Angewandte Physik-Biophysik, and Center for NanoScience (CeNS), Ludwig-Maximilians-Universität München, Germany.
J Am Chem Soc. 2010 Feb 24;132(7):2404-9. doi: 10.1021/ja9099714.
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.
超灵敏和超分辨率荧光显微镜的动态发展要求具有更高光稳定性和新功能的改良荧光标记物。我们使用单分子光谱法研究了水溶性苝二酰亚胺荧光团（PDI），通过将荧光团连接到 DNA 上，将其固定在水性缓冲液中。在这些条件下，观察到与单分子相容的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。我们还展示了如何通过使用不同浓度的还原剂和氧化剂来控制 PDI 的荧光，通过光诱导电子转移反应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）概念来解释这些性质。最后，我们评估了如何将 PDI 的这种荧光控制用于水相或有机相中的超分辨率“闪烁显微镜”，以及更普遍地用于单分子光谱学。
