Liquid immiscibility in a CTGS (Ca₃TaGa₃Si₂O₁₄) melt

Although many studies have indicated that Ca₃TaGa₃Si₂O₁₄ (CTGS) grows congruently from a stoichiometric melt when using the Czochralski (Cz) technique, the occurrence of a secondary phase during growth when using the micro-pulling down (μ-PD) technique has been reported. We have examined the detailed growth mechanism of μ-PD grown CTGS as well as its congruency. Differential thermal analysis (DTA) at an elevated temperature up to 1650 °C shows no peaks associated with the presence of a secondary phase, whereas a secondary phase related peak was detected at an elevated temperature up to 1490 °C with the same heating rate. Back-scattered electron images (BEIs) revealed the occurrence of Ca₃Ta₂Ga₄O₁₄ (CTG) as a secondary phase. The secondary phase appears at the very early stage of growth, which is not possible to explain by a eutectic reaction. The experimental results suggest that liquid immiscibility was present in the melt at around 1490 °C during the growth of s-CTGS. Liquid immiscibility produces Si-rich and Si-poor melts, from which different phases with different compositions are solidified. The μ-PD technique poses a more static environment in the melt than that of Cz technique due to low melt convection and the lack of stirring, which enables liquid immiscibility to emerge.