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

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dc.citation.firstpage17031en_US
dc.citation.journalTitleAtmospheric Chemistry and Physicsen_US
dc.citation.lastpage17050en_US
dc.citation.volumeNumber21en_US
dc.contributor.authorBui, Alexander A.T.en_US
dc.contributor.authorWallace, Henry W.en_US
dc.contributor.authorKavassalis, Sarahen_US
dc.contributor.authorAlwe, Hariprasad D.en_US
dc.contributor.authorFlynn, James H.en_US
dc.contributor.authorErickson, Matt H.en_US
dc.contributor.authorAlvarez, Sergioen_US
dc.contributor.authorMillet, Dylan B.en_US
dc.contributor.authorSteiner, Allison L.en_US
dc.contributor.authorGriffin, Robert J.en_US
dc.date.accessioned2021-12-15T22:10:19Zen_US
dc.date.available2021-12-15T22:10:19Zen_US
dc.date.issued2021en_US
dc.description.abstractExchanges 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.en_US
dc.identifier.citationBui, Alexander A.T., Wallace, Henry W., Kavassalis, Sarah, et al.. "Transport-driven aerosol differences above and below the canopy of a mixed deciduous forest." <i>Atmospheric Chemistry and Physics,</i> 21, (2021) Copernicus Publications: 17031-17050. https://doi.org/10.5194/acp-21-17031-2021.en_US
dc.identifier.digitalacp-21-17031-2021en_US
dc.identifier.doihttps://doi.org/10.5194/acp-21-17031-2021en_US
dc.identifier.urihttps://hdl.handle.net/1911/111792en_US
dc.language.isoengen_US
dc.publisherCopernicus Publicationsen_US
dc.rightsThis work is distributed under the Creative Commons Attribution 4.0 License.en_US
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en_US
dc.titleTransport-driven aerosol differences above and below the canopy of a mixed deciduous foresten_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpublisher versionen_US
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