A Dynamic Diffusion-Controlled Antisolvent Method for Preparing High-Quality Halide Perovskite Single Crystals toward Ultrasensitive X-ray Detection

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 CsPbBr 3 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 × 10 6 μC Gy 1– cm –2 ) and robust γ-ray stability (>10 4 Gy), outperforming the previously reported CsPbBr 3 single crystal. The method is also broadly applicable to MAPbBr 3 and FAPbBr 3 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.