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Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls
  • Published Date:
    2016
  • Source:
    Atmospheric Chemistry and Physics, 16(3), 1603-1618.
Filetype[PDF-2.35 MB]


Details:
  • Personal Author:
  • Description:
    Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA), but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (gamma) for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC(4)RS) and ground-based (SOAS) observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx = NO + NO2) over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2) react significantly with both NO (high-NOx pathway) and HO2 (low-NOx pathway), leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3% from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA) and formaldehyde (a product of isoprene oxidation). Isoprene SOA production is mainly contributed by two immediate gasphase precursors, isoprene epoxydiols (IEPOX, 58% of isoprene SOA) from the low-NOx pathway and glyoxal (28 %) from both low-and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation), but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume). The US Environmental Protection Agency (EPA) projects 2013-2025 decreases in anthropogenic emissions of 34% for NOx (leading to a 7% increase in isoprene SOA) and 48% for SO2 (35% decrease in isoprene SOA). Reducing SO2 emissions decreases sulfate and isoprene SOA by a similar magnitude, representing a factor of 2 co-benefit for PM2.5 from SO2 emission controls.
  • DOI:
    http://dx.doi.org/10.5194/acp-16-1603-2016
  • Document Type:
    Journal Article
  • Collection(s):
    Office of Oceanic and Atmospheric Research (OAR)
  • Main Document Checksum:
  • Supporting Files:
    No Additional Files
    1. Top-down constraints on global N2O emissions at optimal resolution: application of a new dimension reduction technique
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      Wells, K. C.; Millet, D. B.; Bousserez, N.; Henze, D. K.; Griffis, T. J.; Chaliyakunnel, S.; Dlugokencky, E. J.; Saikawa, E.; Xiang, G.; Prinn, R. G.; O'Doherty, S.; Young, D.; Weiss, R. F.; Dutton, G. S.; Elkins, J. W.; Krummel, P. B.; Langenfelds, R.; Steele, L. P.;
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      2018
      Source:
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      Description:
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    2. Does vapor pressure deficit drive the seasonality of delta C-13 of the net land-atmosphere CO2 exchange across the United States?
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      Raczka, B.; Biraud, S. C.; Ehleringer, J. R.; Lai, C. T.; Miller, J. B.; Pataki, D. E.; Saleska, S. R.; Torn, M. S.; Vaughn, B. H.; Wehr, R.; Bowling, D. R.;
      Published Date:
      2017
      Source:
      Journal of Geophysical Research-Biogeosciences, 122(8), 1969-1987.
      Description:
      The seasonal pattern of the carbon isotope content (delta C-13) of atmospheric CO2 depends on local and nonlocal land-atmosphere exchange and atmospheric transport. Previous studies suggested that the delta C-13 of the net land-atmosphere CO2 flux (d...
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      Dieng, D.; Laux, P.; Smiatek, G.; Heinzeller, D.; Bliefernicht, J.; Sarr, A.; Gaye, A. T.; Kunstmann, H.;
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      2018
      Source:
      Journal of Geophysical Research-Atmospheres, 123(15), 7950-7973.
      Description:
      In this study, we analyze a set of agroclimatological indices across West Africa and assess their projected changes for the future. We apply the regional climate model CCLM (COnsortium for Small-scale MOdelling in CLimate Mode) with a high spatial re...
      File Type:
      Filetype[PDF - 11.77 MB]
    4. NOx Lifetime and NOy Partitioning During WINTER
      Personal Author:
      Kenagy, H. S.; Sparks, T. L.; Ebben, C. J.; Wooldrige, P. J.; Lopez-Hilfiker, F. D.; Lee, B. H.; Thornton, J. A.; McDuffie, E. E.; Fibiger, D. L.; Brown, S. S.; Montzka, D. D.; Weinheimer, A. J.; Schroder, J. C.; Campuzano-Jost, P.; Day, D. A.; Jimenez, J. L.; Dibb, J. E.; Campos, T.; Shah, V.; Jaegle, L.; Cohen, R. C.;
      Published Date:
      2018
      Source:
      Journal of Geophysical Research-Atmospheres, 123(17), 9813-9827.
      Description:
      Although urban NOx lifetimes have been examined extensively during summertime conditions, wintertime NOx chemistry has been comparatively less studied. We use measurements of NOx and its oxidation products from the aircraft-based WINTER (Wintertime I...
