A three-dimensional total odd nitrogen (NOy) simulation during SONEX using a stretched-grid chemical transport model

The relative importance of various odd nitrogen (NOy) sources including lightning, aircraft, and surface emissions on upper tropospheric total odd nitrogen is illustrated as a first application of the three-dimensional Stretched-Grid University of Maryland/Goddard Chemical-Transport Model (SG-GCTM). The SG-GCTM has been developed to look at the effect of localized sources and/or small-scale mixing processes on the large-scale or global chemical balance. For this simulation the stretched grid was chosen so that its maximum resolution is located over eastern North America and the North Atlantic; a region that includes most of the Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) flight paths, The SONEX period (October-November 1997) is simulated by driving the SG-GCTM with assimilated data from the Goddard Earth Observing System-Stratospheric Tracers of Atmospheric Transport Data Assimilation System (GEOS-STRAT DAS). A new algorithm is used to estimate the lightning flash rates needed to calculate NOy emission by lightning. This algorithm parameterizes the flash rate in terms of upper tropospheric convective mass flux. Model-calculated upper tropospheric NOy and NOy measurements from the NASA DC-8 aircraft are compared. Spatial variations in NOy were well captured especially with the stretched-grid run; however, model-calculated peaks due to "stratospheric" NOy are occasionally too large. The lightning algorithm reproduces the temporally and spatially averaged total flash rate accurately; however, the use of emissions from observed lightning flashes significantly improves the simulation on a few days, especially November 3, 1997, showing that significant uncertainty remains in parameterizing lightning in chemistry and transport models. Aircraft emissions contributed similar to 15% of the upper tropospheric NOy averaged along SONEX flight paths within the North Atlantic Flight Corridor with the contribution exceeding 40% during portions of some flights.