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Materials Science Laboratory - Columnar-to-Equiaxed Transition in Solidification Processing and Microstructure Formation in Casting of Technical Alloys under Diffusive and Magnetically Controlled Convective Conditions

The Materials Science Laboratory - Columnar-to-Equiaxed Transition in Solidification Processing and Microstructure Formation in Casting of Technical Alloys under Diffusive and Magnetically Controlled Convective Conditions (MSL-CETSOL and MICAST) are two investigations which supports research into metallurgical solidification, semiconductor crystal growth (Bridgman and zone melting), and measurement of thermo-physical properties of materials. This is a cooperative investigation with the European Space Agency (ESA) and National Aeronautics and Space Administration (NASA) for accommodation and operation aboard the International Space Station (ISS). Research Summary: Materials Science Laboratory - Columnar-to-Equiaxed Transition in Solidification Processing (CETSOL) and Microstructure Formation in Casting of Technical Alloys under Diffusive and Magnetically Controlled Convective Conditions (MICAST) are two complementary investigations which will examine different growth patterns and evolution of microstructures during crystallization of metallic alloys in microgravity. The aim of these experiments is to deepen the quantitative understanding of the physical principles that govern solidification processes in cast alloys by directional solidification.

Gandin, Charles-Andre

Influence of gravity-free solidification on microsegregation

Single crystalline germanium has been grown for the first time in space aboard Skylab Mission No. 2. The crystal growth experiment, designed to characterize the influence of gravity-free solidification on microsegregation of a semiconductor material, contained three crystals. One was doped with Ga; the second with Sb; and the third with B. Portions of the germanium crystals were remelted and subsequently resolidified at 5 microns per second under controlled conditions by the gradient freeze technique. Detailed spreading resistance measurements made on the Ga doped Ge crystals indicate that microsegregation in space is reduced by two to five-fold in the bulk and eight-fold near the surface, while macrosegregation in space is reduced by six-fold in the bulk. The effective segregation coefficient for Ga in Ge was analyzed extensively and was found to be larger for space solidification. This has the implication that the solute boundary layer at the growth interface in space is correspondingly thinner. The solidification interface is significantly smoother and is found to be initially convex toward the melt in space. A convective mixing model has been advanced to explain the absence of gravity on convective mixing and solute segregation during solidification.

Yue, J. T.

MPS Solidification Model. Volume 2: Operating guide and software documentation for the unsteady model

The operation of solidification Model 2 is described and documentation of the software associated with the model is provided. Model 2 calculates the macrosegregation in a rectangular ingot of a binary alloy as a result of unsteady horizontal axisymmetric bidirectional solidification. The solidification program allows interactive modification of calculation parameters as well as selection of graphical and tabular output. In batch mode, parameter values are input in card image form and output consists of printed tables of solidification functions. The operational aspects of Model 2 that differ substantially from Model 1 are described. The global flow diagrams and data structures of Model 2 are included. The primary program documentation is the code itself.

Maples, A. L.

Influence of gravity driven convection on the directional solidification of Bi/MnBi eutectic composites

The role of gravity on Bridgman-Stockharger directional solidification of eutectic Bi/MnBi has been studied in reduced gravity aboard NASA sounding rocket SPAR flight experiments and contrasted with normal gravity investigations. The directional solidification of eutectic Bi/MnBi results in a low volume fraction, faceted/nonfaceted aligned rod eutectic whose MnBi rod size, interrod spacing, thermal and magnetic properties are sensitive functions of solidification processing conditions. The morphology of the low-gravity samples showed striking differences compared with identically processed, normal gravity samples grown in the same apparatus. The MnBi rod diameter and interrod spacing distributions were significantly smaller, approximately 50 percent, for the low gravity samples compared with identically processed one gravity samples. Accompanying the smaller MnBi rod diameters observed in the flight samples, was an increase in permanent magnet properties which reached greater than 97 percent of the theoretical maximum. Gravitationally induced thermal instabilities in one-gravity which result in irregular interface movement and associated difficulty of the faceted MnBi phase to branch are suggested to explain the morphological differences between one and low gravity solidification.

Pirich, R. G.

The Effect of Solidification Rate on Morphological Stability

At low solidification rates, the criterion for the onset of morphological instability parallels closely the criterion of constitutional supercooling. At somewhat larger rates of solidification, however, the results of the perturbation theory of morphological instability differ significantly from the predictions of constitutional supercooling. This arises because the critical wave length for instability decreases as solidification rate increases and thus the effects of capillarity (solid-liquid surface tension) play a strong stabilizing role. This gives rise to the concept of absolute stability, according to which the system will always be stable for a sufficiently large rate of solidification. This enhanced stabilization by capillarity is present only so long as local equilibrium is maintained at the solid-liquid interface. If the interfacial temperature drops below its equilibrium value by an amount dependent on growth rate, oscillatory morphological instabilities can occur. The differences among these various stability criteria are illustrated by means of some simple two-dimensional diagrams that should supplant the conventional plots of (temperature gradient)/(growth rate) vs. alloy concentration.

