient
isoprene-epoxydiols-derived secondary organic aerosol (IEPOX-SOA), Atmos.
Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016,
2016.
Jain, S., Fischer, K. B., and Petrucci, G. A.: The Influence of Absolute
Mass Loading of Secondary Organic Aerosols on Their Phase State,
Atmosphere-Basel, 9, 131, https://doi.org/10.3390/atmos9040131, 2018.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang,
Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A.
C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L.,
Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y.
L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara,
P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J.,
Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P.
I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer,
S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A.,
Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina,
K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M.,
Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger,
U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere,
Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Kaiser, J. C., Riemer, N., and Knopf, D. A.: Detailed heterogeneous oxidation
of soot surfaces in a particle-resolved aerosol model, Atmos. Chem. Phys.,
11, 4505–4520, https://doi.org/10.5194/acp-11-4505-2011, 2011.
Kidd, C., Perraud, V., Wingen, L. M., and Finlayson-Pitts, B. J.:
Integrating phase and composition of secondary organic aerosol from the
ozonolysis of alpha-pinene, P. Natl. Acad. Sci. USA, 111, 7552–7557,
https://doi.org/10.1073/pnas.1322558111, 2014.
Kolesar, K. R., Li, Z., Wilson, K. R., and Cappa, C. D.: Heating-Induced
Evaporation of Nine Different Secondary Organic Aerosol Types, Environ. Sci.
Technol., 49, 12242–12252, https://doi.org/10.1021/acs.est.5b03038, 2015.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and
phase state of organic compounds: dependency on molecular properties and
implications for secondary organic aerosols in the atmosphere, Phys. Chem.
Chem. Phys., 13, 19238–19255, https://doi.org/10.1039/c1cp22617g, 2011.
Krapf, M., El Haddad, I., Bruns, E. A., Molteni, U., Daellenbach, K. R.,
Prevot, A. S. H., Baltensperger, U., and Dommen, J.: Labile Peroxides in
Secondary Organic Aerosol, Chem-Us, 1, 603–616,
https://doi.org/10.1016/j.chempr.2016.09.007, 2016.
Kristensen, K., Cui, T., Zhang, H., Gold, A., Glasius, M., and Surratt, J.
D.: Dimers in a-pinene secondary organic aerosol: effect of hydroxyl radical,
ozone, relative humidity and aerosol acidity, Atmos. Chem. Phys., 14,
4201–4218, https://doi.org/10.5194/acp-14-4201-2014, 2014.
Kristensen, K., Watne, A. K., Hammes, J., Lutz, A., Petaja, T., Hallquist,
M., Bilde, M., and Glasius, M.: High-Molecular Weight Dimer Esters Are Major
Products in Aerosols from alpha-Pinene Ozonolysis and the Boreal Forest,
Environ. Sci. Tech. Let., 3, 280–285,
https://doi.org/10.1021/acs.estlett.6b00152, 2016.
Kroll, J. H., Smith, J. D., Che, D. L., Kessler, S. H., Worsnop, D. R., and
Wilson, K. R.: Measurement of fragmentation and functionalization pathways in
the heterogeneous oxidation of oxidized organic aerosol, Phys. Chem. Chem.
Phys., 11, 8005–8014, https://doi.org/10.1039/b905289e, 2009.
Kroll, J. H., Lim, C. Y., Kessler, S. H., and Wilson, K. R.: Heterogeneous
Oxidation of Atmospheric Organic Aerosol: Kinetics of Changes to the Amount
and Oxidation State of Particle-Phase Organic Carbon, J. Phys. Chem. A, 119,
10767–10783, https://doi.org/10.1021/acs.jpca.5b06946, 2015.
Kuwata, M. and Martin, S. T.: Phase of atmospheric secondary organic
material affects its reactivity, P. Natl. Acad. Sci. USA, 109, 17354–17359,
https://doi.org/10.1073/pnas.1209071109, 2012.
Kwok, E. S. C. and Atkinson, R.: Estimation of Hydroxyl Radical
Reaction-Rate Constants for Gas-Phase Organic-Compounds Using a
Structure-Reactivity Relationship – an Update, Atmos. Environ., 29,
1685–1695, https://doi.org/10.1016/1352-2310(95)00069-B, 1995.
