References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-10-22279-2010

A sea-state based source function for size- and composition-resolved marine aerosol production

Long

M. S.

¹ Keene

W. C.

¹ Kieber

D. J.

² Erickson

D. J.

³ Maring

⁴

Department of Environmental Sciences, University of Virginia, Charlottesville, VA, USA

Department of Chemistry, College of Environmental Science and Forestry, State University of New York, Syracuse, NY, USA

Computer Science and Mathematics Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA

NASA Headquarters: Radiation Sciences Program, Washington DC, USA

28 09 2010

10 9 22279 22315

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A parameterization for the size- and composition-resolved production fluxes of nascent marine aerosol was developed from prior experimental observations and extrapolated to ambient conditions based on estimates of air entrainment by the breaking of wind-driven ocean waves. Production of particulate organic carbon (OCaer) was parameterized based on Langmuir equilibrium-type association of organic matter to bubble plumes in seawater and resulting aerosol as constrained by measurements of aerosol produced from productive and oligotrophic seawater. This novel approach is the first to parameterize size- and composition-resolved aerosol production based on explicit evaluation of wind-driven air entrainment/detrainment fluxes and chlorophyll-a as a proxy for surfactants in surface seawater. Production fluxes were simulated globally with an eight aerosol-size-bin version of the NCAR Community Atmosphere Model (CAM v3.5.07). Simulated production fluxes fell within the range of published estimates based on observationally constrained parameterizations. Because the parameterization does not consider contributions from spume drops, the simulated global mass flux (1.5×103 Tg y−1) is near the lower end of published estimates. The simulated production of aerosol number (1.4×106 cm−2 s−1) and OCaer (29 Tg C y−1) fall near the upper end of published estimates and suggest that primary marine aerosols may have greater influences on the physicochemical evolution of the troposphere, radiative transfer and climate, and associated feedbacks on the surface ocean than suggested by previous model studies.

References 1

% vor jede Referenz Andreae, M. O. and Rosenfeld, D.: Aerosol-cloud-precipitation interactions. Part 1. The nature and sources of cloud-active aerosols, Earth Sci. Rev., 89, 13–41, 2008.

Andreas, E. L, Edson, J. B., Monahan, E. C., Rouault, M. P., and Smith, S.D.: The spray contribution to net evaporation from the sea: A review of recent progress, Bound.-Lay. Meteorol., 72, 3–52, 1995.

Blenkinsopp, C. E. and Chaplin, J. R.: Void fraction measurements in breaking waves, Proc. Royal Soc. A, 463(2088), 3151–3170, 2007.

Carlson, C. A., Ducklow, H. W., and Michaels, A. F.: Annual flux of dissolved organic carbon from the euphotic zone in the northwestern Sargasso Sea, Nature, 371, 405–408, 1994.

Chameides, W. L. and Stelson, A. W.: Aqueous-phase chemical processes in deliquescent sea salt aerosols: A mechanism that couples the atmospheric cycles of S and sea salt, J. Geophys. Res., 97, 20565–20580, 1992.

Clarke, A. D., Owens, S. R., and Zhou, J.: An ultrafine sea salt flux from breaking waves: Implications for cloud condensation nuclei in the remote marine atmosphere, J. Geophys. Res., 111, D06202, doi:10.1029/2005JD006565, 2006.

Deane, G. B.: Sound generation and air entrainment by breaking waves in the surf zone, J. Acoust. Soc. Am., 102(5), 2671–2689, 1997.

Deane, G. B. and Stokes, M. D.: Entrainment processes and bubble size distributions in the surf zone, J. Geophys. Res., 29, 1393–1403, 1999.

Decesari, S., Facchini, M. C., Mircea, M., Cavalli, F., Emblico, L., Fuzzi, S., Moretti, F., and Tagliavini, E.: Source attribution of water-soluble organic aerosol by nuclear magnetic resonance spectroscopy, Environ. Sci. Technol., 41, 2479–2484, 2007.

Doval, M. and Hansell, D. A.: Organic carbon and apparent oxygen utilization in the western South Pacific and central Indian Oceans, Mar. Chem., 68, 249–264, 2000.

