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• W2897966160 abstract "A two-dimensional (2D) $J$-resolved magic-angle spinning nuclear magnetic resonance (NMR) spectrum of silica glass at $^{29}mathrm{Si}$ natural abundance levels, 4.7%, was measured using the shifted-echo phase-incremented echo train acquisition (SE-PIETA) pulse sequence. At $^{29}mathrm{Si}$ natural abundance levels the ${J}_{text{Si-O-Si}}$ coupling splittings appear as overlapping doublet patterns arising from isolated $^{29}mathrm{Si}ensuremath{-}mathrm{O}ensuremath{-}^{29}mathrm{Si}$ linkages. The experimental 2D $J$-resolved spectrum is analyzed to obtain a bivariate probability distribution correlating the central Si-O-Si angle of a ${mathrm{Q}}^{4}ensuremath{-}{mathrm{Q}}^{4}$ linkage to its mean Si-O-Si angle (seven angles) using relationships between $^{29}mathrm{Si}$ isotropic chemical shifts and geminal ${J}_{text{Si-O-Si}}$ coupling of a ${mathrm{Q}}^{4}ensuremath{-}{mathrm{Q}}^{4}$ to its local structure. To obtain a self-consistent bivariate probability distribution it was necessary to introduce an additional dependence of the $^{29}mathrm{Si}$ chemical shift of a ${mathrm{Q}}^{4}$ on mean Si-O distance as well as mean Si-O-Si angle. The implication of this necessary modification is a positive correlation between Si-O-Si angle and Si-O distance in the silica glass, consistent with recent $^{17}mathrm{O}$ NMR measurements on ambient and densified silica glasses but running opposite to the trend generally found in crystalline silica polymorphs. From the analysis of the $^{29}mathrm{Si}$ 2D $J$-resolved spectrum we determine a Si-O-Si bond angle distribution in silica glass as having a mean at $147.{8}^{ensuremath{circ}}$, a mode at ${147}^{ensuremath{circ}}$, and a standard deviation of $10.{7}^{ensuremath{circ}}$. Our statistical model for analyzing the experimental $^{29}mathrm{Si}$ 2D $J$-resolved spectrum also indicates that the individual Si-O-Si bond angle distributions are relatively uncorrelated." @default.
• W2897966160 created "2018-10-26" @default.
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• W2897966160 date "2018-10-08" @default.
• W2897966160 modified "2023-10-17" @default.
• W2897966160 title "Correlating structural distributions in silica glass with two-dimensional <mml:math xmlns:mml=http://www.w3.org/1998/Math/MathML><mml:mi>J</mml:mi></mml:math> -resolved spectroscopy" @default.
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• W2897966160 doi "https://doi.org/10.1103/physrevb.98.134202" @default.
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