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通过铟氧化还原化学介导的 InAs 量子点的可扩展合成。

Scalable Synthesis of InAs Quantum Dots Mediated through Indium Redox Chemistry.

机构信息

Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.

出版信息

J Am Chem Soc. 2020 Mar 4;142(9):4088-4092. doi: 10.1021/jacs.9b12350. Epub 2020 Feb 19.

DOI:10.1021/jacs.9b12350
PMID:32073841
Abstract

Next-generation optoelectronic applications centered in the near-infrared (NIR) and short-wave infrared (SWIR) wavelength regimes require high-quality materials. Among these materials, colloidal InAs quantum dots (QDs) stand out as an infrared-active candidate material for biological imaging, lighting, and sensing applications. Despite significant development of their optical properties, the synthesis of InAs QDs still routinely relies on hazardous, commercially unavailable precursors. Herein, we describe a straightforward single hot injection procedure revolving around In(I)Cl as the key precursor. Acting as a simultaneous reducing agent and In source, In(I)Cl smoothly reacts with a tris(amino)arsenic precursor to yield colloidal InAs quantitatively and at gram scale. Tuning the reaction temperature produces InAs cores with a first excitonic absorption feature in the range of 700-1400 nm. A dynamic disproportionation equilibrium between In(I), In metal, and In(III) opens up additional flexibility in precursor selection. CdSe shell growth on the produced cores enhances their optical properties, furnishing particles with center emission wavelengths between 1000 and 1500 nm and narrow photoluminescence full-width at half-maximum (FWHM) of about 120 meV throughout. The simplicity, scalability, and tunability of the disclosed precursor platform are anticipated to inspire further research on In-based colloidal QDs.

摘要

下一代以近红外 (NIR) 和短波红外 (SWIR) 波长为中心的光电应用需要高质量的材料。在这些材料中,胶体 InAs 量子点 (QD) 作为一种用于生物成像、照明和传感应用的红外活性候选材料脱颖而出。尽管其光学性质有了显著的发展,但 InAs QD 的合成仍然经常依赖于危险且商业上不可用的前体。在此,我们描述了一种简单的单热注入程序,以 In(I)Cl 为关键前体。In(I)Cl 作为一种同时的还原剂和 In 源,与三(氨基)砷前体平稳反应,以定量和克级规模生成胶体 InAs。调节反应温度可以产生第一激子吸收特征在 700-1400nm 范围内的 InAs 核。In(I)、In 金属和 In(III)之间的动态歧化平衡为前体选择提供了额外的灵活性。在生成的核上进行 CdSe 壳生长可以增强它们的光学性质,为颗粒提供中心发射波长在 1000nm 到 1500nm 之间的光致发光,半峰全宽 (FWHM) 约为 120meV。所揭示的前体平台的简单性、可扩展性和可调节性有望激发对基于 In 的胶体 QD 的进一步研究。

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