Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 106, Issue 20, Pages 8107-8112Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0811875106
Keywords
electron transfer; molecular switch; sensor; single-molecule spectroscopy
Categories
Funding
- Biophotonics III Program of the BMBF/VDI [13N9234]
- Nanosystems Initiative Munich
- Ludwig-Maximilians-Universitat-Innovative Functional NanoSystems''
- Elite Network of Bavaria
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Fluorescent molecular switches have widespread potential for use as sensors, material applications in electro-optical data storages and displays, and superresolution fluorescence microscopy. We demonstrate that adjustment of fluorophore properties and environmental conditions allows the use of ordinary fluorescent dyes as efficient single-molecule switches that report sensitively on their local redox condition. Adding or removing reductant or oxidant, switches the fluorescence of oxazine dyes between stable fluorescent and non-fluorescent states. At low oxygen concentrations, the off-state that we ascribe to a radical anion is thermally stable with a lifetime in the minutes range. The molecular switches show a remarkable reliability with intriguing fatigue resistance at the single-molecule level: Depending on the switching rate, between 400 and 3,000 switching cycles are observed before irreversible photodestruction occurs. A detailed picture of the underlying photoinduced and redox reactions is elaborated. In the presence of both reductant and oxidant, continuous switching is manifested by blinking'' with independently controllable on- and off-state lifetimes in both deoxygenated and oxygenated environments. This continuous switching mode'' is advantageously used for imaging actin filament and actin filament bundles in fixed cells with subdiffraction-limited resolution.
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