Intrinsic chiroptical responsivity in self‐powered organic photodiodes for polarization‐tunable optical convolution

Abstract The intrinsic chiroptical properties of organic semiconductors provide a powerful platform for polarization‐encoded optoelectronic signal processing. Here, we develop self‐powered chiral organic photodiodes (COPs) based on chiral non‐fullerene acceptors blended with achiral polymer donors, in which the circularly polarized light (CPL)‐dependent responsivity provides the physical foundation for tunable convolutional weighting. Owing to their polarization‐dependent photocurrent, mathematically formulated as the product of the CPL amplitude and a sine function of the retarder rotation angle, these COPs act as bias‐free, dynamically reconfigurable convolutional filters capable of robust feature extraction under noisy optical propagation conditions. This materials‐driven modulation mechanism enables effective contrast enhancement and noise suppression without external bias or additional circuit elements. When incorporated into an optical convolutional framework, CPL‐responsive COPs improve the structural similarity index measure of extracted feature maps from 0.15 to 0.80 and increase handwritten‐digit classification accuracy from 76% to 87% compared with natural‐light‐based counterparts. These results establish chiral organic photodiodes as a promising materials platform for low‐power, noise‐tolerant optical information processing. image