Integrated approach towards understanding interactions of mineral dust aerosol with warm clouds

Mineral dust is ubiquitous in the atmosphere and represents a dominant type of particulate matter by mass. Dust particles can serve as cloud condensation nuclei (CCN), giant CCN (GCCN), or ice nuclei (IN), thereby, affecting cloud microphysics, albedo, and lifetime. Despite its well-recognized importance, assessments of dust impacts on clouds and climate remain highly uncertain. This thesis addresses the role of dust as CCN and GCCN with the goal of improving our understanding of dust-warm cloud interactions and their representation in climate models.;Most studies to date focus on the soluble fraction of aerosol particles when describing cloud droplet nucleation, and overlook the interactions of the hydrophilic insoluble fraction with water vapor. A new approach to include such interactions (expressed by the process of water vapor adsorption) is explored, by combining multilayer Frenkel-Halsey-Hill (FHH) physical adsorption isotherm and curvature (Kelvin) effects.;The importance of adsorption activation theory (FHH-AT) is corroborated by measurements of CCN activity of mineral aerosols generated from clays, calcite, quartz, and desert soil samples from Northern Africa, East Asia/China, and Northern America. A new aerosol generation setup for CCN measurements was developed based on a dry generation technique capable of reproducing natural dust aerosol emission. Based on the dependence of critical supersaturation with particle dry diameter, it is found that the FHH-AT is a better framework for describing fresh (and unprocessed) dust CCN activity than the classical Kohler theory (KT). Ion Chromatography (IC) measurements performed on fresh regional dust samples indicate negligible soluble fraction, and support that water vapor adsorption is the prime source of CCN activity in the dust.;CCN measurements with the commonly used wet generated mineral aerosol (from atomization of a dust aqueous suspension) are also carried out. Results indicate that the method is subject to biases as it generates a bimodal size distribution with a broad range of hygroscopicity. It is found that smaller particles generated in the more hygroscopic peak follow CCN activation by KT, while the larger peak is less hydrophilic with activation similar to dry generated dust that follow FHH-AT.;Droplet activation kinetics measurements demonstrate that dry generated mineral aerosol display retarded activation kinetics with an equivalent water vapor uptake coefficient that is 30 - 80% lower relative to ammonium sulfate aerosol. Wet generated mineral aerosols, however, display similar activation kinetics to ammonium sulfate. These results suggest that at least a monolayer of water vapor (the rate-limiting step for adsorption) persists during the timescale of aerosol generation in the experiment, and questions the atmospheric relevance of studies on mineral aerosol generated from wet atomization method.;A new parameterization of cloud droplet formation from insoluble dust CCN for regional and global climate models is also developed. The parameterization framework considers cloud droplet formation from dust CCN activating via FHH-AT, and soluble aerosol with activation described through KT. The parameterization is validated against a numerical parcel model, agreeing with predictions to within 10% (R2 ∼ 0.98).;The potential role of dust GCCN activating by FHH-AT within warm stratocumulus and convective clouds is also evaluated. It is found that under pristine aerosol conditions, dust GCCN can act as collector drops with implications to dust-cloud-precipitation linkages. Biases introduced from describing dust GCCN activation by KT are also addressed.;The results demonstrate that dust particles do not require deliquescent material to act as CCN in the atmosphere. Furthermore, the impact of dust particles as giant CCN on warm cloud and precipitation must be considered. Finally, the new parameterization of cloud droplet formation can be implemented in regional and global models providing an improved treatment of mineral aerosol on clouds and precipitation. The new framework is uniquely placed to address dust aerosol indirect effects on climate.