Lai, C., Liu, Y., Ma, J., Ma, Q., and He, H.: Degradation kinetics of
levoglucosan initiated by hydroxyl radical under different environmental
conditions, Atmos. Environ., 91, 32–39,
https://doi.org/10.1016/j.atmosenv.2014.03.054, 2014.
Lai, C., Liu, Y., Ma, J., Ma, Q., Chu, B., and He, H.: Heterogeneous
Kinetics of cis-Pinonic Acid with Hydroxyl Radical under Different
Environmental Conditions, J. Phys. Chem. A, 119, 6583–6593,
https://doi.org/10.1021/acs.jpca.5b01321, 2015.
Lakey, P. S. J., Berkemeier, T., Krapf, M., Dommen, J., Steimer, S. S.,
Whalley, L. K., Ingham, T., Baeza-Romero, M. T., Pöschl, U., Shiraiwa, M.,
Ammann, M., and Heard, D. E.: The effect of viscosity and diffusion on the
HO2 uptake by sucrose and secondary organic aerosol particles, Atmos.
Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016,
2016.
Lambe, A. T., Onasch, T. B., Croasdale, D. R., Wright, J. P., Martin, A. T.,
Franklin, J. P., Massoli, P., Kroll, J. H., Canagaratna, M. R., Brune, W. H.,
Worsnop, D. R., and Davidovits, P.: Transitions from functionalization to
fragmentation reactions of laboratory secondary organic aerosol (SOA)
generated from the OH oxidation of alkane precursors, Environ. Sci.
Technol., 46, 5430–5437, https://doi.org/10.1021/es300274t, 2012.
Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B., Hueglin, C.,
and Prévôt, A. S. H.: Source apportionment of submicron organic aerosols
at an urban site by factor analytical modelling of aerosol mass spectra,
Atmos. Chem. Phys., 7, 1503–1522, https://doi.org/10.5194/acp-7-1503-2007,
2007.
Li, R., Palm, B. B., Ortega, A. M., Hlywiak, J., Hu, W. W., Peng, Z., Day,
D. A., Knote, C., Brune, W. H., de Gouw, J. A., and Jimenez, J. L.: Modeling
the Radical Chemistry in an Oxidation Flow Reactor: Radical Formation and
Recycling, Sensitivities, and the OH Exposure Estimation Equation, J.
Phys. Chem. A, 119, 4418–4432, https://doi.org/10.1021/jp509534k,
2015.
Li, Y. J., Liu, P. F., Gong, Z. H., Wang, Y., Bateman, A. P., Bergoend, C.,
Bertram, A. K., and Martin, S. T.: Chemical Reactivity and Liquid/Nonliquid
States of Secondary Organic Material, Environ. Sci. Technol., 49,
13264–13274, https://doi.org/10.1021/acs.est.5b03392, 2015.
Liu, M. J., Wiegel, A. A., Wilson, K. R., and Houle, F. A.: Aerosol
Fragmentation Driven by Coupling of Acid-Base and Free-Radical Chemistry in
the Heterogeneous Oxidation of Aqueous Citric Acid by OH Radicals, J.
Phys. Chem. A, 121, 5856–5870,
https://doi.org/10.1021/acs.jpca.7b04892, 2017.
McNeill, V. F., Yatavelli, R. L. N., Thornton, J. A., Stipe, C. B., and
Landgrebe, O.: Heterogeneous OH oxidation of palmitic acid in single
component and internally mixed aerosol particles: vaporization and the role
of particle phase, Atmos. Chem. Phys., 8, 5465–5476,
https://doi.org/10.5194/acp-8-5465-2008, 2008.
Moog, R. S., Ediger, M. D., Boxer, S. G., and Fayer, M. D.: Viscosity
Dependence of the Rotational Reorientation of Rhodamine-B in Mono-Alcohol and
Poly-Alcohol – Picosecond Transient Grating Experiments, J. Phys. Chem.-Us,
86, 4694–4700, https://doi.org/10.1021/j100221a011, 1982.
