The Liquid–Liquid Phase Transition, Anomalous Properties, and Glass Behavior of Polymorphic Liquids

Giovambattista, Nicolás

doi:10.1002/9781118540350.ch6

Cited by 7 publications

(2 citation statements)

References 88 publications

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“…That is, LDA and HDA appear to be glasses of two distinct liquid states, a finding that supports two-liquid theories of water. A firstorder liquid-liquid transition has been recognized for some waterlike models [11][12][13][14] (for a recent review, see [15]), but its appearance is still highly disputed (see the most recent controversy on the extensively studied ST2 water model for an example [16][17][18]). However, it is striking that at temperatures above the hypothesized liquid-liquid critical point terminating the liquid-liquid transition line, two-state descriptions nicely reproduce the anomalous properties of water [19][20][21].…”

Section: Introductionmentioning

confidence: 99%

Shrinking water's no man's land by lifting its low-temperature boundary

et al. 2015

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Investigation of the properties and phase behavior of noncrystalline water is hampered by rapid crystallization in the so-called "no man's land." We here show that it is possible to shrink the no man's land by lifting its low-temperature boundary, i.e., the pressure-dependent crystallization temperature T x (p). In particular, we investigate two types of high-density amorphous ice (HDA) in the pressure range of 0.10-0.50 GPa and show that the commonly studied unannealed state, uHDA, is up to 11 K less stable against crystallization than a pressure-annealed state called eHDA. We interpret this finding based on our previously established microscopic picture of uHDA and eHDA, respectively [M. Seidl et al., Phys. Rev. B 88, 174105 (2013)]. In this picture the glassy uHDA matrix contains ice I h -like nanocrystals, which simply grow upon heating uHDA at pressures 0.20 GPa. By contrast, they experience a polymorphic phase transition followed by subsequent crystal growth at higher pressures. In comparison, upon heating purely glassy eHDA, ice nuclei of a critical size have to form in the first step of crystallization, resulting in a lifted T x (p). Accordingly, utilizing eHDA enables the study of amorphous ice at significantly higher temperatures at which we regard it to be in the ultraviscous liquid state. This will boost experiments aiming at investigating the proposed liquid-liquid phase transition.

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Section: Introductionmentioning

confidence: 99%

Shrinking water's no man's land by lifting its low-temperature boundary

et al. 2015

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“…In the last 20 years an increasingly growing number of discoveries of liquid polymorphism appeared in the literature. − Liquid–liquid transformations (LLTs) have been suggested by simulations to occur in correlation with changes of the directional bonding in molecular liquids such as water − and fused quartz or else in atomic liquids such as Si. − On the other hand, LLTs have been experimentally discovered in some elemental liquids − and more complex systems …”

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confidence: 99%

Simple-to-Complex Transformation in Liquid Rubidium

Gorelli

Panfilis²,

Bryk

et al. 2018

J. Phys. Chem. Lett.

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We investigated the atomic structure of liquid Rb along an isothermal path at 573 K, up to 23 GPa, by X-ray diffraction measurements. By raising the pressure, we observed a liquid-liquid transformation from a simple metallic liquid to a complex one. The transition occurs at 7.5 ± 1 GPa which is slightly above the first maximum of the T-P melting line. This transformation is traced back to the density-induced hybridization of highest electronic orbitals leading to the accumulation of valence electrons between Rb atoms and to the formation of interstitial atomic shells, a behavior that Rb shares with Cs and is likely to be common to all alkali metals.

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Nuclear quantum effects on the dynamics and glass behavior of a monatomic liquid with two liquid states

Eltareb

López

Giovambattista

2022

The Journal of Chemical Physics

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We perform path integral molecular dynamics (PIMD) simulations of a monatomic liquid that exhibits a liquid-liquid phase transition (LLPT) and liquid-liquid critical point. PIMD simulations are performed using different values of the Planck's constant h, allowing us to study the behavior of the liquid as nuclear quantum effects (NQE, i.e., atoms delocalization) are introduced, from the classical liquid ( h=0) to increasingly quantum liquids ( h>0). By combining the PIMD simulations with the ring-polymer molecular dynamics (RPMD) method, we also explore the dynamics of the classical and quantum liquids. We find that (i) the glass transition temperature of the low-density liquid (LDL) is anomalous, i.e., TgLDL(P) decreases upon compression. Instead, (ii) the glass transition temperature of the high-density liquid (HDL) is normal, i.e., TgHDL(P) increases upon compression. (iii) NQE shift both TgLDL(P) and TgHDL(P) towards lower temperatures but NQE are more pronounced on HDL. We also study the glass behavior of the ring-polymer systems associated to the quantum liquids studied (via the PI formulation of statistical mechanics). There are two glass states in all the systems studied, LDA and HDA, which are the glass counterpart of LDL and HDL. In all cases, the pressure-induced LDA-HDA transformation is sharp, reminiscent of a first-order phase transition. In the low-quantum regime, the LDA-HDA transformation is reversible, with identical LDA forms before the compression and after the decompression. However, in the high-quantum regime, the atoms become more delocalized in the final LDA than in the initial LDA, raising questions on the reversibility of the LDA-HDA transformation.

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The Liquid–Liquid Phase Transition, Anomalous Properties, and Glass Behavior of Polymorphic Liquids

Cited by 7 publications

References 88 publications

Shrinking water's no man's land by lifting its low-temperature boundary

Shrinking water's no man's land by lifting its low-temperature boundary

Simple-to-Complex Transformation in Liquid Rubidium

Nuclear quantum effects on the dynamics and glass behavior of a monatomic liquid with two liquid states

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