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Title: The diverse chemical mixing state of aerosol particles in the southeastern United States

Abstract

Aerosols in the atmosphere are chemically complex with thousands of chemical species distributed in different proportions across individual particles in an aerosol population. An internal mixing assumption, with species present in the same proportions across all aerosols, is used in many models and calculations of secondary organic aerosol (SOA) formation, cloud activation, and aerosol optical properties. However, many of these effects depend on the distribution of species within individual particles, and important information can be lost when internal mixtures are assumed. Herein, we show that – as found during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, Alabama, at a rural, forested location – aerosols frequently are not purely internally mixed, even in the accumulation mode (0.2–1.0µm). A range of aerosol sources and the mixing state were determined using computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (CCSEM-EDX) and scanning transmission X-ray microscopy–near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). Particles that were dominated by SOA and inorganic salts (e.g., ammonium sulfate) were the majority of particles by number fraction from 0.2 to 5µm with an average of 78% SOA in the accumulation mode. However, during certain periods contributions by sea spray aerosol (SSA) and mineral dust were significant tomore » accumulation (22% SSA and 26% dust) and coarse-mode number concentrations (38% SSA and 63% dust). The fraction of particles containing key elements (Na, Mg, K, Ca, and Fe) were determined as a function of size for specific classes of particles. Within internally mixed SOA/sulfate particles <5% contained Na, Mg, K, Ca, or Fe, though these nonvolatile cations were present in particles from the other sources (e.g., SSA and dust). Mass estimates of the aerosol elemental components were used to determine the extent of internal versus external mixing by calculating the mixing state index ( χ). The aerosol population was more externally mixed than internally mixed during all time periods analyzed. Accumulation mode aerosol ranged from more internally mixed during SOA periods to mostly externally mixed during dust periods. Supermicron aerosols were most externally mixed during SOA time periods, when more SOA particles added a distinct supermicron class, and more internally mixed when dominated by a single particle type (e.g., SSA or dust). Furthermore, these results emphasize that neither external nor internal mixtures fully represent the mixing state of atmospheric aerosols, even in a rural, forested environment, which has important implications for air quality and climate modeling.« less

Authors:
 [1];  [2];  [2];  [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Univ. of the Pacific, Stockton, CA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Xiamen Univ., Xiamen (China)
  4. 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
OSTI Identifier:
1471086
Report Number(s):
[PNNL-SA-138963]
[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: 16]; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Bondy, Amy L., Bonanno, Daniel, Moffet, Ryan C., Wang, Bingbing, Laskin, Alexander, and Ault, Andrew P. The diverse chemical mixing state of aerosol particles in the southeastern United States. United States: N. p., 2018. Web. doi:10.5194/acp-18-12595-2018.
Bondy, Amy L., Bonanno, Daniel, Moffet, Ryan C., Wang, Bingbing, Laskin, Alexander, & Ault, Andrew P. The diverse chemical mixing state of aerosol particles in the southeastern United States. United States. doi:10.5194/acp-18-12595-2018.
Bondy, Amy L., Bonanno, Daniel, Moffet, Ryan C., Wang, Bingbing, Laskin, Alexander, and Ault, Andrew P. Thu . "The diverse chemical mixing state of aerosol particles in the southeastern United States". United States. doi:10.5194/acp-18-12595-2018. https://www.osti.gov/servlets/purl/1471086.
@article{osti_1471086,
title = {The diverse chemical mixing state of aerosol particles in the southeastern United States},
author = {Bondy, Amy L. and Bonanno, Daniel and Moffet, Ryan C. and Wang, Bingbing and Laskin, Alexander and Ault, Andrew P.},
abstractNote = {Aerosols in the atmosphere are chemically complex with thousands of chemical species distributed in different proportions across individual particles in an aerosol population. An internal mixing assumption, with species present in the same proportions across all aerosols, is used in many models and calculations of secondary organic aerosol (SOA) formation, cloud activation, and aerosol optical properties. However, many of these effects depend on the distribution of species within individual particles, and important information can be lost when internal mixtures are assumed. Herein, we show that – as found during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, Alabama, at a rural, forested location – aerosols frequently are not purely internally mixed, even in the accumulation mode (0.2–1.0µm). A range of aerosol sources and the mixing state were determined using computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (CCSEM-EDX) and scanning transmission X-ray microscopy–near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS). Particles that were dominated by SOA and inorganic salts (e.g., ammonium sulfate) were the majority of particles by number fraction from 0.2 to 5µm with an average of 78% SOA in the accumulation mode. However, during certain periods contributions by sea spray aerosol (SSA) and mineral dust were significant to accumulation (22% SSA and 26% dust) and coarse-mode number concentrations (38% SSA and 63% dust). The fraction of particles containing key elements (Na, Mg, K, Ca, and Fe) were determined as a function of size for specific classes of particles. Within internally mixed SOA/sulfate particles <5% contained Na, Mg, K, Ca, or Fe, though these nonvolatile cations were present in particles from the other sources (e.g., SSA and dust). Mass estimates of the aerosol elemental components were used to determine the extent of internal versus external mixing by calculating the mixing state index (χ). The aerosol population was more externally mixed than internally mixed during all time periods analyzed. Accumulation mode aerosol ranged from more internally mixed during SOA periods to mostly externally mixed during dust periods. Supermicron aerosols were most externally mixed during SOA time periods, when more SOA particles added a distinct supermicron class, and more internally mixed when dominated by a single particle type (e.g., SSA or dust). Furthermore, these results emphasize that neither external nor internal mixtures fully represent the mixing state of atmospheric aerosols, even in a rural, forested environment, which has important implications for air quality and climate modeling.},
doi = {10.5194/acp-18-12595-2018},
journal = {Atmospheric Chemistry and Physics (Online)},
number = [16],
volume = [18],
place = {United States},
year = {2018},
month = {8}
}

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    Works referencing / citing this record:

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