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This thesis studies different Eu optical centers in MgS:Eu and CaS:Eu thin films produced by Chemically Controlled Pulse Laser Deposition (CCPLD) and evaluates their suitability for the development of spectral storage devices of the future. The produced thin films consist of one or more optically active layer(s), MgS:Eu, CaS:Eu or a similar material, and a corresponding ZnS capping layer that functions as a protecting barrier for the other layers and preserves their composition and integrity. Given that the synthesis of the materials used to produce the multilayer structures in this work proved a great challenge, careful attention was given to the optimization of all fabrication parameters. Mass Spectrometry was used during the deposition of the thin films and the data obtained resulted on improvements and optimization of the deposition process. Scanning electron microscopy studies of these thin films were conducted to study degradation upon long-term storage. Microscopy results show that the morphology of the produced thin films is correlated to the growth environment during deposition and deterioration of the deposited materials could be initiated by nano-gaps and cracks in the capping layer of the thin films. In addition to optical centers in MgS:Eu and CaS:Eu, new centers were created by changing the thin film growth environment inside a hi-vacuum chamber, modifying the composition of the ablation target material, or both. For example, introducing O2, or alternatively HCl, inside the CCPLD chamber while producing MgS:Eu thin films results in the formation of impurity associated centers across lattice sites throughout the deposited structures. In another method of impurity doping studied, Cl- and Na+ were introduced into the MgS:Eu and CaS:Eu lattices by mixing trace amounts of the impurity ions into these materials in polycrystalline form and making this mixture a deposition target by hi-pressure cold compression technique. The introduction of these impurity ions will alter the crystal field environment around the Eu ions thus creating new optical centers with a shift in energy of their characteristic Zero Phonon Line. After extensive characterization of the optical properties of the thin films produced, laser-induced fluorescence spectroscopy and absorption spectroscopy measurements confirm that they are suitable candidates to be used in conjunction with power-gated spectral holeburning technique and could potentially provide ultrahigh, terabits per square inch, storage densities. / Physics

Semiconductors such as CuInGaSe2 and CdTe have been investigated as absorber layer materials for thin film solar cells since their band gap matches with the solar spectrum. Films as thin as 2m are sufficient for the absorption of the visible part of solar radiation, because they are characterized by a high absorption coefficient. However, the scarcity and high costs of Indium, Gallium and Tellurium have led to concerns on the sustainability of these technologies. The semiconductor Cu2ZnSnS4 (Copper Zinc Tin Sulphide) consisting of abundantly available elements promises to be an excellent photovoltaic absorber material. The present study is focused on the growth and characterization of CZTS/ZnS thin film heterostructure suitable for PV applications. Ultrasonic Spray Pyrolysis (USP), a variation of Spray Pyrolysis is a thin film deposition technique where the solution to be sprayed is atomized by ultrasonic frequencies. The details of the USP experimental set up and the deposition principle are presented in the thesis. The active layers of the solar cell, viz. the CZTS absorber layer and ZnS emitter layer were grown by this technique. The metal top contact was deposited using e-beam evaporation. The effects of copper concentration and sodium diffusion on the Cu2ZnSnS4 film properties were investigated. The films have shown preferred orientation along (112) direction confirming kesterite structure. The optical studies revealed that a reduction of copper in the films will bring the band gap energy to 1.5eV, which will match with the solar spectrum. Sodium diffusion in the CZTS films is found to passivate the grain boundaries and enhance the electrical conductivity. These properties render CZTS films as good photovoltaic absorber layers. ZnS has a high band gap and is non toxic unlike CdS. The influences of variation in substrate temperature and spray duration on the ZnS film properties were examined. The optical studies conducted on ZnS films revealed that they are highly transparent in the visible region of the solar spectrum. The films were found to possess a band gap of 3.5 eV. These properties make them potential candidates as solar cell emitter layers. The CZTS/ZnS heterojunction solar cell was fabricated and subjected to electrical characterization in dark and illuminated conditions. A conversion efficiency of 1.16% was achieved for the device.

