Supercooled Liquids and Polyamorphism

Ha, Alice; Cohen, Itai; Zhao, Xiaolin; Lee, Michelle; Kivelson, Daniel

doi:10.1021/jp9530820

Cited by 150 publications

(149 citation statements)

References 33 publications

(45 reference statements)

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“…[10][11][12][13] There are some striking similarities between the slushy state of supercooled glycerol and the glacial state of TPP. For example, the rheological experiments on the glacial state of TPP shows that the maximum G′ is order of 10 6 Pa, 12 close to 10 7 Pa of the slushy phase of glycerol.…”

Section: Discussionmentioning

confidence: 99%

Aging and Solidification of Supercooled Glycerol

et al. 2010

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We experimentally investigate the solidification of supercooled glycerol during aging that has recently been observed by Zondervan et al. We find that a slow cooling at 5 K/h prior to the aging is required for solidification to take place. Furthermore, we show that the time of onset depends strongly on the aging temperature which we varied between 220 and 240 K. The nature of the solid phase remains unclear. The experiments show that upon heating the solid glycerol melts at the crystal melting point. However, rheology experiments in the plate-plate geometry revealed the growth of a soft, slushlike phase that is distinct from a crystal grown by seeding at the same aging temperature. The slushlike glycerol grows from a nucleation point at almost the same speed as a seeded crystal quenched to the same temperature, but its shear modulus is almost 2 orders of magnitude lower than the crystal phase, which we measure independently. While solidification was reproducible in the Couette geometry, it was not in the plate-plate geometry.

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Section: Discussionmentioning

confidence: 99%

Aging and Solidification of Supercooled Glycerol

et al. 2010

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“…All of the controversies come from the fact that this transition accompanies microcrystal formation and thus the final state, which is called "glacial phase," often contains microcrystallites. This led many researchers to explain the transition by non-LLT scenarios, which include a defect-ordered phase scenario predicted by a frustration limited domain theory (29,30,33,34), a microcrystallization scenario (35-38), and a liquid-crystal or plastic-crystal phase scenario (39). Each scenario captures a certain feature of the glacial phase, but fails in explaining all of the experimental results in a consistent manner.…”

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confidence: 99%

“…One of the hottest and long-standing debates is on the nature of the transition found in a molecular liquid, triphenyl phosphite (TPP), by Kivelson and his coworkers (29). The transition is very easy to access experimentally, because it takes place at ambient pressure and at a temperature range between 230 and 210 K and the transformation speed is slow enough to follow the kinetics.…”

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confidence: 99%

“…The transition is very easy to access experimentally, because it takes place at ambient pressure and at a temperature range between 230 and 210 K and the transformation speed is slow enough to follow the kinetics. Since the finding of this transition (29,30), many researchers thus have been interested in this intriguing phenomenon and there have been hot discussions on the nature of the transition (20,21). Some people interpreted this as a liquid-associated phenomenon (9,10,31,32), but others interpret it differently.…”

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confidence: 99%

“…refractive index (or, density) (9,10,29,30), and the polarity associated with local molecular ordering (12) has been suggested for LLT in TPP. There have been structural studies on LLT by X-ray and neutron scattering measurements, focusing on local liquid structures at an inter-and intramolecular scale (36,38,(52)(53)(54) and mesoscopic structures (34,55).…”

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Microscopic identification of the order parameter governing liquid–liquid transition in a molecular liquid

Murata

Tanaka

2015

Proc. Natl. Acad. Sci. U.S.A.

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A liquid-liquid transition (LLT) in a single-component substance is an unconventional phase transition from one liquid to another. LLT has recently attracted considerable attention because of its fundamental importance in our understanding of the liquid state. To access the order parameter governing LLT from a microscopic viewpoint, here we follow the structural evolution during the LLT of an organic molecular liquid, triphenyl phosphite (TPP), by timeresolved small-and wide-angle X-ray scattering measurements. We find that locally favored clusters, whose characteristic size is a few nanometers, are spontaneously formed and their number density monotonically increases during LLT. This strongly suggests that the order parameter of LLT is the number density of locally favored structures and of nonconserved nature. We also show that the locally favored structures are distinct from the crystal structure and these two types of orderings compete with each other. Thus, our study not only experimentally identifies the structural order parameter governing LLT, but also may settle a longstanding debate on the nature of the transition in TPP, i.e., whether the transition is LLT or merely microcrystal formation.liquid-liquid transition | order parameter | X-ray scattering | locally favored structure | transition kinetics L iquid-liquid transition (LLT) is an intriguing phenomenon in which a liquid transforms into another one via a first-order transition. This means that there can be more than two liquid states for a single-component substance. Despite its counterintuitive nature, there have recently been many pieces of experimental and numerical evidence for the existence of LLT, for various liquids such as water (1-5), aqueous solutions (6-8), triphenyl phosphite (9-12), l-butanol (13), phosphorus (14), silicon (15, 16), germanium (17), and Y 2 O 3 -Al 2 O 3 (18,19). This suggests that the LLT may be rather universally observed for various types of liquids. However, none of the LLTs reported so far is free from criticisms (20, 21), mainly because these LLTs take place under experimentally difficult conditions [e.g., at high temperature and pressure (14,15,(17)(18)(19)] or in a supercooled state below the melting point (1-3, 5-7, 9, 10), where the transition is inevitably contaminated by microcrystal formation. The latter is not limited to experiments but arises in numerical simulations, often causing many controversies vs. crystallization (26-28)]. For ST2 water, however, this issue has recently been settled by an extensive simulation study by Palmer et al. (4).One of the hottest and long-standing debates is on the nature of the transition found in a molecular liquid, triphenyl phosphite (TPP), by Kivelson and his coworkers (29). The transition is very easy to access experimentally, because it takes place at ambient pressure and at a temperature range between 230 and 210 K and the transformation speed is slow enough to follow the kinetics. Since the finding of this transition (29, 30), many researchers thus have been inte...

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Amorphous Ices

Tournier¹

2021

Encyclopedia of Glass Science, Technology, History, and Culture

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Supercooled Liquids and Polyamorphism

Cited by 150 publications

References 33 publications

Aging and Solidification of Supercooled Glycerol

Aging and Solidification of Supercooled Glycerol

Microscopic identification of the order parameter governing liquid–liquid transition in a molecular liquid

Amorphous Ices

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