The group III nitride semiconductor grown on c-plane sapphire by radio frequency plasma assisted molecular beam epitaxy has been studied. To archive good quality GaN film, nitridation and low temperature buffer layer were applied to overcome the issue of lattice mismatch. Low temperature and long period nitridation process shows better improved of optical properties and crystal quality of GaN film. Buffer layer grown with slightly Ga-rich, substrate temperature at 522¢J, for 2 minutes leads to better GaN film. High substrate temperature and sufficient nitrogen to gallium ratio are two important factors to control the growth of the good quality GaN epilayer. Chemical etching and observation of surface reconstructions were used to characterize the polarity of group III nitrides. The Ga-polarity GaN film shows 2x surface reconstruction with high chemical resistance while the N-polarity is sensitive to chemical and displays the 3x reconstruction pattern. The process of indium incorporated with GaN is very sensitive to growth temperature. The indium content decreased with increasing the substrate temperature and also decreased along the growth direction. The N-polar GaN with an indium-facilitated growth technique was also studied. Upon the incorporation of indium during growth, the photoluminescence intensity and electron mobility of GaN has been enhanced by a factor of 15 and 6 respectively. The electron concentration drastically increases by several orders of magnitude. The biaxial strain of GaN film estimated with Micro-Raman technique reduces from 0.6729 to 0.5044GPa. The full-widths at half maximum of asymmetric (10-12) x-ray reflection which related to the density of overall threading dislocations increases from 593 to744 arcsec. In contrast, the symmetric (0002) reflection related only to threading dislocations having a non-zero c-component Burgers vectors reduces from 528 to 276 arcsec. The enhancement of GaN optical property is generally attributed to the reduction of non-zero c-component dislocations. The reduction in density is confirmed by cross-sectional transmission electron microscopy.

In this thesis, we study a series of Si doped InN films. These samples are grown on sapphire (0001) by molecular beam epitaxy (MBE). We have doped Si in InN films successfully. In this experiment, we control Si cell temperature to change carrier concentration of samples during InN film growth. The carrier concentration and mobility are explored by van der Pauw Hall measurement. As carrier concentration increases, mobility decreases. Carrier concentration changes with Si cell temperature from 6.16x1018 cm-3 to 1.19x1020 cm-3. Photoluminescence (PL) emission peak energy shows blue shift when carrier concentration increases, but the intensity decreases and full width at half maximum (FWHM) broadens. The PL peak of InN film with 1.19x1020 cm-3 split into two peaks 0.74 eV and 0.89 eV. In Raman spectra, Raman modes position and FWHM do not change with carrier concentration. In temperature dependence PL, the dependence of PL spectra shows decrease when carrier concentration increases. In power dependence PL, the PL emission peak energy of InN films with 6.16x1018 cm-3 and 8.50x1018 cm-3 show blue shift, while the PL peaks of InN films with 1.43x1019 cm-3 and 2.27x1019 cm-3 show no significant move. The fitting of power density vs. intensity is linear for all samples, but all slope of them are less than 1 expect for InN film with 1.43x1019 cm-3.

III-nitrides are a promising material system with unique material properties, which allows them to be utilized in a variety of semiconductor devices. III-nitrides grown by NH3-MOMBE are typically grown with high carbon levels (> 1021 cm-3) as a result of the incomplete surface pyrolysis of the metal-organic sources. Recent research has involved the compensating nature of carbon in III-nitrides to produce semi-insulating films, which can provide low-leakage buffer layers in transistor devices. The aim of this work is to investigate the possibility of forming a 2DEG, which utilizes the highly carbon-doped GaN layers grown by NH3-MOMBE to produce low-leakage buffer layers in the fabrication of HEMTs. These low leakage GaN buffers would provide increased HEMT performance, with better pinch-off, higher breakdown voltages and increased power densities. Additionally, methods of controlling and/or reducing the incorporation of carbon will be undertaken in an attempt to broaden the range of possible device applications for NH3-MOMBE. To realize these transistor devices, optimization and improved understanding of the growth conditions for both GaN and AlGaN will be explored with the ultimate goal of determining the feasibility of III-nitride transistors grown by NH3-MOMBE.