Currently conventional sources like coal, petroleum and natural gas meet the energy requirements of developing and undeveloped countries. Over a period of time there is high risk of these energy sources getting depleted. Hence an alternate source of energy i.e. renewable energy is the need of the hour. The advantages of renewable energy like higher sustainability, lesser maintenance, low cost of operation, and minimal impact on the environment make the role of renewable energy sources significant. Out of the various renewable energy sources like solar energy, wind energy, hydropower, biogas, tidal and geothermal, usage of solar energy is gradually increasing. Among various solar energy sources, Photovoltaics has dominated over the past two decades since it is free clean energy and availability of abundant sunlight on earth. Over the past few decades, thin film solar cells (TFSC) have gained considerable interest as an economically feasible alternative to conventional silicon (Si) photovoltaic devices. TFSCs have the potential to be as efficient as Si solar cells both in terms of conversion efficiency as well as cost. The advantages of TFSC are that they are easy to prepare, lesser thickness, requires lesser materials, light weight, low cost and opto-electronic properties can be tuned by varying the process parameters. The present study is focused on the fabrication of AgInS2/ZnS heterojunction thin film solar cell. AgInS2 absorber layer is deposited using both vacuum (sputtering/sulfurization) and non-vacuum (ultrasonic spray pyrolysis) techniques. ZnS window layer is prepared using thermal evaporation technique, detailed experimental investigation has been conducted and the results have been reported in this work. The thesis is divided into 6 chapters. Chapter 1 gives general introduction about solar cells and working principle of solar cell. It also discusses thin film solar cell technology and its advantages. Layers of thin film solar cell structure, Significance of each layers and possible materials to be used are emphasized. A detailed overview of the available literature on both AgInS2 absorber layer and ZnS window layer has been presented. Based on the literature review, objectives of the present work are defined. Chapter 2 explains the theory and experimental details of deposition techniques used for the growth of AgInS2 and ZnS films. Details of characterization techniques to study film properties are described in detail. Chapter 3 presents a systematic study of AgInS2 thin films deposited by sulfurization of sputtered Ag-In metallic precursors. Initially, AgInS2 films are deposited by varying the substrate temperature and properties of as-deposited films are characterized. Structural, morphological, electrical and optical properties of AgInS2 films are explained. From these studies, samples with better properties at particular substrate temperature are optimized. By fixing the substrate temperature, deposition time of silver is varied by keeping other deposition conditions same and the properties of films are discussed. It was observed that deposition time of silver doesn’t have much impact on structural properties of AgInS2 films. However, opto-electric properties of AgInS2 films are enhanced. Based on characterization studies, deposition time of silver is optimized. Deposition time of indium is varied by keeping substrate temperature and silver deposition to optimized value. The properties of as-deposited films are discussed. Based on the above studies, the optimized p type films have a band gap of 1.64 eV, carrier concentration of 1013 ions/cm3 and Resistivity of order 103 Ω-cm. Chapter 4 presents a systematic study of AgInS2 thin films deposited by ultrasonic spray pyrolysis. AgInS2 films are deposited by varying the substrate temperature and properties of as deposited films are characterized. Structural, morphological, electrical and optical properties of AgInS2 films are explained. From these studies, samples with better properties at particular substrate temperature are optimized. By fixing the substrate temperature, concentration of silver molarity in the precursor solution is varied by keeping other deposition conditions same and the properties of films are discussed. Structural, optical and electrical properties of AgInS2 films are enhanced with the increase in silver concentration. Based on characterization studies, concentration of silver is optimized. Similarly concentration of indium molarity in the precursor solution is varied and the properties of as-deposited films are discussed. Finally, sulfur molarity in the precursor solution is varied and properties of films are discussed. It was observed that increasing sulfur after certain limit does not have any effect on the properties of the films. Based on the above studies, this method resulted in the films with resistivity of 103 Ω-cm and band gap of 1.64 eV. These films showed a carrier concentration of 1013 ions/cm3. Chapter 5 describes the growth of ZnS films using thermal evaporation technique. Influence of thickness on the properties of ZnS films is explained. Samples with good crystallinity, high transmission, and wider gap are selected for device fabrication. This p type layer showed a band gap of 3.52 eV. Solar cells have been fabricated using the AgInS2 films developed by both sputtering and ultrasonic spray pyrolysis techniques. A maximum cell efficiency of 0.92 percent has been achieved for the cell with 0.950 µm thick sputtered AgInS2 layer and thermally evaporated 42 nm thick ZnS layer. In comparison, the ultrasonic spray pyrolysis deposited films gave an efficiency of 0.54 percent. These values are comparable to those mentioned in a couple of reports earlier. Chapter 6 summarizes the conclusions drawn from the present investigations and scope of future work is suggested.