Precision Synthesis and Atomistic Analysis of Deep-Blue Cubic Quantum Dots Made via Self-Organization

Precision Synthesis and Atomistic Analysis of Deep-Blue Cubic Quantum Dots Made via Self-Organization
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自组织深蓝色立方量子点的精密合成和原子分析

DOI:
10.1021/jacs.2c08227
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发表时间:
2022
影响因子:
15
通讯作者:
Nakamura Eiichi
Nakamura Eiichi
中科院分区:
化学1区
文献类型:
--
作者:
Chevalier Olivier J. G. L.;Nakamuro Takayuki;Sato Wataru;Miyashita Satoru;Chiba Takayuki;Kido Junji;Shang Rui;Nakamura Eiichi

文献摘要

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当晶体尺寸接近几纳米时,原子变得不等价,键振动,量子效应出现。为了研究分子科学中常见的具有结构控制的量子点,我们需要原子精确的合成和分析。我们在这里描述的合成溴化铅钙钛矿神奇大小的纳米团簇通过自组织的苹果酸铅螯合物和PbBr 3-在环境条件下。毫秒和埃分辨率的电子显微镜分析揭示了单个量子点的结构和动力学行为-由64个铅原子组成的结构均匀的立方体,其中8个苹果酸分子位于立方体的8个角上,油基铵阳离子亲脂并稳定边缘和表面。由于缺乏平移对称性,立方体应该被看作是一个分子而不是一个晶体。该量子点在λ 460 nm处表现出定量的光致发光和稳定的电致发光,半峰宽小于15 nm,反映了最小的结构缺陷。这种控制合成和精确分析表明电影化学表征纳米材料的潜力超出了传统的限制。
As a crystal approaches a few nanometers in size, atoms become nonequivalent, bonds vibrate, and quantum effects emerge. To study quantum dots (QDs) with structural control common in molecular science, we need atomic precision synthesis and analysis. We describe here the synthesis of lead bromide perovskite magic-sized nanoclusters via self-organization of a lead malate chelate complex and PbBr3–under ambient conditions. Millisecond and angstrom resolution electron microscopic analysis revealed the structure and the dynamic behavior of individual QDs─structurally uniform cubes made of 64 lead atoms, where eight malate molecules are located on the eight corners of the cubes, and oleylammonium cations lipophilize and stabilize the edges and faces. Lacking translational symmetry, the cube is to be viewed as a molecule rather than a nanocrystal. The QD exhibits quantitative photoluminescence and stable electroluminescence at ≈460 nm with a narrow half-maximum linewidth below 15 nm, reflecting minimum structural defects. This controlled synthesis and precise analysis demonstrate the potential of cinematic chemistry for the characterization of nanomaterials beyond the conventional limit.