 Molecular Beam Epitaxy is an advanced method for the synthesis of single-crystal thin-film structures. However, the growth behavior varies case by case due to the complicated kinetic process. In this thesis, the epitaxial growth processes of AlxIn1-xN alloy and Bi2Se3 thin-films are studied. Heteroepitaxial growth of AlxIn1-xN alloy on GaN(0001) substrate is carried out in the Nitrogen-rich flux conditions. A series of transient growth stages are identified from the initiation of the deposition. A significant effect of source beam-flux on the incorporation rate of Indium atoms is observed and measured. A correlation between the incorporation rate and the growth conditions (flux ratio and growth temperature) is revealed by the dependence of the growth-rate of the film on beam fluxes. A mathematic model is then suggested to explain the effect, through which the measured results indicating a surface diffusing and trapping process is indicated. Unexpected behavior of the lattice-parameter evolution of the growth front during deposition is also observed, indicating a complex strain-relaxation process of the epilayers. For three-dimensional (3D) topological insulator of Bi2Se3, growths are attempted on various substrate surfaces, including clean Si(111)-(7x7), Hydrogen terminated Si(111), Bismuth induced Si(111) reconstructed surfaces, GaN(0001), and some selenide “psudo-substrates”. The specific formation process of this quintuple-layered material in MBE is investigated, from which the Van der Waals epitaxy growth characteristics inherent to deposition of Bi2Se3 is determined, and the mechanism of the “two-step growth” technique for this material is further clarified. Among the various substrates, those that are inert to chemical reaction with Bi/Se are important for the growth. The epilayers’ lattice-misfit with the substrate is also a crucial factor to the structural quality of the Bi2Se3 epifilms, such as the defects density and the single-crystalline domain size. The effect of a vicinal substrate on suppressing the twin-defects in film is also addressed. Using a suitable substrate and adapting an optimal condition, ultra-thin films of Bi2Se3 with a superior structural quality have been achieved. Multilayered Bi2Se3 structures with ZnSe and In2Se3 spacers are attempted. Finally the high-quality superlattices of Bi2Se3/In2Se3 are successfully synthesized. The hetero-interfaces in the superlattice structure of Bi2Se3/In2Se3 are sharp, and the individual layers are uniform with thicknesses being strictly controlled. The behaviors of strain evolution during the hetero-growth process are finally investigated. An exponential relaxation of misfit strain is observed. And the correlation between the residual strain and the starting surface in the initial growth stage is also identified. / published_or_final_version / Physics / Doctoral / Doctor of Philosophy

