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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. However the results are consistent with a previous prediction for D(T) that assumed no thermodynamic transitions occur in “no man’s land.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. BATTELLE (PACIFIC NW LAB)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1512076
Report Number(s):
PNNL-SA-119195
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal 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
Country of Publication:
United States
Language:
English

Citation Formats

Xu, Yuntao, Petrik, Nikolay G., Smith, Ronald S., Kay, Bruce D., and Kimmel, Gregory 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, Ronald S., Kay, Bruce D., & Kimmel, Gregory 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, Ronald S., Kay, Bruce D., and Kimmel, Gregory A. Tue . "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_1512076,
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, Ronald S. and Kay, Bruce D. and Kimmel, Gregory 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. However 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 = {2016},
month = {12}
}

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