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Title: Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Abstract. Few measurements of aerosol chemical composition have been made during the winter–spring transition (following polar sunrise) to constrain Arctic aerosol–cloud–climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiagvik (Barrow),Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24847particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99%, by number, of 2.5–7.5µmdiameter particles, 65–95% from 0.5–2.5µm, and50–60% from 0.1–0.5µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with94%, by number, internally mixed with secondary sulfate (39%, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40% of 1.0–4.0µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay,consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particlesmore » were observed in all samples and comprised 40–50%, by number,of 0.1–0.4µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. In conclusion, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud formation, in the winter Arctic.« less
Authors:
ORCiD logo [1] ;  [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [5] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Univ. of Pacific, Stockton, CA (United States)
  3. Univ. of Pacific, Stockton, CA (United States); Sonoma Technology, Petaluma, CA (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Xiamen Univ., Xiamen (China)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Report Number(s):
PNNL-SA-136257
Journal ID: ISSN 1680-7324
Grant/Contract Number:
AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 18; Journal Issue: 6; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES
OSTI Identifier:
1502416

Kirpes, Rachel M., Bondy, Amy L., Bonanno, Daniel, Moffet, Ryan C., Wang, Bingbing, Laskin, Alexander, Ault, Andrew P., and Pratt, Kerri A.. Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic. United States: N. p., Web. doi:10.5194/acp-18-3937-2018.
Kirpes, Rachel M., Bondy, Amy L., Bonanno, Daniel, Moffet, Ryan C., Wang, Bingbing, Laskin, Alexander, Ault, Andrew P., & Pratt, Kerri A.. Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic. United States. doi:10.5194/acp-18-3937-2018.
Kirpes, Rachel M., Bondy, Amy L., Bonanno, Daniel, Moffet, Ryan C., Wang, Bingbing, Laskin, Alexander, Ault, Andrew P., and Pratt, Kerri A.. 2018. "Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic". United States. doi:10.5194/acp-18-3937-2018. https://www.osti.gov/servlets/purl/1502416.
@article{osti_1502416,
title = {Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic},
author = {Kirpes, Rachel M. and Bondy, Amy L. and Bonanno, Daniel and Moffet, Ryan C. and Wang, Bingbing and Laskin, Alexander and Ault, Andrew P. and Pratt, Kerri A.},
abstractNote = {Abstract. Few measurements of aerosol chemical composition have been made during the winter–spring transition (following polar sunrise) to constrain Arctic aerosol–cloud–climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiagvik (Barrow),Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24847particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99%, by number, of 2.5–7.5µmdiameter particles, 65–95% from 0.5–2.5µm, and50–60% from 0.1–0.5µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with94%, by number, internally mixed with secondary sulfate (39%, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40% of 1.0–4.0µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay,consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40–50%, by number,of 0.1–0.4µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. In conclusion, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud formation, in the winter Arctic.},
doi = {10.5194/acp-18-3937-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 6,
volume = 18,
place = {United States},
year = {2018},
month = {3}
}