Tandem solar cells (TSC) have been introduced to better absorb the spectrum of sunlight and reduce optical loss. Among these, perovskite–organic tandem solar cells (P-OTSC) have emerged as a prominent topic over the last decade due to their complementary absorption spectrum. Additionally, incorporating diverse pigmented protein complexes in TSC fabrication is becoming more common. Natural chlorophyll-containing photosystems have garnered significant attention for their naturally solar-tuned absorption spectra. Photosystem I protein (PSI), is the most robust component of oxygenic photosynthesis and contains over 100 Chl a molecules/complex with two sharp absorbance peaks at 430 and 665 nm. PSI offers a second and complementary active layer because P-OTSCs often have a low extinction coefficient in the red wavelength region. In this research, the performance of P-OTSCs was enhanced by improving the absorption spectrum by utilizing an isolated plant PSI complex. The circuit current density (Jsc) increased from 14.23 mA/cm² to 14.95 mA/cm², and the power conversion efficiency (PCE) of P-OTSCs increased from 19.32 % to 20.24 %. We also observed that the external quantum efficiency (EQE) shows an apparent increase in the long wavelength region, reflecting the absorbance of light by PSI. This work is the first to report the integration of PSI into perovskite–organic tandem solar cells, and it motivates new design considerations that can further boost efficiency and utilize natural, earth-abundant pigment proteins.
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