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

Abstract

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:
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)
OSTI Identifier:
1502416
Report Number(s):
PNNL-SA-136257
Journal ID: ISSN 1680-7324
Grant/Contract Number:  
AC05-76RL01830
Resource 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
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

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., 2018. 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. Tue . "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}
}

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Cited by: 14 works
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Figures / Tables:

Figure 1 Figure 1: Representative SEM images and EDX spectra of individual particles corresponding to the main particle types observed by CCSEMEDX, and the average EDX spectrum for each particle type. Average spectra show the relative peak areas of all elements analyzed by CCSEM-EDX. (a) Fresh SSA particle comprised of sodium chloridemore » core (red) and magnesium chloride shell (black). The spectrum for the core is offset for clarity. (b) Partially aged SSA particle containing sodium and more sulfur than chlorine. (c) Organic + sulfate particle. (d) Organic + sulfate particle on silicon substrate. (e) Aluminum- and silicon-containing dust particle. Carbon and oxygen peaks include some signal from TEM grid substrate background for particles (a), (b), (c), and (e). Aluminum and silicon peaks are due to sample holder and silicon substrate background, respectively, for particle (d).« less

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    Raman microspectroscopy and vibrational sum frequency generation spectroscopy as probes of the bulk and surface compositions of size-resolved sea spray aerosol particles
    journal, January 2013

    • Ault, Andrew P.; Zhao, Defeng; Ebben, Carlena J.
    • Physical Chemistry Chemical Physics, Vol. 15, Issue 17
    • DOI: 10.1039/c3cp43899f

    Chemical composition and sources of aerosol particles at Zeppelin Mountain (Ny Ålesund, Svalbard): An electron microscopy study
    journal, March 2012


    Single-Particle Characterization of Summertime Arctic Aerosols Collected at Ny-Ålesund, Svalbard
    journal, April 2010

    • Geng, Hong; Ryu, JiYeon; Jung, Hae-Jin
    • Environmental Science & Technology, Vol. 44, Issue 7
    • DOI: 10.1021/es903268j

    Single-Particle SEM-EDX Analysis of Iron-Containing Coarse Particulate Matter in an Urban Environment: Sources and Distribution of Iron within Cleveland, Ohio
    journal, April 2012

    • Ault, Andrew P.; Peters, Thomas M.; Sawvel, Eric J.
    • Environmental Science & Technology, Vol. 46, Issue 8
    • DOI: 10.1021/es204006k

    Transported Mineral Dust Deposition Case Study at a Hydrologically Sensitive Mountain Site: Size and Composition Shifts in Ambient Aerosol and Snowpack
    journal, January 2016

    • Jessica L. Axson, Jessica L. Axson; Shen, Hongru; Amy L. Bondy, Amy L. Bondy
    • Aerosol and Air Quality Research, Vol. 16, Issue 3
    • DOI: 10.4209/aaqr.2015.05.0346

    Direct Observation of Heterogeneous Chemistry in the Atmosphere
    journal, February 1998


    Contribution of sea surface carbon pool to organic matter enrichment in sea spray aerosol
    journal, February 2014

    • Quinn, Patricia K.; Bates, Timothy S.; Schulz, Kristen S.
    • Nature Geoscience, Vol. 7, Issue 3
    • DOI: 10.1038/ngeo2092

    Atmospheric Aerosol Chemistry: Spectroscopic and Microscopic Advances
    journal, November 2016


    Quantitative Time-Resolved Monitoring of Nitrate Formation in Sea Salt Particles Using a CCSEM/EDX Single Particle Analysis
    journal, December 2002

    • Laskin, Alexander; Iedema, Martin J.; Cowin, James P.
    • Environmental Science & Technology, Vol. 36, Issue 23
    • DOI: 10.1021/es020551k

    Sea spray aerosol as a unique source of ice nucleating particles
    journal, December 2015

    • DeMott, Paul J.; Hill, Thomas C. J.; McCluskey, Christina S.
    • Proceedings of the National Academy of Sciences, Vol. 113, Issue 21
    • DOI: 10.1073/pnas.1514034112

    Effect of Prudhoe Bay emissions on atmospheric aerosol growth events observed in Utqiaġvik (Barrow), Alaska
    journal, March 2017


    Increased Arctic cloud longwave emissivity associated with pollution from mid-latitudes
    journal, April 2006


    A single parameter representation of hygroscopic growth and cloud condensation nucleus activity
    journal, January 2007

    • Petters, M. D.; Kreidenweis, S. M.
    • Atmospheric Chemistry and Physics, Vol. 7, Issue 8
    • DOI: 10.5194/acp-7-1961-2007

    Single-particle characterization of the high-Arctic summertime aerosol
    journal, January 2014

    • Sierau, B.; Chang, R. Y. -W.; Leck, C.
    • Atmospheric Chemistry and Physics, Vol. 14, Issue 14
    • DOI: 10.5194/acp-14-7409-2014

    Using Raman Microspectroscopy to Determine Chemical Composition and Mixing State of Airborne Marine Aerosols over the Pacific Ocean
    journal, December 2013


    Inside versus Outside: Ion Redistribution in Nitric Acid Reacted Sea Spray Aerosol Particles as Determined by Single Particle Analysis
    journal, September 2013

