Supercooled and glassy water: Metastable liquid(s), amorphous solid(s), and a no-man’s land

Handle, Philip H.; Loerting, Thomas; Sciortino, Francesco

doi:10.1073/pnas.1700103114

Cited by 119 publications

(96 citation statements)

References 130 publications

(138 reference statements)

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“…This model is able to reproduce the complex pattern of thermodynamic anomalies which characterise liquid and supercooled water [48]. In that study an accurate evaluation of the number of PEL basins sampled at each T and ρ has been carried out, providing access to the configurational entropy.…”

Section: Resultsmentioning

confidence: 99%

The Adam–Gibbs relation and the TIP4P/2005 model of water

Handle

Sciortino

2018

Molecular Physics

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We report a numerical test of the Adam–Gibbs relation for the TIP4P/2005 model of water. The configurational entropy is here evaluated as the logarithm of the number of different basins in the potential energy landscape sampled in equilibrium conditions. Despite the non-monotonic behaviour which characterise the density dependence of the diffusion coefficient, the Adam–Gibbs relation is satisfied within the numerical precision in a wide range of densities and temperatures. We also show that expressions based on the excess entropy (the logarithm of the number of sampled microstates in phase space) fail in the region of densities where a tetrahedral hydrogen bond network develops.

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Section: Resultsmentioning

confidence: 99%

The Adam–Gibbs relation and the TIP4P/2005 model of water

Handle

Sciortino

2018

Molecular Physics

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“…Recently, the presence of LLT in ST2 water was confirmed convincingly by Palmer et al (5,11). Although there is supporting evidence for polymorphism in water (1)(2)(3)(4)(5)12), the debate is still continuing for LLT in real water because of the experimental difficulty in accessing it in pure water (recent efforts to access LLT of pure water from the low-temperature side) (4,(13)(14)(15)(16)(17). There have also been efforts to access LLT of water by using aqueous solutions (18)(19)(20)(21)(22)(23)), yet which is often controversial.…”

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confidence: 86%

“…Contrary to this intuition, there has been a growing body of experimental and numerical evidence that even a single-component substance may have more than two isotropic homogeneous liquid states, and there is a first-order phase transition between these states, which is called "liquid-liquid transition" (LLT). Candidates of liquids exhibiting LLT include water (1)(2)(3)(4)(5), phosphorus (6), silicon (7), and Y2O3 − Al2O3 (8). LLT is now one of the most mysterious phenomena in condensed matter physics, posing a fundamental question on the very nature of the liquid state.…”

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confidence: 99%

Link between molecular mobility and order parameter during liquid–liquid transition of a molecular liquid

Murata

Tanaka

2019

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

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Liquid-liquid transition (LLT) is the transformation of one liquid to another via first-order phase transition. For example, LLT in a molecular liquid, triphenyl phosphite, is macroscopically the transformation from liquid I in a supercooled state to liquid II in a glassy state. Reflecting the transformation from the liquid to glassy state, the LLT is accompanied by considerable slowing down of overall molecular dynamics, but little is known about how this proceeds at a molecular level coupled with the evolution of the order parameter. We report such information by performing time-resolved simultaneous measurements of dielectric spectroscopy and phase contrast microscopy/Raman spectroscopy by using a dielectric cell with transparent electrodes. We find that the temporal change in molecular mobility crucially depends on whether LLT is nucleation growth type occurring in the metastable state or SD type occurring in the unstable state. Furthermore, our results suggest that the molecular mobility is controlled by the local order parameter: more specifically, the local activation energy of molecular rotation is controlled by the local fraction of locally favored structures formed in the liquid. Our study sheds light on the temporal change in the molecular dynamics during LLT and its link to the order parameter evolution.liquid-liquid transition | phase ordering dynamics | order parameter | local molecular dynamics | dielectric relaxation Significance Contrary to a common sense that a liquid state is unique for a pure system, there have been a number of indications for the presence of more than two liquid states. The transition between the liquid states is called "liquid-liquid transition." There has so far been little information on how local molecular dynamics changes during the transformation. Here, we reveal the correlation between the order parameter and molecular dynamics by real-time dielectric spectroscopy measurements during the transformation from liquid I to liquid II in a molecular liquid, triphenyl phosphite. Our results suggest that the local order parameter controls local dynamics. Our finding sheds light on the nature of liquid-liquid transition from a perspective of molecular-level dynamics.

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“…metastable states | perovskite | pressure | compression−decompression | bandgap M etastable materials can, in some cases, exhibit striking properties that are absent in thermodynamically stable states, and are of great significance in applications such as supramolecular polymers, graphene adlayers, and high-entropy alloys (1)(2)(3)(4). The most frequently adopted method to achieve metastable states (e.g., supercooled transient liquid) is through fast quenching from a high temperature (5,6). Such a heating/quenching strategy has limited utility for materials that are vulnerable to high temperature, such as organic-containing materials.…”

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confidence: 99%

Isothermal pressure-derived metastable states in 2D hybrid perovskites showing enduring bandgap narrowing

Liu

Gong

Kong

et al. 2018

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

151

168

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Materials in metastable states, such as amorphous ice and supercooled condensed matter, often exhibit exotic phenomena. To date, achieving metastability is usually accomplished by rapid quenching through a thermodynamic path function, namely, heating-cooling cycles. However, heat can be detrimental to organic-containing materials because it can induce degradation. Alternatively, the application of pressure can be used to achieve metastable states that are inaccessible via heating-cooling cycles. Here we report metastable states of 2D organic-inorganic hybrid perovskites reached through structural amorphization under compression followed by recrystallization via decompression. Remarkably, such pressure-derived metastable states in 2D hybrid perovskites exhibit enduring bandgap narrowing by as much as 8.2% with stability under ambient conditions. The achieved metastable states in 2D hybrid perovskites via compression-decompression cycles offer an alternative pathway toward manipulating the properties of these "soft" materials.

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Supercooled and glassy water: Metastable liquid(s), amorphous solid(s), and a no-man’s land

Cited by 119 publications

References 130 publications

The Adam–Gibbs relation and the TIP4P/2005 model of water

The Adam–Gibbs relation and the TIP4P/2005 model of water

Link between molecular mobility and order parameter during liquid–liquid transition of a molecular liquid

Isothermal pressure-derived metastable states in 2D hybrid perovskites showing enduring bandgap narrowing

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