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Elucidating the Single-Molecule Fluo...

Smyder, Julie.

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Elucidating the Single-Molecule Fluorescence Intermittency and Quantum Yield of Nanoscale Particles with Confocal and Scanning Probe Microscopies.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Elucidating the Single-Molecule Fluorescence Intermittency and Quantum Yield of Nanoscale Particles with Confocal and Scanning Probe Microscopies./
Author:	Smyder, Julie.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2020,
Description:	165 p.
Notes:	Source: Dissertations Abstracts International, Volume: 82-07, Section: B.
Contained By:	Dissertations Abstracts International82-07B.
Subject:	Nanoscience. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28148356
ISBN:	9798557045117

Elucidating the Single-Molecule Fluorescence Intermittency and Quantum Yield of Nanoscale Particles with Confocal and Scanning Probe Microscopies.
Smyder, Julie.

Elucidating the Single-Molecule Fluorescence Intermittency and Quantum Yield of Nanoscale Particles with Confocal and Scanning Probe Microscopies. - Ann Arbor : ProQuest Dissertations & Theses, 2020 - 165 p.

Source: Dissertations Abstracts International, Volume: 82-07, Section: B.

Thesis (Ph.D.)--University of Rochester, 2020.

This item must not be sold to any third party vendors.

The single-molecule confocal fluorescence studies of quantum dots and single-walled carbon nanotubes reported here provide insight regarding the effects of excitation parameters and the nature of the low ensemble quantum yield, respectively, to clarify important aspects of experimental design. In one project, the fluorescence dynamics of quantum dots excited with a continuous wave laser were compared with those excited with a pulsed laser at the same average power. The results indicate that caution should be used when designing single-molecule experiments with a pulsed laser as the excitation source. The most significant difference in the blinking statistics was in the on-state falloff values (44 +/- 3 s for continuous wave and 20 +/- 2 s for pulsed), showing a lower probability of long-lived on states under pulsed excitation. Compared to continuous wave excitation, pulsed excitation resulted in faster rates of photobleaching and decreases in fluorescence lifetime over time, highlighting the enhancement of nonradiative processes with pulsed laser exposure. Conversely, the power law exponents were very similar for both types of excitation, demonstrating the usefulness of blinking statistics as a metric when comparing experiments with different excitation parameters despite variations in exciton populations. In the following study, the bright fractions of single-walled carbon nanotube samples were quantified by correlating fluorescence and atomic force microscopy topography images of samples deposited on patterned quartz substrates. Low ensemble quantum yield values were definitively verified to be a result of the large fraction of non-emissive single-walled carbon nanotubes rather than poor emission from all particles in the ensemble. In contrast to previous studies, our method demonstrates the importance of correlation when studying these highly heterogenous samples. For DNA-wrapped single-walled carbon nanotubes, 11% of the particles displayed bright fluorescence; for sodium cholate-wrapped single-walled carbon nanotubes, the bright fraction was 22%, although the sample was considerably smaller. Background information regarding the photophysics, structure, preparation, and applications of these particles is provided, and potential follow-up experiments for both studies are briefly outlined.

ISBN: 9798557045117Subjects--Topical Terms:

587832
Nanoscience.
Subjects--Index Terms:

Atomic force microscopy

Elucidating the Single-Molecule Fluorescence Intermittency and Quantum Yield of Nanoscale Particles with Confocal and Scanning Probe Microscopies.
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520 $a The single-molecule confocal fluorescence studies of quantum dots and single-walled carbon nanotubes reported here provide insight regarding the effects of excitation parameters and the nature of the low ensemble quantum yield, respectively, to clarify important aspects of experimental design. In one project, the fluorescence dynamics of quantum dots excited with a continuous wave laser were compared with those excited with a pulsed laser at the same average power. The results indicate that caution should be used when designing single-molecule experiments with a pulsed laser as the excitation source. The most significant difference in the blinking statistics was in the on-state falloff values (44 +/- 3 s for continuous wave and 20 +/- 2 s for pulsed), showing a lower probability of long-lived on states under pulsed excitation. Compared to continuous wave excitation, pulsed excitation resulted in faster rates of photobleaching and decreases in fluorescence lifetime over time, highlighting the enhancement of nonradiative processes with pulsed laser exposure. Conversely, the power law exponents were very similar for both types of excitation, demonstrating the usefulness of blinking statistics as a metric when comparing experiments with different excitation parameters despite variations in exciton populations. In the following study, the bright fractions of single-walled carbon nanotube samples were quantified by correlating fluorescence and atomic force microscopy topography images of samples deposited on patterned quartz substrates. Low ensemble quantum yield values were definitively verified to be a result of the large fraction of non-emissive single-walled carbon nanotubes rather than poor emission from all particles in the ensemble. In contrast to previous studies, our method demonstrates the importance of correlation when studying these highly heterogenous samples. For DNA-wrapped single-walled carbon nanotubes, 11% of the particles displayed bright fluorescence; for sodium cholate-wrapped single-walled carbon nanotubes, the bright fraction was 22%, although the sample was considerably smaller. Background information regarding the photophysics, structure, preparation, and applications of these particles is provided, and potential follow-up experiments for both studies are briefly outlined.
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