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Title: Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K

Understanding deeply supercooled water is key to unraveling many of water’s anomalous properties. However, this 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, i.e. deep within water’s “no man’s land.” 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, G( T) and D( T) have super-Arrhenius (“fragile”) temperature dependences, but both crossover 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. Furthermore the results are consistent with a previous prediction for D(T) that assumed no thermodynamic transitions occur in “no man’s land.
Authors:
 [1] ; ORCiD logo [1] ;  [1] ;  [1] ; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-119195
Journal ID: ISSN 0027-8424; KC0301050
Grant/Contract Number:
AC05-76RL01830; KC0301050-16248
Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 113; Journal Issue: 52; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; supercooled water; self-diffusion; crystallization kinetics; dynamic crossover
OSTI Identifier:
1335529
Alternate Identifier(s):
OSTI ID: 1344658