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Title: Nanosecond Freezing of Water at High Pressures: Nucleation and Growth near the Metastability Limit

The fundamental study of phase transition kinetics has motivated experimental methods toward achieving the largest degree of undercooling possible, more recently culminating in the technique of rapid, quasi-isentropic compression. This approach has been demonstrated to freeze water into the high-pressure ice VII phase on nanosecond timescales, with some experiments undergoing heterogeneous nucleation while others, in apparent contradiction, suggest a homogeneous nucleation mode. We show through a combination of theory, simulation, and analysis of experiments that these seemingly contradictory results are in agreement when viewed from the perspective of classical nucleation theory. We find that, perhaps surprisingly, classical nucleation theory is capable of accurately predicting the solidification kinetics of ice VII formation under an extremely high driving force ( | Δ μ / k B T | 1 ) but only if amended by two important considerations: (i) transient nucleation and (ii) separate liquid and solid temperatures. Finally, this is the first demonstration of a model that is able to reproduce the experimentally observed rapid freezing kinetics.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Report Number(s):
LLNL-JRNL-749524
Journal ID: ISSN 0031-9007; 934727
Grant/Contract Number:
AC52-07NA27344
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 15; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; classical transport; interface & surface thermodynamics; nucleation; thermodynamics; finite-element method
OSTI Identifier:
1477944
Alternate Identifier(s):
OSTI ID: 1477545

Myint, Philip C., Chernov, Alexander A., Sadigh, Babak, Benedict, Lorin X., Hall, Burl M., Hamel, Sebastien, and Belof, Jonathan L.. Nanosecond Freezing of Water at High Pressures: Nucleation and Growth near the Metastability Limit. United States: N. p., Web. doi:10.1103/PhysRevLett.121.155701.
Myint, Philip C., Chernov, Alexander A., Sadigh, Babak, Benedict, Lorin X., Hall, Burl M., Hamel, Sebastien, & Belof, Jonathan L.. Nanosecond Freezing of Water at High Pressures: Nucleation and Growth near the Metastability Limit. United States. doi:10.1103/PhysRevLett.121.155701.
Myint, Philip C., Chernov, Alexander A., Sadigh, Babak, Benedict, Lorin X., Hall, Burl M., Hamel, Sebastien, and Belof, Jonathan L.. 2018. "Nanosecond Freezing of Water at High Pressures: Nucleation and Growth near the Metastability Limit". United States. doi:10.1103/PhysRevLett.121.155701.
@article{osti_1477944,
title = {Nanosecond Freezing of Water at High Pressures: Nucleation and Growth near the Metastability Limit},
author = {Myint, Philip C. and Chernov, Alexander A. and Sadigh, Babak and Benedict, Lorin X. and Hall, Burl M. and Hamel, Sebastien and Belof, Jonathan L.},
abstractNote = {The fundamental study of phase transition kinetics has motivated experimental methods toward achieving the largest degree of undercooling possible, more recently culminating in the technique of rapid, quasi-isentropic compression. This approach has been demonstrated to freeze water into the high-pressure ice VII phase on nanosecond timescales, with some experiments undergoing heterogeneous nucleation while others, in apparent contradiction, suggest a homogeneous nucleation mode. We show through a combination of theory, simulation, and analysis of experiments that these seemingly contradictory results are in agreement when viewed from the perspective of classical nucleation theory. We find that, perhaps surprisingly, classical nucleation theory is capable of accurately predicting the solidification kinetics of ice VII formation under an extremely high driving force (|Δμ/kBT|≈1) but only if amended by two important considerations: (i) transient nucleation and (ii) separate liquid and solid temperatures. Finally, this is the first demonstration of a model that is able to reproduce the experimentally observed rapid freezing kinetics.},
doi = {10.1103/PhysRevLett.121.155701},
journal = {Physical Review Letters},
number = 15,
volume = 121,
place = {United States},
year = {2018},
month = {10}
}

Works referenced in this record:

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journal, September 2001
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Kinetics of Phase Change. I General Theory
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