This thesis presents the characterization and calibration of the MOPITT-A instrument which uses the technique of correlation spectroscopy to ensure carbon monoxide in the atmosphere. A theoretical model is developed for the instrument and compared to MOPITT-A measurements collected under controlled laboratory conditions, which were designed to emulate atmospheric signals. It is shown that the model and measurements are in very good agreement with each other and that the MOPITT-A instrument behaves as expected. It was found that the gain of the instrument varies with time. The cause of the gain variation is not known but it is suggested that frosting inside the detector nest would be consistent with the observed nature of the variation.

Retrievals of atmospheric information from satellite observations permit the investigation of otherwise inaccessible atmospheric phenomena. The recovery of this information from optical instrumentation located in orbit requires both an inversion algorithm like the Saskatchewan Multiplicative Algebraic Reconstruction Technique and a forward model like the SASKTRAN radiative transfer model. These are used together at the University of Saskatchewan to retrieve sulphate aerosol extinction profiles from the radiance measurements made by the Canadian built OSIRIS instrument. Although these retrievals are highly successful the process currently does not consider the polarization of light or OSIRIS's polarization sensitivities because SASKTRAN is a scalar model. In this work the development of a vector version of SASKTRAN that can perform polarized radiative transfer calculations is presented.<p> The vector SASKTRAN's results compare favorably with vector SCIATRAN, another polarized model that is in development at the University of Bremen. Comparisons of the stratospheric aerosol retrieval vectors generated from the scalar and vector SASKTRAN results indicate that the polarized calculations are an important factor in future work to improve the aerosol retrievals and to recover particle size or composition information.

Thin films are used in many energy conversion applications, ranging from photodetectors to solar cells. Accurately predicting the radiative properties of thin films when they possess rough surfaces is critical in many instances, but can be challenging due to the complexity arising from light scattering and interferences at the microscale. This work describes measurements of the spectral transmittance and reflectance of several thin-film materials (including crystalline silicon wafers and a polycrystalline diamond film) in the mid-infrared spectral region (2 20 m) using a Fourier-transform infrared (FT-IR) spectrometer. The transmittance and reflectance were calculated using thin-film optics for the double-side polished samples and scalar scattering theory for the single-side polished samples. The effects of partial coherence are considered using a fringe smoothing technique. The interval used for fringe smoothing was assumed to be linearly dependent on the wavenumber. Good agreement between the predicted and measured transmittance was achieved for the double-side polished silicon wafers and for the diamond film. The disagreement for some single-side polished silicon wafers may be inherently related to their surface microstructures, as suggested from surface topographic data and images obtained from surface profilometry and microscopy. By comparing the intervals used for fringe smoothing with the instrumental resolution, beam divergence in the spectrometer was found to be a major factor contributing to the partial coherence. Future research is proposed to investigate the correlation between the detailed surface characteristics and the conical-conical transmittance and reflectance.

Currently, the effect of the vertical resolution on the brightness temperature (BT) has not been examined in depth. The uncertainty of the freezing level (FL) retrieved using two different satellites' data is large. Various radiative transfer (RT) codes yield different BTs in strong scattering conditions. The purposes of this research were: 1) to understand the uncertainty of the BT contributed by the vertical resolution numerically and analytically; 2) to reduce the uncertainty of the FL retrieval using new thermodynamic observations; and 3) to investigate the characteristics of four different RT codes. Firstly, a plane-parallel RT Model (RTM) of n layers in light rainfall was used for the analytical and computational derivation of the vertical resolution effect on the BT. Secondly, a new temperature profile based on observations was absorbed in the Texas A&M University (TAMU) algorithm. The Precipitation Radar (PR) and Tropical Rainfall Measuring Mission (TRMM) Microwave Imager (TMI) data were utilized for the improved FL retrieval. Thirdly, the TAMU, Eddington approximation (EDD), Discrete Ordinate, and backward Monte Carlo codes were compared under various view angles, rain rates, FLs, frequencies, and surface properties. The uncertainty of the BT decreased as the number of layers increased. The uncertainty was due to the optical thickness rather than due to relative humidity, pressure distribution, water vapor, and temperature profile. The mean TMI FL showed a good agreement with mean bright band height. A new temperature profile reduced the uncertainty of the TMI FL by about 10%. The differences of the BTs among the four different RT codes were within 1 K at the current sensor view angle over the entire dynamic rain rate range of 10-37 GHz. The differences between the TAMU and EDD solutions were less than 0.5 K for the specular surface. In conclusion, this research suggested the vertical resolution should be considered as a parameter in the forward model. A new temperature profile improved the TMI FL in the tropics, but the uncertainty still exists with low FL. Generally, the four RT codes agreed with each other, except at nadir, near limb or in heavy rainfall. The TAMU and the EDD codes had better agreement than other RT codes.

