Impact of climate variability on tropospheric ozone.

A simulation with the climate-chemistry model (CCM) E39/C is presented, which covers both the troposphere and stratosphere dynamics and chemistry during the period 1960 to 1999. Although the CCM, by its nature, is not exactly representing observed day-by-day meteorology, there is an overall model's tendency to correctly reproduce the variability pattern due to an inclusion of realistic external forcings, like observed sea surface temperatures (e.g. El Niño), major volcanic eruption, solar cycle, concentrations of greenhouse gases, and Quasi-Biennial Oscillation. Additionally, climate-chemistry interactions are included, like the impact of ozone, methane, and other species on radiation and dynamics, and the impact of dynamics on emissions (lightning). However, a number of important feedbacks are not yet included (e.g. feedbacks related to biogenic emissions and emissions due to biomass burning). The results show a good representation of the evolution of the stratospheric ozone layer, including the ozone hole, which plays an important role for the simulation of natural variability of tropospheric ozone. Anthropogenic NO(x) emissions are included with a step-wise linear trend for each sector, but no interannual variability is included. The application of a number of diagnostics (e.g. marked ozone tracers) allows the separation of the impact of various processes/emissions on tropospheric ozone and shows that the simulated Northern Hemisphere tropospheric ozone budget is not only dominated by nitrogen oxide emissions and other ozone pre-cursors, but also by changes of the stratospheric ozone budget and its flux into the troposphere, which tends to reduce the simulated positive trend in tropospheric ozone due to emissions from industry and traffic during the late 80s and early 90s. For tropical regions the variability in ozone is dominated by variability in lightning (related to ENSO) and stratosphere-troposphere exchange (related to Northern Hemisphere Stratospheric dynamics and solar activity). Since tropospheric background chemistry is regarded only, the results are quantitatively limited with respect to derived trends. However, the main results are regarded to be robust. Although the horizontal resolution is rather coarse in comparison to regional models, such kind of simulations provide useful and necessary information on the impact of large-scale processes and inter-annual/decadal variations on regional air quality.