Emissions from solid fuel use play a role both in climate forcing of the atmosphere and in the health ofthe global population through exposures in homes and contributions of solid fuel use to ambient and regional air pollution. Assessments of the overall impacts from emissions from household solid fuels used in cookstoves at a population level have been hampered by large variations in reported emission factors measured using different approaches with inconsistent conclusions between fuel types. In this thesis, emissions from traditional Indian cookstoves are evaluated for animal dung and brushwood, two of the most commonly utilized fuels in India, using both uncontrolled in-home measurements and minimally-directed cooking tasks performed in rural Indian kitchens. Following the validation of a moisture probe for use with dung fuels, emissions measurements from both the minimally directed and uncontrolled cooking tests demonstrated a negative correlation between fine particulate (PM2.5) emission factors and global forcing using 100-year global warming potentials. While the United Nations Clean Development Mechanism and voluntary carbon markets have featured emissions from cookstoves with a value of approximately 10 million dollars per year in 2020, these measurements that for the first time also include formation of secondary organic aerosol imply cookstoves are climate neutral at ~10 grams of primary PM2.5 per kilogram of dry fuel, which falls squarely in the middle of the range of emissions typically reported in global inventories (5-12 g/kg dry fuel). Emissions from solid fuels in cookstoves also cause major health burdens in global populations. In 2016, emissions from solid fuels were estimated to cause 2.6 million deaths and 77 million DALYS on a global basis, greater than Malaria, HIV and TB combined. Current global burden of disease approaches, however, do not incorporate the approximately 500 million people who live in homes that primarily cook outdoors. To refine estimates of the health burdens caused by solid fuel use, models were developed to estimate personal exposure contributions from outdoor emissions to allow the incorporation of outdoor cooking into Global Burden of Disease models. Notably, emissions from outdoor cooking can be much higher than those of indoor cooking while still contributing to personal exposures at levels less than the World Health Organization Air Quality Guidelines (WHO AQG) and interim targets due to the greater dispersion of pollutants in outdoor environments. While particulate matter emissions from solid fuel use are comprised of a wide variety of compounds, many unique to different fuel types, polycyclic aromatic hydrocarbons (PAHs) have been recognized as some of the more toxic constituents of particulate matter emissions, and are associated with cancer endpoints. In these emissions measurements, the ratio of high- to low-temperature combustion was predictive of synthesis of 2-3 ring particulate bound PAHs. Increased elemental carbon (EC) emissions, however, were better predicted by increases in modified combustion efficiency (MCE), since EC emissions reflect the balance between increased PAH synthesis and soot formation which reduces PAH concentrations. To estimate overall health implications of emissions from these stoves a modified box-model was used to estimate personal exposures to mixed fuels used in the Chulha, which would result in an average of approximately 2.7 cancers per 100,000 individuals cooking with these fuels. To alleviate these health burdens a suite of interventions are necessary, however, the effectiveness of different interventions approaches has not been systematically evaluated. Meta-analysis of randomized control trials of interventions indicated that use of simple chimneys and hoods were often more effective than the installation of unvented advanced combustion cookstoves in homes.

Trinity is a large-scale piece of program music for a symphony orchestra expanded to include two electric guitars (doubling on acoustic guitar), piano (doubling on Fender Rhodes Electric Piano), electric bass guitar and drumset. The main philosophical impetus for this piece is the programmatic depiction (in the manner of a tone poem) of a concept which is based on and combines archetypal characters drawn primarily from literary sources. This dissertation is titled Trinity and uses the thesis that the three chosen archetypes, The Architect, The Leper and the Gunslinger, are three aspects of the same über-archetype which is representative of both humanity the human individual - this concept being a composite of Ayn Rand's "Fountainhead," Friedrich Nietzsche's Übermensch and god (as a human construct). The description of the trinity is - in a similar manner to Christian belief - the description of an individual through the lens of three contrasting, complementary and singular personalities, which is both god and human; it is a deified version of the Übermensch as represented by the Architect, Leper and Gunslinger.

This piece utilizes symmetrical and asymmetrical synthetic scales (and their associated aggregates), multiple and simultaneous tonal centers, drone and repetition/sequencing and looping and a rhythmic concept which uses the employment of multiple and simultaneous rhythmic cells in various meters and subdivisions (of the meter) in a manner reminiscent of melodic counterpoint. Trinity is five movements long and arranged similar to a Romantic-era symphony- an introduction, followed by three movements - one for each archetype, then a finale. The five movements are bookended by related music intended to function in a musical analogue to "Once upon a time..." and "...happily ever after."

