The arrival of the Cassini-Huygens mission to the Saturn system ushered in a new era in the study of Titan. Armed with a variety of instruments capable of remote sensing and in situ investigations of Titan's atmosphere and surface, Cassini and Huygens have provided a wealth of new information about Titan and have finally allowed humankind to see its surface. This work focuses on two discoveries made by the Cassini Plasma Spectrometer (CAPS): the detection of oxygen ions (O<super>+</super>) precipitating into Titan's atmosphere (Hartle et al., 2006) and the discovery of very large positive (Waite et al., 2007; Crary et al., 2009) and negative ions (Coates et al., 2007, 2009) present in Titan's thermosphere.Through the use of a photochemical model, I demonstrate that the observed densities of CO, CO₂ and H₂O can be explained by a combination of O and OH or H₂O input to the upper atmosphere. Given the detection of O<super>+</super> precipitation into Titan's upper atmosphere, it is no longer necessary to invoke outgassing from Titan's interior as a source for atmospheric CO or to assume that the observed CO is the remnant of a larger primordial abundance in Titan's atmosphere. Instead, it is most likely that the oxygen bearing species in Titan's atmosphere are the result of external input, most likely from Enceladus.I have also used very high resolution mass spectrometry to investigate the com- position of Titan aerosol analogues, or "tholins". Although there are an enormous number of molecules present in tholin samples, they exhibit numerous patterns, in- cluding very regular spectral spacing. These patterns may help constrain the com- position of the very large ions observed in the CAPS spectra, since the resolution of the instrument makes identification of the molecules impossible. Additionally, tholins produced with CO possess molecules of prebiotic interest, including all 5 nucleotide bases and the 2 smallest amino acids (glycine and alanine). This indicates that chemistry occurring in Titan's upper atmosphere may be capable of forming incredibly complex organic molecules, which may have implications for the origin of life on Earth and elsewhere in the universe.

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Microorganisms are critical to the functioning of terrestrial and aquatic ecosystems and may also play a role in the functioning of the atmosphere. However, little is known about the diversity and function of microorganisms in the atmosphere. To investigate the forces driving the assembly of bacterial microbial communities in the atmosphere, I measured temporal variation in bacterial diversity and composition over diurnal and inter-day time scales. Results suggest that bacterial communities in the atmosphere markedly vary over diurnal time scales and are likely structured by inputs from both local terrestrial and long-distance sources. To assess the potential functions of bacteria and fungi in the atmosphere, I characterized total and potentially active communities using both RNA- and DNA-based data. Results suggest there are metabolically active microorganisms in the atmosphere that may affect atmospheric functions including precipitation development and carbon cycling. This dissertation includes previously published and unpublished co-authored material.

Using methods from dynamical systems theory in observations, low-order and general circulation models (GCMs), this dissertation explores (a) the response of midlatitude jet and eddy energy to climate change and variability, and (b) variability in predictability of the first kind of the El Niño/Southern Oscillation (ENSO) phenomenon. First, an analysis framework inspired by the Lorenz-1984 model is developed to study the relationship of the probability structure of the North Atlantic jet stream and storm track (location and strength) with (a) hemispheric surface temperature gradients (equator-to-pole gradient and ocean-land contrast), and (b) ENSO. Both the equator-to-pole gradient and the ocean-land contrast are projected to decrease in response to greenhouse gas forcing. The shifts in the probability structure of jet and eddy energy in relation to decreasing surface temperature gradients are in the opposite direction than the shifts for El Niño forcing. However, in climate change projections, the El Niño-like tropical pacific warming dominates the response of the jet/eddy energy probability, resulting in a strengthening and equatorward shift of the subtropical jet. The response of the subpolar jet is separate (poleward shift and strengthening), indicating that the combined effect of the tropical and extratropical SST changes under strong greenhouse gas forcing may set up conditions for a separation of the jet stream in the North Atlantic. Then, ENSO predictability of the first kind is examined in observations and in pre-industrial model simulations, using local lyapunov exponents. Multidecadal variations in ENSO predictability are shown in a 2000-yr long simulation from the Geophysical Fluid Dynamics Laboratory (GFDL) CM2.1 model. The GCM is found to be less predictable than nature and than an intermediate model of the tropical Pacific (Zebiak-Cane model). Finally, it is shown that increased predictability is associated with a deeper thermocline in the west Pacific up to five years prior to the peak of the event, along with an earlier deepening of the thermocline in the east Pacific in the months preceding the peak. This dissertation therefore illustrates that the analysis of key features of tropical and extratropical climate in a physically meaningful "reduced space" can provide a focused interpretation of GCM projections for climate change and variability.

