Dipartimento di Chimica e Chimica Industriale , Università degli Studi di Genova , Via Dodecaneso 31 , 16146 Genova , Italy.
Department of Theoretical Chemistry, Faculty of Science , Vrije Universiteit Amsterdam , de Boelelaan 1083 , 1081 HV Amsterdam , The Netherlands.
Nano Lett. 2018 Dec 12;18(12):7822-7831. doi: 10.1021/acs.nanolett.8b03598. Epub 2018 Nov 12.
Fully inorganic cesium lead halide perovskite (CsPbX) nanocrystals (NCs) have been extensively studied due to their excellent optical properties, especially their high photoluminescence quantum yield (PLQY) and the ease with which the PL can be tuned across the visible spectrum. So far, most strategies for synthesizing CsPbX NCs are highly sensitive to the processing conditions and ligand combinations. For example, in the synthesis of nanocubes of different sizes, it is not uncommon to have samples that contain various other shapes, such as nanoplatelets and nanosheets. Here, we report a new colloidal synthesis method for preparing shape-pure and nearly monodispersed CsPbBr nanocubes using secondary amines. Regardless of the length of the alkyl chains, the oleic acid concentration, and the reaction temperature, only cube-shaped NCs were obtained. The shape purity and narrow size distribution of the nanocubes are evident from their sharp excitonic features and their ease of self-assembly in superlattices, reaching lateral dimensions of up to 50 μm. We attribute this excellent shape and phase purity to the inability of secondary amines to find the right steric conditions at the surface of the NCs, which consequently limits the formation of low-dimensional structures. Furthermore, no contamination from other phases was observed, not even from CsPbBr, presumably due to the poor ability of secondary aliphatic amines to coordinate to PbBr and, hence, to provide a reaction environment that is depleted in Pb.
全无机铯铅卤钙钛矿(CsPbX)纳米晶体(NCs)由于其优异的光学性质而得到了广泛的研究,特别是其高光致发光量子产率(PLQY)和易于在可见光谱范围内调谐 PL 的特性。到目前为止,合成 CsPbX NCs 的大多数策略都对处理条件和配体组合高度敏感。例如,在合成不同尺寸的纳米立方体时,常见的情况是样品中含有各种其他形状,如纳米薄片和纳米片。在这里,我们报告了一种使用仲胺制备形状纯且近单分散 CsPbBr 纳米立方体的新胶体合成方法。无论烷基链的长度、油酸浓度和反应温度如何,仅获得立方体形 NCs。纳米立方体的形状纯度和窄的尺寸分布从其尖锐的激子特征和在超晶格中的自组装能力明显看出,达到了高达 50μm 的横向尺寸。我们将这种优异的形状和相纯度归因于仲胺无法在 NCs 的表面找到合适的空间条件,从而限制了低维结构的形成。此外,没有观察到其他相的污染,甚至没有 CsPbBr 的污染,这可能是由于仲脂肪胺与 PbBr 的配位能力差,从而提供了贫 Pb 的反应环境。