Physics and engineering of organic solar cells
Potscavage, William J., Jr.
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Organic solar cells have the potential to be portable power sources that are light-weight, flexible, and inexpensive. However, the highest power conversion efficiency for organic solar cells to date is ~8%, and most high-efficiency solar cells have an area of less than 1 cm². This thesis advances the field of organic solar cells by studying the physics and engineering of the devices to understand the reverse saturation current, which is related to efficiency, and the effects of area scaling. The most commonly accepted models to describe the physics of organic photovoltaic devices are reviewed and applied to planar heterojunction solar cells based on pentacene / C60 as a model system. The equivalent circuit model developed for inorganic solar cells is shown to work well to describe the behavior of organic devices and parameterize their current-voltage characteristics with five parameters. Changes in the parameters with different material combinations or device structures are analyzed to better understand the operation of the presented organic solar cells. A one-dimensional diffusion model for the behavior of excitons and treatment of the organic layers as planes is demonstrated to adequately model the external quantum efficiency and photocurrent in pentacene / C60 solar cells. The origin of the open-circuit voltage is studied using cells with different electrodes and different donor materials. While changing the electrodes does not affect open-circuit voltage, it is greatly modified by changes in the donor. Tests with additional semiconductors show the change in open-circuit voltage is not consistent from donor to donor as the acceptor is varied, suggesting a more complex relation than just the difference in energy levels. Study of the temperature dependence of the equivalent circuit parameters shows that the reverse saturation current, which has a significant role in determining the open-circuit voltage, has a thermally activated behavior. From this behavior, the reverse saturation current is related back to charge transfer at the donor / acceptor heterojunction to suggest that both the effective energy barrier presented by the energy levels and the electronic coupling are important in determining the reverse saturation current and open-circuit voltage. This marks a shift from just considering a built-in voltage or the energy levels to also considering the electronic coupling of the donor and acceptor materials. Temperature-dependent performance characteristics are also used to show key differences between organic and inorganic devices. Finally, the effect of area scaling is explored with pentacene / C60 solar cells having areas of 0.11, 7, and 36.4 cm². Analysis with the equivalent circuit model shows that performance decreases as area increases because of an increasing series resistance presented by the transparent electrode. A metal grid, to provide low resistance pathways for current, fabricated on top of the transparent electrode is proposed to reduce the effective resistance. The grid is unique in that it is placed between the electrode and the semiconductor layer and must be passivated to prevent shorts through the thin semiconductor to the back metal electrode. Analysis of the grid predicts greatly reduced series resistance, and experimental results show reduced resistance and improved performance for the 7 cm² and 36.4 cm² devices when including the grid.