Henri Nguyen-Thi

The Samson phase, β-Mg2Al3, revisited

Co-Authors: Michael Feuerbacher, Carsten Thomas, Julien P. A. Makongo, Stefan Hoffmann, Wilder Carrillo-Cabrera, Raul Cardoso, Yuri Grin, Guido Kreiner, Jean-Marc Joubert, Thomas Schenk, Joseph Gastaldi, Henri Nguyen-Thi, Nathalie Mangelinck-Noël, Bernard Billia, Patricia Donnadieu, Aleksandra Czyrska-Filemonowicz, Anna Zielinska-Lipiec, Beata Dubiel, Thomas Weber, Philippe Schaub, Günter Krauss, Volker Gramlich, Jeppe Christensen, Sven Lidin, Daniel Fredrickson, Marek Mihalkovic, Wieslawa Sikora, Janusz Malinowski, Stefan Brühne, Thomas Proffen, Wolf Assmus, Marc de Boissieu, Francoise Bley, Jean-Luis Chemin, Jürgen Schreuer Abstract. The Al−Mg phase diagram has been reinvestigated in the vicinity of the stability range of the Samson phase, β-Mg2Al3 (cF1168). For the composition Mg 38.5 Al 61.5, this cubic phase, space group Fd-3m (no 227), a = 28.242(1) Å, V = 22526(2) Å3, undergoes at 214 °C a first-order phase transition to rhombohedral β′-Mg2Al3(hR293), a = 19.968(1) Å, c = 48.9114(8) Å, V = 16889(2) Å3, (i.e. 22519 Å3 for the equivalent cubic unit cell) space group R3m (no 160), a subgroup of index four of Fd-3m. The structure of the β-phase has been redetermined at ambient temperature as well as in situ at 400 °C. It essentially agrees with Samsons model, even in most of the many partially occupied and split positions. The structure of β′-Mg2Al3is closely related to that of the β-phase. Its atomic sites can be derived from those of the β-phase by group-theoretical considerations. The main difference between the two structures is that all atomic sites are fully occupied in case of the β′-phase. The reciprocal space, Bragg as well as diffuse scattering, has been explored as function of temperature and the β- to β′-phase transition was studied in detail. The microstructures of both phases have been analyzed by electron microscopy and X-ray topography showing them highly defective. Finally, the thermal expansion coefficients and elastic parameters have been determined. Their values are somewhere in between those of Al and Mg.

Thermoelectric magnetic force acting on the solid during directional solidification under a static magnetic field

Thermoelectric magnetic force (TEMF), which is induced by the interaction between the thermoelectric current and the applied magnetic field, acting on the solid during directional solidification under a static magnetic field was derived. Equipping the derived equation, an analytical calculation of the velocity of a solid spherical particle submitted to the TEMF was carried out. The experiment with corresponding phenomenon was performed and recorded by the in situ synchrotron X-ray imaging, which permitted a direct measurement of the velocity of the TEMF-driven motion of detached fragments. The measurement of the velocities showed a reasonable agreement with the calculation results.

Fragmentation in an Al–7 wt-%Si alloy studied in real time by X-ray synchrotron techniques

Abstract One mechanism for the formation of equiaxed grains is the detachment of dendrite fragments which is believed to be at the origin of the central equiaxed core region in casting processes. Unfortunately, the dynamics of the fragmentation phenomena cannot be revealed by classical methods. Investigation of a unrefined Al–7 wt-%Si alloy using in situ and real time synchrotron X-radiography and X-ray topography at the European Synchrotron Radiation Facility, has allowed verification of the existence of dendrite fragmentation and of cascade fragmentation during directional solidification, and to study the evolution of the growth and sedimentation of the equiaxed grains formed from these fragments. An examination of the crystallographic misorientation of dendrites as fragmentation is ongoing. These results contribute to the understanding of the characteristics of the columnar to equiaxed transition and to knowledge of the origin of new equiaxed grains in unrefined alloys.

Measurement of solute profiles by means of synchrotron X-ray radiography during directional solidification of Al - 4 wt% Cu alloys

In the present study, we report on an image analysis procedure, which enables to extract from synchrotron radiographs the long range solute profiles in the whole sample and in both phases (solid and liquid). This image analysis is based on the measurement of local density differences, and is applied to study the directional solidification of Al - 4wt% Cu alloy, from planar to onset of the initial instability. Dedicated experiments were carried out at the European Synchrotron Radiation Facility (ESRF) in Grenoble (France). In order to validate this analysis the value of a key solidification parameter, namely the partition coefficient, was experimentally determined during the planar solidification, and a very good agreement was found with value found usually in the literature. On a further step, the evolution of the microstructure and solute profile during the initial transient of solidification was analysed in detail.

Thermoelectric magnetic flows in melt during directional solidification

Thermoelectric magnetic (TEM) flows in melts, which are generated by TEM forces in liquids, were uncovered by the shape evolution of the planar solid/liquid interface during directional solidification. The solid/liquid interface developing from an initially tilted shape to a nearly flat one has been in situ and real-time observed by means of synchrotron X-ray radiography. The corresponding numerical 3D simulations and velocity measurements of flows in the melt confirm that TEM flows exist and respond to this interface shape change. This observation provides visible evidence for TEM flows in melt and their influence on the solid/liquid interface dynamics when directional solidification is conducted in a magnetic field.

