2015
DOI: 10.1073/pnas.1510256112
|View full text |Cite
|
Sign up to set email alerts
|

Glass-to-cryogenic-liquid transitions in aqueous solutions suggested by crack healing

Abstract: Observation of theorized glass-to-liquid transitions between lowdensity amorphous (LDA) and high-density amorphous (HDA) water states had been stymied by rapid crystallization below the homogeneous water nucleation temperature (∼235 K at 0.1 MPa). We report optical and X-ray observations suggestive of glass-toliquid transitions in these states. Crack healing, indicative of liquid, occurs when LDA ice transforms to cubic ice at 160 K, and when HDA ice transforms to the LDA state at temperatures as low as 120 K.… Show more

Help me understand this report

Search citation statements

Order By: Relevance

Paper Sections

Select...
4

Citation Types

2
12
0

Year Published

2016
2016
2019
2019

Publication Types

Select...
6

Relationship

0
6

Authors

Journals

citations
Cited by 10 publications
(14 citation statements)
references
References 51 publications
2
12
0
Order By: Relevance
“…The HDA-to-LDA transition has been proposed to be a first-order phase transition (4)(5)(6)(7)(8) and could occur in the ultraviscous liquid state at temperatures above the glass transition (9). Similar observations have been reported by studying water confined in protein crystals and aqueous solutions (10,11), which indicate the occurrence of the transition between two viscous liquid states of water. However, there is contradicting evidence that the transition from HDA to LDA involves several intermediate forms (12,13) and it is questioned whether the amorphous ices are thermodynamically linked with supercooled water (14,15).…”
supporting
confidence: 63%
“…The HDA-to-LDA transition has been proposed to be a first-order phase transition (4)(5)(6)(7)(8) and could occur in the ultraviscous liquid state at temperatures above the glass transition (9). Similar observations have been reported by studying water confined in protein crystals and aqueous solutions (10,11), which indicate the occurrence of the transition between two viscous liquid states of water. However, there is contradicting evidence that the transition from HDA to LDA involves several intermediate forms (12,13) and it is questioned whether the amorphous ices are thermodynamically linked with supercooled water (14,15).…”
supporting
confidence: 63%
“…By contrast, samples vitrified at ambient pressure do not show crack healing until the LDA water crystallizes. 281 As crack healing requires rather high molecular mobility this strongly reinforces the argument that HDA turns into a mobile liquid at 120 K while LDA turns into a mobile liquid just before crystallization near 150 K. [90][91][92][93] This is consistent with calorimetric glass transition temperatures for HDA 83 and LDA. 100 Unexpectedly, the amorphous solutions do not crystallize to ice I but rather to host-guest compounds (type I clathrates) in which the tartrate is trapped in ice cages.…”
Section: Other Salt Solutionssupporting
confidence: 68%
“…The mobility of water molecules at the polyamorphic transition was further probed in pressure-vitrified sodium potassium tartrate solution 278 by manually cracking the frozen phase and monitoring its evolution. 281 The cracks persist as long as water is in the HDA state but crack healing is observed once the HDA -LDA transition is induced upon heating at E120 K and 1 bar. By contrast, samples vitrified at ambient pressure do not show crack healing until the LDA water crystallizes.…”
Section: Other Salt Solutionsmentioning
confidence: 99%
See 2 more Smart Citations