Publications

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In recent years pyrolysis of interferometrically-patterned photoresists has produced three-dimensionally nanopatterned, electrically conductive carbon films with applications from energy storage to biological sensing. We investigate here conditions for rapid thermal pyrolysis that drastically reduce film processing time (from hours to minutes) while preserving the films' unique nanoscale morphology, film adhesion, and electrochemical properties. We specifically show that heating rate dramatically affects nanoscale morphology, while reducing atmosphere composition, dwell time, and dwell temperature impact the electrochemical performance of these rapidly pyrolyzed nanostructures. Accelerated processing with rapid thermal pyrolysis may facilitate the expanded applicability and rapid fabrication of these promising nanostructured materials. © 2012 Elsevier Ltd. All rights reserved.

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Formation of complex nanomaterials would ideally involve single-pot reaction conditions with one reactive site per nanoparticle, resulting in a high yield of incrementally modified or oriented structures. Many studies in nanoparticle functionalization have sought to generate highly uniform nanoparticles with tailorable surface chemistry necessary to produce such conjugates, with limited success. In order to overcome these limitations, we have modified commercially available nanoparticles with multiple potential reaction sites for conjugation with single ssDNAs, proteins, and small unilamellar vesicles. These approaches combined heterobifunctional and biochemical template chemistries with single molecule optical methods for improved control of nanomaterial functionalization. Several interesting analytical results have been achieved by leveraging techniques unique to SNL, and provide multiple paths for future improvements for multiplex nanoparticle synthesis and characterization. Hyperspectral imaging has proven especially useful for assaying substrate immobilized fluorescent particles. In dynamic environments, temporal correlation spectroscopies have been employed for tracking changes in diffusion/hydrodynamic radii, particle size distributions, and identifying mobile versus immobile sample fractions at unbounded dilution. Finally, Raman fingerprinting of biological conjugates has been enabled by resonant signal enhancement provided by intimate interactions with nanoparticles and composite nanoshells.