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Title: Chemical Speciation of Sulfur in Marine Cloud Droplets and Particles: Analysis of Individual Particles from the Marine Boundary Layer Over the California Current

Abstract

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 complementary combination of 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 (TOFSIMS), 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 an air mass that originated over the open ocean and then passed through the area of the California current located along the northern California coast. Based on 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-SO42-) in sea-salt particles with the characteristic ratios of CH3SO3-/nss-SO42-> 0.6. Although this value seems too high for a mid-latitude site, our model calculations suggest that high CH3SO3-/nss-SO42- ratios are expected during the early stagesmore » of dimethyl sulfide (DMS) oxidation when CH3SO3H forms more rapidly than H2SO4.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
985029
Report Number(s):
PNNL-SA-55376
Journal ID: ISSN 0148-0227; 19792; KP1704020; TRN: US201016%%1722
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Geophysical Research
Additional Journal Information:
Journal Volume: 113; Journal Issue: d4; Journal ID: ISSN 0148-0227
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; ABSORPTION; AEROSOLS; BONDING; BOUNDARY LAYERS; CHLORIDES; CLOUDS; DIMETHYL SULFIDE; FINE STRUCTURE; INTERSTITIALS; IONIZATION; MASS SPECTROSCOPY; MICROANALYSIS; MICROSCOPY; MORPHOLOGY; OXIDATION; RESIDUES; SCANNING ELECTRON MICROSCOPY; SPECTROSCOPY; SULFATES; SULFUR; sea salt particles; methanesulfonate; nss-sulfate; Environmental Molecular Sciences Laboratory

Citation Formats

Hopkins, Rebecca J, Desyaterik, Yury, Tivanski, Alexei V, Zaveri, Rahul A, Berkowitz, Carl M, Tyliszczak, T, Gilles, Marry K, and Laskin, Alexander. Chemical Speciation of Sulfur in Marine Cloud Droplets and Particles: Analysis of Individual Particles from the Marine Boundary Layer Over the California Current. United States: N. p., 2008. Web. doi:10.1029/2007JD008954.
Hopkins, Rebecca J, Desyaterik, Yury, Tivanski, Alexei V, Zaveri, Rahul A, Berkowitz, Carl M, Tyliszczak, T, Gilles, Marry K, & Laskin, Alexander. Chemical Speciation of Sulfur in Marine Cloud Droplets and Particles: Analysis of Individual Particles from the Marine Boundary Layer Over the California Current. United States. https://doi.org/10.1029/2007JD008954
Hopkins, Rebecca J, Desyaterik, Yury, Tivanski, Alexei V, Zaveri, Rahul A, Berkowitz, Carl M, Tyliszczak, T, Gilles, Marry K, and Laskin, Alexander. 2008. "Chemical Speciation of Sulfur in Marine Cloud Droplets and Particles: Analysis of Individual Particles from the Marine Boundary Layer Over the California Current". United States. https://doi.org/10.1029/2007JD008954.
@article{osti_985029,
title = {Chemical Speciation of Sulfur in Marine Cloud Droplets and Particles: Analysis of Individual Particles from the Marine Boundary Layer Over the California Current},
author = {Hopkins, Rebecca J and Desyaterik, Yury and Tivanski, Alexei V and Zaveri, Rahul A and Berkowitz, Carl M and Tyliszczak, T and Gilles, Marry K and Laskin, Alexander},
abstractNote = {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 complementary combination of 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 (TOFSIMS), 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 an air mass that originated over the open ocean and then passed through the area of the California current located along the northern California coast. Based on 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-SO42-) in sea-salt particles with the characteristic ratios of CH3SO3-/nss-SO42-> 0.6. Although this value seems too high for a mid-latitude site, our model calculations suggest that high CH3SO3-/nss-SO42- ratios are expected during the early stages of dimethyl sulfide (DMS) oxidation when CH3SO3H forms more rapidly than H2SO4.},
doi = {10.1029/2007JD008954},
url = {https://www.osti.gov/biblio/985029}, journal = {Journal of Geophysical Research},
issn = {0148-0227},
number = d4,
volume = 113,
place = {United States},
year = {Wed Feb 27 00:00:00 EST 2008},
month = {Wed Feb 27 00:00:00 EST 2008}
}