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This thesis explores the natural forces controlling variability of the tropospheric oxidants on interannual to glacial-interglacial time scales. The oxidants (primarily OH and ozone) determine the lifetime of many trace gases of human interest, including air pollutants and long-lived greenhouse gases such as methane. The oxidants respond to meteorological conditions, precursor emissions (natural and anthropogenic), and surface and overhead stratospheric boundary conditions, all of which have changed since the Last Glacial Maximum (LGM; ~21ka). This dissertation first examines in mechanistic detail the effect of variability in the lightning source of nitrogen oxides \((NO_x)\) precursors on interannual variability (IAV) of the oxidants in the recent past. An optimized technique is presented to constrain the lightning \(NO_x\) source in the GEOS-Chem global chemical transport model (CTM) to time-varying satellite data from the Lightning Imaging Sensor. This constraint improves the ability of the CTM to reproduce observed IAV in 9-year (1998-2006) hindcasts of tropical ozone and OH. IAV in ozone and OH is more sensitive to lightning than to biomass burning, despite greater IAV in \(NO_x\) from the latter source. The sensitivity of OH to lightning reflects positive chemical feedbacks on ozone production, \(HO_x\) recycling, and loss frequencies. This dissertation next introduces an offline-coupled climate-biosphere-chemistry framework for determining oxidant levels at and since the LGM. Detailed simulations of tropospheric composition are performed by GEOS-Chem driven by meteorological fields from the GISS ModelE general circulation model, land cover from the BIOME4-TG global terrestrial equilibrium vegetation model, and fire emissions from the LMfire model. Time slice simulations are presented for the present day, preindustrial, and two different possible representations of the LGM climate. Sensitivity of the results to uncertainty in lightning and biomass burning emissions is tested. Though well-buffered, all simulations find net reduced oxidative capacities relative to the present day. The most important parameters for controlling tropospheric oxidants over glacial-interglacial periods are changes in overhead ozone, tropospheric \(H_2O\), and lightning. The results are discussed in the context of the ice-core record, particularly for methane. / Engineering and Applied Sciences

This thesis considers atmospheric superrotation, a state of westerly equatorial winds which must be maintained by up-gradient eddy momentum fluxes. Superrotation has appeared in simulations of warm climates that generate enhanced Madden-Julian Oscillation (MJO)-like variability. This led to hypotheses that the warmer atmospheres of the early Pliocene and Eocene may have been superrotating, and that the phenomenon may be relevant to future climate projections. / Earth and Planetary Sciences

At present, the East Asian Monsoon (EAM) influences water availability for nearly one third of the global population. The intensity and position of the EAM has varied considerably since its onset, but disagreement still exists related to the precise latitudinal and intensity shifts of the Westerly Jet and associated storm fronts, which mark the northern extent of the monsoon. Paleoclimate research can assist in improved assessment and prediction of EAM intensity, radiative forcing, and biogeochemical cycles in the Japan Sea and North Pacific, especially under the currently changing climate. My research primarily focuses on using major-, trace- and rare earth elements in sediments from International Ocean Drilling Program Expedition 346 in the Japan (Ulleung Basin) and East China Seas (Okinawa Trough) to track variability in the EAM on millennial time scales. Using geochemical and multivariate statistical techniques (Q-Mode Factor analysis and Constrained Least Squares multiple linear regressions), I differentiated compositionally similar terrigenous aluminosilicate materials (continental crust components, eolian dusts, volcanic ash) from these sediment archives. I successfully constructed a robust record of aluminosilicate provenance, which enables more precise determinations of EAM position and intensity than previously possible. Most of my research focused on the interpretation of aluminosilicate records over several different timescales from three sites from Expedition 346. In tandem with this research, I also refined values of the well-known, and widely used, Standard Reference Material (SRM) Hawaiian Volcano Observatory Basalt (BHVO-2). In the Okinawa trough (Sites U1428/U1429), I identified and tracked the increase in flux of five continental crust materials, loesses, and volcanic ashes during glacial cycles, continental shelf exposure, and the migration of paleo-rivers in the last 400 kyr. Additionally, I constructed a 12 Myr record, which identified and quantified the dust fluxes to Ulleung Basin (Site U1430), and emphasized the importance of the Taklimakan and Gobi Deserts as main sources of dust to the Japan Sea and Pacific through the Cenozoic. Collectively, these aluminosilicate flux reconstructions are first to identify multiple specific Asian source regions through the Cenozoic, and highlight the complexity of accurately reconstructing monsoons and other aspects of paleoclimate from sediment in dynamic environments.

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