Tailoring chirality in van der Waals crystals for circular polarization encoded pattern recognition

Circular polarization possesses two orthogonal states that are analogous to the binary logic in digital communication systems, playing a crucial role in information encoding for optical perception and analysis. However, conventional detection of circular polarized light (CPL) and subsequent electrical communication depend on the interconnection of discrete chiroptical and electrical components, imposing significant limitations on the area efficiency and functional integration. Implementing CPL sensitivity (chirality) into optoelectronically active solid-state media with complementary metal-oxide-semiconductor (CMOS) compatibility has thus been a long-term goal, yet it remains elusive. Here, we report the fusion of chirality and optoelectronic activity in chiral molecules intercalated van der Waals crystals. The resultant highly ordered superlattices exhibit wavelength-dependent chiroptical-electrical behaviour, i.e. the band-specific circular dichroic (CD) features and preferential CPL photoresponse, enabling the transmission of richer information comparing to the wavelength-only encoding scheme. Moreover, the CPL distinguishability of the superlattices is evaluated using the second-harmonic generation (SHG) anisotropy factor g _SHG−CD , reaching up to 0.68 which is in the highest level comparing to other representative chiral systems. By employing the superlattices as dual-band circular polarization-selective photosensors, we achieve nearly two-fold enhancement in the pattern recognition accuracy from 50–93.6% through effectively perceiving the information encoded in the polarization dimension. Our work opens a reliable path to solid-state materials with tailored chiral-optoelectronic properties, offering a CMOS-compatible platform for concisely structured heterogeneous hardware.