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Large-scale multi-heterostructure and optimal band alignment are significantly challenging but vital for photoelectrochemical (PEC)-type photodetector and water splitting. Herein, the centimeter-scale bismuth chalcogenides-based cascade heterostructure is successfully synthesized by a sequential vapor phase deposition method. The multi-staggered band alignment of Bi 2 Te 3 /Bi 2 Se 3 /Bi 2 S 3 is optimized and verified by X-ray photoelectron spectroscopy. The PEC photodetectors based on these cascade heterostructures demonstrate the highest photoresponsivity (103 mA W −1 at −0.1 V and 3.5 mAW −1 at 0 V under 475 nm light excitation) among the previous reports based on two-dimensional materials and related heterostructures. Furthermore, the photodetectors display a fast response (≈8 ms), a high detectivity (8.96 × 10 9 Jones), a high external quantum efficiency (26.17%), and a high incident photon-to-current efficiency (27.04%) at 475 nm. Due to the rapid charge transport and efficient light absorption, the Bi 2 Te 3 /Bi 2 Se 3 /Bi 2 S 3 cascade heterostructure demonstrates a highly efficient hydrogen production rate (≈0.416 mmol cm −2 h −1 and ≈14.320 μmol cm −2 h −1 with or without sacrificial agent, respectively), which is far superior to those of pure bismuth chalcogenides and its type-II heterostructures. The large-scale cascade heterostructure offers an innovative method to improve the performance of optoelectronic devices in the future.

Van der Waals heterostructures have a great potential for the emerging self-powered photoelectrochemical photodetectors due to their outstanding photoelectric conversion capability and efficient interfacial carrier transportation. By considering the band...

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