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Title: Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity

Abstract

The impact of sea spray aerosol (SSA) on climate depends on the size and chemical composition of individual particles that make-up the total SSA ensemble. While the organic fraction of SSA has been characterized from a bulk perspective, there remains a lack of understanding as to the composition of individual particles within the SSA ensemble. To better understand the molecular components within SSA particles and how SSA composition changes with ocean biology, simultaneous measurements of seawater and SSA were made during a month-long mesocosm experiment performed in an ocean-atmosphere facility. Herein, we deconvolute the composition of freshly emitted SSA devoid of anthropogenic and terrestrial influences by characterizing classes of organic compounds as well as specific molecules within individual SSA particles. Analysis of SSA particles show that the diversity of molecules within the organic fraction varies between two size fractions (submicron and supermicron) with contributions from fatty acids, monosaccharides, polysaccharides and siliceous material. Significant changes in the distribution of these compounds within individual particles are observed to coincide with the rise and fall of phytoplankton and bacterial populations within the seawater. Furthermore, water uptake is impacted as shown by hygroscopicity measurements of model systems composed of representative organic compounds. Thus, themore » how changes in the hygroscopic growth of SSA evolves with composition can be elucidated. Overall, this study provides an important connection between biological processes that control the composition of seawater and changes in single particle composition which will enhances our ability to predict the impact of SSA on climate.« less

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1358472
Report Number(s):
PNNL-SA-117125
Journal ID: ISSN 2451-9294; 48375; KP1704020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chem; Journal Volume: 2; Journal Issue: 5
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Cochran, Richard E., Laskina, Olga, Trueblood, Jonathan V., Estillore, Armando D., Morris, Holly S., Jayarathne, Thilina, Sultana, Camille M., Lee, Christopher, Lin, Peng, Laskin, Julia, Laskin, Alexander, Dowling, Jacqueline A., Qin, Zhen, Cappa, Christopher D., Bertram, Timothy H., Tivanski, Alexei V., Stone, Elizabeth A., Prather, Kimberly A., and Grassian, Vicki H. Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity. United States: N. p., 2017. Web. doi:10.1016/j.chempr.2017.03.007.
Cochran, Richard E., Laskina, Olga, Trueblood, Jonathan V., Estillore, Armando D., Morris, Holly S., Jayarathne, Thilina, Sultana, Camille M., Lee, Christopher, Lin, Peng, Laskin, Julia, Laskin, Alexander, Dowling, Jacqueline A., Qin, Zhen, Cappa, Christopher D., Bertram, Timothy H., Tivanski, Alexei V., Stone, Elizabeth A., Prather, Kimberly A., & Grassian, Vicki H. Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity. United States. doi:10.1016/j.chempr.2017.03.007.
Cochran, Richard E., Laskina, Olga, Trueblood, Jonathan V., Estillore, Armando D., Morris, Holly S., Jayarathne, Thilina, Sultana, Camille M., Lee, Christopher, Lin, Peng, Laskin, Julia, Laskin, Alexander, Dowling, Jacqueline A., Qin, Zhen, Cappa, Christopher D., Bertram, Timothy H., Tivanski, Alexei V., Stone, Elizabeth A., Prather, Kimberly A., and Grassian, Vicki H. Mon . "Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity". United States. doi:10.1016/j.chempr.2017.03.007.
@article{osti_1358472,
title = {Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity},
author = {Cochran, Richard E. and Laskina, Olga and Trueblood, Jonathan V. and Estillore, Armando D. and Morris, Holly S. and Jayarathne, Thilina and Sultana, Camille M. and Lee, Christopher and Lin, Peng and Laskin, Julia and Laskin, Alexander and Dowling, Jacqueline A. and Qin, Zhen and Cappa, Christopher D. and Bertram, Timothy H. and Tivanski, Alexei V. and Stone, Elizabeth A. and Prather, Kimberly A. and Grassian, Vicki H.},
abstractNote = {The impact of sea spray aerosol (SSA) on climate depends on the size and chemical composition of individual particles that make-up the total SSA ensemble. While the organic fraction of SSA has been characterized from a bulk perspective, there remains a lack of understanding as to the composition of individual particles within the SSA ensemble. To better understand the molecular components within SSA particles and how SSA composition changes with ocean biology, simultaneous measurements of seawater and SSA were made during a month-long mesocosm experiment performed in an ocean-atmosphere facility. Herein, we deconvolute the composition of freshly emitted SSA devoid of anthropogenic and terrestrial influences by characterizing classes of organic compounds as well as specific molecules within individual SSA particles. Analysis of SSA particles show that the diversity of molecules within the organic fraction varies between two size fractions (submicron and supermicron) with contributions from fatty acids, monosaccharides, polysaccharides and siliceous material. Significant changes in the distribution of these compounds within individual particles are observed to coincide with the rise and fall of phytoplankton and bacterial populations within the seawater. Furthermore, water uptake is impacted as shown by hygroscopicity measurements of model systems composed of representative organic compounds. Thus, the how changes in the hygroscopic growth of SSA evolves with composition can be elucidated. Overall, this study provides an important connection between biological processes that control the composition of seawater and changes in single particle composition which will enhances our ability to predict the impact of SSA on climate.},
doi = {10.1016/j.chempr.2017.03.007},
journal = {Chem},
number = 5,
volume = 2,
place = {United States},
year = {Mon May 01 00:00:00 EDT 2017},
month = {Mon May 01 00:00:00 EDT 2017}
}
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  • The surface properties of atmospheric aerosol particles largely control their impact on climate by affecting their ability to uptake water, react heterogeneously, and nucleate ice in clouds. However, in the vacuum of a conventional electron microscope, the native surface structure often undergoes chemical rearrangement resulting in surfaces that are quite different from their atmospheric configurations. Herein, we report the development of a cryo-TEM approach where sea spray aerosol particles are flash frozen in their native state and then probed by electron microscopy. This unique approach allows for the detection of not only mixed salts, but also soft materials including wholemore » hydrated bacteria, diatoms, virus particles, marine vesicles, as well as gel networks within hydrated salt droplets. As a result, we anticipate this method will open up a new avenue of analysis for aerosol particles, not only for ocean-derived aerosols, but for those produced from other sources where there is interest in the transfer of organic or biological species from the biosphere to the atmosphere.« less
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  • The surface properties of atmospheric aerosol particles largely control their impact on climate by affecting their ability to uptake water, react heterogeneously, and nucleate ice in clouds. However, in the vacuum of a conventional electron microscope, the native surface structure often undergoes chemical rearrangement resulting in surfaces that are quite different from their atmospheric configurations. Herein, we report the development of a cryo-TEM approach where sea spray aerosol particles are flash frozen in their native state and then probed by electron microscopy. This unique approach allows for the detection of not only mixed salts, but also soft materials including wholemore » hydrated bacteria, diatoms, virus particles, marine vesicles, as well as gel networks within hydrated salt droplets. As a result, we anticipate this method will open up a new avenue of analysis for aerosol particles, not only for ocean-derived aerosols, but for those produced from other sources where there is interest in the transfer of organic or biological species from the biosphere to the atmosphere.« less