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Constitutional supercooling and corresponding microstructure transition triggered by high magnetic field gradient during directional solidification of Al-Fe eutectic alloy

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Abstract

Directional solidification experiments of eutectic AlFe alloys were carried out under different high magnetic field gradients. High magnetic field gradient changed the microstructure selection during solidification process, induced the solidification microstructure to undergo eutectic instability, cellular transition, single-phase instability, and dendrite transition, which is similar to the planar-cellular-dendritic crystal growth pattern transition usually induced by an increasing growth velocity without magnetic field. The single phase was proved to be formed through an independent nucleation mechanism during single-phase instability. The effect of high magnetic field gradient on solidification was analyzed. Through the coupling effect of magnetic force and Lorentz force on solute migration and diffusion during solidification, high magnetic field gradient triggered a constitutional supercooling at the front of solid-liquid interface, which led to the growth pattern transition. A solidification model of eutectic alloy under high magnetic field gradient was proposed, and the microstructure selection map of AlFe alloy under gradient magnetic field was qualitatively drawn for the first time. This work proved that an alloy material with a microstructure usually obtained at high growth velocity can be obtained at a low growth velocity by applying a high magnetic field gradient, and suggested a new potential method for the future controlling of alloy structures and properties.

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We investigated applying a magnetic field (up to 6 T) during directional solidification of a hypereutectic Al–8 wt. %Fe alloy, finding that it dramatically affected the final microstructure. A eutectic area appeared at the top of the samples, and as the magnetic flux density increased, the eutectic area clearly enlarged. In addition, the Al3Fe phase was twisted and fractured, and some phases aggregated and distributed randomly in the samples. We also investigated the volume fraction distribution of the Al3Fe phase, revealing that applying the magnetic field during solidification caused dramatic disorder in the solute and phase distributions. The magnetic force induced by the interaction between the magnetic field gradient and the magnetic materials appeared to be the main reason not only for the occurrence and enlargement of the eutectic area but also for the movement of Fe-enriched zones during directional solidification. Otherwise, the deformation and fracture of the Al3Fe phase, the morphological instability in the interface between the eutectic area and the Al3Fe phase, and the random distribution of the aggregated Al3Fe phase appeared to come from the thermoelectric magnetic force/thermoelectric magnetic convection under the magnetic field.
Article
The conditions for fully eutectic growth in Al-Fe alloys at a temperature gradient of 20 K mm-1 are reported for ranges of composition from 2.2 to 6.1 wt % Fe and of growth velocity from 0.03 to 10 mm sec-1. All six main classes of growth structure (i.e. Al-Al3Fe or Al-Al6Fe eutectics either alone or together with primary αAl or Al3Fe) were obtained, some of them reported for the first time for steady-state conditions. Observed concentration-dependences both of the limiting growth velocity for primary Al3Fe and of the interphase spacing for the fully eutectic Al-Al6Fe displacing it are in good agreement with theory. Hardness levels for the Al-Al6Fe eutectic as a function of concentration are similar to those for αAl dendritic structures grown in much thinner sections under splat-cooling conditions. The significance of some observed transitions in growth morphology for eutectic cells, Al6Fe eutectic rods and αAl dendrites is discussed.
Article
Eutectic solidification is very important in the development of new materials in which the periodic multiphase structures may have a remarkable or enhanced functionality. The morphology evolution during eutectic solidification is investigated experimentally using slab-geometry slides of succinonitrile-(D)camphor (SCN-DC) transparent organic eutectic material. By specifically focusing on the effect of pulling velocity on microstructure in directional growth, the temperature gradient and the thickness are kept the same in all the experiments. It is found that eutectic seeds first occur in the grain boundary channel or the specimen side-wall groove. And the growth of eutectic seeds is both parallel to the direction of temperature gradient and along the liquid/solid interface at the same time. At a low pulling velocity (0.064-0.44 mu m/s), the macroscopic growth morphology is flat, and the inner microstructure is rod-shaped, which is parallel to the growth direction. It is obvious that the eutectic spacing becomes smaller with the increase of pulling velocity. At a high pulling velocity (0.67-1.56 mu m/s), the macroscopic growth morphology becomes cellular. However, the inner microstructure is still rod-shaped, but its distribution is radially outward. And the eutectic spacing decreases as pulling velocity increases.
