III-nitride optoelectronic devices have become ubiquitous due to their ability to emit light efficiently in the blue and green spectral ranges. Specifically, III-nitride light emitting diodes (LEDs) have become widespread due to their high brightness and efficiency. However, III-nitride devices such as single photon sources are also the subject of research and are promising for various applications. In order to improve design efficient devices and improve current ones, the relationship between the structure of the constituent materials and their optical properties must be studied. The optical properties of materials are often examined by photoluminescence or cathodoluminescence, whilst traditional microscopy techniques such a transmission electron microscopy and scanning electron microscopy are used to elucidate their structure and composition. This thesis describes the use of a dual-beam focussed ion beam/scanning electron microscope (FIB/SEM) in bridging the gap between these two types of techniques and providing a platform on which to perform correlative studies between the optical and structural properties of III-nitride materials. The heteroepitaxial growth of III-nitrides has been known to produce high defect densities, which can harm device performance. We used this correlative approach to identify hexagonal defects as the source of inhomogeneous electroluminescence (EL) in LEDs. Hyperspectral EL mapping was used to show the local changes in the emission induced by the defects. Following this the FIB/SEM was used to prepare TEM samples from the apex of the defects, revealing the presence of p-doped material in the active region caused by the defect. APSYS simulations confirmed that the presence of p-doped material can enhance local EL. The deleterious effects of defects on the photoelectrochemical etching of cavities were also studied. We performed TEM analysis of an edge-defect contained in unetched material on the underside of a microdisk using FIB/SEM sample preparation methods. The roughness and morphology of microdisk and nanobeam cavities was studied using FIB-tomography (FIBT), demonstrating how the dual-beam instrument may be used to access the 3D morphology of cavities down to the resolution of the SEM and the slicing thickness of the FIB. This tomography approach was further extended with electron tomography studies of the nanobeam cavities, a technique which provided fewer issues in terms of image series alignment but also the presence of reconstruction artefacts which must be taken into account when quantitatively analysing the data. The use of correlative techniques was also used to establish the link between high Si content in an interlayer running along the length of microrods with changes in the optical emission of these rods. The combination of CL, FIB/SEM and TEM-based techniques has made it possible to gain a thorough understanding of the link between the structural and optical properties in a wide variety of III-nitride materials and devices.

The burgeoning field of nanotechnology motivates comprehensive elucidation of nanoscale materials. This thesis addresses transmission electron microscope characterisation of nanoparticle morphology, concerning specifically the crystal- lographic status of novel intermetallic GaPd2 nanocatalysts and advancement of electron tomographic methods for high-fidelity three-dimensional analysis. Going beyond preceding analyses, high-resolution annular dark-field imaging is used to verify successful nano-sizing of the intermetallic compound GaPd2. It also reveals catalytically significant and crystallographically intriguing deviations from the bulk crystal structure. So-called ‘non-crystallographic’ five-fold twinned nanoparticles are observed, adding a new perspective in the long standing debate over how such morphologies may be achieved. The morphological complexity of the GaPd2 nanocatalysts, and many cognate nanoparticle systems, demands fully three-dimensional analysis. It is illustrated how image processing techniques applied to electron tomography reconstructions can facilitate more facile and objective quantitative analysis (‘nano-metrology’). However, the fidelity of the analysis is limited ultimately by artefacts in the tomographic reconstruction. Compressed sensing, a new sampling theory, asserts that many signals can be recovered from far fewer measurements than traditional theories dictate are necessary. Compressed sensing is applied here to electron tomographic reconstruction, and is shown to yield far higher fidelity reconstructions than conventional algorithms. Reconstruction from extremely limited data, more robust quantitative analysis and novel three-dimensional imaging are demon- strated, including the first three-dimensional imaging of localised surface plasmon resonances. Many aspects of transmission electron microscopy characterisation may be enhanced using a compressed sensing approach.

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