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

Title: The Proton Density of States in Confined Water (H2O)

Abstract

The hydrogen density of states (DOS) in confined water has been probed by inelastic neutron scattering spectra in a wide range of its P–T phase diagram. The liquid–liquid transition and the dynamical crossover from the fragile (super-Arrhenius) to strong (Arrhenius) glass forming behavior have been studied, by taking into account the system polymorphism in both the liquid and amorphous solid phases. The interest is focused in the low energy region of the DOS ( E < 10 meV) and the data are discussed in terms of the energy landscape (local minima of the potential energy) approach. In this latest research, we consider a unit scale energy (EC) linked to the water local order governed by the hydrogen bonding (HB). All the measured spectra, scaled according to such energy, evidence a universal power law behavior with different exponents ( γ ) in the strong and fragile glass forming regions, respectively. In the first case, the DOS data obey the Debye squared-frequency law, whereas, in the second one, we obtain a value predicted in terms of the mode-coupling theory (MCT) ( γ ≃ 1.6 ).

Authors:
; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1572573
Grant/Contract Number:  
FG02-90ER45429
Resource Type:
Published Article
Journal Name:
International Journal of Molecular Sciences (Online)
Additional Journal Information:
Journal Name: International Journal of Molecular Sciences (Online) Journal Volume: 20 Journal Issue: 21; Journal ID: ISSN 1422-0067
Publisher:
MDPI AG
Country of Publication:
Switzerland
Language:
English

Citation Formats

Chen, Sow-Hsin, Corsaro, Carmelo, Mallamace, Francesco, Fazio, Enza, and Mallamace, Domenico. The Proton Density of States in Confined Water (H2O). Switzerland: N. p., 2019. Web. doi:10.3390/ijms20215373.
Copy to clipboard
Chen, Sow-Hsin, Corsaro, Carmelo, Mallamace, Francesco, Fazio, Enza, & Mallamace, Domenico. The Proton Density of States in Confined Water (H2O). Switzerland. doi:10.3390/ijms20215373.
Copy to clipboard
Chen, Sow-Hsin, Corsaro, Carmelo, Mallamace, Francesco, Fazio, Enza, and Mallamace, Domenico. Tue . "The Proton Density of States in Confined Water (H2O)". Switzerland. doi:10.3390/ijms20215373.
Copy to clipboard
@article{osti_1572573,
title = {The Proton Density of States in Confined Water (H2O)},
author = {Chen, Sow-Hsin and Corsaro, Carmelo and Mallamace, Francesco and Fazio, Enza and Mallamace, Domenico},
abstractNote = {The hydrogen density of states (DOS) in confined water has been probed by inelastic neutron scattering spectra in a wide range of its P–T phase diagram. The liquid–liquid transition and the dynamical crossover from the fragile (super-Arrhenius) to strong (Arrhenius) glass forming behavior have been studied, by taking into account the system polymorphism in both the liquid and amorphous solid phases. The interest is focused in the low energy region of the DOS ( E < 10 meV) and the data are discussed in terms of the energy landscape (local minima of the potential energy) approach. In this latest research, we consider a unit scale energy (EC) linked to the water local order governed by the hydrogen bonding (HB). All the measured spectra, scaled according to such energy, evidence a universal power law behavior with different exponents ( γ ) in the strong and fragile glass forming regions, respectively. In the first case, the DOS data obey the Debye squared-frequency law, whereas, in the second one, we obtain a value predicted in terms of the mode-coupling theory (MCT) ( γ ≃ 1.6 ).},
doi = {10.3390/ijms20215373},
journal = {International Journal of Molecular Sciences (Online)},
number = 21,
volume = 20,
place = {Switzerland},
year = {2019},
month = {10}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.3390/ijms20215373
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Comparison of Raman- and neutron-scattering data for glass-forming systems
journal, October 1995

Volume of supercooled water under pressure and the liquid-liquid critical point
journal, October 2010

  • Mishima, Osamu
  • The Journal of Chemical Physics, Vol. 133, Issue 14
  • DOI: 10.1063/1.3487999

