Perovskite photovoltaics is one of the fastest growing opto-electronic technologies with device efficiencies currently exceeding 23%. The opportunity to deposit these abundant materials with large area solution processing techniques could make perovskites viable for low-cost production. However, since perovskite materials are prone to degradation, their lifetime needs to be improved to that of silicon solar cells before these devices can be commercialized. Moreover, unlike most semiconductors, trap densities in polycrystalline perovskite films in high-performing devices have been determined to be relatively large, suggesting a remarkable defect tolerance in perovskite films that needs to be understood in the context of the nature of the trap states and any residual non- radiative losses. These non-radiative losses are observed as photoluminescence heterogeneity within perovskite films, even for high-performing perovskite systems. In this work, we explore the degradation kinetics of perovskite devices under stress conditions and find that further stability improvements should focus on the mitigation of trap generation during ageing. Furthermore, we fabricate perovskite solar cells with a novel back-contact structure, in which electron- and hole-selective electrodes are co-positioned on the back side of the cell and spaced by 100 μm. By utilising grazing-incidence X-ray diffraction, we show that even in the earliest stages of conversion of precursors to perovskite we achieve remarkably high open-circuit voltages, suggesting that the defect tolerance of perovskites appears at an early stage in the conversion process. Moreover, we employ scanning X-ray diffraction with nanofocused beam and obtain detailed information, revealing overlapping grains located at different depths within perovskite films. We find that the critical grain size is the longer-range structural super-grains rather than the grains viewed with conventional microscopy techniques. These findings further highlight the presence of structural defects in perovskite materials and provide important insights towards improving the optoelectronic behaviour of these materials.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:767776 |
| Date | January 2019 |
| Creators | Alsari Almheiri, Mejd |
| Contributors | Friend, Richard |
| Publisher | University of Cambridge |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | https://www.repository.cam.ac.uk/handle/1810/288606 |
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