The properties of two-dimensional (2D) van der Waals materials can be tuned through nanostructuring or controlled layer stacking, where interlayer hybridization induces exotic electronic states and transport phenomena. Here we describe a viable approach and underlying mechanism for the assisted self-assembly of twisted layer graphene. The process, which can be implemented in standard chemical vapour deposition growth, is best described by analogy to origami and kirigami with paper. It involves the controlled induction of wrinkle formation in single-layer graphene with subsequent wrinkle folding, tearing and re-growth. Inherent to the process is the formation of intertwined graphene spirals and conversion of the chiral angle of 1D wrinkles into a 2D twist angle of a 3D superlattice. The approach can be extended to other foldable 2D materials and facilitates the production of miniaturized electronic components, including capacitors, resistors, inductors and superconductors.

Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology Beijing China

Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Beijing China

Beijing Key Laboratory of Optoelectronic Functional Materials and Micro Nano Devices Department of Physics Renmin University of China Beijing China

CAS Center for Excellence in Topological Quantum Computation University of the Chinese Academy of Sciences Beijing China

Center for Transformative Science ShanghaiTech University Shanghai China

Central European Institute of Technology Brno University of Technology Brno Czech Republic

Department of Physics University of Oxford Oxford UK

Institute of Physical Engineering Faculty of Mechanical Engineering Brno University of Technology Brno Czech Republic

Institute of Physics Chinese Academy of Sciences Beijing China

Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen China

International Center for Quantum Materials Collaborative Innovation Center of Quantum Matter Peking University Beijing China

School of Natural Sciences Technical University Munich Munich Germany

School of Physical Science and Technology ShanghaiTech University Shanghai China

School of Physical Sciences University of the Chinese Academy of Sciences Beijing China

Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai China

ShanghaiTech Laboratory for Topological Physics ShanghaiTech University Shanghai China

State Key Laboratory for Mesoscopic Physics Frontiers Science Center for Nano optoelectronics School of Physics Peking University Beijing China

State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China

State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics Tsinghua University Beijing China

Vacuum Interconnected Nanotech Workstation Suzhou Institute of Nano Tech and Nano Bionics Chinese Academy of Sciences Suzhou China

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