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Published September 27, 2018 | Supplemental Material + Published
Journal Article Open

Regional Similarities and NOₓ-Related Increases in Biogenic Secondary Organic Aerosol in Summertime Southeastern United States

Abstract

During the 2013 Southern Oxidant and Aerosol Study, Fourier transform infrared spectroscopy (FTIR) and aerosol mass spectrometer (AMS) measurements of submicron mass were collected at Look Rock (LRK), Tennessee, and Centreville (CTR), Alabama. Carbon monoxide and submicron sulfate and organic mass concentrations were 15–60% higher at CTR than at LRK, but their time series had moderate correlations (r ~ 0.5). However, NOₓ had no correlation (r = 0.08) between the two sites with nighttime‐to‐early‐morning peaks 3–10 times higher at CTR than at LRK. Organic mass (OM) sources identified by FTIR Positive Matrix Factorization (PMF) had three very similar factors at both sites: fossil fuel combustion‐related organic aerosols, mixed organic aerosols, and biogenic organic aerosols (BOA). The BOA spectrum from FTIR is similar (cosine similarity > 0.6) to that of lab‐generated particle mass from the photochemical oxidation of both isoprene and monoterpenes under high NOₓ conditions from chamber experiments. The BOA mass fraction was highest during the night at CTR but in the afternoon at LRK. AMS PMF resulted in two similar pairs of factors at both sites and a third nighttime NOx‐related factor (33% of OM) at CTR but a daytime nitrate‐related factor (28% of OM) at LRK. NOₓ was correlated with BOA and LO‐OOA for NOₓ concentrations higher than 1 ppb at both sites, producing 0.5 ± 0.1 μg/m³ for CTR‐LO‐OOA and 1.0 ± 0.3 μg/m³ for CTR‐BOA additional biogenic OM for each 1 ppb increase of NOₓ.

Additional Information

© 2018 American Geophysical Union. Received 7 FEB 2018; Accepted 24 JUL 2018; Accepted article online 4 AUG 2018; Published online 17 SEP 2018. We thank Ashley Corrigan, Janin Guzman‐Morales, and Katie Kolesar for assistance at the LRK field site and Annmarie Carlton, Joost deGouw, Jose Jimenez, and Allen Goldstein for organizing the SOAS campaign. We thank Eric Edgerton for gas concentration and meteorological measurements at Centreville and the IMPROVE network for ozone concentration at Look Rock. We thank Joost deGouw and Allen Goldstein for sharing bVOC measurements at Centreville. We appreciate the support of Sherri Hunt for this project. This work was supported by U.S. Environmental Protection Agency (EPA) grant RD‐83540801. Lu Xu and Nga L. Ng acknowledge National Science Foundation grant 1242258 and U.S. Environmental Protection Agency STAR grant RD‐83540301. The U.S. EPA through its Office of Research and Development collaborated in the research described here. It has been subjected to Agency administrative review and approved for publication but may not necessarily reflect official Agency policy. The EPA does not endorse any products or commercial services mentioned in this publication. Timothy Bertram was supported by the Office of Science (Office of Biological and Environmental Research), U.S. Department of Energy (grant DE‐SC0006431). LRK AMS and FTIR measurements used in this study are curated at http://doi.org/10.6075/J0P26W1T, and all measurements are also available at the project archive http://esrl.noaa.gov/csd/groups/csd7/measurements/2013senex/Ground/DataDownload. CMAQ model code is available via https://github.com/USEPA/CMAQ.

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Published - Liu_et_al-2018-Journal_of_Geophysical_Research_3A_Atmospheres.pdf

Supplemental Material - jgrd54860-sup-0001-si.pdf

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