Vertical distribution and sources of tropospheric ozone over South China in spring 2004: Ozonesonde measurements and modeling analysis

The Transport of Air Pollutant and Tropospheric Ozone over China (TAPTO-China) science initiative is a two-year (TAPTO 2004 and 2005) field measurement campaign to help improve our understanding of the physical and chemical processes that control the tropospheric ozone budget over the Chinese subcontinent (including the Asian Pacific rim) and its surrounding SE Asia. In this paper, we use two state-of-the-art 3-D global chemical transport models (GEOS-Chem and Global Modeling Initiative or GMI) to examine the characteristics of vertical distribution and quantify the sources of tropospheric ozone by analysis of TAPTO in-situ ozonesonde data obtained at five stations in South China during spring (April and May) 2004: Lin’an (30.30N, 119.75E), Tengchong (25.01N, 98.30E), Taipei (25.0N, 121.3E), Hong Kong (22.21N, 114.30E) and Sanya (18.21N, 110.31E). The observed tropospheric ozone concentrations show strong spatial and temporal variability, which is largely captured by the models. The models simulate well the observed vertical gradients of tropospheric ozone at higher latitudes but are too low at lower latitudes. Model tagged ozone simulations suggest that stratosphere has a large impact on the upper and middle troposphere (UT/MT) at Lin’an and Tengchong. Continental SE Asian biomass burning emissions are maximum in March but still contribute significantly to the photochemical production of tropopheric ozone in South China in early April. Asian anthropogenic emissions are the major contribution to lower tropospheric ozone at all stations. On the other hand, there are episodes of influence from European/North American anthropogenic emissions. For example, model tagged ozone simulations show that over Lin’an in April 2004, stratosphere contributes 20% (13 ppbv) at 5 km, Asian boundary layer contributes 70% (46 ppbv) to ozone in the boundary layer, European boundary layer contributes 5% (3-4 ppbv) at 1.2 km, and North American boundary layer contributes 4.5% (3 ppbv) at 1.2 km. Lastly, our analysis suggests that lightning NOx emissions have substantial impact on the UT/MT ozone over South China. We argue that model underestimate of ozone concentrations, especially at lower latitudes, is likely due to too low lightning NOx emissions.