Symmetry-Breaking-Induced Polarization Sensitivity in PtS2/CrOCl van der Waals Heterostructures for High-Performance Photodetectors.

Photodetectors underpin optical imaging, communication, and emerging photonic technologies. However, most devices are limited to intensity detection and underutilize the polarization degree of freedom, which is vital for feature discrimination and high-density information encoding. Herein, we introduce symmetry breaking by integrating double rotational symmetry CrOCl with triple rotational symmetry PtS2 to construct a PtS2/CrOCl van der Waals heterostructure. The crystal symmetry contrast enhances interfacial anisotropic states, while localized holes in CrOCl and high-mobility electrons in PtS2 create intrinsic spatial charge separation that suppresses carrier recombination. Consequently, the device achieves a high responsivity of 25.9 A W-1 and an external quantum efficiency of 7942%. Benefiting from lattice-anisotropy-photon coupling, the PtS2/CrOCl heterostructure exhibits strong polarization sensitivity across a broad spectral range from 405 to 1064 nm, with an anisotropy ratio up to ∼8. This performance supports polarization-resolved single-pixel imaging and near-infrared polarized optical communication. Our results demonstrate that symmetry-breaking-induced anisotropy engineering provides a powerful strategy for high-performance, broadband, and polarization-sensitive photodetection, offering promising opportunities for next-generation photonic information technologies.