Zhong Yangguang, Liao Kun, Du Wenna, Zhu Jiangrui, Shang Qiuyu, Zhou Fan, Wu Xianxin, Sui Xinyu, Shi Jianwei, Yue Shuai, Wang Qi, Zhang Yanfeng, Zhang Qing, Hu Xiaoyong, Liu Xinfeng
CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, P.R. China.
University of Chinese Academy of Sciences, Beijing 100049, P.R. China.
ACS Nano. 2020 Nov 24;14(11):15605-15615. doi: 10.1021/acsnano.0c06380. Epub 2020 Nov 10.
Single-crystal perovskites with excellent photophysical properties are considered to be ideal materials for optoelectronic devices, such as lasers, light-emitting diodes and photodetectors. However, the growth of large-scale perovskite single-crystal films (SCFs) with high optical gain by vapor-phase epitaxy remains challenging. Herein, we demonstrated a facile method to fabricate large-scale thin CsPbBr SCFs (∼300 nm) on the -plane sapphire substrate. High temperature is found to be the key parameter to control low reactant concentration and sufficient surface diffusion length for the growth of continuous CsPbBr SCFs. Through the comprehensive study of the carrier dynamics, we clarify that the trapped-related exciton recombination has the main effect under low carrier density, while the recombination of excitons and free carriers coexist until free carriers plays the dominate role with increasing carrier density. Furthermore, an extremely low-threshold (∼8 μJ cm) amplified spontaneous emission was achieved at room temperature due to the high optical gain up to 1255 cm at a pump power of 20 times threshold (∼20 ). A microdisk array was prepared using a focused ion beam etching method, and a single-mode laser was achieved on a 3 μm diameter disk with the threshold of 1.6 μJ cm. Our experimental results not only present a versatile method to fabricate large-scale SCFs of CsPbBr but also supply an arena to boost the optoelectronic applications of CsPbBr with high performance.
具有优异光物理性质的单晶钙钛矿被认为是用于光电器件(如激光器、发光二极管和光电探测器)的理想材料。然而,通过气相外延生长具有高光学增益的大规模钙钛矿单晶薄膜(SCFs)仍然具有挑战性。在此,我们展示了一种在 c 面蓝宝石衬底上制备大规模 CsPbBr 单晶薄膜(约 300 纳米)的简便方法。发现高温是控制低反应物浓度和足够的表面扩散长度以生长连续 CsPbBr 单晶薄膜的关键参数。通过对载流子动力学的综合研究,我们阐明在低载流子密度下,陷阱相关的激子复合起主要作用,而随着载流子密度增加,激子与自由载流子的复合共存,直到自由载流子起主导作用。此外,由于在 20 倍阈值(约 20 μJ/cm²)的泵浦功率下高达 1255 cm⁻¹ 的高光学增益,在室温下实现了极低阈值(约 8 μJ/cm²)的放大自发发射。使用聚焦离子束蚀刻方法制备了微盘阵列,并在直径为 3 μm 的盘上实现了阈值为 1.6 μJ/cm² 的单模激光器。我们的实验结果不仅提供了一种制备大规模 CsPbBr 单晶薄膜的通用方法,还为推动 CsPbBr 的高性能光电器件应用提供了一个平台。