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A common deficiency of many cloud-physics parameterizations including the NASA’s microphysics of clouds with aerosol-cloud interactions (hereafter called McRAS-AC) is that they simulate lesser (larger) than the observed ice cloud particle number (size). A single column model (SCM) of McRAS-AC physics of the GEOS4 Global Circulation Model (GCM) together with an adiabatic parcel model (APM) for ice-cloud nucleation (IN) of aerosols were used to systematically examine the influence of introducing ammonium sulfate (NH4 )2 SO4 aerosols in McRAS-AC and its influence on the optical properties of both liquid and ice clouds. First an (NH4 )2 SO4 parameterization was included in the APM to assess its effect on clouds vis-à-vis that of the other aerosols. Subsequently, several evaluation tests were conducted over the ARM Southern Great Plain (SGP) and thirteen other locations (sorted into pristine and polluted conditions) distributed over marine and continental sites with the SCM. The statistics of the simulated cloud climatology were evaluated against the available ground and satellite data. The results showed that inclusion of (NH4 )2 SO4 into McRASAC of the SCM made a remarkable improvement in the simulated effective radius of ice cloud particulates. However, the corresponding ice-cloud optical thickness increased even more than the observed. This can be caused by lack of horizontal cloud advection not performed in the SCM. Adjusting the other tunable parameters such as precipitation efficiency can mitigate this deficiency. Inclusion of ice cloud particle splintering invoked empirically further reduced simulation biases. Overall, these changes make a substantial improvement in simulated cloud optical properties and cloud distribution particularly over the Intertropical Convergence Zone (ITCZ) in the GCM.