Brightening of Long, Polymer-Wrapped Carbon Nanotubes by sp3 Functionalization in Organic Solvents
Brightening of Long, Polymer-Wrapped Carbon Nanotubes by sp3 Functionalization in Organic Solvents
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DOI：
10.1021/acsnano.9b03792
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发表时间：
2019-08-01
期刊：
影响因子：
17.1
通讯作者：
Zaumseil, Jana
中科院分区：
文献类型：
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作者：
Berger, Felix J.;Luettgens, Jan;Zaumseil, Jana
将具有sp(3)缺陷的半导体单壁碳纳米管(SWNTs)功能化，作为发光激子陷阱，是提高其光致发光量子产率(PLQY)和增加光学性能的有力手段。然而，目前用于引入这些缺陷的合成方法仅限于表面活性剂包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能。相比之下，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和更高的PLQY，并且很容易加工成薄膜用于器件应用。在这里，我们介绍了一种简单且可扩展的相转移方法来将重氮盐溶解在有机非卤化溶剂中，以控制与聚合物包裹的单壁碳纳米管的反应，产生发光的芳基缺陷。绝对PLQY测量被用来可靠地量化缺陷诱导的增亮。对缺陷密度和陷阱深度的优化可以得到高达4%的PLQY，其中90%的光子通过缺陷通道发射。我们进一步揭示了初始单壁碳纳米管的质量和长度对由sp(3)缺陷引起的相对增亮的强烈影响。高效、简单地制备大量针对缺陷定制的聚合物分类单壁碳纳米管，使得气溶胶喷雾打印和旋涂薄膜具有明亮且几乎没有重吸收的缺陷发射，这是基于碳纳米管的近红外发光器件所需要的。
The functionalization of semiconducting single walled carbon nanotubes (SWNTs) with sp(3) 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 defect channel. We further reveal the strong impact of initial SWNT quality and length on the relative brightening by sp(3) defects. The efficient and simple production of large quantities of defect-tailored polymer-sorted SWNTs enables aerosol-jet printing and spin-coating of thin films with bright and nearly reabsorption-free defect emission, which are desired for carbon nanotube-based near-infrared light-emitting devices.