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

Title: Quantum effects in the dynamics of deeply supercooled water

Journal Article · · Physical Review E
 [1];  [2];  [1];  [3];  [1]
  1. Univ. of Tennessee, Knoxville, TN (United States). Department of Chemistry and Joint Institute for Neutron Sciences; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  3. Arizona State Univ., Tempe, AZ (United States). Dept. of Chemistry and Biochemistry

In spite of its simple chemical structure, water remains one of the most puzzling liquids with many anomalies at low temperatures. Combining neutron scattering and dielectric relaxation spectroscopy, we show that quantum fluctuations are not negligible in deeply supercooled water. Our dielectric measurements reveal the anomalously weak temperature dependence of structural relaxation in vapor-deposited water close to the glass transition temperature Tg~136K. We demonstrate that this anomalous behavior can be explained well by quantum effects. In conclusion, these results have significant implications for our understanding of water dynamics.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1265363
Alternate ID(s):
OSTI ID: 1180248
Journal Information:
Physical Review E, Vol. 91, Issue 2; ISSN 2470-0045
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 19 works
Citation information provided by
Web of Science

References (82)

Crystallization of Amorphous Water Ice in the Solar System journal December 1996
Volume of supercooled water under pressure and the liquid-liquid critical point journal October 2010
Metastable liquid–liquid transition in a molecular model of water journal June 2014
Universal scaling between structural relaxation and vibrational dynamics in glass-forming liquids and polymers journal December 2007
Thermodynamic determination of fragility in liquids and a fragile-to-strong liquid transition in water journal April 1999
A Relation Between Fast and Slow Motions in Glassy and Liquid Selenium journal March 1992
Dynamics of sugar solutions as studied by dielectric spectroscopy journal September 2005
Anomalously large isotope effect in the glass transition of water journal November 2014
Phase behaviour of metastable water journal November 1992
Inelastic neutron scattering studies of hydrogen bonding in ices journal October 1996
Quantum diffusion in liquid water from ring polymer molecular dynamics journal October 2005
Neutron spectroscopic investigation of dynamics of water ice journal June 2002
The glass transition and fragility of supercooled confined water journal October 2004
Preparation of Amorphous Solid Water journal January 1972
The Physics of Heating by Time-Dependent Fields: Microwaves and Water Revisited journal August 2008
Densities of vibrational states and heat capacities of crystalline and amorphous H 2 O ice determined by neutron scattering journal July 1991
Dielectric Properties of Ice I journal August 1969
Calorimetric Study of Waterʼs Glass Transition in Nanoscale Confinement, Suggesting a Value of 210 K for Bulk Water journal December 2011
Supercooled water: A molecular dynamics simulation study with a polarizable potential journal August 2006
Amorphous Water journal June 2004
Continuous trends journal June 2014
The aperiodic crystal picture and free energy barriers in glasses journal March 1987
Glass-liquid transition and the enthalpy of devitrification of annealed vapor-deposited amorphous solid water: a comparison with hyperquenched glassy water journal June 1989
Hydrogen-Bond Equilibria and Lifetimes in a Monohydroxy Alcohol journal September 2011
X‐ray and neutron scattering studies of the structure of hyperquenched glassy water journal July 1992
Relaxation Dynamics in Glycerol−Water Mixtures. 2. Mesoscopic Feature in Water Rich Mixtures journal May 2005
Multiphonon contributions in inelastic neutron scattering spectra of ice journal June 1997
Supercooled and glassy water journal October 2003
The dielectric relaxation of water between 0°C and 35°C journal June 1999
Nuclear Quantum Effects in Water journal July 2008
Dielectric relaxation of the amorphous ices journal May 2008
Nonexponential relaxations in strong and fragile glass formers journal September 1993
Two phases? journal June 2014
The putative liquid-liquid transition is a liquid-solid transition in atomistic models of water journal October 2011
Structural transitions in amorphous water ice and astrophysical implications journal August 1994
The Glass Transition of Water, Based on Hyperquenching Experiments journal December 2001
State of water at 136 K determined by its relaxation time journal January 2005
Enthalpy relaxation of glassy water journal January 1990
Dielectric relaxation time of bulk water at 136–140K, background loss and crystallization effects journal April 2005
