This project is concerned with both the study of different Multiple Quantum Wells (MQWs) structures using the In0.53Ga0.47As/In0.52Al0.48As material system lattice matched to InP and a systematic investigation of the properties of InAs QD systems within GaAs with the aim of achieving enhancements of solar cell performance. The key challenge is the growth of QDs solar cell structures which exhibit sufficient absorption (enhanced infrared absorption) to increase short circuit current density (Jsc) but which can still maintains a high open circuit voltage (Voc). The research consists of epitaxial growth using state-of–the-art MBE, optical absorption, photoluminescence and high resolution x-ray diffraction measurements as well as device fabrication and characterization of novel solar cell structures. Optimization was performed on these novel cells to further improve their efficiency by inserting stacks of QD into different regions of the device. The effect of localized doping of such structures was used in an attempt to maintain and enhance the open-circuit voltage which in turn increases the device efficiency. The fabricated devices were characterized using measurements of the dark/light current-voltage (I-V) characteristics and spectral response (50-480 K). Solar cell external quantum efficiencies under standard air mass (AM) 1.5 spectrum were determined and the suitability of these new cells under solar concentration were assessed. Full physical simulations are performed using SILVACO semiconductors modelling software to generate models of multi-junction solar cells that were crucial in informing iterations to growth and fabrication and help to reconcile theory with experiment. One of the key findings, of this thesis, is the fact that Intermediate band photovoltaic devices using material based on InAs/GaAs vertically stacked quantum dot arrays, can be used in applications according to specific configuration criteria such as high temperature operation conditions. The intermediate band cell, including an inter-dot doped configuration, has been found to be a potential candidate as the inter dot doping profile reduces the efficiency degradation below the GaAs values including an enhancement in the open circuit voltage. It has been proved that these devices not only have a good performance at high temperatures but also by changing the vertical stacking QD layer periodicity can enhance the short circuit current density while keeping a large open circuit voltage. It was confirmed in practical device operation that thermal energy is required to enable the intermediate band in InAs/GaAs QD materials. The impact of this works can help in the future improvements of the intermediate band solar cells based on InAs on GaAs QD. The best overall efficiency of 11.6 % obtained in this work is an excellent value for so simple devices configuration. The Si3N4, tested for the first time on InAs/GaAs QD materials, reduces the reflectance on the device surface to a value of 2% and the operational wavelength can be tuned by controlling the layer thickness. A 100 nm Si3N4 antireflective coating proved to be an excellent coating from 700 to 1000 nm. In terms of short circuit current density a 37% enhancement was achieved.

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The deterministic generation and manipulation of quantum states has attracted much interest ever since the rise of quantum mechanics. Large-scale, distributed quantum states are the basis for novel applications such as quantum communication, quantum remote sensing, distributed quantum computing or quantum voting protocols. The necessary infrastructure will be provided by distributed quantum networks, allowing for quantum bit processing and storage at single nodes. Quantum states of light then allow for inter-node transmission of quantum information. Transmission losses in optical fibers may be overcome by quantum repeaters, the quantum equivalent of classical signal amplifiers. The fragility of quantum superposition states makes building such networks very challenging. Hybrid solutions combine the strengths of different physical systems: Efficient quantum memories can be realized using alkali atoms such as rubidium. Leading in the deterministic generation of single photons and polarization entangled photon pairs are semiconductor InAs/GaAs quantum dots grown by the Stranski-Krastanov method. Despite remarkable progress in the last twenty years, complex quantum optical protocols could not be realized due to low degree of entanglement, low brightness and broad wavelength distribution. In this work, an emerging family of epitaxially grown GaAs/AlGaAs quantum dots obtained by droplet etching and nanohole infilling is studied. Under pulsed resonant two-photon excitation, they emit single pairs of entangled photons with high purity and unprecedented degree of entanglement. Entanglement fidelities up to f = 0.94 are observed, which are only limited by the optical setup or a residual exciton fine structure. The samples exhibit a very narrow wavelength distribution at rubidium memory transitions. Strain tuning is applied via piezoelectric actuators to allow for reversible fine-tuning of the emission frequency. In a next step, active feedback is employed to stabilize the frequency of single photons emitted by two separate quantum dots to an atomic rubidium standard. The transmission of a rubidium-based Faraday filter serves as the error signal for frequency stabilization. A residual frequency deviation of < 30MHz is achieved, which is less than 1.5% of the quantum dot linewidth. Long-term stability is demonstrated by Hong-Ou-Mandel interference between photons from the two quantum dots. Their internal dephasing limits the expected visibility to V = 40%. For frequency-stabilized dots, V = (41 ± 5)% is observed as opposed to V = (31 ± 7)% for free-running emission. This technique reaches the maximally expected visibility for the given system and therefore facilitates quantum networks with indistinguishable photons from distributed sources. Based on the presented techniques and improved emission quality, pivotal quantum communication protocols can now be implemented with quantum dots, such as transferring entanglement between photon pairs. Embedding quantum dots in a dielectric antenna ensures a bright emission. For the first time, entanglement swapping between two pairs of photons emitted by a single quantum dot is realized. A joint Bell measurement heralds the successful generation of the Bell state Ψ+ with a fidelity of up to (0.81 ± 0.04). The state's nonlocal nature is confirmed by violating the CHSH-Bell inequality with S = (2.28 ± 0.13). The photon source is tuned into resonance with rubidium transitions, facilitating implementation of hybrid quantum repeaters. This work thus represents a major step forward for the application of semiconductor based entangled photon sources in real-world scenarios.

