InGaN heterostructures are at the core of blue light emitting diodes (LEDs) which are the basic building blocks for energy efficient and environment friendly modern white light generating sources. Through quantum confinement and electronic band structure tuning on the opposite end of the spectrum, Ge1−xSnx alloys have recently attracted significant interest due to its potential role as a silicon compatible infra-red (IR) optical material for photodetectors and LEDs owing to transition to direct bandgap with increasing Sn. This thesis is dedicated to establishing an understanding of the optical processes and carrier dynamics in InGaN heterostructures for achieving more efficient visible light emitters and terahertz generating nanocavities and in colloidal Ge1−xSnx quantum dots (QDs) for developing efficient silicon compatible optoelectronics. To alleviate the electron overflow, which through strong experimental evidence is revealed to be the dominating mechanism responsible for efficiency degradation at high injection in InGaN based blue LEDs, different strategies involving electron injectors and optimized active regions have been developed. Effectiveness of optimum electron injector (EI) layers in reducing electron overflow and increasing quantum efficiency of InGaN based LEDs was demonstrated by photoluminescence (PL) and electroluminescence spectroscopy along with numerical simulations. Increasing the two-layer EI thickness in double heterostructure LEDs substantially reduced the electron overflow and increased external quantum efficiency (EQE) by three fold. By incorporating δ p-doped InGaN barriers in multiple quantum well (MQW) LEDs, 20% enhancement in EQE was achieved due to improved hole injection without degrading the layer quality. Carrier diffusion length, an important physical parameter that directly affects the performance of optoelectronic devices, was measured in epitaxial GaN using PL spectroscopy. The obtained diffusion lengths at room temperature in p- and n-type GaN were 93±7 nm and 432±30 nm, respectively. Moreover, near field scanning optical microscopy was employed to investigate the spatial variations of extended defects and their effects on the optical quality of semipolar and InGaN heterostructures, which are promoted for higher efficiency light emitters owing to reduced internal polarization fields. The near-field PL from the c+ wings in heterostructures was found to be relatively strong and uniform across the sample but the emission from the c- wings was substantially weaker due to the presence of high density of threading dislocations and basal plane stacking faults. In case of heterostructures, striated regions had weaker PL intensities compared to other regions and the meeting fronts of different facets were characterized by higher Indium content due to the varying internal field. Apart from being the part and parcel of blue LEDs, InGaN heterostructures can be utilized in generation of coherent lattice vibrations at terahertz frequencies. In analogy to LASERs based on photon cavities where light intensity is amplified, acoustic nanocavity devices can be realized for sustaining terahertz phonon oscillations which could potentially be used in acoustic imaging at the nanoscale and ultrafast acousto-optic modulation. Using In0.03Ga0.97N/InxGa1-xN MQWs with varying x, coherent phonon oscillations at frequencies of 0.69-0.80 THz were generated, where changing the MQW period (11.5 nm -10 nm) provided frequency tuning. The magnitude of phonon oscillations was found to increase with indium content in quantum wells, as demonstrated by time resolved differential transmission spectroscopy. Design of an acoustic nanocavity structure was proposed based on the abovementioned experimental findings and also supported by full cavity simulations. Optical gap engineering and carrier dynamics in colloidal Ge1−xSnx QDs were investigated in order to explore their potential in optoelectronics. By changing the Sn content from 5% to 23% in 2 nm-QDs, band-gap tunability from 1.88 eV to 1.61 eV, respectively, was demonstrated at 15 K, consistent with theoretical calculations. At 15 K, time resolved PL spectroscopy revealed slow decay (3 − 27 μs) of luminescence, due to recombination of spin-forbidden dark excitons and effect of surface states. Increase in temperature to 295 K led to three orders of magnitude faster decay (9 − 28 ns) owing to the effects of thermal activation of bright excitons and carrier detrapping from surface states. These findings on the effect of Sn incorporation on optical properties and carrier relaxation and recombination processes are important for future design of efficient Ge1−xSnx QDs based optoelectronic devices. This thesis work represents a comprehensive optical study of InGaN heterostructures and colloidal Ge1−xSnx QDs which would pave the way for more efficient InGaN based LEDs, realization of terahertz generating nanocavities, and efficient Ge1−xSnx based silicon compatible optoelectronic devices.

