Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water

Kringle, Loni M.; Kay, Bruce D.; Kimmel, Gregory A.

doi:10.1021/acs.jpcb.3c01465

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

Journal Article · Tue Apr 25 00:00:00 EDT 2023 · Journal of Physical Chemistry. B

DOI:https://doi.org/10.1021/acs.jpcb.3c01465· OSTI ID:1974563

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Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Physical Sciences Division

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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC05-76RL01830; FWP 16248

OSTI ID:: 1974563

Report Number(s):: PNNL-SA-182629

Journal Information:: Journal of Physical Chemistry. B, Vol. 127, Issue 17; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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