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Myerson, Allan S.

Publications and source records attributed to Myerson, Allan S..

Diffusion, Viscosity and Crystal Growth in Microgravity

The diffusivity of TriGlycine Sulfate (TGS), Potassium Dihydrogen Phosphate (KDP), Ammonium Dihydrogen Phosphate (ADF) and other compounds of interest to microgravity crystal growth, in supersaturated solutions as a function of solution concentration, 'age' and 'history was studied experimentally. The factors that affect the growth of crystals from water solutions in microgravity have been examined. Three non-linear optical materials have been studied, potassium dihydrogen phosphate (KDP), ammonium dihydrogen phosphate (ADP) and triglycine sulfate (TGC). The diffusion coefficient and viscosity of supersaturated water solutions were measured. Also theoretical model of diffusivity and viscosity in a metastable state, model of crystal growth from solution including non-linear time dependent diffusivity and viscosity effect and computer simulation of the crystal growth process which allows simulation of the microgravity crystal growth were developed.

Myerson, Allan S.↗

Metastable Solution Thermodynamic Properties and Crystal Growth Kinetics

The crystal growth rates of NH4H2PO4, KH2PO4, (NH4)2SO4, KAl(SO4)2 central dot 12H2O, NaCl, and glycine and the nucleation rates of KBr, KCl, NaBr central dot 2H2O, (NH4)2Cl, and (NH4)2SO4 were expressed in terms of the fundamental driving force of crystallization calculated from the activity of supersaturated solutions. The kinetic parameters were compared with those from the commonly used kinetic expression based on the concentration difference. From the viewpoint of thermodynamics, rate expressions based on the chemical potential difference provide accurate kinetic representation over a broad range of supersaturation. The rates estimated using the expression based on the concentration difference coincide with the true rates of crystallization only in the concentration range of low supersaturation and deviate from the true kinetics as the supersaturation increases.

Kim, Soojin↗

Thermodynamic Studies of Levitated Microdroplets of Highly Supersaturated Electrolyte Solutions

Highly supersaturated electrolyte solutions are studied by employing an electrodynamic levitator trap (ELT) technique. The ELT technique involves containerless suspension of a microdroplet thus eliminating dust, dirt, and container walls which normally cause heterogeneous nucleation. This allows very high supersaturations to be achieved. A theoretical study of the experimental results obtained for the water activity in microdroplets of various electrolyte solutions is based on the development of the Cahn-Hilliard formalism for electrolyte solutions. A correspondence of 96-99% between the theory and experiment for the all solutions studied was achieved and allowed the determination of an analytical expression for the spinodal concentration n(sub spin) and its calculation for various electrolyte solutions at 298 K.

Myerson, Allan S.↗

Gravity Induced Formation of Concentration Gradients in Supersaturated Binary Solutions

Experimental and theoretical studies of the formation of solute concentration gradient in supersaturated binary solutions in a gravitational field were carried out. The formation of solute concentration gradient was associated with the gravity induced redistribution of subcritical solute clusters. The birth-death process of the new solute-rich phase domains (subcritical solute clusters) was described in terms of the time-dependent Ginzburg Landau model developed for metastable state relaxation in binary (solute + solvent) non-critical solutions in the presence of a gravitational field. A new mathematical Ansatz was developed for solution of the model equations. This Ansatz has allowed to approach for the first time the following important problems: (1) Microstructure of solute distribution inside of the subcritical solute clusters. The analytical results obtained demonstrate that solute inside of the subcritical solute clusters is heterogeneously distributed with a spatially periodic structure. (2) Macrostructure of the solute subcritical clusters distribution in a gravitational field. The subcritical solute clusters are found to be distributed heterogeneously in a gravitational field. This heterogeneity, which is due to the heterogeneous birth-death process of the subcritical solute clusters in a gravitational field, initiates a noticeable solute concentration gradient in vertical columns of supersaturated binary solutions. An analysis and comparison of theoretical results and experimental data related to the solute concentration gradient formation in a gravitational field are presented. It is also demonstrated that the critical radius of solute clusters (radius of nucleation) and induction time are gravity-dependent.

Izmailov, Alexander F.↗

Relationship Between Solution Shear Viscosity and Density at the Saturation Point

Properties of supersaturated solutions such as the density, viscosity, and solute diffusivity are dependent on the solute concentration. The diffusion-boundary-layer equations are derived and solved for the natural convection case with the viscosity and density dependent on the solute concentration. The solution obtained demonstrates that, at the vicinity of the saturation concentration c(sub s), there is a non-trivial dependence of the solution viscosity eta on its density rho: eta(c(sub s)) = eta(rho(sub s)) varies as rho(sub s)(exp 1/2), where rho(sub s) = rho(c(sub s)). This result has been verified in experiments with aqueous solutions of inorganic and organic salts.

