Surface ozone and its precursors at Summit, Greenland: comparison between observations and model simulations

Recent studies have shown significant challenges for atmospheric models to simulate tropospheric ozone (O<sub>3</sub>) and its precursors in the Arctic. In this study, ground-based data were combined with a global 3-D chemical transport model (GEOS-Chem) to examine the abundance and s...

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Bibliographic Details
Main Authors: Y. Huang, S. Wu, L. J. Kramer, D. Helmig, R. E. Honrath
Format: Article
Language:English
Published: Copernicus Publications 2017-12-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/17/14661/2017/acp-17-14661-2017.pdf
Description
Summary:Recent studies have shown significant challenges for atmospheric models to simulate tropospheric ozone (O<sub>3</sub>) and its precursors in the Arctic. In this study, ground-based data were combined with a global 3-D chemical transport model (GEOS-Chem) to examine the abundance and seasonal variations of O<sub>3</sub> and its precursors at Summit, Greenland (72.34° N, 38.29° W; 3212 m a.s.l.). Model simulations for atmospheric nitrogen oxides (NO<sub><i>x</i></sub>), peroxyacetyl nitrate (PAN), ethane (C<sub>2</sub>H<sub>6</sub>), propane (C<sub>3</sub>H<sub>8</sub>), carbon monoxide (CO), and O<sub>3</sub> for the period July 2008–June 2010 were compared with observations. The model performed well in simulating certain species (such as CO and C<sub>3</sub>H<sub>8</sub>), but some significant discrepancies were identified for other species and further investigated. The model generally underestimated NO<sub><i>x</i></sub> and PAN (by  ∼  50 and 30 %, respectively) for March–June. Likely contributing factors to the low bias include missing NO<sub><i>x</i></sub> and PAN emissions from snowpack chemistry in the model. At the same time, the model overestimated NO<sub><i>x</i></sub> mixing ratios by more than a factor of 2 in wintertime, with episodic NO<sub><i>x</i></sub> mixing ratios up to 15 times higher than the typical NO<sub><i>x</i></sub> levels at Summit. Further investigation showed that these simulated episodic NO<sub><i>x</i></sub> spikes were always associated with transport events from Europe, but the exact cause remained unclear. The model systematically overestimated C<sub>2</sub>H<sub>6</sub> mixing ratios by approximately 20 % relative to observations. This discrepancy can be resolved by decreasing anthropogenic C<sub>2</sub>H<sub>6</sub> emissions over Asia and the US by  ∼ 20 %, from 5.4 to 4.4 Tg year<sup>−1</sup>. GEOS-Chem was able to reproduce the seasonal variability of O<sub>3</sub> and its spring maximum. However, compared with observations, it underestimated surface O<sub>3</sub> by approximately 13 % (6.5 ppbv) from April to July. This low bias appeared to be driven by several factors including missing snowpack emissions of NO<sub><i>x</i></sub> and nitrous acid in the model, the weak simulated stratosphere-to-troposphere exchange flux of O<sub>3</sub> over the summit, and the coarse model resolution.
ISSN:1680-7316
1680-7324