Van der Waals heterostructures are comprised of stacked atomically thin two-dimensional crystals and serve as novel materials providing unprecedented properties. However, the random natures in positions and shapes of exfoliated two-dimensional crystals have required the repetitive manual tasks of optical microscopy-based searching and mechanical transferring, thereby severely limiting the complexity of heterostructures. To solve the problem, here we develop a robotic system that searches exfoliated two-dimensional crystals and assembles them into superlattices inside the glovebox. The system can autonomously detect 400 monolayer graphene flakes per hour with a small error rate (<7%) and stack four cycles of the designated two-dimensional crystals per hour with few minutes of human intervention for each stack cycle. The system enabled fabrication of the superlattice consisting of 29 alternating layers of the graphene and the hexagonal boron nitride. This capacity provides a scalable approach for prototyping a variety of van der Waals superlattices.

The dry release transfer of two-dimensional (2D) materials such as graphene, hexagonal boron nitride (h-BN), and transition metal dichalcogenides (TMDs) is a versatile method for fabricating high-quality van der Waals heterostructures. Up until now, polydimethylpolysiloxane (PDMS) sheets have been widely used for the dry release transfer of TMD materials. However, this method has been known to have limitations that make it difficult to transfer few-layer-thick graphene and h-BN because of the difficulty to fabricate these materials on PDMS. As an alternative method, we demonstrate the dry release transfer of single-and bi-layer graphene and few-layer h-BN in this study by utilizing poly(propylene) carbonate (PPC) films. Because of the strong adhesion between PPC and 2D materials around room temperature, we demonstrate that single-to few-layer graphene, as well as few-layer h-BN, can be fabricated on a spin-coated PPC film/290-nm-thick SiO2/Si substrate via the mechanical exfoliation method. In addition, we show that these few-layer crystals are clearly distinguishable using an optical microscope with the help of optical interference. Because of the thermoplastic properties of PPC film, the adhesion force between the 2D materials and PPC significantly decreases at about 70 °C. Therefore, we demonstrate that single-to few-layer graphene, as well as fewlayer h-BN flakes, on PPC can be easily dry-transferred onto another h-BN substrate. This method enables a multilayer van der Waals heterostructure to be constructed with a minimum amount of polymer contamination. We demonstrate the fabrication of encapsulated h-BN/graphene/h-BN devices and graphene/few-layer h-BN/graphene vertical-tunnel-junction devices using this method. Since devices fabricated by this method do not require an edge-contact scheme, our finding provide a simples method for constructing high-quality graphene and h-BN-based van der Waals heterostructures.*

The fascinating point of 2D and layered materials is that they can be assembled into van der Waals (vdW) heterostructures, in which atomic layers are integrated by vdW force. There are almost infinite potential combinations in vdW heterostructures owing to the multiple degrees of freedom, i.e., the choice of materials, stacking order, and lateral orientation angle at the interfaces. In this article, we review the fabrication technique of vdW heterostructures, which has played an essential role in the development of the 2D materials research field. First, we describe the primary technique of mechanical exfoliation to fabricate and identify high-quality atomic layers. We then discuss the assembly of atomic layers into vdW heterostructures. Finally, we introduce the recent advancement of fabrication techniques using autonomous robotic assembly. We hope this article would help the readers to acquire basic knowledge of vdW assembly and motivate them to fabricate vdW heterostructures.

Hexagonal boron nitride (h-BN) crystals grown under ultrahigh pressures and ultrahigh temperatures exhibit a high crystallinity and are used throughout the world as ideal substrates and insulating layers in van der Waals heterostructures. However, in their central region, these crystals have domains which contain a significant density of carbon impurities. In this study, we utilized cathodoluminescence and far-ultraviolet photoluminescence to reveal that the carbon (C)-rich domain can exist even after exfoliation. Then, we studied the carrier transport of graphene in h-BN/ graphene/h-BN van der Waals heterostructures, precisely arranging the graphene to straddle the border of the C-rich domain in h-BN. We found that the carrier mobility of graphene on the C-rich h-BN domain was significantly suppressed. In addition, characteristic bending of the Landau fan diagram was observed on the electron-doped side. These results suggest that the C-rich domain in h-BN forms an impurity level and induces extrinsic carrier scattering into adjacent graphene.