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The hygroscopic dopants used in Spiro‐OMeTAD hole transport material (HTM) in state‐of‐the‐art perovskite solar cells (PSCs) inevitably induce premature degradation of the devices. Here, two multifunctional polymer interface materials based on the perylene diimides (PDI) unit are developed. It is found that quasi‐two‐dimensional (2D) polymer 2DP‐PDI can form a denser film and exhibit better hydrophobicity...
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