The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime

Cunsolo, Alessandro

doi:10.1155/2015/137435

Title: The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime

Abstract

Relevant advances in the knowledge of the water dynamics at mesoscopic scales are reviewed, while mainly focusing on the contribution provided by high resolution inelastic X-ray scattering (IXS). In particular it is discussed how the use of IXS has improved our understanding of viscoelastic properties of water at THz frequencies. This specifically involves some solid-like features such as the onset of shear wave propagation, a sound velocity surprisingly similar to the one of ice, and an anomalously low sound absorption coefficient. All these properties can be explained by assuming the coupling of THz density fluctuations with a structural relaxation process connected to the breaking and forming of hydrogen bonds (HBs). This review also includes more recent IXS results demonstrating that, upon approaching supercritical conditions, relaxation phenomena in water gradually lose their structural character becoming essentially collisional in character. Furthermore, GHz spectroscopy results on supercooled water, suggesting the occurrence of a structural arrest, are discussed. An overview of the new opportunities offered by next generation IXS spectrometers finally concludes this review.

Authors:

Cunsolo, Alessandro ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)

Publication Date:: Thu Feb 26 00:00:00 EST 2015

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1324811

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: Advances in Condensed Matter Physics

Additional Journal Information:: Journal Volume: 2015; Journal ID: ISSN 1687-8108

Publisher:: Hindawi

Country of Publication:: United States

Language:: ENGLISH

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats


                    Cunsolo, Alessandro. The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime.  United States: N. p., 2015. 
        Web.  doi:10.1155/2015/137435.

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                    Cunsolo, Alessandro. The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime.  United States.  https://doi.org/10.1155/2015/137435

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                    Cunsolo, Alessandro. 2015.  
        "The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime".  United States.  https://doi.org/10.1155/2015/137435.  https://www.osti.gov/servlets/purl/1324811.

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@article{osti_1324811,

  title        = {The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime},

  author       = {Cunsolo, Alessandro},

  abstractNote = {Relevant advances in the knowledge of the water dynamics at mesoscopic scales are reviewed, while mainly focusing on the contribution provided by high resolution inelastic X-ray scattering (IXS). In particular it is discussed how the use of IXS has improved our understanding of viscoelastic properties of water at THz frequencies. This specifically involves some solid-like features such as the onset of shear wave propagation, a sound velocity surprisingly similar to the one of ice, and an anomalously low sound absorption coefficient. All these properties can be explained by assuming the coupling of THz density fluctuations with a structural relaxation process connected to the breaking and forming of hydrogen bonds (HBs). This review also includes more recent IXS results demonstrating that, upon approaching supercritical conditions, relaxation phenomena in water gradually lose their structural character becoming essentially collisional in character. Furthermore, GHz spectroscopy results on supercooled water, suggesting the occurrence of a structural arrest, are discussed. An overview of the new opportunities offered by next generation IXS spectrometers finally concludes this review.},

  doi          = {10.1155/2015/137435},

  url          = {https://www.osti.gov/biblio/1324811},
  journal      = {Advances in Condensed Matter Physics},

  issn         = {1687-8108},

  number       = ,

  volume       = 2015,

  place        = {United States},

  year         = {Thu Feb 26 00:00:00 EST 2015},

  month        = {Thu Feb 26 00:00:00 EST 2015}

}

Copy to clipboard

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Journal Article Tung, Chi-Huan; Chang, Shou-Yi; Yip, Sidney; ... - Journal of Chemical Physics

In this study, a method for characterizing the topological fluctuations in liquids is proposed. This approach exploits the concept of the weighted gyration tensor of a collection of particles and permits the definition of a local configurational unit (LCU). The first principal axis of the gyration tensor serves as the director of the LCU, which can be tracked and analyzed by molecular dynamics simulations. Analysis of moderately supercooled Kob–Andersen mixtures suggests that orientational relaxation of the LCU closely follows viscoelastic relaxation and exhibits a two-stage behavior. The slow relaxing component of the LCU corresponds to the structural, Maxwellian mechanical relaxation.more »« less
https://doi.org/10.1063/5.0189938
The hydrogen-bond collective dynamics in liquid methanol

