The physical boundary layer, or interface, between two different phases of matter is the site of chemical and physical processes that are critical to many research fields. Many of these interfaces contain electric charge, which influences the structure and composition of the interfacial region and the interactions between the interface...
This thesis describes the relationships between nanoscale structure and particle transport in two systems: i) the transport and conversion of excitons in colloidal quantum dot (QD) assemblies and ii) the transport of carriers in flashing electron ratchets. One major crux in the creation of efficient photocatalytic systems is the low...
Spin-orbit coupling (SOC) is a powerful phenomenon that dictates the functional properties of transition metal complexes essential for information processing, catalysis, and magnetism. Though it is relegated to lower energy scales within the orbital description of first-row transition metal complexes, SOC impacts crucial aspects of electronic structure such as promoting...
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...
This thesis describes a series of fundamental studies that address the role of electrostatic interactions in modulating i) the permeability of the ligand shell of a colloidal quantum dot (QD) to an anionic redox probe; ii) the resulting yield of photoinduced electron exchange within the QD ‒ redox probe complex;...