Unravelling the contribution of local structures to the anomalies of water: The synergistic action of several factors
journal, March 2019

  • Martelli, Fausto
  • The Journal of Chemical Physics, Vol. 150, Issue 9
  • DOI: 10.1063/1.5087471

Diffusion and Nuclear Spin Relaxation in Water
journal, September 1958

Colloquium : Water’s controversial glass transitions
journal, February 2016

Significant‐Structure Theory Applied to Water and Heavy Water
journal, February 1966

  • Jhon, Mu Shik; Grosh, Joe; Ree, Taikyue
  • The Journal of Chemical Physics, Vol. 44, Issue 4
  • DOI: 10.1063/1.1726878

Dynamic crossover in hydration water of curing cement paste: the effect of superplasticizer
journal, January 2012

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

  • Palmer, Jeremy C.; Martelli, Fausto; Liu, Yang
  • Nature, Vol. 510, Issue 7505
  • DOI: 10.1038/nature13405

Relation between the Widom line and the dynamic crossover in systems with a liquid-liquid phase transition
journal, November 2005

  • Xu, L.; Kumar, P.; Buldyrev, S. V.
  • Proceedings of the National Academy of Sciences, Vol. 102, Issue 46
  • DOI: 10.1073/pnas.0507870102

Hyper-Raman Scattering Observation of the Boson Peak in Vitreous Silica
journal, June 2000

Comparative analysis of Silica-gel/Water and Zeolite/water Pair on adsorption Refrigeration System
journal, July 2019

Two‐State Theory of the Structure of Water
journal, April 1965

  • Davis, C. M.; Litovitz, T. A.
  • The Journal of Chemical Physics, Vol. 42, Issue 7
  • DOI: 10.1063/1.1696333

Phase behaviour of metastable water
journal, November 1992

  • Poole, Peter H.; Sciortino, Francesco; Essmann, Ulrich
  • Nature, Vol. 360, Issue 6402
  • DOI: 10.1038/360324a0

The new insight into dynamic crossover in glass forming liquids from the apparent enthalpy analysis
journal, August 2012

  • Martinez-Garcia, Julio Cesar; Martinez-Garcia, Jorge; Rzoska, Sylwester J.
  • The Journal of Chemical Physics, Vol. 137, Issue 6
  • DOI: 10.1063/1.4739750

Relationship between melting and amorphization of ice
journal, December 1996

Perspective: Supercooled liquids and glasses
journal, August 2012

  • Ediger, M. D.; Harrowell, Peter
  • The Journal of Chemical Physics, Vol. 137, Issue 8
  • DOI: 10.1063/1.4747326

Evidence of the existence of the low-density liquid phase in supercooled, confined water
journal, December 2006

  • Mallamace, F.; Broccio, M.; Corsaro, C.
  • Proceedings of the National Academy of Sciences, Vol. 104, Issue 2
  • DOI: 10.1073/pnas.0607138104

The Microscopic Basis of the Glass Transition in Polymers from Neutron Scattering Studies
journal, March 1995

Interaction and percolation in the L 64 triblock copolymer micellar system
journal, December 1999

  • Lobry, Laurent; Micali, Norberto; Mallamace, Francesco
  • Physical Review E, Vol. 60, Issue 6
  • DOI: 10.1103/PhysRevE.60.7076

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

  • Chen, S. -H.; Mallamace, F.; Mou, C. -Y.
  • Proceedings of the National Academy of Sciences, Vol. 103, Issue 35
  • DOI: 10.1073/pnas.0603253103

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

  • Speedy, R. J.; Angell, C. A.
  • The Journal of Chemical Physics, Vol. 65, Issue 3
  • DOI: 10.1063/1.433153

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

A Theory of Water and Ionic Solution, with Particular Reference to Hydrogen and Hydroxyl Ions
journal, August 1933

  • Bernal, J. D.; Fowler, R. H.
  • The Journal of Chemical Physics, Vol. 1, Issue 8
  • DOI: 10.1063/1.1749327

