1Max Planck Institute for Chemistry, Biogeochemistry Department, Mainz, Germany
2Institute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, Germany
3Leibniz Institute for Tropospheric Research, Leipzig, Germany
*German Weather Service, DWD Offenbach, Germany
Abstract. We have investigated the formation of cloud droplets under (pyro-)convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.5–20 m s−1) and aerosol particle number concentrations (NCN=103–105 cm−3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation:
1. An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10−3 m s−1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCD/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w.
2. An updraft-limited regime that is characterized by low w/NCN ratios (<≈10−4 m s−1 cm3), low maximum values of water vapour supersaturation (Smax<≈0.2%), and low activated fractions of aerosol particles (NCD/NCN<≈20%). In this regime NCD is directly proportional to w and practically independent of NCN.
3. An aerosol- and updraft-sensitive regime, which is characterized by parameter values in between the two other regimes and covers most of the conditions relevant for pyro-convection. In this regime NCD depends non-linearly on both NCN and w.
In sensitivity studies we have tested the influence of aerosol particle hygroscopicity on NCD. Within the range of effective hygroscopicity parameters that is characteristic for continental atmospheric aerosols (κ≈0.05–0.6), we found that NCD depends rather weakly on the actual value of κ. Only for aerosols with very low hygroscopicity (κ<0.05) and in the updraft-limited regime also for aerosols with higher than average hygroscopicity (κ>0.3) did the relative differential quotients (ΔNCD/NCD)/(Δκ/κ) exceed values of ~0.2, indicating that a 50% difference in κ would change NCD by more than 10%. Realistic changes in the aerosol particle size distribution had practically no effect on the aerosol-limited regime and limited influence on the aerosol- and updraft sensitive regime (ΔNCD/NCD<30%) but can have strong effects at low supersaturation in the updraft-limited regime (ΔNCD/NCD>30% at Smax<0.1%). Overall, the results of this and related studies suggest that the variability of initial cloud droplet number concentration in (pyro-)convective clouds is mostly dominated by the variability of updraft velocity and aerosol particle number concentration in the accumulation mode. Coarse mode particles and the variability of particle composition and hygroscopicity appear to be play major roles only at low supersaturation in the updraft-limited regime of CCN activation (Smax<0.2%).