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The work contained in this dissertation is focused on the optical properties of direct band gap semiconductors which crystallize in a wurtzite structure: more specifically, the III-nitrides and ZnO. By using cathodoluminescence spectroscopy, many of their properties have been investigated, including band gaps, defect energy levels, carrier lifetimes, strain states,

The work contained in this dissertation is focused on the optical properties of direct band gap semiconductors which crystallize in a wurtzite structure: more specifically, the III-nitrides and ZnO. By using cathodoluminescence spectroscopy, many of their properties have been investigated, including band gaps, defect energy levels, carrier lifetimes, strain states, exciton binding energies, and effects of electron irradiation on luminescence. Part of this work is focused on p-type Mg-doped GaN and InGaN. These materials are extremely important for the fabrication of visible light emitting diodes and diode lasers and their complex nature is currently not entirely understood. The luminescence of Mg-doped GaN films has been correlated with electrical and structural measurements in order to understand the behavior of hydrogen in the material. Deeply-bound excitons emitting near 3.37 and 3.42 eV are observed in films with a significant hydrogen concentration during cathodoluminescence at liquid helium temperatures. These radiative transitions are unstable during electron irradiation. Our observations suggest a hydrogen-related nature, as opposed to a previous assignment of stacking fault luminescence. The intensity of the 3.37 eV transition can be correlated with the electrical activation of the Mg acceptors. Next, the acceptor energy level of Mg in InGaN is shown to decrease significantly with an increase in the indium composition. This also corresponds to a decrease in the resistivity of these films. In addition, the hole concentration in multiple quantum well light emitting diode structures is much more uniform in the active region when Mg-doped InGaN (instead of Mg-doped GaN) is used. These results will help improve the efficiency of light emitting diodes, especially in the green/yellow color range. Also, the improved hole transport may prove to be important for the development of photovoltaic devices. Cathodoluminescence studies have also been performed on nanoindented ZnO crystals. Bulk, single crystal ZnO was indented using a sub-micron spherical diamond tip on various surface orientations. The resistance to deformation (the "hardness") of each surface orientation was measured, with the c-plane being the most resistive. This is due to the orientation of the easy glide planes, the c-planes, being positioned perpendicularly to the applied load. The a-plane oriented crystal is the least resistive to deformation. Cathodoluminescence imaging allows for the correlation of the luminescence with the regions located near the indentation. Sub-nanometer shifts in the band edge emission have been assigned to residual strain the crystals. The a- and m-plane oriented crystals show two-fold symmetry with regions of compressive and tensile strain located parallel and perpendicular to the ±c-directions, respectively. The c-plane oriented crystal shows six-fold symmetry with regions of tensile strain extending along the six equivalent a-directions.
ContributorsJuday, Reid (Author) / Ponce, Fernando A. (Thesis advisor) / Drucker, Jeff (Committee member) / Mccartney, Martha R (Committee member) / Menéndez, Jose (Committee member) / Shumway, John (Committee member) / Arizona State University (Publisher)
Created2013
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Description
This dissertation is on the study of structural and optical properties of some III-V and II-VI compound semiconductors. The first part of this dissertation is a study of the deformation mechanisms associated with nanoindentation and nanoscratching of InP, GaN, and ZnO crystals. The second part is an investigation of some

