Supercooled water survives in no-man’s-land

Physics Today ◽  
2017 ◽  
2017 ◽  
Vol 1 (4) ◽  
pp. 187-196 ◽  
Author(s):  
Prithwish K. Nandi ◽  
Christian J. Burnham ◽  
Zdenek Futera ◽  
Niall J. English

2021 ◽  
Vol 118 (14) ◽  
pp. e2022884118
Author(s):  
Loni Kringle ◽  
Wyatt A. Thornley ◽  
Bruce D. Kay ◽  
Greg A. Kimmel

The origin of water’s anomalous properties has been debated for decades. Resolution of the problem is hindered by a lack of experimental data in a crucial region of temperatures, T, and pressures where supercooled water rapidly crystallizes—a region often referred to as “no man’s land.” A recently developed technique where water is heated and cooled at rates greater than 109 K/s now enables experiments in this region. Here, it is used to investigate the structural relaxation and crystallization of deeply supercooled water for 170 K < T < 260 K. Water’s relaxation toward a new equilibrium structure depends on its initial structure with hyperquenched glassy water (HQW) typically relaxing more quickly than low-density amorphous solid water (LDA). For HQW and T > 230 K, simple exponential relaxation kinetics is observed. For HQW at lower temperatures, increasingly nonexponential relaxation is observed, which is consistent with the dynamics expected on a rough potential energy landscape. For LDA, approximately exponential relaxation is observed for T > 230 K and T < 200 K, with nonexponential relaxation only at intermediate temperatures. At all temperatures, water’s structure can be reproduced by a linear combination of two, local structural motifs, and we show that a simple model accounts for the complex kinetics within this context. The relaxation time, τrel, is always shorter than the crystallization time, τxtal. For HQW, the ratio, τxtal/τrel, goes through a minimum at ∼198 K where the ratio is about 60.


2016 ◽  
Vol 113 (52) ◽  
pp. 14921-14925 ◽  
Author(s):  
Yuntao Xu ◽  
Nikolay G. Petrik ◽  
R. Scott Smith ◽  
Bruce D. Kay ◽  
Greg A. Kimmel

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.


Physics Today ◽  
2017 ◽  
Vol 70 (2) ◽  
pp. 18-21 ◽  
Author(s):  
Ashley G. Smart

1998 ◽  
Vol 08 (PR6) ◽  
pp. Pr6-109-Pr6-113
Author(s):  
P. Gallo ◽  
F. Sciortino ◽  
P. Tartaglia ◽  
S.-H. Chen

Author(s):  
A. Danison ◽  
J. Boddu ◽  
J. Rostron ◽  
J. Hamilton
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