Wang Wenzhen, Meng Hua, Qi Huanzhen, Xu Haitao, Du Wenbin, Yang Yiheng, Yi Yongsheng, Jing Shengqi, Xu Shanhu, Hong Feng, Qin Juan, Huang Jian, Xu Zhan, Zhu Yanyan, Xu Run, Lai Jianming, Xu Fei, Wang Linjun, Zhu Jingtao
School of Materials Science and Engineering, Shanghai University, Nanchen Road, Shanghai, 200444, China.
Department of Physics, Shaoxing University, 508 Huancheng West Road, Shaoxing, 312000, China.
Adv Mater. 2020 Aug;32(33):e2001540. doi: 10.1002/adma.202001540. Epub 2020 Jul 6.
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 × 10 cm and hence a higher crystalline quality for the CH NH PbI (MAPbI ) 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 × 10 cm , higher mobility increased by 187% to 150.2 cm V s , and higher mobility-lifetime product increased by around 450% to 1.6 × 10 cm V , as compared with the ITC-grown reference sample. The high performance of the CMTP-based MAPbI 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.
高质量的大尺寸钙钛矿单晶对于基础研究和高能探测应用非常重要。在此，展示了一种简单便捷的溶液法，其通过稳定的自供应方式具有连续质量传输过程（CMTP），可使半导体单晶的生长以恒定生长速率持续稳定，直至达到预期的晶体尺寸。X射线摇摆曲线显示（400）平面的半高宽显著减小（36弧秒），表明角位错为6.8×10⁻⁴cm，因此与传统的逆温结晶（ITC）方法相比，通过CMTP生长的CH₃NH₃PbI₃（MAPbI₃）单晶具有更高的晶体质量。此外，与ITC生长的参考样品相比，基于CMTP的单晶具有更低的陷阱密度，降低了近200%至4.5×10¹⁴cm⁻³，更高的迁移率提高了187%至150.2cm²V⁻¹s⁻¹，以及更高的迁移率-寿命乘积提高了约450%至1.6×10⁻³cm²V⁻¹。基于CMTP的MAPbI₃X射线探测器的高性能与传统的高质量CdZnTe器件相当，表明CMTP方法是一种用于高质量电子级半导体单晶的经济高效策略。
