Core/shell ZrTiO4/LiAlSi2O6 nanocrystals: A synchrotron X-ray diffraction study of high-pressure compression

In situ synchrotron X-ray diffraction studies have been performed on an optically transparent lithium-aluminosilicate glass-ceramic composite with nanometer-sized LiAlSi2O6 crystals embedded in a host matrix. The pressure-induced evolution of X-ray diffraction patterns was followed in compression up to 50 GPa and in subsequent decompression to ambient conditions. In the low-pressure range, the diffraction patterns illustrated a progressive shift and broadening of the diffraction lines consistent with a gradual densification of the LiAlSi2O6 phase. The unit cell volume of the LiAlSi2O6 nanocrystalline phase calculated for the compression sequence between ambient pressure and 12.5 GPa decreased by about 13.5%. At higher pressures, the diffraction patterns displayed considerable line broadenings indicating a partial amorphization of the nanocrystalline phase. Additionally, the patterns revealed the increasing presence of the ZrTiO4 phase which was nucleated in the host matrix prior to the crystallization of the LiAlSi2O6 main nanocrystalline phase. The diffraction pattern of the composite quenched from 50 GPa to ambient pressure conditions did not show full reversibility of pressure-induced changes. Despite the dominating presence of the broad diffraction bands, the diffraction pattern of the pressure-quenched material suggested that the decompressed structure carries at least a partial signature of the initial ambient LiAlSi2O6 phase.