Date of Award

2015

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Graduate Group

Chemical and Biomolecular Engineering

First Advisor

John C. Crocker

Abstract

Programmable DNA interactions are an effective and versatile tool in the field of colloidal directed self-assembly. Colloidal systems are programmed by manipulating a variety of tunable parameters, such as particle sizes and DNA interaction strengths, and can self-assemble into a large and growing variety of colloidal crystal and gel structures. Since isotropically-interacting spherical particles generally form close-packed structures, the production and use of building blocks with anisotropic interactions, such as polyhedral particles, colloidal clusters, and patchy colloids, has been a rich research area in recent years.

This work represents a true expansion of the capabilities of DNA-directed colloidal assemblies, and presents scalable and facile processes for the high-yield generation of stable colloidal clusters and patchy particles with targeted symmetries. We have developed, in Colloidal Crystal Templating and Reprogrammable DNA Interactions, highly tunable tools for the synthesis of such anisotropic building blocks for DNA-directed assembly applications. Notably, these processes are scalable both in batch size and in the size of the resulting building blocks due to the three-dimensional nature of the templates. More notably, these systems are highly tunable and expandable. The templates are only limited by the ever-expanding library of colloidal crystals generated using DNA interactions. The tunability of DNA interactions is virtually unlimited due to DNA's ability to be reprogrammed and edited by enzymes. Finally, the constituent particles are not limited to polystyrene and gold, but can be of any material that can be synthesized into colloids on the micro- and nano-scales and subsequently functionalized with DNA.

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