This dissertation is on the study of structural and optical properties of some III-V and II-VI compound semiconductors. The first part of this dissertation is a study of the deformation mechanisms associated with nanoindentation and nanoscratching of InP, GaN, and ZnO crystals. The second part is an investigation of some fundamental issues regarding compositional fluctuations and microstructure in GaInNAs and InAlN alloys. In the first part, the microstructure of (001) InP scratched in an atomic force microscope with a small diamond tip has been studied as a function of applied normal force and crystalline direction in order to understand at the nanometer scale the deformation mechanisms in the zinc-blende structure. TEM images show deeper dislocation propagation for scratches along <110> compared to <100>. High strain fields were observed in <100> scratches, indicating hardening due to locking of dislocations gliding on different slip planes. Reverse plastic flow have been observed in <110> scratches in the form of pop-up events that result from recovery of stored elastic strain. In a separate study, nanoindentation-induced plastic deformation has been studied in c-, a-, and m-plane ZnO single crystals and c-plane GaN respectively, to study the deformation mechanism in wurtzite hexagonal structures. TEM results reveal that the prime deformation mechanism is slip on basal planes and in some cases, on pyramidal planes, and strain built up along particular directions. No evidence of phase transformation or cracking was observed in both materials. CL imaging reveals quenching of near band-edge emission by dislocations. In the second part, compositional inhomogeneity in quaternary GaInNAs and ternary InAlN alloys has been studied using TEM. It is shown that exposure to antimony during growth of GaInNAs results in uniform chemical composition in the epilayer, as antimony suppresses the surface mobility of adatoms that otherwise leads to two-dimensional growth and elemental segregation. In a separate study, compositional instability is observed in lattice-matched InAlN films grown on GaN, for growth beyond a certain thickness. Beyond 200 nm of thickness, two sub-layers with different indium content are observed, the top one with lower indium content.
ContributorsHuang, Jingyi (Author) / Ponce, Fernando A. (Thesis advisor) / Carpenter, Ray W (Committee member) / Smith, David J. (Committee member) / Yu, Hongbin (Committee member) / Treacy, Michael Mj (Committee member) / Arizona State University (Publisher)
Created2013
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Description
There has been recent interest in demonstrating solar cells which approach the detailed-balance or thermodynamic efficiency limit in order to establish a model system for which mass-produced solar cells can be designed. Polycrystalline CdS/CdTe heterostructures are currently one of many competing solar cell material systems. Despite being polycrystalline, efficiencies u

There has been recent interest in demonstrating solar cells which approach the detailed-balance or thermodynamic efficiency limit in order to establish a model system for which mass-produced solar cells can be designed. Polycrystalline CdS/CdTe heterostructures are currently one of many competing solar cell material systems. Despite being polycrystalline, efficiencies up to 21 % have been demonstrated by the company First Solar. However, this efficiency is still far from the detailed-balance limit of 32.1 % for CdTe. This work explores the use of monocrystalline CdTe/MgCdTe and ZnTe/CdTe/MgCdTe double heterostructures (DHs) grown on (001) InSb substrates by molecular beam epitaxy (MBE) for photovoltaic applications.

Undoped CdTe/MgCdTe DHs are first grown in order to determine the material quality of the CdTe epilayer and to optimize the growth conditions. DH samples show strong photoluminescence with over double the intensity as that of a GaAs/AlGaAs DH with an identical layer structure. Time-resolved photoluminescence of the CdTe/MgCdTe DH gives a carrier lifetime of up to 179 ns for a 2 µm thick CdTe layer, which is more than one order of magnitude longer than that of polycrystalline CdTe films. MgCdTe barrier layers are found to be effective at confining photogenerated carriers and have a relatively low interface recombination velocity of 461 cm/s. The optimal growth temperature and Cd/Te flux ratio is determined to be 265 °C and 1.5, respectively.

Monocrystalline ZnTe/CdTe/MgCdTe P-n-N DH solar cells are designed, grown, processed into solar cell devices, and characterized. A maximum efficiency of 6.11 % is demonstrated for samples without an anti-reflection coating. The low efficiency is mainly due to the low open-circuit voltage (Voc), which is attributed to high dark current caused by interface recombination at the ZnTe/CdTe interface. Low-temperature measurements show a linear increase in Voc with decreasing temperature down to 77 K, which suggests that the room-temperature operation is limited by non-radiative recombination. An open-circuit voltage of 1.22 V and an efficiency of 8.46 % is demonstrated at 77 K. It is expected that a coherently strained MgCdTe/CdTe/MgCdTe DH solar cell design will produce higher efficiency and Voc compared to the ZnTe/CdTe/MgCdTe design with relaxed ZnTe layer.
ContributorsDiNezza, Michael John (Author) / Zhang, Yong-Hang (Thesis advisor) / Johnson, Shane (Committee member) / Tao, Meng (Committee member) / Holman, Zachary (Committee member) / Arizona State University (Publisher)
Created2014
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Description
Group III-nitride semiconductors have wide application in optoelectronic devices. Spontaneous and piezoelectric polarization effects have been found to be critical for electric and optical properties of group III-nitrides. In this dissertation, firstly, the crystal orientation dependence of the polarization is calculated and in-plane polarization is revealed. The in-plane polarization is