Sekerka, R. F.

Progress Toward Monolithic Peritectic Solidification

Reducing convection during plane-front, two-phase peritectic solidification reduces banding. Experiments show reducing radial thermal gradients and flattening solidification interface reduces compositional banding associated with plane-front, two-phase peritectic solidification. Possibility of coupled two-phase peritectic composite solidification still exists. Previously thought banding was inevitable.

Larson, David J., Jr.

Directional solidification of flake and spheroidal graphite cast iron in low and normal gravity environment

A NASA KC-135 research aircraft, flying repeated low-g trajectories that yield 20-30 sec of 0.1-0.001 g microgravity, has been used to study microgravity solidification's elimination of sedimentation and convection (with formation of unique and advantageous microstructures) for the case of eutectic-composition cast irons. The solidification interface of hypereutectic flake and spheroidal graphite cast irons has been slowly advanced through a 4 mm-diameter rod sample. Sample solidification rates have been correlated with accelerometer data, while independently controlling thermal gradients and solidification rates.

Hendrix, J. C.

On producing an alloy of uniform composition during rapid solidification processing

The fundamental mechanisms responsible for both micro scale and macro scale compositional variations during cellular and dendritic solidification are discussed. It is shown that presently available models for cellular and dendritic growth in alloys predict only the elimination of macrosegregation during rapid solidification but that microsegregation still persists even in this regime. A simple model is proposed here to describe the complete elimination of microsegregation in the rapid solidification regime. A solid of ideally uniform composition can be produced with no micro or macro segregation at both very low large solidifation rates.

Laxmanan, V.

Efficient estimation of diffusion during dendritic solidification

A very efficient finite difference method has been developed to estimate the solute redistribution during solidification with diffusion in the solid. This method is validated by comparing the computed results with the results of an analytical solution derived by Kobayashi (1988) for the assumptions of a constant diffusion coefficient, a constant equilibrium partition ratio, and a parabolic rate of the advancement of the solid/liquid interface. The flexibility of the method is demonstrated by applying it to the dendritic solidification of a Pb-15 wt pct Sn alloy, for which the equilibrium partition ratio and diffusion coefficient vary substantially during solidification. The fraction eutectic at the end of solidification is also obtained by estimating the fraction solid, in greater resolution, where the concentration of solute in the interdendritic liquid reaches the eutectic composition of the alloy.

Yeum, K. S.

The influence of buoyant forces and volume fraction of particles on the particle pushing/entrapment transition during directional solidification of Al/SiC and Al/graphite composites

Directional solidification experiments in a Bridgman-type furnace were used to study particle behavior at the liquid/solid interface in aluminum metal matrix composites. Graphite or silicon-carbide particles were first dispersed in aluminum-base alloys via a mechanically stirred vortex. Then, 100-mm-diameter and 120-mm-long samples were cast in steel dies and used for directional solidification. The processing variables controlled were the direction and velocity of solidification and the temperature gradient at the interface. The material variables monitored were the interface energy, the liquid/particle density difference, the particle/liquid thermal conductivity ratio, and the volume fraction of particles. These properties were changed by selecting combinations of particles (graphite or silicon carbide) and alloys (Al-Cu, Al-Mg, Al-Ni). A model which consideres process thermodynamics, process kinetics (including the role of buoyant forces), and thermophysical properties was developed. Based on solidification direction and velocity, and on materials properties, four types of behavior were predicted. Sessile drop experiments were also used to determine some of the interface energies required in calculation with the proposed model. Experimental results compared favorably with model predictions.

Stefanescu, Doru M.

Observation of alloy solidification using high-speed video

A high-speed video instrumentation system was used to observe solidification of undercooled Ti-51 at. pct Al. The camera system developed by Battelle is capable of operation at rates up to 12,000 frames per second. The system digitizes and stores video images acquired by a 64 x 64 pixel silicon photodiode array. In a joint effort with Vanderbilt University the camera was used to observe three transformations of the undercooled alloys, using containerless processing by electromagnetic levitation. The first was solidification where nucleation was induced at an undercooling of 9 percent Tl, where Tl is the liquidus temperature of the alloy, and the second was solidification where nucleation was spontaneous at an undercooling of 15 percent Tl. The third event was a solid-state nucleation and growth transformation following the solidification at an undercooling of 15 percent Tl.

