In this work, we present the first crystal growth of cubic Tb2O3 single crystals by a controlled atmosphere flux method which uses a heavy metal free solvent working at less than half the melting temperature of this sesquioxide. Cubic millimeter-sized crystals extracted from as-grown boules are phase (powder XRD) and chemically (GDMS) pure and exhibit a Verdet constant in the visible and near-infrared spectral ranges, which is at least three times higher than that of a commercial Tb3Ga5O12 (TGG) crystal. The 1.36 mm thick crystals display a transmission coefficient higher than 77% over the 525 nm–1.38 μm spectral range. The absorption spectrum, magnetic susceptibility and specific heat measurements on the single crystals confirm the absence of detectable Tb4+ cations and other impurities.
Piezoelectric single crystals based on the perovskite ferroelectric system (K,Na)NbO3 have been widely investigated over the past 20 years due to large piezoelectric coefficients, high transition temperatures, low density, and the nontoxic chemical composition. Various crystal growth methods were examined, including high-temperature solution growth, solid-state crystal growth, Bridgman–Stockbarger method, and the floating zone method. Increased understanding of the crystal growth process and post-growth treatments resulted in improved crystal quality and larger sizes. Recently, crystals with high piezoelectric and electromechanical coupling coefficients exceeding 1000 pC/N and 0.90, respectively, were reported. Moreover, their large potential for high-frequency ultrasonic medical imaging was demonstrated. This work provides a review of the development of piezoelectric (K,Na)NbO3-based single crystals, including their growth, defect chemistry, domain structures, electromechanical properties, and applications. Approaches for reducing growth defects, controlling point defects, and domain engineering are discussed. The remaining open issues are presented and an outlook on the future is provided.
is a perovskite that remains in the simple cubic phase at all temperatures, hence with no first-order Raman-active phonon mode allowed by symmetry. Yet, it exhibits an intense Raman spectrum with sharp and well-defined features. Here, we report the evolution of the Raman spectrum of single crystals in a broad temperature range (4–1200 K) and discuss its origin with the support of detailed first-principle calculations of the lattice dynamics. Phonon calculations are performed not only for the cubic phase of , but also for the low-symmetry phases with octahedra tilts that have been suspected to exist at the nanoscale. We show that the Raman spectrum shows no direct evidence for these nanodomains, but can instead be explained by classical second-order Raman scattering. We provide an assignment of the dominant features to phonon mode combinations. In particular, we show that the high frequency range of the spectrum is dominated by overtones and shows an image of the phonon density of states corresponding to the stretching modes of the oxygen octahedra.