Photoexcited Aromatic Reactants Give Multicolor Carbon Nanotube Fluorescence from Quantum Defects
Photoexcited Aromatic Reactants Give Multicolor Carbon Nanotube Fluorescence from Quantum Defects
复制标题
光激发芳香族反应物因量子缺陷而发出多色碳纳米管荧光
DOI：
10.1021/acsnano.9b07606
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发表时间：
2020
期刊：
影响因子：
17.1
通讯作者：
Weisman, R. Bruce
中科院分区：
文献类型：
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作者：
Zheng, Yu;Bachilo, Sergei M.;Weisman, R. Bruce
单壁碳纳米管 (SWCNT) 的共价功能化对于改变其电子特性和产生荧光量子缺陷非常有价值。我们在此报告了以前未报告的此类反应，涉及光激发芳香族化合物与单壁碳纳米管侧壁的相互作用。当单壁碳纳米管的水悬浮液暴露于有机芳香族化合物，然后受到紫外线照射时，纳米管中会形成荧光缺陷，其形成速度取决于芳环取代基。在与苯胺或碘苯胺的反应中，1 分钟内就会出现强光谱边带。总 SWCNT 光致发光可增强约 5 倍。值得注意的是，反应后的单壁碳纳米管的发射光谱取决于反应过程中是否存在溶解氧。对于 (6,5) SWCNT，存在氧气时的处理会产生比原始位置红移 160 meV 的额外发射带，而无氧处理会导致两个额外的发射带红移 140 和 270 meV。方差光谱显示存在具有三个不同发射带（原始加两个偏移）的单个“多色”纳米管。在单壁碳纳米管中轻松生成双荧光量子缺陷可以提供更接近标准电信波长的发射，从而推进了作为单光子源在量子信息处理中的应用前景。
Covalent functionalization of single-wall carbon nanotubes (SWCNTs) can be valuable for modifying their electronic properties and creating fluorescent quantum defects. We report here a previously unreported category of such reactions involving interactions of photoexcited aromatic compounds with SWCNT sidewalls. When aqueous suspensions of SWCNTs are exposed to organic aromatic compounds and then irradiated by UV light, fluorescent defects are formed in the nanotubes at rates that depend on the aromatic ring substituents. In reactions with aniline or iodoaniline, strong spectral sidebands appear within 1 min. Total SWCNT photoluminescence can be enhanced by a factor as large as ∼5. Notably, emission spectra of reacted SWCNTs depend on the presence or absence of dissolved oxygen during the reaction. For (6,5) SWCNTs, treatment when oxygen is present gives an additional emission band red-shifted by 160 meV from the pristine position, whereas treatment without oxygen leads to two additional emission bands red-shifted by 140 and 270 meV. Variance spectroscopy shows the presence of individual “multicolor” nanotubes with three distinct emission bands (pristine plus two shifted). The facile generation of dual fluorescent quantum defects in SWCNTs provides emission closer to standard telecom wavelengths, advancing the prospects for applications as single-photon sources in quantum information processing.