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Tin disulfide (SnS2) is a two-dimensional (2D) material with excellent properties and high prospects for low-cost solutions to catalytic and optoelectronic applications. In this work, vertical nanoflakes of SnS2 have been synthesized using custom-designed close space sublimation (CSS) system and investigated for applications in photoelectrochemical (PEC) water oxidation and metal-semiconductor-metal (MSM) photodetector. For the PEC application, vertical SnS2 nanoflakes grown directly on transparent conductive substrates have been used as photoanodes, which produce record photocurrents of 4.5 mA cm−2 for oxidation of a sulfite hole scavenger and 2.6 mA cm−2 for water oxidation without any hole scavenger, both at 1.23 VRHE in neutral electrolyte under simulated AM1.5G sunlight, and stable photocurrents for iodide oxidation in acidic electrolyte. This remarkable performance has been attributed to three main reasons: (1) high intrinsic carrier mobility of 330 cm2 V−1 s−1 and long photoexcited carrier lifetime of 1.3 ns in the nanoflakes, (2) the nanoflake height that balances the competing requirements of light absorption and charge transport, and (3) the unique stepped morphology of these nanoflakes that improves photocurrent by exposing multiple edge sites in every nanoflake. In another application, these SnS2 nanoflakes have been used to enhance the performance of lead sulfide quantum dot (PbS QDs) photodetectors by providing a high-mobility channel for photoexcited charges from PbS QDs, which results in 2 orders of magnitude enhancement in responsivity. The physical models and experimental findings presented in this dissertation can help engineer more cost-effective solutions for PEC water splitting and optoelectronics based on 2D metal dichalcogenides.

In this work cadmium telluride thin film photovoltaic devices have successfully been produced using a novel closed-field magnetron sputtering technique. This technique offers the possibility of producing cells in an all-in-one vacuum process with the potential to provide a new lower cost production route. The sputtered cadmium telluride layers were characterised in detail using a range of advanced microscopy based techniques both in the as deposited and after the cadmium chloride treated state, a treatment that is necessary to produce a working cell. In the as deposited condition the cadmium telluride layer was seen to have a fine-grained columnar structure containing a high density of stacking faults. After the cadmium chloride treatment these grains recrystallized and the new grains were equiaxed with a much lower density of intragranular defects. Similar effects were also observed in samples prepared using close space sublimation. To understand this recrystallization behaviour during the cadmium chloride treatment, the key treatment parameters were systematically varied. Chemical analysis in Scanning Transmission Electron Microscopy (STEM) showed that chlorine travelled down the cadmium telluride grain boundaries and accumulated adjacent to the cadmium telluride/cadmium sulphide interface. This interface is where the cadmium telluride grains were found to recrystallise first during interrupted cadmium chloride treatments. The nature of the stacking faults was examined using High Resolution Transmission Electron Microscopy (HR-TEM). This showed that in localised regions up to one plane of atoms per sequence was missing based on the expected zinc blende structure. This changed the packing of the atoms such that a local change in crystal structure occurred. This local change in phase was successfully mapped using Electron Backscatter Diffraction in planar section produced using Focused Ion Beam milling. This was subsequently studied in more detail using Transmission Electron Backscatter Diffraction in the Scanning Electron Microscope, where the intra-granular arrangement of the phases was observed. HR-TEM was used to quantitatively measure the linear defects in the cadmium telluride layer after thermal annealing with and without the cadmium chloride present. This showed that annealing alone resulted in only a modest reduction in the density of linear defects and grain recrysallisation only occurred in the presence of cadmium chloride. Cadmium magnesium telluride (CMT) was successfully grown epitaxially onto the cadmium telluride as an electron reflector layer to improve cell performance. During deposition the cell experienced high temperatures and this caused the stacking faults to return in a cell that had been previously cadmium chloride treated. This resulted in a reduction in cell efficiency, providing another link between linear defects and a degradation in cell performance.

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