Article
In this study Ni-Ni3Si eutectic in situ composites are obtained by Bridgman directional solidification technique when the solidification rate varies from 6.0 mu m/s to 40.0 mu m/s. At the low solidification rates the lamellar spacing is decreased with increasing the solidification rate. When the solidification rate is higher than 25 mu m/s, the lamellar spacing tends to be increased, because the higher undercooling makes the mass transport less effective. The adjustments of lamellar spacing are also observed during the directional solidification process, which is consistent with the minimum undercooling criterion. Moreover, the transitions from planar interface to cellular, then to dendritic interface, and finally to cellular interface morphologies with increasing velocity are observed by sudden quenching when the crystal growth tends to be stable. Copyright
Article
Recently, the studies on the effects of high magnetic fields on solidification processes have been paid much attention both from the fundamental and applied points of view. With the aid of the enhanced Lorentz force and magnetization effect caused by the remarkably increased magnetic field intensity, several interesting phenomena, such as the control of fluid flow and particle migration in a melt, crystal orientation, and phase alignment, have been obtained. Moreover, the magnetic force induced by the interaction of magnetization and high magnetic field gradient has been evidenced to show significant effects on the microstructure evolution of alloys. In this paper, the recent development of the control of the solidification process by high magnetic fields is reviewed from the view point of uniform magnetic fields and magnetic field gradients.
Article
Coupling with the thermodynamic database and incorporating the effects of local non-equilibrium and off-diagonal diffusional interactions, an extended morphological stability analysis was performed for a planar interface upon rapid solidification of concentrated multi-component alloys. Compared with the previous work, the model is able to clarify the effects of concentration dependence and diffusional interactions on the interface stability. Taking the Al–Mg–Zn alloy as an example, the neutral stability, i.e. the critical Zn concentration (with Mg concentration fixed) for the breakdown of the planar interface, was studied. The stability mechanisms for the neutral Zn concentration subjected to different Mg concentrations and the off-diagonal diffusion effect were clarified. In particular, for high Mg concentrations, a stage of absolute instability dependent on the Mg diffusion effect but independent of the Zn concentration happens. Although the off-diagonal diffusion is several orders of magnitude smaller than the solute diffusion coefficients, it can significantly change the Zn concentration for the neutral stability conditions.
Article
Most theoretical work on dendrite growth has focused on dilute binary alloys, while most industrial alloys are concentrated multi-component systems. By incorporating the local non-equilibrium effects both at the interface and in the bulk liquid, the thermodynamic database and diffusional interaction, a model was developed for dendrite growth in undercooled concentrated multi-component alloys. An experimental study of dendrite growth in undercooled Ni–18 at.% Cu–18 at.% Co melts was carried out and the measured interface velocities (V) were well predicted by the present model over the whole undercooling range (ΔT = 30–313 K). During dendrite growth the partition coefficients change non-monotonically due to interaction between the species and changes in the dendrite tip radius. Interaction between the species also leads to a lower interface velocity and larger ΔT and V as the ΔT–V relation plateaus. The previous definition of constitutional undercooling, i.e. the sum of the contributions of each solute, is not applicable to concentrated multi-component alloys. The controlling mechanisms during dendrite growth are discussed with respect to the results of the calculations.
Article
The effect of a high axial magnetic field (up to 12 T) on the microstructure in a directionally solidified Al–Al2Cu eutectic alloy has been investigated experimentally. The results show that a high magnetic field decreases the eutectic spacing and degenerates the lamellar structure into a wavy one at a low growth speed. X-ray diffraction, selected-area electron diffraction and high-resolution electron microscopy analyses indicate that the field changes the preferred orientation. The Al2Cu crystal is oriented with the 〈0 0 1〉-crystal direction along the solidification direction (i.e., the magnetic field direction). At a pulling velocity of 0.5 μm/s, the magnetic field (B ⩾ 4T) is responsible for the segregation; which consists of Al striations on the longitudinal section and Al-rich zones on the transverse section. The effects of the field may be attributed to the orientation of the Al2Cu and the Al crystals and the decrease of the diffusion coefficient caused by the magnetic field.
