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Structural Characterization of III-V Bismide Materials Grown by Molecular Beam Epitaxy

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III-V-bismide semiconductor alloys are a class of materials with applications in the mid and long wave infrared spectrum. The quaternary alloy InAsSbBi is attractive because it can be grown

III-V-bismide semiconductor alloys are a class of materials with applications in the mid and long wave infrared spectrum. The quaternary alloy InAsSbBi is attractive because it can be grown lattice-matched to commercially available GaSb substrates, and the adjustment of the Bi and Sb mole fractions enables both lattice constant and bandgap to be tuned independently. This dissertation provides a comprehensive study of the surface morphology and the structural and chemical properties of InAsSbBi alloys grown by molecular beam epitaxy.

210 nm thick InAsSbBi layers grown at temperatures from 280 °C to 430 °C on (100) on-axis, (100) offcut 1° to (011), and (100) offcut 4° to (111)A GaSb substrates are investigated using Rutherford back scattering, X-ray diffraction, transmission electron microscopy, Nomarski optical microscopy, atomic force microscopy, and photoluminescence spectroscopy. The results indicate that the layers are coherently strained and contain dilute Bi mole fractions.

Large surface droplets with diameters and densities on the order of 3 µm and 106 cm-2 are observed when the growth is performed with As overpressures around 1%. Preferential orientation of the droplets occurs along the [011 ̅] step edges offcut (100) 1° to (011) substrate. The surface droplets are not observed when the As overpressure is increased to 4%. Small crystalline droplets with diameters and densities on the order of 70 nm and 1010 cm-2 are observed between the large droplets for the growth at 430°C. Analysis of one of the small droplets indicates a misoriented zinc blende structure composed of In, Sb, and Bi, with a 6.543 ± 0.038 Å lattice constant.

Lateral variation in the Bi mole fraction is observed in InAsSbBi grown at high temperature (400 °C, 420 °C) on (100) on-axis and (100) offcut 4° to (111)A substrates, but is not observed for growth at 280 °C or on (100) substrates that are offcut 1° to (011). Improved crystal and optical quality is observed in the high temperature grown InAsSbBi and CuPtB type atomic ordering on the {111}B planes is observed in the low temperature grown InAsSbBi. Strain induced tilt is observed in coherently strained InAsSbBi grown on offcut substrates.

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  • 2020

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MBE Growth and Characterization of III-V Bismide Semiconductor Alloys for Mid- and Long-Wave Infrared Applications

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The molecular beam epitaxy growth of the III-V semiconductor alloy indium arsenide antimonide bismide (InAsSbBi) is investigated over a range of growth temperatures and V/III flux ratios. Bulk and quantum

The molecular beam epitaxy growth of the III-V semiconductor alloy indium arsenide antimonide bismide (InAsSbBi) is investigated over a range of growth temperatures and V/III flux ratios. Bulk and quantum well structures grown on gallium antimonide (GaSb) substrates are examined. The relationships between Bi incorporation, surface morphology, growth temperature, and group-V flux are explored. A growth model is developed based on the kinetics of atomic desorption, incorporation, surface accumulation, and droplet formation. The model is applied to InAsSbBi, where the various process are fit to the Bi, Sb, and As mole fractions. The model predicts a Bi incorporation limit for lattice matched InAsSbBi grown on GaSb.The optical performance and bandgap energy of InAsSbBi is examined using photoluminescence spectroscopy. Emission is observed from low to room temperature with peaks ranging from 3.7 to 4.6 μm. The bandgap as function of temperature is determined from the first derivative maxima of the spectra fit to an Einstein single oscillator model. The photoluminescence spectra is observed to significantly broaden with Bi content as a result of lateral composition variations and the highly mismatched nature of Bi atoms, pairs, and clusters in the group-V sublattice.
A bowing model is developed for the bandgap and band offsets of the quinary alloy GaInAsSbBi and its quaternary constituents InAsSbBi and GaAsSbBi. The band anticrossing interaction due to the highly mismatched Bi atoms is incorporated into the relevant bowing terms. An algorithm is developed for the design of mid infrared GaInAsSbBi
quantum wells, with three degrees freedom to independently tune transition energy, in plane strain, and band edge offsets for desired electron and hole confinement.
The physical characteristics of the fundamental absorption edge of the relevant III-V binaries GaAs, GaSb, InAs, and InSb are examined using spectroscopic ellipsometry. A five parameter model is developed that describes the key physical characteristics of the absorption edge, including the bandgap energy, the Urbach tail, and the absorption coefficient at the bandgap.
The quantum efficiency and recombination lifetimes of bulk InAs0.911Sb0.089 grown by molecular beam epitaxy is investigated using excitation and temperature dependent steady state photoluminescence. The Shockley-Read-Hall, radiative, and Auger recombination lifetimes are determined.

