Single-Molecule Fluorescence Photoswitching of a Diarylethene-Perylenebisimide Dyad: Non-destructive Fluorescence Readout
Single-Molecule Fluorescence Photoswitching of a Diarylethene-Perylenebisimide Dyad: Non-destructive Fluorescence Readout
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DOI：
10.1021/ja110686t
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发表时间：
2011-04-06
影响因子：
15
通讯作者：
Irie, Masahiro
中科院分区：
文献类型：
--
作者：
Fukaminato, Tuyoshi;Doi, Takao;Irie, Masahiro
单分子荧光光开关在超高密度（Tbits/inch(2)）光学存储器和超高分辨率荧光成像中发挥着重要作用。尽管目前已有多种荧光光致变色分子和荧光蛋白应用于光存储器和超高分辨率成像，但由于缺乏“无损荧光读出能力”，其性能并不理想。在这里，我们报告了具有无损读出能力的分子的新分子设计原理。该分子由受体光致变色二芳基乙烯和供体荧光苝双酰亚胺单元组成。当二芳基乙烯单元在可见光和紫外光照射下在开环异构体和闭环异构体之间转换时，荧光被可逆猝灭。荧光猝灭基于从供体单元到受体单元的电子转移。荧光光开关和无损读出能力在溶液（整体态）和单分子水平上得到了证明。飞秒时间分辨瞬态和荧光寿命测量证实荧光猝灭归因于分子内电子转移。
Single-molecule fluorescence photoswitching plays an essential role in ultrahigh-density (Tbits/inch(2)) optical memories and super-high-resolution fluorescence imaging. Although several fluorescent photochromic molecules and fluorescent proteins have been applied, so far, to optical memories and super-high-resolution imaging, their performance is unsatisfactory because of the absence of "non-destructive fluorescence readout capability". Here we report on a new molecular design principle of a molecule having non-destructive readout capability. The molecule is composed of acceptor photochromic diarylethene and donor fluorescent perylenebisimide units. The fluorescence is reversibly quenched when the diarylethene unit converts between the open- and the closed-ring isomers upon irradiation with visible and UV light. The fluorescence quenching is based on an electron transfer from the donor to the acceptor units. The fluorescence photoswitching and non-destructive readout capability were demonstrated in solution (an ensemble state) and at the single-molecule level. Femtosecond time-resolved transient and fluorescent lifetime measurements confirmed that the fluorescence quenching is attributed to the intramolecular electron transfer.