Article
The eutectic Sn–0.7 wt%Cu alloy is considered an important alternative to replace the classic eutectic Sn–Pb alloy, used to join metallic surfaces in electronic devices. The stable Sn–Cu eutectic is composed of a mixture of a tin-rich phase and fibrous Cu6Sn5 intermetallic particles. The morphology, size and distribution of stable and metastable intermetallic particles may affect the mechanical properties of the alloy. The distribution of these intermetallics is characterized by the interphase spacing, which depends on thermal parameters such as the growth rate (v) and the cooling rate (T˙) during solidification. The aim of this study is to investigate the microstructural evolution of a eutectic Sn–0.7 wt%Cu solder alloy during transient solidification. The resulting microstructural morphology depends on v and T˙, and in the case of soldering processes the control of these parameters is essential for the design of the final microstructure. A gradual cellular to dendritic transition was observed to occur for growth rates ranging from 0.3 to 0.5 mm s−1 and cooling rates from 0.9 to 1.5 K s−1. The cellular region was shown to be characterized by aligned eutectic colonies, and experimental growth laws relating cellular, dendritic and interphase spacings to both v and T˙ have been proposed.
Article
As one of the semiconductor-metal eutectic (SME) composites, Si-TaSi2 eutectic composite has many characters such as the high melting point of TaSi2 material, the large density of TaSi2 fibers incorporated into the Si matrix, three-dimensional array of Schottky junctions grown in the composite spontaneously. So it is an ideal candidate for field emission array cathodes. In this paper, the directionally solidified Si-TaSi2 eutectic in situ composite for field emission is prepared by means of the electron beam floating zone melting (EBFZM) technique on the basis of Czochralski (CZ) method. The Si-TaSi2 eutectic in situ composite, which has high-aligned and uniformly distributed TaSi2 fibers in the Si matrix, can be obtained when the solidification rate changes from 0.3 to 9.0 mm/min. As the solidification rate is increased, both the fibers’ diameter and inter-rod spacing are decreased, while the fibers’ density and the volume fraction are increased. Moreover, the transition from a planar interface to cellular interface and then to planar interface morphologies with increasing velocity is observed with the zero power method.
Article
In this work, Mn–Sb alloys were melted and held in various magnetic field gradients for various times. The corresponding distributions of the alloying elements in the alloys in liquid state were revealed by a quenching method. It was found that the primary MnSb showed a relatively uniform distribution in the alloy quenched in the magnetic field gradient of BdB/dz=0T2/m, while it was mainly distributed in the lower and upper part of the alloys quenched in negative and positive magnetic field gradients, respectively. The experimental results show that it is possible to in situ control the distributions of alloying elements in alloys in the liquid state using high gradient magnetic fields if there is a difference in magnetic susceptibility.
Article
Bi–MnBi composite has been directionally solidified to investigate the influence of a strong magnetic field on its microstructure, growth characteristics and magnetic properties. Experimental results show that MnBi eutectic fiber is aligned, regularized and coarsened during directional solidification under an axial strong magnetic field. In particular, the alignment of irregular eutectic fiber under a magnetic field may offer a new method to prepare regular fiber composite and extend the range of uses of such composite. It has also been found that the strong magnetic field has modified the growth mode of the MnBi fiber and enhanced the transition from non-faceted to faceted. The distribution of the solute Mn in front of the MnBi fiber at the liquid–solid interface has been measured and the result shows that the magnetic field has enhanced the enrichment of the solute Mn in front of the MnBi fiber. Moreover, magnetic measurement reveals a pronounced promotion of the magnetic anisotropy and the remanence (Br) under the magnetic field. Based on these experimental results, a simple theory of solute enrichment in front of a ferromagnetic fiber and fiber coarsening under a strong magnetic field has been proposed.
Article
Co–24.0at.% Sn eutectic alloy melt was undercooled to different degrees below the equilibrium eutectic temperature. The dependence of solidification behavior on undercooling was established based on the experimental results of the solidification microstructure, crystal orientation and crystal growth velocity. In the entire undercooling range studied (0–203K), coupled eutectic growth of the α-Co and β-Co3Sn2 phases invariably takes place during the rapid solidification stage. The eutectic solidification interface advances in the alloy melt in seaweed morphologies rather than the well-known dendritic mode due to the weak interface energy anisotropy. But a critical undercooling of 175K exists, from which the eutectic solidification interface changes from a fractal into a compact seaweed pattern, accompanied with an abrupt increase of growth velocity. At high undercoolings the enhancement of the interface tip stability with the rise of crystal growth velocity should be responsible for the growth mode transition.