Group III-nitride semiconductors have wide application in optoelectronic devices. Spontaneous and piezoelectric polarization effects have been found to be critical for electric and optical properties of group III-nitrides. In this dissertation, firstly, the crystal orientation dependence of the polarization is calculated and in-plane polarization is revealed. The in-plane polarization is sensitive to the lateral characteristic dimension determined by the microstructure. Specific semi-polar plane growth is suggested for reducing quantum-confined Stark effect. The macroscopic electrostatic field from the polarization discontinuity in the heterostructures is discussed, b ased on that, the band diagram of InGaN/GaN quantum well/barrier and AlGaN/GaN heterojunction is obtained from the self-consistent solution of Schrodinger and Poisson equations. New device design such as triangular quantum well with the quenched polarization field is proposed. Electron holography in the transmission electron microscopy is used to examine the electrostatic potential under polarization effects. The measured potential energy profiles of heterostructure are compared with the band simulation, and evidences of two-dimensional hole gas (2DHG) in a wurtzite AlGaN/ AlN/ GaN superlattice, as well as quasi two-dimensional electron gas (2DEG) in a zinc-blende AlGaN/GaN are found. The large polarization discontinuity of AlN/GaN is the main source of the 2DHG of wurtzite nitrides, while the impurity introduced during the growth of AlGaN layer provides the donor states that to a great extent balance the free electrons in zinc-blende nitrides. It is also found that the quasi-2DEG concentration in zinc-blende AlGaN/GaN is about one order of magnitude lower than the wurtzite AlGaN/GaN, due to the absence of polarization. Finally, the InAlN/GaN lattice-matched epitaxy, which ideally has a zero piezoelectric polarization and strong spontaneous polarization, is experimentally studied. The breakdown in compositional homogeneity is triggered by threading dislocations with a screw component propagating from the GaN underlayer, which tend to open up into V-grooves at a certain thickness of the InxAl1-xN layer. The V-grooves coalesce at 200 nm and are filled with material that exhibits a significant drop in indium content and a broad luminescence peak. The structural breakdown is due to heterogeneous nucleation and growth at the facets of the V-grooves.
ContributorsWei, Qiyuan (Author) / Ponce, Fernando A. (Thesis advisor) / Tsen, Kong-Thon (Committee member) / Shumway, John (Committee member) / Menéndez, Jose (Committee member) / Smith, David (Committee member) / Arizona State University (Publisher)
Created2012
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Description
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

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.
ContributorsHill, Arlinda (Author) / Ponce, Fernando A. (Thesis advisor) / Chamberlin, Ralph V (Committee member) / Sankey, Otto F (Committee member) / Smith, David J. (Committee member) / Tsen, Kong-Thon (Committee member) / Arizona State University (Publisher)
Created2011
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Description
A dual chamber molecular beam epitaxy (MBE) system was rebuilt for the growth of 6.1 Angstrom II-VI and III-V compound semiconductor materials that are to be used in novel optoelectronic devices that take advantage of the nearly continuous bandgap availability between 0 eV and 3.4 eV. These devices include multijunction

A dual chamber molecular beam epitaxy (MBE) system was rebuilt for the growth of 6.1 Angstrom II-VI and III-V compound semiconductor materials that are to be used in novel optoelectronic devices that take advantage of the nearly continuous bandgap availability between 0 eV and 3.4 eV. These devices include multijunction solar cells and multicolor detectors. The MBE system upgrade involved the conversion of a former III-V chamber for II-VI growth. This required intensive cleaning of the chamber and components to prevent contamination. Special features including valved II-VI sources and the addition of a cold trap allowed for the full system to be baked to 200 degrees Celsius to improve vacuum conditions and reduce background impurity concentrations in epilayers. After the conversion, the system was carefully calibrated and optimized for the growth of ZnSe and ZnTe on GaAs (001) substrates. Material quality was assessed using X-ray diffraction rocking curves. ZnSe layers displayed a trend of improving quality with decreasing growth temperature reaching a minimum full-width half-maximum (FWHM) of 113 arcsec at 278 degrees Celsius. ZnTe epilayer quality increased with growth temperature under Zn rich conditions attaining a FWHM of 84 arcsec at 440 degrees Celsius. RHEED oscillations were successfully observed and used to obtain growth rate in situ for varying flux and temperature levels. For a fixed flux ratio, growth rate decreased with growth temperature as the desorption rate increased. A directly proportional dependence of growth rate on Te flux was observed for Zn rich growth. Furthermore, a method for determining the flux ratio necessary for attaining the stoichiometric condition was demonstrated.
ContributorsDettlaff, W. Hank G (Author) / Zhang, Yong-Hang (Thesis advisor) / Vasileska, Dragica (Committee member) / Johnson, Shane (Committee member) / Arizona State University (Publisher)
Created2012
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Description
This thesis mainly focuses on the study of quantum efficiency (QE) and its measurement, especially for nanowires (NWs). First, a brief introduction of nano-technology and nanowire is given to describe my initial research interest. Next various fundamental kinds of recombination mechanisms are described; both for radiative and non-radiative processes. This

