Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water
Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water
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DOI：
10.1021/ja9099714
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发表时间：
2010-02-24
影响因子：
15
通讯作者：
Tinnefeld, Philip
中科院分区：
文献类型：
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作者：
Cordes, Thorben;Vogelsang, Jan;Tinnefeld, Philip
超灵敏和超分辨率荧光显微镜的动态发展需要改进的荧光标记物，具有更高的光稳定性和新功能。我们使用单分子光谱来研究水溶性苝二甲酰亚胺荧光团（PDI），通过将荧光团附着到 DNA 来固定在水缓冲液中。在这些条件下，观察到与单分子兼容有机荧光团相当的明亮荧光，具有均匀的光谱和荧光衰减时间分布。我们还展示了如何使用不同浓度的还原剂和氧化剂通过光诱导电子转移反应来控制 PDI 的荧光，从而产生闪烁或稳定的发射。我们通过 PDI 的氧化还原电位和最近引入的 ROXS（还原和氧化系统）概念来解释这些特性。最后，我们评估了如何将 PDI 的荧光控制用于水性或有机介质中的超分辨率“闪烁显微镜”，更广泛地用于单分子光谱学
Dynamic developments in ultrasensitive and superresolution fluorescence microscopy call for improved fluorescence markers with increased photostability and new functionalities We used single-molecule spectroscopy to study water-soluble perylene dicarboximide fluorophores (PDI), which were immobilized in aqueous buffer by attaching the fluorophore to DNA Under these conditions bright fluorescence, comparable to that of single-molecule compatible organic fluorophores, is observed with homogeneous spectral and fluorescence decay time distributions. We additionally show how the fluorescence of the PDI can be controlled through photoinduced electron-transfer reactions by using different concentrations of reductants and oxidants, yielding either blinking or stable emission. We explain these properties by the redox potentials of PDI and the recently introduced ROXS (reducing and oxidizing system) concept Finally, we evaluate how this fluorescence control of PDIs can be used for superresolution "Blink-Microscopy" in aqueous or organic media and more generally for single-molecule spectroscopy