TROPOSPHERIC OZONE AND ITS RADIATIVE EFFECTS DUE TO ANTHROPOGENIC AND LIGHTNING EMISSIONS: GLOBAL AND REGIONAL MODELING

Abstract

We analyze the contribution of North American (NA) lightning and anthropogenic emissions to summertime ozone concentrations, radiative forcing, and exports from North America using the global University of Maryland chemistry transport model (UMD-CTM) and the regional scale Weather Research and Forecasting model with chemistry (WRF-Chem). Lightning NO contributes by 15&ndash;20 ppbv to upper tropospheric ozone concentrations over the United States with the effects of NA lightning on ozone seen as far east as North Africa and Europe. Using the UMD-CTM, we compare changes in surface and column ozone amounts due to the NOx State Implementation Plan (SIP) Call with the natural variability in ozone due to changes in meteorology and lightning. Comparing early summer 2004 with 2002, surface ozone decreased by up to 5 ppbv due to the NO_x SIP Call while changes in meteorology and lightning resulted in a 0.3&ndash;1.4 ppbv increase in surface ozone. Ozone column variability was driven primarily by changes in lightning NO emissions, especially over the North Atlantic. As part of our WRF-Chem analysis, we modify the radiation schemes to use model-calculated ozone (interactive ozone) instead of climatological ozone profiles and conduct multiple 4-day simulations of July 2007. We found that interactive ozone increased the outgoing longwave radiation (OLR) by 3 W m<super>&minus;2</super> decreasing the bias with respect to remotely sensed OLR. The improvement is due to a high bias in the climatological ozone profiles. The interactive ozone had a small impact on mean upper troposphere temperature (&minus;0.15°C). The UMD-CTM simulations indicate that NA anthropogenic emissions are responsible for more ozone export but less ozone radiative forcing than lightning NO emissions. Over the North Atlantic, NA anthropogenic emissions contributed 0.15&ndash;0.30 W m<super>&minus;2</super> to the net downward radiative flux at the tropopause while NA lightning contributed 0.30&ndash;0.50 W m<super>&minus;2</super>. The ozone export from anthropogenic emissions was almost twice as large as that from lightning emissions. The WRF-Chem simulations show that the export of reactive nitrogen was 23%&ndash;28% of the boundary layer emissions and 26%&ndash;38% of the total emissions including lightning NO.