skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: 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:
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. 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}
}

Works referenced in this record:

S PATIALLY H ETEROGENEOUS D YNAMICS IN S UPERCOOLED L IQUIDS
journal, October 2000


Supercooled liquids and the glass transition
journal, March 2001


Heterogeneous dynamics in liquids: fluctuations in space and time
journal, May 2002


Theory of Structural Glasses and Supercooled Liquids
journal, May 2007


Dynamics on the Way to Forming Glass: Bubbles in Space-Time
journal, March 2010


Relaxation of spatially heterogeneous dynamic domains in supercooled ortho‐terphenyl
journal, October 1995


Irreversible reorganization in a supercooled liquid originates from localized soft modes
journal, July 2008


Perspective: Supercooled liquids and glasses
journal, August 2012


Spatial Heterogeneities in Structural Temperature Cause Kovacs’ Expansion Gap Paradox in Aging of Glasses
journal, March 2020


Stringlike Cooperative Motion in a Supercooled Liquid
journal, March 1998


Dynamical Heterogeneities in a Supercooled Lennard-Jones Liquid
journal, October 1997


Connection between Adam-Gibbs Theory and Spatially Heterogeneous Dynamics
journal, February 2003


Clusters of mobile molecules in supercooled water
journal, July 2005


Static and dynamic heterogeneities in water
journal, December 2004

  • Stanley, H. Eugene; Buldyrev, Sergey V.; Franzese, Giancarlo
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 363, Issue 1827
  • https://doi.org/10.1098/rsta.2004.1505

Origin of the emergent fragile-to-strong transition in supercooled water
journal, September 2018


The dielectric relaxation time of supercooled water
journal, March 1982


Self-Diffusion of Supercooled Water to 238 K Using PGSE NMR Diffusion Measurements
journal, January 1999


Viscosity of deeply supercooled water and its coupling to molecular diffusion
journal, September 2015


Transitions between inherent structures in water
journal, March 2002


Water: A Tale of Two Liquids
journal, April 2016


Phase behaviour of metastable water
journal, November 1992


Singularity-free interpretation of the thermodynamics of supercooled water
journal, June 1996


The relationship between liquid, supercooled and glassy water
journal, November 1998


Growing correlation length in supercooled water
journal, June 2009


Metastable liquid–liquid transition in a molecular model of water
journal, June 2014


Understanding water’s anomalies with locally favoured structures
journal, April 2014


The structural origin of anomalous properties of liquid water
journal, December 2015


Relationship between structural order and the anomalies of liquid water
journal, January 2001


Prediction of entropy and dynamic properties of water below the homogeneous nucleation temperature
journal, May 2003


Maxima in the thermodynamic response and correlation functions of deeply supercooled water
journal, December 2017


Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature
journal, June 2014


A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum
journal, April 2016


Growth rate of crystalline ice and the diffusivity of supercooled water from 126 to 262 K
journal, December 2016


Reversible structural transformations in supercooled liquid water from 135 to 245 K
journal, September 2020


On the time required to freeze water
journal, December 2016


Supercooled Liquids and Glasses
journal, January 1996


Relaxation in glassforming liquids and amorphous solids
journal, September 2000


Cooling rate, heating rate, and aging effects in glassy water
journal, May 2004


Structural order in glassy water
journal, June 2005


Inherent structure in water
journal, July 1983


Spatially inhomogeneous bimodal inherent structure of simulated liquid water
journal, January 2011


Potential energy landscape of TIP4P/2005 water
journal, April 2018


Temperature Dependence of Inhomogeneous Broadening:  On the Meaning of Isosbestic Points
journal, October 2005


Detailed comparison of the Williams–Watts and Cole–Davidson functions
journal, October 1980


Homogeneous ice nucleation rates and crystallization kinetics in transiently-heated, supercooled water films from 188 K to 230 K
journal, May 2019


Aging as dynamics in configuration space
journal, March 2000


Aging and energy landscapes: application to liquids and glasses
journal, December 2002


Crossover (or Kovacs) Effect in an Aging Molecular Liquid
journal, January 2004


Structural relaxation in the glass transition region of water
journal, July 2005


Aging effects manifested in the potential-energy landscape of a model glass former
journal, August 2010


Energy landscape-driven non-equilibrium evolution of inherent structure in disordered material
journal, May 2017


Metabasin dynamics and local structure in supercooled water
journal, April 2007


A Topographic View of Supercooled Liquids and Glass Formation
journal, March 1995


Energy barriers and activated dynamics in a supercooled Lennard-Jones liquid
journal, March 2003


The anomalies and criticality of liquid water
journal, October 2020


Translational and rotational dynamics of high and low density TIP4P/2005 water
journal, June 2019


Effect of defects on molecular mobility in liquid water
journal, November 1991


Network defects and molecular mobility in liquid water
journal, March 1992


Anomalous low-temperature thermal properties of glasses and spin glasses
journal, January 1972


Pressure-induced transformations in glasses
journal, September 1993


Logarithmic Kinetics of the Amorphous-Amorphous Transformations in SiO 2 and GeO 2 Glasses under High Pressure
journal, February 1998


Mixturelike Behavior Near a Liquid-Liquid Phase Transition in Simulations of Supercooled Water
journal, March 2011


Entropy-driven liquid–liquid separation in supercooled water
journal, October 2012


Thermodynamics of supercooled and stretched water: Unifying two-structure description and liquid-vapor spinodal
journal, July 2019


Supercooled liquids for pedestrians
journal, June 2009


Trap Models and Slow Dynamics in Supercooled Liquids
journal, January 2003


From Coupled Elementary Units to the Complexity of the Glass Transition
journal, September 2010


THz Spectroscopy of Liquid H 2 O and D 2 O
journal, April 1999


Temperature Dependence of Homogeneous Nucleation in Ice
journal, June 2019


Physics of the Liquid-Liquid Critical Point
journal, October 2003


Dynamics of supercooled water in confined geometry
journal, January 2000


Glass Transition and Relaxation Processes in Supercooled Water
journal, December 2004


Dynamics of Water Intercalated in Graphite Oxide
journal, January 2010


Pressure Dependence of Fragile-to-Strong Transition and a Possible Second Critical Point in Supercooled Confined Water
journal, September 2005


The violation of the Stokes-Einstein relation in supercooled water
journal, August 2006


Confined Water as Model of Supercooled Water
journal, March 2016


The fragile-to-strong dynamic crossover transition in confined water: nuclear magnetic resonance results
journal, April 2006


Investigating hydration dependence of dynamics of confined water: Monolayer, hydration water and Maxwell–Wagner processes
journal, April 2008


Dynamic Crossovers and Stepwise Solidification of Confined Water: A 2 H NMR Study
journal, December 2013


Vibrational dynamics of confined supercooled water
journal, June 2019


Viscous Liquids and the Glass Transition: A Potential Energy Barrier Picture
journal, November 1969