The light scattering problem and its application in atmospheric science is studied in this thesis. In the first part of this thesis, light scattering theory of single irregular particles is investigated. We first introduce the basic concepts of the light scattering problem. T-matrix ansatz, as well as the null-field technique, are introduced in the following sections. Three geometries, including sphere, cylinder and hexagonal column, are defined subsequently. Corresponding light scattering properties (i.e., T-matrix and Mueller Matrix) of those models with arbitrary sizes are simulated via the T-matrix method. In order to improve the efficiency for the algorithms of single-light scattering, we present a user-friendly database software package of the single-scattering properties of individual dust-like aerosol particles. The second part of this thesis describes this database in detail. Its application to radiative transfer calculations in a spectral region from ultraviolet (UV) to far-infrared (far-IR) is introduced as well. To expand the degree of morphological freedom of the commonly used spheroidal and spherical models, triaxial ellipsoids were assumed to be the overall shape of dust-like aerosol particles. The software package allows for the derivation of the bulk optical properties for a given distribution of particle microphysical parameters (i.e., refractive index, size parameter and two aspect ratios). The array-oriented single-scattering property data sets are stored in the NetCDF format. The third part of this thesis examines the applicability of the tri-axial ellipsoidal dust model. In this part, the newly built database is equipped in the study. The precomputed optical properties of tri-axial models are imported to a polarized addingdoubling radiative transfer (RT) model. The radiative transfer property of a well-defined atmosphere layer is consequently simulated. Furthermore, several trial retrieval procedures are taken based on a combination of intensity and polarization in the results of RT simulation. The retrieval results show a high precision and indicate a further application in realistic studies.

Laser-Induced Breakdown spectroscopy (LIBS) and Laser-Induced Thermal Emission (LITE) emission based laser remote sensing were investigated with the application to the remote measurements of trace chemical species. In particular, UVvisible LIBS and Mid-IR LITE systems were developed and measurements of remote targets and chemical surfaces were studied. The propagation through the atmosphere of the multi-wavelength backscattered LIBS and LITE optical spectrum with atmospheric absorption effects on the returned lidar signal was investigated. An enhanced model of the atmospheric effects on emission-based laser-remote sensing was developed and found to be consistent and in agreement with our experimental results. LITE measurements were performed which involved heating a remote hard target and recording the vibrational band emission spectra produced. Sample heating was carried out using a 1.5W cw-CO2 10.6 μm wavelength laser, and a 9W cw-diode laser operating at 809nm. The emission spectra over the wavelength range of 8 to 14 μm was observed which can be potentially used to detect and identify chemical composition of the target. LITE spectra of DMMP and DIMP (chemical agent simulants), paints, and energetic materials on various substrates were measured for the first time. A LIBS study was carried out with a 1.064 μm Nd:YAG laser (10 ns pulses, 50mJ per pulse) and remote LIBS measurements were performed for aluminum, copper, steel and plastics over the spectral range of 200 – 1000nm. LIBS measurements as a function of range were studied, and compared to a modified lidar equation suitable for emission based lidar remote sensing. A computer simulation model was developed for emission-based LIDAR remote sensing such as LIBS and LITE. This involved the development and modification of atmospheric transmission modeling programs which use the HITRAN, PNNL and other atmospheric spectral databases to model the transmission of the atmosphere over a wide range of wavelengths from the deep-UV near 200 nm to the mid-IR near 14 microns. A comparison of HITRAN simulations with the PNNL database calculated spectra was carried out and used for the first time for improvements of the HITRAN database line intensities. In addition, a Principal Component Analysis (PCA) of the LIBS and LITE lidar return signal as a function of range was performed. This PCA analysis showed, for the first time, the degradation of the chemical selectivity (i.e. identification capability) of the emission lidar system as the range was increased and the effect of atmospheric absorption spectral lines on the propagated LIBS and LITE lidar multi-wavelength spectral signal.

