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Saville, D. A.

Publications and source records attributed to Saville, D. A..

At least 19 records

Electrohydrodynamic Flows in Electrochemical Systems

Recent studies have established a new class of assembly processes with colloidal suspensions. Particles are driven together to form large crystalline structures in both dc and ac fields. The current work centers on this new class of flows in ac fields. In the research carried out under the current award, it was established that: (i) Small colloidal particles crystallize near an electrode due to electrohydrodynamic flows induced by an sinusoidally varying applied potential. (ii) These flows originate due to disturbances in the electrode polarization layer arising from the presence of the particles. Inasmuch as the charge and the field strength both scale on the applied field, the flows are proportional to the square of the applied voltage. (iii) Suspensions of two different sorts of particles can be crystallized and will form well-ordered binary crystals. (iv) At high frequencies the EHD flows die out. Thus, with a homogeneous system the particles become widely spaced due to dipolar repulsion. With a binary suspension, however, the particles may become attractive due to dipolar attraction arising from differences in electrokinetic dipoles. Consequently binary crystals form at both high and low frequencies.

Saville, D. A.

Assembly of Colloidal Aggregates by Electrohydrodynamic Flow: Kinetic Experiments and Scaling Analysis

Electric fields generate transverse flows near electrodes that sweep colloidal particles into densely packed assemblies. We interpret this behavior in terms of electrohydrodynamic motion stemming from distortions of the field by the particles that alter the body force distribution in the electrode charge polarization layer. A scaling analysis shows how the action of the applied electric field generates fluid motion that carries particles toward one another. The resulting fluid velocity is proportional to the square of the applied field and decreases inversely with frequency. Experimental measurements of the particle aggregation rate accord with the electrohydrodynamic theory over a wide range of voltages and frequencies.

Ristenpart, W. D.

Electrohydrodynamic Stability of a Liquid Bridge: The "ALEX" Experiment

To provide insight into the roles of electrical forces, experiments on the stability of a liquid bridge were carried out during the 1996 Life And Microgravity Science Mission on the space shuttle Columbia. In terrestrial laboratories a Plateau configuration (where the bridge is surrounded by a matched density liquid) is necessary to avoid deformation due to buoyancy. This complicates the electrical boundary conditions, since charge is transported across the liquid-liquid interface. In the microgravity environment, a cylindrical bridge can be deployed in a gas which considerably simplifies the boundary condition. Nevertheless, to provide a tie-in to terrestrial experiments, two-phase experiments were carried out. The agreement with previous work was excellent. Then several experiments were conducted with a bridge deployed in a dielectric gas, SF6. In experiments with steady fields, it was found that the bridge was less stable than predicted by a linearized stability analysis using the Taylor-Melcher leaky dielectric model.

Burcham, C. L.

The roles of fluid motion and other transport phenomena in the morphology of materials

Two crystallization problems were studied: the growth of protein crystals, in particular the influence of colloidal forces and convection, and the influence of interface resistance on the growth of dendritic crystals. The protein study involved both experimental and theoretical work; the work of dendrites was entirely theoretical. In the study of protein crystallization, experiments were carried out where crystals were grown in the presence and absence of natural convection. No evidence was found that convection retards crystal growth. The theoretical study focused on the influence of colloidal forces (electrostatic and London-van der Waals) on the interaction between a protein molecule and a flat crystal surface. It was shown that the interaction is extremely sensitive to colloidal forces and that electrostatic interactions play a strong role in deciding whether or not a molecule will find a favorable site for adsorption. In the study of dendritic growth, the role of an interfacial resistance on the selection processes was examined. Using a computational scheme, it was found that the selected velocity is strongly dependent on the magnitude of the interfacial resistance to heat transfer. This is a possible explanation for discrepancies between the theoretical and experimental results on succinonitrile.

Saville, D. A.

Experiments on the stability of a liquid bridge in an axial electric field

The behavior of a neutrally buoyant liquid bridge was studied in the presence of axial electric fields. Silicone oil and a castor-oil-eugenol mixture were used to form cylinders with slenderness ratios larger than pi with strong, axial, dc electric fields. Below a certain field strength, a smooth transition to an axisymmetric, vaselike shape occurred. Circulation patterns were observed in these bridges. At lower field strengths, the bridge shape was more deformed and, at a well-defined field, pinch-off occurred. With ac fields, the field strength required to stabilize the bridge was higher and the collapse of the cylinder was much sharper. Upon interchanging the fluids, a steady axial field was found to destabilize cylinders with slenderness ratios less than 3. This behavior is consistent with that anticipated if the fluids behave as leaky dielectrics but not if they act as perfect dielectrics.

