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

Abstract

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:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1335529
Alternate Identifier(s):
OSTI ID: 1344658
Report Number(s):
PNNL-SA-119195
Journal ID: ISSN 0027-8424; KC0301050
Grant/Contract Number:  
AC05-76RL01830; KC0301050-16248
Resource Type:
Journal Article: 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)
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

Citation Formats

Xu, Yuntao, Petrik, Nikolay G., Smith, R. Scott, Kay, Bruce D., and Kimmel, Greg A. Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K. United States: N. p., 2016. Web. doi:10.1073/pnas.1611395114.
Xu, Yuntao, Petrik, Nikolay G., Smith, R. Scott, Kay, Bruce D., & Kimmel, Greg A. Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K. United States. doi:10.1073/pnas.1611395114.
Xu, Yuntao, Petrik, Nikolay G., Smith, R. Scott, Kay, Bruce D., and Kimmel, Greg A. Mon . "Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K". United States. doi:10.1073/pnas.1611395114.
@article{osti_1335529,
title = {Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K},
author = {Xu, Yuntao and Petrik, Nikolay G. and Smith, R. Scott and Kay, Bruce D. and Kimmel, Greg A.},
abstractNote = {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.},
doi = {10.1073/pnas.1611395114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 52,
volume = 113,
place = {United States},
year = {Mon Dec 12 00:00:00 EST 2016},
month = {Mon Dec 12 00:00:00 EST 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1073/pnas.1611395114

Citation Metrics:
Cited by: 13 works
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Works referenced in this record:

Kinetics of Phase Change. I General Theory
journal, December 1939

  • Avrami, Melvin
  • The Journal of Chemical Physics, Vol. 7, Issue 12, p. 1103-1112
  • DOI: 10.1063/1.1750380