Matching Items (6)

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Characterization of MBE-grown semiconductor materials for photovoltaic applications

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The research described in this dissertation involved the use of transmission electron microscopy (TEM) to characterize II-VI and III-V compound semiconductor quantum dots (QDs) and dilute-nitride alloys grown by molecular

The research described in this dissertation involved the use of transmission electron microscopy (TEM) to characterize II-VI and III-V compound semiconductor quantum dots (QDs) and dilute-nitride alloys grown by molecular beam epitaxy (MBE) and intended for photovoltaic applications. The morphology of CdTe QDs prepared by the post-annealing MBE method were characterized by various microscopy techniques including high-resolution transmission electron microscopy (HR-TEM), and high-angle annular-dark-field scanning transmission electron microscopy (HAADF-STEM). Extensive observations revealed that the of QD shapes were not well-defined, and the QD size and spatial distribution were not determined by the amount of CdTe deposition. These results indicated that the formation of II-VI QDs using a post-annealing treatment did not follow the conventional growth mechanism for III-V and IV-IV materials. The structural properties of dilute-nitride GaAsNx films grown using plasma-assisted MBE were characterized by TEM and HAADF-STEM. A significant amount of the nitrogen incorporated into the dilute nitride films was found to be interstitial, and that fluctuations in local nitrogen composition also occurred during growth. Post-growth partial relaxation of strain resulted in the formation of {110}-oriented microcracks in the sample with the largest substitutional nitrogen composition. Single- and multi-layered InAs QDs grown on GaAsSb/GaAs composite substrates were investigated using HR-TEM and HAADF-STEM. Correlation between the structural and optoelectronic properties revealed that the GaAsSb barrier layers had played an important role in tuning the energy-band alignments but without affecting the overall structural morphology. However, according to both XRD measurement and electron microscopy the densities of dislocations increased as the number of QD layers built up. An investigation of near-wetting layer-free InAs QDs incorporated with AlAs/GaAs spacer layers was carried out. The microscopy observations revealed that both embedded and non-embedded near-wetting layer-free InAs QDs did not have well-defined shapes unlike conventional InAs QDs. According to AFM analysis and plan-view TEM characterization, the InAs QDs incorporated with spacer layers had smaller dot density and more symmetrical larger sizes with an apparent bimodal size distribution (two distinct families of large and small dots) in comparison with conventional InAs QDs grown without any spacer layer.

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Date Created
  • 2014

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Correlative X-ray microscopy studies of CuIn₁-xGaxSe₂ solar cells

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It is well known that the overall performance of a solar cell is limited by the worst performing areas of the device. These areas are usually micro and nano-scale defects

It is well known that the overall performance of a solar cell is limited by the worst performing areas of the device. These areas are usually micro and nano-scale defects inhomogenously distributed throughout the material. Mitigating and/or engineering these effects is necessary to provide a path towards increasing the efficiency of state-of-the-art solar cells. The first big challenge is to identify the nature, origin and impact of such defects across length scales that span multiple orders of magnitude, and dimensions (time, temperature etc.). In this work, I present a framework based on correlative X-ray microscopy and big data analytics to identify micro and nanoscale defects and their impact on material properties in CuIn1-xGaxSe2 (CIGS) solar cells.

Synchrotron based X-ray Fluorescence (XRF) and X-ray Beam Induced Current (XBIC) are used to study the effect that compositional variations, between grains and at grain boundaries, have on CIGS device properties. An experimental approach is presented to correcting XRF and XBIC quantification of CIGS thin film solar cells. When applying XRF and XBIC to study low and high gallium CIGS devices, it was determined that increased copper and gallium at grain boundaries leads to increased collection efficiency at grain boundaries in low gallium absorbers. However, composition variations were not correlated with changes in collection efficiency in high gallium absorbers, despite the decreased collection efficiency observed at grain boundaries.

Understanding the nature and impact of these defects is only half the battle; controlling or mitigating their impact is the next challenge. This requires a thorough understanding of the origin of these defects and their kinetics. For such a study, a temperature and atmosphere controlled in situ stage was developed. The stage was utilized to study CIGS films during a rapid thermal growth process. Comparing composition variations across different acquisition times and growth temperatures required the implementation of machine learning techniques, including clustering and classification algorithms. From the analysis, copper was determined to segregate the faster than indium and gallium, and clustering techniques showed consistent elemental segregation into copper rich and copper poor regions. Ways to improve the current framework and new applications are also discussed.

