The power conversion efficiency (PCE) of Cs 2 AgBiBr 6 -based perovskite solar cells (PSCs) is still low owing to the inherent defects of Cs 2 AgBiBr 6 films. Herein, we demonstrate a carboxy-chlorophyll derivative (C-Chl)-sensitized mesoporous TiO 2 (m-TiO 2 ) film as an electron transport layer (ETL) to enhance and extend the absorption spectrum of Cs 2 AgBiBr 6 -based PSCs. The C-Chl-based device achieves a significantly improved PCE, exceeding 3% for the first time, with an increase of 27% in short-circuit current density. Optoelectronic investigations confirm that the introduction of C-Chl reduces the defects, accelerates the electron extraction, and suppresses charge recombination at the interface of ETL/perovskite. Moreover, the unencapsulated PSCs display restrained hysteresis and great stability under ambient conditions.
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