Article
Ag–Cu eutectic alloy was undercooled by the glass flux method and the solidification structure was investigated. It is revealed that when undercooling is not more than 70 K, the large difference in composition between two eutectic phases and very large thermal diffusion coefficient of the liquid result in cellular growth of the lamellar eutectics from the nucleation site. The variation in interface temperature during rapid solidification gives rise to a systematic change in microstructure within the sample. With the distance along the growth direction increasing, the finest lamellar spacing across the cellular eutectic rises, which indicates a gradually decreasing growth velocity of the primary eutectics. The primary lamellar eutectics near the nucleation site solidify under conditions far from equilibrium, and therefore are supersaturated with solute, and then partially remelted and ripened into anomalous eutectics. As undercooling increases, the area of the anomalous eutectics enlarges.
Article
Effect of a 0.2-T static magnetic field on the microstructure of a direct chill cast Al-9.8wt%Zn alloy slab was investigated. The static magnetic field transferred the microstructure from a mixture of equiaxed and columnar grains with the primary trunks growing in directions to twinned lamellar feathery grains with the primary and secondary arms growing in directions. The application of the static magnetic field results in the reduction of the heat discharge and solute mixing capacity through a damping effect on convection and thus a delay of the melt transformation to solid and a request to reduce the liquid/solid interface energy through reducing the interface area due to the loss of undercooling. The delay and the request account for the growth direction change and the formation of lamellas. The difference between the Al and Zn atomic radii and the related incoming flow facilitate the formation of the twins.
Article
The solidification structure of Ag–Cu eutectic alloy at different undercoolings was investigated. A critical undercooling of 76K is revealed, at which a transition from cellular to dendritic growth of lamellar eutectic occurs, accompanied with an abrupt rise of growth velocity. It is suggested that the large difference in composition between the two eutectic phases and the very large thermal diffusion coefficient of the liquid result in the cellular growth of lamellar eutectic at low undercoolings.
Article
The levitation in air of water, other diamagnetic substances and even living organisms was recently achieved by using the extremely strong magnetic field provided by a Bitter-type hybrid magnet. We too have succeeded in levitating water, but in the lower fields of an ordinary 10 T superconducting magnet. To achieve this we make use of gravitational and magnetically induced buoyancy forces in the host paramagnetic atmosphere (pressurized air or oxygen), rather than simply the diamagnetic force on the levitating object, to balance the gravitational force. This permits the magnetic levitation in air of paramagnetic as well as diamagnetic substances, which was widely believed to be impossible. The physics underlying this effect is essentially the same as that of magnetohydrostatic ore separation, where a ferromagnetic fluid is used. Because our process can levitate subtances at a stable position in an atmosphere, we have named it `magneto-Archimedes levitation'.
Article
The solidification microstructures for Al-0.5–4 at.% Fe alloys under constrained growth conditions have been calculated using analytical models of the growth kinetics of dendritic, eutectic and plane front interface morphologies of stable and metastable phases. Laser remelting experiments are carried out on an Al-4at.% Fe alloy with a low beam velocity (10 mm/s) in order to complete previous experimental results on the solidification microstructures obtained at intermediate growth rates by Bridgman experiments and at high growth rates by rapid laser resolidification. Comparison of predicted with experimentally determined solidification microstructure maps shows satisfactory agreement in view of the limited knowledge of the thermophysical properties of this system. These maps are useful for the interpretation of microstructures and phases forming under medium to high solidification rates and for the understanding and development of rapid solidification processing. Further the modelling is useful for improving available phase diagram information.
Article
Three binary Sn–Cu solder alloys of near-eutectic composition have been directionally solidified at different growth rates. The competition between primary tetragonal Sn cells/dendrites and eutectic is interpreted with the coupled zone concept. It is also found that Sn–Cu is a weakly irregular eutectic system with Cu6Sn5 leading the eutectic, but two different eutectic morphologies (coarse and fine) form simultaneously during eutectic growth. At higher growth rates, the eutectic interface breaks down into a cellular eutectic with the fine eutectic in the centre of the cells and the coarse one at the cell boundaries. This is explained by the segregation of Pb impurities ahead of the eutectic interface.
