|Institution:||University of Cambridge|
|Keywords:||Nanocrystals; Multiple excition generaion; Perovskite Nanocrystals; LEDs; PV; LSCs|
|Full text PDF:||https://www.repository.cam.ac.uk/handle/1810/263670|
The application and efficiency of optoelectronic devices depends on the ability to control the absorption and emission processes of photons in semiconductors. This thesis looks at three different applications of spectral management across a broad range of optoelectronic devices: photovoltaics (PVs), luminescent solar concentrators (LSCs) and light-emitting diodes (LEDs).Multiple excitation generation (MEG) a process in which multiple charge-carrier pairs are generated from a single optical excitation - is a promising way to improve the photocurrent in photovoltaic devices and offers the potential to break the Shockley-Queisser limit. Here we present solar cells fabricated from PbSe nanorods which show external quantum efficiencies exceeding 100 %. This demonstrates the potential for substantial improvements in PV device performance due to MEG.Through spatial and spectral concentration, LSCs have the potential to reduce the cost of photovoltaic energy production and are attractive prospects for photobioreactors and building-integrated applications. Here we introduce versatile star-shaped donor-acceptor molecules based on a central BODIPY acceptor with oligofluorene donor side units. We perform comprehensive device measurements and Monte Carlo ray tracing simulations of LSCs. We find that the measured structures permit waveguide propagation lengths on a par with state-of-the-art nanocrystalline emitters, while proposed hypothetical structures can be seen as viable candidates for photobioreactor and energy production roles and should be synthesized.The efficiency of nanocrystal-based LEDs is inherently limited by the types of crystals used. Cesium lead halide perovskite nanocrystals exhibit photoluminescence quantum efficiencies approaching 100%. However, due to the large surface areas and anion mobility halogen exchange between perovskite nanocrystals of different compositions occurs rapidly, limiting applications. Here, we report significantly reduced halide exchange between chloride and iodide CsPbX3 (X= Cl, I) perovskite nanocrystals. We investigate perovskite-based multi-crystal component samples and their resulting optical and electrical interactions in bulk heterojunction LEDs. Efficient photon reabsorption from CsPbCl3 to CsPbI3 nanocrystals was found to improve LED device performance.