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....
Proteins are known to have diverse biomedical functions and excellent catalytic performance; however, they are also fragile outside living cells, challenging their use in industrial applications. Metal-organic frameworks (MOFs) are highly porous crystalline materials that consist of metal cluster nodes and organic linkers. With their rigid structures, MOFs can effectively...
Noble metal nanoparticles (NPs) have shown promise as imaging agents, drug delivery platforms, and plasmonic sensors. Anisotropic gold NPs, such as gold nanostars, have particularly received attention due to their shape-dependent optical and spectral properties. With their 3D anisotropic structure with branches protruding into different directions and high surface areas,...
Recent progress in the field of nanomaterials has enabled significant advances in optoelectronic devices such as solar cells, light-emitting diodes, photocatalysts, and sensors. Nanoparticles feature superior optical and electronic properties that arise from quantum confinement and therefore cannot be attained used bulk materials. However, further developments in the field of...
Metallic conductivity and broken inversion symmetry were long thought to be contraindicated properties, under the assumption that long-range Coulombic interactions (screened by free charge carriers) were necessary for coordinated polar displacements. Within the past decade, the discovery of polar metals has prompted a rethinking of the relationship between metallicity and...
Two-dimensional (2D) covalent organic frameworks (COFs) are a class of crystalline polymer networks that polymerize and crystallize into layered structures, characterized by their atomically precise structure, permanent porosity and high modularity. Imine-linked COFs are one of the most important and promising classes of macromolecular sheets, which form by the condensation...
This thesis describes the synthesis and photophysical characterization of low-dimensionalmaterials—including thin-film semiconductors, colloidal quantum dots, and molecules—with the
broader motivation of integrating them into mixed-dimensional heterostructures with novel
responses to external stimuli. Due to their high surface area to volume ratio and incomplete
dielectric screening, mixed-dimensional heterostructures have high sensitivity...
Label-free assays, and particularly those based on the combination of mass spectroscopy with surface chemistries, enable high-throughput experiments of a broad range of reactions. However, these methods can still require the incorporation of functional groups that allow immobilization of reactants and products to surfaces prior to analysis. In this thesis,...
While Li-ion batteries are currently the preferred energy storage technology, multivalent alternatives such as Mg should be considered. Magnesium metal has a high volumetric capacity and has been shown to cycle with no dendrite formation. However, the highly charged Mg2+ ion cannot easily diffuse into the oxide cathodes favored in...
Nanoparticles (NPs) are emerging as attractive drug carriers in therapeutic and diagnostic applications. The physiochemical properties of NPs, such as particle size, shape, and surface chemistry, play important roles in the functions of engineered nanoconstructs−NP cores with surface ligands. Recent work has screened these properties by monitoring cellular uptake and/or...
The building blocks of life are proteins. These incredible nanostructures are responsible for forming the diverse infrastructure of living systems and for performing countless biological functions. In Nature, these materials and systems achieve structural complexity and function through highly regulated and controlled assembly of protein building blocks, driven by specific...
Recent progress in semiconductor synthesis and photophysics has revealed a host of new materials with exciting properties for applications in optoelectronic devices such as sensors, photovoltaics, solid state lighting, and more. One of the most significant recent additions to the field is the class of hybrid and inorganic materials that...
Realizing electromagnetic metamaterials which operate in the optical regime requires creating precise arrangements of sub-100 nm building blocks. As such, fabricating these materials using conventional lithographic methods is extremely costly. On the other hand, bottom-up assembly of nanoparticles into crystalline superlattices offers opportunities to explore the scalable fabrication of 2-...
Amyloid beta oligomers (AβOs) are a key instigator of neurodegeneration in Alzheimer’s disease (AD). The work presented in this thesis includes three disease-modifying approaches to disrupt pathological AβO-related mechanisms in AD: (1) inhibiting AβO buildup, (2) blocking AβO-induced tau phosphorylation, and (3) neutralizing AβOs. These three approaches were tested in...
Gold nanoparticles (AuNPs) display unique characteristics compared to their macro-counterparts that are dependent on shape, size, and attached surface molecules. Methods have been developed to precisely control both size and shape of AuNPs for specific applications. The biocompatibility, plasmonic properties, and ease of functionalization with thiolated molecules, make gold nanoparticles...
Functional electronic materials have transformed modern society toward a highly digitized and interconnected global community. The ever-growing demand for electronic devices with superior functionality poses a great challenge to the state-of-the-art field-effect transistors owing to the limited charge density afforded by silicon. Materials scientists and chemists have been working closely...
Biomedical imaging is an essential part of medicine that enables the non-invasive observation of biological phenomena. This, in turn, allows for more accurate and earlier diagnoses, monitoring of therapies, and even fundamental research into biological processes. Molecular imaging, a fast-growing subdiscipline of biomedical imaging, seeks to image biochemical processes at...
Amyloid beta oligomers (AβOs) are a key instigator of neurodegeneration in Alzheimer’s disease (AD). The work presented in this thesis includes three disease-modifying approaches to disrupt pathological AβO-related mechanisms in AD: (1) inhibiting AβO buildup, (2) blocking AβO-induced tau phosphorylation, and (3) neutralizing AβOs. These three approaches were tested in...
The construction of new C–C bonds remains a central facet of organic chemistry due to its critical role in the synthesis of pharmaceutical compounds and organic materials. Mild and selective methodologies are often required for efficient formation of these bonds in natural product total synthesis, medicinal chemistry campaigns, and more....
Understanding the mechanisms associated with chemical catalysis is vital for not only the rational improvement of their capabilities, but also for the advancement of the fundamental knowledge affiliated with the systems in question. These new insights can help predict new reactivities towards more challenging substrates which will allow for easier...