      File Type:
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    5. Observation of viscosity transition in alpha-pinene secondary organic aerosol
      Personal Author:
      Jarvinen, E.; Ignatius, K.; Nichman, L.; Kristensen, T. B.; Fuchs, C.; Hoyle, C. R.; Hoppel, N.; Corbin, J. C.; Craven, J.; Duplissy, J.; Ehrhart, S.; El Haddad, I.; Frege, C.; Gordon, H.; Jokinen, T.; Kallinger, P.; Kirkby, J.; Kiselev, A.; Naumann, K. H.; Petaja, T.; Pinterich, T.; Prevot, A. S. H.; Saathoff, H.; Schiebel, T.; Sengupta, K.; Simon, M.; Slowik, J. G.; Trostl, J.; Virtanen, A.; Vochezer, P.; Vogt, S.; Wagner, A. C.; Wagner, R.; Williamson, C.; Winkler, P. M.; Yan, C.; Baltensperger, U.; Donahue, N. M.; Flagan, R. C.; Gallagher, M.; Hansel, A.; Kulmala, M.; Stratmann, F.; Worsnop, D. R.; Mohler, O.; Leisner, T.; Schnaiter, M.;
      Published Date:
      2016
      Source:
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      Description:
      Under certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requir...
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    6. Quantifying the vertical transport of CHBr3 and CH2Br2 over the western Pacific
      Personal Author:
      Butler, R.; Palmer, P. I.; Feng, L.; Andrews, S. J.; Atlas, E. L.; Carpenter, L. J.; Donets, V.; Harris, N. R. P.; Montzka, S. A.; Pan, L. L.; Salawitch, R. J.; Schauffler, S. M.;
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    7. Convective transport of formaldehyde to the upper troposphere and lower stratosphere and associated scavenging in thunderstorms over the central United States during the 2012DC3 study
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      Fried, A.; Barth, M. C.; Bela, M.; Weibring, P.; Richter, D.; Walega, J.; Li, Y.; Pickering, K.; Apel, E.; Hornbrook, R.; Hills, A.; Riemer, D. D.; Blake, N.; Blake, D. R.; Schroeder, J. R.; Luo, Z. J.; Crawford, J. H.; Olson, J.; Rutledge, S.; Betten, D.; Biggerstaff, M. I.; Diskin, G. S.; Sachse, G.; Campos, T.; Flocke, F.; Weinheimer, A.; Cantrell, C.; Pollack, I.; Peischl, J.; Froyd, K.; Wisthaler, A.; Mikoviny, T.; Woods, S.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Atmospheres, 121(12), 7430-7460.
      Description:
      We have developed semi-independent methods for determining CH2O scavenging efficiencies (SEs) during strong midlatitude convection over the western, south-central Great Plains, and southeastern regions of the United States during the 2012 Deep Convec...
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    8. HTAP_v2.2: a mosaic of regional and global emission grid maps for 2008 and 2010 to study hemispheric transport of air pollution
      Personal Author:
      Janssens-Maenhout, G.; Crippa, M.; Guizzardi, D.; Dentener, F.; Muntean, M.; Pouliot, G.; Keating, T.; Zhang, Q.; Kurokawa, J.; Wankmuller, R.; van der Gon, H. D.; Kuenen, J. J. P.; Klimont, Z.; Frost, G.; Darras, S.; Koffi, B.; Li, M.;
      Published Date:
      2015
      Source:
      Atmospheric Chemistry and Physics, 15(19), 11411-11432.
      Description:
      The mandate of the Task Force Hemispheric Transport of Air Pollution (TF HTAP) under the Convention on Long-Range Transboundary Air Pollution (CLRTAP) is to improve the scientific understanding of the intercontinental air pollution transport, to quan...
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      Filetype[PDF - 3.54 MB]
    9. Nighttime chemistry at a high altitude site above Hong Kong
      Personal Author:
      Brown, S. S.; Dube, W. P.; Tham, Y. J.; Zha, Q. Z.; Xue, L. K.; Poon, S.; Wang, Z.; Blake, D. R.; Tsui, W.; Parrish, D. D.; Wang, T.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Atmospheres, 121(5), 2457-2475.
      Description:
      Nighttime reactions of nitrogen oxides influence ozone, volatile organic compounds, and aerosol and are thus important to the understanding of regional air quality. Despite large emissions and rapid recent growth of nitrogen oxide concentrations, the...
      File Type:
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    10. Derivation of Soil Moisture Recovery Relation Using Soil Conservation Service (SCS) Curve Number Method
      Personal Author:
      Kim, J.; Johnson, L. E.; Cifelli, R.; Choi, J.; Chandrasekar, V.;
      Published Date:
      2018
      Source:
      Water, 10(7), 21.
      Description:
      Soil moisture retention (SMR) capacity plays a key role in estimating the direct runoff when a multi-pulse storm event occurs. It is very important to know how much SMR will be recovered during the intervals of no rain of a multi-pulse storm. This st...
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      Filetype[PDF - 7.02 MB]
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      Personal Author:
      Fairall, C. W.; Matrosov, S. Y.; Williams, C. R.; Walsh, E. J.;
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      2018
      Source:
      Journal of Atmospheric and Oceanic Technology, 35(3), 593-608.
      Description:
      The NOAA W-band radar was deployed on a P-3 aircraft during a study of storm fronts off the U.S. West Coast in 2015 in the second CalWater (CalWater-2) field program. This paper presents an analysis of measured equivalent radar reflectivity factor Z(...
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      Mahish, M.; Jefferson, A.; Collins, D. R.;
      Published Date:
      2018
      Source:
      Atmosphere, 9(2), 18.
