Self‐Powered Visible‐Infrared Polarization Photodetection Driven by Ferroelectric Photovoltaic Effect in a Dion–Jacobson Hybrid Perovskite

Abstract Ferroelectric materials, particularly the emerging layered hybrid ferroelectrics, have shown great potential for high‐sensitive polarization photodetection owing to their striking bulk photovoltaic effect (BPVE). Despite recent great achievements, the linear photoresponse range based on single‐mode BPVE is still limited in the shortwave region due to the large intrinsic bandgaps. Herein, first, the realization of self‐powered visible–infrared polarization photodetection by exploiting dual‐modal BPVE in a newly developed layered Dion–Jacobson (D‐J) hybrid ferroelectric (BDA)(EA) 2 Pb 3 Br 10 (1, BDA is 1,4‐butadiammonium, EA is ethylammonium) is reported. Crystallographic investigations indicate that 1 adopts a typical trilayered D‐J perovskite structure with a fascinating ferroelectric feature and a giant two‐photon absorption coefficient as giant as 4.73 cm MW –1 . Meanwhile, the bulk single crystal device of 1 exhibits excellent self‐powered direct detection performance under both visible light (405 nm) and near‐infrared light (800 nm), with a current on/off ratio as high as 10 3 . More intriguingly, the device displays high sensitivity to the polarization of illuminated light, showing a considerable anisotropy up to 4.2 (405 nm) and 4.8 (800 nm), which are much larger than the detectors achieved by geometry anisotropy. The realization of self‐powered visible‐infrared dual‐modal polarization photodetection in 1 indicates the tremendous potential of hybrid ferroelectrics in various optoelectronic applications.