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Date Created
  • 2018

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Layer structured gallium chalcogenides: controlled synthesis and emerging properties

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Layer structured two dimensional (2D) semiconductors have gained much interest due to their intriguing optical and electronic properties induced by the unique van der Waals bonding between layers. The extraordinary

Layer structured two dimensional (2D) semiconductors have gained much interest due to their intriguing optical and electronic properties induced by the unique van der Waals bonding between layers. The extraordinary success for graphene and transition metal dichalcogenides (TMDCs) has triggered a constant search for novel 2D semiconductors beyond them. Gallium chalcogenides, belonging to the group III-VI compounds, are a new class of 2D semiconductors that carry a variety of interesting properties including wide spectrum coverage of their bandgaps and thus are promising candidates for next generation electronic and optoelectronic devices. Pushing these materials toward applications requires more controllable synthesis methods and facile routes for engineering their properties on demand.

In this dissertation, vapor phase transport is used to synthesize layer structured gallium chalcogenide nanomaterials with highly controlled structure, morphology and properties, with particular emphasis on GaSe, GaTe and GaSeTe alloys. Multiple routes are used to manipulate the physical properties of these materials including strain engineering, defect engineering and phase engineering. First, 2D GaSe with controlled morphologies is synthesized on Si(111) substrates and the bandgap is significantly reduced from 2 eV to 1.7 eV due to lateral tensile strain. By applying vertical compressive strain using a diamond anvil cell, the band gap can be further reduced to 1.4 eV. Next, pseudo-1D GaTe nanomaterials with a monoclinic structure are synthesized on various substrates. The product exhibits highly anisotropic atomic structure and properties characterized by high-resolution transmission electron microscopy and angle resolved Raman and photoluminescence (PL) spectroscopy. Multiple sharp PL emissions below the bandgap are found due to defects localized at the edges and grain boundaries. Finally, layer structured GaSe1-xTex alloys across the full composition range are synthesized on GaAs(111) substrates. Results show that GaAs(111) substrate plays an essential role in stabilizing the metastable single-phase alloys within the miscibility gaps. A hexagonal to monoclinic phase crossover is observed as the Te content increases. The phase crossover features coexistence of both phases and isotropic to anisotropic structural transition.

Overall, this work provides insights into the controlled synthesis of gallium chalcogenides and opens up new opportunities towards optoelectronic applications that require tunable material properties.

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  • 2018

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Growth and characterization of InGaAsP alloy nanowires with widely tunable bandgaps for optoelectronic applications

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The larger tolerance to lattice mismatch in growth of semiconductor nanowires (NWs) offers much more flexibility for achieving a wide range of compositions and bandgaps via alloying within a single

The larger tolerance to lattice mismatch in growth of semiconductor nanowires (NWs) offers much more flexibility for achieving a wide range of compositions and bandgaps via alloying within a single substrate. The bandgap of III-V InGaAsP alloy NWs can be tuned to cover a wide range of (0.4, 2.25) eV, appealing for various optoelectronic applications such as photodetectors, solar cells, Light Emitting Diodes (LEDs), lasers, etc., given the existing rich knowledge in device fabrication based on these materials.

This dissertation explores the growth of InGaAsP alloys using a low-cost method that could be potentially important especially for III-V NW-based solar cells. The NWs were grown by Vapor-Liquid-Solid (VLS) and Vapor-Solid (VS) mechanisms using a Low-Pressure Chemical Vapor Deposition (LPCVD) technique. The concept of supersaturation was employed to control the morphology of NWs through the interplay between VLS and VS growth mechanisms. Comprehensive optical and material characterizations were carried out to evaluate the quality of the grown materials.

The growth of exceptionally high quality III-V phosphide NWs of InP and GaP was studied with an emphasis on the effects of vastly different sublimation rates of the associated III and V elements. The incorporation of defects exerted by deviation from stoichiometry was examined for GaP NWs, with an aim towards maximization of bandedge-to-defect emission ratio. In addition, a VLS-VS assisted growth of highly stoichiometric InP thin films and nano-networks with a wide temperature window from 560◦C to 720◦C was demonstrated. Such growth is shown to be insensitive to the type of substrates such as silicon, InP, and fused quartz. The dual gradient method was exploited to grow composition-graded ternary alloy NWs of InGaP, InGaAs, and GaAsP with different bandgaps ranging from 0.6 eV to 2.2 eV, to be used for making laterally-arrayed multiple bandgap (LAMB) solar cells. Furthermore, a template-based growth of the NWs was attempted based on the Si/SiO2 substrate. Such platform can be used to grow a wide range of alloy nanopillar materials, without being limited by typical lattice mismatch, providing a low cost universal platform for future PV solar cells.

