Sintering Aid‐Assisted Growth of 0.95(K0.5Na0.5)NbO3–0.05(Bi0.5Na0.5)(Zr0.85Sn0.15)O3 Single Crystals by the Solid‐State Crystal Growth Method and Their Characterization

In this work, 0.95(K 0.5 Na 0.5 )NbO 3 –0.05(Bi 0.5 Na 0.5 )(Zr 0.85 Sn 0.15 )O 3 (KNN–BNZS) lead‐free piezoelectric single crystals are grown by the solid‐state crystal growth (SSCG) method and their phase transitions and properties characterized. Addition of an appropriate amount of Li 2 CO 3 and Bi 2 O 3 sintering aids considerably promotes single‐crystal growth. Chemical composition of the single crystal is similar to the nominal composition with a slight deficiency in Na and K as evaluated by electron probe microanalysis (EPMA). X‐Ray diffraction (XRD), electrical property measurements, and temperature‐controlled Raman scattering reveal that the phase transition near room temperature is from a rhombohedral to an orthorhombic or tetragonal phase. Wide temperature range Raman scattering and dielectric properties consistently indicate transitions associated with the phase transformations or boundaries of a phase coexistence region and further details. Nontrivial frequency dependence of dielectric properties is successfully parameterized by capacitance relaxations described by Debye and Cole–Cole responses with special constant phase elements with fixed exponents of 0.5 (Warburg elements). High‐frequency dielectric constants and additional dielectric relaxations and dc relaxations are deconvoluted. The modeling parameters indicate the phase transition temperatures (or boundaries of the phase coexistence region) unambiguously. Polarization–electric field and bipolar strain–electric field hysteresis loops show that the single crystal is a classic lossy ferroelectric material.