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Published May 7, 2013 | Supplemental Material + Published
Journal Article Open

Bringing the ocean into the laboratory to probe the chemical complexity of sea spray aerosol

Abstract

The production, size, and chemical composition of sea spray aerosol (SSA) particles strongly depend on seawater chemistry, which is controlled by physical, chemical, and biological processes. Despite decades of studies in marine environments, a direct relationship has yet to be established between ocean biology and the physicochemical properties of SSA. The ability to establish such relationships is hindered by the fact that SSA measurements are typically dominated by overwhelming background aerosol concentrations even in remote marine environments. Herein, we describe a newly developed approach for reproducing the chemical complexity of SSA in a laboratory setting, comprising a unique ocean-atmosphere facility equipped with actual breaking waves. A mesocosm experiment was performed in natural seawater, using controlled phytoplankton and heterotrophic bacteria concentrations, which showed SSA size and chemical mixing state are acutely sensitive to the aerosol production mechanism, as well as to the type of biological species present. The largest reduction in the hygroscopicity of SSA occurred as heterotrophic bacteria concentrations increased, whereas phytoplankton and chlorophyll-a concentrations decreased, directly corresponding to a change in mixing state in the smallest (60–180 nm) size range. Using this newly developed approach to generate realistic SSA, systematic studies can now be performed to advance our fundamental understanding of the impact of ocean biology on SSA chemical mixing state, heterogeneous reactivity, and the resulting climate-relevant properties.

Additional Information

© 2013 National Academy of Sciences. Edited by Mark H. Thiemens, University of California at San Diego, La Jolla, CA, and approved March 21, 2013 (received for review January 10, 2013). Published online before print April 25, 2013. This Direct Submission article had a prearranged editor. We thank Suresh Dhaniyala, Robert Pomeroy, Paul Harvey, and the entire staff of the Scripps Institution of Oceanography Hydraulics Laboratory for helpful discussions and technical development of the sealed wave-channel. This overall study was supported by the National Science Foundation (NSF) Center for Chemical Innovation, the Center for Aerosol Impacts on Climate and the Environment (CAICE) under Grant CHE1038028. Partial support was provided to CAICE collaborators for the intensive study measurements by NSF Grant ATM0837913 (to C.D.C. and S.D.F.), Office of Naval Research Grant N00014-10-1-0200 (to J.H.S., S.P.H., and W.M.), an NSF Graduate Research Fellowship (to C.J.E.), an Irving M. Klotz professorship (to F.M.G.), NSF PO Grant OCE-1155123 (to G.B.D.), Gordon and Betty Moore Foundation Marine Microbiology Initiative (to F.A.) and NSF Grant ATM0841602 (to P.J.D. and R.C.S.). Author contributions: K.A.P., T.H.B., V.H.G., and M.J.M. designed research; G.B.D., M.D.S., P.J.D., A.P.A., D.B.C., C.E.C., L.A.C.-R., C.J.E., S.D.F., T.L.G., M.J.K., R.L.M., W.M., M.J.R., O.S.R., R.C.S., and D.Z. performed research; G.B.D., M.D.S., L.I.A., B.P.P., F.A., J.H.S., G.C.R., L.M.R., W.F.L., B.E.P., and N.G.S. contributed new reagents/analytic tools; K.A.P., G.B.D., M.D.S., P.J.D., J.H.S., R.C.M., C.D.C., F.M.G., A.P.A., J.B., D.B.C., C.E.C., L.A.C.-R., C.J.E., T.L.G., S.P.H., W.M., M.J.R., R.C.S., and D.Z. analyzed data; and K.A.P., T.H.B., V.H.G., and C.D.C. wrote the paper.

Attached Files

Published - PNAS-2013-Prather-7550-5.pdf

Supplemental Material - pnas.201300262SI.pdf

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