Abstract
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO4 2−), sodium (Na+), ammonium (NH4 +), and nitrate (NO3 −) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m−3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m−3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.
The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m−3 (STP). The nonsea-salt sulfate (ns-SO4 2−) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO4 2− from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a ‘sea-salt inversion layer’ was reflected in the profiles of those aerosol components, e.g., Na+ and NO3 −, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently ‘remote’ northern hemispheric regions.
Similar content being viewed by others
References
Andreae, M. O., 1982, Marine aerosol chemistry at Cape Grim, Tasmania and Townsville, Queensland, J. Geophys. Res. 87, 8875–8885.
Andreae, M. O., 1985, The emission of sulfur to the remote atmosphere, in J. N., Galloway, R. J., Charlson, M. O., Andreae, and H., Rodhe (eds.), The Biogeochemical Cycling of Sulfur and Nitrogen in the Remote Atmosphere D. Reidel, Dordrecht, pp. 5–25.
Andreae, M. O., 1986, The ocean as a source of atmospheric sulfur compounds, in P., Buat-Ménard (ed.), The Role of Air-Sea Exchange in Geochemical Cycling, D. Reidel, Dordrecht, pp. 331–362.
Andreae, M. O. and Raemdonck, H., 1983. Dimethylsulfide in the surface ocean and the marine atmosphere: a global view, Science 221, 744–747.
Andreae, M. O., Ferek, R. J., Bermond, F., Byrd, K. P., Engstrom, R. T., Hardin, S., Houmere, P. D., LeMarrec, F., Raemdonck, H., and Chatfield, R. B., 1985, Dimethylsulfide in the marine atmosphere, J. Geophys. Res. 90, 12,891–12,900.
Appel, B. R., Wall, S. M., Tokiwa, Y. and Halk, M., 1980, Simultaneous nitric acid, particulate nitrate and acidity measurements in ambient air, Atmos. Environ. 14, 549–554.
Atkinson, R. J., Pitts, J. N.Jr., and Aschmann, S. M., 1984, Tropospheric reactions of dimethyl sulfide with NO3 and OH radicals, J. Phys. Chem. 88, 1584–1587.
Ayers, G. P., Ivey, J. P., and Goodman, H. S., 1986, Sulfate and methanesulfonate in the maritime aerosol at Cape Grim, Tasmania, J. Atmos. Chem. 4, 173–185.
Bates, T. S. and Cline, J. D., 1985, The role of the ocean in a regional sulfur cycle, J. Geophys. Res. 90, 9168–9172.
Bates, T. S., Cline, J. D., Gammon, R. H., and Kelly-Hansen, S. R., 1987, Regional and seasonal variations in the flux of oceanic dimethylsulfide to the atmosphere, J. Geophys. Res., 92, 2930–2938.
Blanchard, D. C., 1983, The production, distribution, and bacterial enrichment of the sea-salt aerosol, in P. S., Liss and W. G. N., Slinn (eds.), Air-Sea Exchange of Gases and Particles, D. Reidel, Dordrecht, pp. 407–454.
Blanchard, D. C. and Woodcock, A. H., 1980, The production, concentration, and vertical distribution of the sea-salt aerosol, Annals New York Acad. Sci., 338, 330–347.
Bonsang, B., Nguen, B. C., Gaudry, A., and Lambert, G., 1980, Sulfate enrichment in marine aerosols owing to biogenic gaseous sulfur compounds, J. Geophys. Res. 85, 7410–7416.
Church, T. M., Tramontano, J. M., Whelpdale, D. M., Andreae, M. O., Galloway, J. N., Keene, W. C., Knap, A. H., and Tokos, J., 1987, Atmospheric and precipitation chemistry over the North Atlantic Ocean; shipboard results from April–May 1984, J. Geophys. Res., to be submitted.
