Phase-Modulated Multidimensional Perovskites for High-Sensitivity Self-Powered UV Photodetectors

2D Ruddlesden-Popper perovskites (PVKs) have recently shown overwhelming potential in various optoelectronic devices on account of enhanced stability to their 3D counterparts. So far, regulating the phase distribution and orientation of 2D perovskite thin films remains challenging to achieve efficient charge transport. This work elucidates the balance struck between sufficient gradient sedimentation of perovskite colloids and less formation of small-n phases, which results in the layered alignment of phase compositions and thus in enhanced photoresponse. The solvent engineering strategy, together with the introduction of poly(3,4-ethylene-dioxythiophene):polystyrene sulfonate (PEDOT:PSS) and PC71BM layer jointly contribute to outstanding self-powered performance of indium tin oxide/PEDOT:PSS/PVK/PC71BM/Ag device, with a photocurrent of 18.4 mu A and an on/off ratio up to 2800. The as-fabricated photodetector exhibits high sensitivity characteristics with the peak responsivity of 0.22 A W-1 and the detectivity up to 1.3 x 10(12) Jones detected at UV-A region, outperforming most reported perovskite-based UV photodetectors and maintaining high stability over a wide spectrum ranging from UV to visible region. This discovery supplies deep insights into the control of ordered phases and crystallinity in quasi-2D perovskite films for high-performance optoelectronic devices.

Automated summary

2D Ruddlesden-Popper perovskites (PVKs) have shown great potential in optoelectronic devices due to their enhanced stability compared to 3D perovskites. This work reveals the importance of achieving a balance between gradient sedimentation and small-n phase formation in 2D perovskite thin films, leading to layered alignment of phase compositions and improved photoresponse. Through solvent engineering and the use of PEDOT:PSS and PC71BM layers, an indium tin oxide/PEDOT:PSS/PVK/PC71BM/Ag device with a photocurrent of 18.4 μA and an on/off ratio of 2800 is achieved. The fabricated photodetector exhibits high sensitivity with a peak responsivity of 0.22 A W-1 and a detectivity of up to 1.3 x 10(12) Jones in the UV-A region, surpassing most reported perovskite-based UV photodetectors and maintaining stability across a wide spectrum. This discovery provides valuable insights into controlling ordered phases and crystallinity in quasi-2D perovskite films for high-performance optoelectronic devices.