Structural order in glassy water

Giovambattista, Nicolás; Debenedetti, Pablo G.; Sciortino, Francesco; Stanley, H. Eugene

doi:10.1103/physreve.71.061505

Cited by 68 publications

(86 citation statements)

References 60 publications

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“…4 and 10); computer simulation studies of glassy water are comparatively more limited. To our knowledge, only a few fullatom water models have been employed in computational studies of glassy water: the TIP4P, [29][30][31] SPC/E, [32][33][34][35][36] and ST2 model. 24,29,37,38 As is the case in the liquid state, these models have limitations in reproducing experimental data.…”

Section: Introductionmentioning

confidence: 99%

Heating-induced glass-glass and glass-liquid transformations in computer simulations of water

Chiu

Starr

Giovambattista

2014

The Journal of Chemical Physics

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Water exists in at least two families of glassy states, broadly categorized as the low-density (LDA) and high-density amorphous ice (HDA). Remarkably, LDA and HDA can be reversibly interconverted via appropriate thermodynamic paths, such as isothermal compression and isobaric heating, exhibiting first-order-like phase transitions. We perform out-of-equilibrium molecular dynamics simulations of glassy water using the ST2 model to study the evolution of LDA and HDA upon isobaric heating. Depending on pressure, glass-to-glass, glass-to-crystal, glass-to-vapor, as well as glass-to-liquid transformations are found. Specifically, heating LDA results in the following transformations, with increasing heating pressures: (i) LDA-to-vapor (sublimation), (ii) LDA-to-liquid (glass transition), (iii) LDA-to-HDA-to-liquid, (iv) LDA-to-HDA-to-liquid-to-crystal, and (v) LDAto-HDA-to-crystal. Similarly, heating HDA results in the following transformations, with decreasing heating pressures: (a) HDA-to-crystal, (b) HDA-to-liquid-to-crystal, (c) HDA-to-liquid (glass transition), (d) HDA-to-LDA-to-liquid, and (e) HDA-to-LDA-to-vapor. A more complex sequence may be possible using lower heating rates. For each of these transformations, we determine the corresponding transformation temperature as function of pressure, and provide a P-T "phase diagram" for glassy water based on isobaric heating. Our results for isobaric heating dovetail with the LDA-HDA transformations reported for ST2 glassy water based on isothermal compression/decompression processes [Chiu et al., J. Chem. Phys. 139, 184504 (2013)]. The resulting phase diagram is consistent with the liquid-liquid phase transition hypothesis. At the same time, the glass phase diagram is sensitive to sample preparation, such as heating or compression rates. Interestingly, at least for the rates explored, our results suggest that the LDA-to-liquid (HDA-to-liquid) and LDA-to-HDA (HDA-to-LDA) transformation lines on heating are related, both being associated with the limit of kinetic stability of LDA (HDA).

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Section: Introductionmentioning

confidence: 99%

Heating-induced glass-glass and glass-liquid transformations in computer simulations of water

Chiu

Starr

Giovambattista

2014

The Journal of Chemical Physics

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“…For comparison, we note that in the SPC/E model, the tetrahedral order for LDA (or, more precisely, HGW) and HDA at T = 77 K are, respectively, 0.82−0.84 (at −500 ≤ P ≤ 400 MPa and 0.9 ≤ ρ ≤ 1.0 g/cm 3 ) and 0.67 − 0.70 (at 1400 ≤ P ≤ 2200 MPa and 1.3 ≤ ρ ≤ 1.4 g/cm 3 ). 49 The distribution of tetrahedral order parameter for the individual molecules, P(q), during the LDA-HDA compression cycle at T = 80 K is shown in Fig. 7 for selected pressures.…”

Section: B Structure Of Lda and Hdamentioning

confidence: 99%

Pressure-induced transformations in computer simulations of glassy water

Chiu

Starr

Giovambattista

2013

The Journal of Chemical Physics

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Glassy water occurs in at least two broad categories: low-density amorphous (LDA) and highdensity amorphous (HDA) solid water. We perform out-of-equilibrium molecular dynamics simulations to study the transformations of glassy water using the ST2 model. Specifically, we study the known (i) compression-induced LDA-to-HDA, (ii) decompression-induced HDA-to-LDA, and (iii) compression-induced hexagonal ice-to-HDA transformations. We study each transformation for a broad range of compression/decompression temperatures, enabling us to construct a "P-T phase diagram" for glassy water. The resulting phase diagram shows the same qualitative features reported from experiments. While many simulations have probed the liquid-state phase behavior, comparatively little work has examined the transitions of glassy water. We examine how the glass transformations relate to the (first-order) liquid-liquid phase transition previously reported for this model. Specifically, our results support the hypothesis that the liquid-liquid spinodal lines, between a lowdensity and high-density liquid, are extensions of the LDA-HDA transformation lines in the limit of slow compression. Extending decompression runs to negative pressures, we locate the sublimation lines for both LDA and hyperquenched glassy water (HGW), and find that HGW is relatively more stable to the vapor. Additionally, we observe spontaneous crystallization of HDA at high pressure to ice VII. Experiments have also seen crystallization of HDA, but to ice XII. Finally, we contrast the structure of LDA and HDA for the ST2 model with experiments. We find that while the radial distribution functions (RDFs) of LDA are similar to those observed in experiments, considerable differences exist between the HDA RDFs of ST2 water and experiment. The differences in HDA structure, as well as the formation of ice VII (a tetrahedral crystal), are a consequence of ST2 overemphasizing the tetrahedral character of water. © 2013 AIP Publishing LLC.

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“…This is because the presence of GM1 makes water to be interfacial up to 16 Å. Compared to TIP3P water model, the computed q values are little bit higher than those reported earlier [64][65][66] which may be due to the presence of lipid bilayer. This is supported by the plot showing the average water-water hydrogen bonds and waterlipid hydrogen bonds per water molecule at different distance from the P atom of the bilayer along Z axis in the three systems (Fig.…”

Section: Structure Of Watermentioning

confidence: 43%

Insights into the behavioral difference of water in the presence of GM1

2015

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Edited by A. ChattopadhyayKeywords: GM1 Rough surface Behavioral difference of water Structure Dynamic Delayed convergence of interfacial property to bulk property a b s t r a c t Studies on the structure and dynamics of interfacial water, emphasizing on the properties of water near the surface of biomolecules, are well reported, but there is a lack of evidence on the behavior of water near a comparatively rough surface containing molecules with a bulky head group like GM1.In this report we comparatively analyze the structure and dynamics of water as a function of distance from the lipid head group in GM1 containing lipid bilayers, with the lipid bilayers where GM1 is not present. This approach effectively demonstrates the behavioral difference and hence delayed convergence from bound water to bulk water in the presence of GM1 compared to a relatively smooth surface.

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Structural order in glassy water

Cited by 68 publications

References 60 publications

Heating-induced glass-glass and glass-liquid transformations in computer simulations of water

Heating-induced glass-glass and glass-liquid transformations in computer simulations of water

Pressure-induced transformations in computer simulations of glassy water

Insights into the behavioral difference of water in the presence of GM1

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