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.
Kringle, Loni M., et al. "Structural relaxation and crystallization in supercooled water from 170 to 260 K." Proceedings of the National Academy of Sciences of the United States of America, vol. 118, no. 14, Apr. 2021. https://doi.org/10.1073/pnas.2022884118
Kringle, Loni M., Thornley, Wyatt A., Kay, Bruce D., & Kimmel, Gregory A. (2021). Structural relaxation and crystallization in supercooled water from 170 to 260 K. Proceedings of the National Academy of Sciences of the United States of America, 118(14). https://doi.org/10.1073/pnas.2022884118
Kringle, Loni M., Thornley, Wyatt A., Kay, Bruce D., et al., "Structural relaxation and crystallization in supercooled water from 170 to 260 K," Proceedings of the National Academy of Sciences of the United States of America 118, no. 14 (2021), https://doi.org/10.1073/pnas.2022884118
@article{osti_1797429,
author = {Kringle, Loni M. and Thornley, Wyatt A. and Kay, Bruce D. and Kimmel, Gregory A.},
title = {Structural relaxation and crystallization in supercooled water from 170 to 260 K},
annote = {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 = {2021},
month = {04}}
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1797429
Report Number(s):
PNNL-SA-158074
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 14 Vol. 118
Stanley, H. Eugene; Buldyrev, Sergey V.; Franzese, Giancarlo
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 363, Issue 1827https://doi.org/10.1098/rsta.2004.1505