Search

In recent years several methods have been developed that derive total tropospheric 03 columns from satellite measurements. However, one issue that has not been paid much attention to is the interpretation of (extratropical) total tropospheric O3 columns. Different processes contribute to the total tropospheric 03 column: stratosphere-troposphere exchange, tropospheric O 3 production and loss, transport and the height of the tropopause. Each process contributes differently to the total tropospheric O3 column variability depending on season, geographical location, and altitude. This paper investigates the contribution of these different processes on total tropospheric O3 column variability using a chemistry-climate model simulation of tropospheric 03, and reflects on the implications for total tropospheric 03 column measurements. On the basis of tropospheric 03 column (satellite) measurements and without other sources of information (e.g., model simulations, observations of other trace species) it is not possible to determine the separate contributions by the aforementioned processes to the extratropical total tropospheric 03 column variability. Furthermore, typical extratropical synoptic-scale (daily) total tropospheric 03 column variability is of the order of 10 DU (1-σ value), implying the errors in (satellite) measurements should be of the order of magnitude at maximum (~10 DU) for daily measurements. For tropical total tropospheric O3 column (satellite) measurements the requirements are less stringent because the most important variability occurs on seasonal timescales. Errors in tropical total tropospheric 03 column (TTOC) measurements should be of the order of 5 DU for monthly means. Copyright 2005 by the American Geophysical Union.

A sulfur cycle model is coupled to a global chemistry-climate model. The simulated surface sulfate concentrations are generally within a factor of 2 of observed concentrations, and display a realistic seasonality for most background locations. However, the model tends to underestimate sulfate and overestimate surface SO2 at relatively polluted locations. A possible explanation for this is that additional oxidation reactions not considered in the model, may be important. Calculated tropospheric sulfate column abundances exceed those of previous studies, which is predominantly associated with a less efficient nucleation scavenging in wet convective updrafts. Through the simultaneous calculation of the sulfur cycle and tropospheric photochemistry, simulated H2O2 and SO2 concentrations are strongly linked, especially in polluted areas. The coupled model simulates a stronger oxidant limitation and, consequently, a smaller contribution to sulfate formation by H2O2 oxidation of SO2 when compared to sulfur cycle models that use monthly averaged oxidant distributions as input. In the polluted NH, the differences in calculated sulfate columns are largest in winter and relatively small in summer. Therefore, the coupling between the sulfur cycle and the oxidant chemistry is expected to have a minor impact on the calculation of the indirect and direct radiative forcing by sulfate. An empirical relation between sulfate concentration and cloud drop number concentration, derived from cloud measurements at Grean Dun Fell (UK), is applied to the simulated cloud and sulfate fields to derive distributions of effective could drop radii. Additionally, a relation between wind speed and cloud drop number concentration is applied over marine regions to account for the effect of seasalt aerosol on cloud formation when sulfate concentrations are relatively low. Calculated droplet radii are systematically underestimated by about 10-20% in the NH compared to satellite derived values, but they a