Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: The Boson peak in confined water: An experimental investigation of the liquid-liquid phase transition hypothesis

Abstract

The Boson peak (BP) of deeply cooled confined water is studied by using inelastic neutron scattering (INS) in a large interval of the (P, T) phase plane. By taking into account the different behavior of such a collective vibrational mode in both strong and fragile glasses as well as in glass-forming materials, we were able to determine the Widom line that characterizes supercooled bulk water within the frame of the liquid-liquid phase transition (LLPT) hypothesis. The peak frequency and width of the BP correlated with the water polymorphism of the LLPT scenario, allowing us to distinguish the “low-density liquid” (LDL) and “high-density liquid” (HDL) phases in deeply cooled bulk water.Moreover, the BP properties afford a further confirmation of theWidom line temperature T W as the (P, T) locus in which the local structure of water transforms from a predominately LDL form to a predominately HDL form.

Authors:
 [1];  [2];  [3];  [4];  [4]
+ Show Author Affiliations
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering; Univ. of Messina (Italy). Dept. of Physics and Earth Sciences; National Research Council (CNR) Inst. for Chemical-Physical Processes (IPCF), Messina (Italy)
  2. Univ. of Messina (Italy). Dept. of Physics and Earth Sciences; National Research Council (CNR) Inst. for Chemical-Physical Processes (IPCF), Messina (Italy)
  3. Dept. of Environmental, Security, Territory, Food, and Health Sciences, Messina (Italy)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Nuclear Science and Engineering
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1437127
Grant/Contract Number:  
FG02-90ER45429
Resource Type:
Accepted Manuscript
Journal Name:
Frontiers of Physics
Additional Journal Information:
Journal Volume: 10; Journal Issue: 5; Journal ID: ISSN 2095-0462
Publisher:
Springer
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; supercooled water; liquid-liquid phase transition (LLPT); inelastic neutron scattering

Citation Formats

Mallamace, Francesco, Corsaro, Carmelo, Mallamace, Domenico, Wang, Zhe, and Chen, Sow-Hsin. The Boson peak in confined water: An experimental investigation of the liquid-liquid phase transition hypothesis. United States: N. p., 2015. Web. doi:10.1007/s11467-015-0487-8.
Copy to clipboard
Mallamace, Francesco, Corsaro, Carmelo, Mallamace, Domenico, Wang, Zhe, & Chen, Sow-Hsin. The Boson peak in confined water: An experimental investigation of the liquid-liquid phase transition hypothesis. United States. https://doi.org/10.1007/s11467-015-0487-8
Copy to clipboard
Mallamace, Francesco, Corsaro, Carmelo, Mallamace, Domenico, Wang, Zhe, and Chen, Sow-Hsin. Sat . "The Boson peak in confined water: An experimental investigation of the liquid-liquid phase transition hypothesis". United States. https://doi.org/10.1007/s11467-015-0487-8. https://www.osti.gov/servlets/purl/1437127.
Copy to clipboard
@article{osti_1437127,
title = {The Boson peak in confined water: An experimental investigation of the liquid-liquid phase transition hypothesis},
author = {Mallamace, Francesco and Corsaro, Carmelo and Mallamace, Domenico and Wang, Zhe and Chen, Sow-Hsin},
abstractNote = {The Boson peak (BP) of deeply cooled confined water is studied by using inelastic neutron scattering (INS) in a large interval of the (P, T) phase plane. By taking into account the different behavior of such a collective vibrational mode in both strong and fragile glasses as well as in glass-forming materials, we were able to determine the Widom line that characterizes supercooled bulk water within the frame of the liquid-liquid phase transition (LLPT) hypothesis. The peak frequency and width of the BP correlated with the water polymorphism of the LLPT scenario, allowing us to distinguish the “low-density liquid” (LDL) and “high-density liquid” (HDL) phases in deeply cooled bulk water.Moreover, the BP properties afford a further confirmation of theWidom line temperature T W as the (P, T) locus in which the local structure of water transforms from a predominately LDL form to a predominately HDL form.},
doi = {10.1007/s11467-015-0487-8},
journal = {Frontiers of Physics},
number = 5,
volume = 10,
place = {United States},
year = {Sat Dec 05 00:00:00 EST 2015},
month = {Sat Dec 05 00:00:00 EST 2015}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1007/s11467-015-0487-8
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: The pressure-temperature phase diagram of bulk water in the frame of its polimorphism and of the LLPT model. The LDA, the HDA, the LDL and HDL phases and the Widom line (the locus of TW, dotted line) are reported together with the melting Tm, the homogeneous nucleation temperaturemore » TH and the crystallization TX loci. The LL critical point C’ and the line of the density maxima, Tmd, are also reported. Dark red and green large symbols, as illustrated in the text, deal with the findings of this work.« less
All figures and tables (5 total)
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:

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

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

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

The boson peak of deeply cooled confined water reveals the existence of a low-temperature liquid-liquid crossover
journal, November 2014

  • Cupane, Antonio; Fomina, Margarita; Schirò, Giorgio
  • The Journal of Chemical Physics, Vol. 141, Issue 18
  • DOI: 10.1063/1.4895793

Phase behaviour of metastable water
journal, November 1992

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

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

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

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

  • Wikfeldt, K. T.; Nilsson, A.; Pettersson, L. G. M.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 44
  • DOI: 10.1039/c1cp22076d

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

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

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

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

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

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

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

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

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

Multiscale materials modelling at the mesoscale
journal, August 2013

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

Boson Peak in Deeply Cooled Confined Water: A Possible Way to Explore the Existence of the Liquid-to-Liquid Transition in Water
journal, June 2014

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

Pressure and density dependence of the boson peak in polymers
journal, October 2008

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

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

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

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

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

How Much Can Human Life Span Be Extended?
journal, July 2005

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

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 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

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

  • Wikfeldt, K. T.; Nilsson, A.; Pettersson, L. G. M.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 44
  • DOI: 10.1039/c1cp22076d

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

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

The boson peak of deeply cooled confined water reveals the existence of a low-temperature liquid-liquid crossover
journal, November 2014

  • Cupane, Antonio; Fomina, Margarita; Schirò, Giorgio
  • The Journal of Chemical Physics, Vol. 141, Issue 18
  • DOI: 10.1063/1.4895793

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

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

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

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

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

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

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Molecular-scale processes affecting growth rates of ice at moderate supercooling
    journal, July 2018

    Two structural relaxations in protein hydration water and their dynamic crossovers
    journal, July 2016

    • Camisasca, G.; De Marzio, M.; Corradini, D.
    • The Journal of Chemical Physics, Vol. 145, Issue 4
    • DOI: 10.1063/1.4959286
      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Fig. 1 (p. 2)figure
      Fig. 2 (p. 3)figure
      Fig. 3 (p. 5)figure
      Fig. 4 (p. 5)figure
      Fig. 5 (p. 6)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: