Browsing by Subject "Superlattice"
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Item Colloidal nanocrystal assemblies : self-organization, properties, and applications in photovoltaics(2011-12) Goodfellow, Brian William; Korgel, Brian Allan, 1969-; Chelikowsky, James R; Dodabalapur, Ananth; Ekerdt, John G; Vanden Bout, David AColloidal nanocrystal assemblies offer an attractive opportunity for designer metamaterials. The ability to permute chemical composition, size, shape, and arrangement of nanocrystals leads to an astounding number of unique materials properties that find use in an extensive array of applications---ranging from solar cells to medicine. However, to take full advantage of these materials in useful applications, the nature of their assembly and their behavior under external stimuli must be well understood. Additionally, the assembly of colloidal nanocrystals into thin films provides a promising pathway to the solution-processing of inorganic materials that are prohibitively too expensive and/or difficult to deposit by conventional methods. Nanocrystal superlattices (NCSLs) of sterically stabilized nanocrystals were assembled by slow evaporation of colloidal dispersions on various substrates. Detailed analysis of the NCSL structures was carried out using transmission and scanning electron microscopy (TEM and SEM) and small-angle x-ray scattering (SAXS). Body-centered cubic (bcc) NCSLs, in particular, were studied in detail and ligand packing frustration was proposed as a significant driving force for their assembly. The behavior of NCSLs was also studied by SAXS under mild heating and solvent vapor exposure revealing several remarkable order-order, order-disorder, and amorphous-crystalline structural transitions. Colloidal Cu(In [subscript 1-x] Ga [subscript x])Se₂ (CIGS) nanocrystals were synthesized by arrested precipitation and formulated into inks. These inks were spray deposited into thin films under ambient conditions to serve as the active light absorbing material in printed low-cost photovoltaic (PV) devices. These devices, which were fabricated without the need for high temperature processes, have achieved power conversion efficiencies above 3 % under AM1.5 illumination. While the efficiencies of these devices are still too low for commercial viability, this work does provide a proof of concept that reasonable efficient solar cells can be created with a low-cost printable process using nanocrystal inks. Since high temperatures are not used to form the light-absorbing layer, nanocrystal-based solar cells were built on flexible light weight plastic substrates. The main obstacle to achieving high power conversation efficiencies was found to be the ability to extract the photo induced charge carriers. Nanocrystal films suffer from poor transport that leads to high recombination rates in thicker films. To date, the best efficiencies have been achieved with thin light absorber layers that only absorb a fraction of the incident light.Item Emerging phenomena in oxide heterostructures(2010-08) Lee, Jaekwang; Demkov, Alexander A.; Kleinman, Leonard; Chelikowsky, James R.; Macdonald, Allan H.; Hwang, Gyeong S.Oxide interfaces have attracted considerable attention in recent years due to emerging novel properties that do not exist in the corresponding parent compounds. Furthermore, modern atomic-scale growth and probe techniques enable the formation and study of new artificial interface states distinct from the bulk state. A central issue in controlling the novel behavior in oxide heterostructures is to understand how various physical variables (spin, charge, lattice and/or orbital hybridization) interact with each other. In particular, density function theory (DFT) has provided significant insight into underlying physics of materials at the atomic level, giving quantitative results consistent with experiment. In this dissertation using density functional theory methods, we explore the electronic, magnetic and structural properties developed near the interface in SrTiO3/LaAlO3, EuO/LaAlO3, Fe/PbTiO3/Pt, Fe//BaTiO3/Pt and Cs/SrTiO3 heterostructures. We study the interplay between physical interactions, and quantify parameters that determine physical properties of hetetrostructures. These theoretical studies help understanding how physical variables couple with each other and how they determine new properties at oxide interfaces.