化学
卟啉
锌
电荷(物理)
超分子化学
碳纳米管
接受者
重组
纳米技术
光化学
分子
有机化学
凝聚态物理
物理
材料科学
基因
量子力学
生物化学
作者
Shahrzad Kazemi,Ajyal Z. Alsaleh,Paul A. Karr,Francis D’Souza
摘要
The importance of diameter-sorted single-wall carbon nanotubes (SWCNTs) noncovalently bound to a donor–acceptor molecular cleft, 1, in prolonging the lifetime of charge-separated states is successfully demonstrated. For this, using a multistep synthetic procedure, a wide-band capturing, multimodular, C60-bisstyrylBODIPY-(zinc porphyrin)2, molecular cleft 1, was newly synthesized and shown to bind diameter-sorted SWCNTs. The molecular cleft and its supramolecular assemblies were characterized by a suite of physicochemical techniques. Free-energy calculations suggested that both the (6,5) and (7,6) SWCNTs bound to 1 act as hole acceptors during the photoinduced sequential electron transfer events. Consequently, selective excitation of 1 in 1:SWCNT hybrids revealed a two-step electron transfer, leading to the formation of charge-separated states. Due to the distant separation of the cation and anion radical species within the supramolecules, improved lifetimes of the charge-separated states could be achieved. The present supramolecular strategy of improving charge separation involving SWCNTs and donor–acceptor molecular clefts highlights the potential application of these hybrid materials for various light energy harvesting and optoelectronic applications.
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