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AGU: Journal of Geophysical Research, Atmospheres

 

Keywords

  • sea salt particles
  • methanesulfonate
  • nss-sulfate

Index Terms

  • Atmospheric Composition and Structure: Cloud physics and chemistry
  • Atmospheric Composition and Structure: Chemical kinetic and photochemical properties
  • Atmospheric Composition and Structure: Aerosols and particles
  • Atmospheric Composition and Structure: Troposphere: composition and chemistry
  • Atmospheric Composition and Structure: Middle atmosphere: composition and chemistry
Abstract
Cited By (0)
 

Abstract

Chemical speciation of sulfur in marine cloud droplets and particles: Analysis of individual particles from the marine boundary layer over the California current

Rebecca J. Hopkins

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, USA

Yury Desyaterik

William R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington, USA

Alexei V. Tivanski

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, USA

Rahul A. Zaveri

Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland, Washington, USA

Carl M. Berkowitz

Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland, Washington, USA

Tolek Tyliszczak

Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California, USA

Mary K. Gilles

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, USA

Alexander Laskin

William R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington, USA

Detailed chemical speciation of the dry residue particles from individual cloud droplets and interstitial aerosol collected during the Marine Stratus Experiment (MASE) was performed using a combination of complementary microanalysis techniques. Techniques include computer controlled scanning electron microscopy with energy dispersed analysis of X rays (CCSEM/EDX), time-of-flight secondary ionization mass spectrometry (TOF-SIMS), and scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Samples were collected at the ground site located in Point Reyes National Seashore, approximately 1 km from the coast. This manuscript focuses on the analysis of individual particles sampled from air masses that originated over the open ocean and then passed through the area of the California current located along the northern California coast. On the basis of composition, morphology, and chemical bonding information, two externally mixed, distinct classes of sulfur containing particles were identified: chemically modified (aged) sea salt particles and secondary formed sulfate particles. The results indicate substantial heterogeneous replacement of chloride by methanesulfonate (CH3SO3 −) and non-sea-salt sulfate (nss-SO4 2−) in sea-salt particles with characteristic ratios of nss-S/Na > 0.10 and CH3SO3 −/nss-SO4 2− > 0.6.

Received 11 May 2007; accepted 16 November 2007; published 27 February 2008.

Citation: Hopkins, R. J., Y. Desyaterik, A. V. Tivanski, R. A. Zaveri, C. M. Berkowitz, T. Tyliszczak, M. K. Gilles, and A. Laskin (2008), Chemical speciation of sulfur in marine cloud droplets and particles: Analysis of individual particles from the marine boundary layer over the California current, J. Geophys. Res., 113, D04209, doi:10.1029/2007JD008954.

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