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- All Subjects: Condensed Matter Physics
- All Subjects: Cathodoluminescence
- Creators: Kaindl, Robert
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 thesis focuses on how domain formation and local disorder mediate non-equilibrium order in the context of condensed matter physics. More specifically, the data supports c-axis CDW ordering in the context of the rare-earth Tritellurides. Experimental studies were performed on Pd:ErTe3 by ultra-fast pump-probe and x-ray free electron laser (XFEL). Ginzburg Landau models were used to simulate domain formation. Universal scaling analysis on the data reveals that topological defects govern the relaxation of domain walls in Pd:ErTe3. This thesis presents information on progress towards using light to control material domains.
ContributorsMiller, Alex (Author) / Teitelbaum, Samuel (Thesis director) / Belitsky, Andrei (Committee member) / Kaindl, Robert (Committee member) / Barrett, The Honors College (Contributor) / Department of Physics (Contributor) / School of Mathematical and Statistical Sciences (Contributor)
Created2023-05
Description
The performance of kilometer-scale electron accelerators, which are used for high energy physics and next-generation light sources as well as meter-scale ultra-fast electron diffraction setups is limited by the brightness of electron sources. A potential emerging candidate for such applications is the family of alkali and bi-alkali antimonides. Much of the physics of photoemission from such semiconductor photocathodes is not fully understood even today, which poses a hindrance to the complete exploration and optimization of their photoemission properties. This thesis presents the theoretical and experimental measurements which lead to advances in the understanding of the photoemission process and properties of cesium-antimonide photocathodes. First, the growth of high quantum efficiency (QE), atomically smooth and chemically homogeneous Cs$_3$Sb cathodes on lattice-matched strontium titanate substrates (STO) is demonstrated. The roughness-induced mean transverse energies (MTE) simulations indicate that the contribution to MTE from nanoscale surface roughness of Cs$_3$Sb cathodes grown on STO is inconsequential over typically used field gradients in photoinjectors. Second, the formulation of a new approach to model photoemission from cathodes with disordered surfaces is demonstrated. The model is used to explain near-threshold photoemission from thin film Cs$_3$Sb cathodes. This model suggests that the MTE values may get limited to higher values due to the defect density of states near the valence band maximum. Third, the detailed measurements of MTE and kinetic energy distribution spectra along with QE from Cs$_3$Sb cathodes using the photoemission electron microscope are presented. These measurements indicate that Cs$_3$Sb cathodes have a work function in the range of 1.5-1.6 eV. When photoemitting near this work function energy, the MTE nearly converges to the thermal limit of 26 meV. However, the QE is extremely low, of the order of 10$^{-7}$, which limits the operation of these photocathodes for high current applications. Lastly, the growth of Cs$_3$Sb cathodes using the ion beam assisted molecular beam deposition (IBA-MBE) technique is demonstrated. This technique has the potential to grow epitaxial Cs$_3$Sb cathodes in a more reproducible, easier fashion. Structural characterization of such cathodes via tools such as reflection high energy electron diffraction (RHEED) and x-ray diffraction (XRD) will be necessary to investigate the role of the IBA-MBE technique in facilitating the epitaxial, ordered growth of alkali-antimonides.
ContributorsSaha, Pallavi (Author) / Karkare, Siddharth (Thesis advisor) / Bennett, Peter (Committee member) / Nemanich, Robert (Committee member) / Kaindl, Robert (Committee member) / Arizona State University (Publisher)
Created2023
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
Description
High critical-temperature (Tc) superconductivity in the cuprates has been a defining challenge of condensed matter physics for the 35 years since their discovery. One strategy to address this challenge has been to look for "cuprate analog'' materials: alternative transition metal oxides that exhibit ingredients that are considered proxies for cuprate physics. These key ingredients include a quasi-2D structure based on the CuO2 planes, a nominal oxidation state for Cu2+: 3d9 with a single hole in the uppermost dx2-y2 orbital, and a strong O(2p) and Cu(3d) hybridization. Nickelates have been an obvious choice of study in this context due to the proximity of Ni to Cu on the periodic table. After a 30 year wait, superconductivity in nickelates was realized for the first time in 2019 in hole-doped NdNiO2 (Li et al, 2019). This material contains NiO2 planes (analog to the CuO2 planes of the cuprates), and realizes a Ni1+ oxidation state (analog to Cu2+). NdNiO2 is simply the infinite-layer member of a larger family of materials represented by the chemical formula Rn+1NinO2n+2 (R= La, Pr, Nd; n >= 2), where n refers to the number of NiO2 planes along the c axis. In this thesis, a comprehensive description of the electronic structure of the Rn+1NinO2n+2 family of layered rare-earth nickelates (for n= oo and n=2-6) using state-of-the-art first-principles methods is presented. Specifically, different levels of theory are used to describe the electronic structure of this family of materials: from density-functional band theory (DFT) to incorporating correlation effects at the mean-field level via DFT+U, and finally including dynamical many-body effects via DFT+dynamical mean-field theory (DFT+DMFT). It is shown that the cuprate-like character of the layered nickelate series increases from the n=oo to the n=3 members. Namely, as n decreases the electronic structure becomes more single-band-like, and the degree of p-d hybridization increases while correlations are dominated by the dx2-y2 orbitals. Insights from these calculations allowed for the prediction of the n=4-6 nickelates as ideal candidates for nickelate superconductivity. Indeed, superconductivity was subsequently observed in the quintuple layer nickelate Nd6Ni5O12 (Pan et al, 2021). That superconductivity arises in this layered rare-earth nickelate series, suggests that a new family of superconductors has been uncovered, currently with two members, n=oo and n=5.
ContributorsLaBollita, Harrison (Author) / S. Botana, Antia (Thesis advisor) / Erten, Onur (Committee member) / Mundy, Julia (Committee member) / Kaindl, Robert (Committee member) / Arizona State University (Publisher)
Created2023