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Converting non‐visual light into photocurrent while maintaining high visual transparency is vital for semitransparent organic solar cells (ST‐OSCs) application, yet often challenging over insufficient invisible light‐harvesting. Herein, spectrally selective optical manipulation for ST‐OSCs with high visual light transparency and full‐spectral non‐visual light reflection is proposed by matching the optical admittance of ultrathin Ag films using ZnS and MgF2. The reflection of optically enhanced ST‐OSCs at the spectral region beyond the human eye's response spectrum is improved and the transmission in the visual region is simultaneously enhanced. By further integrating an anti‐reflective structure, the optimal structure boosts the average visible transmittance and power conversion efficiency of ST‐OSCs to 44.3% and 12.6%, respectively, yielding a record light utilization efficiency of 5.6%. Corresponding flexible ST‐OSCs with high mechanical stability implies that this work provides a facile and universal strategy for ST‐OSCs aiming at building integrated photovoltaics. [ABSTRACT FROM AUTHOR]

Photodiode‐type solar‐blind photodetectors (SBPDs) with the self‐powered feature hold great promise for applications in unattended secure communication, flame detection, and missile warning. However, the responsivity of SBPDs is usually limited due to the severe solar‐blind (SB) light extinction in substrates and charge transport layers. Herein, a spectrally selective hole extraction structure (SHE) is proposed for high‐efficiency perovskite SBPDs. The SHE consisting of a tandem Fabry–Perot cavity and energy‐level‐matched hole transport layer endows the device with narrowband absorption in the SB region and optimized charge extraction capability from the CsPbI2Br perovskite. The optimized SHE exhibits a peak transmittance of 27% at 255 nm and a half maximum at full width of 28 nm. Under SB light illumination, the champion device achieves a responsivity of 56.20 mA W−1 and a detectivity (D*) of 2.86 × 1013 Jones, which are the record values among the reported results. The approach demonstrated here paves the way for the optical and electrical design of perovskite photodetectors with spectrally selective detection. [ABSTRACT FROM AUTHOR]