In this thesis, I present the development and benchmarking of several theoretical methods designed to enable the rigorous modeling of magnetic properties of molecules containing one or a few heavy atoms, particularly single-molecule magnets. The new methods use a full four-component treatment of relativity, allowing spin–orbit effects to be taken...
Oxide/aqueous and metal/metal oxide interfaces are essential for environmental remediation, catalysis, and corrosion inhibition, in addition to their potential implementation as energy transducers, consumer electronics, and coating products. While these interfaces are critically important, they are difficult to access experimentally under aqueous flow conditions. This thesis describes results obtained with...
When attached to another species (e.g. a nanoparticle), the sequence specificity of DNA can be repurposed to program interactions between such entities and to direct their formation into ordered structures. The research presented in this thesis aims to push the boundaries of structures that can be made via this approach....
Harnessing the metabolic potential of methanotrophic bacteria is a compelling strategy for the bioremediation of environmentally harmful methane gas. Methanotrophs can activate a 105 kcal/mol C-H bond in methane at ambient conditions using metalloenzymes called methane monooxygenases (MMOs). Particulate methane monooxygenase (pMMO) is a copper-dependent, membrane-bound enzyme that is the...
The work of this dissertation seeks to enhance the understanding of DNA-driven nanoparticle assembly and introduce kinetic routes to control mesoscale crystal habit and size. Chapter 1 describes the state of the art in the field of nanoparticle assembly and, specifically, DNA- mediated nanoparticle assembly, where the concept of a...
Techniques in atomic physics have delivered some of the most precise measurements ever made, with frequency measurements reaching fractional precisions of 10^18 . High precision measurements can be used to test fundamental physics, such as pursuing a variation in fundamental constants. A finite drift in measurable constants such as the...
Small molecules such as indanes, chromanes, tetralins and their derivatives play a significant role in drug discovery due to their potent biological activity. This research herein presents a facile Brønsted acid-catalyzed allylsilane annulation methodology to generate fused ring systems such as indanes. The reaction goes through a homoallylic intermediate which...
In this dissertation, efforts are detailed to utilize semiquinoid bridging ligands to impart strong magnetic coupling between metal centers. Chapter 1 introduces the synthetic challenge of realizing molecule-based magnets with high operating temperatures due to weak magnetic coupling between spin centers through large, diamagnetic ligands. An alternative strategy is described...
This dissertation develops computational models to study the optical coupling between plasmonic nanoparticles and quantum emitters. A large number of nanophotonic applications function by using either plasmon enhanced fields to enhance optical processes within quantum emitters or the sensitivity of plasmon resonances to their environment. Developing computational methods to fully...
Synthetic organic chemistry continues to be a driver in the discovery and development of new molecules for applications in biology, medicine, crop science, polymer science, and materials science. Central to the continued development of this field is the pursuit of new strategies and methods for the efficient construction of molecules...