Chemistry and Physics Faculty Articles

Document Type

Article

Publication Date

11-16-2001

Keywords

Aerosols and particles, Chemical kinetic and photochemical properties, Pollution, Troposphere

Publication Title

Journal of Geophysical Research: Atmospheres

ISSN

2169-897X

Volume

106

Issue/No.

D21

First Page

27619

Last Page

27634

Peer Reviewed

1

Abstract

A series of controlled experiments were carried out in the Calspan Corporation's 600 m3environmental chamber to study some secondary organic aerosol formation processes. Three precursor-ozone systems were studied: cyclopentene-ozone, cyclohexene-ozone, and α-pineneozone. Additionally, SO2 was added to the initial gas mixture in several instances and was likely present at trace levels in the ostensibly organic-only experiments. It was found that all three systems readily formed new submicron aerosols at very low reactant levels. The chemical composition of formed aerosols was consistent with some previous studies, but the yields of organic products were found to be lower in the Calspan experiments. A three-step procedure is proposed to explain the observed particle nucleation behavior: HO · production → H2SO4 formation → H2SO4-H2O (perhaps together with NH3) homogeneous nucleation. It is also proposed that some soluble organic products would partition into the newly formed H2SO4-H2O nuclei, enhance water condensation, and quickly grow these nuclei into a larger size range. While the observations in the two cycloolefin-ozone systems could be well explained by these proposed mechanisms, the exact nature of the nucleation process in the α-pinene-ozone system remains rather opaque and could be the result of nucleation involving certain organics. The results from three simple modeling studies further support these proposals. Their applicability to the marine boundary layer (MBL) is also discussed in some detail. Particularly, such a particle nucleation and growth process could play an important role in secondary aerosol formation and, quite likely, CCN formation as well in certain MBL regions.

Comments

©2001 by the American Geophysical Union

DOI

10.1029/2001JD900170

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