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Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets.

Journal article
Authors Ben H Lee
Claudia Mohr
Felipe D Lopez-Hilfiker
Anna Lutz
Mattias Hallquist
Lance Lee
Paul Romer
Ronald C Cohen
Siddharth Iyer
Theo Kurtén
Weiwei Hu
Douglas A Day
Pedro Campuzano-Jost
Jose L Jimenez
Lu Xu
Nga Lee Ng
Hongyu Guo
Rodney J Weber
Robert J Wild
Steven S Brown
Abigail Koss
Joost de Gouw
Kevin Olson
Allen H Goldstein
Roger Seco
Saewung Kim
Kevin McAvey
Paul B Shepson
Tim Starn
Karsten Baumann
Eric S Edgerton
Jiumeng Liu
John E Shilling
David O Miller
William Brune
Siegfried Schobesberger
Emma L D'Ambro
Joel A Thornton
Published in Proceedings of the National Academy of Sciences of the United States of America
Volume 113
Issue 6
Pages 1516-21
ISSN 1091-6490
Publication year 2016
Published at Department of Chemistry and Molecular Biology
Pages 1516-21
Language en
Links dx.doi.org/10.1073/pnas.1508108113
Subject categories Analytical Chemistry, Organic Chemistry, Climate Research, Environmental chemistry, Meteorology and Atmospheric Sciences

Abstract

Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene- and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas-particle equilibrium and (ii) have a short particle-phase lifetime (∼2-4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment.

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