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Title: Water: A Tale of Two Liquids

Abstract

Water is the most abundant liquid on earth and also the substance with the largest number of anomalies in its properties. It is a prerequisite for life and as such a most important subject of current research in chemical physics and physical chemistry. In spite of its simplicity as a liquid, it has an enormously rich phase diagram where different types of ices, amorphous phases, and anomalies disclose a path that points to unique thermodynamics of its supercooled liquid state that still hides many unraveled secrets. In this review we describe the behavior of water in the regime from ambient conditions to the deeply supercooled region. The review describes simulations and experiments on this anomalous liquid. Several scenarios have been proposed to explain the anomalous properties that become strongly enhanced in the supercooled region. Among those, the second critical-point scenario has been investigated extensively, and at present most experimental evidence point to this scenario. Starting from very low temperatures, a coexistence line between a high-density amorphous phase and a low-density amorphous phase would continue in a coexistence line between a high-density and a low-density liquid phase terminating in a liquid–liquid critical point, LLCP. On approaching this LLCP from the one-phasemore » region, a crossover in thermodynamics and dynamics can be found. This is discussed based on a picture of a temperature-dependent balance between a high-density liquid and a low-density liquid favored by, respectively, entropy and enthalpy, leading to a consistent picture of the thermodynamics of bulk water. Ice nucleation is also discussed, since this is what severely impedes experimental investigation of the vicinity of the proposed LLCP. Experimental investigation of stretched water, i.e., water at negative pressure, gives access to a different regime of the complex water diagram. Different ways to inhibit crystallization through confinement and aqueous solutions are discussed through results from experiments and simulations using the most sophisticated and advanced techniques. These findings represent tiles of a global picture that still needs to be completed. In conclusion, some of the possible experimental lines of research that are essential to complete this picture are explored.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [7];  [8];  [9];  [10];  [11];  [7];  [12];  [13];  [14];  [2]
+ Show Author Affiliations
  1. Dipartimento di Matematica e Fisica, Università Roma Tre, Via della Vasca Navale 84, 00146 Rome, Italy
  2. Department of Physics, AlbaNova University Center, Stockholm University, SE-106 91 Stockholm, Sweden
  3. Department of Chemistry and Biochemistry, Arizona State University, Tempe, Arizona 85287, United States
  4. Institute for Physical Science and Technology and Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, Maryland 20742, United States
  5. Institut Lumière Matière, UMR5306 Université Claude Bernard Lyon 1-CNRS, Université de Lyon, Institut Universitaire de France, 69622 Villeurbanne, France
  6. Department of Chemistry, Indian Institute of Technology Delhi, Hauz Khas, New Delhi 110016, India
  7. Center for Polymer Studies and Department of Physics, Boston University, Boston, Massachusetts 02215, United States
  8. Institute of Physical Chemistry, University of Innsbruck, 6020 Innsbruck, Austria
  9. Department of Chemical and Biological Engineering, Princeton University, Princeton, New Jersey 08544, United States
  10. Institute of Industrial Science, University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan, School of Mathematics, University of Bristol, Bristol BS8 1TW, United Kingdom
  11. Biomedical and X-ray Physics, Department of Applied Physics, AlbaNova University Center, KTH Royal Institute of Technology, SE-106 91 Stockholm, Sweden
  12. Institute of Industrial Science, University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan
  13. Departamento de Quimica Fisica, Facultad de Ciencias Quimicas, Universidad Complutense de Madrid, 28040 Madrid, Spain
  14. International Centre for Quantum Materials and School of Physics, Peking University, Beijing 100871, China, Collaborative Innovation Center of Quantum Matter, Beijing 100871, China
Publication Date:
Research Org.:
Princeton Univ., NJ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Swedish Research Council (SRC); European Research Council (ERC); Japan Society for the Promotion of Science (JSPS); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1355807
Alternate Identifier(s):
OSTI ID: 1435719
Grant/Contract Number:  
SC0002128; 09-BLAN-0404-01; CHE 12-13265; 21224011; 25000002; 11174006; 11290162; 11525520; 2012CB921404; 2015CB856801
Resource Type:
Published Article
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Name: Chemical Reviews Journal Volume: 116 Journal Issue: 13; Journal ID: ISSN 0009-2665
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gallo, Paola, Amann-Winkel, Katrin, Angell, Charles Austen, Anisimov, Mikhail Alexeevich, Caupin, Frédéric, Chakravarty, Charusita, Lascaris, Erik, Loerting, Thomas, Panagiotopoulos, Athanassios Zois, Russo, John, Sellberg, Jonas Alexander, Stanley, Harry Eugene, Tanaka, Hajime, Vega, Carlos, Xu, Limei, and Pettersson, Lars Gunnar Moody. Water: A Tale of Two Liquids. United States: N. p., 2016. Web. doi:10.1021/acs.chemrev.5b00750.
