(Ba1-xSrx)TiO₃ (BST, 0.4< x <0.65) single crystals were successfully grown by the TSSG (Top-Seeded Solution Growth) method, using a commercial [100] SrTiO₃ or as-grown [100] BST single crystals as seed crystals. To obtain the BST single crystals with various compositions x, the Ba/sr molar ratios in the solutions were systematically controlled while the Ti ion content among all cations was fixed at 67 mol%. A linear regression curve between their x values and the molar ratios of Sr/(Ba + Sr) in the solutions could be obtained, which in turn could used to select the initial composition to produce BST crystal with an aimed x value. In addition, the isothermal growth was found more effective for obtaining a compositional uniformity than a slow cooling process.