Article
The effects of high magnetic fields on the solidification microstructure of Al–Si alloys were investigated. Al–7.2wt%Si and Al–11.8wt%Si alloys were solidified in various high magnetic fields at different cooling rates. The secondary dendrite arm spacing (SDAS) of the primary Al dendrites and the lamellar spacing (LS) of the eutectics were measured. It was found that the application of a high magnetic field could decrease the SDAS of the primary Al dendrites in Al–7.2wt%Si alloys and the LS of the eutectics in Al–11.8wt%Si alloys. The effects of the high magnetic field on the SDAS decreased with increasing cooling rate. The decrease in the SDAS and LS can be attributed to the decrease of the solute diffusivity in the liquid ahead of the solid/liquid interface during the growth of the dendrite and eutectic. This decrease is caused by the high magnetic field which can damp the convection and avoid its contributions to the diffusion.
Article
The local solidification conditions and mechanisms associated with the flake-to-fiber growth mode transition in Al–Si eutectic alloys are investigated here using Bridgman-type gradient-zone directional solidification. Resulting microstructures are examined through quantitative image analysis of two-dimensional sections and observation of deep-etched sections, showing three-dimensional microstructural features. Several microstructural parameters were investigated in an attempt to quantify this transition, and it was found that the particle aspect ratio is effective in objectively identifying the onset and completion velocity of the flake-to-fiber transition, whereas traditional spacing parameters are not effective indicators of the transition. For a thermal gradient of 7–14K/mm, the transition was found to occur in two stages, appearing over velocity regimes from 0.10 to 0.50mm/s and from 0.50 to 0.95mm/s. The initial stage is dominated by in-plane plate breakup and rod formation within the plane of the plate, whereas the second stage is characterized by the onset of out-of-plane silicon rod growth, leading to the formation of an irregular fibrous structure. The boundary between the two stages is marked by widespread fibrous growth and the disappearance of the remnant flake structure, indicating a transition in the structural feature that governs the relevant diffusion length, from inter-flake spacing to inter-rod spacing.
Article
The stability of the shape of a moving planar liquid‐solid interface during the unidirectional freezing of a dilute binary alloy is theoretically investigated by calculating the time dependence of the amplitude of a sinusoidal perturbation of infinitesimal amplitude introduced into the planar shape. The calculation is accomplished by using gradients of the steady‐state thermal and diffusion fields satisfying the perturbed boundary conditions (capillarity included) to determine the velocity of each element of interface, a procedure justified in some detail. Instability occurs if any Fourier component of an arbitrary perturbation grows; stability occurs if all components decay. A stability criterion expressed in terms of growth parameters and system characteristics is thereby deduced and is compared with the currently used stability criterion of constitutional supercooling; some very marked differences are discussed.
Article
The preparation and characterization of metastable phases of the Al–Fe alloy system by mechanical alloying are reported. In Al-rich (up to 10 at.% Fe) alloys, the supersaturated f.c.c. solid solution of Fe in Al (up to 1 at.% Fe) is formed. Almost complete amorphization is confirmed in the composition range 17–33 at.% Fe. The metastable disordered b.c.c. solid solution of about 10 nm in grain size has also been formed by ball-milling for over 180 h in Fe-rich (above 50 at.% Fe) alloys. Examination of lattice parameter and magnetization have shown that the composition range and degree of disorder are comparable to those formed by crushing and sputter deposition.
Article
An as-quenched structural steel is tempered at 600 and 650 °C for 1 h without and with a 14-T magnetic field. The magnetic field can effectively prevent the directional growth of cementite along martensite plate boundaries and twin boundaries by increasing both the cementite/ferrite interfacial energy and the magnetostrictive strain energy. Finally, particle-like cementite is obtained. Moreover, the magnetic field can obviously retard the formation and growth of `distortion-free' regions in the matrix, though without having any noticeable effect on the orientation distribution of the `distortion-free' part. Investigating this subject contributes to the understanding of the way a magnetic field influences phase transformation in solid metallic materials.
