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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Characterization of Single Quantum Dot Blinking

Amecke-Mönnighoff, Nicole 30 June 2015 (has links) (PDF)
This thesis addresses the observed fluorescence intermittency of single semiconductor nanocrystals, so called Quantum Dots (QDs), which is also referred to as blinking. Despite continuous excitation their fluorescence is randomly interrupted by dark periods that can last over several minutes. Especially the extraction of power law dwell time statistics in bright and dark states indicates very complex underlying processes that are not fully understood to date. Here two approaches are followed to reveal the nature of the blinking mechanism. One addresses the common threshold method for extraction of power law dwell times. Its performance is tested with simulations to a broad range of experimentally determined parameters. Strong deviations are found between input and extracted statistics dependent on input parameters themselves. A comparison with experimental data does not support the assignment of power law statistics for the bright state and indicates the existence of distinct blinking mechanisms. The second approach directly aims at the nature of the dark state, which is mostly attributed to charges in the QD or trap states in its vicinity. A method is developed to detect charging processes on single QDs with their fluorescence. Electrochemistry is combined with confocal microscopy also allowing evaluations of excited state lifetimes and emission spectra. Reduction and oxidation of the QD bands are successfully observed as a quenching of QD fluorescence. Single QD observations identify two independent blinking mechanisms, that are assigned to positive and negative charging. Positive charging is not only observed after hole injection but also the extraction of excited electrons. Three additional quenching mechanisms are identified, two of which are assigned to trap relaxation. Differences between two substrate electrodes demonstrate the importance of the substrate material.
2

Characterization of Single Quantum Dot Blinking: Dwell Time Statistics and Electrochemical Control

Amecke-Mönnighoff, Nicole 20 May 2015 (has links)
This thesis addresses the observed fluorescence intermittency of single semiconductor nanocrystals, so called Quantum Dots (QDs), which is also referred to as blinking. Despite continuous excitation their fluorescence is randomly interrupted by dark periods that can last over several minutes. Especially the extraction of power law dwell time statistics in bright and dark states indicates very complex underlying processes that are not fully understood to date. Here two approaches are followed to reveal the nature of the blinking mechanism. One addresses the common threshold method for extraction of power law dwell times. Its performance is tested with simulations to a broad range of experimentally determined parameters. Strong deviations are found between input and extracted statistics dependent on input parameters themselves. A comparison with experimental data does not support the assignment of power law statistics for the bright state and indicates the existence of distinct blinking mechanisms. The second approach directly aims at the nature of the dark state, which is mostly attributed to charges in the QD or trap states in its vicinity. A method is developed to detect charging processes on single QDs with their fluorescence. Electrochemistry is combined with confocal microscopy also allowing evaluations of excited state lifetimes and emission spectra. Reduction and oxidation of the QD bands are successfully observed as a quenching of QD fluorescence. Single QD observations identify two independent blinking mechanisms, that are assigned to positive and negative charging. Positive charging is not only observed after hole injection but also the extraction of excited electrons. Three additional quenching mechanisms are identified, two of which are assigned to trap relaxation. Differences between two substrate electrodes demonstrate the importance of the substrate material.

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