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Title: Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

Abstract

Abstract Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron‐sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid‐catalyzed multiphase chemistry of isoprene epoxydiols, particle‐phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global modelsmore » neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process‐related interactions, so that these processes can be accurately represented in atmospheric chemistry‐climate models.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5];  [6]; ORCiD logo [1];  [7]; ORCiD logo [8];  [9];  [10]; ORCiD logo [1];  [11]; ORCiD logo [12]; ORCiD logo [13]; ORCiD logo [4]; ORCiD logo [14]; ORCiD logo [15];  [6] more »;  [16]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [17] « less
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Univ. of California, Davis, CA (United States). Dept. of Civil and Environmental Engineering
  3. Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy and Management and Dept. of Civil and Environmental Engineering
  4. Univ. of California, Irvine, CA (United States). Dept. of Earth System Science
  5. Univ. of Colorado, Boulder, CO (United States). Cooperative Inst. for Research in Environmental Sciences, Dept. of Chemistry and Biochemistry
  6. Brookhaven National Lab. (BNL), Upton, NY (United States)
  7. Harvard Univ., Cambridge, MA (United States). School of Engineering and Applied Sciences, Dept. of Earth and Planetary Sciences
  8. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering, School of Earth and Atmospheric Sciences
  9. Univ. of Helsinki (Finland). Dept. of Physics
  10. Colorado State Univ., Fort Collins, CO (United States). Dept. of Atmospheric Science
  11. Lund Univ. (Sweden). Dept. of Physics
  12. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
  13. Pacific Northwest National Laboratory, Richland Washington USA
  14. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences
  15. Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA
  16. Aerodyne Research, Inc., Billerica, MA (United States)
  17. Univ. of California, Davis, CA (United States). Dept. of Environmental Toxicology
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1392240
Alternate Identifier(s):
OSTI ID: 1402338
Report Number(s):
BNL-114255-2017-JA
Journal ID: ISSN 8755-1209; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
Grant/Contract Number:  
SC0012704; AC05-76RL01830; DE‐AC05‐76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Reviews of Geophysics (1985)
Additional Journal Information:
Journal Name: Reviews of Geophysics (1985); Journal Volume: 55; Journal Issue: 2; Journal ID: ISSN 8755-1209
Publisher:
American Geophysical Union (AGU)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Shrivastava, Manish, Cappa, Christopher D., Fan, Jiwen, Goldstein, Allen H., Guenther, Alex B., Jimenez, Jose L., Kuang, Chongai, Laskin, Alexander, Martin, Scot T., Ng, Nga Lee, Petaja, Tuukka, Pierce, Jeffrey R., Rasch, Philip J., Roldin, Pontus, Seinfeld, John H., Shilling, John, Smith, James N., Thornton, Joel A., Volkamer, Rainer, Wang, Jian, Worsnop, Douglas R., Zaveri, Rahul A., Zelenyuk, Alla, and Zhang, Qi. Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol. United States: N. p., 2017. Web. doi:10.1002/2016RG000540.
Shrivastava, Manish, Cappa, Christopher D., Fan, Jiwen, Goldstein, Allen H., Guenther, Alex B., Jimenez, Jose L., Kuang, Chongai, Laskin, Alexander, Martin, Scot T., Ng, Nga Lee, Petaja, Tuukka, Pierce, Jeffrey R., Rasch, Philip J., Roldin, Pontus, Seinfeld, John H., Shilling, John, Smith, James N., Thornton, Joel A., Volkamer, Rainer, Wang, Jian, Worsnop, Douglas R., Zaveri, Rahul A., Zelenyuk, Alla, & Zhang, Qi. Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol. United States. https://doi.org/10.1002/2016RG000540
Shrivastava, Manish, Cappa, Christopher D., Fan, Jiwen, Goldstein, Allen H., Guenther, Alex B., Jimenez, Jose L., Kuang, Chongai, Laskin, Alexander, Martin, Scot T., Ng, Nga Lee, Petaja, Tuukka, Pierce, Jeffrey R., Rasch, Philip J., Roldin, Pontus, Seinfeld, John H., Shilling, John, Smith, James N., Thornton, Joel A., Volkamer, Rainer, Wang, Jian, Worsnop, Douglas R., Zaveri, Rahul A., Zelenyuk, Alla, and Zhang, Qi. Thu . "Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol". United States. https://doi.org/10.1002/2016RG000540. https://www.osti.gov/servlets/purl/1392240.
