Self-sustaining crystallization of amorphous layers of water and heavy water

Koverda, V. P.; Bogdanov, N. M.; Skripov, V. P.

doi:10.1016/0022-3093(83)90054-6

Cited by 26 publications

(12 citation statements)

References 9 publications

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“…Specifically, broadband-dielectric spectroscopy has not been used before to study amorphous water. LDA was studied using this technique either at ambient pressure only for a few frequencies (30)(31)(32) or under high-pressure conditions (33). HDA has never been investigated dielectrically at ambient pressure, to our knowledge.…”

Section: Resultsmentioning

confidence: 99%

Water’s second glass transition

Amann‐Winkel

Gainaru

Handle

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

265

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The glassy states of water are of common interest as the majority of H 2 O in space is in the glassy state and especially because a proper description of this phenomenon is considered to be the key to our understanding why liquid water shows exceptional properties, different from all other liquids. The occurrence of water's calorimetric glass transition of low-density amorphous ice at 136 K has been discussed controversially for many years because its calorimetric signature is very feeble. Here, we report that high-density amorphous ice at ambient pressure shows a distinct calorimetric glass transitions at 116 K and present evidence that this second glass transition involves liquid-like translational mobility of water molecules. This "double T g scenario" is related to the coexistence of two liquid phases. The calorimetric signature of the second glass transition is much less feeble, with a heat capacity increase at T g,2 about five times as large as at T g,1 . By using broadband-dielectric spectroscopy we resolve loss peaks yielding relaxation times near 100 s at 126 K for low-density amorphous ice and at 110 K for high-density amorphous ice as signatures of these two distinct glass transitions. Temperature-dependent dielectric data and heating-rate-dependent calorimetric data allow us to construct the relaxation map for the two distinct phases of water and to extract fragility indices m = 14 for the low-density and m = 20-25 for the high-density liquid. Thus, low-density liquid is classified as the strongest of all liquids known ("superstrong"), and also high-density liquid is classified as a strong liquid.

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Section: Resultsmentioning

confidence: 99%

Water’s second glass transition

Amann‐Winkel

Gainaru

Handle

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

265

301

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“…The highest recorded T C values, 165 K by Olander and Rice [23] and 170 K by Koverda et al [24], were both obtained on films deposited from the dilute vapor phase. Olander and Rice carefully examined the relation between amorphous film properties and the ASW deposition rate, with the object of minimizing the possibility of generating crystallization nuclei during the deposition.…”

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confidence: 87%

“…For this system T g is invariant with composition, at 140 K [27,29]. [24,26], showing steady increases in loss up to the crystallization temperature where sudden decreases occurs. The break at 136 K, attributed to the glass transition by Koverda et al [24], is not reproduced in the study of Johari et al [26], nor is it supported by the present work on related glasses.…”

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confidence: 90%

“…Relaxation studies between VOLUME 93, NUMBER 21 P H Y S I C A L R E V I E W L E T T E R S The most precise method for studying relaxation in condensed phases at this time is dielectric spectroscopy, which has the exceptional ability to detect very small energy dissipations [25]. Koverda, Bogdanov, and Skripov (KBS) [24] and, more recently, Johari, Hallbrucker, and Mayer (JHM) [26] have applied the method to annealed amorphous water films, and their results, for temperature scanning at a fixed frequency of 1 kHz, are shown in Fig. 1.…”

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confidence: 99%

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Dielectric Studies Deny Existence of Ultraviscous Fragile Water

2004

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The glass transition, a relaxation phenomenon, sets the low temperature limit to the liquid state. Glassy water that forms only under extreme quenching conditions is unstable against crystallization. Opinions differ on whether the glass transition can be observed at all. Here we measure the dielectric tan(delta for easily glassforming waterlike aqueous solutions, H2O-H2O2 and H2O-N2H4, to characterize the behavior of such systems during passage through their glass transitions. All show unambiguous Tg values of 136-140 K, the value generally assigned to pure water. However, the behavior of epsilon''/epsilon' is quite different from that in amorphous water in the same temperature range. Our findings eliminate "ultraviscous fragile liquid" as a possible description of water between 136 K and crystallization, but leave "ultraviscous strong liquid" a possibility to be considered.

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“…These studies have focused on probing the crystallization of vapor-deposited LDA, commonly known as amorphous solid water ͑ASW͒, supported on a variety of substrates. [33][34][35][36][37][38][39][40][41] ͑Note that throughout this paper, for brevity we refer to this transformation as ''crystallization of ASW,'' although whether ASW crystallizes directly from the glassy state or first melts into a liquid is still debated.͒ In most studies, it was concluded that transformation proceeds via homogeneous nucleation and isotropic growth of crystallites, [33][34][35][36][37]39 although there was disagreement as to whether transfer of H 2 O molecules across a͒ Author to whom correspondence should be addressed. Electronic mail: mullins@che.utexas.edu the crystal-amorphous matrix interface 35,36,38,39 or longrange diffusion 33,34,37 controls the rate of grain growth.…”

Section: Introductionmentioning

confidence: 99%

Thickness dependent crystallization kinetics of sub-micron amorphous solid water films

Safarik

Meyer

Mullins

2003

The Journal of Chemical Physics

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The kinetics of isothermal crystallization at the free surface of dense, 150–1050 bilayer (BL) (∼55–385 nm) thick amorphous solid water (ASW) films is investigated experimentally, and a model accounting for the observed thickness dependence is proposed. We find that as the ASW film thickness is increased above 150 BL, surface crystallization accelerates, rapidly at first and then more slowly until essentially size-independent kinetics are attained by 1050 BL. The potential origin of this thickness dependence is elucidated by a geometrical model of surface crystallization that we formulated using mechanistic information deduced from available experimental data. This simple mean-field model predicts that as film thickness is reduced below some critical value, the number of grains contributing to surface transformation progressively decreases, forcing each grain to convert a larger surface area and thus slowing crystallization. Good agreement between experimental data and the theory is realized using only two thickness-independent kinetic parameters (per temperature), suggesting that the model describes the basic physics of crystallization in these ASW films. Nucleation and growth rates determined via model fits range from ∼5.5×109 cm−3 s−1 and ∼0.3 Å/s at 136 K to ∼6.5×1010 cm−3 s−1 and ∼1.5 Å/s at 140 K, corresponding to activation energies of 100 and 68 kJ/mol, respectively.

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Self-sustaining crystallization of amorphous layers of water and heavy water

Cited by 26 publications

References 9 publications

Water’s second glass transition

Water’s second glass transition

Dielectric Studies Deny Existence of Ultraviscous Fragile Water

Thickness dependent crystallization kinetics of sub-micron amorphous solid water films

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