Liquid polymorphism: water in nanoconfined and biological environments

Stanley, H. Eugene; Buldyrev, Sergey V.; Franzese, Giancarlo; Kumar, Pradeep; Mallamace, Francesco; Mazza, Marco G.; Stokely, Kevin; Xu, Limei

doi:10.1088/0953-8984/22/28/284101

Cited by 53 publications

(58 citation statements)

References 119 publications

(188 reference statements)

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“…Figure 5 shows that when the mole fraction of the HS in the aqueous solution is increased the position of the LLCP shifts to a lower temperature and higher pressure. This shift can occur because the solvation tendency of the HS in the LDL is stronger than that in the HDL [95][96][97][98]. We also notice a narrowing of the region in the P − T plane between the LDL and HDL limit of mechanical stability (LMS) as x HS increases, suggesting a weakening of the LLPT line as solute content increases.…”

Section: Dmd Simulations On Mixtures Of Jagla Ramp Potential Particlementioning

confidence: 75%

Effect of hydrophobic environments on the hypothesized liquid-liquid critical point of water

et al. 2011

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The complex behavior of liquid water, along with its anomalies and their crucial role in the existence of life, continue to attract the attention of researchers. The anomalous behavior of water is more pronounced at subfreezing temperatures and numerous theoretical and experimental studies are directed towards developing a coherent thermodynamic and dynamic framework for understanding supercooled water. The existence of a liquid-liquid critical point in the deep supercooled region has been related to the anomalous behavior of water. However, the experimental study of supercooled water at very low temperatures is hampered by the homogeneous nucleation of the crystal. Recently, water confined in nanoscopic structures or in solutions has attracted interest because nucleation can be delayed. These systems have a tremendous relevance also for current biological advances; e.g., supercooled water is often confined in cell membranes and acts as a solvent for biological molecules. In particular, considerable attention has been recently devoted to understanding hydrophobic interactions or the behavior of water in the presence of apolar interfaces due to their fundamental role in self-assembly of micelles, membrane formation and protein folding. This article reviews and compares two very recent computational works aimed at elucidating the changes in the thermodynamic behavior in the supercooled region and the liquid-liquid critical point phenomenon for water in contact with hydrophobic environments. The results are also compared to previous reports for water in hydrophobic environments.

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Section: Dmd Simulations On Mixtures Of Jagla Ramp Potential Particlementioning

confidence: 75%

Effect of hydrophobic environments on the hypothesized liquid-liquid critical point of water

et al. 2011

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“…[22][23][24] It would be consistent with a range of thermodynamical and dynamical anomalies [25][26][27][28][29][30][31][32][33] and experiments. [34][35][36][37] Many more computer simulations investigating the phenomenology of the liquid-liquid critical point (LLCP) have been performed since then. [38][39][40][41][42][43][44][45][46][47][48][49][50][51][52][53][54][55] Detailed studies using ST2-RF have been made by Poole et al 56 using molecular dynamics, while Liu et al 57,58 simulated ST2 with Ewald summation (ST2-Ew) for the electrostatic long-range potential using Monte Carlo.…”

Section: Introductionmentioning

confidence: 99%

Finite-size scaling investigation of the liquid-liquid critical point in ST2 water and its stability with respect to crystallization

Kesselring

Lascaris

Franzese

et al. 2013

The Journal of Chemical Physics

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The liquid-liquid critical point scenario of water hypothesizes the existence of two metastable liquid phases-low-density liquid (LDL) and high-density liquid (HDL)-deep within the supercooled region. The hypothesis originates from computer simulations of the ST2 water model, but the stability of the LDL phase with respect to the crystal is still being debated. We simulate supercooled ST2 water at constant pressure, constant temperature, and constant number of molecules N for N ≤ 729 and times up to 1 μs. We observe clear differences between the two liquids, both structural and dynamical. Using several methods, including finite-size scaling, we confirm the presence of a liquid-liquid phase transition ending in a critical point. We find that the LDL is stable with respect to the crystal in 98% of our runs (we perform 372 runs for LDL or LDL-like states), and in 100% of our runs for the two largest system sizes (N = 512 and 729, for which we perform 136 runs for LDL or LDL-like states). In all these runs, tiny crystallites grow and then melt within 1 μs. Only for N ≤ 343 we observe six events (over 236 runs for LDL or LDL-like states) of spontaneous crystallization after crystallites reach an estimated critical size of about 70 ± 10 molecules. © 2013 AIP Publishing LLC. [http://dx

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“…30 Monitoring the behavior of the response functions upon supercooling water has thus provided a useful way to locate the Widom line if the correlation length cannot be determined directly. 31 Although liquid water has been at the center of most studies on liquid-liquid phase transitions, 32 the existence of a liquidliquid Widom line has also been indicated in other systems such as liquid silicon. 33 Recent experimental work on the liquid-gas supercritical region of argon 34 merits special mention.…”

Section: Introductionmentioning

confidence: 99%

Enhanced small-angle scattering connected to the Widom line in simulations of supercooled water

Wikfeldt¹,

Huang²,

Nilsson³

et al. 2011

The Journal of Chemical Physics

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We present extensive simulations on the TIP4P∕2005 water model showing significantly enhanced small-angle scattering (SAS) in the supercooled regime. The SAS is related to the presence of a Widom line (T(W)) characterized by maxima in thermodynamic response functions and Ornstein-Zernike correlation length. Recent experimental small-angle x-ray scattering data [Huang et al., J. Chem. Phys. 133, 134504 (2010)] are excellently reproduced, albeit with an increasing temperature offset at lower temperatures. Assuming the same origin of the SAS in experiment and model this suggests the existence of a Widom line also in real supercooled water. Simulations performed at 1000 bar show an increased abruptness of a crossover from dominating high-density (HDL) to dominating low-density (LDL) liquid and strongly enhanced SAS associated with crossing T(W), consistent with a recent determination of the critical pressure of TIP4P∕2005 at 1350 bar. Furthermore, good agreement with experimental isothermal compressibilities at 1000, 1500, and 2000 bar shows that the high pressure supercooled thermodynamic behavior of water is well described by TIP4P∕2005. Analysis of the tetrahedrality parameter Q reveals that the HDL-LDL structural transition is very sharp at 1000 bar, and that structural fluctuations become strongly coupled to density fluctuations upon approaching T(W). Furthermore, the tetrahedrality distribution becomes bimodal at ambient temperatures, an observation that possibly provides a link between HDL-LDL fluctuations and the structural bimodality in liquid water indicated by x-ray spectroscopic techniques. Computed x-ray absorption spectra are indeed found to show sensitivity to the tetrahedrality parameter.

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Liquid polymorphism: water in nanoconfined and biological environments

Cited by 53 publications

References 119 publications

Effect of hydrophobic environments on the hypothesized liquid-liquid critical point of water

Effect of hydrophobic environments on the hypothesized liquid-liquid critical point of water

Finite-size scaling investigation of the liquid-liquid critical point in ST2 water and its stability with respect to crystallization

Enhanced small-angle scattering connected to the Widom line in simulations of supercooled water

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