Tin(II) sulfide (SnS) is an earth-abundant, inexpensive, and non-toxic absorber material for thin film solar cells. SnS films are deposited by atomic layer deposition (ALD) through the reaction of a tin precursor, bis(N,N'-diisopropylacetamidinato)tin(II), and hydrogen sulfide. The SnS films demonstrate excellent surface morphology, crystal structure, phase purity, stoichiometry, elemental purity, and optical and electrical properties. / Engineering and Applied Sciences

Explaining the work-hardening behavior of crystalline materials and the size dependent plasticity has been a long lasting problem. Plastic deformation mainly arises from the collective motion of dislocations. Although individual dislocation processes are well studied, the study of the overall effects of these processes was challenging before the emergence of computer modeling. Of the computer simulation techniques, discrete dislocation dynamics (DDD) is the most suitable method to model thin films at the micron scale and below. This method allows us to study the quantitative effects of certain mechanisms. / Engineering and Applied Sciences

Solid oxide fuel cells are electrochemical energy conversion devices utilizing solid electrolytes transporting O2- that typically operate in the 800 - 1000 °C temperature range due to the large activation barrier for ionic transport. Reducing electrolyte thickness or increasing ionic conductivity can enable lower temperature operation for both stationary and portable applications. This thesis is focused on the fabrication of free standing ultrathin (<100 nm) oxide membranes of prototypical O2- conducting electrolytes, namely Y2O3-doped ZrO2 and Gd2O3-doped CeO2. Fabrication of such membranes requires an understanding of thin plate mechanics coupled with controllable thin film deposition processes. Integration of free standing membranes into proof-of-concept fuel cell devices necessitates ideal electrode assemblies as well as creative processing schemes to experimentally test devices in a high temperature dual environment chamber. We present a simple elastic model to determine stable buckling configurations for free standing oxide membranes. This guides the experimental methodology for Y2O3-doped ZrO2 film processing, which enables tunable internal stress in the films. Using these criteria, we fabricate robust Y2O3-doped ZrO2 membranes on Si and composite polymeric substrates by semiconductor and micro-machining processes, respectively. Fuel cell devices integrating these membranes with metallic electrodes are demonstrated to operate in the 300 - 500 °C range, exhibiting record performance at such temperatures. A model combining physical transport of electronic carriers in an insulating film and electrochemical aspects of transport is developed to determine the limits of performance enhancement expected via electrolyte thickness reduction. Free standing oxide heterostructures, i.e. electrolyte membrane and oxide electrodes, are demonstrated. Lastly, using Y2O3-doped ZrO2 and Gd2O3-doped CeO2, novel electrolyte fabrication schemes are explored to develop oxide alloys and nanoscale compositionally graded membranes that are thermomechanically robust and provide added interfacial functionality. The work in this thesis advances experimental state-of-the-art with respect to solid oxide fuel cell operation temperature, provides fundamental boundaries expected for ultrathin electrolytes, develops the ability to integrate highly dissimilar material (such as oxide-polymer) heterostructures, and introduces nanoscale compositionally graded electrolyte membranes that can lead to monolithic materials having multiple functionalities. / Engineering and Applied Sciences

Nanocomposite thin films with gold nanoparticles embedded in a host metal oxide prepared by spray pyrolysis deposition have been investigated. A single-step process has been developed using a one-pot solution containing precursors for both gold nanoparticles and host metal oxides. The films obtained display combined features of colouration, electrical conductivity and solar control. In this study two precursors for gold nanoparticles were used: preformed gold colloids and HAuCl₄. Three metal oxide host materials, TiO₂, SnO₂ and ZnO, were investigated. These films were deposited at a substrate temperature of 200-600 &deg;C. Powder X-ray diffraction analysis reveals the presence of metallic gold. SEM inspection typically showed particulate gold of 5-20 nm in diameter, distributed at the surface or within the host matrix. Optical spectroscopy showed an intense absorption in the visible region due to the characteristic surface plasmon resonance (SPR) effects of gold nanoparticles. The wavelength of the SPR peaks varies depending on the refractive index of surrounding host material which is significantly influenced by the substrate deposition temperature. On the other hand, SnO₂ and ZnO, together with the introduction of dopants, were further investigated as suitable materials for transparent conducting oxides (TCO). SnO₂:F films were found to attain very low electrical resistivity, while ZnO films exhibit higher transparency in the visible. A double layered structure with a TCO layer of SnO₂:F on top of a layer embedded with gold nanoparticles has been employed to achieve the combined functionalities of conductivity and colouration. The electrical conductivity is significantly enhanced compared to a nanocomposite single layer film due to the introduction of the TCO top layer. In this thesis, spray pyrolysis deposition has demonstrated a simple and rapid approach to the production of a variety of thin films. It can be immediately integrated with current industrial coating equipment and scaled up for large-scale production process.