Erickson, D. J., Seuzaret, C., Keene, W. C., and Gong, S.-L.: A general circulation model calculation of HCl and ClNO2 production from sea salt dechlorination: Reactive Chlorine Emissions Inventory, J. Geophys. Res., 104, 8347–8372, 1999.

Facchini, M. C., Rinaldi, M., Decesari, S., Carbone, C., Finessi, E., Mircea, M., Fuzzi, S., Ceburnis, D., Flanagan, R., Nilsson, E. D., de Leeuw, G., Martino, M., Woeltjen, J., and O'Dowd, C. D.: Primary submicron marine aerosol dominated by insoluble organic colloids and aggregates, Geophys. Res. Lett., 35, L17814, doi:10.1029/2008GL034210, 2008.

Fairall, C. W., Banner, M. L., Peirson, W. L., Asher, W., and Morison, R. P.: Investigation of the physical scaling of sea spray spume droplet production, J. Geophys. Res., 114, C10001, doi:10.1029/2008JC004918, 2009.

Felizardo, F. C. and Melville, W. K.: Correlations between ambient noise and the ocean surface wave field, J. Phys. Oceanogr., 25, 513–532, 1995.

Gantt, B., Meskhidze, N., and Kamykowski, D.: A new physically-based quantification of marine isoprene and primary organic aerosol emissions, Atmos. Chem. Phys., 9, 4915–4927, doi:10.5194/acp-9-4915-2009, 2009.

Geever, M., O'Dowd, C. D., van Ekeren, S., Flanagan, R., Nilsson, E. D., de Leeuw, G., and Rannik, U.: Submicron sea spray fluxes, Geophys. Res. Lett., 32, L15810, doi:10.1029/2005GL023081, 2005.

Gent, P. R., Yeager, S. G., Neale, R. B., Levis, S., and Bailey, D. A.: Improvements in a half degree atmosphere/land version of the CCSM, Clim. Dynam., 34(6), 819–833, doi:10.1007/s00382-009-0614-8, 2009.

Ghosh, P.: Coalescence of air bubbles at air-water interface, Chem. Eng. Res. Des., 82, 849–854, 2004.

Giribabu, K. and Ghosh, P.: Adsorption of nonionic surfactants at fluid–fluid interfaces: importance in the coalescence of bubbles and drops, Chem. Eng. Sci., 62, 3057–3067, 2007.

Gong, S. L.: A parameterization of sea salt aerosol source function for sub- and super-micron particles,~Global Biogeochem. Cy., 17, 1097, doi:10.1029/2003gb002079, 2003.

Gong, S. L., Barrie, L. A., and Lazare, M.: Canadian Aerosol Module (CAM): A size-segregated simulation of atmospheric aerosol processes for climate and air quality models 2. Global sea-salt aerosol and its budgets, J. Geophys. Res., 107, 4779, doi:10.1029/2001JD002004, 2002.

de Gouw, J. A., Middlebrook, A. M., Warneke, C., Goldan, P. D., Kuster, W. C., Roberts, J. M., Fehsenfeld, F. C., Worsnop, D. R., Canagaratna, M. R., Pszenny, A. A. P., Keene, W. C., Marchewka, M., Bertman, S. B., and Bates, T. S.: Budget of organic carbon in a polluted atmosphere: Results from the New England Air Quality Study in 2002, J. Geophys. Res., 110, D16305, doi:10.1029/2004JD005623, 2005.

Gregg, W. W.: Assimilation of SeaWIFS global ocean chlorophyll data into a three-dimensional global ocean model, J. Mar. Sys., 69, 205–225, 2008.

Gregg, W. W. and Casey, N. W.: Global and regional evaluation of the SeaWiFS chlorophyll Data Set, Remote Sens. Environ., 93, 463–479, 2004.

Hanson, J. L. and Phillips, O. M.: Wind sea growth and dissipation in the open ocean, J. Phys. Oceanogr., 29(8), 1633–1648, 1999.

Hoffman, E. J. and Duce, R. A.: Factors influencing the organic carbon content of marine aerosols: A laboratory study, J. Geophys. Res., 81, 3667–3670, 1976.

