Transport-driven aerosol differences above and below the canopy of a mixed deciduous forest

TitleTransport-driven aerosol differences above and below the canopy of a mixed deciduous forest
Publication TypeJournal Article
Year of Publication2021
AuthorsBui AAT, Wallace HW, Kavassalis S, Alwe HD, Flynn JH, Erickson MH, Alvarez S, Millet DB, Steiner AL, Griffin RJ
JournalAtmospheric Chemistry and Physics
Volume21
Issue22
Pagination17031 - 17050
Date PublishedJan-01-2021
Abstract

Exchanges of energy and mass between the surrounding air and plant surfaces occur below, within, and above a forest's vegetative canopy. The canopy also can lead to vertical gradients in light, trace gases, oxidant availability, turbulent mixing, and properties and concentrations of organic aerosol (OA). In this study, a high-resolution time-of-flight aerosol mass spectrometer was used to measure non-refractory submicron aerosol composition and concentration above (30 m) and below (6 m) a forest canopy in a mixed deciduous forest at the Program for Research on Oxidants: PHotochemistry, Emissions, and Transport tower in northern Michigan during the summer of 2016. Three OA factors are resolved using positive matrix factorization: more-oxidized oxygenated organic aerosol (MO-OOA), isoprene-epoxydiol-derived organic aerosol (IEPOX-OA), and 91Fac (a factor characterized with a distinct fragment ion at m/z 91) from both the above- and the below-canopy inlets. MO-OOA was most strongly associated with long-range transport from more polluted regions to the south, while IEPOX-OA and 91Fac were associated with shorter-range transport and local oxidation chemistry. Overall vertical similarity in aerosol composition, degrees of oxidation, and diurnal profiles between the two inlets was observed throughout the campaign, which implies that rapid in-canopy transport of aerosols is efficient enough to cause relatively consistent vertical distributions of aerosols at this scale. However, four distinct vertical gradient episodes are identified for OA, with vertical concentration differences (above-canopy minus below-canopy concentrations) in total OA of up to 0.8 µg m−3, a value that is 42 % of the campaign average OA concentration of 1.9 µg m−3. The magnitude of these differences correlated with concurrent vertical differences in either sulfate aerosol or ozone. These differences are likely driven by a combination of long-range transport mechanisms, canopy-scale mixing, and local chemistry. These results emphasize the importance of including vertical and horizontal transport mechanisms when interpreting trace gas and aerosol data in forested environments.

URLhttps://acp.copernicus.org/articles/21/17031/2021/
DOI10.5194/acp-21-17031-202110.5194/acp-21-17031-2021-supplement
Short TitleAtmos. Chem. Phys.
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