The work presented in this dissertation examines the interplay between electron transfer reactions and electron spin in photoactive organic molecules. Organic compounds that undergo electron transfer reactions after absorbing light are important in natural photosynthesis, photobiology, and synthetic photovoltaics. These electron transfer reactions depend on the spin states of the...
The development of organic photovoltaic devices benefits from understanding the fundamental processes underlying charge generation in thin films of organic semiconductors. This dissertation exploits model systems of π-stacked chromophores such as perylene-3,4:9,10-bis(dicarboximide) (PDI) and 3,6-bis(aryl)diketopyrrolopyrrole (DPP) to study these processes using ultrafast electronic and vibrational spectroscopy. In particular, the characterization...
This dissertation describes the fundamental studies of photoinduced charge-carrier transfer from colloidal metal chalcogenide quantum dots (QDs) to surface-adsorbed molecular redox partners. In addition, we also present the use of visible-light absorbing QDs in photocatalytic applications. CdS QDs are used as photocatalysts in a C-C coupling reaction, in which no...
Three-dimensional (3D) and two-dimensional (2D) hybrid halide perovskites have emerged as front-runners in solar energy conversion applications with the potential to provide low-cost renewable energy. Being at the interface of chemistry, physics, materials science, and electrical engineering, the field of perovskite solar cells has become a top area of interest...
Bulk heterojunction (BHJ) organic photovoltaic (OPV) devices have been extensively studied to achieve power conversion efficiencies well above 10%. New research into alternative materials that allow for cheaper and more industrially viable fabrication of flexible solar cells has been at the forefront of the energy field for the past few...
Quantum information processing (QIP) is an emerging computational paradigm with the potential to enable a vast increase in computational power, fundamentally transforming fields from structural biology to finance. QIP employs qubits, or quantum bits, as its fundamental units of information, which can exist in not just the classical states of...
Plasmonic chemistry is an emerging field of research that contains great promise for new chemical reactivity, but thus far has been improperly observed. The goals of using plasmonic chemistry typically revolve around the use of nonequilibrium charge carriers that migrate to the surface of a plasmonic substrate to perform redox...
The tools of computational chemistry allow researchers to gain insight into chemical systems that would be difficult or impossible to gain experimentally. This dissertation discusses the application of several of these computational tools to chemical systems of interest. First, we present several studies of plasmon resonance in Ag nanoclusters using...
The nonlinear optical technique, second harmonic generation (SHG), is applied here for the first time to probe single and double strand DNA (ssDNA and dsDNA) chemically attached to fused quartz/water interfaces. DNA interfaces are often a critical functional component of biodetection, thus, the development of molecular biosensors requires a thorough...
Many metal ions are of critical importance in many cellular functions. The very properties of these metal ions that make them useful also make them toxic to the cell. In the course of evolution, many metal ion homeostasis systems have developed to provide balance between the necessity and toxicity of...