Direct Z-Scheme SnSe₂/SnSe Heterostructure Passivated by Al₂O₃ for Highly Stable and Sensitive Photoelectrochemical Photodetectors

To mimic the natural photosynthesis system, a Z-scheme heterostructure is proposed as a viable and effective strategy for efficient solar energy utilization such as photocatalysis and photoelectrochemical (PEC) water splitting due to the high carrier separation efficiency, fast charge transport, strong redox, and wide light absorption. However, it remains a huge challenge to form a direct Z-scheme heterostructure due to the internal electric-field restriction and vital band-alignment at the interface. Herein, the van der Waals heterostructure based on the allotrope SnSe 2 and SnSe is designed and synthesized by a two-step vapor phase deposition method to overcome the limitation in the formation of the Z-scheme heterostructure for the first time. The Z-scheme heterostructure of SnSe 2 /SnSe is confirmed by X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, PEC measurement, density functional theory calculations, and water splitting. Strikingly, the PEC photodetectors based on the Z-scheme heterostructure show a synergistic effect of superior stability from SnSe and fast photoresponse from SnSe 2 . As such, the SnSe 2 /SnSe Z-scheme heterostructure shows a good photodetection performance in the ultraviolet to visible wavelength range. Furthermore, the photodetector shows a faster response/recovery time of 13/14 ms, a higher photosensitivity of 529.13 μA/W, and a higher detectivity of 4.94 × 10 9 Jones at 475 nm compared with those of single components. Furthermore, the photodetection stability of the SnSe 2 /SnSe is also greatly improved by a-thin-Al 2 O 3 -layer passivation. The results imply the promising rational design of a direct Z-scheme heterostructure with efficient charge transfer for high performance of optoelectronic devices.