UC Irvine

This thesis explores the understanding of the chemistry and physics of colloidal quantum dots for practical solar energy photoconversion. Solar cell devices that make use of PbS quantum dots generally rely on constant and unchanged optical properties such that band gap energies remain tuned within the device. The design and development of unique experiments to ascertain mechanisms of optical band gap shifts occurring in PbS quantum dot thin-films exposed to air are discussed. The systematic study of the absorption properties of PbS quantum dot films exposed to air, heat, and UV illumination as a function of quantum dot size has been described. A method to improve the air-stability of films with atomic layer deposition of alumina is demonstrated. Encapsulation of quantum dot films using a protective layer of alumina results in quantum dot solids that maintain tuned absorption for 1000 hours.

This thesis focuses on the use of atomic force microscopy and electrical variants thereof to study the physical and electrical characteristics of quantum dot arrays. These types of studies have broad implications in understanding charge transport mechanisms and solar cell device operation, with a particular emphasis on quantum dot transistors and solar cells. Imaging the channel potential of a PbSe quantum dot thin-film in a transistor showed a uniform distribution of charge coinciding with the transistor current voltage characteristics. In a second study, solar cell device operation of ZnO/PbS heterojunction solar cells was investigated by scanning active cross-sections with Kelvin probe microscopy as a function of applied bias, illumination and device architecture. This technique directly provides operating potential and electric field profiles to characterize drift and diffusion currents occurring in the device. SKPM established a field-free region occurring in the quantum dot layer, indicative of diffusion-limited transport. These results provide the path to optimization of future architectures that may employ drift-based transport in the quantum dot layer for enhanced charge extraction and power conversion efficiency.