The electronic spin state (S) of metal ions is fundamental to the performance of magnets, protein cofactors, and magnetic resonance imaging (MRI) contrast agents. The ability to manipulate the spin state of transition metals allows for the development of advanced materials with emergent properties. This following chapters will introduce two...
Small hydrocarbons and their oxygenated derivatives are critical to atmospheric organic aerosol formation and growth. Secondary organic aerosols (SOAs) constitute a significant portion of total atmospheric organic aerosols, and are often generated through the oxidation of biogenic volatile organic compounds (VOCs) such as isoprene, -pinene, and -caryophyllene. Interfaces of SOA...
Contained in the following dissertation are detailed investigations regarding the thermodynamics of small molecule activation by metalloporphyrin complexes isolated within metal-organic frameworks (MOFs). Chapter 1 provides a description of the role metalloporphyrin complexes play in biological systems and the challenges associated with studying small molecule activation by metalloporphryin sites in...
Chemical probes are versatile and unique tools for biomedical research. A chemical probe is simply a selective small-molecule modulator of protein function that allows the user to ask mechanistic and phenotypic questions about its molecular target in biochemical, cell-based or animal studies. Experiments involving selective inhibitors can help delineate key...
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...