This thesis mainly focuses on the study of quantum efficiency (QE) and its measurement, especially for nanowires (NWs). First, a brief introduction of nano-technology and nanowire is given to describe my initial research interest. Next various fundamental kinds of recombination mechanisms are described; both for radiative and non-radiative processes. This is an introduction for defining the internal quantum efficiency (IQE). A relative IQE measurement method is shown following that. Then it comes to the major part of the thesis discussing a procedure of quantum efficiency measurement using photoluminescence (PL) method and an integrating sphere, which has not been much applied to nanowires (NWs). In fact this is a convenient and useful approach for evaluating the quality of NWs since it considers not only the PL emission but also the absorption of NWs. The process is well illustrated and performed with both wavelength-dependent and power-dependent measurements. The measured PLQE is in the range of 0.3% ~ 5.4%. During the measurement, a phenomenon called photodegradation is observed and examined by a set of power-dependence measurements. This effect can be a factor for underestimating the PLQE and a procedure is introduced during the sample preparation process which managed to reduce this effect for some degree.
ContributorsChen, Dongzi (Author) / Ning, Cun-Zheng (Thesis advisor) / Zhang, Yong-Hang (Committee member) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2012
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Description
The work contained in this dissertation is focused on the structural and optical properties of III-V semiconductor structures for solar cell applications. By using transmission electron microscopy, many of their structural properties have been investigated, including morphology, defects, and strain relaxation. The optical properties of the semiconductor structures have been

The work contained in this dissertation is focused on the structural and optical properties of III-V semiconductor structures for solar cell applications. By using transmission electron microscopy, many of their structural properties have been investigated, including morphology, defects, and strain relaxation. The optical properties of the semiconductor structures have been studied by photoluminescence and cathodoluminescence.

Part of this work is focused on InAs quantum dots (QDs) embedded in AlGaAs matrices. This QD system is important for the realization of intermediate-band solar cells, which has three light absorption paths for high efficiency photovoltaics. The suppression of plastic strain relaxation in the QDs shows a significant improvement of the optoelectronic properties. A partial capping followed by a thermal annealing step is used to achieve spool-shaped QDs with a uniform height following the thickness of the capping layer. This step keeps the height of the QDs below a critical value that is required for plastic relaxation. The spool-shaped QDs exhibit two photoluminescence peaks that are attributed to ground and excited state transitions. The luminescence peak width is associated with the QD diameter distribution. An InAs cover layer formed during annealing is found responsible for the loss of the confinement of the excited states in smaller QDs.

The second part of this work is focused on the investigation of the InxGa1-xN thin films having different bandgaps for double-junction solar cells. InxGa1-xN films with x ≤ 0.15 were grown by metal organic chemical vapor deposition. The defects in films with different indium contents have been studied. Their effect on the optical properties of the film have been investigated by cathodoluminescence. InxGa1-xN films with indium contents higher than 20% were grown by molecular beam epitaxy. The strain relaxation in the films has been measured from electron diffraction patterns taken in cross-sectional TEM specimens. Moiré fringes in some of the films reveal interfacial strain relaxation that is explained by a critical thickness model.
ContributorsXie, Hong'en (Author) / Ponce, Fernando A. (Thesis advisor) / Crozier, Peter A. (Committee member) / Mccartney, Martha R (Committee member) / Arizona State University (Publisher)
Created2016
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Description
Light Emitting Diodes even with their longer life, robust build and low power consumption, they are still plagued by some problems the most significant of which are the current droop and thermal droop. Current droop causes a lowering in the Internal Quantum Efficiency with increased current injection while thermal droo

Light Emitting Diodes even with their longer life, robust build and low power consumption, they are still plagued by some problems the most significant of which are the current droop and thermal droop. Current droop causes a lowering in the Internal Quantum Efficiency with increased current injection while thermal droop lowers the whole Internal Quantum Efficiency curve with increase in temperature. The focus here was understanding effects of thermal droop and develop a method to control it.