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  • 2018

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Structural and optical properties of wide bandgap nitride semiconductors using electron microscopy techniques

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ABSTRACT Group III-nitride semiconductor materials have been commercially used in fabrication of light-emitting diodes (LEDs) and laser diodes (LDs) covering the spectral range from UV to visible and infrared, and

ABSTRACT Group III-nitride semiconductor materials have been commercially used in fabrication of light-emitting diodes (LEDs) and laser diodes (LDs) covering the spectral range from UV to visible and infrared, and exhibit unique properties suitable for modern optoelectronic applications. Great advances have recently happened in the research and development in high-power and high-efficiency blue-green-white LEDs, blue LDs and other optoelectronic applications. However, there are still many unsolved challenges with these materials. In this dissertation, several issues concerning structural, electronic and optical properties of III-nitrides have been investigated using a combination of transmission electron microscopy (TEM), electron holography (EH) and cathodoluminescence (CL) techniques. First, a trend of indium chemical inhomogeneity has been found as the indium composition increases for the InGaN epitaxial layers grown by hydride vapor phase epitaxy. Second, different mechanisms contributing to the strain relaxation have been studied for non-polar InGaN epitaxial layers grown on zinc oxide (ZnO) substrate. Third, various structural morphologies of non-polar InGaN epitaxial layers grown on free-standing GaN substrate have been investigated. Fourth, the effect of the growth temperature on the performance of GaN lattice-matched InAlN electron blocking layers has been studied. Finally, the electronic and optical properties of GaN nanowires containing a AlN/GaN superlattice structure have been investigated showing relatively small internal electric field and superlattice- and defect-related emissions along the nanowires.

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Date Created
  • 2011

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Growth, characterization, and thermodynamics of III-nitride semiconductors

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III-nitride alloys are wide band gap semiconductors with a broad range of applications in optoelectronic devices such as light emitting diodes and laser diodes. Indium gallium nitride light emitting diodes

III-nitride alloys are wide band gap semiconductors with a broad range of applications in optoelectronic devices such as light emitting diodes and laser diodes. Indium gallium nitride light emitting diodes have been successfully produced over the past decade. But the progress of green emission light emitting devices has been limited by the incorporation of indium in the alloy, mainly due to phase separation. This difficulty could be addressed by studying the growth and thermodynamics of these alloys. Knowledge of thermodynamic phase stabilities and of pressure - temperature - composition phase diagrams is important for an understanding of the boundary conditions of a variety of growth techniques. In this dissertation a study of the phase separation of indium gallium nitride is conducted using a regular solution model of the ternary alloy system. Graphs of Gibbs free energy of mixing were produced for a range of temperatures. Binodal and spinodal decomposition curves show the stable and unstable regions of the alloy in equilibrium. The growth of gallium nitride and indium gallium nitride was attempted by the reaction of molten gallium - indium alloy with ammonia at atmospheric pressure. Characterization by X-ray diffraction, photoluminescence, and secondary electron microscopy show that the samples produced by this method contain only gallium nitride in the hexagonal phase. The instability of indium nitride at the temperatures required for activation of ammonia accounts for these results. The photoluminescence spectra show a correlation between the intensity of a broad green emission, related to native defects, and indium composition used in the molten alloy. A different growth method was used to grow two columnar-structured gallium nitride films using ammonium chloride and gallium as reactants and nitrogen and ammonia as carrier gasses. Investigation by X-ray diffraction and spatially-resolved cathodoluminescence shows the film grown at higher temperature to be primarily hexagonal with small quantities of cubic crystallites, while the one grown at lower temperature to be pure hexagonal. This was also confirmed by low temperature photoluminescence measurements. The results presented here show that cubic and hexagonal crystallites can coexist, with the cubic phase having a much sharper and stronger luminescence. Controlled growth of the cubic phase GaN crystallites can be of use for high efficiency light detecting and emitting devices. The ammonolysis of a precursor was used to grow InGaN powders with different indium composition. High purity hexagonal GaN and InN were obtained. XRD spectra showed complete phase separation for samples with x < 30%, with ~ 9% indium incorporation in the 30% sample. The presence of InGaN in this sample was confirmed by PL measurements, where luminescence from both GaN and InGaN band edge are observed. The growth of higher indium compositions samples proved to be difficult, with only the presence of InN in the sample. Nonetheless, by controlling parameters like temperature and time may lead to successful growth of this III-nitride alloy by this method.

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Date Created
  • 2011