Mysak, E. R.: Gentle photoionization of organic constituents using vacuum
ultraviolet aerosol mass spectrometry, PhD Thesis, Department of Chemistry,
University of North Carolina at Chapel Hill, Chapel Hill, NC, 2006.
Nah, T., Kessler, S. H., Daumit, K. E., Kroll, J. H., Leone, S. R., and
Wilson, K. R.: OH-initiated oxidation of sub-micron unsaturated fatty
acid particles, Phys. Chem. Chem. Phys., 15, 18649–18663,
https://doi.org/10.1039/c3cp52655k, 2013.
Nah, T., Kessler, S. H., Daumit, K. E., Kroll, J. H., Leone, S. R., and
Wilson, K. R.: Influence of molecular structure and chemical functionality on
the heterogeneous OH-initiated oxidation of unsaturated organic
particles, J. Phys. Chem. A, 118, 4106–4119,
https://doi.org/10.1021/jp502666g, 2014.
Park, J. H., Ivanov, A. V., and Molina, M. J.: Effect of relative humidity
on OH uptake by surfaces of atmospheric importance, J. Phys. Chem. A,
112, 6968–6977, https://doi.org/10.1021/jp8012317, 2008.
Peng, Z., Day, D. A., Stark, H., Li, R., Lee-Taylor, J., Palm, B. B., Brune,
W. H., and Jimenez, J. L.: HOx radical chemistry in oxidation flow
reactors with low-pressure mercury lamps systematically examined by modeling,
Atmos. Meas. Tech., 8, 4863–4890, https://doi.org/10.5194/amt-8-4863-2015,
2015.
Petters, M. D., Prenni, A. J., Kreidenweis, S. M., DeMott, P. J., Matsunaga,
A., Lim, Y. B., and Ziemann, P. J.: Chemical aging and the
hydrophobic-to-hydrophilic conversion of carbonaceous aerosol, Geophys. Res.
Lett., 33, L24806, https://doi.org/10.1029/2006GL027249, 2006.
Pöschl, U., Rudich, Y., and Ammann, M.: Kinetic model framework for aerosol
and cloud surface chemistry and gas-particle interactions – Part 1: General
equations, parameters, and terminology, Atmos. Chem. Phys., 7, 5989–6023,
https://doi.org/10.5194/acp-7-5989-2007, 2007.
Putman, A. L., Offenberg, J. H., Fisseha, R., Kundu, S., Rahn, T. A., and
Mazzoleni, L. R.: Ultrahigh-resolution FT-ICR mass spectrometry
characterization of α-pinene ozonolysis SOA, Atmos. Environ., 46,
164–172, https://doi.org/10.1016/j.atmosenv.2011.10.003, 2012.
Renbaum-Wolff, L., Grayson, J. W., Bateman, A. P., Kuwata, M., Sellier, M.,
Murray, B. J., Shilling, J. E., Martin, S. T., and Bertram, A. K.: Viscosity
of alpha-pinene secondary organic material and implications for particle
growth and reactivity, P. Natl. Acad. Sci. USA, 110, 8014–8019,
https://doi.org/10.1073/pnas.1219548110, 2013.
Ruehl, C. R., Nah, T., Isaacman, G., Worton, D. R., Chan, A. W., Kolesar, K.
R., Cappa, C. D., Goldstein, A. H., and Wilson, K. R.: The influence of
molecular structure and aerosol phase on the heterogeneous oxidation of
normal and branched alkanes by OH, J. Phys. Chem. A, 117, 3990–4000,
https://doi.org/10.1021/jp401888q, 2013.
Shilling, J. E., Chen, Q., King, S. M., Rosenoern, T., Kroll, J. H., Worsnop,
D. R., DeCarlo, P. F., Aiken, A. C., Sueper, D., Jimenez, J. L., and Martin,
S. T.: Loading-dependent elemental composition of a-pinene SOA particles,
Atmos. Chem. Phys., 9, 771–782, https://doi.org/10.5194/acp-9-771-2009,
2009.
Shiraiwa, M., Pfrang, C., and Pöschl, U.: Kinetic multi-layer model of
aerosol surface and bulk chemistry (KM-SUB): the influence of interfacial
transport and bulk diffusion on the oxidation of oleic acid by ozone, Atmos.
