Ion-migration-induced dual interface dipoles for high-performance perovskite solar cells
Low exciton binding energy and well-aligned energy levels are crucial for achieving efficient perovskite solar cells (PSCs). Here, we introduce pyridinium tetrafluoroborate (PyHBF 4 ) into the perovskite layer to regulate the interfaces between the perovskite and the charge transport layers effectively. This results in dual interface dipoles due to the migration of BF 4 − , which accelerates the separation of hole-electron pairs and the extraction of carriers. Ab initio and DFT calculations, combined with various experimental characterizations, reveal that the thermodynamically favored combination of PyH + and I − causes BF 4 − to separate from the PyH + cation and migrate downward along the Pb-I framework within the perovskite layer. In addition, the formation of the secondary compound PyHI on the top surface enhances cation-π interaction with Spiro-OMeTAD and increases the hydrophobicity of the perovskite film. Consequently, the PyHBF 4 -treated PSCs achieve a champion efficiency of 24.93%, along with improved thermal, humidity, and operational stability.
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