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Single self-assembled semiconductor quantum dots (QDs) are able to emit single-photons and entangled-photons pairs. They are therefore considered as potential candidate building blocks for quantum information processing (QIP) and communication. To exploit them fully, the ability to precisely control their optical properties is needed due to several reasons. For example, the stochastic nature of their growth ends up with only little probability of finding any two or more QDs emitting indistinguishable photons. These are required for two-photon quantum interference (partial Bell-state measurement), which lies at the heart of linear optics QIP. Also, most of the as-grown QDs do not fulfil the symmetries required for generation of entangled-photon pairs. Additionally, tuning is required to establish completely new systems, for example, 87Rb atomic-vapors based hybrid semiconductoratomic (HSA) interface or QDs with significant heavy-hole (HH)-light-hole (LH) mixings. The former paves a way towards quantum memories and the latter makes the optical control of hole spins much easier required for spin- based QIP. This work focuses on the optical properties of a new type of QDs optimized for HSA experiments and their broadband tuning using strain. It was created by integrating the membranes, containing QDs, onto relaxor-ferroelectric actuators and was quantified with a spatial resolution of ~1 µm by combining measurements of the µ-photoluminescence of the regions surrounding the QDs and dedicated modeling. The emission of a neutral exciton confined in a QD usually consists of two fine-structure-split lines which are linearly polarized along orthogonal directions. In our QDs we tune the emission energies as large as ~23meV and the fine-structure-splitting by more than 90 µeV. For the first time, we demonstrate that strain is able to tune the angle between the polarization direction of these two lines up to 40° due to increased strain-induced HH-LH mixings up to ~55%. Compared to other quantum emitters, QDs can be easily integrated into optoelectronic devices, which enable, for example, the generation of non-classical light under electrical injection. A novel method to create sub-micrometer sized current-channels to efficiently feed charge carriers into single QDs is presented in this thesis. It is based on focused-laserbeam assisted thermal diffusion of manganese interstitial ions from the top GaMnAs layer into the underlying layer of resonant tunneling diode structures. The combination of the two methods investigated in this thesis may lead to new QDbased devices, where direct laser writing is employed to preselect QDs by creating localized current-channels and strain is used to fine tune their optical properties to match the demanding requirements imposed by QIP concepts.

Recombination mechanisms in gallium arsenide have been studied using temperature-dependent time-resolved photoluminescence-decay. New analytical methods are presented to improve the accuracy in bulk lifetime measurement, and these have been used to resolve the temperature-dependent lifetime. Fits to temperature-dependent lifetime yield measurement of the radiative-efficiency, revealing that samples grown by the Czochralski and molecular-beam-epitaxy methods are limited by radiative-recombination at 77K, with defect-mediated nonradiative-recombination becoming competitive at 300K and above. In samples grown with both doping types using molecular-beam-epitaxy, a common exponential increase in capture cross-section characterized by a high value of E_infinity=(258 +/- 1)meV was observed from the high-level injection lifetime over a wide temperature range (300-700K). This common signature was also observed from 500-600K in the hole-lifetime observed in n-type Czochralski GaAs where E_infinity=(261 +/- 7)meV was measured, which indicates that this signature parametrizes the exponential increase in hole-capture cross-section. The high E_infinity value rules out all candidate defects except for EL2, by comparison with hole-capture cross-section data previously measured by others using deep-level transient spectroscopy. / Thesis / Doctor of Philosophy (PhD)