Chem. Phys., 10, 3673–3691, https://doi.org/10.5194/acp-10-3673-2010, 2010.
Shiraiwa, M., Pfrang, C., Koop, T., and Pöschl, U.: Kinetic multi-layer
model of gas-particle interactions in aerosols and clouds (KM-GAP): linking
condensation, evaporation and chemical reactions of organics, oxidants and
water, Atmos. Chem. Phys., 12, 2777–2794,
https://doi.org/10.5194/acp-12-2777-2012, 2012.
Slade, J. H. and Knopf, D. A.: Heterogeneous OH oxidation of biomass
burning organic aerosol surrogate compounds: assessment of volatilisation
products and the role of OH concentration on the reactive uptake
kinetics, Phys. Chem. Chem. Phys., 15, 5898–5915,
https://doi.org/10.1039/c3cp44695f, 2013.
Slade, J. H. and Knopf, D. A.: Multiphase OH oxidation kinetics of organic
aerosol: The role of particle phase state and relative humidity, Geophys.
Res. Lett., 41, 5297–5306, https://doi.org/10.1002/2014gl060582, 2014.
Slade, J. H., Thalman, R., Wang, J., and Knopf, D. A.: Chemical aging of
single and multicomponent biomass burning aerosol surrogate particles by OH:
implications for cloud condensation nucleus activity, Atmos. Chem. Phys., 15,
10183–10201, https://doi.org/10.5194/acp-15-10183-2015, 2015.
Slade, J. H., Shiraiwa, M., Arangio, A., Su, H., Pöschl, U., Wang, J., and
Knopf, D. A.: Cloud droplet activation through oxidation of organic aerosol
influenced by temperature and particle phase state, Geophys. Res. Lett., 44,
1583–1591, https://doi.org/10.1002/2016GL072424, 2017.
Smith, J. D., Kroll, J. H., Cappa, C. D., Che, D. L., Liu, C. L., Ahmed, M.,
Leone, S. R., Worsnop, D. R., and Wilson, K. R.: The heterogeneous reaction
of hydroxyl radicals with sub-micron squalane particles: a model system for
understanding the oxidative aging of ambient aerosols, Atmos. Chem. Phys., 9,
3209–3222, https://doi.org/10.5194/acp-9-3209-2009, 2009.
Song, M., Liu, P. F., Hanna, S. J., Li, Y. J., Martin, S. T., and Bertram, A.
K.: Relative humidity-dependent viscosities of isoprene-derived secondary
organic material and atmospheric implications for isoprene-dominant forests,
Atmos. Chem. Phys., 15, 5145–5159, https://doi.org/10.5194/acp-15-5145-2015,
2015.
Tolocka, M. P., Heaton, K. J., Dreyfus, M. A., Wang, S. Y., Zordan, C. A.,
Saul, T. D., and Johnston, M. V.: Chemistry of particle inception and growth
during alpha-pinene ozonolysis, Environ. Sci. Technol., 40, 1843–1848,
https://doi.org/10.1021/es051926f, 2006.
Tong, H., Arangio, A. M., Lakey, P. S. J., Berkemeier, T., Liu, F., Kampf, C.
J., Brune, W. H., Pöschl, U., and Shiraiwa, M.: Hydroxyl radicals from
secondary organic aerosol decomposition in water, Atmos. Chem. Phys., 16,
1761–1771, https://doi.org/10.5194/acp-16-1761-2016, 2016.
Varutbangkul, V., Brechtel, F. J., Bahreini, R., Ng, N. L., Keywood, M. D.,
Kroll, J. H., Flagan, R. C., Seinfeld, J. H., Lee, A., and Goldstein, A. H.:
Hygroscopicity of secondary organic aerosols formed by oxidation of
cycloalkenes, monoterpenes, sesquiterpenes, and related compounds, Atmos.
