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- All Subjects: Pyrites
- Creators: Newman, Nathan
- Creators: Juday, Reid
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
A series of pyrite thin films were synthesized using a novel sequential evaporation
technique to study the effects of substrate temperature on deposition rate and micro-structure of
the deposited material. Pyrite was deposited in a monolayer-by-monolayer fashion using
sequential evaporation of Fe under high vacuum, followed by sulfidation at high S pressures
(typically > 1 mTorr to 1 Torr). Thin films were synthesized using two different growth processes; a
one-step process in which a constant growth temperature is maintained throughout growth, and a
three-step process in which an initial low temperature seed layer is deposited, followed by a high
temperature layer, and then finished with a low temperature capping layer. Analysis methods to
analyze the properties of the films included Glancing Angle X-Ray Diffraction (GAXRD),
Rutherford Back-scattering Spectroscopy (RBS), Transmission Electron Microscopy (TEM),
Secondary Ion Mass Spectroscopy (SIMS), 2-point IV measurements, and Hall effect
measurements. Our results show that crystallinity of the pyrite thin film improves and grain size
increases with increasing substrate temperature. The sticking coefficient of Fe was found to
increase with increasing growth temperature, indicating that the Fe incorporation into the growing
film is a thermally activated process.
technique to study the effects of substrate temperature on deposition rate and micro-structure of
the deposited material. Pyrite was deposited in a monolayer-by-monolayer fashion using
sequential evaporation of Fe under high vacuum, followed by sulfidation at high S pressures
(typically > 1 mTorr to 1 Torr). Thin films were synthesized using two different growth processes; a
one-step process in which a constant growth temperature is maintained throughout growth, and a
three-step process in which an initial low temperature seed layer is deposited, followed by a high
temperature layer, and then finished with a low temperature capping layer. Analysis methods to
analyze the properties of the films included Glancing Angle X-Ray Diffraction (GAXRD),
Rutherford Back-scattering Spectroscopy (RBS), Transmission Electron Microscopy (TEM),
Secondary Ion Mass Spectroscopy (SIMS), 2-point IV measurements, and Hall effect
measurements. Our results show that crystallinity of the pyrite thin film improves and grain size
increases with increasing substrate temperature. The sticking coefficient of Fe was found to
increase with increasing growth temperature, indicating that the Fe incorporation into the growing
film is a thermally activated process.
ContributorsWertheim, Alex (Author) / Newman, Nathan (Thesis advisor) / Singh, Rakesh (Committee member) / Bertoni, Mariana (Committee member) / Arizona State University (Publisher)
Created2014
Description
Pyrite is a 0.95 eV bandgap semiconductor which is purported to have great potential in widespread, low–cost photovoltaic cells. A thorough material selection process was used in the design of a pyrite sequential vapor deposition chamber aimed at reducing and possibly eliminating contamination during thin film growth. The design process focused on identifying materials that do not produce volatile components when exposed to high temperatures and high sulfur pressures. Once the materials were identified and design was completed, the ultra–high vacuum growth system was constructed and tested.
Pyrite thin films were deposited using the upgraded sequential vapor deposition chamber by varying the substrate temperature from 250°C to 420°C during deposition, keeping sulfur pressure constant at 1 Torr. Secondary Ion Mass Spectrometry (SIMS) results showed that all contaminants in the films were reduced in concentration by orders of magnitude from those grown with the previous system. Characterization techniques of Rutherford Back–scattering Spectrometry (RBS), X–Ray Diffraction (XRD), Raman Spectroscopy, Optical Profilometry and UV/Vis/Near–IR Spectroscopy were performed on the deposited thin films. The results indicate that stoichiometric ratio of S:Fe, structural–quality (epitaxy), optical roughness and percentage of pyrite in the deposited thin films improve with increase in deposition temperature. A Tauc plot of the optical measurements indicates that the pyrite thin films have a bandgap of 0.94 eV.
Pyrite thin films were deposited using the upgraded sequential vapor deposition chamber by varying the substrate temperature from 250°C to 420°C during deposition, keeping sulfur pressure constant at 1 Torr. Secondary Ion Mass Spectrometry (SIMS) results showed that all contaminants in the films were reduced in concentration by orders of magnitude from those grown with the previous system. Characterization techniques of Rutherford Back–scattering Spectrometry (RBS), X–Ray Diffraction (XRD), Raman Spectroscopy, Optical Profilometry and UV/Vis/Near–IR Spectroscopy were performed on the deposited thin films. The results indicate that stoichiometric ratio of S:Fe, structural–quality (epitaxy), optical roughness and percentage of pyrite in the deposited thin films improve with increase in deposition temperature. A Tauc plot of the optical measurements indicates that the pyrite thin films have a bandgap of 0.94 eV.
