Assembly of Arbitrary Designer Heterostructures with Atomically Clean Interfaces

Abstract Van der Waals heterostructures are an excellent platform for studying intriguing interface phenomena, such as moiré and proximity effects. Many of these phenomena occurring in such heterostructures' interfaces and surfaces have so far been hampered because of their high sensitivity to disorder and interface contamination. Here, it reports a dry polymer‐based assembly technique to fabricate arbitrary designer van der Waals heterostructures with atomically clean surfaces. The key features of the suspended dry pick‐up and flip‐over assembly technique are: 1) the heterostructure surface never comes into contact with polymers, 2) the assemble is entirely solvent‐free, 3) it is entirely performed in a glovebox, and 4) it only requires temperatures below 130 °C. By performing ambient atomic force microscopy and atomically‐resolved scanning tunneling microscopy on example heterostructures, it demonstrates the fabrication of air‐sensitive heterostructures with ultra‐clean interfaces and surfaces. It envisions that, due to the avoidance of polymer melting, this technique is potentially compatible with heterostructure assembly under ultra‐high vacuum conditions, which promises ultimate heterostructure quality.