Atmospheric Chemistry and Physics Discussions
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10.5194/acpd-8-4831-2008
http://www.atmos-chem-phys-discuss.net/8/4831/2008/
http://www.atmos-chem-phys-discuss.net/8/4831/2008/acpd-8-4831-2008.html
http://www.atmos-chem-phys-discuss.net/8/4831/2008/acpd-8-4831-2008.pdf
4831
4876
2008-03-05
Characterization of the South Atlantic marine boundary layer aerosol using an Aerodyne Aerosol Mass Spectrometer
S. R. Zorn
zorns@mpch-mainz.mpg.de
F. Drewnick
M. Schott
T. Hoffmann
S. Borrmann
Max Planck Institute for Chemistry, Particle Chemistry Department, Mainz, Germany
University of Mainz, Institute for Atmospheric Physics, Mainz, Germany
University of Mainz, Institute of Inorganic and Analytical Chemistry, Mainz, Germany
Measurements of the submicron fraction of the atmospheric aerosol in the
marine boundary layer were performed from January to March 2007 (Southern
Hemisphere summer) onboard the French research vessel Marion Dufresne in the
Southern Atlantic and Indian Ocean (20° S–60° S,
70° W–60° E). For chemical composition measurements an Aerodyne
High-Resolution-Time-of-Flight AMS was used to measure mass concentrations
and species-resolved size distributions of non-refractory aerosol components
in the submicron range.
<br><br>
Within the "standard" AMS compounds (ammonium,
chloride, nitrate, sulfate, organics) "sulfate" is the dominating species in
the marine boundary layer reaching concentrations between 50 ng m<sup>−3</sup> and
3 μg m<sup>−3</sup>. Furthermore, what is seen as "sulfate" by the AMS seems
to be mostly sulfuric acid. Another sulfur containing species that can
ubiquitously be found in marine environments is methanesulfonic acid (MSA).
Since MSA has not been directly measured before with an AMS, and is not part
of the standard AMS analysis, laboratory experiments needed to be performed
in order to be able to identify it within the AMS raw data and to extract
mass concentrations for MSA from the field measurements. To identify
characteristic air masses and their source regions backwards trajectories
were used and averaged concentrations for AMS standard compounds were
calculated for each air mass type. Sulfate mass size distributions were
measured for these periods showing a distinct difference between oceanic air
masses and those from African outflow. While the peak size in the mass
distribution was roughly 250 nm in marine air masses it was shifted to 470 nm in African outflow
air. Correlations between the mass concentrations of sulfate, organics and
MSA were calculated which show a narrow correlation for MSA with
sulfate/sulfuric acid coming from the ocean but not with continental sulfate.
Allan, J. D., Delia, A. E., Coe, H., Bower, K. N., Alfarra, M. R., Jimenez, J. L., Middlebrook, A. M., Drewnick, F., Onasch, T. B., Canagaratna, M. R., Jayne, J. T., and Worsnop, D. R.: A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data, J. Aerosol Sci., 35, 909–922, 2004.
Bates, T. S., Quinn, P. K., Coffman, D. J., Johnson, J. E., and Middlebrook, A. M.: Dominance of organic aerosols in the marine boundary layer over the Gulf of Maine during NEAQS 2002 and their role in aerosol light scattering, J. Geophys. Res., 110, D18202, doi:10.1029/2005JD005797, 2005.
Bonsang, B., Polle, C., and Lambert, G.: Evidence for marine production of isoprene, Geophys. Res. Lett., 19, 1129–1132, 1992.
Charlson, R. J., Lovelock, J. E., Andreae, M. O., and Warren, S. G.: Oceanic phytoplankton, atmospheric sulphur, cloud albedo and climate, Nature, 326, 655–661, 1987.
Chasteen, T. G. and Bentley, R.: Volatile Organic Sulfur Compounds of Environmental Interest: Dimethyl Sulfide and Methanethiol. An Introductory Overview, J. Chem. Educ., 81, 1524–1528, 2004.
Coe, H., Allan, J. D., Alfarra, M. R., Bower, K. N., Flynn, M. J., McFiggans, G. B., Topping, D. O., Williams, P. I., O'Dowd, C. D., Dall'Osto, M., Beddows, D. C. S., and Harrison, R. M.: Chemical and physical characteristics of aerosol particles at a remote coastal location, Mace Head, Ireland, during NAMBLEX, Atmos. Chem. Phys., 6, 3289–3301, 2006.
Dall'Osto, M., Beddows, D. C. S., Kinnersley, R. P., Harrison, R. M., Donovan, R. J., and Heal, M. R.: Characterization of individual airborne particles by using aerosol time-of-flight mass spectrometry at Mace Head, Ireland, J. Geophys. Res., 109, D21302, doi:10.1029/2004JD004747, 2004.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop,, D. R., and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, 2006.
