Electronic‐Grade High‐Quality Perovskite Single Crystals by a Steady Self‐Supply Solution Growth for High‐Performance X‐ray Detectors

Abstract High‐quality perovskite single crystals with large size are highly desirable for the fundamental research and high energy detection application. Here, a simple and convenient solution method, featuring continuous‐mass transport process (CMTP) by a steady self‐supply way, is shown to keep the growth of semiconductor single crystals continuously stable at a constant growth rate until an expected crystal size is achieved. A significantly reduced full width at half‐maximum (36 arcsec) of the (400) plane from the X‐ray rocking curve indicates a low angular dislocation of 6.8 × 10⁶ cm⁻² and hence a higher crystalline quality for the CH₃NH₃PbI₃(MAPbI₃) single crystals grown by CMTP as compared to the conventional inverse temperature crystallization (ITC) method. Furthermore, the CMTP‐based single crystals have lower trap density, reduced by nearly 200% to 4.5 × 10⁹ cm⁻³, higher mobility increased by 187% to 150.2 cm² V⁻¹ s⁻¹, and higher mobility–lifetime product increased by around 450% to 1.6 × 10⁻³ cm² V⁻¹, as compared with the ITC‐grown reference sample. The high performance of the CMTP‐based MAPbI₃ X‐ray detector is comparable to that of a traditional high‐quality CdZnTe device, indicating the CMTP method as being a cost‐efficient strategy for high‐quality electronic‐grade semiconductor single crystals.