Abstract
Micron-sized water droplets in a cryogenic flow tube were probed by IR spectroscopy. The analysis of the IR spectra suggests that there is a relative increase of about 30% in the fraction, f(L), of low density domains in water on cooling over the temperature range between 300 and 240 K. The results derived from the experiments agree qualitatively with those of molecular dynamics (MD) simulations in terms of the increase in the f(L) values. The MD simulations show that the intensities of the mode at about 100 cm(-1) for the molecules in the low density domains are reduced in comparison to the average, while the intensities and frequencies of the librational mode at 600 cm(-1) are increased. Furthermore, the reorientations (dielectric relaxation times) in these domains are found to be somewhat slower, pointing to the fact that these low density "cages" live longer than the average local molecular environments in supercooled water.
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