Transport properties of glass-forming liquids suggest that dynamic crossover temperature is as important as the glass transition temperature
journal, December 2010

  • Mallamace, F.; Branca, C.; Corsaro, C.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 52
  • DOI: 10.1073/pnas.1015340107

The role of the dynamic crossover temperature and the arrest in glass-forming fluids
journal, September 2011

A Fundamental Equation for Water Covering the Range from the Melting Line to 1273 K at Pressures up to 25 000 MPa
journal, October 1989

  • Saul, A.; Wagner, W.
  • Journal of Physical and Chemical Reference Data, Vol. 18, Issue 4
  • DOI: 10.1063/1.555836

Universal link between the boson peak and transverse phonons in glass
journal, October 2008

  • Shintani, Hiroshi; Tanaka, Hajime
  • Nature Materials, Vol. 7, Issue 11
  • DOI: 10.1038/nmat2293

Theory of Structural Glasses and Supercooled Liquids
journal, May 2007

Vibrational excitations in systems with correlated disorder
journal, March 2008

  • Schirmacher, W.; Schmid, B.; Tomaras, C.
  • physica status solidi (c), Vol. 5, Issue 3
  • DOI: 10.1002/pssc.200777584

Density minimum of confined water at low temperatures: a combined study by small-angle scattering of X-rays and neutrons
journal, January 2012

  • Erko, M.; Wallacher, D.; Hoell, A.
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 11
  • DOI: 10.1039/c2cp24075k

Evidence of dynamic crossover phenomena in water and other glass-forming liquids: experiments, MD simulations and theory
journal, November 2009

Effect of hydrogen bond cooperativity on the behavior of water
journal, January 2010

  • Stokely, K.; Mazza, M. G.; Stanley, H. E.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 4
  • DOI: 10.1073/pnas.0912756107

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

  • Angell, C. A.; Shuppert, J.; Tucker, J. C.
  • The Journal of Physical Chemistry, Vol. 77, Issue 26
  • DOI: 10.1021/j100644a014

Polymeric Micelles of Biodegradable Diblock Copolymers: Enhanced Encapsulation of Hydrophobic Drugs
journal, April 2018

Densities and partial molar volumes of supercooled aqueous solutions
journal, August 1983

  • Sorensen, C. M.
  • The Journal of Chemical Physics, Vol. 79, Issue 3
  • DOI: 10.1063/1.445908

Dynamic crossover in deeply cooled water confined in MCM-41 at 4 kbar and its relation to the liquid-liquid transition hypothesis
journal, September 2015

  • Wang, Zhe; Le, Peisi; Ito, Kanae
  • The Journal of Chemical Physics, Vol. 143, Issue 11
  • DOI: 10.1063/1.4930855

Effect of Densification on the Density of Vibrational States of Glasses
journal, September 2006

The Boson peak interpretation and evolution in confined amorphous water
journal, May 2019

  • Mallamace, Francesco; Corsaro, Carmelo; Mallamace, Domenico
  • Science China Physics, Mechanics & Astronomy, Vol. 62, Issue 10
  • DOI: 10.1007/s11433-018-9380-x

Single-particle dynamics of water molecules in confined space
journal, May 1995

  • Bellissent-Funel, M. -C.; Chen, S. H.; Zanotti, J. -M.
  • Physical Review E, Vol. 51, Issue 5
  • DOI: 10.1103/PhysRevE.51.4558

Structure of Ice VI
journal, October 1965

Water, in the Liquid and Five Solid Forms, under Pressure
journal, January 1912

  • Bridgman, P. W.
  • Proceedings of the American Academy of Arts and Sciences, Vol. 47, Issue 13
  • DOI: 10.2307/20022754

The thermodynamical response functions and the origin of the anomalous behavior of liquid water
journal, January 2013

  • Mallamace, Francesco; Corsaro, Carmelo; Mallamace, Domenico
  • Faraday Discussions, Vol. 167
  • DOI: 10.1039/c3fd00073g