Shockley Read Hall recombination plays a dominant role in the thermal droop effect when the current injection is low. Since the blue light emitting diode is based on Gallium Nitride, we need to take into consideration the effect of piezoelectric polarization in the quantum wells. The effects of the piezoelectric fields were studied based on the Gallium Nitride plane orientations. It was found in a Gallium Nitride light emitting diodes simulation study that more the number of quantum wells, lower would be the Radiative recombination rate. The problem of exacerbated spatial separation of electron hole wavefunctions in a thick single quantum well structure lead to the development of a dual well structure where one well assisted the other during high temperature operations. The Electron Blocking Layer was reduced in thickness and was made only 10 nm thick with a 5 nm Gallium Nitride buffer between it and the active region wells. The main reason for reducing the electron blocking layer thickness was to reduce the valance band offset and improve hole transport into the active region. Three different dual well designs were simulated of 3nm, 6nm and 9nm wide wells. The output parameters like the Power Spectral Density, Electron bound density, Light Output Power and Electron-Hole wavefunction overlaps were calculated. It was found that one of the wells acted as an assisting well where it had very little radiative recombination activity in it at room temperature.

As the temperature increased, it was observed that the electrons in the main well started to overflow out of it and into the assisting well where the radiative recombination rate increased significantly. This lead to a boost in Internal Quantum Efficiency.
ContributorsDas, Shiladitya (Author) / Zhao, Yuji (Thesis advisor) / Vasileska, Dragica (Committee member) / Ning, Cun-Zheng (Committee member) / Arizona State University (Publisher)
Created2017
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Description
In this dissertation research, conventional and aberration-corrected (AC) transmission electron microscopy (TEM) techniques were used to evaluate the structural and compositional properties of thin-film semiconductor compounds/alloys grown by molecular beam epitaxy for infrared photo-detection. Imaging, diffraction and spectroscopy techniques were applied to TEM specimens in cross-section geometry to extract information

In this dissertation research, conventional and aberration-corrected (AC) transmission electron microscopy (TEM) techniques were used to evaluate the structural and compositional properties of thin-film semiconductor compounds/alloys grown by molecular beam epitaxy for infrared photo-detection. Imaging, diffraction and spectroscopy techniques were applied to TEM specimens in cross-section geometry to extract information about extended structural defects, chemical homogeneity and interface abruptness. The materials investigated included InAs1-xBix alloys grown on GaSb (001) substrates, InAs/InAs1-xSbx type-II superlattices grown on GaSb (001) substrates, and CdTe-based thin-film structures grown on InSb (001) substrates.

The InAsBi dilute-bismide epitaxial films were grown on GaSb (001) substrates at relatively low growth temperatures. The films were mostly free of extended defects, as observed in diffraction-contrast images, but the incorporation of bismuth was not homogeneous, as manifested by the lateral Bi-composition modulation and Bi-rich surface droplets. Successful Bi incorporation into the InAs matrix was confirmed using lattice expansion measurements obtained from misfit strain analysis of high-resolution TEM (HREM) images.

Analysis of averaged intensity line profiles in HREM and scanning TEM (STEM) images of the Ga-free InAs/InAs1-xSbx type-II strained superlattices indicated slight variations in layer thickness across the superlattice stack. The interface abruptness was evaluated using misfit strain analysis of AC-STEM images, electron energy-loss spectroscopy and 002 dark-field imaging. The compositional profiles of antimony across the superlattices were fitted to a segregation model and revealed a strong antimony segregation probability.

The CdTe/MgxCd1-xTe double-heterostructures were grown with Cd overflux in a dual-chamber molecular beam epitaxy with an ultra-high vacuum transfer loadlock. Diffraction-contrast images showed that the growth temperature had a strong impact on the structural quality of the epilayers. Very abrupt CdTe/InSb interfaces were obtained for epilayers grown at the optimum temperature of 265 °C, and high-resolution imaging using AC-STEM revealed an interfacial transition region with a width of a few monolayers and smaller lattice spacing than either CdTe or InSb.
ContributorsLu, Jing (Author) / Smith, David J. (Thesis advisor) / Alford, Terry L. (Committee member) / Crozier, Peter A. (Committee member) / McCartney, Martha R. (Committee member) / Zhang, Yong-Hang (Committee member) / Arizona State University (Publisher)
Created2017