The development of lead-free ferroelectric materials with competitive functional performance remains a key objective in condensed matter physics and materials science. Although perovskite-based solid solutions provide a versatile platform for tuning electromechanical response, their practical utilisation is frequently hindered by limited control over compositional homogeneity, short-range structural correlations, and synthesis reproducibility.
Here, we introduce a crystal-growth-based synthesis strategy enabling the preparation of high-quality ceramics and single crystals of complex Pb-free ferroelectrics without reliance on conventional multi-step solid-state processing. Floating-zone and pedestal growth techniques are employed to achieve enhanced compositional uniformity and controlled local structural order, both critical for stabilising functional phases and maximising macroscopic response.
The approach is illustrated on representative systems, including (Ba,Ca)TiO3-based compounds and rare-earth RE2(Ti,Zr)2O7 oxides. Diffraction methods combined with high-resolution microscopy reveal a high degree of structural homogeneity and well-defined crystallographic features. These structural improvements translate into reproducible and robust functional properties, comparable to or surpassing those of materials prepared by standard routes.
More generally, the proposed synthesis concept provides a transferable framework for the design and investigation of advanced ferroic systems. It supports systematic exploration of composition–structure–property relationships, particularly in regimes where local disorder and structural complexity extend beyond the scope of conventional crystallographic descriptions.