The impact of North American anthropogenic emissions and lightning on long-range transport of trace gases and their export from the continent during summers 2002 and 2004

摘要

We analyze the contribution of North American (NA) lightning and anthropogenic emissions to ozone concentrations, radiative forcing, and export fluxes from North America during summers 2002 and 2004 using the University of Maryland Chemical Transport Model (UMD-CTM) driven by GEOS-4 reanalysis. Reduced power plant emissions (NOx SIP Call) and cooler temperatures in 2004 compared to 2002 resulted in lower ambient ozone concentrations over the eastern United States. Lightning flash rates in early summer 2004 were 50% higher than 2002 over the United States. Over the North Atlantic, changes in ozone column between early summer 2002 and 2004 due to changes in lightning and meteorology exceeded the change due to emission reductions by a factor of 7. Late summer changes in lightning had a much smaller impact on ozone columns. In summer 2004, net downward radiative flux at the tropopause due to ozone produced from anthropogenic emissions ranged from 0.15 to 0.30 W m−2 across the North Atlantic, while that due to ozone produced from lightning NO emissions ranged from 0.20 to 0.50 W m−2. Enhanced lofting of polluted air followed by stronger westerly winds led to more net export of NOx, NOy, and ozone in early summer 2004 than 2002 despite reduced anthropogenic emissions. Ozone export fluxes across the eastern NA boundary due to anthropogenic emissions were factors of 1.6 and 2 larger than those due to lightning in 2004 and 2002, respectively. Doubling the NA lightning NO source increased downwind ozone enhancements due to lightning NO emissions by one third.