Autonomous robotic searching and assembly of two-dimensional crystals to build van der Waals superlattices.

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.