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Experimental and model estimates of the contributions from biogenic monoterpenes and sesquiterpenes to secondary organic aerosol in the southeastern United States

Xu, Lu and Pye, Havala O. T. and He, Jia and Chen, Yunle and Murphy, Benjamin N. and Ng, Nga Lee (2018) Experimental and model estimates of the contributions from biogenic monoterpenes and sesquiterpenes to secondary organic aerosol in the southeastern United States. Atmospheric Chemistry and Physics, 18 (17). pp. 12613-12637. ISSN 1680-7324. http://resolver.caltech.edu/CaltechAUTHORS:20180912-122527741

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Abstract

Atmospheric organic aerosol (OA) has important impacts on climate and human health but its sources remain poorly understood. Biogenic monoterpenes and sesquiterpenes are important precursors of secondary organic aerosol (SOA), but the amounts and pathways of SOA generation from these precursors are not well constrained by observations. We propose that the less-oxidized oxygenated organic aerosol (LO-OOA) factor resolved from positive matrix factorization (PMF) analysis on aerosol mass spectrometry (AMS) data can be used as a surrogate for fresh SOA from monoterpenes and sesquiterpenes in the southeastern US. This hypothesis is supported by multiple lines of evidence, including lab-in-the-field perturbation experiments, extensive ambient ground-level measurements, and state-of-the-art modeling. We performed lab-in-the-field experiments in which the ambient air is perturbed by the injection of selected monoterpenes and sesquiterpenes, and the subsequent SOA formation is investigated. PMF analysis on the perturbation experiments provides an objective link between LO-OOA and fresh SOA from monoterpenes and sesquiterpenes as well as insights into the sources of other OA factors. Further, we use an upgraded atmospheric model and show that modeled SOA concentrations from monoterpenes and sesquiterpenes could reproduce both the magnitude and diurnal variation of LO-OOA at multiple sites in the southeastern US, building confidence in our hypothesis. We estimate the annual average concentration of SOA from monoterpenes and sesquiterpenes in the southeastern US to be roughly 2µgm^(−3).


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-18-12613-2018DOIArticle
ORCID:
AuthorORCID
Xu, Lu0000-0002-0021-9876
Pye, Havala O. T.0000-0002-2014-2140
Ng, Nga Lee0000-0001-8460-4765
Additional Information:© Author(s) 2018. This work is distributed under the Creative Commons Attribution 4.0 License. Received: 29 Nov 2017 – Discussion started: 02 Jan 2018 – Revised: 15 Aug 2018 – Accepted: 18 Aug 2018 – Published: 31 Aug 2018. Data availability. Data can be obtained by request (ng@chbe.gatech.edu).
Funders:
Funding AgencyGrant Number
Environmental Protection Agency (EPA)RD-83540301
NSFAGS-1555034
NSFAGS-1455588
NSFAGS-1428738
Presidential Early Career Award for Scientist and Engineers (PECASE)UNSPECIFIED
Record Number:CaltechAUTHORS:20180912-122527741
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20180912-122527741
Official Citation:Xu, L., Pye, H. O. T., He, J., Chen, Y., Murphy, B. N., and Ng, N. L.: Experimental and model estimates of the contributions from biogenic monoterpenes and sesquiterpenes to secondary organic aerosol in the southeastern United States, Atmos. Chem. Phys., 18, 12613-12637, https://doi.org/10.5194/acp-18-12613-2018, 2018.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:89575
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:12 Sep 2018 19:30
Last Modified:12 Sep 2018 20:36

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