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Title: Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway

Abstract

With a large global emission rate and high reactivity, isoprene has a profound effect upon atmospheric chemistry and composition. The atmospheric pathways by which isoprene converts to secondary organic aerosol (SOA) and how anthropogenic pollutants such as nitrogen oxides and sulfur affect this process are a subject of intense research because particles affect Earth’s climate and local air quality. In the absence of both nitrogen oxides and reactive aqueous seed particles, we measure SOA mass yields from isoprene photochemical oxidation of up to 15%, which are factors of 2, or more, higher than those typically used in coupled chemistry-climate models. SOA yield is initially constant with the addition of increasing amounts of nitric oxide (NO) but then sharply decreases for input concentrations above 10 ppbv. Online measurements of aerosol molecular composition show that the fate of second-generation RO2 radicals is key to understanding the efficient SOA formation and the NOx dependent yields described here and in the literature. These insights allow for improved quantitative estimates of SOA formation in the pre-industrial atmosphere and in biogenic-rich regions with limited anthropogenic impacts and suggest a more complex representation of NOx dependent SOA yields may be important in models.

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ;
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:
1340826
Report Number(s):
PNNL-SA-117433
Journal ID: ISSN 0013-936X; KP1701000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Environmental Science and Technology; Journal Volume: 50; Journal Issue: 18
Country of Publication:
United States
Language:
English
Subject:
Isoprene secondary organic aerosol; dihydroxydihydroperoxides; pre-industrial atmosphere

Citation Formats

Liu, Jiumeng, D’Ambro, Emma L., Lee, Ben H., Lopez-Hilfiker, Felipe D., Zaveri, Rahul A., Rivera-Rios, Jean C., Keutsch, Frank N., Iyer, Siddharth, Kurten, Theo, Zhang, Zhenfa, Gold, Avram, Surratt, Jason D., Shilling, John E., and Thornton, Joel A. Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway. United States: N. p., 2016. Web. doi:10.1021/acs.est.6b01872.
Liu, Jiumeng, D’Ambro, Emma L., Lee, Ben H., Lopez-Hilfiker, Felipe D., Zaveri, Rahul A., Rivera-Rios, Jean C., Keutsch, Frank N., Iyer, Siddharth, Kurten, Theo, Zhang, Zhenfa, Gold, Avram, Surratt, Jason D., Shilling, John E., & Thornton, Joel A. Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway. United States. doi:10.1021/acs.est.6b01872.
Liu, Jiumeng, D’Ambro, Emma L., Lee, Ben H., Lopez-Hilfiker, Felipe D., Zaveri, Rahul A., Rivera-Rios, Jean C., Keutsch, Frank N., Iyer, Siddharth, Kurten, Theo, Zhang, Zhenfa, Gold, Avram, Surratt, Jason D., Shilling, John E., and Thornton, Joel A. Tue . "Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway". United States. doi:10.1021/acs.est.6b01872.
@article{osti_1340826,
title = {Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway},
author = {Liu, Jiumeng and D’Ambro, Emma L. and Lee, Ben H. and Lopez-Hilfiker, Felipe D. and Zaveri, Rahul A. and Rivera-Rios, Jean C. and Keutsch, Frank N. and Iyer, Siddharth and Kurten, Theo and Zhang, Zhenfa and Gold, Avram and Surratt, Jason D. and Shilling, John E. and Thornton, Joel A.},
abstractNote = {With a large global emission rate and high reactivity, isoprene has a profound effect upon atmospheric chemistry and composition. The atmospheric pathways by which isoprene converts to secondary organic aerosol (SOA) and how anthropogenic pollutants such as nitrogen oxides and sulfur affect this process are a subject of intense research because particles affect Earth’s climate and local air quality. In the absence of both nitrogen oxides and reactive aqueous seed particles, we measure SOA mass yields from isoprene photochemical oxidation of up to 15%, which are factors of 2, or more, higher than those typically used in coupled chemistry-climate models. SOA yield is initially constant with the addition of increasing amounts of nitric oxide (NO) but then sharply decreases for input concentrations above 10 ppbv. Online measurements of aerosol molecular composition show that the fate of second-generation RO2 radicals is key to understanding the efficient SOA formation and the NOx dependent yields described here and in the literature. These insights allow for improved quantitative estimates of SOA formation in the pre-industrial atmosphere and in biogenic-rich regions with limited anthropogenic impacts and suggest a more complex representation of NOx dependent SOA yields may be important in models.},
doi = {10.1021/acs.est.6b01872},
journal = {Environmental Science and Technology},
number = 18,
volume = 50,
place = {United States},
year = {Tue Sep 20 00:00:00 EDT 2016},
month = {Tue Sep 20 00:00:00 EDT 2016}
}