Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
Publication date: 30th March 2023
Conventional computational approaches overestimate the charge-carrier mobilities in hybrid perovskites, meaning that the fundamental physics of charge transport in these materials is incompletely understood. Here, we show that much of the mobility overestimation is caused by the neglect of cation disorder. Hybrid perovskite crystals are not perfectly ordered because the organic cation can rotate inside the inorganic cage, and the resulting fluctuations in the orientation of the cation’s dipole moment result in a disordered energetic landscape for the carriers to navigate. We include these effects by carrying out supercell simulations of methylammonium lead iodide (MAPbI3), in which we include cation orientational disorder. We calculate the resulting polaron mobilities for both carriers (i.e., taking into account their coupling to the vibrations), showing that disorder increases their effective masses, causing a reduction of carrier mobilities. The effect is especially pronounced for electrons and explains the systematic overestimation of mobilities in previous work.
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International Conference on Hybrid and Organic Photovoltaics (HOPV) is celebrated yearly in May. The main topics are the development, function and modeling of materials and devices for hybrid and organic solar cells. The field is now dominated by perovskite solar cells but also other hybrid technologies, as organic solar cells, quantum dot solar cells, and dye-sensitized solar cells and their integration into devices for photoelectrochemical solar fuel production.
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