Title: Designing Quantum Dot Architectures and Surfaces for Light Emitting Diodes
Description: Quantum Dots (QD) have become a commercial reality for tunable displays and light-emitting diodes. The Department of Energy believes further improvements in efficacy and stability will allow for widespread adoption of solid-state lighting in the United States. QD geometric and compositional architecture, crystal phase and surface chemistry are arguably some of the important aspects governing QD performance in these applications. Chapter I outlines the efforts of QD design, encapsulation and performance for phosphor converted, “on-chip” LEDs. Cadmium chalcogenide QDs with a quantum well geometry and ZnS encapsulation (CdS/CdSxSe1-x/CdS/ZnS) resist photoluminescence bleaching on chip under harsh accelerated ageing tests. Trends in device performance are linked primarily to success of ZnS passivation. Chapter II presents findings regarding crystal structure control (Zinc Blende vs Wurtzite) for CdX (X = S, Se) systems by focusing on crystal phase conversion. The ZB to W transition for CdX is shown to be size, material and surfactant dependent.

Chapter III focuses on expanding the precursor compound library for CdSe with aryl substituted cyclic selenones (imidazole and pyrimidine-based compounds). These molecules are shown to react sluggishly at ZB synthetic conditions and that the rate is heavily influenced by compound sterics. Chapter IV presents the findings of a metal carboxylate displacement study on PbS NCs with various L-type ligands. Upon displacement and purification with N,N,N′,N′-tetramethylethylene-1,2-diamine, tri-n-butylamine, and n-octylamine, oriented attachment occurs along the 100 plane and with bis(dimethylphosphino)ethane and tri-n-butylphosphine, attachment is suppressed. This difference allows for the study of ligand density dependent optical properties without the confounding attachment of nanocrystals in solution. A decreasing trend of time resolved photoluminescence lifetime values as a function of ligand density is observed.