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Title: The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles

Covering 71% of the Earth’s surface, oceans represent a significant global source of atmospheric aerosols. The size and composition of sea spray aerosols (SSA) affect their ability to serve as cloud seeds and thus understanding the factors controlling their composition is critical to predicting their impact on clouds and climate. SSA particles have been shown to be an external mixture of particles with different compositions. Film and jet drop production mechanisms ultimately determine the individual particle compositions which are comprised of an array of salt/organic mixtures ranging from pure sea salt to nearly pure organic particles. It is often assumed that the majority of submicron SSA are formed by film drops produced from bursting hydrophobic organic-rich bubble film caps at the sea surface, and in contrast, jet drops are postulated to produce larger supermicron particles from underlying seawater comprised largely of salts and water soluble organic species. However, here we show that jet drops produced by bursting sub-100 m bubbles account for up to 40 % of all submicron particles. They have distinct chemical compositions, organic volume fractions and ice nucleating activities from submicron film drops. Thus a substantial fraction of submicron particles will not necessarily be controlled by themore » composition of the sea surface microlayer as has been assumed in many studies. This finding has significant ramifications for the size-resolved mixing states of SSA particles which must be taken into consideration when accessing SSA impacts on clouds.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [2] ;  [1] ;  [1]
  1. Univ. of California, San Diego, CA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-124917
Journal ID: ISSN 0027-8424; 49300; KP1703010
Grant/Contract Number:
AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 27; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; marine aerosol; sea spray aerosol; global aerosol-climate models; climate modeling; Global Modeling; Environmental Molecular Sciences Laboratory
OSTI Identifier:
1398221

Wang, Xiaofei, Deane, Grant B., Moore, Kathryn A., Ryder, Olivia S., Stokes, M. Dale, Beall, Charlotte M., Collins, Douglas B., Santander, Mitchell V., Burrows, Susannah M., Sultana, Camille M., and Prather, Kimberly A.. The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles. United States: N. p., Web. doi:10.1073/pnas.1702420114.
Wang, Xiaofei, Deane, Grant B., Moore, Kathryn A., Ryder, Olivia S., Stokes, M. Dale, Beall, Charlotte M., Collins, Douglas B., Santander, Mitchell V., Burrows, Susannah M., Sultana, Camille M., & Prather, Kimberly A.. The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles. United States. doi:10.1073/pnas.1702420114.
Wang, Xiaofei, Deane, Grant B., Moore, Kathryn A., Ryder, Olivia S., Stokes, M. Dale, Beall, Charlotte M., Collins, Douglas B., Santander, Mitchell V., Burrows, Susannah M., Sultana, Camille M., and Prather, Kimberly A.. 2017. "The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles". United States. doi:10.1073/pnas.1702420114. https://www.osti.gov/servlets/purl/1398221.
@article{osti_1398221,
title = {The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles},
author = {Wang, Xiaofei and Deane, Grant B. and Moore, Kathryn A. and Ryder, Olivia S. and Stokes, M. Dale and Beall, Charlotte M. and Collins, Douglas B. and Santander, Mitchell V. and Burrows, Susannah M. and Sultana, Camille M. and Prather, Kimberly A.},
abstractNote = {Covering 71% of the Earth’s surface, oceans represent a significant global source of atmospheric aerosols. The size and composition of sea spray aerosols (SSA) affect their ability to serve as cloud seeds and thus understanding the factors controlling their composition is critical to predicting their impact on clouds and climate. SSA particles have been shown to be an external mixture of particles with different compositions. Film and jet drop production mechanisms ultimately determine the individual particle compositions which are comprised of an array of salt/organic mixtures ranging from pure sea salt to nearly pure organic particles. It is often assumed that the majority of submicron SSA are formed by film drops produced from bursting hydrophobic organic-rich bubble film caps at the sea surface, and in contrast, jet drops are postulated to produce larger supermicron particles from underlying seawater comprised largely of salts and water soluble organic species. However, here we show that jet drops produced by bursting sub-100 m bubbles account for up to 40 % of all submicron particles. They have distinct chemical compositions, organic volume fractions and ice nucleating activities from submicron film drops. Thus a substantial fraction of submicron particles will not necessarily be controlled by the composition of the sea surface microlayer as has been assumed in many studies. This finding has significant ramifications for the size-resolved mixing states of SSA particles which must be taken into consideration when accessing SSA impacts on clouds.},
doi = {10.1073/pnas.1702420114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 27,
volume = 114,
place = {United States},
year = {2017},
month = {6}
}