Glass transition for amorphous solid water journal February 1984
Water's second glass transition journal October 2013
Density minimum and liquid–liquid phase transition journal October 2005
Scaled Equation of State for Supercooled Water near the Liquid-Liquid Critical Point journal November 2006
Origins of Apparent Fragile-to-Strong Transitions of Protein Hydration Waters journal November 2008
Clearing the water journal April 2012
Ultrafast X-ray probing of water structure below the homogeneous ice nucleation temperature journal June 2014
Structural dynamics of supercooled water from quasielastic neutron scattering and molecular simulations journal April 2011
Design considerations in the use of interdigitated microsensor electrode arrays (IMEs) for impedimetric characterization of biomimetic hydrogels journal November 2010
Rotational dynamics in supercooled water from nuclear spin relaxation and molecular simulations journal May 2012
Insights into Phases of Liquid Water from Study of Its Unusual Glass-Forming Properties journal February 2008
Observation of fragile-to-strong dynamic crossover in protein hydration water journal June 2006
Hydrogen network fluctuations and dielectric spectrometry of liquids journal July 2002
Note: Equation of state and compressibility of supercooled water: Simulations and experiment journal May 2011
Glassy dynamics journal January 2000
Water II is a "strong" liquid journal June 1993
Pressure Dependence of Fragile-to-Strong Transition and a Possible Second Critical Point in Supercooled Confined Water journal September 2005
Hydrogen bonding in glassy liquid water from Raman spectroscopic studies journal November 1998
Temperature dependence of dielectric relaxation in H 2 O and D 2 O ice. A dissipative quantum tunneling approach journal July 1993
Fragile-to-strong liquid transition in deeply supercooled confined water journal January 2004
Excess of Proton Mean Kinetic Energy in Supercooled Water journal March 2008
The glass–liquid transition of hyperquenched water journal December 1987
Liquid Fragility and the Glass Transition in Water and Aqueous Solutions journal August 2002
The relationship between liquid, supercooled and glassy water journal November 1998
No fragile-to-strong crossover in LiCl-H 2 O solution journal March 2012
Neutron Scattering Studies of Vapor Deposited Amorphous Ice journal September 1997
Hopping of ions in ice journal January 1974
The dielectric relaxation time of ice V, its partial anti-ferroelectric ordering and the role of Bjerrum defects journal August 2001
New insights into the fragility dilemma in liquids journal April 2001
Competing quantum effects in the dynamics of a flexible water model journal July 2009
Dielectric Behavior of Cubic and Hexagonal Ices at Low Temperatures journal May 1970
Infrared and vapor flux studies of vapor-deposited amorphous and crystalline water ice films between 90 and 145 K journal December 2001
Heat capacity and glass transition of pure and doped cubic ices† journal January 1987
Liquid-liquid transition in ST2 water journal December 2012
Heat capacity and glass transition behavior of amorphous ice journal June 1988
Role of Quantum Effects in the Glass Transition journal February 2013
Two Calorimetrically Distinct States of Liquid Water Below 150 Kelvin journal July 1996
Resolving the controversy on the glass transition temperature of water? journal September 2011
Vitreous Ice: Irreversible Transformations During Warm-Up journal May 1965
The fragile-to-strong dynamic crossover transition in confined water: nuclear magnetic resonance results journal April 2006
Liquid–liquid transition without macroscopic phase separation in a water–glycerol mixture journal March 2012
Frozen-in states of orientational and positional disorder in molecular solids journal January 1980
The existence of supercooled liquid water at 150?K journal April 1999

Cited By (3)

Ultrastable and polyamorphic states of vapor-deposited 2-methyltetrahydrofuran journal June 2019
Amorphous and crystalline ices studied by dielectric spectroscopy journal June 2019
Neutron scattering in the biological sciences: progress and prospects journal December 2018

Similar Records

Role of quantum fluctuations in structural dynamics of liquids of light molecules
Journal Article · Fri Dec 16 00:00:00 EST 2016 · Journal of Chemical Physics · OSTI ID:1265363

Reversible structural transformations in supercooled liquid water from 135 to 245 K
Journal Article · Fri Sep 18 00:00:00 EDT 2020 · Science · OSTI ID:1265363

Dynamic Heterogeneity and Kovacs’ Memory Effects in Supercooled Water
Journal Article · Tue Apr 25 00:00:00 EDT 2023 · Journal of Physical Chemistry. B · OSTI ID:1265363