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Discussion papers
https://doi.org/10.5194/acp-2018-717
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-717
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 10 Aug 2018

Research article | 10 Aug 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Biogenic emissions and land-atmosphere interactions as drivers of the diurnal evolution of secondary organic aerosol in the southeastern US

Juhi Nagori1,2, Ruud H. H. Jannsen3, Juliane L. Fry4, Maarten Krol1,2, Jose L. Jimenez5,6, Weiwei Hu5,6, and Jordi Vilà-Guerau de Arellano1 Juhi Nagori et al.
  • 1Meteorology and Air Quality, Wageningen University, Wageningen, the Netherlands
  • 2Institute of Marine and Atmospheric Research, University of Utrecht, Utrecht, the Netherlands
  • 3Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
  • 4Department of Chemistry, Reed College, Portland, OR, USA
  • 5Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
  • 6Department of Chemistry, University of Colorado, Boulder, CO, USA

Abstract. The interactions between biogenic volatile organic compounds (BVOCs), like isoprene and monoterpenes, and anthropogenic emissions of nitrogen and sulfur oxides lead to high concentrations of secondary organic aerosol (SOA) in the southeastern United States. To improve our understanding of SOA formation, we study the diurnal evolution of SOA in a land-atmosphere coupling context, based on comprehensive surface and upper air observations from a characteristic day during the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. We use a mixed layer model (MXLCH-SOA) that is updated with new chemical pathways and an interactive land surface scheme that describes both biogeochemical and biogeophysical couplings between the land surface and the atmospheric boundary layer (ABL).

MXLCH-SOA reproduces observed BVOC and surface heat fluxes, gas-phase chemistry and ABL dynamics well, with the exception of isoprene and monoterpene mixing ratios measured close to the land surface. This is likely due to the fact that these species do not have uniform profiles throughout the atmospheric surface layer, due to their fast reaction with OH and incomplete mixing near the surface. SOA formation from isoprene through the intermediate species IEPOX and ISOPOOH is in good agreement with the observations, with a mean isoprene SOA yield of 1.8%, and mean monoterpene yield of 10.7%.

However, SOA from monoterpenes, oxidized by OH and O3, dominates the locally produced SOA (69%). Isoprene SOA is produced primarily through OH oxidation via ISOPOOH and IEPOX (31%).

A sensitivity analysis of the coupled land surface-boundary layer-SOA formation system to changing temperatures reveals that SOA concentrations are buffered under increasing temperatures: a rise in BVOCs emissions is offset by decreases in OH concentrations and the efficiency with which SVOCs partition into the aerosol phase.

Juhi Nagori et al.
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Juhi Nagori et al.
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Short summary
Secondary organic aerosols (SOA) are produced through a complex interaction of sunlight, volatile organic compounds emitted from trees, anthropogenic emissions and atmospheric chemistry. We are able to successfully model the formation and diurnal evolution of SOA, using a model that takes into consideration the surface and boundary layer dynamics (1–2 km from the surface) and photochemistry, above the southeastern US using data collected during the SOAS campaign to constrain the model.
Secondary organic aerosols (SOA) are produced through a complex interaction of sunlight,...
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