Journal Article Bellissima, Stefano; Cunsolo, Alessandro; DePanfilis, Simone; ... - Scientific Reports

The relatively simple molecular structure of hydrogen-bonded (HB) systems is often belied by their exceptionally complex thermodynamic and microscopic behaviour. For this reason, after a thorough experimental, computational and theoretical scrutiny, the dynamics of molecules in HB systems still eludes a comprehensive understanding. Aiming at shedding some insight into this topic, we jointly used neutron Brillouin scattering and molecular dynamics simulations to probe the dynamics of a prototypical hydrogen-bonded alcohol, liquid methanol. The comparison with the most thoroughly investigated HB system, liquid water, pinpoints common behaviours of their THz microscopic dynamics, thereby providing additional information on the role of HBmore »« less
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https://doi.org/10.1038/srep39533

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The numerical integration and 3-D finite element formulation of a viscoelastic model of glass

Technical Report Chambers, R

The use of glasses is widespread in making hermetic, insulating seals for many electronic components. Flat panel displays and fiber optic connectors are other products utilizing glass as a structural element. When glass is cooled from sealing temperatures, residual stresses are generated due to mismatches in thermal shrinkage created by the dissimilar material properties of the adjoining materials. Because glass is such a brittle material at room temperature, tensile residual stresses must be kept small to ensure durability and avoid cracking. Although production designs and the required manufacturing process development can be deduced empirically, this is an expensive and timemore »« less

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Title: The THz Spectrum of Density Fluctuations of Water: The Viscoelastic Regime

Abstract

Citation Formats

X-Ray Bragg Diffraction in Asymmetric Backscattering Geometry journal, December 2006

Structural relaxation in the dynamics of glycerol: a joint visible, UV and x-ray inelastic scattering study journal, January 2006

Application of Adam-Gibbs' theory to thermodynamic recovery and structural relaxation book, January 1987

Observable Fast Kinetic Eigenmode in Binary Noble-Gas Mixtures? journal, August 1988

Collective Dynamical Properties of Liquid Water journal, October 1988

Enhanced Density Fluctuations in Supercooled H 2 O, D 2 O, and Ethanol-Water Solutions: Evidence from Small-Angle X-Ray Scattering journal, March 1981

Sound propagation in liquid water: The puzzle continues journal, March 1994

Effect of Pressure on the Viscosity of Water journal, August 1965

Comparison of simple potential functions for simulating liquid water journal, July 1983

Quantum effects in the dynamics of He probed by inelastic x-ray scattering journal, July 2001

Molecular dynamics in H2O and D2O analysis by inelastic scattering of 10 Å neutrons journal, February 1977

High‐resolution low‐frequency Raman spectra of liquid H 2 O and D 2 O journal, December 1990

Anomalous properties of supercooled water. Heat capacity, expansivity, and proton magnetic resonance chemical shift from 0 to -38% journal, December 1973

Fast sound in two-component liquids journal, December 1986

High frequency dynamics in liquids and supercritical fluids: A comparative inelastic x-ray scattering study journal, February 2009

Collective excitations in liquid lead journal, June 1980

High frequency dynamics and structural relaxation process in liquid ammonia journal, August 2007

Anomalous Heat Capacities of Supercooled Water and Heavy Water journal, July 1973

Microscopic relaxation in supercritical and liquid neon journal, February 2001

Raman Spectral Studies of Water Structure journal, June 1964

Brillouin Scattering in Simple Liquids: Argon and Neon journal, October 1969

Raman Spectral Studies of the Effects of Temperature on Water and Electrolyte Solutions journal, February 1966

