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Title: Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water

Abstract

Understanding the properties of supercooled water is important for developing a comprehensive theory for liquid water and amorphous ices. Because of rapid crystallization for deeply supercooled water, experiments on it are typically carried out under conditions in which the temperature and/or pressure are rapidly changing. As a result, information on the structural relaxation kinetics of supercooled water as it approaches (metastable) equilibrium is useful for interpreting results obtained in this experimentally challenging region of phase space. Here, we used infrared spectroscopy and the fast time resolution obtained by transiently heating nanoscale water films to investigate relaxation kinetics (aging) in supercooled water. When the structural relaxation of the water films was followed using a temperature jump protocol analogous to the classic experiments of Kovacs, similar memory effects were observed. In particular, after suitable aging at one temperature, water’s structure displayed an extremum versus the number of heat pulses upon changing to a second temperature before eventually relaxing to a steady-state structure characteristic of that temperature. A random double well model based on the idea of dynamic heterogeneity in supercooled water accounts for the observations.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Physical Sciences Division
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
OSTI Identifier:
1974563
Report Number(s):
PNNL-SA-182629
Journal ID: ISSN 1520-6106
Grant/Contract Number:  
AC05-76RL01830; FWP 16248
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B
Additional Journal Information:
Journal Volume: 127; Journal Issue: 17; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical structure; circuits; equilibrium; kinetics; liquids

Citation Formats

Kringle, Loni M., Kay, Bruce D., and Kimmel, Gregory A. Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water. United States: N. p., 2023. Web. doi:10.1021/acs.jpcb.3c01465.
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Kringle, Loni M., Kay, Bruce D., & Kimmel, Gregory A. Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water. United States. https://doi.org/10.1021/acs.jpcb.3c01465
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Kringle, Loni M., Kay, Bruce D., and Kimmel, Gregory A. Tue . "Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water". United States. https://doi.org/10.1021/acs.jpcb.3c01465. https://www.osti.gov/servlets/purl/1974563.
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@article{osti_1974563,
title = {Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water},
author = {Kringle, Loni M. and Kay, Bruce D. and Kimmel, Gregory A.},
abstractNote = {Understanding the properties of supercooled water is important for developing a comprehensive theory for liquid water and amorphous ices. Because of rapid crystallization for deeply supercooled water, experiments on it are typically carried out under conditions in which the temperature and/or pressure are rapidly changing. As a result, information on the structural relaxation kinetics of supercooled water as it approaches (metastable) equilibrium is useful for interpreting results obtained in this experimentally challenging region of phase space. Here, we used infrared spectroscopy and the fast time resolution obtained by transiently heating nanoscale water films to investigate relaxation kinetics (aging) in supercooled water. When the structural relaxation of the water films was followed using a temperature jump protocol analogous to the classic experiments of Kovacs, similar memory effects were observed. In particular, after suitable aging at one temperature, water’s structure displayed an extremum versus the number of heat pulses upon changing to a second temperature before eventually relaxing to a steady-state structure characteristic of that temperature. A random double well model based on the idea of dynamic heterogeneity in supercooled water accounts for the observations.},
doi = {10.1021/acs.jpcb.3c01465},
journal = {Journal of Physical Chemistry. B},
number = 17,
volume = 127,
place = {United States},
year = {Tue Apr 25 00:00:00 EDT 2023},
month = {Tue Apr 25 00:00:00 EDT 2023}
}
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