Tailoring of a visible-light-absorbing biaxial ferroelectric towards broadband self-driven photodetection.

In terms of strong light-polarization coupling, ferroelectric materials with bulk photovoltaic effects afford a promising avenue for optoelectronic devices. However, due to severe polarization deterioration caused by leakage current of photoexcited carriers, most of ferroelectrics are merely capable of absorbing 8–20% of visible-light spectra. Ferroelectrics with the narrow bandgap (<2.0 eV) are still scarce, hindering their practical applications. Here, we present a lead-iodide hybrid biaxial ferroelectric, (isopentylammonium)2(ethylammonium)2Pb3I10, which shows large spontaneous polarization (~5.2 μC/cm2) and a narrow direct bandgap (~1.80 eV). Particularly, the symmetry breaking of 4/mmmFmm2 species results in its biaxial attributes, which has four equivalent polar directions. Accordingly, exceptional in-plane photovoltaic effects are exploited along the crystallographic [001] and [010] axes directions inside the crystallographic bc-plane. The coupling between ferroelectricity and photovoltaic effects endows great possibility toward self-driven photodetection. This study sheds light on future optoelectronic device applications. 2D lead-iodide ferroelectrics usually possess a wide bandgap along with the lacking of ferroelectric bulk photovoltaic effects due to the monolayered inorganic perovskite sheets. Here, the authors present a pathway to increase the thickness of inorganic sheets while retaining ferroelectricity.