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  • 2020

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Towards high-efficiency thin-film solar cells: from theoretical analysis to experimental exploration

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GaAs single-junction solar cells have been studied extensively in recent years, and have reached over 28 % efficiency. Further improvement requires an optically thick but physically thin absorber to provide

GaAs single-junction solar cells have been studied extensively in recent years, and have reached over 28 % efficiency. Further improvement requires an optically thick but physically thin absorber to provide both large short-circuit current and high open-circuit voltage. By detailed simulation, it is concluded that ultra-thin GaAs cells with hundreds of nanometers thickness and reflective back scattering can potentially offer efficiencies greater than 30 %. The 300 nm GaAs solar cell with AlInP/Au reflective back scattering is carefully designed and demonstrates an efficiency of 19.1 %. The device performance is analyzed using the semi-analytical model with Phong distribution implemented to account for non-Lambertian scattering. A Phong exponent m of ~12, a non-radiative lifetime of 130 ns, and a specific series resistivity of 1.2 Ω·cm2 are determined.

Thin-film CdTe solar cells have also attracted lots of attention due to the continuous improvements in their device performance. To address the issue of the lower efficiency record compared to detailed-balance limit, the single-crystalline Cd(Zn)Te/MgCdTe double heterostructures (DH) grown on InSb (100) substrates by molecular beam epitaxy (MBE) are carefully studied. The Cd0.9946Zn0.0054Te alloy lattice-matched to InSb has been demonstrated with a carrier lifetime of 0.34 µs observed in a 3 µm thick Cd0.9946Zn0.0054Te/MgCdTe DH sample. The substantial improvement of lifetime is due to the reduction in misfit dislocation density. The recombination lifetime and interface recombination velocity (IRV) of CdTe/MgxCd1-xTe DHs are investigated. The IRV is found to be dependent on both the MgCdTe barrier height and width due to the thermionic emission and tunneling processes. A record-long carrier lifetime of 2.7 µs and a record-low IRV of close to zero have been confirmed experimentally.

The MgCdTe/Si tandem solar cell is proposed to address the issue of high manufacturing costs and poor performance of thin-film solar cells. The MBE grown MgxCd1-xTe/MgyCd1-yTe DHs have demonstrated the required bandgap energy of 1.7 eV, a carrier lifetime of 11 ns, and an effective IRV of (1.869 ± 0.007) × 103 cm/s. The large IRV is attributed to thermionic-emission induced interface recombination. These understandings can be applied to fabricating the high-efficiency low-cost MgCdTe/Si tandem solar cell.

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  • 2015

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Structural and optical properties of molecular beam epitaxy grown inAsBi bulk layers and quantum wells

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InAsBi is a narrow direct gap III-V semiconductor that has recently attracted considerable attention because its bandgap is tunable over a wide range of mid- and long-wave infrared wavelengths for

InAsBi is a narrow direct gap III-V semiconductor that has recently attracted considerable attention because its bandgap is tunable over a wide range of mid- and long-wave infrared wavelengths for optoelectronic applications. Furthermore, InAsBi can be integrated with other III-V materials and is potentially an alternative to commercial II-VI photodetector materials such as HgCdTe.

Several 1 μm thick, nearly lattice-matched InAsBi layers grown on GaSb are examined using Rutherford backscattering spectrometry and X-ray diffraction. Random Rutherford backscattering measurements indicate that the average Bi mole fraction ranges from 0.0503 to 0.0645 for the sample set, and ion channeling measurements indicate that the Bi atoms are substitutional. The X-ray diffraction measurements show a diffraction sideband near the main (004) diffraction peak, indicating that the Bi mole fraction is not laterally uniform in the layer. The average out of plane tetragonal distortion is determined by modeling the main and sideband diffraction peaks, from which the average unstrained lattice constant of each sample is determined. By comparing the Bi mole fraction measured by random Rutherford backscattering with the InAsBi lattice constant for the sample set, the lattice constant of zinc blende InBi is determined to be 6.6107 Å.

Several InAsBi quantum wells tensilely strained to the GaSb lattice constant with dilute quantities of Bi are characterized using photoluminescence spectroscopy. Investigation of the integrated intensity as a function of carrier excitation density spanning 5×1025 to 5×1026 cm-3 s-1 indicates radiative dominated recombination and high quantum efficiency over the 12 to 250 K temperature range. The bandgap of InAsBi is ascertained from the photoluminescence spectra and parameterized as a function of temperature using the Einstein single oscillator model. The dilute Bi mole fraction of the InAsBi quantum wells is determined by comparing the measured bandgap energy to that predicted by the valence band anticrossing model. The Bi mole fraction determined by photoluminescence agrees reasonably well with that estimated using secondary ion mass spectrometry.