The absorptance in vertical nanowire (nw) arrays is typically dominated by three optical phenomena: radial mode resonances, near-field evanescent wave coupling, and Fabry–Perot (F-P) mode resonances. The contribution of these optical phenomena to GaAs, InP and InAs nw absorptance was simulated using the finite element method. The study compared the absorptance between finite and semi-infinite nws with varying geometrical parameters, including the nw diameter (D), array period (P), and nw length (L). Simulation results showed that the resonance peak wavelength of the HE1n radial modes linearly red-shifted with increasing D. The absorptance and spectral width of the resonance peaks increased as L increased, with an absorptance plateau for very long nws that depended on D and P. Near-field coupling between neighbouring nanowires (nws) was observed to increase with increasing diameter to period ratio (D/P). The effect of F-P modes was more pronounced for shorter nws and weakly coupled light. Based on the collective observation of the correlation between nw geometry and optical phenomena in GaAs, InP, and InAs nw arrays, a periodic array of vertical InSb nws was designed for photodetectors in the low-atmospheric absorption window (λ = 3-5 μm) within the mid-wavelength infrared (MWIR) spectrum (λ = 3-8 μm). Simulations, using the finite element method, were implemented to optimize the nw array geometrical parameters (D, P, and L) for high optical absorptance (~0.8), which exceeded that of a thin film of equal thickness. The results further showed that the HE1n resonance wavelengths in InSb nw arrays can be tuned by adjusting D and P, thus enabling multispectral absorption throughout the near infrared (NIR) to MWIR region. Optical absorptance was investigated for a practical photodetector consisting of a vertical InSb nw array embedded in bisbenzocyclobutene (BCB) as a support layer for an ultrathin Ni contact layer. Polarization sensitivity of the photodetector was examined. Lastly, how light flux enters the nw top and sidewalls on HE11 resonance was investigated. / Dissertation / Doctor of Philosophy (PhD)

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<p>III-V nanowire (NW) ensemble devices were fabricated using novel approaches to address key NW optoelectronic issues concerning electrical contacts, doping, surface effects and underlying electrostatics physics.</p> <p>NWs were first embedded in a filling medium, thus achieving low sheet resistance front contacts while preventing shunts. Various filling materials were assessed for porosity, surface roughness and thermal stability, giving Cyclotene as an ideal filing material. Sonication was also introduced as a novel method to achieve perfect planarization.</p> <p>The presence of the Cyclotene also enabled the NWs to be characterized precisely and easily by secondary ion mass spectrometry (SIMS) to give the NW dopant concentration with excellent spatial resolution. Additionally, SIMS characterization demonstrated the ability to characterize the height uniformity of individual segments in a heterostructure NW ensemble.</p> <p>The focus of the work shifted towards surface effects on NW device performance. Therefore, Poisson's equation was solved to provide a comprehensive model of NW surface depletion as a function of interface state density, NW radius and doping density. Underlying physics was examined where surface depletion was found to significantly reduce the conductivity of thin NWs, leading to carrier inversion for some.</p> <p>This model was then applied in conjunction with a transport model to fit current-voltage curves of an AlInP-passivated GaAs NW ensemble device. A 55% decrease in surface state density was achieved upon passivation, corresponding to an impressive four order of magnitude increase in the effective carrier concentration. Additionally, conventional and time-resolved photoluminescence measurements showed intensity and carrier lifetime improvement greater than 20x upon passivation.</p> <p>Finally, the model was extended to describe radial pn junction NWs with surface depletion to give radial energy band profiles for any arbitrary set of NW parameters. Specific cases were analyzed to extract pertinent underlying physics, while the built-in potential was optimized for the design for an optimal device.</p> / Doctor of Philosophy (PhD)