Atmospheric aerosols serve an important role in climate and air quality. However, there are still significant gaps in our scientific understanding of their impacts on climate. One of the greatest factors contributing to uncertainties in our estimations of these impacts can be attributed to the gap in the sources and formation pathways of secondary organic aerosols (SOAs). Carbonyl compounds, in particular, glyoxal and methylglyoxal, are two oxidation products of both anthropogenic and biogenic volatile organic compounds (VOCs) in the atmosphere. Field and modeling studies have indicated that these two compounds can serve as potentially important precursors to SOAs, and alter the physical and chemical properties of the aerosols. The mechanisms and atmospheric significance of these processes pose important questions which need to be addressed. Here, we report experiments targeted to study the following topics: 1) the chemical kinetics of methylglyoxal uptake to aqueous aerosols, and the subsequent formation of SOA material; 2) the oxidative aging of SOA material formed by methylglyoxal; 3) the impact of methylglyoxal on the cloud condensation nuclei (CCN) activity of the aerosol. These studies were conducted using either aerosols generated from bulk solutions of the organic and ammonium sulfate or by exposing the gas-phase organic to pure ammonium sulfate seed aerosols. A number of techniques were utilized including: a custom-built Aerosol Chemical Ionization Mass Spectrometer (Aerosol-CIMS), UV-Vis spectrophotometer, pendant drop tensiometry (PDT), continuous flow stream-wise thermal gradient CCN counter (CFSTGC), aerosol flow tube reactors, and an aerosol chamber. We found that the uptake of methylglyoxal to aerosols is a potentially significant source of light-absorbing SOA in the atmosphere. Additionally, the presence of methylglyoxal leads to surface tension depression with important implications for aerosol CCN activity. The aqueous-phase reaction products of glyoxal and methylglyoxal when NH4^+ is present include species featuring unsaturated C=C bonds such as aldol condensation products and imidazoles. Upon oxidation by O3 and OH, these particles show an increase in light absorption, accompanied by the formation of smaller, more volatile organic acids. Aerosol chamber studies conducted where pure ammonium sulfate particles were exposed to gas-phase methylglyoxal and/or acetaldehyde show significant enhancements in CCN activity, which can increase cloud droplet number concentrations by up to 20%. The results of this work will provide for a more accurate representation of gas-aerosol interactions and cloud formation in climate and atmospheric chemistry models.