Izmailov, Alexander F.↗

Supersaturated Electrolyte Solutions: Theory and Experiment

Highly supersaturated electrolyte solutions can be prepared and studied employing an electrodynamic levitator trap (ELT) technique. The ELT technique involves containerless suspension of a microdroplet thus eliminating dust, dirt, and container walls which normally cause heterogeneous nucleation. This allows very high supersaturations to be achieved. A theoretical study of the experimental results obtained for the water activity in microdroplets of various electrolyte solutions is based on the development of the Cahn-Hilliard formalism for electrolyte solutions. In the approach suggested the metastable state for electrolyte solutions is described in terms of the conserved order parameter omega(r,t) associated with fluctuations of the mean solute concentration n(sub 0). Parameters of the corresponding Ginzburg-Landau free energy functional which defines the dynamics of metastable state relaxation are determined and expressed through the experimentally measured quantities. A correspondence of 96-99 % between theory and experiment for all solutions studied was achieved and allowed the determination of an analytical expression for the spinodal concentration n(sub spin), and its calculation for various electrolyte solutions at 298 K. The assumption that subcritical solute clusters consist of the electrically neutral Bjerrum pairs has allowed both analytical and numerical investigation of the number-size N(sub c) of nucleation monomers (aggregates of the Bjerrum pairs) which are elementary units of the solute critical clusters. This has also allowed estimations for the surface tension Alpha, and equilibrium bulk energy Beta per solute molecule in the nucleation monomers. The dependence of these properties on the temperature T and on the solute concentration n(sub 0) through the entire metastable zone (from saturation concentration n(sub sat) to spinodal n(sub spin) is examined. It has been demonstrated that there are the following asymptotics: N(sub c), = I at spinodal concentration and N(sub c) = infinity at saturation.

Izmailov, Alexander F.↗

Concentration Dependence of Solution Shear Viscosity and Solute Mass Diffusivity in Crystal Growth from Solutions

The physical properties of a supersaturated binary solution such as its density rho, shear viscosity eta, and solute mass diffusivity D are dependent on the solute concentration c: rho = rho(c), eta = eta(c), and D = D(c). The diffusion boundary layer equations related to crystal growth from solution are derived for the case of natural convection with a solution density, a shear viscosity, and a solute diffusivity that are all depen- dent on solute concentration. The solution of these equations has demonstrated the following. (1) At the vicinity of the saturation concentration c(sub s) the solution shear viscosity eta depends on rho as eta(sub s) = eta(rho(sub s))varies as square root of rho(c(sub s)). This theoretically derived result has been verified in experiments with several aqueous solutions of inorganic and organic salts. (2) The maximum solute mass transfer towards the growing crystal surface can be achieved for values of c where the ratio of d ln(D(c)/dc) to d ln(eta(c)/dc) is a maximum.

Izmailov, Alexander F.↗

Theory of Metastable State Relaxation in a Gravitational Field for Non-Critical Binary Systems with Non-Conserved Order Parameter

A new mathematical ansatz is developed for solution of the time-dependent Ginzburg-Landau nonlinear partial differential equation describing metastable state relaxation in binary (solute+solvent) non-critical solutions with non-conserved scalar order parameter in presence of a gravitational field. It has been demonstrated analytically that in such systems metastability initiates heterogeneous solute redistribution which results in the formation of a non-equilibrium singly-periodic spatial solute structure in the new solute-rich phase. The critical radius of nucleation and the induction time in these systems are gravity-dependent. It has also been proved that metastable state relaxation in vertical columns of supersaturated non-critical binary solutions leads to formation of the solute concentration gradient. Analytical expression for this concentration gradient is found and analysed. It is concluded that gravity can initiate phase separation (nucleation or spinodal decomposition).

Izmailov, Alexander F.↗

Statistics of Experiments on Cluster Formation and Transport in a Gravitational Field

Metastable state relaxation in a gravitational field is investigated in the case of non-critical binary solutions. A relaxation description is presented in terms of the time-dependent Ginzburg-Landau formalism for a non-conserved order parameter. A new ansatz for solution of the corresponding partial nonlinear stochastic differential equation is discussed. It is proved that, for the supersaturated solution under consideration, the metastable state relaxation in a gravitational field leads to formation of solute concentration gradients due to the sedimentation of subcritical solute clusters. The pure discussion of the possible methods to compare theoretical results and experimental data related to solute sedimentation in a gravitational field is presented. It is shown that in order to describe these experiments it is necessary to deal both with the value of the solute concentration gradient and with its formation rate. The stochastic nature of the sedimentation process is shown.

Izmailov, Alexander F.↗

Theory of Metastable State Relaxation for Non-Critical Binary Systems with Non-Conserved Order Parameter

A new mathematical ansatz for a solution of the time-dependent Ginzburg-Landau non-linear partial differential equation is developed for non-critical systems such as non-critical binary solutions (solute + solvent) described by the non-conserved scalar order parameter. It is demonstrated that in such systems metastability initiates heterogeneous solute redistribution which results in formation of the non-equilibrium singly-periodic spatial solute structure. It is found how the time-dependent period of this structure evolves in time. In addition, the critical radius r(sub c) for solute embryo of the new solute rich phase together with the metastable state lifetime t(sub c) are determined analytically and analyzed.

Izmailov, Alexander↗

Metastable State Relaxation in a Gravitational Field

A metastable state relaxation equation for a physical system placed into a gravitational field is constructed for non-critical supersaturated solutions which arc in the immediate neighborhood of the coexistence line. Solutions of this equation are obtained in two different regimes: stationary and dynamic. The sedimentation time which can be defined as the time of the subcritical solute cluster redistribution corresponding to the final steady state in the gravitational field is found. The formation of the concentration gradient is proved analytically and its expression through the model parameters is obtained. The following analysis gives the expression for the sedimentation time which does not depend on the column height. The law of the concentration change with respect to the column height is also found and analyzed.

Izmailov, Alexander F.↗