Chem. Phys., 6, 2367–2388, https://doi.org/10.5194/acp-6-2367-2006, 2006.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirila, P.,
Leskinen, J., Makela, J. M., Holopainen, J. K., Pöschl, U., Kulmala, M.,
Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic
secondary organic aerosol particles, Nature, 467, 824–827,
https://doi.org/10.1038/nature09455, 2010.
Wang, B. B., O'Brien, R. E., Kelly, S. T., Shilling, J. E., Moffet, R. C.,
Gilles, M. K., and Laskin, A.: Reactivity of Liquid and Semisolid Secondary
Organic Carbon with Chloride and Nitrate in Atmospheric Aerosols, J. Phys.
Chem. A, 119, 4498–4508, https://doi.org/10.1021/jp510336q, 2015.
Wiegel, A. A., Wilson, K. R., Hinsberg, W. D., and Houle, F. A.: Stochastic
methods for aerosol chemistry: a compact molecular description of
functionalization and fragmentation in the heterogeneous oxidation of
squalane aerosol by OH radicals, Phys. Chem. Chem. Phys., 17,
4398–4411, https://doi.org/10.1039/c4cp04927f, 2015.
Wiegel, A. A., Liu, M. J., Hinsberg, W. D., Wilson, K. R., and Houle, F. A.:
Diffusive confinement of free radical intermediates in the OH radical
oxidation of semisolid aerosols, Phys. Chem. Chem. Phys., 19, 6814–6830,
https://doi.org/10.1039/c7cp00696a, 2017.
Wollenhaupt, M., Carl, S. A., Horowitz, A., and Crowley, J. N.: Rate
coefficients for reaction of OH with acetone between 202 and 395 K,
J. Phys. Chem. A, 104, 2695–2705, https://doi.org/10.1021/jp993738f, 2000.
Yasmeen, F., Vermeylen, R., Maurin, N., Perraudin, E., Doussin, J.-F., and
Claeys, M.: Characterisation of tracers for aging of á-pinene secondary
organic aerosol using liquid chromatography/negative ion electrospray
ionisation mass spectrometry, Environ. Chem., 9, 236–246,
https://doi.org/10.1071/en11148, 2012.
Yu, J. Z., Cocker, D. R., Griffin, R. J., Flagan, R. C., and Seinfeld, J.
H.: Gas-phase ozone oxidation of monoterpenes: Gaseous and particulate
products, J. Atmos. Chem., 34, 207–258,
https://doi.org/10.1023/A:1006254930583, 1999.
Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Allan, J. D., Coe, H.,
Ulbrich, I., Alfarra, M. R., Takami, A., Middlebrook, A. M., Sun, Y. L.,
Dzepina, K., Dunlea, E., Docherty, K., DeCarlo, P. F., Salcedo, D., Onasch,
T., Jayne, J. T., Miyoshi, T., Shimono, A., Hatakeyama, S., Takegawa, N.,
Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian,
K., Williams, P., Bower, K., Bahreini, R., Cottrell, L., Griffin, R. J.,
Rautiainen, J., Sun, J. Y., Zhang, Y. M., and Worsnop, D. R.: Ubiquity and
dominance of oxygenated species in organic aerosols in
anthropogenically-influenced Northern Hemisphere midlatitudes, Geophys. Res.
Lett., 34, L13801, https://doi.org/10.1029/2007gl029979, 2007.
Zhang, X., Lambe, A. T., Upshur, M. A., Brooks, W. A., Be, A. G., Thomson,
R. J., Geiger, F. M., Surratt, J. D., Zhang, Z. F., Gold, A., Graf, S.,
Cubison, M. J., Groessl, M., Jayne, J. T., Worsnop, D. R., and Canagaratna,
M. R.: Highly Oxygenated Multifunctional Compounds in alpha-Pinene Secondary
Organic Aerosol, Environ. Sci. Technol., 51, 5932–5940,
https://doi.org/10.1021/acs.est.6b06588, 2017.
Ziemann, P. J. and Atkinson, R.: Kinetics, products, and mechanisms of
secondary organic aerosol formation, Chem. Soc. Rev., 41, 6582–6605,
https://doi.org/10.1039/c2cs35122f, 2012.
Short summary
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.
We investigated the influence of relative humidity (RH) on the heterogeneous oxidation of...
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