Close-to-Equilibrium Crystallization for Large-Scale and High-Quality Perovskite Single Crystals

The growth of large semiconductor crystals is crucial for advancing modern electronics and optoelectronics. While various crystal growth techniques have been developed for lead halide perovskites, a significant challenge remains: as crystal size increases, performance tends to deteriorate dramatically. This study addresses the inherent limitations of perovskite crystal growth by designing a novel strategy for near-equilibrium growth system to maintain optimal conditions throughout the process. The system consists of three independent units: a solution supply unit, a crystal growth unit, and a solution recycling unit, which together ensure a constant solution concentration and temperature. By systematically optimizing temperature control and solution feeding rates, large and high-quality FAPbBr₃ single crystals, including a notable crystal measuring 51 × 45 × 10 mm³ are successfully produced. This crystal demonstrates a mobility-lifetime product of 2.83 × 10⁻² cm² V⁻¹ and an ultralow detection limit of 319.22 pGy_air, significantly surpassing existing perovskite crystals of similar size. The approach can serve as a universal platform for the controlled synthesis of all kinds of perovskite single crystals, laying the foundations for their use in various optoelectronic applications.