Evolution of the structure of amorphous ice: From low-density amorphous through high-density amorphous to very high-density amorphous ice

Martoňák, Roman; Donadio, Davide; Parrinello, Michele

doi:10.1063/1.1870852

Cited by 87 publications

(96 citation statements)

References 62 publications

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“…However, the topological differences in the underlying hydrogen bond networks observed here is striking and consistent with the presence of a first-order phase boundary between the amorphous phases of ice, as noted in Ref. 100,101 . Furthermore, this finding complements the distinctive features of HDA and LDA observed via the g OO (r) above.…”

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid supporting

confidence: 59%

“…All P(N ) were normalized to unity and therefore do not reflect the total number of rings of a given size. P(N ) of low-and high-density-like clusters bears strong similarities with those found for the LDA and HDA ice phases 100,101 . Instead of a predominance of N = 6 membered rings, as expected in the structures of LDA 100,101 , we found that the largest majority of rings contain N = 5 members with significantly large populations of smaller rings among the high-and low-density-like water molecules in the IPES of ambient liquid water.…”

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid supporting

confidence: 48%

“…In the case of LDA, which is more ordered, one finds a narrower distribution of rings centered about the most predominant six-membered ring, whereas in the case of HDA, which is more disordered, one finds a much broader distribution of rings with a substantial population having more than six members. In fact, the existence of larger rings provides a pathway of having more compact and disordered packing of water molecules in the amorphous ice and liquid phases of water 100,101 . Here, we have used a geometric definition of intact hydrogen bonds 102 in conjunction with the criteria of King 103 to find the shortest-path closed rings containing N members among water molecules characterized by I > I min only and I < I min only, and computed the resultant normalized probability distributions, P(N ), depicted in Figure 5(c).…”

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid mentioning

confidence: 99%

“…These differential topologies can be quantified using ring statistics analysis-a tool which has been instrumental in theoretically characterizing and delineating the evolution of the HDA and LDA phases 100,101 . In the case of LDA, which is more ordered, one finds a narrower distribution of rings centered about the most predominant six-membered ring, whereas in the case of HDA, which is more disordered, one finds a much broader distribution of rings with a substantial population having more than six members.…”

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid mentioning

confidence: 99%

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Local structure analysis in ab initio liquid water

et al. 2015

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Within the framework of density functional theory, the inclusion of exact exchange and non-local van der Waals/dispersion (vdW) interactions is crucial for predicting a microscopic structure of ambient liquid water that quantitatively agrees with experiment. In this work, we have used the local structure index (LSI) order parameter to analyze the local structure in such highly accurate ab initio liquid water. At ambient conditions, the LSI probability distribution, P(I), was unimodal with most water molecules characterized by more disordered high-density-like local environments. With thermal excitations removed, the resultant bimodal P(I) in the inherent potential energy surface (IPES) exhibited a 3:1 ratio between high-and low-density-like molecules, with the latter forming small connected clusters amid the predominant population. By considering the spatial correlations and hydrogen bond network topologies among water molecules with the same LSI identities, we demonstrate that the signatures of the experimentally observed low-(LDA) and highdensity (HDA) amorphous phases of ice are present in the IPES of ambient liquid water. Analysis of the LSI autocorrelation function uncovered a persistence time of ∼ 4 ps-a finding consistent with the fact that natural thermal fluctuations are responsible for transitions between these distinct yet transient local aqueous environments in ambient liquid water.

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Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid supporting

confidence: 59%

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid supporting

confidence: 48%

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid mentioning

confidence: 99%

Section: Signature Of Polyamorphism In the Ipes Of Ambient Liquid mentioning

confidence: 99%

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Local structure analysis in ab initio liquid water

et al. 2015

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“…Both ice 0 and ice i are significantly more stable (∼40 meV/molecule at the PBESOL-D3 level, configuration taken from Ref. 46) than low density amorphous ice, which is of comparable density to ice 0 and ice i, suggesting that ordered structures may be more effective at mediating the nucleation of ice I h . …”

Section: Discussionmentioning

confidence: 99%

Communication: On the stability of ice 0, ice i, and Ih

Quigley

Slater

2014

The Journal of Chemical Physics

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Using ab initio methods, we examine the stability of ice 0, a recently proposed tetragonal form of ice implicated in the homogeneous freezing of water [J. Russo, F. Romano, and H. Tanaka, Nat. Mater. 13, 670 (2014)]. Vibrational frequencies are computed across the complete Brillouin Zone using Density Functional Theory (DFT), to confirm mechanical stability and quantify the free energy of ice 0 relative to ice I h . The robustness of this result is tested via dispersion corrected semi-local and hybrid DFT, and Quantum Monte-Carlo calculation of lattice energies. Results indicate that popular molecular models only slightly overestimate the stability of ice zero. In addition, we study all possible realisations of proton disorder within the ice zero unit cell, and identify the ground state as ferroelectric. Comparisons are made to other low density metastable forms of ice, suggesting that the ice i structure [C. J. Fennel and J. D. Gezelter, J. Chem. Theory Comput.

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