ContributorsWalimbe, Aditya (Author) / Newman, Nathan (Thesis advisor) / Alford, Terry (Committee member) / Singh, Rakesh (Committee member) / Arizona State University (Publisher)
Created2016
Description
Measurements of the geometrical magnetoresistance of a conventional semiconductor, gallium arsenide (GaAs), and a more recently developed semiconductor, iron pyrite (FeS2) were measured in the Corbino disc geometry as a function of magnetic field to determine the carrier mobility (μm). These results were compared with measurements of the Hall mobility (μH) made in the Van der Pauw configuration. The scattering coefficient (ξ), defined as the ratio between magnetoresistance and Hall mobility (μm/μH), was determined experimentally for GaAs and natural pyrite from 300 K to 4.2 K. The effect of contact resistance and heating on the measurement accuracy is discussed.
ContributorsRavi, Aditya (Author) / Newman, Nathan (Thesis advisor) / Singh, Rakesh (Committee member) / Ferry, David K. (Committee member) / Arizona State University (Publisher)
Created2016
Description
This dissertation covers my doctoral research on the cathodoluminescence (CL) study of the optical properties of III-niride semiconductors.
The first part of this thesis focuses on the optical properties of Mg-doped gallium nitride (GaN:Mg) epitaxial films. GaN is an emerging material for power electronics, especially for high power and high frequency applications. Compared to traditional Si-based devices, GaN-based devices offer superior breakdown properties, faster switching speed, and reduced system size. Some of the current device designs involve lateral p-n junctions which require selective-area doping. Dopant distribution in the selectively-doped regions is a critical issue that can impact the device performance. While most studies on Mg doping in GaN have been reported for epitaxial grown on flat c-plane substrates, questions arise regarding the Mg doping efficiency and uniformity in selectively-doped regions, where growth on surfaces etched away from the exact c-plane orientation is involved. Characterization of doping concentration distribution in lateral structures using secondary ion mass spectroscopy lacks the required spatial resolution. In this work, visualization of acceptor distribution in GaN:Mg epilayers grown by metalorganic chemical vapor deposition (MOCVD) was achieved at sub-micron scale using CL imaging. This was enabled by establishing a correlation among the luminescence characteristics, acceptor concentration, and electrical conductivity of GaN:Mg epilayers. Non-uniformity in acceptor distribution has been observed in epilayers grown on mesa structures and on miscut substrates. It is shown that non-basal-plane surfaces, such as mesa sidewalls and surface step clusters, promotes lateral growth along the GaN basal planes with a reduced Mg doping efficiency. The influence of surface morphology on the Mg doping efficiency in GaN has been studied.
The second part of this thesis focuses on the optical properties of InGaN for photovoltaic applications. The effects of thermal annealing and low energy electron beam irradiation (LEEBI) on the optical properties of MOCVD-grown In0.14Ga0.86N films were studied. A multi-fold increase in luminescence intensity was observed after 800 °C thermal annealing or LEEBI treatment. The mechanism leading to the luminescence intensity increase has been discussed. This study shows procedures that significantly improve the luminescence efficiency of InGaN, which is important for InGaN-based optoelectronic devices.
The first part of this thesis focuses on the optical properties of Mg-doped gallium nitride (GaN:Mg) epitaxial films. GaN is an emerging material for power electronics, especially for high power and high frequency applications. Compared to traditional Si-based devices, GaN-based devices offer superior breakdown properties, faster switching speed, and reduced system size. Some of the current device designs involve lateral p-n junctions which require selective-area doping. Dopant distribution in the selectively-doped regions is a critical issue that can impact the device performance. While most studies on Mg doping in GaN have been reported for epitaxial grown on flat c-plane substrates, questions arise regarding the Mg doping efficiency and uniformity in selectively-doped regions, where growth on surfaces etched away from the exact c-plane orientation is involved. Characterization of doping concentration distribution in lateral structures using secondary ion mass spectroscopy lacks the required spatial resolution. In this work, visualization of acceptor distribution in GaN:Mg epilayers grown by metalorganic chemical vapor deposition (MOCVD) was achieved at sub-micron scale using CL imaging. This was enabled by establishing a correlation among the luminescence characteristics, acceptor concentration, and electrical conductivity of GaN:Mg epilayers. Non-uniformity in acceptor distribution has been observed in epilayers grown on mesa structures and on miscut substrates. It is shown that non-basal-plane surfaces, such as mesa sidewalls and surface step clusters, promotes lateral growth along the GaN basal planes with a reduced Mg doping efficiency. The influence of surface morphology on the Mg doping efficiency in GaN has been studied.
The second part of this thesis focuses on the optical properties of InGaN for photovoltaic applications. The effects of thermal annealing and low energy electron beam irradiation (LEEBI) on the optical properties of MOCVD-grown In0.14Ga0.86N films were studied. A multi-fold increase in luminescence intensity was observed after 800 °C thermal annealing or LEEBI treatment. The mechanism leading to the luminescence intensity increase has been discussed. This study shows procedures that significantly improve the luminescence efficiency of InGaN, which is important for InGaN-based optoelectronic devices.
ContributorsLiu, Hanxiao (Author) / Ponce, Fernando A. (Thesis advisor) / Zhao, Yuji (Committee member) / Newman, Nathan (Committee member) / Fischer, Alec M (Committee member) / Arizona State University (Publisher)
Created2020