This dissertation seeks to explore how physical forces, notably through the use of magnetic nanoparticles and applied fields, can influence the structural outcomes of colloidal crystals engineered with DNA. Chapter 1 describes how both DNA and magnetic fields can direct the assembly of nanoparticles into periodic and sometimes crystalline materials....
The lanthanides, with their limited orbital effects and high oxophilicity, represent a class of catalytic metals highly distinguished from more commonly-utilized transition metals. Homogeneous lanthanide catalysts often afford high catalytic rates and impressive selectivity. However, challenges regarding the synthesis and utilization of highly air- and water-sensitive organo-lanthanide complexes have limited...
Electrochemical cell devices are increasingly being sought for energy conversion and storage applications due to their high efficiencies and their potential for operating free of greenhouse gas (GHG) emissions. Solid Acid Electrochemical Cells (SAECs), which most commonly employ CsH2PO4 (CDP) as the electrolyte component, are uniquely suited to meet the...
This dissertation investigates the use of organic and semiconductor nanomaterials as chromophores in solar fuels production and energy transfer-mediated [2+2] cycloadditions. A series of novel N-annulated perylene chromophore amphiphiles was synthesized via a modular synthesis. These perylene amphiphiles were found to self-assemble in aqueous solution, forming extended ribbon-like nanostructures that...
Discrete molecules, linear and branched polymers, and disordered cross-linked networks are well studied objects of chemical synthesis. However, two-dimensional polymers (2DPs) have been long missing from this continuum of molecular architectures, both in chemical synthesis and in Nature. Recently, new polymerization strategies and characterization methods have enabled the unambiguous realization...
Raman spectroscopy is an analytical technique that utilizes inelastic scattering of light to obtain structural information of analyte molecules. The weak intrinsic process of Raman scattering, however, can be greatly enhanced when molecules are placed on or near a surface of noble metal with nanostructures. Discovered over 40 years, surface-enhanced...
The objective of molecular imaging is to noninvasively visualize biochemical events in a living system at the cellular level. Magnetic resonance imaging (MRI) is a promising modality for this goal due to its excellent resolution, unlimited depth penetration, and absence of harmful ionizing radiation. MRI techniques frequently use Gd(III)-based contrast...
This dissertation describes investigations into the two primary mechanisms by which the optical bandgap of colloidal quantum dots (QDs) may be post-synthetically modified: (i) by the quantum-confined Stark effect and (ii) by exciton-delocalizing surface capping ligands. This work demonstrates that through the use of ligand-exchange strategies that enable either of...
It is said across numerous disciplines, from biology to architecture to software engineering, that “form ever follows function.” This adage highlights the intimate relationship between structural characteristics and functional properties in many disparate fields of work. Here, we discuss how the catalytic activity and compressibility of metal–organic frameworks (MOFs) are...
Deciphering the targets of axonal projections plays a pivotal role in interpreting neuronal function and pathology. Neuronal tracers are indispensable neurobiology tools for elucidating advanced functions and interactions between different subregions of the brain. Commercially available neuronal tracers include small molecule dyes, viruses, and synthetic nanoparticles. Among these options, viral...