With extraordinary recent growth of the solar photovoltaic industry, it is paramount to address the biggest barrier to its high-penetration across global electrical grids: the inherent variability of the solar resource. This resource variability arises from largely unpredictable meteorological phenomena and from the predictable rotation of the earth around the sun and about its own axis. To achieve very high photovoltaic penetration, the imbalance between the variable supply of sunlight and demand must be alleviated. The research detailed herein consists of the development of a computational model which seeks to optimize the combination of 3 supply-side solutions to solar variability that minimizes the aggregate cost of electricity generated therefrom: Storage (where excess solar generation is stored when it exceeds demand for utilization when it does not meet demand), interconnection (where solar generation is spread across a large geographic area and electrically interconnected to smooth overall regional output) and smart curtailment (where solar capacity is oversized and excess generation is curtailed at key times to minimize the need for storage.) This model leverages a database created in the context of this doctoral work of satellite-derived photovoltaic output spanning 10 years at a daily interval for 64,000 unique geographic points across the globe. Underpinning the model's design and results, the database was used to further the understanding of solar resource variability at timescales greater than 1-day. It is shown that--as at shorter timescales--cloud/weather-induced solar variability decreases with geographic extent and that the geographic extent at which variability is mitigated increases with timescale and is modulated by the prevailing speed of clouds/weather systems. Unpredictable solar variability up to the timescale of 30 days is shown to be mitigated across a geographic extent of only 1500km if that geographic extent is oriented in a north/south bearing. Using technical and economic data reflecting today's real costs for solar generation technology, storage and electric transmission in combination with this model, we determined the minimum cost combination of these solutions to transform the variable output from solar plants into 3 distinct output profiles: A constant output equivalent to a baseload power plant, a well-defined seasonally-variable output with no weather-induced variability and a variable output but one that is 100% predictable on a multi-day ahead basis. In order to do this, over 14,000 model runs were performed by varying the desired output profile, the amount of energy curtailment, the penetration of solar energy and the geographic region across the continental United States. Despite the cost of supplementary electric transmission, geographic interconnection has the potential to reduce the levelized cost of electricity when meeting any of the studied output profiles by over 65% compared to when only storage is used. Energy curtailment, despite the cost of underutilizing solar energy capacity, has the potential to reduce the total cost of electricity when meeting any of the studied output profiles by over 75% compared to when only storage is used. The three variability mitigation strategies are thankfully not mutually exclusive. When combined at their ideal levels, each of the regions studied saw a reduction in cost of electricity of over 80% compared to when only energy storage is used to meet a specified output profile. When including current costs for solar generation, transmission and energy storage, an optimum configuration can conservatively provide guaranteed baseload power generation with solar across the entire continental United States (equivalent to a nuclear power plant with no down time) for less than $0.19 per kilowatt-hour. If solar is preferentially clustered in the southwest instead of evenly spread throughout the United States, and we adopt future expected costs for solar generation of $1 per watt, optimal model results show that meeting a 100% predictable output target with solar will cost no more than $0.08 per kilowatt-hour.

Atmosphere-ocean and atmosphere-land interactions are important processes which determine the development of monsoon systems. In this study, a new atmosphere-ocean surface interaction scheme, referred to as AOSIS, is developed and verified with observed data. AOSIS, together with ALSIS (Atmosphere-Land Surface Interaction Scheme), is then coupled into CEMSYS4 (Computational Environmental Modelling System) to investigate the influences of atmosphere-ocean and atmosphere-land surface interactions on the Australian Monsoon, especially the monsoon onset, break and withdrawal. Numerical experiments are carried out and the simulations are compared with the NCEP (National Center for Environmental Prediction, America) data. AOSIS is constructed with three basic components, i.e., a two-layer ocean temperature model, a wind-wave model and a surface flux model. We divide the ocean into a mixed layer and a deep layer. However, the depth of the mixed layer is not constant but varies with time, depending on surface wind shear and buoyancy flux. In AOSIS, we adapted the approach of relating the stages of wave development by wave age and proposed a new expression for calculating the ocean surface roughness length, $z_{0m}$, with consideration of waves. We test AOSIS in a stand along mode against the Moana data and the NCEP data. The comparison with the Moana data shows that AOSIS has considerable skill in simulating SST (sea surface temperature) and energy fluxes, with the simulated values in good agreement with observed data. AOSIS is also successful in simulating the warm and cool effects considered in the COARE (Coupled Ocean-Atmosphere Response Experiment) scheme. Comparison with the NCEP data also confirms that AOSIS simulates SST well. AOSIS and ALSIS are then coupled into CEMSYS4. We apply the system to the simulation of SST and surface energy fluxes over the Australian region and compared the results with the NCEP data. It is found that the simulated SST and energy fluxes are in good agreement with the NCEP data. Further, we study the synoptic events of the Australian Monsoon onset, break and withdrawal and examine the impacts of atmosphere-ocean and atmosphere-land surface interactions on such synoptic events.