Crutzen, P. J. and Gidel, L. T., 1983, A two-dimensional photochemical model of the atmosphere. 2: The tropospheric budgets of the anthropogenic chlorocarbons CO, CH4, CH3Cl and the effect of various NO x sources on tropospheric ozone, J. Geophys. Res. 88, 6641–6661.
Darzi, M. and Winchester, J. W., 1982, Aerosol characteristics at Mauna Loa Observatory, Hawaii, after East Asian dust storm episodes, J. Geophys. Res. 87, 1251–1258.
Daum, P. H. and Leahy, D. F., 1983, The Brookhaven National Laboratory Filter Pack System for Collection and Determination of Air Pollutants, Brookhaven National Lab., Upton, NY, Informal Report BNL 31381R.
Evans, R. G., 1955, The Atomic Nucleus, McGraw-Hill, New York.
Ferek, R. J., Chatfield, R. B., and Andreae, M. O., 1986, Vertical distribution of dimethylsulfide in the marine atmosphere, Nature 320, 514–516.
Grosjean, D., 1984, Photooxidation of methyl sulfide, ethyl sulfide, and methanethiol, Environ. Sci. Technol., 18, 460–468.
Hatakeyama, S., Izumi, K., and Akimoto, H., 1985, Yield of SO2 and formation of aerosol in the photo-oxidation of DMS under atmospheric conditions, Atmos. Environ. 19, 135–141.
Herrmann, J. and Jaeschke, W., 1984, Measurements of H2S and SO2 over the Atlantic Ocean, J. Atmos. Chem. 1, 111–123.
Holmén, K. and Liss, P., 1984, Models for air-water gas transfer: an experimental investigation, Tellus 36B, 92–100.
Huebert, B. J. and Lazrus, A. L., 1980, Tropospheric gas-phase and particulate nitrate measurements, J. Geophys. Res. 85, 7322–7328.
John, W., Hering, S., Reischl, G., Sasaki, G., and Goren, S., 1983, Characteristics of Nuclepore filters with large pore size-II. Filtration properties, Atmos. Environ. 17, 373–382.
Klockow, D., Jablonski, B., and Niessner, R., 1979, Possible artifacts in filter sampling of atmospheric sulphuric acid and acidic sulphates, Atmos. Environ., 13, 1665–1676.
Kritz, M. A., 1982, Exchange of sulfur between the free troposphere, marine boundary layer and the sea surface, J. Geophys. Res. 87, 8795–8803.
Küchemann, D. and Weber, J., 1953, Aerodynamics of Propulsion, McGraw-Hill, New York.
Larson, R. E., 1973, Measurements of radioactive aerosol using thin plastic scintillators, Nucl. Instr. Meth. 108, 467–470.
Liu, S. C., McAfee, J. R., and Cicerone, R. J., 1984, Radon 222 and tropospheric vertical transport, J. Geophys. Res. 89, 7291–7297.
McLeod, H., Jourdain, J. L., Poulet, G., and Le, Bras, G., 1984, Kinetic study of reactions of some organic sulfur compounds with OH radicals, Atmos. Environ. 18, 2621–2626.
Maroulis, P. J., Torres, A. L., Goldberg, A. B., Bandy, A. R., 1980, Atmospheric SO2 measurements on project GAMETAG, J. Geophys. Res. 85, 7345–7349.
Merrill, J. T., Bleck, R., and Avila, L., 1985, Modeling atmospheric transport to the Marshall Islands, J. Geophys. Res. 90, 12,927–12,936.
Mopper, K. and Zika, R. G., 1986, Free amino acids in marine rains: evidence for oxidation and potential role in nitrogen cycling, Nature 325, 246–249.
National Research Council, 1983, Acid Deposition: Atmospheric Processes in Eastern North America, National Academy Press, Washington, D.C.
Nguyen, B. C., Bonsang, B., and Lambert, G., 1974, The atmospheric concentration of sulfur dioxide and sulfate aerosols over antarctic, subantarctic areas and oceans, Tellus 26, 241–249.
