Accounting for non-linear chemistry of ship plumes in the GEOS-Chem global chemistry transport model

Abstract

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 NOx emissions in GEOS-Chem, our approach also releases the secondary compounds ozone and HNO3, 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-NOx-VOC-aerosol chemistry. We also ran simulations with the standard model (emitting 10 molecules O3 and 1 molecule HNO3 per ship NOx 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 NOx concentrations over the North Atlantic in July than our improved GEOS-Chem model. "Instant dilution" overestimates NOx 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 NOx and ozone concentrations in the lower troposphere over the Pacific Ocean. The comparisons show that the improved GEOS-Chem model simulates NOx concentrations in between the instant dilution model and the model without ship emissions, which results in lower O3 concentrations than the instant dilution model. The relative differences in simulated NOx 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. © Author(s) 2011.