DISTRIBUTION AND BUDGET OF O-3 IN THE TROPOSPHERE CALCULATED WITH A CHEMISTRY GENERAL-CIRCULATION MODEL

We present results of global tropospheric chemistry simulations with the coupled chemistry/atmospheric general circulation model ECHAM. Ultimately, the model will be used to study climate changes induced by anthropogenic influences on the chemistry of the atmosphere; meteorological parameters that are important for the chemistry, such as temperature, humidity, air motions, cloud and lain characteristics, and mixing processes are calculated on-line. The chemical part of the model describes background tropospheric CH4-CO-NOx-HOx photochemistry. Emissions of NO and CO, surface concentrations of CH4, and stratospheric concentrations of O-3 and NOy are prescribed as boundary conditions. Calculations of the tropospheric O-3 budget indicate that seasonal variabilities of the photochemical production and of injection from the stratosphere are represented realistically, although some aspects of the model still need improvement. Comparisons of calculated O-3 surface concentrations and O-3 profiles with available measurements show that the model reproduces O-3 distributions in remote tropical and midlatitudinal sites. Also, the model matches typical profiles connected with deep convection in the Intertropical Convergence Zone (ITCZ). However, the model tends to underestimate O-3 concentrations at the poles and in relatively polluted regions. These underestimates are caused by the poor representation of tropopause foldings in midlatitudes, which form a significant source of tropospheric O-3 from the stratosphere, too weak transport to the poles, and the neglect of higher hydrocarbon chemistry. Also, mixing of polluted continental boundary layer air into the free troposphere may be underestimated. We discuss how these model deficiencies will be improved in the future.