Deterministic control of the quantum properties of single indium arsenide artificial atoms with indium phosphide nanoscale architectures

This thesis presents optical spectra of single InAs quantum dots on InP with an unprecedented signal-to-noise ratio and spectral resolution that has facilitated comprehensive characterization and made a significant contribution to their understanding. InAs quantum dots on InP are the leading contenders for a variety of quantum electrooptic devices that require wavelengths in the 1.5 mum range, most notably triggered single/entangled photon sources for quantum key distribution. As of yet, spectroscopic data for InAs on InP has only provided proof of emission, but no high quality data has been available, preventing any conclusive understanding of their properties. The work presented in this thesis dramatically improves upon previous reports by key optimizations at each experimental stage: growth, processing, and optical setup. The spectra clearly resolve, for the first time, the structure within the s-shell and p-shell, with fine resolution, allowing quantitative evaluation of exciton complexes such as trions, biexcitons, and triplet states. By measuring numerous dots, the behavioral trends of these species with respect to dot geometry is deduced. Also, for the first time, magnetic-field dependent spectra are obtained for individual InAs/InP dots. A remarkable discovery was the strong relation of the exciton g-factor to dot height.This thesis also demonstrates deterministic nanometer-scale control of the quantum dot dimensions---with the goal being to exploit the structure/quantum property relation in these dots. This was accomplished by using the apex of an in-situ grown nanoscale InP pyramid as a nucleation site. The dimension of this top (001) surface on which the dot nucleates is responsive to manometer-scale changes in the pyramid base dimensions, which can be precisely controlled with lithography. The InAs grown on top of these mesas then conform to the size, where the available area can be purposely relaxed or constrained. For similar height, the resulting dots have diameters larger or smaller as compared to dots formed on planar substrates, ultimately allowing control of the aspect ratio. Control of lateral dot dimensions is corroborated by SEM images and also by magneto-optical spectra, thereby demonstrating deterministic control of the quantum properties.