Diagnosis of an underestimation of summertime sulfate using the Community Multiscale Air Quality model

We evaluate the simulations of SO2 and sulfate using the Community Multiscale Air Quality model (CMAQ) version 4.6 with the observations over the United States in 2002. MM5 was used for meteorological simulations. While the general seasonal cycles of SO2 and sulfate are simulated well by the model, we find significant systematic biases in the summer. The model low bias in sulfate is considerably more severe than the model bias in SO2. Both ACM and RADM schemes are used in the model to test the sensitivities of simulated sulfate to cloud processing. We carry out detailed modeling analysis and diagnostics for July 2002. Compared to satellite observations of cloud liquid water path, CMAQ cloud modules greatly overestimates convective (sub-grid) precipitating clouds, leading to large overestimation of sulfate wet scavenging. Limiting convective precipitating cloud fraction in the cloud modules to <10% and hence significantly reducing wet scavenging lead to much improved agreement between simulated and observed sulfate. The average lifetime of sulfate in the model increases from 1–2 days to 3–4 days for July. We show that a potential model problem of excessive wet scavenging of sulfate does not necessarily lead to apparent problems in model simulations of sulfate wet deposition rate compared to surface observations. In general, there is still a lack of direct observational constraints from air quality monitoring measurements on model simulated cloud processing of SO2 and sulfate.

► We evaluate the simulations of SO2 and sulfate using CMAQ4.6 over the USA in 2002. ► We find systematic low biases for sulfate in the summer. ► We find module greatly overestimates (sub-grid) convective clouds. ► We find to limit convective cloud fraction and hence to improve model performance.