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Waveguides are desirable components for energy transmission throughout the electromagnetic spectrum. This thesis experimentally examines a thick slot waveguide for THz guiding and field enhancement. The waveguide is machined from planar copper sheets using the novel technique of femtosecond laser micromachining. In-plane photoconductive THz coupling to a thick slot waveguide is demonstrated using Discontinuous Galerkin Time Domain (DGTD) simulation. The results reveal positive implications for broadband low-loss/dispersion transmission lines up to 1.5 THz. / Graduate / 0544 / 0607 / 0756 / levismith3@hotmail.com

This thesis explores the factors controlling the distribution of black carbon (BC) in the atmosphere/troposphere and its implications for climate forcing. BC is of great climate interest because of its warming potential. Estimates of BC climate forcing have large uncertainty, in part due to poor knowledge of the distribution of BC in the atmosphere. This dissertation first examines the factors controlling the sources of BC in the Arctic in winter and spring using a global chemical transport model (GEOS-Chem). Emission inventories of BC and wet scavenging of aerosols in the model are updated to reproduce observed atmospheric concentrations of BC as well as observed snow BC content in the Arctic in winter-spring. The simulation shows a dominant contribution of fuel (fossil fuel and biofuel) combustion to BC in Arctic spring. Arctic snow BC content is dominated by fuel combustion sources in winter, but has equal contributions from open fires and fuel combustion in spring. The estimated decrease in Arctic snow albedo due to BC deposition in spring is 0.6%, resulting in a regional surface radiative forcing of 1.2 W m-2. The dissertation then extends the evaluation of the BC simulation to the global scale using aircraft observations over source regions, continental outflow and remote regions and ground-based measurements. The observed low BC concentrations over the remote oceans imply more efficient BC removal than is currently implemented in models. The simulation that has total BC emissions of 6.5 Tg C a-1 and a mean tropospheric lifetime of 4.2 days for 2009 (vs. 6.8 &plusmn 1.8 days for the AeroCom models) captures the principal features of observed BC. The simulation estimates a global mean BC absorbing aerosol optical depth of 0.0017 and a top-of-atmosphere direct radiative forcing (DRF) of 0.19 W m-2, with a range of 0.17-0.31 W m-2 based on uncertainties in the BC atmospheric distribution. The DRF is lower than previous estimates, which could be biased high because of excessive BC concentrations over the oceans and in the free troposphere. / Engineering and Applied Sciences

Biofuel production from microalgal biomass offers a clean and sustainable liquid fuel alternative to fossil fuels. In addition, algae cultivation is advantageous over traditional biofuel feedstocks as (i) it does not compete with food production, (ii) it potentially has a much greater areal productivity, (iii) it does not require arable land, and (iv) it can use marginal sources of water not suitable for irrigation or drinking. However, current algae cultivation technologies suffer from (i) low solar energy conversion effiencies, (ii) large thermal fluctuations which negatively affect the productivity, and (iii) large evaporative losses which make the process highly water intensive. This thesis reports a numerical study that address these key issues of planktonic as well as benthic algal photobioreactor technologies. First, radiant energy transfer in planktonic algal photobioreactors containing cells with different levels of pigmentation was studied. Chlamydomonas reinhardtii and its truncated chlorophyll antenna transformant tla1 were used as model organisms. Based on these simulations guidelines are derived for scaling the size and microorganism concentration of photobioreactors cultivating cells with different levels of pigmentation to achieve maximum photosynthetic productivity. To achieve this, the local irradiance obtained from the solution of the radiative transport equation (RTE) was coupled with the specific photosynthetic rates of the microorganisms to predict both the local and total photosynthetic rates in a photobioreactor. For irradiances less than 50 W/m2, the use of genetically modified strains with reduced pigmentation was shown to have negligible effect on increasing photobioreactor productivity. However, at irradiances up to 1000 W/m2, improvements of up to 30% were possible with cells having 63% less pigment concentration. It was determined that the ability of tla1 to transmit light deeper into the photobioreactor was the primary mechanism by which a photobioreactor using the modified strain can achieve greater productivity. Furthermore, it was determined photobioreactors using each strain have dead zones in which the local photosynthetic rate is negligible due to nearly complete light attenuation. These dead zones occur at local optical thicknesses greater than 169 and 275 in photobioreactors using the wild strain and the genetically modified strain, respectively. In addition, a thermal model of an algae biofilm photobioreactor was developed to assess the thermal fluctuations and evaporative loss rate of these novel photobioreactors under varying outdoor conditions. The model took into account air temperature, irradiance, relative humidity, and wind speed as inputs and computed the temperature and evaporative loss rate as a function of time and location in the photobioreactor. The model was run for a week-long period in each season using weather data from Memphis, TN. The range of the daily algae temperature variation was observed to be 13.2C, 12.4C, 12.8C, and 9.4C in the spring, summer, winter, and fall, respectively. Furthermore, without active cooling, the characteristic evaporative water loss from the system is approximately 6.3 L/m2-day, 7.0 L/m2-day, 4.9 L/m2-day, and 1.5 L/m2-day in the spring, summer, fall, and winter, respectively. / text