Amorphous oxide semiconductors are of potential interest in the display industry due to their high carrier mobility, transparency at visible wavelengths and excellent operational stability. In this dissertation, n-channel zinc-tin oxide thin-film transistors are fabricated based on a solution-based deposition approach, which allows low fabrication cost and high throughput. The effects of device configuration and process conditions on transistor performance are investigated, and circuit applications including inverters, amplifiers, and ring oscillators are demonstrated. Charge transport in the zinc-tin oxide field-effect transistors is also investigated. A transition from thermally-activated to band-like transport is observed with increasing carrier concentration in high mobility samples, which agrees well with the key predictions of the multiple trap and release model and also Mott’s mobility edge model. In addition, velocity distribution of charge carriers is studied with a time-resolved technique. This provides a more detailed picture of charge transport in field-effect transistors. P-channel organic semiconductor field-effect transistors are also investigated with a view to combine them with n-channel amorphous oxide transistors to create a hybrid organic-inorganic complementary technology. / text

Amorphous Oxide semiconductors have gained large interest in the display industry owing to their high carrier mobilities and low fabrication costs. In this thesis, n-channel solution based zinc-tin oxide (ZTO) thin-film transistors (TFTs) are studied from a circuit design perspective. The study includes an iterative process of circuit design, layout and test procedure of the fabricated devices in the lab. The device models used in circuit simulations are refined following the data fed back from each of these iterations which has enabled more accurate design of complex circuits using ZTO devices. The requirement and development of a physical compact model for performing accurate and predictive circuit simulations has been presented. The use of ZTO devices in low cost, transparent and flexible electronic applications has been investigated through the study of basic circuit blocks such as amplifiers, ring oscillators, inverters and a four stage Operational Amplifier. / text

Amorphous Oxide Semiconductors (AOS) are widely being explored in the field of flexible and transparent electronics. In this thesis, solution processed zinc-tin oxide (ZTO) n-channel TFT based circuits are studied. Inverters, single stage amplifiers and ring oscillators are designed, fabricated and tested. 7-stage ring oscillators with output frequencies up to 106kHz and 5-stage ring oscillators with frequencies up to 75kHz are reported. A stable three stage op-amp with a buffered output is designed for a gain of 39.9dB with a unity gain frequency of 27.7kHz. A 7-stage ring oscillator with output frequency close to 1MHz is simulated and designed. The op-amp and the ring oscillator are ready to be fabricated and tested. An RPI model for a-Si, adapted to fit the ZTO device characteristics, is used for simulation. Development of a new model based on the physics behind charge transport in ZTO devices is explored. An expression for gate bias dependent mobility in ZTO devices is derived. / text

A broadband coupling approach applied to a single mode, sol-gel, planar integrated optical waveguide (IOW) was used to create a multichannel attenuated total reflection (ATR) spectrometer. Initial attempts to create an achromatic coupling element for sol-gel waveguides, based upon previous work applied to vacuum deposited glass devices, did not lead to an easily achievable design. Instead a simplified, non-achromatic approach based upon impinging an incident light beam with a large numerical aperture onto an incoupling prism was used. This simplified broadband coupling approach was used to create a sol-gel IOW-ATR spectrometer that transmitted light down to at least 400 nm, and produced a measurable bandwidth of ~ 250 nm; both phenomena are marked improvements upon the capabilities of previously reported devices. An experimental demonstration of this device proved it capable of measuring the visible spectrum of a thin film of horse heart cytochrome c adsorbed to the sol-gel surface at a submonolayer coverage. The broadband spectral capabilities of this sol-gel device were also used to experimentally validate a new method for determining the angular orientation of molecules bound to an arbitrary waveguide surface. In addition to the sol-gel IOW work, the simplified broadband coupling approach was applied to a previously reported multilayered electroactive waveguide device, which was used to collect electrically modulated, broadband spectra for thin films of cytochrome c, as well as a dicarboxyferrocene moiety. Both of these IOW-ATR spectrometers represent improved tools for probing the near-surface chemical environments of molecular assemblies.

