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- Title
Differences in BVOC oxidation and SOA formation above and below the forest canopy.
- Authors
Schulze, Benjamin C.; Wallace, Henry W.; Flynn, James H.; Lefer, Barry L.; Erickson, Matt H.; Jobson, B. Thomas; Dusanter, Sebastien; Griffith, Stephen M.; Hansen, Robert F.; Stevens, Philip S.; Griffin, Robert J.
- 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). The nitrate radical (NO3) is especially reactive towards isoprene and monoterpenes such as α-pinene. A zero-dimensional model has been used to investigate differences in oxidation and SOA production from these two BVOCs, especially with respect to hydroxyl radical (OH) and NO3, above and below a forest canopy in rural Michigan using local data and data from a monitoring site in Detroit. In all modeled scenarios, NO3 concentrations are relatively small (0.5-3 pptv); however, daytime concentrations below the canopy are two-to-three times larger than those above. In the rural scenario, NO3 contributes up to 20% of daytime oxidation of α-pinene below the canopy, and this contribution increases to around 40% in the polluted cases. Oxidation of isoprene is almost entirely dominated by reaction with OH, as expected. The most significant first-generation RONO2 formation mechanism varies significantly between scenarios and by canopy location. Nonetheless, in every scenario, daytime production of first-generation RONO2 through NO3 + α-pinene is more significant below the canopy than above. While SOA mass loadings are moderate (2 μg m-3 or less), total SOA production is consistently enhanced below the canopy, due to the combined effects of elevated isoprene and reduced NO concentrations. Furthermore, below the canopy, the total amount of RONO2 SOA produced through NO3 oxidation of α-pinene during the daytime (10:00-18:00), while small in absolute terms, is more than twice as large as the amount produced above the canopy during that time period in every scenario. In the rural ambient case, a minimum of 74% of α-pinene RONO2 SOA is formed solely from initial oxidation by NO3. The relative abundances of HO2 and NO are shown to substantially impact both total SOA production and RONO2 SOA composition. The results presented emphasize the need for more detailed studies regarding the influence of NO3 throughout forest canopies in different environments.
- Subjects
OXIDATION of volatile organic compounds; ATMOSPHERIC aerosols; GAS phase reactions; TROPOSPHERE; FOREST canopies; HYDROXYL group
- Publication
Atmospheric Chemistry & Physics Discussions, 2016, p1
- ISSN
1680-7367
- Publication type
Article
- DOI
10.5194/acp-2016-485