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.

No abstract

The Hecht equation is often used to calculate the 1 mobility-lifetime product (μτ ) of semiconductors by assuming 2 a uniform electric field based on the Shockley-Ramo theory. 3 However, the Schottky contacts are usually found at high resis-4 tivity semiconductor/metal interface, leading to a nonuniform 5 electric field inside the bulk semiconductor. We used a slice model 6 instead of the Hecht equation to calculate the charge collection 7 efficiency (CCE) and found that the CCE in a nonuniform field 8 can deviate significantly from that given by the Hecht equation in 9 a uniform field, with the difference relying heavily on the space 10 charge distribution and the μτ value. For semiconductors with 11 a high ionized acceptor impurity concentration of 5 × 10 9 cm −3 , 12 such as MAPbI 3 , the electron μτ value may be seriously 13 underestimated when adopting the Hecht equation assuming a 14 uniform field. The invalid application of the Hecht equation for 15 a Schottky interface may be one of the possible reasons for 16 the underestimation of electron μτ value for p-type perovskite 17 materials with relatively low resistivity. 18 Index Terms-Hecht equation, MAPbI 3 single crystal, 19 mobility-lifetime product. 20 23 due to their excellent carrier transport properties [1]-[9]. For 24 example, Dong et al. [10] reported first an excellent long 25 diffusion length of 175 μm for a MAPbI 3 single crystal.