Modeling study of cloud droplet nucleation and in‐cloud sulfate production during the Sanitation of the Atmosphere (SANA) 2 campaign

Based upon the measurements of vertical profiles of gaseous SO2, H2O2, O3, and meteorological parameters from aircraft and of the aerosol chemical composition and gaseous NH3, HNO3, and SO2 at the surface in southeastern Germany (Melpitz) during the Sanitation of the Atmosphere (SANA) 2 campaign, realistic modeling of cloud droplet nucleation and in-cloud sulfate production was performed with an explicit microphysical cloud model with size-resolved chemistry and cloud top entrainment. For the fair weather cumulus observed during the measurements, the calculated cloud droplet number concentrations could be as high as 2000 cm−3 (and precloud aerosol sulfate up to 9.1 μg m−3), indicating strong sulfur pollution at Melpitz during the campaign. The in-cloud sulfate production is within 1.5–5.0 μg m−3, depending on the initial gaseous NH3 concentration in the parcel. This result shows the necessity of gaseous NH3 vertical profile measurements. Entrainment can reduce the cloud droplet number concentration and cause the distribution of in-cloud produced sulfate to shift toward larger particle sizes. Under the cases we studied, we do not find a significant effect of cloud top gaseous H2O2 entrainment on the in-cloud sulfate production. For the adiabatic cases the departure of bulk water H2O2 from the Henry's law equilibrium is very small. When entrainment included, however, bulk water H2O2 concentrations could be clearly less than the equilibrium values, and the deficiencies are higher (>20%) for droplets larger than 10 μm radius. Our results suggest that entrainment could be one of the important factors to account for the measured H2O2 deficiency in cloud water.