Modification of liquid/solid interface shape in directionally solidifying Al–Cu alloys by a transverse magnetic field

Al-0.85wt%Cu and Al-2.5wt%Cu alloys were directionally solidified under different transverse magnetic field (TMF) intensities to investigate the influence of TMF on the liquid/solid interface shape with respect to the various length scales appearing (planar, cellular, and dendritic interfaces). Results show that planar and cellular interfaces tilt to one side and then level off with increasing TMF although the dendritic interface appears not to behave in this manner. In situ synchrotron X-ray imaging was applied during directional solidification of the Al-4wt%Cu alloy under a 0.08T TMF, revealing leveling of the initially sloped interface. Solute redistribution, caused by thermoelectric magnetic convection (TEMC), responds to the changes in the interface shape. Because different typical length scales should be used in estimating the velocity of TEMC for planar, cellular, and dendritic interfaces, the maximum velocity of the convection ahead of the interface is obtained under different TMF intensities; correspondingly, leveling of the interface’s degree of slop varies with TMF.

Investigation of gravity effects on solidification of binary alloys with in situ X-ray radiography on earth and in microgravity environment

As most of the phenomena involved during solidification are dynamic, in situ and real-time X-ray imaging should be retained as the method of choice for investigating the solidification front evolution of metallic alloys grown from the melt. On Earth, natural convection in the melt is well known to be the major source of various disturbing effects which can significantly modify or mask important physical mechanisms. Microgravity environment is an efficient way to eliminate buoyancy and convection to provide benchmark data for the validation of models and numerical simulations. In addition, a comparative study of solidification experiments carried out on Earth and in space can also enlighten the effects of gravity. In the frame of the ESA - MAP programme entitled XRMON, an experimental set-up has been developed to perform directional solidification in microgravity conditions with in situ X-ray radiography observation. In the first part of this paper, we will present a brief review of some effects induced by gravity on the solidification process and investigated by mean of synchrotron X-ray radiography at ESRF (European Synchrotron Radiation Facility). In the second part of this paper, we will describe some results obtained with a prototype of the XRMON-Gradient Furnace set-up. These preliminary results show the large capabilities of the experimental set-up in terms of thermal behaviour, as well as X-ray observation.

Direct simulation of a directional solidification experiment observed in situ and real-time using X-ray imaging

It has been shown in the last decade that in situ and real-time observation of metallic alloy solidification is possible by using X-ray monitoring conducted at third generation synchrotron sources. A detailed analysis of a Bridgman experiment carried out at ESRF with an Al - 3.5 wt% Ni alloy was presented earlier [1]. This article proposes a direct simulation of the solidification of the entire sample for this experiment, in which all the dendritic grains are individually represented as they nucleate and grow in the experiment. This is possible by extracting from the radiographs a list of all the nucleated grains, including the positions and orientations of their main trunks. Simulation is performed using a two-dimensional (2D) Cellular Automaton (CA)-Finite Element (FE) model. As a result of the coupling between the CA and FE methods, consequences of the macroscopic transport of heat, liquid momentum and solute mass on the development of the dendritic grain structure are accounted for, and vice versa. The macroscopic deformation of the columnar front observed during the experiment is reproduced, as well as the columnar-to-equiaxed transition. The influence of flow patterns on macrosegregation is also discussed.

Characterization of Motion of Dendrite Fragment by X-Ray Radiography on Earth and under Microgravity Environment

In the frame of ESA-MAP (Microgravity Application Promotion) project entitled XRMON (In situ X-Ray MONitoring of advanced metallurgical processes under microgravity and terrestrial conditions), a microgravity (μg) experiment in the XRMON-GF (Gradient Furnace) setup was successfully launched in 2012 on board MASER 12 sounding rocket. During this experiment, in situ and real time observations of the formation of the solidification microstructures in diffusive conditions were carried out for the first time by using X-ray radiography. In addition, two reference experiments with the same control parameters but in ground-based conditions were performed to enable us a direct comparison with the μg experiment and therefore to enlighten the effects of gravity upon microstructure formation. This communication reports on fragmentation phenomenon observed during those experiments. For 1g upward solidification, fragmentations mainly take place in the upper part of the mushy zone. After their detachments, dendrite fragments are carried away by buoyancy force in the bulk liquid where they are gradually remelted. For μg experiment and horizontal solidification, this type of fragmentation is not observed. However, a great number of fragmentations are surprisingly revealed by in situ observation in the deep part of the mushy zone, when the liquid fraction is very small. Moreover, as soon as they are detached, the dendrite fragments move toward the cold part of the mushy zone, even in the case of μg experiment. The observations suggest that sample shrinkage may be at the origin of this fragment motion.

Influence of natural convection on microstructure evolution during the initial solidification transient: comparison of phase-field modeling with in situ synchrotron X-ray monitoring data

The influence of natural convection on the evolution of the solid-liquid (s/l) interface during the initial transient of upward directional solidification was studied on Al-4 wt.% Cu alloy by coupling the two dimensional quantitative phase-field model with the Navier-Stokes equations. The simulations were compared with in situ and real-time synchrotron X-ray monitoring data. The origin of natural convection in experiment was the presence of a small unavoidable horizontal temperature gradient. Due to the stringent requirement on the phase-field interface width parameters, the simulated domain could not be chosen as large as the size of the experimental sample. As the calculated fluid flow strength would be weakened by using a smaller domain, a horizontal temperature gradient ten times larger than the estimated experimental value was applied in simulation to recover a fluid flow washing the s/l interface similarly to experiments. Direct comparison to experimental measurements demonstrated that the phase-field simulations with convection qualitatively reproduced the evolution of all the characteristic parameters measured in experiments. Based on these results, the effects of natural convection on the growth dynamics of the s/l interface during directional solidification of alloy were further clarified.