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Brighteningof Long Polymer-Wrapped Carbon Nanotubesby sp3 Functionalization in Organic Solvents

机译:提亮肤色长的聚合物包裹碳纳米管通过sp3在有机溶剂中的功能化

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摘要

The functionalization of semiconducting single-walled carbon nanotubes (SWNTs) with sp3 defects that act as luminescent exciton traps is a powerful means to enhance their photoluminescence quantum yield (PLQY) and to add optical properties. However, the synthetic methods employed to introduce these defects are currently limited to aqueous dispersions of surfactant-coated SWNTs, often with short tube lengths, residual metallic nanotubes, and poor film-formation properties. In contrast to that, dispersions of polymer-wrapped SWNTs in organic solvents feature unrivaled purity, higher PLQY, and are easily processed into thin films for device applications. Here, we introduce a simple and scalable phase-transfer method to solubilize diazonium salts in organic nonhalogenated solvents for the controlled reaction with polymer-wrapped SWNTs to create luminescent aryl defects. Absolute PLQY measurements are applied to reliably quantify the defect-induced brightening. The optimization of defect density and trap depth results in PLQYs of up to 4% with 90% of photons emitted through the defectchannel. We further reveal the strong impact of initial SWNT qualityand length on the relative brightening by sp3 defects.The efficient and simple production of large quantities of defect-tailoredpolymer-sorted SWNTs enables aerosol-jet printing and spin-coatingof thin films with bright and nearly reabsorption-free defect emission,which are desired for carbon nanotube-based near-infrared light-emittingdevices.
机译:具有sp 3 缺陷的半导体单壁碳纳米管(SWNTs)的功能化可以用作发光激子陷阱,是增强其光致发光量子产率(PLQY)和增加光学性质的有力手段。但是,用于引入这些缺陷的合成方法目前仅限于表面活性剂涂覆的单壁碳纳米管的水分散体,通常具有较短的管长,残留的金属纳米管和较差的成膜性。与此相反,聚合物包裹的单壁碳纳米管在有机溶剂中的分散体具有无与伦比的纯度,较高的PLQY,并且易于加工成薄膜用于设备应用。在这里,我们介绍了一种简单且可扩展的相转移方法,以将重氮盐溶解在有机非卤代溶剂中,以便与聚合物包裹的单壁碳纳米管进行受控反应,从而产生发光的芳基缺陷。绝对PLQY测量可用于可靠地量化缺陷引起的增白。缺陷密度和陷阱深度的优化可导致PLQY高达4%,其中90%的光子通过缺陷发出渠道。我们进一步揭示了初始SWNT质量的强大影响sp 3 缺陷导致相对增亮的长度和长度。高效,简单地生产大量定制的缺陷聚合物分类的单壁碳纳米管可进行气溶胶喷射印刷和旋涂具有明亮且几乎没有重吸收的缺陷发射的薄膜,碳纳米管基近红外发光所需要的设备。

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