Chen Jingxuan, Jia Donglin, Zhuang Rongshan, Hua Yong, Zhang Xiaoliang
School of Materials Science and Engineering, Beihang University, Beijing, 100191, China.
Yunnan Key Laboratory for Micro/Nano Materials & Technology, School of Materials and Energy, Yunnan University, Kunming, 650091, China.
Adv Mater. 2022 Sep;34(37):e2204259. doi: 10.1002/adma.202204259. Epub 2022 Aug 15.
Perovskite quantum dots (PQDs) have emerged as competitive optoelectronic materials for photovoltaic applications due to their ideal bandgap energy, high defect tolerance, and solution processability. However, the highly dynamic surface and imperfect cubic structure of PQDs generally result in unfavorable charge-carrier transport within the PQD solids and serious nonradiative recombination. Herein, a highly orientated PQD solid is demonstrated using precursor engineering accompanied by a chemical stripping treatment (CST). A combination of systematic experimental studies and theoretical calculations is conducted to fundamentally understand the resurfacing of PQDs using the CST approach. The results reveal that the highly ordered PQDs can result in a high orientation of PQD solids, significantly promoting charge-carrier transport within the PQD solids. Meanwhile, the ideal cubic-structured PQD with an iodine-rich surface dramatically decreases surface trap states, thereby substantially diminishing trap-assisted nonradiative recombination. Consequently, the inorganic PQD solar cell delivers a power conversion efficiency of up to 16.25%. This work provides a feasible avenue to construct highly orientated PQD solids with improved photophysical properties for high-performance optoelectronic devices.
钙钛矿量子点(PQDs)因其理想的带隙能量、高缺陷容忍度和溶液可加工性,已成为用于光伏应用的有竞争力的光电器件材料。然而,PQDs高度动态的表面和不完美的立方结构通常会导致PQD固体内部电荷载流子传输不利以及严重的非辐射复合。在此,通过前驱体工程结合化学剥离处理(CST)展示了一种高度取向的PQD固体。进行了系统的实验研究和理论计算相结合,从根本上理解使用CST方法对PQDs进行表面重构。结果表明,高度有序的PQDs可导致PQD固体的高度取向,显著促进PQD固体内部的电荷载流子传输。同时,具有富碘表面的理想立方结构PQD极大地降低了表面陷阱态,从而大幅减少了陷阱辅助非辐射复合。因此,无机PQD太阳能电池的功率转换效率高达16.25%。这项工作为构建具有改善光物理性质的高度取向PQD固体以用于高性能光电器件提供了一条可行途径。