Sensitivity to grid resolution in the ability of a chemical transport model to simulate observed oxidant chemistry under high-isoprene conditions
Item
Title (Dublin Core)
Sensitivity to grid resolution in the ability of a chemical transport model to simulate observed oxidant chemistry under high-isoprene conditions
Description (Dublin Core)
Formation of ozone and organic aerosol in continental atmospheres depends on whether isoprene emitted by vegetation is oxidized by the high-NO<sub><i>x</i></sub> pathway (where peroxy radicals react with NO) or by low-NO<sub><i>x</i></sub> pathways (where peroxy radicals react by alternate channels, mostly with HO<sub>2</sub>). We used mixed layer observations from the SEAC<sup>4</sup>RS aircraft campaign over the Southeast US to test the ability of the GEOS-Chem chemical transport model at different grid resolutions (0.25° × 0.3125°, 2° × 2.5°, 4° × 5°) to simulate this chemistry under high-isoprene, variable-NO<sub><i>x</i></sub> conditions. Observations of isoprene and NO<sub><i>x</i></sub> over the Southeast US show a negative correlation, reflecting the spatial segregation of emissions; this negative correlation is captured in the model at 0.25° × 0.3125° resolution but not at coarser resolutions. As a result, less isoprene oxidation takes place by the high-NO<sub><i>x</i></sub> pathway in the model at 0.25° × 0.3125° resolution (54 %) than at coarser resolution (59 %). The cumulative probability distribution functions (CDFs) of NO<sub><i>x</i></sub>, isoprene, and ozone concentrations show little difference across model resolutions and good agreement with observations, while formaldehyde is overestimated at coarse resolution because excessive isoprene oxidation takes place by the high-NO<sub><i>x</i></sub> pathway with high formaldehyde yield. The good agreement of simulated and observed concentration variances implies that smaller-scale non-linearities (urban and power plant plumes) are not important on the regional scale. Correlations of simulated vs. observed concentrations do not improve with grid resolution because finer modes of variability are intrinsically more difficult to capture. Higher model resolution leads to decreased conversion of NO<sub><i>x</i></sub> to organic nitrates and increased conversion to nitric acid, with total reactive nitrogen oxides (NO<sub><i>y</i></sub>) changing little across model resolutions. Model concentrations in the lower free troposphere are also insensitive to grid resolution. The overall low sensitivity of modeled concentrations to grid resolution implies that coarse resolution is adequate when modeling continental boundary layer chemistry for global applications.
Creator (Dublin Core)
Yu, Karen
Jacob, Daniel J.
Fisher, Jenny A.
Kim, Patrick S.
Marais, Eloise A.
Miller, Christopher C.
Travis, Katherine R.
Zhu, Lei
Yantosca, Robert M.
Sulprizio, Melissa P.
Cohen, Ron C.
Dibb, Jack E.
Fried, Alan
Mikoviny, Tomas
Ryerson, Thomas B.
Wennberg, Paul O.
Wisthaler, Armin
Date (Dublin Core)
2018-09-10
Type (Dublin Core)
Text
Format (Dublin Core)
application/pdf
Identifier (Dublin Core)
10.5194/acp-16-4369-2016
https://acp.copernicus.org/articles/16/4369/2016/
Source (Dublin Core)
eISSN: 1680-7324
Language (Dublin Core)
eng