      Description:
      A 4-year record of aerosol size and hygroscopic growth factor distributions measured at the Department of Energy's Southern Great Plains (SGP) site in Oklahoma, U.S. were used to estimate supersaturation (S)-dependent cloud condensation nuclei concen...
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      Mahoney, K.; Swales, D.; Mueller, M. J.; Alexander, M.; Hughes, M.; Malloy, K.;
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      2018
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      Journal of Climate, 31(16), 6281-6297.
      Description:
      Atmospheric rivers (ARs) are well-known producers of precipitation along the U.S. West Coast. Depending on their intensity, orientation, and location of landfall, some ARs penetrate inland and cause heavy rainfall and flooding hundreds of miles from ...
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    14. Detecting changes in Arctic methane emissions: limitations of the inter-polar difference of atmospheric mole fractions
      Personal Author:
      Dimdore-Miles, O. B.; Palmer, P. I.; Bruhwiler, L. P.;
      Published Date:
      2018
      Source:
      Atmospheric Chemistry and Physics, 18(24), 17895-17907.
      Description:
      We consider the utility of the annual inter-polar difference (IPD) as a metric for changes in Arctic emissions of methane (CH4). The IPD has been previously defined as the difference between weighted annual means of CH4 mole fraction data collected a...
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    15. Widespread Reemergence of Sea Surface Temperature Anomalies in the Global Oceans, Including Tropical Regions Forced by Reemerging Winds
      Personal Author:
      Byju, P.; Dommenget, D.; Alexander, M. A.;
      Published Date:
      2018
      Source:
      Geophysical Research Letters, 45(15), 7683-7691.
      Description:
      Sea surface temperature anomalies (SSTA) in portions of the extratropics are known to recur from one winter to the next without persisting through the intervening summer. Previous studies identified only a limited number of midlatitude regions where ...
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      Personal Author:
      Richardson, K.; Asmutis-Silvia, R.; Drinkwin, J.; Gilardi, K. V. K.; Giskes, I.; Jones, G.; O'Brien, K.; Pragnell-Raasch, H.; Ludwig, L.; Antonelis, K.; Barco, S.; Henry, A.; Knowlton, A.; Landry, S.; Mattila, D.; MacDonald, K.; Moore, M.; Morgan, J.; Robbins, J.; van der Hoop, J.; Hogan, E.;
      Published Date:
      2019
      Source:
      Marine Pollution Bulletin, 138, 222-229.
      Description:
      Abandoned, lost or discarded fishing gear (ALDFG) comprises a significant amount of global marine debris, with diverse impacts to marine environments, wildlife, and the fishing industry. Building evidence on ALDFG is critical to holistically understa...
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    17. Episodic Reversal of Autumn Ice Advance Caused by Release of Ocean Heat in the Beaufort Sea
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      Smith, M.; Stammerjohn, S.; Persson, O.; Rainville, L.; Liu, G. Q.; Perrie, W.; Robertson, R.; Jackson, J.; Thomson, J.;
      Published Date:
      2018
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      Journal of Geophysical Research-Oceans, 123(5), 3164-3185.
      Description:
      High-resolution measurements of the air-ice-ocean system during an October 2015 event in the Beaufort Sea demonstrate how stored ocean heat can be released to temporarily reverse seasonal ice advance. Strong on-ice winds over a vast fetch caused mixi...
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    18. Characterization of organic residues of size-resolved fog droplets and their atmospheric implications
      Personal Author:
      Chakraborty, A.; Ervens, B.; Gupta, T.; Tripathi, S. N.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Atmospheres, 121(8), 4317-4332.
      Description:
      Size-resolved fog water samples were collected in two consecutive winters at Kanpur, a heavily polluted urban area of India. Samples were analyzed by an aerosol mass spectrometer after drying and directly in other instruments. Residues of fine fog dr...
      File Type:
      Filetype[PDF - 724.45 KB]
    19. Sources, seasonality, and trends of southeast US aerosol: an integrated analysis of surface, aircraft, and satellite observations with the GEOS-Chem chemical transport model
      Personal Author:
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      Published Date:
      2015
      Source:
      Atmos. Chem. Phys., 15(18), 10411-10433.
      File Type:
      Filetype[PDF - 4.19 MB]
    20. Characterization of cumulus cloud fields using trajectories in the center of gravity versus water mass phase space: 1. Cloud tracking and phase space description
      Personal Author:
      Heiblum, R. H.; Altaratz, O.; Koren, I.; Feingold, G.; Kostinski, A. B.; Khain, A. P.; Ovchinnikov, M.; Fredj, E.; Dagan, G.; Pinto, L.; Yaish, R.; Chen, Q.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Atmospheres, 121(11), 6336-6355.
      Description:
      We study the evolution of warm convective cloud fields using large eddy simulations of continental and trade cumulus. Individual clouds are tracked a posteriori from formation to dissipation using a 3-D cloud-tracking algorithm, and results are prese...
      File Type:
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