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Gallo, Paola, Amann-Winkel, Katrin, Angell, Charles Austen, Anisimov, Mikhail Alexeevich, Caupin, Frédéric, Chakravarty, Charusita, Lascaris, Erik, Loerting, Thomas, Panagiotopoulos, Athanassios Zois, Russo, John, Sellberg, Jonas Alexander, Stanley, Harry Eugene, Tanaka, Hajime, Vega, Carlos, Xu, Limei, & Pettersson, Lars Gunnar Moody. Water: A Tale of Two Liquids. United States. https://doi.org/10.1021/acs.chemrev.5b00750
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Gallo, Paola, Amann-Winkel, Katrin, Angell, Charles Austen, Anisimov, Mikhail Alexeevich, Caupin, Frédéric, Chakravarty, Charusita, Lascaris, Erik, Loerting, Thomas, Panagiotopoulos, Athanassios Zois, Russo, John, Sellberg, Jonas Alexander, Stanley, Harry Eugene, Tanaka, Hajime, Vega, Carlos, Xu, Limei, and Pettersson, Lars Gunnar Moody. Tue . "Water: A Tale of Two Liquids". United States. https://doi.org/10.1021/acs.chemrev.5b00750.
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@article{osti_1355807,
title = {Water: A Tale of Two Liquids},
author = {Gallo, Paola and Amann-Winkel, Katrin and Angell, Charles Austen and Anisimov, Mikhail Alexeevich and Caupin, Frédéric and Chakravarty, Charusita and Lascaris, Erik and Loerting, Thomas and Panagiotopoulos, Athanassios Zois and Russo, John and Sellberg, Jonas Alexander and Stanley, Harry Eugene and Tanaka, Hajime and Vega, Carlos and Xu, Limei and Pettersson, Lars Gunnar Moody},
abstractNote = {Water is the most abundant liquid on earth and also the substance with the largest number of anomalies in its properties. It is a prerequisite for life and as such a most important subject of current research in chemical physics and physical chemistry. In spite of its simplicity as a liquid, it has an enormously rich phase diagram where different types of ices, amorphous phases, and anomalies disclose a path that points to unique thermodynamics of its supercooled liquid state that still hides many unraveled secrets. In this review we describe the behavior of water in the regime from ambient conditions to the deeply supercooled region. The review describes simulations and experiments on this anomalous liquid. Several scenarios have been proposed to explain the anomalous properties that become strongly enhanced in the supercooled region. Among those, the second critical-point scenario has been investigated extensively, and at present most experimental evidence point to this scenario. Starting from very low temperatures, a coexistence line between a high-density amorphous phase and a low-density amorphous phase would continue in a coexistence line between a high-density and a low-density liquid phase terminating in a liquid–liquid critical point, LLCP. On approaching this LLCP from the one-phase region, a crossover in thermodynamics and dynamics can be found. This is discussed based on a picture of a temperature-dependent balance between a high-density liquid and a low-density liquid favored by, respectively, entropy and enthalpy, leading to a consistent picture of the thermodynamics of bulk water. Ice nucleation is also discussed, since this is what severely impedes experimental investigation of the vicinity of the proposed LLCP. Experimental investigation of stretched water, i.e., water at negative pressure, gives access to a different regime of the complex water diagram. Different ways to inhibit crystallization through confinement and aqueous solutions are discussed through results from experiments and simulations using the most sophisticated and advanced techniques. These findings represent tiles of a global picture that still needs to be completed. In conclusion, some of the possible experimental lines of research that are essential to complete this picture are explored.},
doi = {10.1021/acs.chemrev.5b00750},
journal = {Chemical Reviews},
number = 13,
volume = 116,
place = {United States},
year = {Tue Jul 05 00:00:00 EDT 2016},
month = {Tue Jul 05 00:00:00 EDT 2016}
}
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Crossover Equation and the Vapor Pressure of Supercooled Water
journal, November 2009

The Boson peak in supercooled water
journal, June 2013

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Formation of Glasses from Liquids and Biopolymers
journal, March 1995

Water and water-like liquids: relationships between structure, entropy and mobility
journal, January 2013

  • Nayar, Divya; Chakravarty, Charusita
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 34
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Relation between the two-body entropy and the relaxation time in supercooled water
journal, January 2015

Tuning the Liquid-Liquid Transition by Modulating the Hydrogen-Bond Angular Flexibility in a Model for Water
journal, July 2015

Liquid–liquid transition without macroscopic phase separation in a water–glycerol mixture
journal, March 2012

  • Murata, Ken-ichiro; Tanaka, Hajime
  • Nature Materials, Vol. 11, Issue 5
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The existence of supercooled liquid water at 150?K
journal, April 1999

  • Smith, R. Scott; Kay, Bruce D.
  • Nature, Vol. 398, Issue 6730
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