Measurements of the fluctuations of humidity, temperature and velocity were made in the marine boundary layer. The humidity fluctuations were measured with a Lyman-alpha humidiometer. Temperature fluctuations were measured with a dry thermocouple and a platinum resistance thermometer. Velocity fluctuations were measured with a three component sonic anemometer. These measurements were made from the Floating Instrument Platform (FLIP) operated by the Scripps Institution of Oceanography near San Diego in February, 1969 and during the Barbados Oceanographic and Meteorological Expedition (BOMEX) in May 1969. The data were processed by digital techniques and the various spectra, cospectra and quadspectra between the velocities, humidity and temperature were obtained. Integrals of the cospectra were produced which allowed estimates of the fluxes of latent and sensible heat to be made. The normalized spectra of humidity fluctuations in San Diego and BOMEX have similar shapes. The normalized cospectra between vertical velocity and humidity in San Diego and BOMEX have similar shapes. Universal forms for the normalized humidity spectrum and the normalized cospectrum between vertical velocity and humidity may exist. The normalized spectra of the temperature fluctuations in San Diego and BOMEX have different shapes. The differences in shapes may be related to stronger radiation effects during BOMEX than in San Diego. The normalized cospectra between vertical velocity and temperature in San Diego and BOMEX also have different shapes. It is probable that a universal form does not exist for the normalized temperature spectrum or for the normalized cospectrum between vertical velocity and temperature. Directly measured values of the latent and sensible heat fluxes were used to test the validity of the bulk aerodynamic method of predicting the latent and sensible heat fluxes from the mean wind speed and mean air-sea humidity or temperature differences. The limited results from San Diego indicate that the sensible heat flux may probably be predicted from the mean wind speed and the mean air-sea temperature difference in temperate regions. The bulk aerodynamic method was not useful for predicting the sensible heat flux in BOMEX. The observed values for the sensible heat flux were much larger than would be predicted. The latent heat flux could be predicted from the mean wind speed and the mean air-sea absolute humidity difference with a probable error of less than 20%. The validity of the formula developed by Bowen (1926) for predicting the Bowen ratio (sensible heat flux/latent heat flux) was tested with directly measured values of the Bowen ratio. It was found that in San Diego the Bowen ratio could be predicted with a probable error of 15%. The Bowen ratio predicted for BOMEX was too low by a factor of two or more. The ability to predict the Bowen ratio from the ratio of the temperature fluctuations to the humidity fluctuations in the 0.05-0.1 Hz range was investigated. The method predicted the Bowen ratio with a probable error of 15% in San Diego and 20% in BOMEX. / Graduation date: 1971

Graduation date: 1970

Mariner 9 and Viking spacecraft observations during the 1970's have provided evidence for planetary-scale wave-like disturbances in the Mars atmosphere. It has been suggested that possible sources of the wave activity are dynamical instabilities (e.g., barotropic and/or baroclinic instabilities). An other candidate source is forced, quasi-stationary planetary waves. In connection with Mars' enormous relief, both mechanical forcing and large-scale thermal contrasts due to spatially varying surface thermal-inertia and albedo patterns should provide a strong source for planetary-wave activity. In this thesis, we attempt to model aspects of the observed wave activity, focusing on forced planetary waves in the wintertime atmosphere of Mars. Our approach is to apply two dynamical models: a linear primitive equations model and a quasi-linear 'wave, mean-flow' model. Both models have spherical geometry and represent deviations from zonal symmetry in terms of Fourier modes. The former model permits a separation of responses to different elements that make up the total forcing mechanism, whereas the latter is used principally to investigate the role forced planetary waves may play in the Mars polar warming phenomenon. Basic states representing relatively 'non-dusty' and 'highly dusty' conditions near winter solstice allow wavenumber-1 and -2 disturbances to propagate meridionally and vertically into the winter jet. Higher wavenumbers are strongly vertically trapped. Stationary waves in the northern and southern extratropics differ strongly in amplitude, phase and horizontal wave pattern. The possibility for near-resonant, long-period modes in Mars' winter atmosphere is also examined. For several wave-amplitude measures and dissipation strengths, dusty low-frequency responses are an order of magnitude larger than non-dusty ones. Wave, mean-flow simulations using wavenumber-1 or -2 forcings indicate north polar warmings can occur for the dusty basic states. The sensitivity (magnitude, location, and time scale) of a simulated warming to the wave forcing and the dissipation strength is investigated. / Graduation date: 1993