Industry, urban development, and other anthropogenic influences have substantially altered the composition and size-distribution of atmospheric aerosol particles over the last century. This, in turn, has altered cloud albedo, lifetime, and patterns which together are thought to exert a negative radiative forcing on the climate; these are the indirect effects of atmospheric aerosols. The specifics of the process by which aerosol particles seed cloud particles are complex and highly uncertain. The goal of this thesis is to refine understanding of the role of various aerosol types in determining cloud properties. We approach this goal by constructing a new highly detailed aerosol-cloud process model that is designed to simulate condensation upon complex aerosol populations. We use this model to investigate the microphysics of aerosol-cloud interactions, specifically considering the role of cloud dynamics and of the ubiquitous mixed soot / sulfate aerosols.

We describe the Mixed Eulerian-Lagrangian Aerosol Model (MELAM). This new computer model of aerosol microphysics is specifically tailored to simulate condensation and activation as accurately as possible. It specifically calculates aerosol thermodynamics, condensation, coagulation, gas and aqueous phase chemistry, and dissolution. The model is able to consider inorganic aerosols and aerosols with both inorganics and insoluble cores; the specific chemical system to be considered is specified by the user in text input files. Aerosol particles may be represented using "sectional distributions" or using a "representative sample" distribution which tracks individual particles. We also develop a constant updraft speed, adiabatic parcel model and a variable updraft speed, episodically entraining parcel model to provide boundary conditions to MELAM and allow simulations of aerosol activation in cloud updrafts.

Using MELAM and the parcel models, we demonstrate that aerosol activation depends on the composition and size distribution of the sub-cloud aerosol population, on the updraft speed through a parcel's lifting condensation level, on the vertical profile of the updraft speed, and on entrainment. We use a convective parameterization that was developed for use in global or regional models to drive the episodically entraining, variable updraft speed parcel model. Ultimately, reducing the uncertainty of the global impact of the indirect effects of aerosols will depend on successfully linking cloud parameterizations to models of aerosol activation; our work represents a step in that direction.

We also consider the activation of mixed soot / sulfate particles in cloud updrafts. We constrain for the first time a model of condensation onto these mixed particles that incorporates the contact angle of the soot / solution interface and the size of the soot core. We find that as soot ages and its contact angle with water decreases, mixed soot / sulfate aerosols activate more readily than the equivalent sulfate aerosols that do not have soot inclusions. We use data from the Aerosol Characterization Experiments (ACE) 1 and 2, and from the Indian Ocean Experiment (INDOEX) to define representative aerosol distributions for clean, polluted, and very polluted marine environments. Using these distributions, we argue that the trace levels of soot observed in clean marine environments do not substantially impact aerosol activation, while the presence of soot significantly increases the number of aerosol that activate in polluted areas.