@article{osti_1392240,
title = {Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol},
author = {Shrivastava, Manish and Cappa, Christopher D. and Fan, Jiwen and Goldstein, Allen H. and Guenther, Alex B. and Jimenez, Jose L. and Kuang, Chongai and Laskin, Alexander and Martin, Scot T. and Ng, Nga Lee and Petaja, Tuukka and Pierce, Jeffrey R. and Rasch, Philip J. and Roldin, Pontus and Seinfeld, John H. and Shilling, John and Smith, James N. and Thornton, Joel A. and Volkamer, Rainer and Wang, Jian and Worsnop, Douglas R. and Zaveri, Rahul A. and Zelenyuk, Alla and Zhang, Qi},
abstractNote = {Abstract Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron‐sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid‐catalyzed multiphase chemistry of isoprene epoxydiols, particle‐phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process‐related interactions, so that these processes can be accurately represented in atmospheric chemistry‐climate models.},
doi = {10.1002/2016RG000540},
journal = {Reviews of Geophysics (1985)},
number = 2,
volume = 55,
place = {United States},
year = {Thu Jun 15 00:00:00 EDT 2017},
month = {Thu Jun 15 00:00:00 EDT 2017}
}

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Overview of the Focused Isoprene eXperiment at the California Institute of Technology (FIXCIT): mechanistic chamber studies on the oxidation of biogenic compounds
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Molecular characterization of brown carbon (BrC) chromophores in secondary organic aerosol generated from photo-oxidation of toluene
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Evidence for ambient dark aqueous SOA formation in the Po Valley, Italy
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Oligomer formation within secondary organic aerosols: equilibrium and dynamic considerations
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Effect of varying experimental conditions on the viscosity of α -pinene derived secondary organic material
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Secondary Organic Aerosol Formation by Glyoxal Hydration and Oligomer Formation:  Humidity Effects and Equilibrium Shifts during Analysis
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Aqueous benzene-diols react with an organic triplet excited state and hydroxyl radical to form secondary organic aerosol
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Long-term volatility measurements of submicron atmospheric aerosol in Hyytiälä, Finland
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The effect of physical and chemical aerosol properties on warm cloud droplet activation
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A two-dimensional volatility basis set: 1. organic-aerosol mixing thermodynamics
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Organosulfate formation during the uptake of pinonaldehyde on acidic sulfate aerosols
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Elemental composition and oxidation of chamber organic aerosol
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Bounding the role of black carbon in the climate system: A scientific assessment: BLACK CARBON IN THE CLIMATE SYSTEM
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Experimental determination of chemical diffusion within secondary organic aerosol particles
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Isoprene nitrates: preparation, separation, identification, yields, and atmospheric chemistry
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The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions
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Effective Henry’s Law Partitioning and the Salting Constant of Glyoxal in Aerosols Containing Sulfate
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CCN activity of organic aerosols observed downwind of urban emissions during CARES
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Toward Direct Measurement of Atmospheric Nucleation
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Cloud droplet activation of mixed organic-sulfate particles produced by the photooxidation of isoprene
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Nitrogen management is essential to prevent tropical oil palm plantations from causing ground-level ozone pollution
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O/C and OM/OC Ratios of Primary, Secondary, and Ambient Organic Aerosols with High-Resolution Time-of-Flight Aerosol Mass Spectrometry
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High-resolution mass spectrometry analysis of secondary organic aerosol generated by ozonolysis of isoprene
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Evidence for a significant proportion of Secondary Organic Aerosol from isoprene above a maritime tropical forest
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Chamber studies of SOA formation from aromatic hydrocarbons: observation of limited glyoxal uptake
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Biogenic carbon and anthropogenic pollutants combine to form a cooling haze over the southeastern United States
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Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX
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Radiative forcing of organic aerosol in the atmosphere and on snow: Effects of SOA and brown carbon
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Hygroscopic Influence on the Semisolid-to-Liquid Transition of Secondary Organic Materials
