Seong-Jun Yang1,2,Ju-Hyun Jung1,2,Eunsook Lee3,Edmund Han4,Min-Yeong Choi1,2,Daesung Jung5,Shinyoung Choi1,2,Jun-Ho Park1,2,Dongseok Oh3,Siwoo Noh3,Ki-Jeong Kim3,Pinshane Huang4,Chan-Cuk Hwang3,Cheoljoo Kim1,2
Pohang University of Science and Technology1,Institute for Basic Science (IBS)2,ohang Accelerator Laboratory3,University of Illinois at Urbana-Champaign4,Sungkyunkwan University5
Seong-Jun Yang1,2,Ju-Hyun Jung1,2,Eunsook Lee3,Edmund Han4,Min-Yeong Choi1,2,Daesung Jung5,Shinyoung Choi1,2,Jun-Ho Park1,2,Dongseok Oh3,Siwoo Noh3,Ki-Jeong Kim3,Pinshane Huang4,Chan-Cuk Hwang3,Cheoljoo Kim1,2
Pohang University of Science and Technology1,Institute for Basic Science (IBS)2,ohang Accelerator Laboratory3,University of Illinois at Urbana-Champaign4,Sungkyunkwan University5
Modulation of thicknesses and atomic structures can broadly program the physical properties of crystalline films. The layer-by-layer assembly of atomically thin crystals provides a powerful means to arbitrarily design films at the atomic level, which are unattainable with existing growth technologies. However, atomically clean assembly of the materials with high scalability and reproducibility remains challenging. Here, we report programmed crystal assembly of graphene and monolayer hexagonal boron nitride, assisted by van der Waals interactions, to form wafer-scale films of pristine interfaces with near-unity yield. The atomic configurations of the films are tailored with layer-resolved compositions and in-plane crystalline orientations. We demonstrate batch-fabricated tunnel device arrays with modulation of the resistance over orders of magnitude by thickness control of the hexagonal boron nitride barrier with single-atom thick precision and large-scale, twisted multilayer graphene with programmable electronic band structures and crystal symmetries. Our results constitute an important development in the artificial design of large-scale films.