On the Relationships between Low-Density Amorphous Solid Water and Ice Ih

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Abstract
New experimental and theoretical studies of low-density amorphous solid water (H2O(as)) and of polycrystalline ice lh are reported and integrated with other available data. A variety of evidence is put forward to support the conclusion that low-density H20(as) is derived from ice lh by slightly increasing the dispersion in the O—O separation and by introducing a distribution O—O—O angles (width c. 8°). Our theoretical analysis focusses attention on the consequences of strong intermolecular coupling of OH oscillators. The vibrational modes of both ice lh and H20(as) are found to be complex mixtures of molecular motions, so the identification of regions of the Raman or infrared spectra of these materials with particular isolated molecule modes is not useful. The theory developed gives a good, but not perfect, account of the OH stretching regions of the observed Raman and infrared spectra of ice lh and, to a lesser degree of low-density H20(as).

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