Article
The linear perturbation theory of Mullins and Sekerka for the stability of a planar interface is extended to the case of large thermal peclet numbers. It is shown that an absolute stability criterion for a planar interface exists for undercooled melts also. In light of these results, the conventional constitutional supercooling criterion is reexamined and a more general planar interface stability criterion is proposed which is valid for low as well as high growth rate conditions. The results of this stability analysis are applied to dendritic growth from pure undercooled melt.RésuméNous avons étendu la théorie linéaire de la perturbation de Mullins et Sekerka pour la stabilité d'une interface plane au cas des grands nombres de Péclet. Nous montrons qu'il existe un critère de stabilité absolue pour une interface plane dans un matériau surfondu. A la lumière de ces résultats, nous réexaminons le critère de surfusion constitutionnelle classique et nous proposons un critère plus général pour la stabilité d'une interface plane, critère valable aussi bien pour les faibles que pour les fortes vitesses de croissance. Nous appliquons les résultats de cette analyse de la stabilité à la croissance dendritique dans un corps pur surfondu.ZusammenfassungDie lineare Störungstheorie von Mullins und Sekerka für die Stabilität einer ebenen Grenzfläche wird auf den Fall groβer thermischer Pecletzahlen erweitert. Es wird gezeigt, daβ ein absolutes Stabilitätskriterium für eine ebene Grenzfläche auch für unterkühlte Schmelzen besteht. Im Hinblick auf diese Ergebnisse wird das herkömmliche Kriterium der konstitutionellen Unterkühlung neu betrachtet. Es wird ein allgemeineres Kriterium für die Stabilität einer ebenen Grenzfläche vorgeschlagen, welches für Wachstumsbedingungen mit kleiner und groβer Geschwindigkeit gilt. Die Ergebnisse dieser Stabilitätsanalyse werden auf das dendritische Wachstum aus einer reinen unterkühlten Schmelze angewendet.
Article
A quantitative analysis is made of the redistribution of solute resulting from solidification in the absence of convection of a binary solution for transient and steady state conditions. Diffusion in the liquid is taken into account and shown to be of importance in determining the solute distribution in both the liquid and the solid. It is shown that the distribution for both normal freezing and zonemelting depends on the rate of solidification. When the speed of solidification is increased abruptly, a band of high solute concentration is formed in the solid; the reverse occurs when the speed is decreased abruptly. Values for the length of the constitutionally supercooled zone of liquid adjacent to a growing solid-liquid interface are calculated.
Article
Bulk layered synthetic Mn–Sb composites, with a gradient structure in morphology and composition towards the surfaces, were fabricated directly in situ under high magnetic field gradient conditions. Both of the primary phases of Mn–Sb binary system, i.e. MnSb and Sb, were found to segregate simultaneously from desired domains with a gradient interface in morphology in those alloys with hypo-eutectic composition. The volume fraction of the segregated phases strongly depended on the product of the magnetic flux density and its gradient.
Article
The effects of magnetic fields (of 0–5 T magnetic flux density) on iron electrodeposition were investigated in terms of current efficiency, morphology and crystal orientation. The AFM images showed that the shape of iron grains was angular in no magnetic field and roundish in magnetic fields. The occurrence of preferred orientation parallel to the substrate plane was influenced by an electric field (overpotential) and not by a magnetic field (MHD effect). By X-ray pole figure measurement, however, it was found that the biaxial texture evolution proceeded in a magnetic field while the uniaxial texture formed in no magnetic field.
Article
We study the morphological instability of the planar solid/liquid interface for a unidirectionally-solidified dilute binary mixture. We use a model developed by Boettinger et al. (1985, 1986), Aziz (1982), and Jackson et al. (1980), which allows for nonequilibrium effects on the interface through velocity-dependent segregation and attachment kinetics. Two types of instabilities are found in the linear stability analysis: (1) a cellular instability, and (2) an oscillatory instability driven by disequilibrium effects. Merchant and Davis (1990) characterized these instabilities subject to the frozen-temperature approximation (FTA). The present work relaxes the FTA by including the effects of latent heat and the full temperature distribution. Thermal effects slightly postpone the onset of the cellular instability but dramatically postpone the onset of the oscillatory instability; however, the absolute-stability conditions, at which at high speed the cellular and oscillatory instabilities are suppressed, remain unchanged from the FTA.