A Dynamic Diffusion-Controlled Antisolvent Method for Preparing High-Quality Halide Perovskite Single Crystals toward...

The scalable synthesis of high-quality halide perovskite single crystals is essential for advanced radiation detection but is constricted by the difficulty of synthesizing high-quality single crystals. Here, we report a dynamic diffusion-controlled antisolvent method that enables the control of the crystallization by modulating the interfacial methanol diffusion. This strategy successfully suppresses the crystal nucleation by further facilitating the growth of millimeter-scale CsPbBr₃ single crystals with ultralow trap density and high orientation (texture coefficient ∼99.9%). As a result, X-ray detectors based on these crystals exhibit ultrasensitive response (1.09 × 10⁶ μC Gy^1- cm^-2) and robust γ-ray stability (>10⁴ Gy), outperforming the previously reported CsPbBr₃ single crystal. The method is also broadly applicable to MAPbBr₃ and FAPbBr₃ systems, offering a versatile pathway toward compositional control. This work provides both a universal crystal growth strategy and mechanistic insight into solvent-antisolvent interface engineering, opening new pathways for perovskite-based optoelectronics and radiation detection technologies.