Our custom-made UHV exfoliation system is composed of a 4-axis multicentered micromanipulator (µM1) as a crystal-holding stamp, another 2-axis multicentered micro-manipulator (µM2) as the substrate-holding stage, and several wobble-sticks for transfer of the samples. For obtaining 2D layers in the desired orientations, µM2 also serves as a goniometer and a heating stage (Figure ). Prior to exfoliation, the bulk 2D crystal was shaped, flattened, and attached to a SiO2/Si wafer using a vacuum-compatible epoxy (Torr Seal epoxy), which was fixed on a custom-made flag-style sample plate with tantalum clips. At the same time, the substrates were fixed on flat flag-style sample plates by tantalum clips. Prior to the exfoliation, the substrates were chemically cleaned and annealed at 200 °C, followed by deposition of a very thin metal (Au and Ag) layer with an adhesive (Ti) layer by in-situ e-beam evaporation of metals inside the UHV exfoliation chamber. To obtain a fresh interface of the 2D layer, a pre-exfoliation of the bulk crystal attached at µM1 was performed under UHV conditions by bringing it into contact with an adhesive tape (double-sided Kapton tape) attached to another sample plate on µM2. For the exfoliation of monolayers on the desired substrates, the metal-coated substrates were fixed at µM2, and the Kapton-cleaved bulk crystal at µM1 was slowly brought into contact with the substrate. Afterward, the bulk crystal was detached slowly. The process released a very large-area monolayer on the metal-coated substrate, which was examined using an optical and