CI study of the water dimer potential surface journal, February 1976

Zur Theorie der spezifischen Wärmen journal, January 1912

Adiabatic and isothermal sound waves: The case of supercritical nitrogen journal, July 2006

Analysis of Recent Measurements of the Viscosity of Glasses journal, June 1925

Thermal conductivity of water: Molecular dynamics and generalized hydrodynamics results journal, October 1997

Collective dynamics in three body water and sound dispersion journal, November 1986

Phonon dispersion in D2O-ice journal, December 1969

Water II is a "strong" liquid journal, June 1993

Etude ultrasonore de l'eau en surfusion jusqu'à — 26°C journal, January 1979

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

Density fluctuations in classical monatomic liquids journal, December 1971

The Ultrahigh Resolution IXS Beamline of NSLS-II: Recent Advances and Scientific Opportunities journal, March 2013

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

The Temperature Dependence of the Viscosity of Supercooled Water journal, December 1963

Brillouin scattering investigations of fast dynamics in glass forming systems journal, September 2002

Thermophysical Properties of Fluid H 2 O journal, January 1984

Stress tensor and viscosity of water: Molecular dynamics and generalized hydrodynamics results journal, August 1995

Relaxation process in deeply supercooled water by Mandelstam-Brillouin scattering journal, January 1989

Onset of a transverse dynamics in the THz spectrum of water journal, February 2013

Kinetic-sound propagation in dilute gas mixtures journal, May 1989

Evidence of Anomalous Acoustic Behavior from Brillouin Scattering in Supercooled Water journal, March 1984

X-ray monochromator with an energy resolution of 8×10−9 at 14.41 keV journal, November 2001

Phase behaviour of metastable water journal, November 1992

High-contrast sub-millivolt inelastic X-ray scattering for nano- and mesoscale science journal, June 2014

Quasielastic neutron scattering investigation of the pressure dependence of molecular motions in liquid water journal, February 2006

Isothermal compressibility of supercooled water and evidence for a thermodynamic singularity at −45°C journal, August 1976

Sound velocity of supercooled water down to −33 °C using acoustic levitation journal, June 1980

Brillouin scattering studies of normal and supercooled water journal, November 1976

Loss of tensile strength in liquids without property discontinuities: A thermodynamic analysis journal, February 1987

The neutron scattering function for hard spheres journal, June 1983

Ultrasonic investigation of the glass transition in glycerol journal, July 1986

Structural relaxation in supercooled water by time-resolved spectroscopy journal, March 2004

Small-angle scattering and the structure of ambient liquid water journal, July 2010

Temperature and density dependence of the structural relaxation time in water by inelastic ultraviolet scattering journal, October 2009

Density dependence of sound dispersion in repulsive Lennard-Jones fluids journal, October 1986

Fast sound in liquid water journal, March 1993

Transition from the collective to the single-particle regimes in a quantum fluid journal, January 2003

Collective Dynamics in Water by High Energy Resolution Inelastic X-Ray Scattering journal, July 1995

Spectroscopic and transport properties of water: Model calculations and the interpretation of experimental results journal, June 1982

Depolarized Rayleigh scattering in water up to supercritical conditions journal, May 1995

Mixing of Longitudinal and Transverse Dynamics in Liquid Water journal, September 1997

A perfect crystal X-ray analyser with 1.5 meV energy resolution journal, September 1996

Comparison of Dielectric and Mechanical Relaxation in Associated Liquids journal, August 1963

Dielectric dispersion in pure polar liquids at very high radio-frequencies II. Relation of experimental results to theory journal, July 1952

Pressure dependence of the large-scale structure of water journal, January 2009

Velocity dispersion and viscous relaxation in supercooled water journal, September 1996

High-frequency transverse dynamics in glasses journal, March 2003

Theoretical and computer-simulation study of the density fluctuations in liquid water journal, December 1989