Sankaran, Subramanian

Electrophoresis of small particles and fluid globules in weak electrolytes

An examination is conducted of the influence of partial ionization on the electrophoresis of small particles and fluid globules, with a view to the nature of conditions under which dissociation-association (D-A) alters electrokinetics. It is found that, since D-A processes are important in cases where double-layer polarization and relaxation would otherwise prevail, the predicted effect on electrophoretic mobility is greatest for the drops and bubbles whose surfaces are fluid and convection within the interface is significant. While the computation scheme used applies only to situations where forcing-field magnitude is small, the results obtained indicate that D-A processes involving ionogenic solutes may be significant in apolar liquids where electrokinetic phenomena are driven by strong forcing fields.

Baygents, J. C.

The fluid mechanics of continuous flow electrophoresis

The overall objective is to establish theoretically and confirm experimentally the ultimate capabilities of continuous flow electrophoresis chambers operating in an environment essentially free of particle sedimentation and buoyancy. The efforts are devoted to: (1) studying the effects of particle concentration on sample conductivity and dielectric constant. The dielectric constant and conductivity were identified as playing crucial roles in the behavior of the sample and on the resolving power and throughput of continuous flow devices; and (2) improving the extant mathematical models to predict flow fields and particle trajectories in continuous flow electrophoresis. A dielectric spectrometer was designed and built to measure the complex dielectric constant of a colloidal dispersion as a function of frequency between 500 Hz and 200 kHz. The real part of the signal can be related to the sample's conductivity and the imaginary part to its dielectric constant. Measurements of the dielectric constants of several different dispersions disclosed that the dielectric constants of dilute systems of the sort encountered in particle electrophoresis are much larger than would be expected based on the extant theory. Experiments were carried out to show that, in many cases, this behavior is due to the presence of a filamentary structure of small hairs on the particle surface. A technique for producing electrokinetically ideal synthetic latex particles by heat treating was developed. Given the ubiquitous nature of hairy surfaces with both cells and synthetic particles, it was deemed necessary to develop a theory to explain their behavior. A theory for electrophoretic mobility of hairy particles was developed. Finally, the extant computer programs for predicting the structure of electro-osmotically driven flows were extended to encompass flow channels with variable wall mobilities.

Saville, D. A.

Particle migration in suspensions by thermocapillary or electrophoretic motion

Two problems of similar mathematical structure are presented: the thermocapillary motion of bubbles and the electrophoresis of colloidal particles. For both problems, it is shown that in a cloud of n particles surrounded by an infinite expanse of fluid, the velocity of each sphere under creeping flow conditions is equal to the velocity of an isolated particle, unchanged by interactions between the particles. However, when the cloud fills a container, conservation of mass shows that this result cannot continue to hold, and the average translational velocity must be calculated subject to a constraint on the mass flux. It is concluded that the average thermocapillary or electrophoretic translational velocity of a particle in the cloud is related to the effective conductivity of the cloud over the whole range of particle volume fractions, provided that the particles are identical, non-conducting and, for the thermocapillary problem, inviscid.

Acrivos, A.

Two puzzling aspects of protein crystal growth

A study is presented of several mechanisms which may reduce crystal growth rates and or terminate crystal growth. It is found that salt gradients which change the local chemical potential of the protein are insufficient to account for the slow crystal growth rates which have been reported. Contaminants which adsorb protein from solution may reduce the effective protein concentration, but the impurity's concentration and its affinity for protein are unknown. Association of protein molecules in bulk solution can reduce the monomer concentration significantly, but extant theory and experiment are not sensitive enough to determine the actual concentration of aggregates in solution. For systems of interest, shear-induced effects were found to be too weak to interfere with normal binding of incoming protein molecules. Although we found that most crystal growth occurs in a regime where both interfacial kinetics and diffusion influence crystal growth, the role of mass transfer rates on the terminal size of crystals is unknown, primarily because no data exist which cover the size range of interest (0.1 mm to 1 mm in length).

Grant, M. L.

