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Title: Water: A Tale of Two Liquids

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
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [7] ;  [8] ;  [9] ;  [10] ;  [11] ;  [7] ;  [12] ;  [13] ;  [14] ;  [2]
  1. Univ. Roma Tre, Rome (Italy). Dipartimento di Matematica e Fisica
  2. Stockholm Univ. (Sweden). AlbaNova Univ. Center, Dept. of Physics
  3. Arizona State Univ., Tempe, AZ (United States). Dept. of Chemistry and Biochemistry
  4. Univ. of Maryland, College Park, MD (United States). Inst. for Physical Science and Technology and Dept. of Chemical and Biomolecular Engineering
  5. Inst. Lumiere Matiere, Villeurbanne (France)
  6. Indian Inst. of Technology Delhi, Hauz Khas, New Delhi (India). Dept. of Chemistry
  7. Boston Univ., MA (United States). Center for Polymer Studies, Dept. of Physics
  8. Univ. of Innsbruck, Innsbruck (Austria). Inst. of Physical Chemistry
  9. Princeton Univ., NJ (United States). Dept. of Chemical and Biological Engineering
  10. Univ. of Tokyo (Japan). Inst. of Industrial Science; Univ. of Bristol, Bristol (United Kingdom). School of Mathematics
  11. KTH Royal Inst. of Technology, Stockholm (Sweden). AlbaNova Univ. Center, Dept. of Applied Physics, Biomedical and X-ray Physics
  12. Univ. of Tokyo (Japan). Inst. of Industrial Science
  13. Univ. Complutense de Madrid, Madrid (Spain). Dept. de Quimica Fisica
  14. Peking Univ., Beijing (China). International Centre for Quantum Materials and School of Physics; Collaborative Innovation Center of Quantum Matter, Beijing (China)
Publication Date:
Grant/Contract Number:
SC0002128; 09-BLAN-0404-01; CHE 12-13265; 21224011; 25000002; 11174006; 11290162; 11525520; 2012CB921404; 2015CB856801
Published Article
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Volume: 116; Journal Issue: 13; Journal ID: ISSN 0009-2665
American Chemical Society
Research Org:
Princeton Univ., NJ (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); 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 (NNSFC)
Country of Publication:
United States
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1435719