论文标题

CSPBBR $ _3 $纳米板的转化通过自组装到溶液中

Temperature Driven Transformation of CsPbBr$_3$ Nanoplatelets into Mosaic Nanotiles in Solution through Self-Assembly

论文作者

Dang, Zhiya, Dhanabalan, Balaji, Castelli, Andrea, Dhall, Rohan, Bustillo, Karen C., Marchelli, Dorwal, Spirito, Davide, Petralanda, Urko, Shamsi, Javad, Manna, Liberato, Krahne, Roman, Arciniegas, Milena P.

论文摘要

二维胶体卤化物钙钛矿纳米晶体是发光应用的有前途的材料。此外,它们可以用作通过物理和化学转化来创建各种材料的组件。最近的研究集中在能够自组装和转化固体底物上的纳米片。然而,该过程背后的机制和组装的原子布置尚不清楚。在这里,我们介绍了溶液中CSPBBR $ _3 $纳米板的自组装堆栈的转换,通过将溶液保持在室温下并监测几个月的纳米晶体形态,从而捕获过程的不同阶段。使用前右传输电子显微镜和表面分析,我们证明了转化机制可以理解为定向的附着,通过以下步骤进行:i)从颗粒表面上解吸配体,从而导致纳米细胞骨骼堆栈的合并,这首先形成了纳米软化; ii)合并邻近的纳米质体,形成更延伸的纳米板; iii)纳米质和纳米板的附着,它们具有与原子结构相似的原子结构的物体,类似于骨折的纳米动物制成的镶嵌物。我们揭示起始纳米片无缝融合,并在小小的和薄纳米质体中无原子尺度上的缺陷。然而,主要由胺/铵离子稳定的老化纳米型和纳米板,通过CSBR的双层连接。在这种情况下,相邻的钙钛矿晶格的原子柱移动半单元,形成了Ruddlesden-Popper Planar故障。

Two-dimensional colloidal halide perovskite nanocrystals are promising materials for light emitting applications. In addition, they can be used as components to create a variety of materials through physical and chemical transformations. Recent studies focused on nanoplatelets that are able to self-assemble and transform on solid substrates. Yet, the mechanism behind the process and the atomic arrangement of their assemblies remain unclear. Here, we present the transformation of self-assembled stacks of CsPbBr$_3$ nanoplatelets in solution, capturing the different stages of the process by keeping the solutions at room temperature and monitoring the nanocrystal morphology over a period of a few months. Using ex-situ transmission electron microscopy and surface analysis, we demonstrate that the transformation mechanism can be understood as oriented attachment, proceeding through the following steps: i) desorption of the ligands from the particles surfaces, causing the merging of nanoplatelet stacks, which first form nanobelts; ii) merging of neighboring nanobelts that form more extended nanoplates; and iii) attachment of nanobelts and nanoplates, which create objects with an atomic structure that resemble a mosaic made of broken nanotiles. We reveal that the starting nanoplatelets merge seamlessly and defect-free on an atomic scale in small and thin nanobelts. However, aged nanobelts and nanoplates, which are mainly stabilized by amine/ammonium ions, link through a bilayer of CsBr. In this case, the atomic columns of neighboring perovskite lattices shift by a half-unit-cell, forming Ruddlesden-Popper planar faults.

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