Emergence of new red-shifted carbon nanotube photoluminescence based on proximal doped-site design.
Emergence of new red-shifted carbon nanotube photoluminescence based on proximal doped-site design.
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DOI：
10.1038/srep28393
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发表时间：
2016-06-27
影响因子：
4.6
通讯作者：
Nakashima N
中科院分区：
文献类型：
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作者：
Shiraki T;Shiraishi T;Juhász G;Nakashima N
单壁碳纳米管 (SWNT) 在近红外 (NIR) 区域表现出独特的光致发光 (PL)。在这里，我们提出了一个基于单壁碳纳米管局部共价功能化的近端修饰的概念。量子力学模拟表明，SWNT 带隙的变化特别基于邻近的掺杂位点设计。因此，我们合成了新设计的双重氮分子并进行了单壁碳纳米管的局部功能化。因此，具有 (6, 5) 手性的双重氮修饰的 SWNT 的新红移 PL (E112*) 在 1250 nm 附近被识别，与原始 SWNT 的 PL 相比具有超过约 270 nm 的斯托克斯位移，并且 PL 波长的偏移取决于修饰剂的亚甲基间隔基长度。本研究表明，SWNT PL 调制是通过近距离局部共价修饰实现的，这对于基本了解 SWNT PL 特性以及基于激子工程的应用（包括光子器件和（生物）成像/传感）非常重要。
Single-walled carbon nanotubes (SWNTs) show unique photoluminescence (PL) in the near-infrared (NIR) region. Here we propose a concept based on the proximal modification in local covalent functionalization of SWNTs. Quantum mechanical simulations reveal that the SWNT band gap changes specifically based on the proximal doped-site design. Thus, we synthesize newly-designed bisdiazonium molecules and conduct local fucntionalisation of SWNTs. Consequently, new red-shifted PL (E112*) from the bisdiazonium-modified SWNTs with (6, 5) chirality is recognized around 1250 nm with over ~270 nm Stokes shift from the PL of the pristine SWNTs and the PL wavelengths are shifted depending on the methylene spacer lengths of the modifiers. The present study revealed that SWNT PL modulation is enable by close-proximity-local covalent modification, which is highly important for fundamental understanding of intrinsic SWNT PL properties as well as exciton engineering–based applications including photonic devices and (bio)imaging/sensing.