Abstract
Random network models of glass structures1 provide satisfactory qualitative descriptions of many properties of glasses (see reviews in refs 2–4). However, to obtain good quantitative agreement between theoretical analyses and experimental observations5–11 it is often necessary to assume that specific ring structures in the random networks have special importance. In the case of vitreous silica (v-SiO2), distributions of loops of SiO4 tetrahedra in the random network have been invoked5–9 to match calculated and experimental X-ray radial distribution functions (RDF). High resolution X-ray photoelectron spectra12 of v-SiO2 and quartz also provide evidence for the occurrence of four-, six- and higher-membered rings of SiO4 tetrahedra in v-SiO2. Raman spectra are also sensitive to local microstructures in vitreous solids. We have therefore examined the question of rings in the structure of v-SiO2 by comparing its Raman spectrum with spectra of crystalline silica polymorphs whose shortest loops contain four (coesite) and six (for example, α-quartz) tetrahedra. This comparison indicates that the sharp shoulder at 490 cm−1 in the spectrum of v-SiO2, previously attributed to a defect structure3 or a longitudinal optic mode14, can be assigned to four-membered ring structure. We discuss here possible basis for the stability of four-membered rings of SiO4 tetrahedra in v-SiO2 at ambient pressure. Possible reasons for the absence of the 490 cm−1 band in the vibrational density-of-states derived for a random network model by Bell and co-workers12,15 are discussed.
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Sharma, S., Mammone, J. & Nicol, M. Raman investigation of ring configurations in vitreous silica. Nature 292, 140–141 (1981). https://doi.org/10.1038/292140a0
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DOI: https://doi.org/10.1038/292140a0
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