Power-law behavior in the viscosity of supercooled liquids journal, August 1986

Equivalence of the sound velocity in water and ice at mesoscopic wavelengths journal, February 1996

Noncritical behavior of density fluctuations in supercooled water journal, September 1993

Transition from Normal to Fast Sound in Liquid Water journal, July 1996

High frequency sound velocity and sound absorption in supercooled water and the thermodynamic singularity at 228°K journal, June 1977

Structural and Collisional Relaxations in Liquids and Supercritical Fluids journal, February 2007

Computer "Experiments" on Classical Fluids. IV. Transport Properties and Time-Correlation Functions of the Lennard-Jones Liquid near Its Triple Point journal, May 1973

X-Ray Bragg Diffraction in Asymmetric Backscattering Geometry
journal, December 2006

Structural relaxation in the dynamics of glycerol: a joint visible, UV and x-ray inelastic scattering study
journal, January 2006

Application of Adam-Gibbs' theory to thermodynamic recovery and structural relaxation
book, January 1987

Observable Fast Kinetic Eigenmode in Binary Noble-Gas Mixtures?
journal, August 1988

Collective Dynamical Properties of Liquid Water
journal, October 1988

Enhanced Density Fluctuations in Supercooled $H_{2}$ O, $D_{2}$ O, and Ethanol-Water Solutions: Evidence from Small-Angle X-Ray Scattering
journal, March 1981

Sound propagation in liquid water: The puzzle continues
journal, March 1994

Effect of Pressure on the Viscosity of Water
journal, August 1965

Comparison of simple potential functions for simulating liquid water
journal, July 1983

Quantum effects in the dynamics of He probed by inelastic x-ray scattering
journal, July 2001

Molecular dynamics in H2O and D2O analysis by inelastic scattering of 10 Å neutrons
journal, February 1977

High‐resolution low‐frequency Raman spectra of liquid H ₂ O and D ₂ O
journal, December 1990

Anomalous properties of supercooled water. Heat capacity, expansivity, and proton magnetic resonance chemical shift from 0 to -38%
journal, December 1973

Fast sound in two-component liquids
journal, December 1986

High frequency dynamics in liquids and supercritical fluids: A comparative inelastic x-ray scattering study
journal, February 2009

Collective excitations in liquid lead
journal, June 1980

High frequency dynamics and structural relaxation process in liquid ammonia
journal, August 2007

Anomalous Heat Capacities of Supercooled Water and Heavy Water
journal, July 1973

Microscopic relaxation in supercritical and liquid neon
journal, February 2001

Raman Spectral Studies of Water Structure
journal, June 1964

Brillouin Scattering in Simple Liquids: Argon and Neon
journal, October 1969

Raman Spectral Studies of the Effects of Temperature on Water and Electrolyte Solutions
journal, February 1966

CI study of the water dimer potential surface
journal, February 1976

Zur Theorie der spezifischen Wärmen
journal, January 1912

Adiabatic and isothermal sound waves: The case of supercritical nitrogen
journal, July 2006

Analysis of Recent Measurements of the Viscosity of Glasses
journal, June 1925

Thermal conductivity of water: Molecular dynamics and generalized hydrodynamics results
journal, October 1997

Collective dynamics in three body water and sound dispersion
journal, November 1986

Phonon dispersion in D2O-ice
journal, December 1969

Water II is a "strong" liquid
journal, June 1993

Etude ultrasonore de l'eau en surfusion jusqu'à — 26°C
journal, January 1979

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

Density fluctuations in classical monatomic liquids
journal, December 1971

The Ultrahigh Resolution IXS Beamline of NSLS-II: Recent Advances and Scientific Opportunities
journal, March 2013

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

The Temperature Dependence of the Viscosity of Supercooled Water
journal, December 1963

Brillouin scattering investigations of fast dynamics in glass forming systems
journal, September 2002