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Direct aqueous photochemistry of isoprene high-NOx secondary organic aerosol
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Autoxidation of Organic Compounds in the Atmosphere
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Secondary Organic Aerosol Formation from Acetylene (C 2 H 2 ): seed effect on SOA yields due to organic photochemistry in the aerosol aqueous phase
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Unimolecular β-Hydroxyperoxy Radical Decomposition with OH Recycling in the Photochemical Oxidation of Isoprene
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Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets
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Isoprene Epoxydiols as Precursors to Secondary Organic Aerosol Formation: Acid-Catalyzed Reactive Uptake Studies with Authentic Compounds
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The effect of gas-phase polycyclic aromatic hydrocarbons on the formation and properties of biogenic secondary organic aerosol particles
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Secondary organic aerosol formation from <i>m</i>-xylene, toluene, and benzene
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A product study of the gas-phase reaction of Isoprene with the OH radical in the presence of NOx
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Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO 2 emission controls
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Photochemical processing of organic aerosol at nearby continental sites: contrast between urban plumes and regional aerosol
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The Formation of Highly Oxidized Multifunctional Products in the Ozonolysis of Cyclohexene
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Complex Refractive Indices of Thin Films of Secondary Organic Materials by Spectroscopic Ellipsometry from 220 to 1200 nm
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The influences of mass loading and rapid dilution of secondary organic aerosol on particle volatility
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Ultraviolet and visible complex refractive indices of secondary organic material produced by photooxidation of the aromatic compounds toluene and m -xylene
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Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies
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Observations of aminium salts in atmospheric nanoparticles and possible climatic implications
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Aqueous Processing of Atmospheric Organic Particles in Cloud Water Collected via Aircraft Sampling
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Heterogeneous Reactions of Glyoxal on Particulate Matter:  Identification of Acetals and Sulfate Esters
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Atmospheric oxalic acid and SOA production from glyoxal: Results of aqueous photooxidation experiments
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Formation of Low Volatility Organic Compounds and Secondary Organic Aerosol from Isoprene Hydroxyhydroperoxide Low-NO Oxidation
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Aging of biomass burning aerosols over West Africa: Aircraft measurements of chemical composition, microphysical properties, and emission ratios
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Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior
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Global modeling of secondary organic aerosol formation from aromatic hydrocarbons: high- vs. low-yield pathways
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Effects of molecular structure on the chemistry of aerosol formation from the OH-radical-initiated oxidation of alkanes and alkenes
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Chemical insights, explicit chemistry, and yields of secondary organic aerosol from OH radical oxidation of methylglyoxal and glyoxal in the aqueous phase
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Molecular transformations of phenolic SOA during photochemical aging in the aqueous phase: competition among oligomerization, functionalization, and fragmentation
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The Atmospheric Aerosol-Forming Potential of Whole Gasoline Vapor
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Particle Phase Acidity and Oligomer Formation in Secondary Organic Aerosol
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Epoxide Pathways Improve Model Predictions of Isoprene Markers and Reveal Key Role of Acidity in Aerosol Formation
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Secondary organic aerosol formation and primary organic aerosol oxidation from biomass-burning smoke in a flow reactor during FLAME-3
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Formation of Light Absorbing Organo-Nitrogen Species from Evaporation of Droplets Containing Glyoxal and Ammonium Sulfate
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Introduction: Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5)
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Identification of significant precursor gases of secondary organic aerosols from residential wood combustion
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