In the present study a parallel three dimensional Volume of Fluid (VOF) method is developed to simulate Marangoni force in immiscible fluids with variable surface tension. Conservation equations are solved based on cell-averaged one-field volume tracking scheme. Evaluating the convective term in the energy equation along the boundary between the fluids highly depends on the position and orientation of the interface; hence, using average cell values simply ignores the interface shape and leads to computational uncertainty. As a remedy to this issue, the original idea behind the volume tracking method is used not only to advect mass and momentum but also energy across cells. To verify the proposed algorithm, results are compared against theoretically predicted thermocapillary migration velocity of a droplet at the limit of zero Marangoni number. However, at relatively high Marangoni numbers, thermal boundary layers are very thin and challenging to resolve. To demonstrate the capabilities of the heat transfer module, simulations of a Fluorinert droplet moving in silicon oil under applied temperature gradient in microgravity are compared against the available experimental results and the migration velocity of the droplet are reported.

Adsorption-mediated self-assembly of nanoparticles at fluid interfaces, driven by reduction in interfacial energy, leads to stabilization of emulsions and foams and can be used for the bottom-up fabrication of functional nanostructured materials. Improved understanding of the parameters that control the self-assembly, the structure of nanoparticles at the interface, the barrier properties of the assembly and the rate of particle attachment and exchange is needed if such nanoparticle assemblies are to be employed for the design and fabrication of novel materials and devices. Here, I report on the use of dynamic surface tension (DST) measurements to probe the kinetics of irreversible adsorption and self-assembly of hydrophobic ethyl-cellulose (EC) nanoparticles at the air-water interface. Using thermodynamic arguments, I make a direct connection between the DST and the time-dependent surface coverage. I show that adsorption models appropriate for surfactants (e.g., Ward and Tordai model) break down for irreversible adsorption of nanoparticles, when the adsorption energy far exceeds the mean energy of thermal fluctuations (kBT) and surface blocking effects give rise to a steric barrier to adsorption. I show instead that irreversible adsorption kinetics are unequivocally characterized in terms of the adsorption rate constant and the maximum (jamming) coverage, both of which are determined on the basis of DST data using the generalized random sequential adsorption theory (RSA) for the first time. Novel accurate estimates of the adsorption energy of 42 nm and 89 nm EC nanoparticles are also provided. Coverage of the interface to the jamming limit of 91%, corresponding to a triangular lattice in 2D, is experimentally demonstrated. Colloidal solutions of EC nanoparticles are stabilized at neutral pH by electrostatic repulsive forces. Strong adsorption of these particles at an interface of like charge suggests the parallel action of attractive hydrophobic forces.

In this thesis, the results from molecular dynamics (MD) simulations of nanoaerosol clusters are discussed. The connecting link of these studies is the Köhler theory, which is the theory of condensational growth and activation of cloud droplets to form clouds. By investigating parameters such as the surface tension, state of mixture and morphology of nanoaerosol particles, conclusions can be drawn to improve the Köhler theory to include the effects of organic compounds previously unaccounted for. For the terrestrial environment, the simulations show that the natural surfactant cis-pinonic acid, an oxidation product evaporated from boreal trees, spontaneously accumulates at the surface of nanoaerosol clusters and thereby reduces the surface tension. The surface tension depression is related to the concentration of the surfactant and the size of the clusters. Surface tension is an important parameter of the Köhler theory. A decrease of the surface tension can lower the critical water vapour supersaturation needed for cloud droplet activation, giving rise to more, but smaller cloud droplets (Twomey effect) which in turn could change the optical properties of the cloud. It was also shown that the three organic surfactants, being model compounds for so called Humic-like substances (HULIS) have the ability to form aggregates inside the nanoaerosol clusters. These HULIS aggregates can also promote the solubilization of hydrophobic organic carbon in the form of fluoranthene, enabling soot taking part in cloud drop formation. Dissolved intermediately surface-active free amino acids were shown to be of some relevance for cloud formation over remote marine areas. The MD simulations showed differences between the interacting forces for spherical and planar interfaces of amino acids solutions. This thesis has emphasized the surface-active properties of organic compounds, including model HULIS and amino acids and their effect on surface tension and molecular orientation including aggregate formation in nanoaerosol clusters and their activation to form droplets. This thesis shows that the Köhler equation does not fully satisfactory describe the condensational growth of nano-sized droplets containing organic surfactants. Different approaches are suggested as revisions of the Köhler theory. / <p>At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Submitted. Paper 5: Manuscript.</p>

Thesis (Ph. D.)--Ohio State University, 2007. / Title from first page of PDF file. Includes bibliographical references (p. 123-126).

Thesis (Ph.D.) -- McMaster University, 1999. / Includes bibliographical references. Also available via World Wide Web.

Thesis (Ph.D.)--University of Tulsa, 1993. / Includes bibliographies.

Thesis (M.App.Sc.) - Carleton University, 2001. / Includes bibliographical references (p. 80-83). Also available in electronic format on the Internet.

Thesis (M. App. Sc.)--Carleton University, 2004. / Includes bibliographical references (p. 97-98). Also available in electronic format on the Internet.

Thesis (Ph. D.)--University of Missouri-Columbia, 1997. / Typescript. Vita. Includes bibliographical references (leaves 158-166). Also available on the Internet.

Thesis (Ph. D.)--University of Missouri-Columbia, 1997. / Typescript. Vita. Includes bibliographical references (leaves 158-166). Also available on the Internet.