Bassler, B. T.

Visualization of solidification front phenomena

Directional solidification experiments have been utilized throughout the Materials Processing in Space Program to provide an experimental platform which minimizes variables in solidification experiments. Because of the wide-spread use of this experimental technique in space-based research, it has become apparent that a better understanding of all the phenomena occurring during solidification can be better understood if direct visualization of the solidification interface were possible.

Workman, Gary L.

Solidification Interface Shape and Location During Processing in High Gradient Furnace with Quench

High Gradient Furnace with Quench (HGFQ) is being developed to facilitate metals processing experiments aboard the International Space Station. The sample is centered in an annular furnace and is held fixed during processing. The furnace itself is made to translate over the sample. Once in process, heat will flow through the sample from the Heater Zone to the Chill Zone. If operating conditions are correct, the solidification interface will stand in the gradient zone. Objectives of the HGFQ process are to provide a high gradient for the solidification with the solidification interface properly positioned in the gradient zone. At the recent RDR for HGFQ, one of the panelists raised the question about the suitability of HGFQ for potential future PIs. Specifically, it was stated by the design team at RDR that the present HGFQ design would provide a radius of curvature of the solidification interface of at least one sample diameter. The RDR panel argued that this was too small, and that most investigators would need a radius of curvature larger than this. The requirements established by the current PIs are shown. These requirements do not contain any specification about the interface shape. However, these requirements do define the envelope of operational parameters for HGFQ. The objectives of the present investigation are to 1) determine a suitable means of quantifying the interface shape, and 2) investigate the interface shape and how it is affected by processing parameters. The processing parameters to be considered are 1) sample material, 2) sample diameter, and 3) gradient zone length.

Woodbury, Keith A.

A Numerical Study of Directional Solidification and Melting in Microgravity

A computational model is presented for the study of the solidification and melting of a pure substance and of a binary alloy. The enthalpy method has been used, and incorporated into a commercial CFD code. Three examples of the use of the model are described: the three-dimensional solidification of a pure substance (succinonitrile), the results of which are compared with experiment; an example of the solidification of a bismuth-tin alloy; and a simulation of a solidification and melting experiment done in space known as the MEPHISTO program.

Chen, P. Y. P.

Exploiting the Temperature/Concentration Dependence of Magnetic Susceptibility to Control Convection in Fundamental Studies of Solidification Phenomena

The objective of this new research project is to demonstrate by experiment, supplemented by mathematical modeling and physical property measurement, that the effects of buoyancy driven convection can be largely eliminated in ground-based experiments, and further reduced in flight, by applying a new technique. That technique exploits the dependence of magnetic susceptibility on composition or temperature. It is emphasized at the outset that the phenomenon to be exploited is fundamentally and practically different from the magnetic damping of convection in conducting liquids that has been the subject of much prior research. The concept suggesting this research is that all materials, even non-conductors, when placed in a magnetic field gradient, experience a force. Of particular interest here are paramagnetic and diamagnetic materials, classes which embrace the "model alloys", such as succinonitrile-acetone, that have been used by others investigating the fundamentals of solidification. Such alloys will exhibit a dependence of susceptibility on composition. The consequence is that, with a properly oriented field (gradient) a force will arise that can be made to be equal to, but opposite, the buoyancy force arising from concentration (or temperature) gradients. In this way convection can be stilled. The role of convection in determining the microstructure, and thereby properties, of materials is well known. Elimination of that convection has both scientific and technological consequences. Our knowledge of diffusive phenomena in solidification, phenomena normally hidden by the dominance of convection, is enhanced if we can study solidification of quiescent liquids. Furthermore, the microstructure, microchemistry and properties of materials (thereby practical value) are affected by the convection occurring during their solidification. Hitherto the method of choice for elimination of convection has been experimentation in microgravity. However, even in low Earth orbit, residual convection has effects. That residual convection arises from acceleration (drag on the spacecraft), displacement from the center of mass or transients in the gravitational field (g-jitter). There is therefore a need for both further reducing buoyancy driven flow in flight and allowing the simulation of microgravity during ground based experiments. Previous investigations, the research project description, theory behind the study and experimental methods as well as plots of magnetic fields and forces are presented.

Evans, J. W.

