skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Pressure Induced Liquid-to-Liquid Transition in Zr-based Supercooled Melts and Pressure Quenched Glasses

Abstract

Through high-energy x-ray diffraction and atomic pair density function analysis we find that Zr-based metallic alloy, heated to the supercooled liquid state under hydrostatic pressure and then quenched to room temperature, exhibits a distinct glassy structure. The PDF indicates that the Zr-Zr distances in this glass are significantly reduced compared to those quenched without pressure. Annealing at the glass transition temperature at ambient pressure reverses structural changes and the initial glassy state is recovered. This result suggests that pressure causes a liquid-to-liquid phase transition in this metallic alloy supercooled melt. Such a pressure induced transition is known for covalent liquids, but has not been observed for metallic liquids. The High Pressure Quenched glasses are stable in ambient conditions after decompression.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1394136
DOE Contract Number:
AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Scientific Reports; Journal Volume: 7; Journal Issue: 1
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dmowski, W., Gierlotka, S., Wang, Z., Yokoyama, Y., Palosz, B., and Egami, T.. Pressure Induced Liquid-to-Liquid Transition in Zr-based Supercooled Melts and Pressure Quenched Glasses. United States: N. p., 2017. Web. doi:10.1038/s41598-017-06890-w.
Dmowski, W., Gierlotka, S., Wang, Z., Yokoyama, Y., Palosz, B., & Egami, T.. Pressure Induced Liquid-to-Liquid Transition in Zr-based Supercooled Melts and Pressure Quenched Glasses. United States. doi:10.1038/s41598-017-06890-w.
Dmowski, W., Gierlotka, S., Wang, Z., Yokoyama, Y., Palosz, B., and Egami, T.. Wed . "Pressure Induced Liquid-to-Liquid Transition in Zr-based Supercooled Melts and Pressure Quenched Glasses". United States. doi:10.1038/s41598-017-06890-w.
@article{osti_1394136,
title = {Pressure Induced Liquid-to-Liquid Transition in Zr-based Supercooled Melts and Pressure Quenched Glasses},
author = {Dmowski, W. and Gierlotka, S. and Wang, Z. and Yokoyama, Y. and Palosz, B. and Egami, T.},
abstractNote = {Through high-energy x-ray diffraction and atomic pair density function analysis we find that Zr-based metallic alloy, heated to the supercooled liquid state under hydrostatic pressure and then quenched to room temperature, exhibits a distinct glassy structure. The PDF indicates that the Zr-Zr distances in this glass are significantly reduced compared to those quenched without pressure. Annealing at the glass transition temperature at ambient pressure reverses structural changes and the initial glassy state is recovered. This result suggests that pressure causes a liquid-to-liquid phase transition in this metallic alloy supercooled melt. Such a pressure induced transition is known for covalent liquids, but has not been observed for metallic liquids. The High Pressure Quenched glasses are stable in ambient conditions after decompression.},
doi = {10.1038/s41598-017-06890-w},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Wed Jul 26 00:00:00 EDT 2017},
month = {Wed Jul 26 00:00:00 EDT 2017}
}
  • Through high-energy x-ray diffraction and atomic pair density function analysis we find that Zr-based metallic alloy, heated to the supercooled liquid state under hydrostatic pressure and then quenched to room temperature, exhibits a distinct glassy structure. The PDF indicates that the Zr-Zr distances in this glass are significantly reduced compared to those quenched without pressure. Annealing at the glass transition temperature at ambient pressure reverses structural changes and the initial glassy state is recovered. This result suggests that pressure causes a liquid-to-liquid phase transition in this metallic alloy supercooled melt. Such a pressure induced transition is known for covalent liquids,more » but has not been observed for metallic liquids. The High Pressure Quenched glasses are stable in ambient conditions after decompression.« less
  • Results of calorimetric, differential thermal analysis, and structural measurements are presented for a series of bulk metallic glass forming compositions in the Zr[endash]Ti[endash]Cu[endash]Ni[endash]Be alloy system. The calorimetric data for five alloys, prepared along the tie line between phase separating and nonphase separating compositions, show that the transition from phase separating to nonphase separating behavior is smooth. The bulk glasses near the center of the tie line exhibit large supercooled liquid regions: [Delta]T[approx]135 K, the largest known for a bulk metallic glass. [copyright] [ital 1999 American Institute of Physics.]
  • Results of calorimetric, differential thermal analysis, and structural measurements are presented for a series of bulk metallic glass forming compositions in the Zr{endash}Ti{endash}Cu{endash}Ni{endash}Be alloy system. The calorimetric data for five alloys, prepared along the tie line between phase separating and nonphase separating compositions, show that the transition from phase separating to nonphase separating behavior is smooth. The bulk glasses near the center of the tie line exhibit large supercooled liquid regions: {Delta}T{approx}135 K, the largest known for a bulk metallic glass. {copyright} {ital 1999 American Institute of Physics.}
  • In forming a metallic glass, the molten alloy should be quenched to avoid crystal nucleation during solidification. Understanding of the variation of the glass formability from system to system is therefore possible by considering the kinetics of crystallization. Recently, the authors have found that the crystallization mechanism is different for an amorphous solid and a supercooled liquid, which they attribute to the effects of viscosity on nucleation. Clarifying the crystallization is helpful to understanding the stabilization mechanism of a supercooled liquid. In this paper, they report the correlation between the supercooled liquid region and the crystallization mechanism by examining themore » glass transition temperature (T[sub g]), the crystallization temperature (T[sub x]), the structure of crystallized products and the morphology for the ternary Zr-Cu alloy systems; they then compare the results with those for the Pd-Ni-P and La-Al-Ni alloys.« less
  • The volumetric properties of silicate glasses and supercooled liquid are examined at high pressures and temperatures using X-ray computed tomography (CT) and absorption. The high pressure X-ray microtomography (HPXMT) system at the Advanced Photon Source, Argonne National Laboratory (GeoSoilEnvironCARS 13-BM-D beamline) consists of two opposing anvils compressed within an X-ray-transparent containment ring supported by thrust bearings and loaded using a 250-ton hydraulic press. This system permits the pressure cell to rotate under the load, while collecting radiographs through at least 180{sup o} of rotation. The 13-BM-D beamline permits convenient switching between monochromatic radiation required for radiography and polychromatic radiation formore » pressure determination by energy dispersive diffraction. We report initial results on several refractory magnesium silicate glasses synthesized by levitation laser heating. Volume changes during room temperature compression of Mg-silicate glasses with 33 mol% and 38 mol% SiO2 up to 11.5 GPa give an isothermal bulk moduli of 93--100 GPa for a K' of 1. These values are consistent with ultrasonic measurements of more silica-rich glasses. The volumetric properties of amorphous MgSiO{sub 3} at 2 GPa were examined during annealing up to 1000 C. We consider the consequences of heating through the glass transition and the implications for thermal expansivity of supercooled liquids at high pressure. Our results illustrate the capabilities of HPXMT for studies of refractory glasses and liquids at high pressure and offer strategies for future studies of liquid densities within the melting interval for magmas in planet interiors.« less