Chemically Tailored Semiconductor Moiré Superlattices of Janus Heterobilayers

Janus monolayers of transition metal dichalcogenides (TMDCs) are promising building blocks for moiré superlattices because of their built‐in electric field and clean fabrication process. In particular, Janus TMDC monolayers can be chemically converted from conventional TMDC monolayers by atomic substitution, enabling the direct formation of lattice‐mismatched heterobilayers from TMDC bilayers. However, the moiré superlattices of Janus heterobilayers have not been studied experimentally. Herein, this work reports the fabrication and characterization of semiconductor moiré superlattices in chemically tailored Janus heterobilayers. The MoSSe/MoSe 2 (or WSSe/WSe 2 ) Janus heterobilayers are prepared by replacing the top layer Se atoms with S atoms in MoSe 2 (or WSe 2 ) bilayer using H 2 plasma treatment. Scanning transmission electron microscopy reveals that an average moiré period of about 14 nm formed due to lattice mismatch resulting from the chalcogen substitutions. The cryogenic photoluminescence spectra show sharp, near‐infrared emissions, which are attributed to excitons trapped by moiré potentials based on comparison with theoretical calculations. The Janus‐based heterostructures provide a long‐period moiré system with built‐in potential even for nontwisted heterobilayers, allowing the functionalization of confined and correlated electron systems.