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The  29 Si MAS NMR spectra of nine pyrope-grossular garnet solid solutions were recorded along with their mid and far infrared spectra. The  29 Si MAS NMR spectra of pyrope and grossular measured previously show one single resonance at -72.0 and -83.9 ppm, respectively. A maximum of up to 13 resonances were observed in composition Py 50 Gr 50  indicating that  29 Si MAS NMR spectroscopy can record both first and second shell dodecahedral interactions in garnet. Complete resonance assignments were done by qualitative crystal chemical considerations combined with the comparison of fitted peak intensities with the calculated probabilities for the various possible localized chemical environments around the Si tetrahedra. The NMR spectra of garnets with compositions Py 90 Gr 10 , Py 10 Gr 90 ,and Py 05 Gr 95  are consistent with a random distribution of the divalent cations Ca and Mg on the triangular dodecahedral sites. Garnets with compositions between 0.15 ≤ X Ca  ≤ 0.75 show evidence for deviations from random mixing. No overt evidence is found to support a model of local cation order in the most pyrope-rich compositions, which had been proposed on the basis of the asymmetric volumes of mixing along the binary. Powder IR spectra show no additional bands in the solid solutions compared to the end-members, and hence all solid solution compositions are consistent with space group Ia3̅d.

A 29 Si MAS NMR and IR spectroscopic investigation of synthetic pyrope-grossular garnet solid solutions