Bias‐Switchable Dual‐Functional Ferroelectric Perovskite Optoelectronics Toward High‐Performance Photodetection and Neuromorphic Photonics

The performance of 2D ferroelectric perovskite optoelectronic devices is still severely limited by complex interfacial morphologies and intrinsic semiconducting characteristics, including large exciton binding energies. Here, we present a facile strategy to address these limitations simultaneously by sensitizing 2D ferroelectric perovskite EA 4 Pb 3 Br 10 films with the conjugated polymer poly(3‐hexylthiophene). This modification effectively optimizes carrier dynamics in the active layer by facilitating hot‐carrier transport, promoting efficient exciton dissociation, and prolonging carrier recombination. As a result, the device achieves a record self‐powered responsivity of 264.7 A W − 1 in ferroelectric perovskite photodetectors, representing a 10 4 ‑fold enhancement over the pristine counterpart. Concurrently, the device exhibits exceptional low‐power photonic synaptic plasticity under small applied biases and can be readily integrated into neural networks for high‐precision fingerprint identification, highlighting its considerable promise for low‐power neuromorphic computing applications. This work demonstrates the synergistic optimization of perovskite films through conjugated polymer sensitization, paving the way for the development of high‐performance 2D ferroelectric perovskite optoelectronics.