Drewnick, F., Hings, S. S., DeCarlo, P. F., Jayne, J. T., Gonin, M., Fuhrer, K., Weimer, S., Jimenez, J. L., Demerjian, K. L., Borrmann, S., and Worsnop, D. R.: A New Time-of-Flight Aerosol Mass Spectrometer (TOF-AMS) – Instrument Description and First Field Deployment, Aerosol Sci. Technol., 39, 637–658, 2005.
Gieray, R., Wieser, P., Engelhardt, T., Swietlicki, E., Hansson, H.-C., Mentes, B., Orsini, D., Martinsson, B., Svenningsson, B., Noone, K. J., and Heintzenberg, J.: Phase Partitioning of Aerosol Constituents in Cloud Based on Single-Particle and Bulk Analysis, Atmos. Environ., 31, 2491–2502, 1997.
Hinds, W. C.: Aerosol Technology: Properties, Behavior and Measurment of Airborne Particles, 2nd ed., Wiley-Interscience, 1998.
Hings, S. S., Walter, S., Schneider, J., Borrmann, S., and Drewnick, F.: Comparison of a quadrupole and a time-of-flight aerosol mass spectrometer during the Feldberg aerosol characterization experiment 2004, Aerosol Sci. Technol., 41, 679–691, 2007.
Huffman, J. A., Jayne, J. T., Drewnick, F., Aiken, A. C., Onasch, T., Worsnop, D. R., and Jimenez, J. L.: Design, modeling, optimization, and experimental tests of a particle beam width probe for the aerodyne aerosol mass spectrometer, Aerosol Sci. Technol., 39, 1143–1163, 2005.
Kulmala, M.: How particles nucleate and grow, Science, 302, 1000–1001, 2003.
Lovelock, J. E., Maggs, R. J., and Wade, R. J.: Halogenated Hydrocarbons in and over the Atlantic, Nature, 241, 194–196, 1973.
Mäkelä, J. M., Hoffmann, T., Holzke, C., Väkevä, M., Suni, T., Mattila, T., Aalto, P. P., Tapper, U., Kaupinnen, E. I., and O'Dowd, C. D.: Biogenic emissions and identification of end-products in coastal ultrafine particles during nucleation bursts, J. Geophys. Res., 107(D19), 8110, doi:10.1029/2001JD000580, 2002.
Meskhidze, N. and Nenes, A.: Phytoplankton and Cloudiness in the Southern Ocean, Science, 314, 1419–1423, 2006.
Murphy, D. M., Thomson, D. S., Middlebrook, A. M., and Schein, M. E.: In situ single-particle characterization at Cape Grim, J. Geophys. Res., 103, 16485–16491, 1998.
NIST Mass Spec Data Center: Stein, S. E., director, Mass Spectra, NIST Chemistry WebBook, NIST Standard Reference Database Number 69, edited by: Linstrom, P. J. and Mallard, W. G., National Institute of Standards and Technology, Gaithersburg MD, 20899, http://webbook.nist.gov/, 2005.
Phinney, L., Leaitch, W. R., Lohmann, U., Boudries, H., Worsnop, D. R., Jayne, J. T., Toom-Sauntry, D., Wadleigh, M., Sharma, S., and Shantz, N.: Characterization of the aerosol over the sub-arctic north east Pacific Ocean, Deep-Sea Res. II, 53, 2410–2433, 2006.
Putaud, J. P., Davison, B. M., Watts, S. F., Mihalopoulos, N., Nguyen, B. C., and Hewitt, C. N.: Dimethylsulfide and its oxidation products at two sites in Brittany (France), Atmos. Environ., 33, 647–659, 1999.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, 2nd ed., Wiley-Interscience, 2006.
Sodemann, H., Palmer, A. S., Schwierz, C., Schwikowski, M., and Wernli, H.: The transport history of two Saharan dust events archived in an Alpine ice core, Atmos. Chem. Phys., 6, 667–688, 2006.
Topping, D., Coe, H., McFiggans, G., Burgess, R., Allan, J. D., Alfarra, M. R., Bower, K., Choularton, T. W., Decesari, S., and Facchini, M. C.: Aerosol chemical characteristics from sampling conducted on the Island of Jeju, Korea during ACE Asia, Atmos. Environ., 38, 2111–2123, 2004.
von Glasow, R. and Crutzen, P. J.: Model study of multiplephase DMS oxidation with a focus on halogens, Atmos. Chem. Phys., 4, 589–608, 2004.
Wernli, H. and Davies, H. C.: A lagrangian-based analysis of extratropical cyclones. I: The method and some applications, Q. J. Roy. Meteor. Soc., 123, 467–489, 1997.
Zhang, Q., Alfarra, M. R., Worsnop, D. R., Allan, J. D., Coe, H., Canagaratna, M. R., and Jimenez, J. L.: Deconvolution and quantification of hydrocarbon-like and oxygenated organic aerosols based on aerosol mass spectrometry, Environ. Sci. Technol., 39, 4938–4952, 2005.