“…While some information has been gained by fitting the isotropic projections of 27 Al 3QMAS NMR spectra into signals from distinct Q Al n (mSi) groups [251], and 29 Si MAS NMR has also been utilized to a minor extent to probe the Al/Si intermixing [63,74], neither of the standard 29 Si and 27 Al NMR tools offers sufficient spectral resolution to address this problem accurately for AS glass networks. Currently, 17 O NMR provides superior insight: the 17 O chemical shift is a sensitive probe to distinguish the relative numbers of Al/Si atoms in its first coordination shell, i.e., to assess the ensemble of {T-O [2] -T 0 } motifs [64,[274][275][276][277][278]. However, it requires expensive 17 O NMR isotopic enrichment, and sometimes fails to provide sufficient resolution and/or accurate signal intensities when applied to multicomponent AS glasses.…”