Nanostructured Inorganic Metal Halide Perovskites for Optoelectronic Applications

Abstract

<p>Semiconductor quantumdots have proven to be promising materials for optoelectronic devices, such as light emitting devices (LEDs) and solar cells, due to their thin linewidth of emission, high photoluminescence quantum yield and high absorption coefficient. Over the last decade, perovskite crystals have gained significant attention due to their extraordinary optoelectronic properties. Therefore, perovskite nanocrystals combine the advantage of both crystalline perovskite and quantum dots. Here, we synthesised high quantum yield (50 - 80 %) monodispersed CsPbX₃ (X= Cl, Br, I) quantum dots, with tuneable emission spectra over the entire visible region, by a colloidal synthesis method. We have then successfully processed them to produce thin films as the emitting layer in an organic LED-type device architecture. Most importantly, we demonstrated field induced halide separation in mixed halide CsPb(Br/I)₃ NCs which is the reason color instability in these LEDs. Perovskite nanocrystal LEDs were found to have low external quantum efficiency (EQE) due to their bulky ligands. As a result, Ruddlesden-Popper (RP) phase layered perovskite was investigated to increase the EQE over perovskite QD LEDs. As a result, we constructed RP perovskite phase CsPbX₃ LEDs with emission through the entire visible spectrum (460-700 nm). Colour tuning was achieved by taking advantage of both quantum confinement effect and halide mixing. The EQE of these LEDs outperformed the literature values in the blue and blue-green spectral regions, with relatively long life time. We also invented a novel perovskite nanocrystals made from thalliumlead halide by replacing caesium with thallium. These materials are potential candidates for various optoelectronic applications. Size-, shape-, and composition- tuning in these nanocrystals were performed by varying the reaction conditions andmixing the halide composition. A weak confinementwas observed in these NCs. Additionally, we have shown the application of TlPbI₃ nanowires as photoconductors. Collectively, this thesis includes the synthesis of various types of inorganic metal halide perovskite nanostructures followed by their implementation into working optoelectronic devices, specifically LEDs.</p>