Density-driven liquid–liquid phase separation in the system AI2O3–Y2O3

Aasland, S.; McMillan, Paul F.

doi:10.1038/369633a0

Cited by 389 publications

(348 citation statements)

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“…The LLT of two distinct forms of liquid water has been intensely studied and debated [1][2][3][4][5][6][7] . Not limited to water, experimental and numerical support for existence of a polyamorphism or LLT has also been found in other systems, for example, in triphenyl phosphate 1 9 and Ce-Al 10,11 .…”

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confidence: 99%

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Liquid–liquid transition in a strong bulk metallic glass-forming liquid

et al. 2013

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Polymorphic phase transitions are common in crystalline solids. Recent studies suggest that phase transitions may also exist between two liquid forms with different entropy and structure. Such a liquid-liquid transition has been investigated in various substances including water, Al 2 O 3 -Y 2 O 3 and network glass formers. However, the nature of liquid-liquid transition is debated due to experimental difficulties in avoiding crystallization and/or measuring at high temperatures/pressures. Here we report the thermodynamic and structural evidence of a temperature-induced weak first-order liquid-liquid transition in a bulk metallic glassforming system Zr 41.2 Ti 13.8 Cu 12.5 Ni 10 Be 22.5 characterized by non-(or weak) directional bonds. Our experimental results suggest that the local structural changes during the transition induce the drastic viscosity changes without a detectable density anomaly. These changes are correlated with a heat capacity maximum in the liquid. Our findings support the hypothesis that the 'strong' kinetics (low fragility) of a liquid may arise from an underlying lambda transition above its glass transition.

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“…T here is a growing interest in density-or entropy-driven liquid-liquid phase transitions (LLTs) [1][2][3][4][5] . The LLT of two distinct forms of liquid water has been intensely studied and debated [1][2][3][4][5][6][7] .…”

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Liquid–liquid transition in a strong bulk metallic glass-forming liquid

et al. 2013

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“…[3][4][5] as well as melts of Al2O3-Y2O3. 6 It has been predicted 7 that LLTs should be common in all molecular liquids. However, an LLT has only been demonstrated in triphenyl phosphite (TPP) and n-butanol.…”

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Order Parameter of the Liquid–Liquid Transition in a Molecular Liquid

Mosses

Syme

Wynne

2014

J. Phys. Chem. Lett.

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Liquid-liquid transitions (LLTs) between amorphous phases of a single (chemically unchanged) liquid were predicted to occur in most molecular liquids but have only been observed in triphenyl phosphite (TPP) and n-butanol, and even these examples have been dismissed as "aborted crystallization". One of the foremost reasons that LLTs remain so controversial is the lack of an obvious order parameter, that is, a physical parameter characterizing the phase transition. Here, using the technique of fluorescence lifetime imaging, we show for the first time that the LLT in TPP is characterized by a change in polarity linked to changes in molecular ordering associated with crystal polymorphs. We conclude that the LLT in TPP is a phase transition associated with frustrated molecular clusters, explaining the paucity of examples of LLTs seen in nature.

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“…We have recently detected and quantified in situ the first-order liquid-liquid phase transitions (LLT) in yttria-alumina liquids (Greaves et al 2008), first proposed to explain polyamorphic phases in rapidly quenched yttria-alumina glasses differing in density and entropy (Aasland & McMillan 1994). Scattering experiments on liquid drops were performed under contactless conditions using aerodynamic levitation furnace methods (Hennet et al 2002), and in so doing reduced the danger of crystallization in the supercooled region.…”

Section: Liquid-liquid Transitions and Critical Pointmentioning

confidence: 99%

Polyamorphism and the universal liquid–liquid critical point in the supercooled state

Greaves

2010

DLS Proc.

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The physics of critical phenomena is well established in systems as diverse as molecular fluids, crystalline alloys and magnetic materials. As the critical point is approached, the susceptibility increases anomalously and fluctuations give rise to dramatic opalescence. Evidence has recently emerged for the existence of a second critical point in the liquid state at supercooled temperatures, below which polyamorphic phases coexist differing in density but sharing the same composition. Whilst much attention has been paid to supercooled water, polyamorphic phases have been observed in many elemental and oxide liquids potentially offering routes to low-entropy glasses. Our recent direct observation of a polyamorphic phase transition in levitated molten yttria-alumina offers the first opportunity to study the associated critical point in a real supercooled system. In situ small-angle X-ray scattering records sharp rises in the average correlation length of density fluctuations and in the compressibility as the transition is approached. Both increases approximate to the universal power-law relations predicted by the three-dimensional Ising model in common with all critical point phenomena. The observation brings the second critical point predicted in liquids into line with other critical phenomena.

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Density-driven liquid–liquid phase separation in the system AI2O3–Y2O3

Cited by 389 publications

References 34 publications

Liquid–liquid transition in a strong bulk metallic glass-forming liquid

Liquid–liquid transition in a strong bulk metallic glass-forming liquid

Order Parameter of the Liquid–Liquid Transition in a Molecular Liquid

Polyamorphism and the universal liquid–liquid critical point in the supercooled state

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