Date of Award

Spring 1-1-2016

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Chemical & Biochemical Engineering

First Advisor

Prashant Nagpal

Second Advisor

Stephanie J. Bryant

Third Advisor

Anushree Chatterjee

Fourth Advisor

Barbara Demmig-Adams

Fifth Advisor

Wei Zhang

Abstract

The unique properties of nanomaterials have engendered a great deal of interest in applying them for applications ranging from solid state physics to bio-imaging. One class of nanomaterials, known collectively as quantum dots, are defined as semiconducting crystals which have a characteristic dimension smaller than the excitonic radius of the bulk material which leads to quantum confinement effects. In this size regime, excited charge carriers behave like prototypical particles in a box, with their energy levels defined by the dimensions of the constituent particle. This is the source of the tunable optical properties which have drawn a great deal of attention with regards to finding appropriate applications for these materials.

This dissertation is divided into multiple sections grouped by the type of application explored. The first sectoin investigates the energetic interactions of physically-coupled quantum dots and DNA, with the goal of gaining insight into how self-assembled molecular wires can bridge the energetic states of physically separated nanocrystals. Chapter 1 begins with an introduction to the properties of quantum dots, the conductive properties of DNA, and the common characterization methods used to characterize materials on the nanoscale. In Chapter 2 scanning tunneling measurements of QD-DNA constructs on the single particle level are presented which show the tunable coupling between the two materials and their resulting hybrid electronic structure. This is expanded upon in Chapter 3 where the conduction of photogenerated charges in QD-DNA hybrid thin films are characterized, which exhibit different charge transfer pathways through the constituent nucleobases depending on the energy of the incident light and resulting electrons. Complementary investigations of energy transfer mediated through DNA are presented in Chapter 4, with confirmation of Dexter-like transfer being facilitated through the oligonucleotides.

The second section quantifies the use of cadmium telluride quantum dots as light-activated therapeutics for treating multi-drug resistant bacterial infectoins. A review of the physiological effects of cadmium chalcogenide quantum dots is first presented in Chapter 5 which provides a foundation for understanding the inherent toxicity of these materials. The phototoxic effect induced by CdTe quantum dots is then introduced in Chapter 6 showing the reduction in growth of gram-negative bacteria. Additional insight is provided in Chapter 7 which discusses the therapeutic mechanism and the oxygen-centered radical species which are formed by the application of light in aqueous media. The section closes with Chapter 8 describing efforts to improve the stability and bio-compatibility of the dots using various surface treatments, and shows that stability can be improved by the passivation of the quantum dots’ anionic facets, though at the cost of overall radical generation.

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