Book Description

The last few years have seen rapid advances in nanoscience and nanotechnology, allowing unprecedented manipulation of nanostructures controlling solar energy capture, conversion, and storage. Quantum confined nanostructures, such as quantum wells (QWs) and quantum dots (QDs) have been projected as potential candidates for the implementation of some high efficiency photovoltaic device concepts, including the intermediate band solar cell (IBSC). In this dissertation research, we investigated multiple inter-related themes, with the main objective of providing a deeper understanding of the physical and optical properties of QD structures relevant to the IBSC concept. These themes are: (i) Quantum engineering and control of energy levels in QDs, via a detailed study of the electronic coupling in multilayer QD structures; (ii) Controlled synthesis of well-organized, good quality, high volume density, and uniform-size QD arrays, in order to maximize the absorption efficiency and to ensure the coupling between the dots and the formation of the minibands; and (iii) Characterization of carrier dynamics and development of techniques to enhance the charge transport and efficient light harvesting. A major issue in a QD-based IBSC is the occurrence of charge trapping, followed by recombination in the dots, which results in fewer carriers being collected and hence low quantum efficiency. In order to collect most of the light-generated carriers, long radiative lifetimes, higher mobilities, and a lower probability of non-radiative recombination events in the solar cell would be desirable. QD size-dependent radiative lifetime and electronic coupling in multilayer QD structures were studied using photoluminescence (PL) and time-resolved photoluminescence (TRPL). For the uncoupled QD structures with thick barriers between the adjacent QD layers, the radiative lifetime was found to increase with the QD size, which was attributed to increased oscillator strength in smaller size dots. On the other hand, in the sample with thin barrier and electronically coupled QDs, the radiative lifetime increases and later decreases with the dot size. This is due to the enhancement of the oscillator strength in the larger size, coherently coupled QDs. In order to improve the quality of multi-layer QD structures, strain compensated barriers were introduced between the QD layers grown on off-oriented GaAs (311)B substrate. The QD shape anisotropy resulted from the growth on off-oriented substrate was studied using polarization-dependent PL measurements both on the surface and the edge of the samples. The transverse electric mode of the edge-emitted PL showed about 5° deviation from the sample surface for the dots grown on (311)B GaAs, which was attributed to the tilted vertical alignment and the shape asymmetry of dots resulted from the substrate orientation. Significant structural quality improvements were attained by introducing strain compensated barriers, i.e., reduction of misfit dislocations and uniform dot size formation. Longer lifetime (~1 ns) and enhanced PL intensity at room temperature were obtained, compared to those in conventional multilayer (In, Ga)As/GaAs QD structures. A significant increase in the open circuit voltage (V oc) was observed for the solar cell devices fabricated with the strain compensated structures. A major issue in a QD IBSC is the occurrence of charge trapping, followed by recombination in the dots, which results in fewer carriers being collected, and hence low quantum efficiency. We proposed and studied a novel structure, in which InAs QDs were sandwiched between GaAsSb (12% Sb) strain-reducing layers (SRLs) with various thicknesses. Both short (~1 ns) and long (~4-6 ns) radiative lifetimes were measured in the dots and were attributed to type-I and type-II transitions, respectively, which were induced by the band alignment modifications at the QD/barrier interface in the structures analyzed, due to the quantum confinement effect resulting from different GaAsSb barrier thicknesses. Based on our findings, a structure with type-II QD/barrier interface with relatively long radiative recombination lifetime may be a viable candidate in designing IBSC.