| Summary: | Semiconductor quantum dots (also referred to as 'nanocrystals‘) are well suited as light-harvesting agents in solar cells because they are robust, have tuneable effective band gaps, and are easy to process. The research presented in this thesis is targeted towards the study of excitonic solar cells employing semiconductor nanocrystals as a light harvesting component. Gaining control of the interfacial charge transfer processes in operation in these devices forms a crucial part of any attempt to optimise their performance. In particular, the use of transient spectroscopic techniques reveals how efficient and long-lived charge separation can be achieved in these solar cell architectures. The primary focus of this research is to investigate the parameters influencing charge transfer in dye-sensitised solar cells (DSSCs) using colloidal quantum dots as light-absorbers. One aim is to study the impact of varying the thermodynamic driving forces provided for interfacial electron transfer on the yield of both the electron injection and hole regeneration reactions occurring within the DSSC; this can be achieved by varying the energetics of each component of the system (metal oxide, quantum dot and hole conductor) in turn. In addition, the interfacial morphology can be modulated by changing the passivating ligands present at the QD surface, and by modifying the structure of the redox mediator (or hole conductor). In doing so, we also attempt to improve our understanding of how charge carrier trapping in quantum dots impacts upon solar cell performance. Furthermore, new strategies towards solar cell design are presented, which show great potential as a result of their favourable photophysical properties. One of these approaches (presented in the final chapter) is to effect the in situ growth of CdS nanocrystals in a conducting polymer, a method which circumvents many of the processing issues associated with the use of nanocrystals in polymer blend solar cell architectures. It is hoped that the work presented in this thesis is used to develop design rules for the construction of semiconductor nanocrystal-based excitonic solar cells. By identifying which key parameters control the rates and yields of electron transfer at the nanocrystal interface, improvements in device efficiency can be realised. It is believed that these studies fill an important gap in our current understanding, and highlight some of the potential benefits and shortcomings of using semiconductor nanocrystals in cheap, solution-processed solar cells.
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