Nguyen, B. C., Bonsang, B., and Gaudry, A., 1983, The role of the ocean in the global atmospheric sulfur cycle, J. Geophys. Res. 88, 10,903–10,914.
Niki, H., Maker, P. D., Savage, C. M., and Breitenbach, L. P., 1983, An FTIP study of the mechanism of the reaction HO+CH3SCH3, Int. J. Chem. Kinet., 15, 647–654.
Parsons, T. R., Maita, Y., and Laili, C. M., 1984, A Manual of Chemical and Biological Methods for Seawater Analysis, Pergamon Press, New York, 173 p.
Polian, G., 1972, Mesures de la radioactivité atmosphérique naturelle par appareils alpha semi-automatiques, Report, CNRS, Gif-sur-Yvette, France.
Prospere, J. M., Savoie, D. L., Nees, R. T., Duce, R. A., and Merrili, J., 1985, Particulate sulfate and nitrate in the boundary layer over the North Pacific Ocean, J. Geophys. Res. 90, 10,586–10,596.
Saltzman, E. S., Gidel, L. T., Zika, R. G., Milne, P. J., Prospero, J. M., Savole, D. L., and Cooper, W. J., 1984, Acrosol chemistry of methane sulfonic acid, in L., Newman (ed.), Gas-Liquid Chemistry of Natural Waters, Brookhaven National Laboratory, Upton, NY, Report BNL 51757, pp. 53/1–8.
Saltzman, E. S., Savoic, D. L., Prospero, J. M., and Zika, R. G., 1985, Atmospheric methanesulfenic acid and non-sea-salt sulfate at Fanning and American Samoa, Geophys. Res. Lett. 12, 437–440.
Saltzman, E. S., Savoie, D. L., Prospero, J. M., and Zika, R. G., 1986, Methanesulfonic acid and non-sea-salt sulfate in Pacific air: regional and seasonal variations, J. Atmos. Chem. 4, 227–240.
Saltzman, E. S., Savoie, D. L., Zika, R. G., and Prospero, J. M., 1983, Methane sulfonic acid in the marine atmosphere, J. Geophys. Res. 88, 10,897–10,902.
Savoie, D. L., and Prospero, J. M., 1982, Particle size distribution of nitrate and sulfate in the marine atmosphere, Geophys. Res. Lett. 9, 1207–1210.
Talbot, R. W., Andreae, M. O., Andreae, T. W., and Harriss, R. C., 1987, Regional aerosol chemistry of the Amazon Basin, J. Geophys. Res., in press.
Tang, I. N., 1980, Deliquescence properties and particle size changes of hygroscopic aerosols, in K., Willeke (ed.), Generation of Aerosols, Ann Arbor Science Publishers, Ann Arbor, MI.
Van, Valin, C. C. and Luria, M., 1985, O3, CO, hydrocarbons and dimethyl sulfide over the western Atlantic Ocean, Eos 66, 833.
Wilkniss, P. E., Lamontagne, R. A., Larson, R. E., Swinnerton, J. R., Dickson, C. R., and Thompson, T., 1973, Atmospheric trace gases in the southern hemisphere, Nature Physical Science 245, 45–47.
Wine, P. H., Kreutter, N. M., Grump, C. A., and Ravishankara, A. R., 1981, Kinetics of OH reactions with the atmospheric sulfur compounds H2S, CH3SH, CH3SCH3 and CH3SSCH3, J. Phys. Chem. 85, 2660–2665.
Winer, A. M., Atkinson, R., and Pitís, J. N.Jr., 1984, Gaseous nitrate radical: possible nighttime atmospheric sink for biogenic organic compounds, Science 224, 156–159.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Andreae, M.O., Berresheim, H., Andreae, T.W. et al. Vertical distribution of dimethylsulfide, sulfur dioxide, aerosol ions, and radon over the Northeast Pacific Ocean. J Atmos Chem 6, 149–173 (1988). https://doi.org/10.1007/BF00048337
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1007/BF00048337