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  • 2016

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Monolithic Heterovalent Integration of Compound Semiconductors and Their Applications

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Compound semiconductors tend to be more ionic if the cations and anions are further apart in atomic columns, such as II-VI compared to III-V compounds, due in part to the

Compound semiconductors tend to be more ionic if the cations and anions are further apart in atomic columns, such as II-VI compared to III-V compounds, due in part to the greater electronegativity difference between group-II and group-VI atoms. As the electronegativity between the atoms increases, the materials tend to have more insulator-like properties, including higher energy band gaps and lower indices of refraction. This enables significant differences in the optical and electronic properties between III-V, II-VI, and IV-VI semiconductors. Many of these binary compounds have similar lattice constants and therefore can be grown epitaxially on top of each other to create monolithic heterovalent and heterocrystalline heterostructures with optical and electronic properties unachievable in conventional isovalent heterostructures.

Due to the difference in vapor pressures and ideal growth temperatures between the different materials, precise growth methods are required to optimize the structural and optical properties of the heterovalent heterostructures. The high growth temperatures of the III-V materials can damage the II-VI barrier layers, and therefore a compromise must be found for the growth of high-quality III-V and II-VI layers in the same heterostructure. In addition, precise control of the interface termination has been shown to play a significant role in the crystal quality of the different layers in the structure. For non-polar orientations, elemental fluxes of group-II and group-V atoms consistently help to lower the stacking fault and dislocation density in the II-VI/III-V heterovalent heterostructures.

This dissertation examines the epitaxial growth of heterovalent and heterocrystalline heterostructures lattice-matched to GaAs, GaSb, and InSb substrates in a single-chamber growth system. The optimal growth conditions to achieve alternating layers of III-V, II-VI, and IV-VI semiconductors have been investigated using temperature ramps, migration-enhanced epitaxy, and elemental fluxes at the interface. GaSb/ZnTe distributed Bragg reflectors grown in this study significantly outperform similar isovalent GaSb-based reflectors and show great promise for mid-infrared applications. Also, carrier confinement in GaAs/ZnSe quantum wells was achieved with a low-temperature growth technique for GaAs on ZnSe. Additionally, nearly lattice-matched heterocrystalline PbTe/CdTe/InSb heterostructures with strong infrared photoluminescence were demonstrated, along with virtual (211) CdZnTe/InSb substrates with extremely low defect densities for long-wavelength optoelectronic applications.

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  • 2019

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Growth, optical properties, and optimization of infrared optoelectronic materials

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High-performance III-V semiconductors based on ternary alloys and superlattice systems are fabricated, studied, and compared for infrared optoelectronic applications. InAsBi is a ternary alloy near the GaSb lattice constant

High-performance III-V semiconductors based on ternary alloys and superlattice systems are fabricated, studied, and compared for infrared optoelectronic applications. InAsBi is a ternary alloy near the GaSb lattice constant that is not as thoroughly investigated as other III-V alloys and that is challenging to produce as Bi has a tendency to surface segregate and form droplets during growth rather than incorporate. A growth window is identified within which high-quality droplet-free bulk InAsBi is produced and Bi mole fractions up to 6.4% are obtained. Photoluminescence with high internal quantum efficiency is observed from InAs/InAsBi quantum wells. The high structural and optical quality of the InAsBi materials examined demonstrates that bulk, quantum well, and superlattice structures utilizing InAsBi are an important design option for efficient infrared coverage.

Another important infrared material system is InAsSb and the strain-balanced InAs/InAsSb superlattice on GaSb. Detailed examination of X-ray diffraction, photoluminescence, and spectroscopic ellipsometry data provides the temperature and composition dependent bandgap of bulk InAsSb. The unintentional incorporation of approximately 1% Sb into the InAs layers of the superlattice is measured and found to significantly impact the analysis of the InAs/InAsSb band alignment. In the analysis of the absorption spectra, the ground state absorption coefficient and transition strength of the superlattice are proportional to the square of the electron-hole wavefunction overlap; wavefunction overlap is therefore a major design parameter in terms of optimizing absorption in these materials. Furthermore in addition to improvements through design optimization, the optical quality of the materials studied is found to be positively enhanced with the use of Bi as a surfactant during molecular beam epitaxy growth.

A software tool is developed that calculates and optimizes the miniband structure of semiconductor superlattices, including bismide-based designs. The software has the capability to limit results to designs that can be produced with high structural and optical quality, and optimized designs in terms of maximizing absorption are identified for several infrared superlattice systems at the GaSb lattice constant. The accuracy of the software predictions are tested with the design and growth of an optimized mid-wave infrared InAs/InAsSb superlattice which exhibits superior optical and absorption properties.

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  • 2016