Hoque, A.: Air Bubble Entrainment by Breaking Waves and Associated Energy Dissipation, Ph.D. Thesis, Toyohashi University of Technology, 2002.

Hultin, K. A. H., Nilsson, E. D., Krejci, R., Mårtinsson, E. M., Ehn, K., Hagström, Å., and de Leeuw, G.: In situ laboratory sea spray production during the MAP 2006 cruise on the North East Atlantic, J. Geophys. Res., 115, D06201, doi:10.1029/2009JD012522, 2009.

James, C. and Lang, S. P.: Truncating criteria for polynomial curve fitting, J. Phys. D: Appl. Phys., 4, 357–363, 1971.

Keene, W. C., Maring, H., Kieber, D. J., Maben, J. R., Pszenny, A. A. P., Dahl, E. E., Izaguirre, M. A., Davis, A. J., Long, M. S., Zhou, X., Smoydzin, L., von Glasow, R., and Sander, R.: Chemical and physical characteristics of nascent aerosols produced by bursting bubbles at a model air-sea interface, J. Geophys. Res., 112, D21202, doi:10.1029/2007JD008464, 2007.

Lamarre, E. and Melville, W. K.: Air entrainment and dissipation in breaking waves, Nature, 351, 469–472, 1991.

Langmann, B, Scannell, C., and O'Dowd, C.: New directions: Organic matter contribution to marine aerosols and cloud condensation nuclei, Atmos. Environ., 42, 7821–7822, doi:10.1029/2007JD008464, 2008.

Lewis, R. and Schwartz, S. E.: Sea Salt Aerosol Production: Mechanisms, Methods, Measurements, and Models – A Critical Review, Geophysical monograph 152, American Geophysical Union, Washington, DC, 413~pp., 2008.

Loewen, M. R. and Melville, W. K.: An experimental investigation of the collective oscillations of bubble plumes entrained by breaking waves, J. Acoust. Soc. Am., 95, 1329–1343, 1993.

Mårtensson, E. M., Nilsson, E. D., deLeeuw, G., Cohen, L. H., and Hansson, H.-C.: Laboratory simulations and parameterization of the primary marine aerosol production, J. Geophys. Res., 108, 4297, doi:10.1029/2002JD002263, 2003.

Melville, W. K. and Rapp, R. J.: Momentum Flux in Breaking Waves, Nature, 317, 514–516, 1985.

Meskhidze, N. and Nenes, A.: Phytoplankton and cloudiness in the southern ocean, Science, 314, 1419–1423, 2006.

Monahan, E. C. and O'Muircheartaigh, I. G.: Whitecaps and the passive remote-sensing of the ocean surface, Int. J. Remote Sens., 7, 627–642, 1986.

Monahan, E. C., Spiel, D. E., and Davidson, K. L.: A model of marine aerosol generation via whitecaps and wave disruption, in Oceanic Whitecaps, edited by: Monahan, E. and Niocaill, G. M., D. Reidel, Norwell, Mass, 167–174, 1986.

O'Dowd, C. D., Smith, M. H., Consterdine, I. E., and Lowe, J. A.: Marine aerosol, sea-salt, and the marine sulphur cycle: A short review, Atmos. Environ., 31, 73–80, 1997.

O'Dowd, C. D., Facchini, M. C., Cavalli, F., Cebrunis, D., Mircea, M., Decesari, S., Fuzzi, S., Yoon, Y. J., and Putard, J.-P.: Biogenically driven organic contribution to marine aerosol, Nature, 431, 676–680, 2004.

O'Dowd , C. D., Langmann, B., Varghese, S., Scannell, C., Ceburnis, D., and Facchini, M. C.: A combined organic-inorganic sea-spray source function, Geophys. Res. Lett., 35, L01801, doi:10.1029/2007GL030331, 2008.

Pierce, J. R. and Adams, P. J.: Global evaluation of CCN formation by direct emission of sea salt and growth of ultrafine sea-salt, J. Geophys. Res., 111, D06203, doi:10.1029/20005JD006186, 2006.

Roelofs, G. J.: A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation, Atmos. Chem. Phys., 8, 709–719, doi:10.5194/acp-8-709-2008, 2008.

