Because the surface plays an important role in the electrical and optical properties of GaN devices, an improved understanding of surface effects should help optimize device performance. In this work, atomic force microscopy (AFM) and related techniques have been used to characterize three unique sets of n-type GaN samples. The sample sets comprised freestanding bulk GaN with Ga polar and N polar surfaces, epitaxial GaN films with laterally patterned Ga- and N-polar regions on a common surface, and truncated, hexagonal GaN microstructures containing Ga-polar mesas and semipolar facets. Morphology studies revealed that bulk Ga-polar surfaces treated with a chemical-mechanical polish (CMP) were the flattest of the entire set, with rms values of only 0.4 nm. Conducting AFM (CAFM) indicated unexpected insulating behavior for N-polar GaN bulk samples, but showed expected forward and reverse-bias conduction for periodically patterned GaN samples. Using scanning Kelvin probe microscopy, these same patterned samples demonstrated surface potential differences between the two polarities of up to 0.5 eV, where N-polar showed the expected higher surface potential. An HCl cleaning procedure used to remove the surface oxide decreased this difference between the two regions by 0.2 eV. It is possible to locally inject surface charge and measure the resulting change in surface potential using CAFM in conjunction with SKPM. After injecting electrons using a 10 V applied voltage between sample and tip, the patterned polarity samples reveal that the N-polar regions become significantly more negatively charged as compared to Ga-polar regions, with up to a 2 eV difference between charged and uncharged N polar regions. This result suggests that the N-polar regions have a thicker surface oxide that effectively stores charge. Removal of this oxide layer using HCl results in significantly decreased surface charging behavior. A phenomenological model was then developed to fit the discharging behavior of N-polar GaN with good agreement to experimental data. Surface photovoltage (SPV) measurements obtained using SKPM further support the presence of a thicker surface oxide for N polar GaN based on steady state and restoration SPV behaviors. Scanning probe microscopy techniques have therefore been used to effectively discriminate between the surface morphological and electrical behaviors of Ga- vs. N-polar GaN.

Group III-Nitrides (GaN, InN & AlN) are considered one of the most important class of semiconducting materials after Si and GaAs. The excellent optical and electrical properties of these nitrides result in numerous applications in lighting, lasers, and high-power/high-frequency devices. Due to the lack of cheap bulk III- Nitride substrates, GaN based devices have been developed on foreign substrates like Si, sapphire and SiC. These technologies have been predominantly developed on the so called Ga-polarity epitaxial stacks with growth in the [0001] direction of GaN. It is this orientation that grows most easily on sapphire by metal organic chemical vapor deposition (MOCVD), the most common combination of substrate and deposition method used thus far. The opposite [000¯1] or N-polar orientation, very different in properties due to the lack of an inversion centre, offers several ad- vantages that could be exploited for better electronic and optoelectronic devices. However, its growth is more challenging and needs better understanding. The aim of the work reported in this dissertation was a systematic investigation of the relation between the various growth parameters which control polarity, surface roughness and mosaicity of GaN on non-miscut sapphire (0001) wafers for power electronics and lighting applications, with emphasis on the realization of N-polar epitaxial layers. GaN is grown on sapphire (0001) in a two-step process, which involves the deposition of a thin low temperature GaN nucleation layer (NL) on surface modified sapphire followed by the growth of high temperature device quality GaN epitaxial layer. The processing technique used is MOCVD. Various processing methods for synthesis of GaN layers are described with particular em- phasis on MOCVD method. The effect of ex situ cleaning followed by an in situ cleaning on the surface morphology of sapphire (0001) wafers is discussed. The characterization tools used in this dissertation for studying the chemical bond nature of nitrided sapphire surface and microstructural evolution (morphological and structural) of GaN layers are described in detail. The effect of nitridation temperature (TN) on structural transformation of non- miscut sapphire (0001) surface has been explored. The structural evolution of nitrided layers at different stages of their process like as grown stage and thermal annealing stage is investigated systematically. The chemical bond environment information of the nitrided layers have been examined by x-ray photoelectron spectroscopy (XPS). It is found that high temperature