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<p>Research in the area of improving the efficiency and manufacturability of alternative energy technologies has been of high interest due to the growing environmental concerns of energy resources. Group III-antimonide-based compound semiconductors have been sought after as excellent candidates for photovoltaic conversion of infrared radiation, outside the spectral range absorbed by the currently available crystalline Si solar cells. The major challenge is the GaSb/Si interface is highly lattice mismatched, and inherently heterovalent. This leads to a high density of structural defects, many of which have not been investigated fully. Both optical and electrical properties of such heteroepitaxy thin films are strongly dependent on the periodicity of the crystal lattice, and the presence of extended defects cause perturbations in the lattice periodicity. Therefore the nature of such extended defects must be understood, in order to better manipulate the growth process to minimize their presence. This thesis demonstrates that through the use of conventional transmission electron microscopy, further insight can be gained into understanding the origin, distribution, propagation, and interaction of various extended defects. From this, a couple of ways to systematically suppress some of the defects have also been implemented, and the mechanism by which they induce such a suppression is also discussed.</p> / Master of Applied Science (MASc)

<p>InP nanowires with short InAs segments were grown on InP (111)B substrates by Au assisted vapour-liquid-solid growth in a gas source molecular beam epitaxy system. Nanowire crystal structure and morphology were investigated by transmission electron microscopy as a function of temperature, growth rate, and V/III flux ratio. At 370C predominantly kinked nanowires with random morphology and low areal density were observed with a rough parasitic 2D film. At 440C, nanowire density was also reduced but the 2D film growth was smoother and nanowires grew straight without kinking. An optimum temperature of 400C maximized areal density with uniform nanowire morphology. At the optimum temperature of 400C, an increase in V/III flux ratio changed the nanowire morphology from rod-shaped to pencil like indicating increased radial growth. Growth rate did not affect the crystal structure of InP nanowires. For InAs nanowires, changing the growth rate from 1 to 0.5 μm/hr reduced the presence of stacking faults to as low as one per nanowire. Short InAs segments in InP nanowires were found to grow through two mechanisms for nanowires of length L and diameter D. The first mechanism described the supply of In to the growth front via purging of In from the Au droplet where L was proportional to D. The second mechanism involved direct deposition of adatoms on the nanowire sidewall and subsequent diffusion to the growth front where L was proportional to 1/D. For intermediate growth durations, a transition between these two mechanisms was observed. For InP and InAs nanowires, the growth mode was varied from axial to radial through the inclusion of Al to form a core shell structure. Al_xIn_1-xAs(P) shells were grown on InAs cores with Al alloy fractions between 0.53 and 0.2. These nanowires were examined by transmission electron microscopy and it was found, for all values of x in InAs-Al_xIn_1-xP structures, that relaxation had occurred through the introduction of dislocations. For InAs-Al_xIn_1-xAs structures, all values except x=0.2 had relaxed through dislocation formation. A critical thickness model was developed to determine the core-shell coherency limits which confirmed the experimental observation of strain relaxation. The effects of passivation on the electronic transport and the optical properties were examined as a function of structural core-shell passivation and chemical passivation. The mechanisms for the observed improvement in mobility for core-shell versus bare InAs nanowires was due to the reduction in ionized impurity scattering from surface states. Similarly an increase in photoluminescence intensity after ammonium sulfide passivation was explained by the reduction of donor type surface states.</p> / Doctor of Philosophy (PhD)

<p>Heteroepitaxial films of group III-antimonide-based semiconductor compounds on Si are amongst the most appealing candidates for solar applications because of the well-established Si platform and also for offering band-gap energies beyond the silicon road map. Nonetheless, high lattice mismatch between GaSb and Si as well as ambiguous nucleation of GaSb on Si are major drawbacks in manufacturing of heteroepitaxial GaSb/Si films because they can generate various defects in films. Atomic-level detection of these defects and delving into their origin, orientation, distribution, propagation, and interaction with each other will therefore provide an insight into inhibiting their formation or reducing their severity. State-of-the-art aberration-corrected transmission electron microscopes have marked a new era in the investigation of interfaces and defects. With sub-angstrom electron probes in scanning transmission electron microscopes, it is possible to pinpoint the individual atomic columns at interfaces and defects.</p> <p>In this thesis, GaSb epilayers grown with molecular beam epitaxy on Si substrates were studied through aberration-corrected scanning transmission electron microscopy. The strain-relief mechanism of the epitaxial GaSb through formation of interfacial misfit dislocations was investigated and the strain distribution in the vicinity of dislocation cores as well as epitaxial layer was analyzed. The specific atomic-number dependent contrast mechanism of the high-angle annular dark-field technique enabled the unprecedented direct observation of anti-phase boundaries, the extended defects of highest interest in polar-on-nonpolar growths. This observation unraveled the ambiguity of nucleation of GaSb at interface regardless of preferential deposition of atomic species during growth procedure. The growth of GaSb at the initial stage of deposition was further investigated to understand the role of an AlSb buffer layer and growth mechanism of GaSb precisely. This investigation showed that AlSb and GaSb epilayers occur by Volmer-Weber growth mode and AlSb islands provide energetically favorable nucleation sites for GaSb film. Furthermore, taking advantage of atomic-resolution detection capability of high-angle annular dark-field in scanning transmission electron microscopy a novel mechanism of strain relief through multiple twining resulting in a lattice-registered growth of GaSb on Si(211) was elucidated. This contribution demonstrates that aberration-corrected scanning transmission electron microscopy provides profound insight into the polar-on-nonpolar growth which can be exploited to suppress the formation of structural defects.</p> / Doctor of Philosophy (PhD)