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Ambient Measurements of Highly Oxidized Gas-Phase Molecules during the Southern Oxidant and Aerosol Study (SOAS) 2013

Massoli, Paola and Stark, Harald and Canagaratna, Manjula R. and Krechmer, Jordan E. and Xu, Lu and Ng, Nga L. and Mauldin, Roy L., III and Yan, Chao and Kimmel, Joel and Misztal, Pawel K. and Jimenez, Jose L. and Jayne, John T. and Worsnop, Douglas R. (2018) Ambient Measurements of Highly Oxidized Gas-Phase Molecules during the Southern Oxidant and Aerosol Study (SOAS) 2013. ACS Earth and Space Chemistry, 2 (7). pp. 653-672. ISSN 2472-3452. https://resolver.caltech.edu/CaltechAUTHORS:20180808-140939979

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Abstract

We present measurements of highly oxidized multifunctional molecules (HOMs) detected in the gas phase using a high-resolution time-of-flight chemical ionization mass spectrometer with nitrate reagent ion (NO_3– CIMS). The measurements took place during the 2013 Southern Oxidant and Aerosol Study (SOAS 2013) at a forest site in Alabama, where emissions were dominated by biogenic volatile organic compounds (BVOCs). Primary BVOC emissions were represented by isoprene mixed with various terpenes, making it a unique sampling location compared to previous NO_3– CIMS deployments in monoterpene-dominated environments. During SOAS 2013, the NO_3–CIMS detected HOMs with oxygen-to-carbon (O:C) ratios between 0.5 and 1.4 originating from both isoprene (C_5) and monoterpenes (C_(10)) as well as hundreds of additional HOMs with carbon numbers between C_3 and C_(20). We used positive matrix factorization (PMF) to deconvolve the complex data set and extract information about classes of HOMs with similar temporal trends. This analysis revealed three isoprene-dominated and three monoterpene-dominated PMF factors. We observed significant amounts of isoprene- and monoterpene-derived organic nitrates (ONs) in most factors. The abundant presence of ONs was consistent with previous studies that have highlighted the importance of NO_x-driven chemistry at the site. One of the isoprene-dominated factors had a strong correlation with SO_2 plumes likely advected from nearby coal-fired power plants and was dominated by an isoprene-derived ON (C_5H_(10)N_2O_8). These results indicate that anthropogenic emissions played a significant role in the formation of low-volatility compounds from BVOC emissions in the region.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acsearthspacechem.8b00028DOIArticle
https://pubs.acs.org/doi/suppl/10.1021/acsearthspacechem.8b00028AuthorSupporting Information
ORCID:
AuthorORCID
Massoli, Paola0000-0002-6378-9366
Stark, Harald0000-0002-0731-1202
Krechmer, Jordan E.0000-0003-3642-0659
Xu, Lu0000-0002-0021-9876
Ng, Nga L.0000-0001-8460-4765
Misztal, Pawel K.0000-0003-1060-1750
Jimenez, Jose L.0000-0001-6203-1847
Worsnop, Douglas R.0000-0002-8928-8017
Additional Information:© 2018 American Chemical Society. Received: March 15, 2018; Revised: May 6, 2018; Accepted: May 8, 2018; Published: May 8, 2018. The authors thank the organizers of the SOAS campaign for their assistance and help during the project at the CTR site, Andrew T. Lambe (Aerodyne Research), Heikki Junninen, Mikael Ehn, Mikko Sipila, and Jani Hakala (University of Helsinki) for their help before and during the project and for the useful comments, Karsten Bauman and Eric Edgerton (ARA) for sharing the SEARCH data, Steven Bertram and Paul Shepson (Western Michigan University) for sharing the 2D-GC and GC-ECD data, and William Brune (Pennsylvania State University) for sharing the HO2, OH, and OHR data. Christopher Knote (NCAR) produced the FLEXPART outputs during the SOAS project. This project was funded by NSF AGS-1243356. L.X. and N.L.N. acknowledge support from NSF AGS-1242258 and U.S. EPA STAR 83540301. J.E.K. and J.L.J. were supported by NSF AGS-1740610 and U.S. EPA STAR 83587701.
Funders:
Funding AgencyGrant Number
NSFAGS-1243356
NSFAGS-1242258
Environmental Protection Agency (EPA)83540301
NSFAGS-1740610
Environmental Protection Agency (EPA)83587701
Issue or Number:7
Record Number:CaltechAUTHORS:20180808-140939979
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180808-140939979
Official Citation:Ambient Measurements of Highly Oxidized Gas-Phase Molecules during the Southern Oxidant and Aerosol Study (SOAS) 2013. Paola Massoli, Harald Stark, Manjula R. Canagaratna, Jordan E. Krechmer, Lu Xu, Nga L. Ng, Roy L. Mauldin, III, Chao Yan, Joel Kimmel, Pawel K. Misztal, Jose L. Jimenez, John T. Jayne, and Douglas R. Worsnop. ACS Earth and Space Chemistry 2018 2 (7), 653-672. DOI: 10.1021/acsearthspacechem.8b00028
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:88666
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:08 Aug 2018 21:20
Last Modified:29 Oct 2019 18:10

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