Abstract: | Compositional segregation usually has negative effects on the growth of solid solution ferroelectric single crystals of Pb(In1/2Nb1/2)O3‐Pb(Mg1/3Nb2/3)O3‐PbTiO3 (abbr. PIN‐PMN‐PT or PIMNT). A modified Bridgman method was adopted in this work to control the segregation and improve the compositional homogeneity significantly. The characteristic of this work is to use multiround growths and gradient composition raw materials in order to keep the PbTiO3 concentration constant during the crystal growth. As an example, the two‐round growth of ternary PIN‐PMN‐PT single crystal is conducted in the same Pt crucible with gradient raw materials, where the first‐round boule was used as the seed crystal for the second‐round growth. Our results show that the as‐grown (Ф80 mm × 270 mm) PIN‐PMN‐PT crystals exhibit higher phase transition temperatures (Tc∼180 °C, Tr/t∼110 °C) and larger coercive field (Ec∼5–5.5 kV/cm), which are much better than the performances of Pb(Mg1/3Nb2/3)O3‐PbTiO3 crystals, and similar dielectric and piezoelectric performances (ε∼5000, tanδ∼1.25%, d33∼1500 pC/N, kt∼60%). And about 85 percent of the crystal boule grown by the two‐round growth technique could maintain its compositions around the morphotropic phase boundary. |