Double Cascading Charge Transfer at Integrated Perovskite/Organic Bulk Heterojunctions for Extended Near‐Infrared Photoresponse and Enhanced Photocurrent

Abstract Nowadays, nearly 48.7% near‐infrared (NIR) irradiation (>800 nm) of the full solar spectrum has actually not been fully utilized since the state‐of‐the‐art perovskite film usually can only absorb the most UV–vis sunlight radiation. Herein, high efficiency integrated Cs_0.15FA_0.85PbI₃ perovskite/organic bulk (PC₆₁BM:D18:Y6) heterojunction solar cells with enhanced low energy photon harvest until 931 nm and a high maintained open circuit voltage of 1.04 V is successfully obtained. In particular, the favorable double cascading charge transfer paths pave an interesting possibility to spatially separate electrons upon visible light excitation and holes upon NIR photon absorption simultaneously at interfaces, significantly suppressing non‐radiative bimolecular recombination and reaching the photocurrent density as high as 27.48 mA cm⁻² and power conversion efficiency of 20.31%. Besides, the strong hydrophobicity of the ternary organic film has effectively prevented ambient humidity penetration and improves the stability of the perovskite in the continuous aging test (humidity > 60%) compared with the control device. This work has opened a significantly new window to improve the NIR light harvest for next generation highly efficient solar cells with full spectrum response.