Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water
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 immobiliz...
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Veröffentlicht in: | Journal of the American Chemical Society 2010-02, Vol.132 (7), p.2404-2409 |
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creator | Cordes, Thorben Vogelsang, Jan Anaya, Milena Spagnuolo, Carla Gietl, Andreas Summerer, Wolfram Herrmann, Andreas Müllen, Klaus Tinnefeld, Philip |
description | 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. |
doi_str_mv | 10.1021/ja9099714 |
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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. 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Am. Chem. Soc</addtitle><description>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.</description><subject>Biotin - chemistry</subject><subject>DNA, Single-Stranded - chemistry</subject><subject>Fluorescent Dyes - chemistry</subject><subject>Imides - chemistry</subject><subject>Oxidation-Reduction</subject><subject>Perylene - analogs & derivatives</subject><subject>Perylene - chemistry</subject><subject>Photochemical Processes</subject><subject>Serum Albumin, Bovine - chemistry</subject><subject>Spectrometry, Fluorescence - methods</subject><subject>Streptavidin - chemistry</subject><subject>Water - chemistry</subject><issn>0002-7863</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2010</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNptkE1Lw0AURQdRbK0u_AOSjYiL6LyZTJJZ2qpVqCh-4DJMJi8ydZLUmaTYf2-ktStXl8s7HHiXkGOgF0AZXM6VpFImEO2QIQhGQwEs3iVDSikLkzTmA3Lg_byvEUthnwwYBQZURkMyfTH1h8XwobGoO4vBMxbNdzC2pv7sL0FTBk_oVhZrDK6NqUzRJzqzVK1Zog9MHbyrFt0h2SuV9Xi0yRF5u715ndyFs8fp_eRqFioeyTYUQkCaJAkyqvMCVSnLXOU8ErFUaRmLKNYasMAYUkXTlAND0AnXDKQoC57zETlbexeu-erQt1llvEZrVY1N57OEcxkxANqT52tSu8Z7h2W2cKZSbpUBzX5ny7az9ezJxtrlFRZb8m-nHjhdA0r7bN50ru6f_Ef0A3Zscko</recordid><startdate>20100224</startdate><enddate>20100224</enddate><creator>Cordes, Thorben</creator><creator>Vogelsang, Jan</creator><creator>Anaya, Milena</creator><creator>Spagnuolo, Carla</creator><creator>Gietl, Andreas</creator><creator>Summerer, Wolfram</creator><creator>Herrmann, Andreas</creator><creator>Müllen, Klaus</creator><creator>Tinnefeld, Philip</creator><general>American Chemical Society</general><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20100224</creationdate><title>Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water</title><author>Cordes, Thorben ; Vogelsang, Jan ; Anaya, Milena ; Spagnuolo, Carla ; Gietl, Andreas ; Summerer, Wolfram ; Herrmann, Andreas ; Müllen, Klaus ; Tinnefeld, Philip</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a349t-55518777e20cbdeaf9fbab34569a8f6546cc1ede618a088312e1c73c2195fd3b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2010</creationdate><topic>Biotin - chemistry</topic><topic>DNA, Single-Stranded - chemistry</topic><topic>Fluorescent Dyes - chemistry</topic><topic>Imides - chemistry</topic><topic>Oxidation-Reduction</topic><topic>Perylene - analogs & derivatives</topic><topic>Perylene - chemistry</topic><topic>Photochemical Processes</topic><topic>Serum Albumin, Bovine - chemistry</topic><topic>Spectrometry, Fluorescence - methods</topic><topic>Streptavidin - chemistry</topic><topic>Water - chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cordes, Thorben</creatorcontrib><creatorcontrib>Vogelsang, Jan</creatorcontrib><creatorcontrib>Anaya, Milena</creatorcontrib><creatorcontrib>Spagnuolo, Carla</creatorcontrib><creatorcontrib>Gietl, Andreas</creatorcontrib><creatorcontrib>Summerer, Wolfram</creatorcontrib><creatorcontrib>Herrmann, Andreas</creatorcontrib><creatorcontrib>Müllen, Klaus</creatorcontrib><creatorcontrib>Tinnefeld, Philip</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>Journal of the American Chemical Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Cordes, Thorben</au><au>Vogelsang, Jan</au><au>Anaya, Milena</au><au>Spagnuolo, Carla</au><au>Gietl, Andreas</au><au>Summerer, Wolfram</au><au>Herrmann, Andreas</au><au>Müllen, Klaus</au><au>Tinnefeld, Philip</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J. 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subjects | Biotin - chemistry DNA, Single-Stranded - chemistry Fluorescent Dyes - chemistry Imides - chemistry Oxidation-Reduction Perylene - analogs & derivatives Perylene - chemistry Photochemical Processes Serum Albumin, Bovine - chemistry Spectrometry, Fluorescence - methods Streptavidin - chemistry Water - chemistry |
title | Single-Molecule Redox Blinking of Perylene Diimide Derivatives in Water |
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