Communication: On the stability of ice 0, ice i, and I<i>h</i>

Quigley, David; Slater, Ben

doi:10.1063/1.4900772

Cited by 29 publications

(30 citation statements)

References 51 publications

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“…[209], where a novel metastable phase was identified, called Ice 0, with a tetragonal unit cell with 12 molecules, whose thermodynamic and structural properties are intermediate between the melt and the solid crystalline phase. The thermodynamic stability of the new phase was originally demonstrated for mW and TIP4P/2005 models of water [209], and additional density functional calculations have confirmed that, among the known metastable ice phases, Ice 0 has the closest free energy to that of stable ice I [240,241].…”

Section: Local Structural Ordering and Homogeneous Crystal Nucleationmentioning

confidence: 99%

Crystal nucleation as the ordering of multiple order parameters

Russo

Tanaka

2016

The Journal of Chemical Physics

107

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Nucleation is an activated process in which the system has to overcome a free energy barrier in order for a first-order phase transition between the metastable and the stable phases to take place. In the liquid-to-solid transition the process occurs between phases of different symmetry, and it is thus inherently a multi-dimensional process, in which all symmetries are broken at the transition. In this Focus Article, we consider some recent studies which highlight the multi-dimensional nature of the nucleation process. Even for a single-component system, the formation of solid crystals from the metastable melt involves fluctuations of two (or more) order parameters, often associated with the decoupling of positional and orientational symmetry breaking. In other words, we need at least two order parameters to describe the free-energy of a system including its liquid and crystalline states. This decoupling occurs naturally for asymmetric particles or directional interactions, focusing here on the case of water, but we will show that it also affects spherically symmetric interacting particles, such as the hard-sphere system. We will show how the treatment of nucleation as a multi-dimensional process has shed new light on the process of polymorph selection, on the effect of external fields on the nucleation process, and on glass-forming ability.

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Section: Local Structural Ordering and Homogeneous Crystal Nucleationmentioning

confidence: 99%

Crystal nucleation as the ordering of multiple order parameters

Russo

Tanaka

2016

The Journal of Chemical Physics

107

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“…28 Both DMC and LRDMC provide excellent benchmark values for weakly interacting systems, as established in a number of studies. [29][30][31][32][33][34][35][36]39,58,59 We used here a standard setup, described in detail in the Supporting Information. The stochastic error associated with the QMC evaluations of the adsorption energy is ca.…”

Section: Qmc Calculationsmentioning

confidence: 99%

“…120 The Jas- been assessed in previous studies. [29][30][31][32][33][34][35][36]39,58,59 This choice of the complex-minus-far method is explained by two considerations: (i) DMC calculations (as well as any many-body electronic structure method) are affected by size-effects due to the periodicity of the system that are much larger that those of DFT, and they are sizeable also in the big supercells considered here; complex-minus-fragments method is instead much more affected by the finite time-step bias, so it would require a τ that is at least one order of magnitude smaller.…”

Section: S1 Dmc Setupmentioning

confidence: 99%

Toward Accurate Adsorption Energetics on Clay Surfaces

et al. 2016

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Clay minerals are ubiquitous in nature, and the manner in which they interact with their surroundings has important industrial and environmental implications. Consequently, a molecular-level understanding of the adsorption of molecules on clay surfaces is crucial. In this regard computer simulations play an important role, yet the accuracy of widely used empirical force fields (FF) and density functional theory (DFT) exchange-correlation functionals is often unclear in adsorption systems dominated by weak interactions. Herein we present results from quantum Monte Carlo (QMC) for water and methanol adsorption on the prototypical clay kaolinite. To the best of our knowledge, this is the first time QMC has been used to investigate adsorption at a complex, natural surface such as a clay. As well as being valuable in their own right, the QMC benchmarks obtained provide reference data against which the performance of cheaper DFT methods can be tested. Indeed using various DFT exchange-correlation functionals yields a very broad range of adsorption energies, and it is unclear a priori which evaluation is better. QMC reveals that in the systems considered here it is essential to account for van der Waals (vdW) dispersion forces since this alters both the absolute and relative adsorption energies of water and methanol. We show, via FF simulations, that incorrect relative energies can lead to significant changes in the interfacial densities of water and methanol solutions at the kaolinite interface. Despite the clear improvements offered by the vdW-corrected and the vdW-inclusive functionals, absolute adsorption energies are often overestimated, suggesting that the treatment of vdW forces in DFT is not yet a solved problem.

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“…The recent theoretical studies of water freezing stated the emergence of ferroelectric ice named ice 0, which may be formed only from supercooled water, followed by formation of ice Ih or Ic [18,19]. This process may take place, according to the cited studies, at temperatures below −23 • C. Previously the rise of ε s at the temperature below −37 • C was discovered for water in silicate material MCM-41 with cylindrical pores [36] at low frequencies of the order of 10 Hz.…”

Section: Discussion Of Resultsmentioning

confidence: 99%

Analysis of Loss Factor of Supercooled Pore Water at Frequencies of 60–140 GHz

Bordonskii

Orlov

Krylov

2019

J. Commun. Technol. Electron.

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The loss factor of supercooled water at the frequencies 11 . . . 180 GHz has been measured. A measuring technique has been proposed, in which wetted nanoporous silicate materials, silica gels, with the mean diameter of the pores being 6 − 9 nm, were used to obtain deeply supercooled water. Results have been obtained for the loss factor of supercooled water, close to volume water for its properties, when cooled down to −45 • C. To ascertain the mechanism of pore water losses, measurements have been made in the range of temperatures 0 . . . − 90 • C. The results obtained have demonstrated the existence of significant excessive losses at the temperatures below −30 • C, compared to the results of computations based on the known models. To allow mathematical description of the increment loss factor, a new addend has been introduced as a sum of two Gaussian functions in the formula described in [T. Meissner, F. J. Wentz, IEEE Trans. Geosci. Remote Sens. 2004. vol. 42, p. 1836. One of these functions has the extremum near −45 • C, and the second one has the extremum in the range of −60 . . . − 70 • C. Additional attenuation at −45 • C is supposed to be connected with the second critical point of water. Attenuation with the center in the range of temperatures −60 . . . − 70 • C is determined by the emergence of conductive films at the boundary between the hard matrix and ferroelectric ice 0. This modification is a transitional form to ice Ih or ice Ic and is formed at the temperature below −23 • C.

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

Cited by 29 publications

References 51 publications

Crystal nucleation as the ordering of multiple order parameters

Crystal nucleation as the ordering of multiple order parameters

Toward Accurate Adsorption Energetics on Clay Surfaces

Analysis of Loss Factor of Supercooled Pore Water at Frequencies of 60–140 GHz

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