title: Single-molecule redox blinking of perylene diimide derivatives in water.
abstract: 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.
authors.affiliation: Angewandte Physik-Biophysik, and Center for NanoScience (CeNS), Ludwig-Maximilians-Universität München, Germany.
authors.forename: Thorben
authors.initials: T
authors.lastname: Cordes
authors.forename: Jan
authors.initials: J
authors.lastname: Vogelsang
authors.forename: Milena
authors.initials: M
authors.lastname: Anaya
authors.forename: Carla
authors.initials: C
authors.lastname: Spagnuolo
authors.forename: Andreas
authors.initials: A
authors.lastname: Gietl
authors.forename: Wolfram
authors.initials: W
authors.lastname: Summerer
authors.forename: Andreas
authors.initials: A
authors.lastname: Herrmann
authors.forename: Klaus
authors.initials: K
authors.lastname: Müllen
authors.forename: Philip
authors.initials: P
authors.lastname: Tinnefeld
mesh_terms: D001710:Biotin / Q000737:chemistry; D004277:DNA, Single-Stranded / Q000737:chemistry; D005456:Fluorescent Dyes / Q000737:chemistry*; D007094:Imides / Q000737:chemistry*; D010084:Oxidation-Reduction; D010569:Perylene / Q000031:analogs & derivatives* / Q000737:chemistry; D055668:Photochemical Processes; D012710:Serum Albumin, Bovine / Q000737:chemistry; D013050:Spectrometry, Fluorescence / Q000379:methods; D019809:Streptavidin / Q000737:chemistry; D014867:Water / Q000737:chemistry*
chemical_list: D004277:DNA, Single-Stranded; D005456:Fluorescent Dyes; D007094:Imides; C521332:perylenediimide; D014867:Water; D012710:Serum Albumin, Bovine; D010569:Perylene; D001710:Biotin; D019809:Streptavidin