Gao Han, He Dong, Chen Zehua, Gao Peili, He Dongsheng, Li Zhaoning, Zhang Xusheng, Xiu Jingwei, Sun Qiang, Chen Shuming, Wei Su-Huai, Yu Shu-Hong, He Zhubing
Department of Materials Science and Engineering, Shenzhen Key Laboratory of Full Spectral Solar Electricity Generation (FSSEG), Southern University of Science and Technology, No. 1088, Xueyuan Rd., Shenzhen 518055, Guangdong, China.
Beijing Computational Science Research Center, Beijing 100193, China.
Sci Adv. 2025 Jan 10;11(2):eads4038. doi: 10.1126/sciadv.ads4038. Epub 2025 Jan 8.
Owing to the predominant merit of tunable bandgaps, tin-lead mixed perovskites have shown great potentials in realizing near-infrared optoelectronics and are receiving increasing attention. However, despite the merit, there is still a lack of fundamental understanding of the bandgap variation as a function of Sn/Pb ratio, mainly because the films are easy to segregate in terms of both composition and phase. Here, we report a fully stoichiometric synthesis of monocrystalline FAPbSnI nanocrystals as well as their atomic-scale imaging. On the basis of the systematic measurements of the monocrystalline materials, strain and Coulomb interaction-induced atomic ordering was revealed to be responsible for the unusual discontinuous bandgap jumping near = 0.5 from the expected bowing effect. As a result, both FAPbSnI and FAPbSnI have the lowest bandgaps of around 1.27 electron volts, while that of FAPbSnI is 1.33 electron volts. Correspondingly, their based light-emitting diodes can emit infrared lights with the wavelengths reaching 930 nanometers.
由于锡铅混合钙钛矿具有可调节带隙这一主要优点,它们在实现近红外光电子学方面展现出巨大潜力,并受到越来越多的关注。然而,尽管有此优点,但对于带隙随锡/铅比例变化的基本理解仍很欠缺,主要原因是薄膜在成分和相方面都容易发生偏析。在此,我们报告了单晶FAPbSnI纳米晶体的全化学计量合成及其原子尺度成像。基于对单晶材料的系统测量,发现应变和库仑相互作用诱导的原子有序排列是导致在锡/铅比例约为0.5时出现与预期弯曲效应不同寻常的不连续带隙跳跃的原因。结果,FAPbSnI和FAPbSnI的带隙最低,约为1.27电子伏特,而FAPbSnI的带隙为1.33电子伏特。相应地,基于它们的发光二极管能够发射波长达到930纳米的红外光。