Title of dissertation: GROWTH OF Zn POLAR BeMgZnO/ZnO HETEROSTRUCTURE WITH TWO DIMENSIONAL ELECTRON GAS (2DEG) AND FABRICATION OF SILVER SCHOTTKY DIODE ON BeMgZnO/ZnO HETEROSTRUCTURE By Md Barkat Ullah, Ph.D A dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Electrical and Computer Engineering at Virginia Commonwealth University. Virginia Commonwealth University,2017 Major Director: Dr. Hadis Morkoç, Professor, Electrical and Computer Engineering This thesis focuses on growth of Zn polar BeMgZnO/ZnO heterostructure on GaN/sapphire template with two dimensional electron gas (2DEG) for the application of UV photodetector/emitter and high speed electronics. The motivation of using BeMgZnO as a barrier layer originates from the need to reach plasmon-LO phonon resonance in order to obtain minimum longitudinal optical (LO) phonon lifetime. Presence of 2DEG was realized in BeMgZnO/ZnO heterostructure only when the Zn polarity was achieved during the nucleation growth of ZnO on GaN/sapphire template. It was found that, polarity of ZnO on (0001) GaN/sapphire template can be controlled by the oxygen to Zn ratio used during the nucleation growth. To obtain high structural and optical quality of BeMgZnO quaternary alloy, growth kinetics of BeMgZnO layer has been studied at the temperature range from 450°C-500°C. We have achieved the growth of single crystal Be.03Mg00.15ZnO alloy at 500 °C, more than 100°C higher compared to what reported in literature, on the (0001) GaN/sapphire template through the control of Zn/(Be+Mg) flux ratio. We have also observed a thermodynamic limitation of Mg incorporation into the wurtzite BeMgZnO alloy where the excess Mg adatom accumulated in the growing surface as a MgO rich cluster. Two dimensional electron gas with high (1.2×1013cm-2) sheet carrier density was achieved at the Be0.03Mg0.41ZnO/ZnO interface through strain engineering by incorporating Be into MgZnO ternary alloy. To obtain the similar sheet carrier density it would require above 60% of Mg in MgZnO/ZnO heterostructure with reduced structural quality. A systematic comparison of sheet carrier density has been made with the already reported results from Zn polar MgZnO/ZnO heterostructure as well as with the theoretical calculation. Silver Schottky diode on Be0.02Mg0.26ZnO/ZnO heterostructure with barrier height 1.07 eV and ideality factor 1.22 was obtained with 8 order of rectification ratio. The temperature-dependent electrical characteristics were studied by using temperature dependent current-voltage (I-V) measurements. Richardson constant value of 34.8 Acm-2K-2 was found experimentally which was close to the theoretical value of 36 Acm-2K-2 known for Be0.02Mg0.26ZnO alloy.

This thesis reports a comprehensive study of quaternary BeMgZnO alloy and BeMgZnO/ZnO heterostructures for UV-optoelectronics electronic applications. It was shown that by tuning Be and Mg contents in the heterostructures, high carrier densities of two-dimensional electron gas (2DEG) are achievable and makes its use possible for high power RF applications. Additionally, optical bandgaps as high as 5.1 eV were achieved for single crystal wurtzite material which allows the use of the alloy for solar blind optoelectronics (Eg>4.5eV) or intersubband devices. A systematic experimental and theoretical study of lattice parameters and bandgaps of quaternary BeMgZnO alloy was performed for the whole range of compositions. Composition independent bowing parameters were determined which allows accurate predictions of experimentally measured values. The BeMgZnO thin films were grown by plasma assisted molecular beam epitaxy (P-MBE) in a wide range of compositions. The optimization of the growth conditions and its effects on the material properties were explored. The surface morphology and electrical characteristics of the films grown on (0001) sapphire were found to critically depend on the metal-to-oxygen ratio. Samples grown under slightly oxygen-rich conditions exhibited the lowest RMS surface roughness (as low as 0.5 nm). Additionally, the films grown under oxygen-rich conditions were semi-insulating (>105 Ω∙cm), while the films grown under metal-rich conditions were semiconducting (~102 Ω∙cm). Additionally, with increasing bandgap Stokes shift increases, reaching ~0.5 eV for the films with 4.6 eV absorption edge suggests the presence of band tail states introduced by potential fluctuations and alloying. From spectrally resolved PL transients, BeMgZnO films grown on a GaN/sapphire template having higher Mg/Be content ratio exhibit smaller localization depth and brighter photoluminescence at low temperatures. The optimum content ratio for better room temperature optical performance was found to be ~2.5. The BeMgZnO material system and heterostructures are promising candidates for the device fabrication. 2DEG densities of MgZnO/ZnO heterostructures were shown to improve significantly (above 1013 cm-2) by adding even a small amount of Be (1-5%). As an essential step toward device fabrication, reliable ohmic contacts to ZnO were established with remarkably low specific contact resistivities below 10-6 Ohm-cm2 for films with 1018 cm-3 carrier density.

Efficient and robust blue InGaN multiple quantum well (MQW) light emitters have become ubiquitous; however, they still have unattained theoretical potential. It is widely accepted that “localization” of carriers due to indium fluctuations theoretically enhance their efficiency by moderating defect-associated nonradiative recombination. To help develop a complete understanding of localization effects on carrier dynamics, this thesis explores degree of localization in InGaN MQWs and its dependence on well thickness and number of wells, through temperature and power dependent photoluminescence measurements. Additionally, silicon-compatible, nontoxic, colloidally synthesizable 2-5 nm Ge1-xSnx alloy quantum-dots (QDs) are explored for potential visible to near-IR optoelectronic applications. While bulk Ge is an indirect gap material, QD confinement allows enhanced direct transitions, and alloying with Sn improves transition oscillator strengths. Temperature dependent steady-state and time-resolved photoluminescence reveal relaxation pathways involving bright/dark excitons and surface states in Ge1-xSnx QDs, showing their great potential for future use.