Further evidence for particle nucleation in clear air adjacent to marine cumulus clouds

Abstract

Observational evidence is presented for the nucleation of condensation nuclei (CN) in the clear air adjacent to an isolated, marine, cumulus cloud. Two separate regions of particle nucleation are identified: one located above the cloud top, and the second located downwind of the cloud near the level of the anvil outflow. The regions of high CN concentrations were located in extremely clean marine air, with unactivated aerosol surface area (excluding the nucleation mode) <2 μm2 cm−3, air temperature −31°C, and higher relative humidities than the undisturbed environment. Vertical profile measurements downwind of the cloud showed that CN concentrations at the level of the anvil outflow (4.9 km) were 8 times greater than at any other level between the surface and 5.3 km. A conceptual model is formulated in which aerosol particles, sulfur dioxide (SO2), sulfuric acid vapor (H2SO4), dimethyl sulfide (DMS), and ozone (O3) from the boundary layer are entrained into the cumulus cloud. Total aerosol number concentrations and unactivated aerosol surface area decrease with height in the cloud due to Brownian diffusion and diffusiophoresis of cloud interstitial aerosol to hydrometeors, coalescence scavenging by cloud droplets, collisional scavenging by ice particles, and subsequent removal by precipitation. The air that is detrained from the cloud raises the relative humidity and vents the clean air, SO2, H2SO4, DMS, and O3 to the near‐cloud environment. Hydroxyl radicals then oxidize the SO2 and DMS to H2SO4. Under the conditions of high relative humidity, low total aerosol surface area, low temperatures, and high SO2 concentrations near cloud top, significant concentrations of new particles can be produced by homogeneous‐bimolecular nucleation of sulfuric acid solution droplets from H2SO4 and H2O vapor molecules. The concentration of CN as a function of time is calculated for the case described in this paper using a bimodal integral nucleation model. The model results show that significant numbers of CN could have been produced within a few hours by the homogeneous‐bimolecular nucleation of sulfuric acid solution droplets under the observed conditions provided the concentration of SO2 near cloud top was enhanced by vertical transport.