The expanding use of nanomaterials in consumer products challenges scientists to understand the impact of these materials before their inevitable release into the environment. In the same way that the widespread use of DDT and asbestos has caused unforeseen negative impacts on both the environment and on human health, the...
My research interests, which span organic, inorganic, physical and biochemistry, have focused broadly on photo-, magneto- and redox-active molecules, especially those with potential applications in organic photovoltaics, spintronics and electronics. My research under the joint supervision of Professor Wasielewski and Professor Fraser Stoddart has concentrated upon understanding electronic and magnetic...
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...
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...
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...