THE DYNAMICS OF DNA-CAPPED GOLD NANOPARTICLE SUPERLATTICE ASSEMBLY IN ELECTROLYTE SOLUTIONS
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Abstract
Highly ordered nanoparticle arrays, or nanoparticle superlattices, are a sought
after class of materials due to their novel physical properties, distinct from both the
individual nanoparticle and the bulk material from which they are composed. Several
successful methods have been established to produce these exotic materials. One method in particular, DNA-mediated assembly, has enabled a stunning variety of lattice
structures to be constructed. By covalently conjugating DNA molecules to nanoparticle
surfaces, this method uses the sequence binding specificity of DNA to mediate the large-scale assembly of nanoparticles. This method however, relies on complex sequence
design, and is optimized to a very specific set of solution parameters, such as pH, ionic
strength, and temperature.
Here, we sought to expand the parameter base in which DNA capped gold
nanoparticles can form superlattices in solution. This was achieved by treating DNA as a
generic polymer, namely by eliminating the complex base-pairing interactions, greatly
simplifying the assembly process. In particular we aimed to understand the solution phase
parameters governing the assembly dynamics of DNA-capped gold nanoparticles. The
adsorption dynamics of individual DNA-capped gold nanoparticles on a positively
charged substrate was first characterized in various electrolyte solutions, establishing a
kinetic model of adsorption. These same parameters were then used to facilitate the self-assembly of three-dimensional DNA-capped gold nanoparticles in solution. Finally,
progress towards the application of solution phase two-dimensional nanoparticle
superlattices was undertaken. We envision that this work characterizing and elucidating
the solution phase dynamics of DNA-capped gold nanoparticles will serve to ultimately
facilitate their application in functional materials.
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2017-05-30
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Keywords
crystallization; Gold Nanoparticles; superlattices; Physical chemistry; Materials Science; DNA; Nanoparticles; Self-assembly
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Committee Chair
Luo, Dan
Committee Co-Chair
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Wiesner, Ulrich B
Pollack, Lois
Pollack, Lois
Degree Discipline
Biological and Environmental Engineering
Degree Name
Ph. D., Biological and Environmental Engineering
Degree Level
Doctor of Philosophy
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Government Document
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dissertation or thesis