Scalable Synthesis of InAs Quantum Dots Mediated through Indium Redox Chemistry
Scalable Synthesis of InAs Quantum Dots Mediated through Indium Redox Chemistry
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DOI：
10.1021/jacs.9b12350
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发表时间：
2020-03-04
影响因子：
15
通讯作者：
Bawendi, Moungi G.
中科院分区：
文献类型：
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作者：
Ginterseder, Matthias;Franke, Daniel;Bawendi, Moungi G.
以近红外（NIR）和短波红外（SWIR）波长为中心的下一代光电应用需要高质量的材料。在这些材料中，胶体InAs量子点（QDs）作为生物成像、照明和传感应用的红外活性候选材料脱颖而出。尽管它们的光学特性有了重大的发展，但InAs量子点的合成仍然经常依赖于危险的、商业上不可用的前体。在这里，我们描述了一个简单的单热注射过程，围绕In(I)CI作为关键前驱体。同时作为还原剂和In源，In(I)Cl与三（氨基）砷前体顺利反应，定量地以克为单位生成胶体InAs。通过调节反应温度可以得到在700 ~ 1400 nm范围内具有第一激子吸收特征的InAs芯。In(I)， In金属和In（III）之间的动态歧化平衡为前驱体选择提供了额外的灵活性。CdSe壳层的生长增强了它们的光学性能，使粒子的中心发射波长在1000 ~ 1500nm之间，半最大光致发光全宽度约为120mev。该前体平台的简单性、可扩展性和可调性有望激发基于in的胶体量子点的进一步研究。
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)CI 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.