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The Effects of Phase Transfers with ...

Schwabacher, James Ciro.

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The Effects of Phase Transfers with Thiol Ligands on the Optical Properties of Water-Soluble Quantum Dots.

Record Type:	Electronic resources : Monograph/item
Title/Author:	The Effects of Phase Transfers with Thiol Ligands on the Optical Properties of Water-Soluble Quantum Dots./
Author:	Schwabacher, James Ciro.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2020,
Description:	127 p.
Notes:	Source: Dissertations Abstracts International, Volume: 82-04, Section: B.
Contained By:	Dissertations Abstracts International82-04B.
Subject:	Physical chemistry. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28022991
ISBN:	9798664797138

The Effects of Phase Transfers with Thiol Ligands on the Optical Properties of Water-Soluble Quantum Dots.
Schwabacher, James Ciro.

The Effects of Phase Transfers with Thiol Ligands on the Optical Properties of Water-Soluble Quantum Dots. - Ann Arbor : ProQuest Dissertations & Theses, 2020 - 127 p.

Source: Dissertations Abstracts International, Volume: 82-04, Section: B.

Thesis (Ph.D.)--Northwestern University, 2020.

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

This dissertation examines the effects of phase transfers with thiol ligands on the optical properties of quantum dots (QDs) in water by investigating two systems: i) dihydrolipoic acid (DHLA)-capped PbS QDs and ii) thiolated DNA-capped core/shell CdSe/CdS QDs. QDs are bright, monodisperse, and tunable hydrophobic nanoparticles with high photoluminescence (PL) quantum yields (QYs). Phase transfers with thiol ligands impart hydrophilicity to QDs synthesized in organic solvents. However, these procedures often decrease the monodispersity, PL QY, and colloidal stability of the QD ensemble that makes QDs desired as Forster resonance energy transfer (FRET) donors or acceptors in biologically relevant environments. This work probes the relationship between an ensemble's polydispersity and its pH response after phase transfer. The bathochromic shifts of the PL of an ensemble of DHLA-capped PbS QDs can be entirely accounted for by FRET between QDs within aggregates. X-ray scattering techniques indicate that PbS-DHLA QD aggregates are mass fractals formed by clusters of tightly packed QDs in acidic environments. This work, expanding upon existing protocols, presents a new phase transfer method that employs a ternary solvent system to functionalize CdSe/CdS QDs with thiolated-DNA strands in less than one hour without intermediate ligands. This thesis provides insight into the challenges of deploying QDs in aqueous environments and highlights potential solutions.

ISBN: 9798664797138Subjects--Topical Terms:

1981412
Physical chemistry.
Subjects--Index Terms:

Aggregation

The Effects of Phase Transfers with Thiol Ligands on the Optical Properties of Water-Soluble Quantum Dots.
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520 $a This dissertation examines the effects of phase transfers with thiol ligands on the optical properties of quantum dots (QDs) in water by investigating two systems: i) dihydrolipoic acid (DHLA)-capped PbS QDs and ii) thiolated DNA-capped core/shell CdSe/CdS QDs. QDs are bright, monodisperse, and tunable hydrophobic nanoparticles with high photoluminescence (PL) quantum yields (QYs). Phase transfers with thiol ligands impart hydrophilicity to QDs synthesized in organic solvents. However, these procedures often decrease the monodispersity, PL QY, and colloidal stability of the QD ensemble that makes QDs desired as Forster resonance energy transfer (FRET) donors or acceptors in biologically relevant environments. This work probes the relationship between an ensemble's polydispersity and its pH response after phase transfer. The bathochromic shifts of the PL of an ensemble of DHLA-capped PbS QDs can be entirely accounted for by FRET between QDs within aggregates. X-ray scattering techniques indicate that PbS-DHLA QD aggregates are mass fractals formed by clusters of tightly packed QDs in acidic environments. This work, expanding upon existing protocols, presents a new phase transfer method that employs a ternary solvent system to functionalize CdSe/CdS QDs with thiolated-DNA strands in less than one hour without intermediate ligands. This thesis provides insight into the challenges of deploying QDs in aqueous environments and highlights potential solutions.
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