Steady‐State Inverse‐Temperature Crystallization Enabling Low Defect Perovskite Single Crystal and Efficient X‐Ray Detectors

Abstract Organic–inorganic halide perovskite single crystals (SCs) have shown great potential in radiation detection applications due to their large radiation stopping power and excellent carrier transport properties. The spatial‐confined inverse‐temperature crystallization (ITC) method has been widely adopted to obtain large‐sized SCs. However, they usually face the problems of uneven stress distribution and high defect density due to the limited crystal growth space and varied growth rate with the increase in temperature, making it difficult to fabricate highly sensitive and stable radiation detectors. In this study, the steady‐state inverse‐temperature crystallization method (SS‐ITC) is developed to regulate the growth process of SCs by controlling the growth speed precisely to achieve a constant rate of growth as the temperature increases. Compared with the conventional ITC‐grown samples, the lattice spacing of SCs prepared by the SS‐ITC method is reduced by 1.2% due to tensile stress relaxation, resulting in a lower defect density of 7.93 × 10 9 cm −3 and a remarkable uniformity over a large area. As a result, the co‐planar X‐ray detectors based on these high‐quality SCs exhibit a high sensitivity of 1.67 × 10 5 µC Gy air −1 cm −2 , representing the best performing MAPbBr 3 ‐based X‐ray detectors reported to date.