nitridation (TN ≥ 800oC) results in an Al-N tetrahedral bond environment on sapphire surface. In contrast, low temperature nitridation (TN = 530oC) results in a complex Al-O-N environment on sapphire surfaces. Microstructural evolution of low temperature GaN NLs has been studied at every stage of processing by scanning electron microscopy (SEM) and atomic force microscopy (AFM). Surface roughness evolution and island size distribution of NLs measured from AFM are discussed. It is found that NLs processed on sapphire wafers nitrided at (TN ≥ 800oC) showed strong wurtzite [0002] orientation with sub-nanometre surface roughness. In contrast, NLs processed at (TN = 530oC) showed zinc blende phase in the as grown stage with higher surface roughness, but acquired a greater degree of wurtzite [0002] orientation after thermal annealing prior to high temperature GaN growth. Polarity, surface quality and crystal quality of subsequently grown high temperature GaN epitaxial layers is described in relation to the structure of the trans- formed nitrided layers. Higher nitridation temperatures (TN ≥ 800oC) consistently yield N-polar GaN whereas lower nitridation temperatures (TN = 530oC) yield Ga-polar GaN. It is found that the relative O atom concentration levels in nitrided layers control the density of inversion domains in N-polar GaN. The effect of various growth parameters (NH3 flow rate, growth temperature, NL thickness) on surface morphology and mosaicity of both Ga & N-polar GaN layers is discussed in detail. We report device quality N-polar GaN epitaxial layers on non-miscut sapphire (0001) wafers by careful optimization of growth temperature. It is found that lower growth temperatures (800oC) are favorable for obtaining smooth N- polar GaN layers. In contrast, N-polar GaN layers grown at higher temperatures (1000 to 1080oC) are rough with hexagonal hillocks.

La polarité est une question critique pour le système de matériaux III-nitrures, qui a un impact sur la qualité des films épitaxies et la performance des dispositifs à base de nitrure. Mais la compréhension des mécanismes élémentaires responsables de l'établissement de la polarité N ou métallique des films sur le substrat non-polaire manque. Les concepts existants sont basés sur des observations empiriques et contiennent des résultats ambigus. Une des raisons principales est le manque d'outils analytiques, permettant la détermination localisée de la polarité et de la structure atomique des couches à l'époque, lorsque les concepts de contrôle de la polarité ont été établis. Dans ce travail, nous développons un concept de contrôle de la polarité dans les couches AlN et GaN épitaxies sur substrat de saphir par EPVOM. La polarité des couches est étudiée par microscopie électronique en transmission (MET) haute résolution corrigée des aberrations et par microscope électronique à balayage en transmission en champ sombre (HAADF-STEM). L'analyse des investigations expérimentales donne les principaux résultats suivants : (i) le mécanisme qui régit la sélection de la polarité ; (ii) la relation entre la nitruration de la surface et les domaines de polarité Al dans les films d'AlN N-polaire ; (iii) possibilité d’inverser la polarité N de films d’AlN de polarité mixte en introduisant un recuit sous oxygène. La compréhension de mécanisme par lequel la polarité est contrôlée ouvre les possibilités d'une ingénierie de polarité dans les films de nitrure et peut donner une idée de la compréhension du contrôle de la polarité dans d'autres systèmes de matériaux (par exemple, les oxydes). / Polarity is a critical issue for III-nitrides material system that has an impact on the quality of epitaxial films and the performance of nitride-based devices. But the understanding of the elementary mechanisms that are responsible for establishing metal or nitrogen polarity of the films on nonpolar substrate is lacking. The existing concepts are based on empirical observations and contain ambiguous results. One of the main reasons for that is the lack of precise analytical tools, allowing localized determination of polarity and atomic structure of layers, at the time, when main concepts for polarity control were established. In this work we develop a concept of polarity control in AlN and GaN layers grown by MOVPE on sapphire substrates. The polarity of the layers is studied by aberration corrected HRTEM and high resolution high-angle annular dark field (HAADF) scanning TEM. The analysis of the experimental investigations yields the following principal results: (i) mechanism that governs polarity selection; (ii) relation between sapphire surface nitridation and Al-polar domains in N-polar AlN films; (iii) possibility of controlled switching the layers polarity from N to Al by oxygen annealing.Understanding of this mechanism by which polarity is controlled opens up the possibilities for polarity engineering in nitride films and can give a clue to understanding polarity control in other material systems (e.g. oxides).