Cooperative molecular motions in water: The liquid-liquid critical point hypothesis

Stanley, H. Eugene; Cruz, Luis; Harrington, S. T.; Poole, Peter H.; Sastry, Srikanth; Sciortino, Francesco; Starr, Francis W.; Zhang, Rong

doi:10.1016/s0378-4371(96)00429-3

Cited by 43 publications

(34 citation statements)

References 86 publications

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“…An alternative is to remove thermal energy by simulating deeply supercooled and pressurized water. In this case, many different water models have indicated the existence of an LLCP associated with a liquid-liquid transition [12][13][15][16]24,29,39,42,[145][146][147][148][149][150][151][152][153][154][155][156] . However, since the LLCP in the models is located at very low temperature, these simulations are challenging and require very long equilibration times.…”

Section: MD Simulationsmentioning

confidence: 99%

“…The fluctuations become less intense the farther away one moves into the one-phase region beyond the critical point where one can no longer distinguish the two phases. A remaining question thus concerns whether the coexistence line between the two liquids, HDL and LDL, also is terminated by a critical point, which could explain the seeming divergence of compressibility and heat capacity as water is deeply supercooled 16,23,29 . Experimentally, the probable location of such a critical point around 800 bar 8 and significantly below the temperature of homogeneous ice nucleation, makes it very challenging to unambiguously determine its existence.…”

Section: Introductionmentioning

confidence: 99%

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A Two-State Picture of Water and the Funnel of Life

Pettersson

2019

Springer Proceedings in Physics

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Here I show that experimental and simulation data on liquid water using vibrational (infrared and Raman) and X-ray (absorption and emission) spectroscopies, as well as recent data from X-ray scattering, are fully consistent with a two-state picture of water. At ambient conditions there are fluctuations between a dominating high-density liquid (HDL) and a low-density form (LDL). These are related to the two forms of amorphous ice at very low temperature, highdensity amorphous (HDA) and low-density amorphous (LDA), which interconvert in a firstorder-like transition. This transition line is assumed to continue into the so-called "No-man's land" as a liquid-liquid transition and terminate in a critical point with very large fluctuations between the two liquid forms. These fluctuations extend in a funnel-like region up to ambient temperatures and pressures and give water its unusual properties which are fundamental to life.With this picture we find simple, intuitive explanations of the anomalous properties of water, such as the density maximum at 4 C, why ice floats, and why the compressibility and heat capacity grow as the liquid is cooled. We summarize by noting that in this picture, water is not a complicated liquid, but two normal liquids with a complicated relationship.

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Section: MD Simulationsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

A Two-State Picture of Water and the Funnel of Life

Pettersson

2019

Springer Proceedings in Physics

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“…Despite this ''unfinished'' situation, the conceptual framework of critical phenomena is increasingly finding application in other fields, ranging from chemistry and biology on the one hand to econophysics (Mantegna and Stanley, 1999) and even liquid water (Stanley et al, 1997;Mishima and Stanley, 1998). Why is this?…”

Section: Calculations Of the ''Thermal'' Scaling Powermentioning

confidence: 99%

Scaling, universality, and renormalization: Three pillars of modern critical phenomena

1999

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This brief overview is designed to introduce some of the advances that have occurred in our understanding of phase transitions and critical phenomena. The presentation is organized around three simple questions: (i) What are the basic phenomena under consideration? (ii) Why do we care? (iii) What do we actually do? To answer the third question, the author shall briefly review scaling, universality, and renormalization, three of the many important themes which have served to provide the framework of much of our current understanding of critical phenomena. The style is that of a colloquium, not that of a mini-review article. [S0034-6861(99)02902-5] I. THE FIRST QUESTION: ''WHAT ARE CRITICAL PHENOMENA?'' S358

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“…5,6 The idea relies on prolongation of the coexistence line of the two amorphous phases above the glass transition temperature T g . The line, which separates low density (HDL) and high density (HDL) liquid phases, 7 should end at a second critical point at temperature located between T g and the homogeneous nucleation temperature T h . Even if the conjecture can appear consistent with the results from many molecular dynamics simulations, it leaves unsolved the question of whether an amorphous can be assumed as a metastable state.…”

Section: Introductionmentioning

confidence: 99%

Structure of bulk water from Raman measurements of supercooled pure liquid and LiCl solutions

et al. 2012

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In spite of decades of efforts, the puzzle of understanding the anomalies of liquid water remains unsolved. Several plausible theoretical scenarios have been proposed, but distinguishing among them requires accessing temperatures below the homogeneous nucleation temperature T h , which for bulk water is an experimentally impossible task. A widely adopted way for bypassing such a difficulty consists in studying the behavior of samples confined in nanopores, supercooled aqueous salt solutions, or in investigating samples transiently heated or cooled. In this paper, we compare the results obtained from Raman experiments on supercooled bulk water and supercooled LiCl aqueous solutions. The obtained results indicate that while at relatively high temperatures water in ionic solution can appear indistinguishable from bulk water, large differences are detected after further cooling. The comparison with very recent experimental data on water confined in nanopores suggests generalizing our result for every kind of confinement. Even if an experiment carried out under space-time constraints can produce results that match those from bulk water (in the temperature range where bulk water data are available), we cannot assume that the matching will persist at lower temperatures. This implies that the interpretation of many literature experimental results should be reconsidered. A coherent picture of existing experimental data can be obtained accepting the idea that amorphous water is not a metastable state and that homogeneous nucleation temperature represents a metastability limit.

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Cooperative molecular motions in water: The liquid-liquid critical point hypothesis

Cited by 43 publications

References 86 publications

A Two-State Picture of Water and the Funnel of Life

A Two-State Picture of Water and the Funnel of Life

Scaling, universality, and renormalization: Three pillars of modern critical phenomena

Structure of bulk water from Raman measurements of supercooled pure liquid and LiCl solutions

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