The range of magnitude of the liquid viscosity, η, as a function of temperature is one of the most impressive of any physical property, changing by approximately 17 orders of magnitude from its extrapolated value at infinite temperature (ηo) to that at the glass transition temperature, Tg. We present experimental measurements of containerlessly processed metallic liquids that suggest that log(η/ηo) as a function of TA/T is a potentially universal scaled curve. In stark contrast to previous approaches, the scaling requires only two fitting parameters, which are on average predictable. The temperature TA corresponds to the onset of cooperative motion and is strongly correlated with Tg, suggesting that the processes underlying the glass transition first appear in the high temperature liquid.
14 November 2016 in Journal of Physics: Condensed Matter
The liquid phase remains poorly understood. In many cases, the densities of liquids and their crystallized solid phases are similar, but since they are amorphous they lack the spatial order of the solid. Their dynamical properties change remarkably over a very small temperature range. At high temperatures, near their melting temperature, liquids flow easily under shear. However, only a few hundred degrees lower flow effectively ceases, as the liquid transforms into a solid-like glass. This temperature-dependent dynamical behavior is frequently characterized by the concept of kinetic fragility (or, generally, simply fragility). Fragility is believed to be an important quantity in glass formation, making it of significant practical interest. The microscopic origin of fragility remains unclear, however, making it also of fundamental interest. It is widely (although not uniformly) believed that the dynamical behavior is linked to the atomic structure of the liquid, yet experimental studies show that although the viscosity changes by orders of magnitude with temperature, the structural change is barely perceptible. In this article the concept of fragility is discussed, building to a discussion of recent results in metallic glass-forming liquids that demonstrate the presumed connection between structural and dynamical changes. In particular, it becomes possible to define a structural fragility parameter that can be linked with the kinetic fragility.
Space levitation processing allows researchers to conduct benchmark tests in an effort to understand the physical phenomena involved in rapid solidification processing, including alloy thermodynamics, nucleation and growth, heat and mass transfer, solid/liquid interface dynamics, macro- and microstructural evolution, and defect formation. Supported by ground-based investigations, a major thrust is to develop and refine robust computational tools based on theoretical and applied approaches. This work is accomplished in conjunction with experiments designed for precise model validation with application to a broad range of industrial processes.
The temperature dependence of the specific volume, thermal expansion coefficient, and specific heat in the equilibrium, supercooled liquids, and glasses of the bulk metallic glass-forming alloys Zr57Cu15.4Ni12.6Al10Nb5 and Zr58.5Cu15.6Ni12.8Al10.3Nb2.8 are determined using the containerless electrostatic levitation technique. Such measurements have not been possible thus far because of rapid crystallization from the supercooled metastable liquids. The results show a decrease in the thermal expansion coefficient with decreasing temperature before the onset of the glass transition. The difference in the rate of decrease between the two alloys indicates larger structural contributions to the thermal expansion for the stronger liquid at high temperatures.
The effect of fluid flow on crystal nucleation in supercooled liquids is not well understood. The variable density and temperature gradients in the liquid make it difficult to study this under terrestrial gravity conditions. Nucleation experiments were therefore made in a microgravity environment using the Electromagnetic Levitation Facility on the International Space Station on a bulk glass-forming Zr57Cu15.4Ni12.6Al10Nb5 (Vit106), as well as Cu50Zr50 and the quasicrystal-forming Ti39.5Zr39.5Ni21 liquids. The maximum supercooling temperatures for each alloy were measured as a function of controlled stirring by applying various combinations of radio-frequency positioner and heater voltages to the water-cooled copper coils. The flow patterns were simulated from the known parameters for the coil and the levitated samples. The maximum nucleation temperatures increased systematically with increased fluid flow in the liquids for Vit106, but stayed nearly unchanged for the other two. These results are consistent with the predictions from the Coupled-Flux model for nucleation.
Metallic glasses have the potential to become transformative materials, but this is hindered by the lack of ability to accurately predict which metallic alloys will form good glasses. Current approaches are limited to empirical rules that often rely on parameters that are unknown until the glasses are made, rendering them not predictive. In this Perspective, properties of metallic liquids at elevated temperatures and how these might lead to better predictions for glass formation are explored. A central topic is liquid fragility, which characterizes the different dynamics of the liquids. What fragility is and how it might be connected to the liquid structure is discussed. Since glass formation is ultimately limited by crystallization during cooling, recent advances in crystal growth and nucleation are also reviewed. Finally, some approaches for improving glass stability and glass rejuvenation for improved plasticity are discussed. Building on a summary of results, some key questions are raised and a prospective for future studies is offered.