Colloidal nanocrystal assemblies : self-organization, properties, and applications in photovoltaics




Goodfellow, Brian William

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Colloidal 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.



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