This dissertation computationally and analytically investigates ways to model solar cells when the lateral motion of charge carriers and light are relevant. We focus on back-contact perovskite solar cells, and assessing the experimental technique of scanning photocurrent microscopy as a means to investigate them. Solar cells are three-dimensional objects frequently modelled as being one-dimensional. However, for more complex designs of solar cell or if the cell is only point-illuminated, one-dimensional modelling is insufficient. In the first study, some conditions for reducing the complexity of two-dimensional drift-diffusion simulations are investigated for a back-contact perovskite cell. Analytic expressions for the relationship in both the low extraction velocity and high extraction velocity regimes are demonstrated, and the conditions where these approximations break down are investigated. These findings are then applied a point-excited film with an extended electrode, a problem encountered during scanning photocurrent microscopy. We show the current recorded in this case should decay exponentially with the distance between excitation and electrode, with a decay constant that can be related to device parameters. The characteristic equilibration time for the system to reach this current is demonstrated to increase linearly with distance. Between this gradient and the exponent, information about the diffusion and recombination mechanics can be extracted from a variety of systems. Photon recycling is the process in whereby photogenerated carriers recombine to generate light that is absorbed again within the solar cell. In the second section, we apply the findings of the first section to show that experimental results published elsewhere are best explained by photon recycling in methylammonium lead iodide perovskite back-contact solar cells. However we do not have an established theoretical model for long-ranged lateral optical transport in these solar cells. Three models are developed: a bimolecular model for unscattered, coherent transport; a photon diffusion model for frequently scattered, noncoherent light; and a monomolecular, assisted-diffusion model. The modal nature of coherent optical transport is considered and modifications to previous one-dimensional theories are made. The nature of the photon diffusion model is discussed, as are theoretical shortcomings. All three models are then solved numerically and compared to experimental results. The low-scattering photon diffusion models correspond well to the experiment. The third investigation involves the performance of different architectures of back-contact perovskite cells. These cells potentially offer increased current due to less shadowing by front electrodes. We compare them to each other and to traditional vertical structures. It is found that, in terms of internal transport, the back-contact solar cells give less efficient performance than the vertical design. The best of the back-contact cells investigated is a flat interdigitated design. The increase in efficiency from optical factors would have to exceed 10% for the overall efficiency of back-contact cells to be higher than vertical devices. We also develop a model of photon recycling appropriate for short-ranged, bulk 2D transport and demonstrate that in perovskites, it produces little change in power conversion efficiency (and small changes in short-circuit voltage) when compared with the standard drift-diffusion equations with the second-order recombination constant is adjusted.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:744279 |
| Date | January 2017 |
| Creators | Lamboll, Robin Davies |
| Contributors | Greenham, Neil C. |
| Publisher | University of Cambridge |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | https://www.repository.cam.ac.uk/handle/1810/268518 |
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