Included with the musical score is a prose document - which explicates the philosophical and metaphorical construct and associated personal implications and which details the compositional techniques used - and a folder containing audio files of the entire score. The audio files were created using live musicians and MIDI-realizations.

Since the industrial revolution, the concentration of atmospheric CO2 has drastically risen. Currently, the CO2 reduction reaction (CO2RR) has been extensively studied to convert CO2 into higher values products like CO, formic acid, methane, etc. Industrially, the first step of the CO2RR is to capture the CO2 using some capture agent, typically an amine. However, as these chemicals bind CO2 quite strongly a large amount of thermal energy is required to liberate the CO2. Thus, it has been proposed to directly reduce the capture agent in the general captured CO2 reduction reaction (c-CO2RR). This work is a prospective on Ag that considers different capture agents, proton source effects, and facets. We show that the proton source chosen has a large effect on the reactivity, we show that methanol is predicted to be a competitive capture agent compared to NH3, and we show that steps and kinks sites hinder or do not improve the c-CO2RR. However, overall, we determine that on Ag the HER dominates and therefore, further catalyst development is necessary.

Understanding the structure and composition of aqueous interfaces is one of the most important current problems in modern science. Aqueous interfaces are ubiquitous in Nature, ranging from aerosols to cellular structures. Aerosol chemistry is presently the most significant unknown factor in predicting climate change, and an understanding of the chemistry that occurs at aerosol interfaces would significantly improve climate models. Similarly, the nature of aqueous biological interfaces has a profound effect on the structure and function of proteins and other biological structures. Despite the importance of these problems, aqueous interfaces remain incompletely understood due to the challenges of experimentally probing them.

Recent experimental and theoretical results have firmly established the existence of enhanced concentrations of selected ions at the air/water interface. In this dissertation, I use an interface-specific technique, UV second harmonic generation (SHG), to further investigate the adsorption of ions to the air/water interface and to extend the study of ion adsorption towards more biologically relevant systems, alcohol/water interfaces.

In Chapter 2, I describe resonant UV-SHG studies of the strongly chaotropic thiocyanate ion adsorbed to the interface formed by water and a monolayer of dodecanol, wherein the Gibbs free energy of adsorption was determined to be -6.7 ± 1.1 and -6.3 ± 1.8 kJ/mol for sodium and potassium thiocyanate, respectively, coincident with the value determined for thiocyanate at the air/water interface. Interestingly, at concentrations near and above 4 M, the resonant SHG signal increases discontinuously, indicating a structural change in the interfacial region.

Recent experimental and theoretical work has demonstrated that the adsorption of bromide is particularly important for chemical reactions on atmospheric aerosols, including the depletion of ozone. In Chapter 3, UV-SHG resonant with the bromide charge-transfer-to-solvent band and a Langmuir adsorption model are used to determine the affinity of bromide for both the air/water and dodecanol/water interfaces in the molar concentration regime. The Gibbs free energy of adsorption for the former is determined to be -1.4 kJ/mol with a lower 90% confidence limit of -4.1 kJ/mol. For the dodecanol/water interface the data are best fit with a Gibbs free energy of +8 kJ/mol with an estimated a lower limit of -4 kJ/mol.

Adsorption of ions to the air/water interface in the millimolar regime is a particularly interesting phenomenon. In Chapter 4, the affinity of sodium chloride and sodium bromide to the air/water interface is probed by UV-SHG. Both salts exhibit a strong adsorption, with free energies greater than -20 kJ/mol. Interestingly, sodium chloride exhibits a stronger affinity for the interface than does sodium iodide, which was previously studied by Poul Peterson. This is counter to both experimental and theoretical results for higher concentrations. It has been predicted that ion adsorption is dictated by strong and opposing electrostatic and entropic forces. The change in order of ion interfacial affinity can be explained by relatively small changes in these forces at different concentrations and ionic strengths.

In Chapters 5 and 6, other work using nonlinear optical techniques is described. Coherent anti-Stokes Raman scattering microscopy is a promising tool for chemically selective imaging based on molecular vibrations. While CARS is currently used as a biological imaging tool, many variations are still being developed, perhaps the most important being multiplex CARS microscopy. Multiplex CARS has the advantage of comparing images based on different molecular vibrations without changing the excitation wavelengths. In Chapter 5, I demonstrate both high spectral and spatial resolution multiplex CARS imaging of polymer films using a simple scheme for chirped CARS with a spectral bandwidth of 300 cm-1.

In Chapter 6, the nonlinear optical properties of KNbO3 nanowires are studied. Using SHG and sum frequency generation, efficient nonlinear optical frequency conversion is demonstrated in single KNbO3 nanowires that act as optical waveguides, yielding a coherent tunable subwavelength light source.