Evaluation of the wet etching properties of several different thin film oxidesgrown by physical vapour deposition was performed in this work. MgO, Al2O3,SiO2, TiO2, HfO2 ZrO2 and Y2O3 were coated on two types of substrates; Si andborosilicate glass and etching tests were performed in different etchingsolutions. MgF2 thin films have also been evaluated. Important aspects of the choice of the thin films was taken into account in orderto match to good optical properties such as refractive index (n), extinction coefficient (k) and optical thickness (TP) as well as good chemical properties in the wet etching process. A description is made of the physics of optical filters and how a combination of different oxides stacked onto each other can create interference filters. A description of the manufacturing process of the thin films where physical vapour deposition (PVD) was used is presented. Thermal shift of the optical spectra caused by porous coatings was investigated and analyses of the thin films by ellipsometry, surface profilometry and transmission spectrophotometry have been performed. The wet etching properties were evaluated by monitoring the transmission insituon transparent borosilicate glass substrates. A method of how to measure the wet etching rate for different thin films is described. A computer software was used to calculate the Pourbaix diagrams in order to understand the chemical behaviour of the etching solutions. The pH can have a significant impact on the etching behaviour. In case of TiO2, it can be dissolved in an alkaline solution of H2O2. The catalytically process behind this is evaluated. Etching rate for both Y2O3 andSiO2 were matched by adjusting the etchant concentration as a case example. The group IVB oxides are difficult to etch. The catalytic etching of TiO2 with peroxide is slow but detectable. Al2O3, Y2O3 and MgO are reasonably easy to etch but have too low refractive indices to be useful in multilayer optical filters. The In-situ etching instrument was found to be very useful for measuring etching rates. / Utvärdering av våtkemiska egenskaper för flera olika oxidtunnfilmer utfördes idetta arbete på tunnfilmer av MgO, Al2O3, SiO2, TiO2, HfO2 ZrO2 and Y2O3 vakuumdeponerade på både kiselwafers och borosilikatglas. Etstester gjordes med ett flertal etslösningar. Även MgF2-tunnfilmer utvärderades. Både optiska och kemiska egenskaper togs i beaktande vid utvärderingen av tunnfilmerna. De optiska lagar som gäller för tunnfilmer redovisas, bl a hur kombinationer av olika oxider kan skapa interferrensfilter. En beskrivning av tillverkningsprocessen varvid PVD användes presenteras. Termiskt skift av det optiska transmissionsspektrat orsakat av porositet undersöktes. Analyser av tunnfilmerna med ellipsometri, profilometri och transmissions spektroskopi utfördes. Våtetsningsegenskaperna utvärderades genom att mäta in-situ vid etsprocessen på transparenta borosilikatglassubstrat. Metoden för att mäta etshastigheten för olika oxider är beskriven. Datorberäkningar av pourbaixdiagram användes för att skapa en förståelse av de kemiska egenskaperna för etslösningarna. Etsegenskaperna påverkas till stordel av lösningens pH. TiO2 kan etsas i basisk lösning av peroxid. Denna process utvärderades, likaså utvärderades etshasigheten för Y2O3 och SiO2 för att erhålla matchande par avoxider som en fallstudie. Grupp IVB oxiderna är mycket svåra att etsa. Katalytisk etsning av TiO2 med peroxid är detekterbar men långsam. Al2O3, Y2O3 och MgO är förhållandevis enkla att etsa men har för låga brytningsindex för att var praktiskt använbara i optiska multilagerfilter. In-situ etsinstrumentet befanns vara ett utmärkt verktyg för att mäta etshastigheten för tunnfilmer.

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