| Literature DB >> 27956609 |
Yuntao Xu1, Nikolay G Petrik1, R Scott Smith1, Bruce D Kay2, Greg A Kimmel2.
Abstract
Understanding deeply supercooled water is key to unraveling many of water's anomalous properties. However, developing this understanding has proven difficult due to rapid and uncontrolled crystallization. Using a pulsed-laser-heating technique, we measure the growth rate of crystalline ice, G(T), for 180 K < T < 262 K, that is, deep within water's "no man's land" in ultrahigh-vacuum conditions. Isothermal measurements of G(T) are also made for 126 K ≤ T ≤ 151 K. The self-diffusion of supercooled liquid water, D(T), is obtained from G(T) using the Wilson-Frenkel model of crystal growth. For T > 237 K and P ∼ 10-8 Pa, G(T) and D(T) have super-Arrhenius ("fragile") temperature dependences, but both cross over to Arrhenius ("strong") behavior with a large activation energy in no man's land. The fact that G(T) and D(T) are smoothly varying rules out the hypothesis that liquid water's properties have a singularity at or near 228 K at ambient pressures. However, the results are consistent with a previous prediction for D(T) that assumed no thermodynamic transitions occur in no man's land.Entities:
Keywords: crystallization kinetics; dynamic crossover; self-diffusion; supercooled water
Year: 2016 PMID: 27956609 PMCID: PMC5206540 DOI: 10.1073/pnas.1611395114
Source DB: PubMed Journal: Proc Natl Acad Sci U S A ISSN: 0027-8424 Impact factor: 11.205