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Chemical evolution of atmospheric organic carbon over multiple generations of oxidation

Author(s)
Massoli, Paola; Nowak, John B.; Canagaratna, Manjula R.; Misztal, Pawel K.; Arata, Caleb; Roscioli, Joseph R.; Herndon, Scott T.; Onasch, Timothy B.; Lambe, Andrew T.; Jayne, John T.; Su, Luping; Knopf, Daniel A.; Goldstein, Allen H.; Worsnop, Douglas R.; Isaacman, Gabriel; Sellon, Rachel E.; Lim, Christopher Yung-Ta; Franklin, Jonathan Pfeil; Moss, Joshua Alexandre; Hunter, James Freeman; Kroll, Jesse; ... Show more Show less
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Abstract
The evolution of atmospheric organic carbon as it undergoes oxidation has a controlling influence on concentrations of key atmospheric species, including particulate matter, ozone and oxidants. However, full characterization of organic carbon over hours to days of atmospheric processing has been stymied by its extreme chemical complexity. Here we study the multigenerational oxidation of α-pinene in the laboratory, characterizing products with several state-of-the-art analytical techniques. Although quantification of some early generation products remains elusive, full carbon closure is achieved (within measurement uncertainty) by the end of the experiments. These results provide new insights into the effects of oxidation on organic carbon properties (volatility, oxidation state and reactivity) and the atmospheric lifecycle of organic carbon. Following an initial period characterized by functionalization reactions and particle growth, fragmentation reactions dominate, forming smaller species. After approximately one day of atmospheric aging, most carbon is sequestered in two long-lived reservoirs—volatile oxidized gases and low-volatility particulate matter.
Date issued
2018-02
URI
http://hdl.handle.net/1721.1/119485
Department
Massachusetts Institute of Technology. Department of Civil and Environmental Engineering
Journal
Nature Chemistry
Publisher
Nature Publishing Group
Citation
Isaacman-VanWertz et al. “Chemical Evolution of Atmospheric Organic Carbon over Multiple Generations of Oxidation.” Nature Chemistry 10, no. 4 (February 26, 2018): 462–468.
Version: Final published version
ISSN
1755-4330
1755-4349

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