Thermophysical Properties of Fluid H ₂ O
journal, January 1984

Stress tensor and viscosity of water: Molecular dynamics and generalized hydrodynamics results
journal, August 1995

Relaxation process in deeply supercooled water by Mandelstam-Brillouin scattering
journal, January 1989

Onset of a transverse dynamics in the THz spectrum of water
journal, February 2013

Kinetic-sound propagation in dilute gas mixtures
journal, May 1989

Evidence of Anomalous Acoustic Behavior from Brillouin Scattering in Supercooled Water
journal, March 1984

X-ray monochromator with an energy resolution of 8×10−9 at 14.41 keV
journal, November 2001

Phase behaviour of metastable water
journal, November 1992

High-contrast sub-millivolt inelastic X-ray scattering for nano- and mesoscale science
journal, June 2014

Quasielastic neutron scattering investigation of the pressure dependence of molecular motions in liquid water
journal, February 2006

Isothermal compressibility of supercooled water and evidence for a thermodynamic singularity at −45°C
journal, August 1976

Sound velocity of supercooled water down to −33 °C using acoustic levitation
journal, June 1980

Brillouin scattering studies of normal and supercooled water
journal, November 1976

Loss of tensile strength in liquids without property discontinuities: A thermodynamic analysis
journal, February 1987

The neutron scattering function for hard spheres
journal, June 1983

Ultrasonic investigation of the glass transition in glycerol
journal, July 1986

Structural relaxation in supercooled water by time-resolved spectroscopy
journal, March 2004

Small-angle scattering and the structure of ambient liquid water
journal, July 2010

Temperature and density dependence of the structural relaxation time in water by inelastic ultraviolet scattering
journal, October 2009

Density dependence of sound dispersion in repulsive Lennard-Jones fluids
journal, October 1986

Fast sound in liquid water
journal, March 1993

Transition from the collective to the single-particle regimes in a quantum fluid
journal, January 2003

Collective Dynamics in Water by High Energy Resolution Inelastic X-Ray Scattering
journal, July 1995

Spectroscopic and transport properties of water: Model calculations and the interpretation of experimental results
journal, June 1982

Depolarized Rayleigh scattering in water up to supercritical conditions
journal, May 1995

Mixing of Longitudinal and Transverse Dynamics in Liquid Water
journal, September 1997

A perfect crystal X-ray analyser with 1.5 meV energy resolution
journal, September 1996

Comparison of Dielectric and Mechanical Relaxation in Associated Liquids
journal, August 1963

Dielectric dispersion in pure polar liquids at very high radio-frequencies II. Relation of experimental results to theory
journal, July 1952

Pressure dependence of the large-scale structure of water
journal, January 2009

Velocity dispersion and viscous relaxation in supercooled water
journal, September 1996

High-frequency transverse dynamics in glasses
journal, March 2003

Theoretical and computer-simulation study of the density fluctuations in liquid water
journal, December 1989

Power-law behavior in the viscosity of supercooled liquids
journal, August 1986

Equivalence of the sound velocity in water and ice at mesoscopic wavelengths
journal, February 1996

Noncritical behavior of density fluctuations in supercooled water
journal, September 1993

Transition from $Normal$ to $Fast$ Sound in Liquid Water
journal, July 1996

High frequency sound velocity and sound absorption in supercooled water and the thermodynamic singularity at 228°K
journal, June 1977

Structural and Collisional Relaxations in Liquids and Supercritical Fluids
journal, February 2007

Computer "Experiments" on Classical Fluids. IV. Transport Properties and Time-Correlation Functions of the Lennard-Jones Liquid near Its Triple Point
journal, May 1973

ESR Study of a Carboxyl Radical Trapped in a Single Crystal of Maleic Acid Irradiated at 77°K
journal, October 1971

Relaxation Processes in Harmonic Glasses?
journal, June 2000

Structural Relaxation in Supercooled Water by Time-Resolved Spectroscopy.
journal, June 2004