Stoichiometric glassy germanate is an important material in geophysics and materials science. Despite the binary Li2O-GeO2 system being primitive, its crystallization mechanism remains undetermined. In this study, we investigated crystallization and structural ordering in glassy ferroelectric Li2Ge4O9. Using isothermally and nonisothermally prepared samples, we demonstrated that the glassy Li 2Ge4O9 shows no direct structural change to the stoichiometric phase; it rather forms α-GeO2 nanocrystals, i.e., it undergoes successive phase transformation. The results suggest that the metastable immiscibility is related to the ordering that occurs prior to crystallization of the stoichiometric phase.
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