ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-11-11707-2011 Accounting for non-linear chemistry of ship plumes in the GEOS-Chem global chemistry transport model Vinken G. C. M. 1 5 Boersma K. F. 1 2 Jacob D. J. 3 Meijer E. W. 4 Eindhoven University of Technology, Eindhoven, The Netherlands Royal Netherlands Meteorological Institute, De Bilt, The Netherlands Harvard University, Cambridge, USA TNO, Utrecht, The Netherlands <i>Invited contribution by G. C. M. Vinken, recipient of the EGU Outstanding Student Poster Award 2011.</i> 23 11 2011 11 22 11707 11722 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/11/11707/2011/acp-11-11707-2011.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/11/11707/2011/acp-11-11707-2011.pdf

We present a computationally efficient approach to account for the non-linear chemistry occurring during the dispersion of ship exhaust plumes in a global 3-D model of atmospheric chemistry (GEOS-Chem). We use a plume-in-grid formulation where ship emissions age chemically for 5 h before being released in the global model grid. Besides reducing the original ship NO<sub>x</sub> emissions in GEOS-Chem, our approach also releases the secondary compounds ozone and HNO<sub>3</sub>, produced during the 5 h after the original emissions, into the model. We applied our improved method and also the widely used "instant dilution" approach to a 1-yr GEOS-Chem simulation of global tropospheric ozone-NO<sub>x</sub>-VOC-aerosol chemistry. We also ran simulations with the standard model (emitting 10 molecules O<sub>3</sub> and 1 molecule HNO<sub>3</sub> per ship NO<sub>x</sub> molecule), and a model without any ship emissions at all. The model without any ship emissions simulates up to 0.1 ppbv (or 50%) lower NO<sub>x</sub> concentrations over the North Atlantic in July than our improved GEOS-Chem model. "Instant dilution" overestimates NO<sub>x</sub> concentrations by 0.1 ppbv (50%) and ozone by 3–5 ppbv (10–25%), compared to our improved model over this region. These conclusions are supported by comparing simulated and observed NO<sub>x</sub> and ozone concentrations in the lower troposphere over the Pacific Ocean. The comparisons show that the improved GEOS-Chem model simulates NO<sub>x</sub> concentrations in between the instant dilution model and the model without ship emissions, which results in lower O<sub>3</sub> concentrations than the instant dilution model. The relative differences in simulated NO<sub>x</sub> and ozone between our improved approach and instant dilution are smallest over strongly polluted seas (e.g. North Sea), suggesting that accounting for in-plume chemistry is most relevant for pristine marine areas.

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