Evidence of the existence of the low-density liquid phase in supercooled, confined water
- 9 January 2007
- journal article
- Published by Proceedings of the National Academy of Sciences in Proceedings of the National Academy of Sciences of the United States of America
- Vol. 104 (2), 424-428
- https://doi.org/10.1073/pnas.0607138104
Abstract
By confining water in a nanoporous structure so narrow that the liquid could not freeze, it is possible to study properties of this previously undescribed system well below its homogeneous nucleation temperature TH = 231 K. Using this trick, we were able to study, by means of a Fourier transform infrared spectroscopy, vibrational spectra (HOH bending and OH-stretching modes) of deeply supercooled water in the temperature range 183 < T < 273 K. We observed, upon decreasing temperature, the building up of a new population of hydrogen-bonded oscillators centered around 3,120 cm(-1), the contribution of which progressively dominates the spectra as one enters into the deeply supercooled regime. We determined that the fractional weight of this spectral component reaches 50% just at the temperature, TL approximately 225 K, where the confined water shows a fragile-to-strong dynamic cross-over phenomenon [Ito, K., Moynihan, C. T., Angell, C. A. (1999) Nature 398:492-494]. Furthermore, the fact that the corresponding OH stretching spectral peak position of the low-density-amorphous solid water occurs exactly at 3,120 cm(-1) [Sivakumar, T. C., Rice, S. A., Sceats, M. G. (1978) J. Chem. Phys. 69:3468-3476.] strongly suggests that these oscillators originate from existence of the low-density-liquid phase derived from the occurrence of the first-order liquid-liquid (LL) phase transition and the associated LL critical point in supercooled water proposed earlier by a computer molecular dynamics simulation [Poole, P. H., Sciortino, F., Essmann, U., Stanley, H. E. (1992) Nature 360:324-328].Keywords
This publication has 33 references indexed in Scilit:
- The fragile-to-strong dynamic crossover transition in confined water: nuclear magnetic resonance resultsThe Journal of Chemical Physics, 2006
- Experimental evidence of a liquid-liquid transition in interfacial waterEurophysics Letters, 2005
- Evidence for Molecular Translational Diffusion during the Crystallization of Amorphous Solid WaterThe Journal of Physical Chemistry B, 1997
- Two Species/Nonideal Solution Model for Amorphous/Amorphous Phase TransitionsMRS Proceedings, 1996
- A Lattice Model of Network-Forming Fluids with Orientation-Dependent Bonding: Equilibrium, Stability, and Implications for the Phase Behavior of Supercooled WaterThe Journal of Physical Chemistry, 1995
- Effect of Hydrogen Bonds on the Thermodynamic Behavior of Liquid WaterPhysical Review Letters, 1994
- Raman isosbestic points from liquid waterThe Journal of Chemical Physics, 1986
- Chemical-bond spectroscopy with neutronsPhysical Review A, 1986
- Isochoric temperature differential of the x-ray structure factor and structural rearrangements in low-temperature heavy waterPhysical Review A, 1983
- Raman scattering and structure of normal and supercooled waterThe Journal of Chemical Physics, 1981