Solidification of II-VI Compounds in a Rotating Magnetic Field

This project is aimed at using a rotating magnetic field (RMF) to control fluid flow and transport during directional solidification of elemental and compound melts. Microgravity experiments have demonstrated that small amounts of residual acceleration of less than a micro-g can initiate and prolong fluid flow, particularly when there is a static component of the field perpendicular to the liquid solid interface. Thus a true diffusion boundary layer is not formed, and it becomes difficult to verify theories of solidification or to achieve diffusion controlled solidification. The RMF superimposes a stirring effect on an electrically conducting liquid, and with appropriate field strengths and frequencies, controlled transport of material through a liquid column can be obtained. As diffusion conditions are precluded and complete mixing conditions prevail, the technique is appropriate for traveling solvent zone or float zone growth methods in which the overall composition of the liquid can be maintained throughout the growth experiment. Crystals grown by RMF techniques in microgravity in previous, unrelated missions have shown exceptional properties. The objective of the project is two-fold, namely (1) using numerical modeling to simulate the behavior of a solvent zone with applied thermal boundary conditions and demonstrate the effects of decreasing gravity levels, or an increasing applied RMF, or both, and (2) to grow elements and II-VI compounds from traveling solvent zones both with and without applied RMFs, and to determine objectively how well the modeling predicts solidification parameters. Numerical modeling has demonstrated that, in the growth of CdTe from a tellurium solution, a rotating magnetic field can advantageously modify the shape of the liquid solid interface such that the interface is convex as seen from the liquid. Under such circumstances, the defect structure is reduced as any defects which are formed tend to grow out and not propagate. The flow of liquid, however, is complex due to the competing flow induced by the rotating magnetic field and the buoyancy driven convection. When the acceleration forces are reduced to one thousandth of gravity, the flow pattern is much simplified and well controlled material transport through the solvent zone can be readily achieved. Triple axis diffractometry and x-ray synchrotron topography have demonstrated that there is no significant improvement in crystal quality for HgCdTe grown on earth from a tellurium solution when a rotating magnetic field is applied. However, modeling shows that the flow in microgravity with a rotating magnetic field would produce a superior product.

Gillies, D. C.

Analysis of X-Ray Microradiographs of Al-Au Interface Quench Profile using Modeling of Solidification Including Double-Diffusion and Convection in the Melt

Experimental data on Al-0.8Au horizontal solidification of a 1 mm thick specimen in a BN crucible shows the effect of growth rate on the solidification interface shape. For translation rates below 0.5 micron/s the interface maintains a plain and flat shape. When the translation rate is 3 to 5 micron/s or more, the interface appearance changes to two planar zones, with the zone closer to the bottom having higher inclination. The interface shapes were measured by first quenching in place during growth. X-ray microscopy shows the interface shape within the quenched sample by viewing through the side of the specimen. In order to provide theoretical explanation of the phenomena, numerical modeling was undertaken using finite element code FIDAP. Double diffusion convection in Al-0.8Au melt and crystal-melt interface curvature during directional solidification was analyzed numerically. Actual thermophysical properties of Al-0.8Au including the binary Al-Au phase diagram were used. Although convection in the sample is weak, for the slower translation rate convection and diffusion is sufficient for the redistribution of initial compositional stratification caused by gravity. When translation rate is raised, neither convection nor diffusion can provide proper mixing so that solidification temperatures differ significantly near the bottom within the bulk of the sample. As a result, the solid-liquid interface appears to have two planar zones with different inclination.

Bune, Andris V.

Real Time Characterization of Solid/Liquid Interfaces During Directional Solidification

A X-Ray Transmission Microscope (XTM) has been developed to observe in real time and in-situ solidification phenomenon at the solid/liquid interface. Recent improvements in the horizontal Bridgman furnace design provides real-time magnification (during solidification) up to 12OX. The increased magnification has enabled for the first time the XTM imaging of real-time growth of fibers and particles with diameters of 3-6 micrometers. Further, morphological transitions from planar to cellular interfaces have also been imaged. Results from recent XTM studies on Al-Bi monotectic system, Al-Au eutectic system and interaction of insoluble particles with s/I interfaces in composite materials will be presented. An important parameter during directional solidification of molten metal is the interfacial undercooling. This parameter controls the morphology and composition at the s/I interface. Conventional probes such as thermocouples, due to their large bead size, do not have sufficient resolution for measuring undercooling at the s/I interface. Further, the intrusive nature of the thermocouples also distorts the thermal field at the s/I interface. To overcome these inherent problems we have recently developed a compact furnace which utilizes a non-intrusive technique (Seebeck) to measure undercooling at the S/I interface. Recent interfacial undercooling measurements obtained for the Pb-Sn system will be presented. The Seebeck measurement furnace in the future will be integrated with the XTM to provide the most comprehensive tool for real time characterization of s/I interfaces during solidification.

Sen, S.