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Hole‐transporting materials (HTMs) play an important role in transporting photogenerated holes, tuning the perovskite crystallization process, and passivating uncoordinated Pb2+ defects for high‐performance inverted perovskite solar cells (PSCs). Herein, a unique cost‐effective small molecule‐type HTM based on a triarylamine core bearing a chloro‐assisted chelating moiety (named TPA‐CAA) is synthesized,...