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Summary In this work, we propose a homoleptic ruthenium(II) complex, [Ru(dabpy)3]Cl2 (RDAB3) containing amine functionalized electron donating anchoring units for DSSCs. The DSSCs were co‐sensitized by coumarin‐based thiophene (CT) and indole (CI) units. The presence of four ancillary amine groups in RDAB3 influences its photovoltaic performance and the introduction of coumarin‐based co‐sensitizers significantly enhances the efficiency. The fabricated DSSCs were explored by UV‐Visible absorption, photocurrent‐voltage assessments, and impedance spectral studies. Co‐sensitized DSSCs showed an improved photovoltaic efficiency than the device sensitized by RDAB3 alone. Under optimized condition, the device made up of RDAB3+CI exhibited a high Jsc = 9.9 mA/cm2 with Voc of 0.7 V, fill factor of 0.773, and solar to power conversion efficiency of 5.35% in standard global AM 1.5 solar irradiation. This performance is found to be higher than the DSSC sensitized with RDAB3 (η = 3.84%) fabricated under same circumstances.

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