Effect of clouds on photolysis and oxidants in the troposphere

[1] Cloud layers in the troposphere influence photolysis rates (J values) and hence concentrations of chemical species. In order to study the impact of clouds on photolysis rates and oxidants, we have developed a simplified version of the National Center for Atmospheric Research ( NCAR) Tropospheric Ultraviolet-Visible (TUV) model and have coupled the simplified TUV ( otherwise known as the fast TUV (FTUV)) into the NCAR/ Atmospheric Chemistry Division global transport chemical model ( Model for Ozone and Related Chemical Tracers (MOZART-2)). The FTUV model has the same physical processes as the TUV model, except that the wavelength bins between 121 and 750 nm are reduced from 140 to 17. As a result, FTUV is about 8 times faster than the original TUV. Differences in the calculated photolysis rates between TUV and FTUV are generally less than 5% in the troposphere. Subgrid vertical distributions of clouds are also considered in the calculation of photolysis rates in MOZART-2. The method used in this study is a mixed maximum and random overlap scheme. The subgrid method increases the computation time for photolysis rates by a factor of 3 compared to a simple method in which clouds are uniformly distributed over the MOZART-2 grids. Our calculation shows that the uniform cloud distribution method tends to significantly overestimate back scattering on the top of clouds and overestimates the impact on photochemistry in the troposphere. The results suggest that clouds have important impacts on tropospheric chemistry. Global mean OH concentration increases by about 20% due to the impact of clouds. As a result, the calculated CH4 lifetime changes to 11 years for clear sky and 9 years for cloudy sky. The latter value is closer to the methane lifetime estimated from previous studies. Calculated CO surface concentrations are compared with observed values, showing an improvement when the impact of clouds on the photolysis rates is taken into account. Clouds also have important impacts on tropospheric ozone budget. Our calculation suggest that because of clouds, the globally averaged photolysis rates of J[O-3], J[CH2O], and J[NO2] are enhanced in the troposphere by about 12, 13, and 13%, respectively, leading to an 8% increase in the tropospheric O-3 concentrations. Our study suggests that clouds strongly influence photolysis rates and hence play an important role in controlling the concentrations of the tropospheric oxidants. Such effects should be carefully considered and included in regional and global chemical transport models.