This thesis is about the growth of ZnO thin films for optoelectronic applications. ZnO thin films were grown using plasma assisted molecular beam epitaxy and were studied using various conventional and novel characterisation techniques. The significance of different growth variables on growth efficiency was investigated. The growth rate of ZnO films was found to be linearly dependent on the Zn flux under O-rich growth conditions. Under Zn-rich conditions, the growth rate was dependent on both atomic and molecular oxygen flux. By characterising the oxygen plasma generated using different RF power and aperture plate designs and correlating the results with the growth rates observed, it was found that atomic oxygen was the dominant growth species under all conditions. Molecular oxygen also participated in the growth process, with its importance dependent on the aperture plate design. In addition, an increase in growth temperature was found to monotonically decrease the growth rate. A growth rate of 1.4 Å/s was achieved at a growth temperature of 650 ℃ by using an oxygen flow rate of 1.6 standard cubic centimetres utilising a plasma source with a 276 hole plate operating at 400 W, and a Zn flux 1.4✕10¹⁵ atoms/cm²⋅s. Characterisation of the MBE grown thin films revealed that the qualities of ZnO thin films were dependent on the growth conditions. Experimental evidence suggested that a maximum adatom diffusion rate can be achieved under Zn-rich conditions, giving samples with the best structural quality. O-rich conditions in general led to statistical roughening which resulted in rough and irregular film surfaces. Experimental results also suggested that by increasing the atomic oxygen content and decreasing the ion content of the plasma, the excitonic emission of the ZnO thin films can possibly be improved. It was also found that the conductivity of the films can possibly be reduced by increasing the plasma ion content. By investigating the evolution of the buffer layer surface during the early stages of growth, dislocation nucleation and surface roughening were found to be important strain relief mechanisms in MBE grown ZnO thin films that affected the crystal quality. The usage of LT-buffer layers was found to improve substrate wetting, and was shown to significantly reduce dislocation propagation. Further strain reduction was achieved via the application of a 1 nm MgO buffer layer, and a significant reduction of carrier concentration and improvement in optical quality was subsequently observed. A carrier concentration of <1✕10¹⁶ cm⁻³ and a near band emission full width half maximum of 2 meV was observed for the best sample. The study of electrical characteristics using the variable magnetic field Hall effect confirmed the existence of a degenerate carrier and a bulk carrier in most MBE grown ZnO thin films. The bulk carrier mobility was measured to be ~120 - 150 cm²/Vs for most as-grown samples, comparable to the best reported value. A typical bulk carrier concentration of ~1✕10¹⁶ - 1✕10¹⁸ cm⁻³ was observed for as-grown samples. Annealing was found to increase the mobility of the bulk carrier to ~120 - 225 cm²/Vs and decrease the bulk carrier concentration by two orders of magnitude. Using time resolved photoluminescence, it was found that the radiative recombination in MBE grown ZnO thin films was dominated by excitonic processes, and followed a T³⁄² trend with temperature. A maximum radiative lifetime of 10 ns was observed for as-grown samples. The non-radiative lifetime in ZnO thin films was dominated by the Shockley-Read-Hall recombination processes. The modelling of the temperature dependence of the non-radiative lifetime suggested that an electron trap at ~0.065 eV and a hole trap at ~0.1 eV may be present in these samples. The application of time resolved photoluminescence also allowed the direct observation of carrier freeze-out in these ZnO films at low temperature.

No description available.

While modern epitaxial methods enable precise, monolayer (ML) control of the thin film deposition process, the complexity of certain device structures is ultimately limited by the capability and cost of the fabrication process. The objective of this work is to develop a pathway toward three-dimensional epitaxy (3DE) - the ability to intentionally and dynamically pattern regions of a film during the deposition process - in order to enable novel device concepts unbound by the traditional device fabrication paradigm. This work pioneers UV-assisted metal organic molecular beam epitaxy (MOMBE) as a particularly selective epitaxy technique to create a pathway toward 3DE of a crucial and topical material system - the III-Nitrides. A novel UV-assisted MOMBE system is developed enabling intense UV irradiation of films during growth. High quality, heavily (unintentionally) carbon-doped GaN is successfully grown by NH₃-based MOMBE and for the first time InGaN, AlGaN, and magnesium-doped GaN are demonstrated by NH₃-based MOMBE. Intense UV irradiation of films during NH₃-based MOMBE significantly enhances photo-desorption of species during the growth process, subsequently affecting the resultant InGaN alloy composition, carbon dopant concentration, or magnesium dopant concentration. A digital micromirror device is introduced to pattern incident UV radiation during InGaN growth, demonstrating that the effects of photoexcitation during MOMBE which have been proposed, discovered, and identified by this thesis indeed can be leveraged to deposit an InGaN film that is compositionally patterned within the growth plane. The results demonstrate that the new approach presented herein is possible for the 3DE of III-Nitrides if additional challenges in practical implementation can be overcome.

Thesis (Ph. D.)--West Virginia University, 2007. / Title from document title page. Document formatted into pages; contains xv, 145 p. : ill. (some col.). Includes abstract. Includes bibliographical references (p. 138-145).

Thesis (Ph.D.) -- McMaster University, 1997. / Includes bibliographical references. Also available via World Wide Web.

Thesis (Ph.D.) -- McMaster University, 1997. / Includes bibliographical references (leaves [100]-105. Also available via World Wide Web.