Optical and Electrical Modulation of Ferroelectric Polarization Enabling Photovoltaic Polarity Reconfiguration in WSe 2 Vertical Homojunction

Two‐dimensional ferroelectric transistors provide nonvolatile reconfigurability for intelligent information processing. However, dynamically reconfigurable photovoltaic polarity remains necessary for complex information processing. Here, we present a vertically stacked WSe 2 homojunction composed of multilayer and ferroelectric‐modulated few‐layer regions, in which the photovoltaic polarity reconfiguration can be realized effectively by gate voltage and light illumination. When the gate voltage induces ferroelectric switching, the bidirectional photoresponsivity can be continuously tuned from ‐0.82 to 0.92 A/W, enabling the real‐time dynamic vehicle recognition. Moreover, the 405 nm laser illumination‐induced ferroelectric switching enables photovoltaic polarity reversal, serving as a strategy for wavelength‐selective optical anti‐counterfeiting encryption. This work provides a new paradigm for multi‐mode programmable reconfigurable optoelectronic devices that integrate simultaneous intelligent information processing and data protection capabilities.