In situ observation of the dynamics in the middle stage of spinodal decomposition of a silicate glass via scanning transmission electron microscopy

Real-space observations in the middle stage of spinodal decomposition have not been achieved because of the small sizes and unclear interfaces of the phases. Here, we performed in situ real-space experiments with heating to quantitatively reveal the local dynamics and structures of a calcium aluminosilicate glass in the middle stage of spinodal decomposition by scanning transmission electron microscopy. This glass separate into CaO–Al2O3–SiO2 phase and SiO2 phases. The observations revealed that the CaO–Al2O3–SiO2 phases with low Ca concentrations behaved as if they were in the middle stage, whereas the CaO–Al2O3–SiO2 phases with high Ca concentrations coarsened as if they were in the final stage. This coexistence of stages suggested that the behaviors of the phases depend not only on time, but also on their local relative concentrations. Differing from the well-known final stage of spinodal decomposition, the phases with relatively high Ca concentrations in the middle stage showed peculiar directional migration guided by the phases with relatively low Ca concentrations. These findings have not been observed before and thus have the potential to provide a new way to control the phase-separated structure.