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

Abstract

Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial 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 (e.g. the ‘climate sensitivity’). 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 a combination of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremelymore » low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic aerosol mass and number with knowledge of particle properties such as volatility and viscosity are crucial for improving understanding of non-linear SOA-related processes. For example, useful insights can be attained by combining bottom-up information related to the molecular speciation of gas- and particle-phase precursors with top-down insights on size evolution dynamics of SOA. Continuing efforts are also needed to rank the most influential processes affecting SOA lifecycle, 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 [1]; ORCiD logo [4]; ORCiD logo [13]; ORCiD logo [5];  [6] more »;  [14]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [15] « less
  1. Pacific Northwest National Laboratory, Richland Washington USA
  2. Department of Civil and Environmental Engineering, University of California, Davis California USA
  3. Department of Environmental Science, Policy and Management and Department of Civil and Environmental Engineering, University of California, Berkeley California USA
  4. Department of Earth System Science, University of California, Irvine California USA
  5. Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA
  6. Brookhaven National Laboratory, Upton New York USA
  7. School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences, Harvard University, Cambridge Massachusetts USA
  8. School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA
  9. Department of Physics, University of Helsinki, Helsinki Finland
  10. Department of Atmospheric Science, Colorado State University, Fort Collins Colorado USA
  11. Department of Physics, Lund University, Lund Sweden
  12. Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena California USA
  13. Department of Atmospheric Sciences, University of Washington, Seattle Washington USA
  14. Aerodyne Research, Inc., Billerica Massachusetts USA
  15. Department of Environmental Toxicology, University of California, Davis California USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1371996
Report Number(s):
PNNL-SA-121416
Journal ID: ISSN 8755-1209; KP1701000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Reviews of Geophysics (1985); Journal Volume: 55; Journal Issue: 2
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. 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, and Zhang, Qi. Thu . "Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol". United States. doi:10.1002/2016RG000540.
@article{osti_1371996,
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 = {Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial 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 (e.g. the ‘climate sensitivity’). 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 a combination of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties 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; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic aerosol mass and number with knowledge of particle properties such as volatility and viscosity are crucial for improving understanding of non-linear SOA-related processes. For example, useful insights can be attained by combining bottom-up information related to the molecular speciation of gas- and particle-phase precursors with top-down insights on size evolution dynamics of SOA. Continuing efforts are also needed to rank the most influential processes affecting SOA lifecycle, 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 01 00:00:00 EDT 2017},
month = {Thu Jun 01 00:00:00 EDT 2017}
}
  • 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 modelsmore » typically do not comprehensively include all important processes. Our review summarizes some of the important developments during the past decade in understanding SOA formation. We also 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.« less
    Cited by 15
  • Cited by 15
  • A series of simulations with the Community Atmosphere Model version 5 (CAM5) with a 7-mode Modal Aerosol Model were conducted to assess the changes in cloud microphysical properties and radiative forcing resulting from marine organic aerosols. Model simulations show that the anthropogenic aerosol indirect forcing (AIF) predicted by CAM5 is decreased in absolute magnitude by up to 0.09 Wm{sup -2} (7 %) when marine organic aerosols are included. Changes in the AIF from marine organic aerosols are associated with small global increases in low-level incloud droplet number concentration and liquid water path of 1.3 cm{sup -3} (1.5 %) and 0.22more » gm{sup -2} (0.5 %), respectively. Areas especially sensitive to changes in cloud properties due to marine organic aerosol include the Southern Ocean, North Pacific Ocean, and North Atlantic Ocean, all of which are characterized by high marine organic emission rates. As climate models are particularly sensitive to the background aerosol concentration, this small but non-negligible change in the AIF due to marine organic aerosols provides a notable link for ocean-ecosystem marine low-level cloud interactions and may be a candidate for consideration in future earth system models.« less
  • Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR)'s Community Atmosphere Model (CAM5) with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7). Emissions of marine primary organic aerosols (POA), phytoplanktonproduced isoprene- and monoterpenes-derived secondary organic aerosols (SOA) and methane sulfonate (MS{sup -}) are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr{sup -1}, for the Gantt et al. (2011) and Vignati et al. (2010) emission parameterizations, respectively. Marine sources of SOA andmore » particulate MS{sup -} (containing both sulfur and carbon atoms) contribute an additional 0.2 and 5.1 Tg yr{sup -1}, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ngm{sup -3}, with values up to 400 ngm{sup -3} over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM) with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2), both Gantt et al. (2011) and Vignati et al. (2010) formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011) parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN). The largest increases (up to 20 %) in CCN (at a supersaturation (S) of 0.2 %) number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming marine organics are internally-mixed with sea-salt provides diverse results with increases and decreases in the concentration of CCN over different parts of the ocean. The sign of the CCN change due to the addition of marine organics to seasalt aerosol is determined by the relative significance of the increase in mean modal diameter due to addition of mass, and the decrease in particle hygroscopicity due to compositional changes in marine aerosol. Based on emerging evidence for increased CCN concentration over biologically active surface ocean areas/periods, our study suggests that treatment of sea spray in global climate models (GCMs) as an internal mixture of marine organic aerosols and sea-salt will likely lead to an underestimation in CCN number concentration.« less
  • No abstract prepared.