Appearance of a fractional Stokes–Einstein relation in water and a structural interpretation of its onset
journal, July 2009

  • Xu, Limei; Mallamace, Francesco; Yan, Zhenyu
  • Nature Physics, Vol. 5, Issue 8
  • DOI: 10.1038/nphys1328

Heat capacity of water at extremes of supercooling and superheating
journal, March 1982

  • Angell, C. A.; Sichina, W. J.; Oguni, M.
  • The Journal of Physical Chemistry, Vol. 86, Issue 6
  • DOI: 10.1021/j100395a032

A correlation between low-energy vibrational spectra and first sharp diffraction peak in chalcogenide glasses
journal, January 1991

Supercooled Liquids and Glasses
journal, January 1996

  • Ediger, M. D.; Angell, C. A.; Nagel, Sidney R.
  • The Journal of Physical Chemistry, Vol. 100, Issue 31
  • DOI: 10.1021/jp953538d

Advances in Computational Studies of the Liquid–Liquid Transition in Water and Water-Like Models
journal, August 2018

Densities of supercooled H 2 O and D 2 O in 25 μ glass capillaries
journal, May 1986

  • Hare, D. E.; Sorensen, C. M.
  • The Journal of Chemical Physics, Vol. 84, Issue 9
  • DOI: 10.1063/1.450660

Low-Temperature Anomalies in Strong and Fragile Glass Formers
journal, March 1997

Neutron and light scattering study of supercooled glycerol
journal, May 1994

Transport properties of supercooled confined water
journal, July 2008

  • Mallamace, F.; Branca, C.; Broccio, M.
  • The European Physical Journal Special Topics, Vol. 161, Issue 1
  • DOI: 10.1140/epjst/e2008-00747-2

A singular thermodynamically consistent temperature at the origin of the anomalous behavior of liquid water
journal, December 2012

  • Mallamace, Francesco; Corsaro, Carmelo; Stanley, H. Eugene
  • Scientific Reports, Vol. 2, Issue 1
  • DOI: 10.1038/srep00993

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

  • Xu, Yuntao; Petrik, Nikolay G.; Smith, R. Scott
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 52
  • DOI: 10.1073/pnas.1611395114

The anomalous behavior of the density of water in the range 30 K < T < 373 K
journal, November 2007

  • Mallamace, F.; Branca, C.; Broccio, M.
  • Proceedings of the National Academy of Sciences, Vol. 104, Issue 47
  • DOI: 10.1073/pnas.0706504104

Water's second glass transition
journal, October 2013

  • Amann-Winkel, K.; Gainaru, C.; Handle, P. H.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 44
  • DOI: 10.1073/pnas.1311718110

Reanalysis of the density of liquid water in the range 0–150 °C and 0–1 kbar
journal, January 1975

  • Kell, G. S.
  • The Journal of Chemical Physics, Vol. 62, Issue 9
  • DOI: 10.1063/1.430986

Universal Form of the Low-Energy (2 to 10 meV) Vibrational Spectrum of Glasses
journal, January 1990

Vibrational Spectrum of Topologically Disordered Systems
journal, August 2001

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

  • Goldstein, Martin
  • The Journal of Chemical Physics, Vol. 51, Issue 9
  • DOI: 10.1063/1.1672587

PVT Properties of Water and Mercury
journal, May 1971

  • Grindley, T.; Lind, John E.
  • The Journal of Chemical Physics, Vol. 54, Issue 9
  • DOI: 10.1063/1.1675455

Possible relation of water structural relaxation to water anomalies
journal, March 2013

  • Mallamace, F.; Corsaro, C.; Stanley, H. E.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 13
  • DOI: 10.1073/pnas.1221805110

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

Little evidence for dynamic divergences in ultraviscous molecular liquids
journal, July 2008

  • Hecksher, Tina; Nielsen, Albena I.; Olsen, Niels Boye
  • Nature Physics, Vol. 4, Issue 9
  • DOI: 10.1038/nphys1033

