Fast, Highly Stable, and Low-Bandgap 2D Halide Perovskite Photodetectors Based on Short-Chained Fluorinated Piperidinium as a Spacer

Ruddlesden–Popper (RP) two-dimensional (2D) halide perovskite (HP), with attractive structural and optoelectronic properties, has shown great potential in optoelectrical devices. However, the relatively wide bandgap (Eg) and stability, which cause inferior efficiency, prevent its feasibility from further applications. To tackle these issues, for the first time, a novel fluorine-containing piperidinium spacer, (3-HCF2CF2CH2OCH2-PPH+), abbreviated as (4FH-PPH+), has been designed for the stable and efficient n = 1 2D HPs. Its fluorophobicity can significantly enhance the noncovalent interactions between cations and [PbI6]4– octahedra. The observed Eg of the fluorinated (4FH-PPH)2PbI4 perovskite is found to be 2.22 eV, which is the lowest value among all fluorinated perovskites reported so far. Interestingly, this fluorinated film-based 2D perovskite photodetector (PD) exhibits the outstanding responsivity of 502 mA W–1, photodetectivity of 5.73 × 1010 cm Hz1/2 W–1, and impressive response/recovery time of 42/46 ms under 450 nm at 20 V. To the best of our knowledge, it is found for the first time that the 2D HP, with the fluorinated short-chained segment included into the organic spacer, shows remarkable stability for up to 49 days. These results strongly demonstrate the potential of the 2D fluorinated short-chained (4FH-PPH)2PbI4 HP with a low Eg as a promising candidate for next-generation optoelectronic devices.