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    Differences in BVOC oxidation and SOA formation above and below the forest canopy

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    Author
    Schulze, Benjamin C.; Wallace, Henry W.; Flynn, James H.; Lefer, Barry L.; Erickson, Matt H.; More... Jobson, B. Tom; Dusanter, Sebastien; Griffith, Stephen M.; Hansen, Robert F.; Stevens, Philip S.; VanReken, Timothy; Griffin, Robert J. Less...
    Date
    2017
    Abstract
    Gas-phase biogenic volatile organic compounds (BVOCs) are oxidized in the troposphere to produce secondary pollutants such as ozone (O3), organic nitrates (RONO2), and secondary organic aerosol (SOA). Two coupled zero-dimensional models have been used to investigate differences in oxidation and SOA production from isoprene and α-pinene, especially with respect to the nitrate radical (NO3), above and below a forest canopy in rural Michigan. In both modeled environments (above and below the canopy), NO3 mixing ratios are relatively small (< 0.5 pptv); however, daytime (08:00–20:00 LT) mixing ratios below the canopy are 2 to 3 times larger than those above. As a result of this difference, NO3 contributes 12 % of total daytime α-pinene oxidation below the canopy while only contributing 4 % above. Increasing background pollutant levels to simulate a more polluted suburban or peri-urban forest environment increases the average contribution of NO3 to daytime below-canopy α-pinene oxidation to 32 %. Gas-phase RONO2 produced through NO3 oxidation undergoes net transport upward from the below-canopy environment during the day, and this transport contributes up to 30 % of total NO3-derived RONO2 production above the canopy in the morning (∼ 07:00). Modeled SOA mass loadings above and below the canopy ultimately differ by less than 0.5 µg m−3, and extremely low-volatility organic compounds dominate SOA composition. Lower temperatures below the canopy cause increased partitioning of semi-volatile gas-phase products to the particle phase and up to 35 % larger SOA mass loadings of these products relative to above the canopy in the model. Including transport between above- and below-canopy environments increases above-canopy NO3-derived α-pinene RONO2 SOA mass by as much as 45 %, suggesting that below-canopy chemical processes substantially influence above-canopy SOA mass loadings, especially with regard to monoterpene-derived RONO2.
    Citation
    Schulze, Benjamin C., Wallace, Henry W., Flynn, James H., et al.. "Differences in BVOC oxidation and SOA formation above and below the forest canopy." Atmospheric Chemistry and Physics, 17, (2017) Copernicus Publications on behalf of the European Geosciences Union: 1828. http://dx.doi.org/10.5194/acp-17-1805-2017.
    Published Version
    http://dx.doi.org/10.5194/acp-17-1805-2017
    Type
    Journal article
    Publisher
    Copernicus Publications on behalf of the European Geosciences Union
    Citable link to this page
    https://hdl.handle.net/1911/94020
    Rights
    This work is distributed under the Creative Commons Attribution 3.0 License.
    Link to License
    https://creativecommons.org/licenses/by/3.0/us/
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    • Civil and Environmental Engineering Publications [208]
    • Faculty Publications [5504]

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    Managed by the Digital Scholarship Services at Fondren Library, Rice University
    Physical Address: 6100 Main Street, Houston, Texas 77005
    Mailing Address: MS-44, P.O.BOX 1892, Houston, Texas 77251-1892
    Site Map