Russell, L. M., Mensah, A. A., Fischer, E. V., Sive, B. C., Varner, R. K., Keene, W. C., Stutz, J., and Pszenny, A. A. P.: Nanoparticle growth following photochemical $\alpha $- and $\beta $-pinene oxidation at Appledore Island during International Consortium for Research on Transport and Transformation/Chemistry of Halogens at the Isles of Shoals 2004, J. Geophys. Res., 112, D10S21, doi:10.1029/2006JD007736, 2007.

Scatchard, G.: Equilibrium thermodynamics and biological chemistry, Science, 95, 27–32, 1942.

Schkolnik, G., Chand, D., Hoffer, A., Andreae, M., Erlick, C., Swietlicki, E., and Rudich, Y.: Constraining the density and complex refractive index of elemental and organic carbon in biomass burning aerosol using optical and chemical measurements, EOS Trans. AGU, 87(52), Fall Meeting Suppl., Abstract A43A-0107, 2006.

Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: from air pollution to climate change – 2nd ed., John Wiley and Sons, Inc, Hoboken, 2006.

Sellegri, K., O'Dowd, C. D., Yoon, Y. J., Jennings, S. G., and de Leeuw, G.: Surfactants and submicron sea spray generation, J. Geophys. Res., 111, D22215, doi:10.1029/2005JD006658, 2006.

Spracklen, D. V., Arnold, S. R., Carslaw, K. S., Sciare, J., and Pio, C.: Globally significant oceanic source of organic carbon aerosol, Geophys. Res. Lett., 35, L12811, doi:10.1029/2008GL033359, 2008.

Stefan, R. L. and Szeri, A. J.: Surfactant scavenging and surface deposition by rising bubbles, J. Coll. Interface Sci., 212, 1–13, 1999.

Thorpe, S. A.: On the cloud of bubbles formed by a breaking wind-wave in deep water, and their role in air-sea gas transfer, Philos. T. Roy. Soc. London, 304A, 155–210, 1982.

Toba, Y., Okada, K., and Jones, I. S. F.: The response of wind-wave spectra to changing winds. Part 1: Increasing winds, J. Phys. Oceanogr., 18, 1231–1240, 1988.

Tseng, R.-S., Viechnicki, J. T., Skop, R. A., and Brown, J. W.: Sea-to-air transfer of surface-active organic compounds by bursting bubbles, J. Geophys. Res., 97, 5201–5206, 1992.

Turekian, V., Macko, S. A., and Keene, W. C.: Concentrations, isotopic compositions, and sources of size-resolved, particulate organic carbon and oxalate in near-surface marine air at Bermuda during spring, J. Geophys. Res., 108, D4157, doi:10.1029/2002JD002053, 2003.

Turpin, B. J. and Lim, H.: Species contributions to PM2.5 mass concentrations: Revisiting common assumptions for estimating organic mass, Aerosol Sci. Technol., 35, 602–610, 2010.

Tyree, C. A., Hellion, V. M., Alexandrova, O. A., and Allen, J. O.: Foam droplets generated from natural and artificial seawaters, J. Geophys. Res., 112, D12204, doi:10.1029/2006JD007729, 2007.

von Glasow, R. and Crutzen, P. J.: Model study of multiphase DMS oxidation with a focus on halogens, Atmos. Chem. Phys., 4, 589–608, doi:10.5194/acp-4-589-2004, 2004.

Zhou X., Davis, A. J., Kieber, D. J., Keene, W. C., Maben, J. R., Maring, H., Dahl, E. E., Izaguirre, M. A., Sander, R., and Smoydzyn, L.: Photochemical production of hydroxyl radical and hydroperoxides in water extracts of nascent marine aerosols produced by bursting bubbles from Sargasso seawater, Geophys. Res. Lett., 35, L20803, doi:10.1029/2008GL035418, 2008.

Zutic, V. and Legovic, T.: Relationship between phytoplankton blooms and dissolved organic matter in the northern Adriatic, in Final Reports on Research Projects Dealing with Eutrophication and Plankton Blooms (Activity H), MAP Technical Reports Series no 37, 53–66, United Nations Environment Programme (UNEP), Athens (Greece), 1990.