Yao Ji-Song, Ge Jing, Wang Kun-Hua, Zhang Guozhen, Zhu Bai-Sheng, Chen Chen, Zhang Qun, Luo Yi, Yu Shu-Hong, Yao Hong-Bin
J Am Chem Soc. 2019 Feb 6;141(5):2069-2079. doi: 10.1021/jacs.8b11447. Epub 2019 Jan 24.
Cubic phase CsPbI quantum dots (α-CsPbI QDs) as a newly emerging type of semiconducting QDs hold tremendous promise for fundamental research and optoelectronic device applications. However, stable and sub-5 nm-sized α-CsPbI QDs have rarely been demonstrated so far due to their highly labile ionic structure and low phase stability. Here, we report a novel strontium-substitution along with iodide passivation strategy to stabilize the cubic phase of CsPbI, achieving the facile synthesis of α-CsPbI QDs with a series of controllable sizes down to sub-5 nm. We demonstrate that the incorporation of strontium ions can significantly increase the formation energies of α-CsPbI QDs and hence reduce the structure distortion to stabilize the cubic phase at the few-nanometer size. The size ranging from 15 down to sub-5 nm of as-prepared stable α-CsPbI QDs allowed us to investigate their unique size-dependent optical properties. Strikingly, the few-nanometer-sized α-CsPbI QDs turned out to retain high photoluminescence and highly close packing in solid state thin films, and the fabricated red light emitting diodes exhibited high brightness (1250 cd m at 9.2 V) and good operational stability (L > 2 h driven by 6 V). The developed cation-substitution strategy will provide an alternative method to prepare uniform and finely size-controlled colloidal lead halide perovskite QDs for various optoelectronic applications.
立方相CsPbI量子点(α-CsPbI QDs)作为一种新兴的半导体量子点,在基础研究和光电器件应用方面具有巨大潜力。然而,由于其离子结构高度不稳定且相稳定性低,迄今为止很少能制备出尺寸稳定且小于5nm的α-CsPbI QDs。在此,我们报道了一种新颖的锶取代及碘化物钝化策略,以稳定CsPbI的立方相,实现了尺寸可控至小于5nm的α-CsPbI QDs的简便合成。我们证明,引入锶离子可显著提高α-CsPbI QDs的形成能,从而减少结构畸变,在几纳米尺寸下稳定立方相。所制备的尺寸范围从15nm至小于5nm的稳定α-CsPbI QDs,使我们能够研究其独特的尺寸依赖性光学性质。令人惊讶的是,几纳米尺寸的α-CsPbI QDs在固态薄膜中具有高光致发光性和高度紧密堆积,所制备的红光发光二极管表现出高亮度(9.2V时为1250cd m)和良好的工作稳定性(6V驱动下L>2h)。所开发的阳离子取代策略将为制备用于各种光电器件应用的均匀且尺寸精细可控的胶体卤化铅钙钛矿量子点提供一种替代方法。