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TitleChemical evolution of atmospheric organic carbon over multiple generations of oxidation.
Publication TypeJournal Article
Year2018
AuthorsIsaacman-VanWertz G, Massoli P, O'Brien R, Lim C, Franklin JP, Moss JA, Hunter JF, Nowak JB, Canagaratna MR, Misztal PK, Arata C, Roscioli JR, Herndon ST, Onasch TB, Lambe AT, Jayne JT, Su L, Knopf DA, Goldstein AH, Worsnop DR, Kroll JH
JournalNat Chem
Volume10
Issue4
Pagination462-468
Date2018 Apr
ISSN1755-4349
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.

DOI10.1038/s41557-018-0002-2
Alternate JournalNat Chem
PubMed ID29483638
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