Microgravity effects on nonequilibrium melt processing of neodymium titanate: thermophysical properties, atomic structure, glass formation and crystallization.

The relationships between materials processing and structure can vary between terrestrial and reduced gravity environments. As one case study, we compare the nonequilibrium melt processing of a rare-earth titanate, nominally 83TiO2-17Nd2O3, and the structure of its glassy and crystalline products. Density and thermal expansion for the liquid, supercooled liquid, and glass are measured over 300-1850 °C using the Electrostatic Levitation Furnace (ELF) in microgravity, and two replicate density measurements were reproducible to within 0.4%. Cooling rates in ELF are 40-110 °C s-1 lower than those in a terrestrial aerodynamic levitator due to the absence of forced convection. X-ray/neutron total scattering and Raman spectroscopy indicate that glasses processed on Earth and in microgravity exhibit similar atomic structures, with only subtle differences that are consistent with compositional variations of ~2 mol. % Nd2O3. The glass atomic network contains a mixture of corner- and edge-sharing Ti-O polyhedra, and the fraction of edge-sharing arrangements decreases with increasing Nd2O3 content. X-ray tomography and electron microscopy of crystalline products reveal substantial differences in microstructure, grain size, and crystalline phases, which arise from differences in the melt processes.

Characterization of oscillation modes in levitated droplets using image and non-image based techniques.

The dynamics of levitated liquid droplets can be used to measure their thermophysical properties by correlating the frequencies at which normal modes of oscillation most strongly resonate when subject to an external oscillatory force. In two preliminary works, it was shown via electrostatic levitation and processing of various metals and alloys that (1) the resonance of the first principal mode of oscillation (mode n = 2) can be used to accurately measure surface tension and (2) that so-called "higher-order resonance" of n = 3 is observable at a predictable frequency. It was also shown, in the context of future space-based experimentation on the Electrostatic Levitation Furnace (ELF), a setup on the International Space Station (ISS) operated by Japan Aerospace Exploration Agency (JAXA), that while the shadow array method in which droplet behavior is visualized would be challenging to identify the n = 3 resonance, the normal mode n = 4 was predicted to be more easily identifiable. In this short communication, experimental evidence of the first three principal modes of oscillation is provided using molten samples of Tin and Indium and it is subsequently shown that, as predicted, an "image-less" approach can be used to identify both n = 2 and n = 4 resonances in levitated liquid droplets. This suggests that the shadow array method may be satisfactorily used to obtain a self-consistent benchmark of thermophysical properties by comparing results from two successive even-mode natural frequencies.

Benchmarking surface tension measurement method using two oscillation modes in levitated liquid metals.

The Faraday forcing method in levitated liquid droplets has recently been introduced as a method for measuring surface tension using resonance. By subjecting an electrostatically levitated liquid metal droplet to a continuous, oscillatory, electric field, at a frequency nearing that of the droplet's first principal mode of oscillation (known as mode 2), the method was previously shown to determine surface tension of materials that would be particularly difficult to process by other means, e.g., liquid metals and alloys. It also offers distinct advantages in future work involving high viscosity samples because of the continuous forcing approach. This work presents (1) a benchmarking experimental method to measure surface tension by excitation of the second principal mode of oscillation (known as mode 3) in a levitated liquid droplet and (2) a more rigorous quantification of droplet excitation using a projection method. Surface tension measurements compare favorably to literature values for Zirconium, Inconel 625, and Rhodium, using both modes 2 and 3. Thus, this new method serves as a credible, self-consistent benchmarking technique for the measurement of surface tension.

Density, excess volume, and structure of Fe-Cr-Ni melts.

The relationship between the excess volume and the structure of Fe-Cr-Ni melts is investigated using containerless levitation and in situ high-energy synchrotron x-ray diffraction techniques. The density of six hypoeutectic Fe-Cr-Ni alloys along the 72 wt. % Fe isopleth was measured in the stable and undercooled regions, and the excess volume was evaluated as a function of Cr concentration. It is found that the 72Fe-Cr-Ni alloys exhibit a positive sign of excess volume and the amount increases with increasing Cr concentration. Analysis of the structure factor and pair distribution function of the alloy family reveals that the short-range order in the melt becomes more pronounced with decreasing Cr concentration; this demonstrates a direct correlation between the excess volume and local liquid structure. A characteristic signature of the icosahedral structure is observed in the structure factor of the melts, and the potential origin of the positive excess volume of the 72Fe-Cr-Ni alloys is qualitatively discussed in relation to the icosahedral structure.

Hypercooling limit, heat of fusion, and temperature-dependent specific heat of Fe-Cr-Ni melts.

Thermophysical properties of Fe-Cr-Ni melts are studied using electrostatic levitation and rapid solidification techniques. Six hypoeutectic Fe0.72Cr w Ni(0.28-w) alloys with a Cr/Ni ratio of around 0.8 were melted and solidified at different degrees of undercooling. From the observed relationship between the undercooling and thermal plateau time, the hypercooling limit and heat of fusion of Fe0.72Cr w Ni(0.28-w) melts are determined as a function of Cr mass fraction. A ratio of specific heat and total hemispherical emissivity of the Fe-Cr-Ni melts is calculated using the time-temperature profiles. A new method is presented to evaluate the temperature dependence of specific heat for undercooled melts and applied to this alloy family.

Faraday forcing of high-temperature levitated liquid metal drops for the measurement of surface tension.

In this work, a method for the measurement of surface tension using continuous periodic forcing is presented. To reduce gravitational effects, samples are electrostatically levitated prior to forcing. The method, called Faraday forcing, is particularly well suited for fluids that require high temperature measurements such as liquid metals where conventional surface tension measurement methods are not possible. It offers distinct advantages over the conventional pulse-decay analysis method when the sample viscosity is high or the levitation feedback control system is noisy. In the current method, levitated drops are continuously translated about a mean position at a small, constant forcing amplitude over a range of frequencies. At a particular frequency in this range, the drop suddenly enters a state of resonance, which is confirmed by large executions of prolate/oblate deformations about the mean spherical shape. The arrival at this resonant condition is a signature that the parametric forcing frequency is equal to the drop's natural frequency, the latter being a known function of surface tension. A description of the experimental procedure is presented. A proof of concept is given using pure Zr and a Ti39.5Zr39.5Ni21 alloy as examples. The results compare favorably with accepted literature values obtained using the pulse-decay method.

Experiments using a Ground-Based Electrostatic Levitator and Numerical Modeling of Melt Convection for the Iron-Cobalt System in Support of Space Experiments.

Materials research is being conducted using an electromagnetic levitator installed in the International Space Station. Various metallic alloys were tested to elucidate unknown links among the structures, processes, and properties. To accomplish the mission of these space experiments, several ground-based activities have been carried out. This paper presents some of our ground-based supporting experiments and numerical modeling efforts. Mass evaporation of Fe50Co50, one of the flight compositions, was predicted numerically and validated by the tests using an electrostatic levitator (ESL). The density of various compositions within the Fe-Co system was measured with ESL. These results serve as reference data for the space experiments. The convection inside a electromagnetically-levitated droplet was also modeled to predict the flow status, shear rate, and convection velocity under various process parameters, which is essential information for designing and analyzing the space experiments of some flight compositions influenced by convection.