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  • 2000-2004  (3)
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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 3117-3120 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Single molecule confocal microscopy is used to study fluorescence intermittency of individual ZnS overcoated CdSe quantum dots (QDs) excited at 488 nm. The confocal apparatus permits the distribution of "on" and "off" times (i.e., periods of sustained fluorescence emission and darkness) to be measured over an unprecedentedly large dynamic range (109) of probability densities, with nonexponential behavior in τoff over a 105 range in time scales. In dramatic contrast, these same τoff distributions in all QDs are described with remarkable simplicity over this 109-fold dynamic range by a simple inverse power law, i.e., P(τoff)∝1/τoff1+α. Such inverse power law behavior is a clear signature of distributed kinetics, such as predicted for (i) an exponential distribution of trap depths or (ii) a distribution of tunneling distances between QD core/interface states. This has important statistical implications for all previous studies of fluorescence intermittency in semiconductor QDs and may have broader implications for other systems such as single polymer molecules. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 1028-1040 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Single molecule confocal microscopy is used to investigate the detailed kinetics of fluorescence intermittency in colloidal II–VI (CdSe) semiconductor quantum dots. Two distinct modes of behavior are observed corresponding to (i) sustained "on" episodes (τon) of rapid laser absorption/fluorescence cycling, followed by (ii) sustained "off" episodes (τoff) where essentially no light is emitted despite continuous laser excitation. Both on-time and off-time probability densities follow an inverse power law, P(τon/off)∝1/τon/offm, over more than seven decades in probability density and five decades in time. Such inverse power law behavior is an unambiguous signature of highly distributed kinetics with rates varying over 105-fold, in contrast with models for switching between "on" and "off" configurations of the system via single rate constant processes. The unprecedented dynamic range of the current data permits several kinetic models of fluorescence intermittency to be evaluated at the single molecule level and indicate the importance of fluctuations in the quantum dot environment. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 8596-8609 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The dramatic modifications of molecular fluorescence in the proximity of a sharp nanoscopic probe is investigated by an apertureless or antenna-based near-field scanning optical microscope, which exploits the interactions between a fluorescent sample and a laser illuminated Si atomic force microscope probe. Specifically, luminescence is monitored from evanescently excited, dye-doped polystyrene nanospheres (RS=20–80 nm) on a fused silica prism surface as a function of probe-sample geometry. The incident laser field is enhanced in the near-field of the probe tip, resulting in images with high sensitivity (σmin(approximate)2 Å2 in a 1 Hz detection bandwidth) and strongly subdiffraction-limited spatial resolution. At probe-sample distances greater than (approximate)λ/2, the images are dominated by far-field interference between (i) direct fluorescence from the molecular sample and (ii) indirect fluorescence from image dipoles induced in the atomic force microscope probe. Near-field "shadowing" of the molecular fluorescence by the probe also occurs and is studied as a function of probe-sample-detector geometry. Finally, effects of probe-sample proximity on the fluorescence emission spectrum are investigated. In summary, the data elucidate several novel near- and far-field molecular fluorescence enhancement effects relevant to further development of molecular and nanostructural spectroscopic methods with spatial resolution well below the diffraction limit. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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