Growth of needle-shaped crystals in the presence of convection

The motion of the freezing front between a needle-shaped crystal and a supercooled liquid is analyzed for situations where there is forced convection aligned with the crystal axis. It is shown that in the absence of capillary effects the shape of the crystal-melt interface is a paraboloid of revolution, similar to that found in situations where diffusion is the sole heat-transfer mechanism. A relation between the supercooling, the product of tip velocity and tip radius, and the strength of the flow is derived which reduces to the well-known Ivantsov theory in the absence of convection.

Saville, D. A.

Electrokinetic properties of particles in concentrated suspensions

The electrokinetic behavior of concentrated suspensions is studied under conditions where the double layer is thin. Bulk electrical conductivity and single particle electrophoretic mobilities were studied as functions of the particle concentration in the suspension. It is found that the interactions between particles affect the conduction processes.

Zukoski, C. F.

Theory of electrophoretic separations. I - Formulation of a mathematical model

A generally applicable model of electrophoretic processes is presented. The model describes the chemical reactions, treating the chemical processes as reactions at equilibrium and accounting for convection, conservation, diffusion, and electromigration of individual species as well as the relation between charge and potential. Conservation relations are described and simplified, taking advantage of the speed of the chemical reactions as compared to the transport processes to adapt the model to the electrophoretic processes involving weak electrolytes. As an application example, isotachophoresis in a one-dimensional column is considered in detail.

Saville, D. A.

Theory of electrophoretic separations. II - Construction of a numerical simulation scheme and its applications

The implementation of a previously derived model describing electrophoretic transport processes is reformulated, and its usefulness is demonstrated by simulating moving boundary electrophoresis and isoelectric focusing with immobilized species. The resulting solution is stable, evolves smoothly when suitable small step sizes are used, and has a loosely defined convergence as the step sizes are made smaller. The major computational problem involves a need to use small spatial step sizes at high current levels.

Palusinski, O. A.

Transport processes research

Fundamental research in reduced gravity on transport processes occurring during crystallization and/or during solidification processes was studied. The details of the transport processes in various materials processing modes will be systematically studied. A Shuttle experiment will be planned to provide a better understanding of the role of fluid motion on the formation of morphological patterns and roles of these patterns in solid composition. The approach to the research will involve theoretical modeling of transport processes, non-incursive ground-based laboratory measurements of model systems, and the definition of requirements for space experimentation.

Saville, D. A.

Electrohydrodynamics

Models of electrohydrodynamic processes involving liquids with poorly ionized solutes at high (applied) field strengths were developed and tested. Extant theories which account for the details of physico-chemical processes associated with charged interfaces deal mainly with low field strengths and fully ionized solutes. The model used to describe processes at high field strengths--the leaky dielectric--omits consideration of electric double-layers, adsorption at interfaces, and chemical processes involved in the dissociation and recombination of solute species. Thus, even though the model depicts some features associated with bulk fluid motion, it fails to give a comprehensive picture. One example of the shortcomings of both the classical model of eletrokinetics at low field strengths and the leaky-dielectric model for high field strengths is found in the field strength dependence of the mobility of small particles in apolar liquids. The research will provide a more general model of electrohydrodynamic phenomena capable of application in diverse circumstances.

Saville, D. A.

Mathematical Models of Continuous Flow Electrophoresis

Development of high resolution continuous flow electrophoresis devices ultimately requires comprehensive understanding of the ways various phenomena and processes facilitate or hinder separation. A comprehensive model of the actual three dimensional flow, temperature and electric fields was developed to provide guidance in the design of electrophoresis chambers for specific tasks and means of interpreting test data on a given chamber. Part of the process of model development includes experimental and theoretical studies of hydrodynamic stability. This is necessary to understand the origin of mixing flows observed with wide gap gravitational effects. To insure that the model accurately reflects the flow field and particle motion requires extensive experimental work. Another part of the investigation is concerned with the behavior of concentrated sample suspensions with regard to sample stream stability particle-particle interactions which might affect separation in an electric field, especially at high field strengths. Mathematical models will be developed and tested to establish the roles of the various interactions.

Saville, D. A.

The formation of small scale granularities in latex particles

A series of latices were synthesized using emulsifier-free emulsion copolymerization of styrene and sodium styrene sulfonic acid. The final latex particles display an internal granular structure which can be ascribed to the primary particles present in the early stages of particle growth. In these systems, the primary particles appear to have maintained their integrity during the swelling and growth stage.

Zukoski, C. F.