Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water

THORBEN CORDES; JAN VOGELSANG; MILENA ANAYA; CARLA SPAGNUOLO; ANDREAS GIETL; WOLFRAM SUMMERER; ANDREAS HERRMANN; KLAUS MU¨ELLEN; PHILIP TINNEFELD

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

ACS

Lugar: Washington; Año: 2010 vol. 132 p. 2404 - 2409

0002-7863

Dynamic developments in ultrasensitive and superresolution fluorescence microscopy call forimproved fluorescence markers with increased photostability and new functionalities. We used singlemolecule 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.