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Description
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
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 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
Description
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.
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.
ContributorsCai, Hui, Ph.D (Author) / Tongay, Sefaattin (Thesis advisor) / Dwyer, Christian (Committee member) / Zhuang, Houlong (Committee member) / Arizona State University (Publisher)
Created2018
Description
III-V multijunction solar cells have demonstrated record efficiencies with the best device currently at 46 % under concentration. Dilute nitride materials such as GaInNAsSb have been identified as a prime choice for the development of high efficiency, monolithic and lattice-matched multijunction solar cells as they can be lattice-matched to both GaAs and Ge substrates. These types of cells have demonstrated efficiencies of 44% for terrestrial concentrators, and with their upright configuration, they are a direct drop-in product for today’s space and concentrator solar panels. The work presented in this dissertation has focused on the development of relatively novel dilute nitride antimonide (GaNAsSb) materials and solar cells using plasma-assisted molecular beam epitaxy, along with the modeling and characterization of single- and multijunction solar cells.
Nitrogen-free ternary compounds such as GaInAs and GaAsSb were investigated first in order to understand their structural and optical properties prior to introducing nitrogen. The formation of extended defects and the resulting strain relaxation in these lattice-mismatched materials is investigated through extensive structural characterization. Temperature- and power-dependent photoluminescence revealed an inhomogeneous distribution of Sb in GaAsSb films, leading to carrier localization effects at low temperatures. Tuning of the growth parameters was shown to suppress these Sb-induced localized states.
The introduction of nitrogen was then considered and the growth process was optimized to obtain high quality GaNAsSb films lattice-matched to GaAs. Near 1-eV single-junction GaNAsSb solar cells were produced. The best devices used a p-n heterojunction configuration and demonstrated a current density of 20.8 mA/cm2, a fill factor of 64 % and an open-circuit voltage of 0.39 V, corresponding to a bandgap-voltage offset of 0.57 V, comparable with the state-of-the-art for this type of solar cells. Post-growth annealing was found to be essential to improve Voc but was also found to degrade the material quality of the top layers. Alternatives are discussed to improve this process. Unintentional high background doping was identified as the main factor limiting the device performance. The use of Bi-surfactant mediated growth is proposed for the first time for this material system to reduce this background doping and preliminary results are presented.
Nitrogen-free ternary compounds such as GaInAs and GaAsSb were investigated first in order to understand their structural and optical properties prior to introducing nitrogen. The formation of extended defects and the resulting strain relaxation in these lattice-mismatched materials is investigated through extensive structural characterization. Temperature- and power-dependent photoluminescence revealed an inhomogeneous distribution of Sb in GaAsSb films, leading to carrier localization effects at low temperatures. Tuning of the growth parameters was shown to suppress these Sb-induced localized states.
The introduction of nitrogen was then considered and the growth process was optimized to obtain high quality GaNAsSb films lattice-matched to GaAs. Near 1-eV single-junction GaNAsSb solar cells were produced. The best devices used a p-n heterojunction configuration and demonstrated a current density of 20.8 mA/cm2, a fill factor of 64 % and an open-circuit voltage of 0.39 V, corresponding to a bandgap-voltage offset of 0.57 V, comparable with the state-of-the-art for this type of solar cells. Post-growth annealing was found to be essential to improve Voc but was also found to degrade the material quality of the top layers. Alternatives are discussed to improve this process. Unintentional high background doping was identified as the main factor limiting the device performance. The use of Bi-surfactant mediated growth is proposed for the first time for this material system to reduce this background doping and preliminary results are presented.
ContributorsMaros, Aymeric (Author) / King, Richard R. (Thesis advisor) / Honsberg, C. (Christiana B.) (Committee member) / Goodnick, Stephen M. (Committee member) / Ponce, Fernando A. (Committee member) / Arizona State University (Publisher)
Created2017
Description
This dissertation focuses on the structural and optical properties of III-V semiconductor materials. Transmission electron microscopy and atomic force microscopy are used to study at the nanometer scale, the structural properties of defects, interfaces, and surfaces. A correlation with optical properties has been performed using cathodoluminescence.
The dissertation consists of four parts. The first part focuses on InAs quantum dots (QDs) embedded in a GaInP matrix for applications into intermediate band solar cells. The CuPt ordering of the group-III elements in Ga0.5In0.5P has been found to vary during growth of InAs QDs capped with GaAs. The degree of ordering depends on the deposition time of the QDs and on the thickness of the capping layer. The results indicate that disordered GaInP occurs in the presence of excess indium at the growth front.
The second part focuses on the effects of low-angle off-axis GaN substrate orientation and growth rates on the surface morphology of Mg-doped GaN epilayers. Mg doping produces periodic steps and a tendency to cover pinholes associated with threading dislocations. With increasing miscut angle, the steps are observed to increase in height from single to double basal planes, with the coexistence of surfaces with different inclinations. The structural properties are correlated with the electronic properties of GaN epilayers, indicating step bunching reduces the p-type doping efficiency. It is also found that the slower growth rates can enhance step-flow growth and suppress step bunching.
The third part focuses on the effects of inductively-coupled plasma etching on GaN epilayers. The results show that ion energy rather than ion density plays the key role in the etching process, in terms of structural and optical properties of the GaN films. Cathodoluminescence depth-profiling indicates that the band-edge emission of etched GaN is significantly quenched.
The fourth part focuses on growth of Mg-doped GaN on trench patterns. Anisotropic growth and nonuniform acceptor incorporation in p-GaN films have been observed. The results indicate that growth along the sidewall has a faster growth rate and therefore a lower acceptor incorporation efficiency, compared to the region grown on the basal plane.
The dissertation consists of four parts. The first part focuses on InAs quantum dots (QDs) embedded in a GaInP matrix for applications into intermediate band solar cells. The CuPt ordering of the group-III elements in Ga0.5In0.5P has been found to vary during growth of InAs QDs capped with GaAs. The degree of ordering depends on the deposition time of the QDs and on the thickness of the capping layer. The results indicate that disordered GaInP occurs in the presence of excess indium at the growth front.
The second part focuses on the effects of low-angle off-axis GaN substrate orientation and growth rates on the surface morphology of Mg-doped GaN epilayers. Mg doping produces periodic steps and a tendency to cover pinholes associated with threading dislocations. With increasing miscut angle, the steps are observed to increase in height from single to double basal planes, with the coexistence of surfaces with different inclinations. The structural properties are correlated with the electronic properties of GaN epilayers, indicating step bunching reduces the p-type doping efficiency. It is also found that the slower growth rates can enhance step-flow growth and suppress step bunching.
The third part focuses on the effects of inductively-coupled plasma etching on GaN epilayers. The results show that ion energy rather than ion density plays the key role in the etching process, in terms of structural and optical properties of the GaN films. Cathodoluminescence depth-profiling indicates that the band-edge emission of etched GaN is significantly quenched.
The fourth part focuses on growth of Mg-doped GaN on trench patterns. Anisotropic growth and nonuniform acceptor incorporation in p-GaN films have been observed. The results indicate that growth along the sidewall has a faster growth rate and therefore a lower acceptor incorporation efficiency, compared to the region grown on the basal plane.
ContributorsSU, PO-YI (Author) / Ponce, Fernando A. (Thesis advisor) / Smith, David J. (Committee member) / Crozier, Peter A. (Committee member) / Zhao, Yuji (Committee member) / Arizona State University (Publisher)
Created2020