Depolarized light scattering studies of the boson peak and the transversal phonons in a glass-forming liquid: OTP
journal, September 1994

What Don't We Know?
journal, July 2005

The Role of Hydrogen Bonding in the Folding/Unfolding Process of Hydrated Lysozyme: A Review of Recent NMR and FTIR Results
journal, November 2018

  • Mallamace, Domenico; Fazio, Enza; Mallamace, Francesco
  • International Journal of Molecular Sciences, Vol. 19, Issue 12
  • DOI: 10.3390/ijms19123825

Supercooled and Glassy Water
journal, June 2003

  • Debenedetti, Pablo G.; Stanley, H. Eugene
  • Physics Today, Vol. 56, Issue 6
  • DOI: 10.1063/1.1595053

Heterogeneity and growing length scales in the dynamics of kinetically constrained lattice gases in two dimensions
journal, October 2005

Multiscale materials modelling at the mesoscale
journal, August 2013

  • Yip, Sidney; Short, Michael P.
  • Nature Materials, Vol. 12, Issue 9
  • DOI: 10.1038/nmat3746

Observation of the density minimum in deeply supercooled confined water
journal, May 2007

  • Liu, D.; Zhang, Y.; Chen, C. -C.
  • Proceedings of the National Academy of Sciences, Vol. 104, Issue 23
  • DOI: 10.1073/pnas.0701352104

The density of supercooled water. II. Bulk samples cooled to the homogeneous nucleation limit
journal, October 1987

  • Hare, D. E.; Sorensen, C. M.
  • The Journal of Chemical Physics, Vol. 87, Issue 8
  • DOI: 10.1063/1.453710

Structure of Water and Hydrophobic Bonding in Proteins. I. A Model for the Thermodynamic Properties of Liquid Water
journal, June 1962

  • Némethy, George; Scheraga, Harold A.
  • The Journal of Chemical Physics, Vol. 36, Issue 12
  • DOI: 10.1063/1.1732472

Model for Melting‐Curve Maxima at High Pressure
journal, April 1967

  • Rapoport, Eliezer
  • The Journal of Chemical Physics, Vol. 46, Issue 8
  • DOI: 10.1063/1.1841150

The fragile-to-strong dynamical crossover and the system viscoelasticity in attractive glass forming colloids
journal, August 2015

Fast Dynamics and Stabilization of Proteins: Binary Glasses of Trehalose and Glycerol
journal, June 2004

Confined Water as Model of Supercooled Water
journal, March 2016

Escaping free-energy minima
journal, September 2002

  • Laio, A.; Parrinello, M.
  • Proceedings of the National Academy of Sciences, Vol. 99, Issue 20
  • DOI: 10.1073/pnas.202427399

Viscosity of glass-forming liquids
journal, November 2009

  • Mauro, J. C.; Yue, Y.; Ellison, A. J.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 47
  • DOI: 10.1073/pnas.0911705106

Size, separation, structural order and mass density of molecules packing in water and ice
journal, October 2013

  • Huang, Yongli; Zhang, Xi; Ma, Zengsheng
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep03005

The Boson peak in supercooled water
journal, June 2013

  • Kumar, Pradeep; Wikfeldt, K. Thor; Schlesinger, Daniel
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01980

Formation of Glasses from Liquids and Biopolymers
journal, March 1995

Relaxation and phonons in viscous and glassy orthoterphenyl by neutron scattering
journal, September 1993

  • Wuttke, J.; Kiebel, M.; Bartsch, E.
  • Zeitschrift f�r Physik B Condensed Matter, Vol. 91, Issue 3
  • DOI: 10.1007/BF01344065

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

Some considerations on the water polymorphism and the liquid-liquid transition by the density behavior in the liquid phase
journal, July 2019

  • Mallamace, Francesco; Corsaro, Carmelo; Mallamace, Domenico
  • The Journal of Chemical Physics, Vol. 151, Issue 4
  • DOI: 10.1063/1.5095687
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: