The surface chemistry of nanoparticles imparts colloidal stability to nanoparticles by acting as barriers between their surrounding environment and the nanoparticles. Gold nanoparticles (AuNPs) are an ideal platform for many studies because of localized surface plasmon resonant properties, chemical stability, and the relative ease of modifying their surfaces with a wide variety of molecular coatings (e.g., alkanethiolates). Understanding and improving the physicochemical stability of these surface-modified nanoparticles is essential for their reproducible use in each application. The long-term colloidal stability of AuNPs relies on the resistance of their surface modifications to thermal degradation, chemical attack and oxidizing conditions. For this purpose, my research has been focused on determining the quality of molecular coatings on gold nanoparticles, and developing techniques, which are complementary to each other, to assess the quality factor of these coatings. Gold nanoparticles with varied qualities of molecular coatings were prepared and tested for their relative stabilities under various physical (e.g., temperature, time, laser irradiation) and chemical (e.g., in presence of metal etchants) conditions. We found that the quality of molecular coatings on AuNPs depends on the process conditions such as solution composition (e.g., the presence of co-surfactants, concentration of excess surfactants), density of capping molecules, and process time, used to form these coatings. We found that higher quality molecular coatings on the gold colloids increased the chances that the particles would remain stable over the over the duration of their intended use. Those colloids modified with relatively higher quality self-assembled monolayers were also more resistant to cyanide etching. These results highlight the importance of methodology for preparing high quality monolayers on nanoparticles and testing their ability to remain stable over the duration of their intended use, for example, during photothermal processes. In addition, the loading of DNA molecules onto AuNPs was tuned to achieve varying densities of DNA, and through this work, achieved the highest reported loading of single-stranded DNA (ss-DNA) molecules on gold nanorods. These high loadings of DNA oligonucleotides could enable a high loading of therapeutics onto the nanorods, which could translate into a higher or more prolonged delivery of therapeutic doses when actived by photothermal or other processes.
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Thesis advisor: Gates, Byron D.
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