Structural relaxation and crystallization in supercooled water from 170 to 260 K
Abstract
The structural relaxation and crystallization of deeply supercooled water are investigated in transiently-heated nanoscale water films using infrared spectroscopy for temperatures between 170 and 260 K. For temperatures above ~230 K, the relaxation kinetics can be fit with a simple exponential decay which is characteristic of normal liquids. At lower temperatures, increasingly non-exponential decay is observed indicating the onset of heterogeneous dynamics. Water’s relaxation rate depends on its initial structure with hyper-quenched glassy water (HQW) typically relaxing more quickly than low-density amorphous solid water (LDA). At all temperatures, the relaxation time, trel is faster than the crystallization time, txtal. For HQW, the ratio, txtal/trel, goes through a minimum at ~198 K where it is about 60. The research was designed and supervised by GAK and BDK. LK and WAT conducted the experiments and analyzed the data. LK and GAK wrote the manuscript, with input from all authors.
- Authors:
-
- BATTELLE (PACIFIC NW LAB)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1797429
- Report Number(s):
- PNNL-SA-158074
- 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: 118; Journal Issue: 14
- Country of Publication:
- United States
- Language:
- English
Citation Formats
Kringle, Loni M., Thornley, Wyatt A., Kay, Bruce D., and Kimmel, Gregory A. Structural relaxation and crystallization in supercooled water from 170 to 260 K. United States: N. p., 2021.
Web. doi:10.1073/pnas.2022884118.
Kringle, Loni M., Thornley, Wyatt A., Kay, Bruce D., & Kimmel, Gregory A. Structural relaxation and crystallization in supercooled water from 170 to 260 K. United States. https://doi.org/10.1073/pnas.2022884118
Kringle, Loni M., Thornley, Wyatt A., Kay, Bruce D., and Kimmel, Gregory A. 2021.
"Structural relaxation and crystallization in supercooled water from 170 to 260 K". United States. https://doi.org/10.1073/pnas.2022884118.
@article{osti_1797429,
title = {Structural relaxation and crystallization in supercooled water from 170 to 260 K},
author = {Kringle, Loni M. and Thornley, Wyatt A. and Kay, Bruce D. and Kimmel, Gregory A.},
abstractNote = {The structural relaxation and crystallization of deeply supercooled water are investigated in transiently-heated nanoscale water films using infrared spectroscopy for temperatures between 170 and 260 K. For temperatures above ~230 K, the relaxation kinetics can be fit with a simple exponential decay which is characteristic of normal liquids. At lower temperatures, increasingly non-exponential decay is observed indicating the onset of heterogeneous dynamics. Water’s relaxation rate depends on its initial structure with hyper-quenched glassy water (HQW) typically relaxing more quickly than low-density amorphous solid water (LDA). At all temperatures, the relaxation time, trel is faster than the crystallization time, txtal. For HQW, the ratio, txtal/trel, goes through a minimum at ~198 K where it is about 60. The research was designed and supervised by GAK and BDK. LK and WAT conducted the experiments and analyzed the data. LK and GAK wrote the manuscript, with input from all authors.},
doi = {10.1073/pnas.2022884118},
url = {https://www.osti.gov/biblio/1797429},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 14,
volume = 118,
place = {United States},
year = {Tue Apr 06 00:00:00 EDT 2021},
month = {Tue Apr 06 00:00:00 EDT 2021}
}
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