    • Ault, Andrew P.; Guasco, Timothy L.; Ryder, Olivia S.
    • Journal of the American Chemical Society, Vol. 135, Issue 39
    • DOI: 10.1021/ja407117x

    Contributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiaġvik, Alaska
    journal, January 2017

    • Gunsch, Matthew J.; Kirpes, Rachel M.; Kolesar, Katheryn R.
    • Atmospheric Chemistry and Physics, Vol. 17, Issue 17
    • DOI: 10.5194/acp-17-10879-2017

    Sea salt aerosols as a reactive surface for inorganic and organic acidic gases in the Arctic troposphere
    journal, January 2015


    Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City
    journal, January 2010

    • Moffet, R. C.; Henn, T. R.; Tivanski, A. V.
    • Atmospheric Chemistry and Physics, Vol. 10, Issue 3
    • DOI: 10.5194/acp-10-961-2010

    Application of the variability-size relationship to atmospheric aerosol studies: estimating aerosol lifetimes and ages
    journal, January 2002

    • Williams, J.; de Reus, M.; Krejci, R.
    • Atmospheric Chemistry and Physics, Vol. 2, Issue 2
    • DOI: 10.5194/acp-2-133-2002

    Long-term trends of black carbon and sulphate aerosol in the Arctic: changes in atmospheric transport and source region emissions
    journal, January 2010

    • Hirdman, D.; Burkhart, J. F.; Sodemann, H.
    • Atmospheric Chemistry and Physics, Vol. 10, Issue 19
    • DOI: 10.5194/acp-10-9351-2010

    Size-Dependent Changes in Sea Spray Aerosol Composition and Properties with Different Seawater Conditions
    journal, May 2013

    • Ault, Andrew P.; Moffet, Ryan C.; Baltrusaitis, Jonas
    • Environmental Science & Technology, Vol. 47, Issue 11
    • DOI: 10.1021/es400416g

    Size-resolved morphological properties of the high Arctic summer aerosol during ASCOS-2008
    journal, January 2016

    • Hamacher-Barth, Evelyne; Leck, Caroline; Jansson, Kjell
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 10
    • DOI: 10.5194/acp-16-6577-2016

    Kinetic Study of Heterogeneous Reaction of Deliquesced NaCl Particles with Gaseous HNO 3 Using Particle-on-Substrate Stagnation Flow Reactor Approach
    journal, October 2007

    • Liu, Y.; Cain, J. P.; Wang, H.
    • The Journal of Physical Chemistry A, Vol. 111, Issue 40
    • DOI: 10.1021/jp072005p

    Reactions at Interfaces As a Source of Sulfate Formation in Sea-Salt Particles
    journal, July 2003


    Analysis of Atmospheric Aerosols
    journal, July 2008


    Vertical Profiles and Chemical Properties of Aerosol Particles upon Ny-Ålesund (Svalbard Islands)
    journal, January 2015

    • Moroni, B.; Becagli, S.; Bolzacchini, E.
    • Advances in Meteorology, Vol. 2015
    • DOI: 10.1155/2015/292081

    Polar amplification of climate change in coupled models
    journal, September 2003


    Chlorine, Bromine AND Iodine in arctic aerosols
    journal, January 1988


    Morphochemical characteristics and mixing state of long range transported wildfire particles at Ny-Ålesund (Svalbard Islands)
    journal, May 2017


    Importance of aerosol composition and mixing state for cloud droplet activation over the Arctic pack ice in summer
    journal, January 2015


    Automated Chemical Analysis of Internally Mixed Aerosol Particles Using X-ray Spectromicroscopy at the Carbon K-Edge
    journal, October 2010

    • Moffet, Ryan C.; Henn, Tobias; Laskin, Alexander
    • Analytical Chemistry, Vol. 82, Issue 19
    • DOI: 10.1021/ac1012909

    Size-segregated compositional analysis of aerosol particles collected in the European Arctic during the ACCACIA campaign
    journal, January 2016

    • Young, G.; Jones, H. M.; Darbyshire, E.
    • Atmospheric Chemistry and Physics, Vol. 16, Issue 6
    • DOI: 10.5194/acp-16-4063-2016

    Sources, distribution, and acidity of sulfate–ammonium aerosol in the Arctic in winter–spring
    journal, December 2011


    The complex response of Arctic aerosol to sea-ice retreat
    journal, January 2014

    • Browse, J.; Carslaw, K. S.; Mann, G. W.
    • Atmospheric Chemistry and Physics, Vol. 14, Issue 14
    • DOI: 10.5194/acp-14-7543-2014

    Arctic Air Pollution: Origins and Impacts
    journal, March 2007


    Future emissions from shipping and petroleum activities in the Arctic
    journal, January 2011

    • Peters, G. P.; Nilssen, T. B.; Lindholt, L.
    • Atmospheric Chemistry and Physics, Vol. 11, Issue 11
    • DOI: 10.5194/acp-11-5305-2011

    Particulate trimethylamine in the summertime Canadian high Arctic lower troposphere
    journal, January 2017

    • Köllner, Franziska; Schneider, Johannes; Willis, Megan D.
    • Atmospheric Chemistry and Physics, Vol. 17, Issue 22
    • DOI: 10.5194/acp-17-13747-2017

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.