Synchronous and Unidirectional Epitaxy of Layer‐Controlled Graphene on Oxidized Single‐Crystal Copper Wafers With Tunable Stacking Order
ABSTRACT The deterministic synthesis of wafer‐scale two‐dimensional (2D) materials with programmable layer number, crystallographic orientation, and stacking order is essential for unlocking their layer‐dependent quantum properties and enabling scalable device integration. Here, we demonstrate a synchronous and unidirectional epitaxy strategy for chemical vapor deposition growth of layer‐controlled graphene on atomically flat oxidized single‐crystal Cu wafers. Using a Cu(111)–Cu 2 O(111) heterogeneous catalytic substrate, we achieved 2‐inch single‐crystalline graphene films with precisely tunable layer numbers (2 to 5). By engineering the atomic steps of high‐index Cu surfaces, we created deterministic spatial patterning of alternating Bernal and rhombohedral stacking in trilayer graphene, as confirmed by near‐field nano‐optics and angle‐resolved photoemission spectroscopy. The resulting wafer‐scale films exhibit exceptional thickness uniformity, high crystallinity, and an ultra‐flat surface. This work provides a unified growth framework that concurrently resolves the intertwined challenges of layer control, wafer‐scale single crystallinity, and stacking order modulation, laying a material foundation for advanced device studies and potential applications.
Authors
- Hanbo Xiao (ORCID: https://orcid.org/0000-0001-8247-3378)
- Buhang Chen
- Luzhao Sun (ORCID: https://orcid.org/0000-0003-0518-0744)
- Ding Pei (ORCID: https://orcid.org/0000-0002-3995-0690)
- 任泽峰
- Hailin Peng (ORCID: https://orcid.org/0000-0003-1569-0238)
- Zhongkai Liu (ORCID: https://orcid.org/0000-0003-3373-8039)
- Kostya S. Novoselov (ORCID: https://orcid.org/0000-0003-4972-5371)
- Xin Gao (ORCID: https://orcid.org/0009-0005-3999-0106)
- Qing Dai (ORCID: https://orcid.org/0000-0002-1750-0867)
- Guanhua Zhang (ORCID: https://orcid.org/0000-0001-7974-486X)
- Song Xiaofeng (ORCID: https://orcid.org/0009-0006-6743-0250)
- Zhongfan Liu (ORCID: https://orcid.org/0000-0001-5554-1902)
- Chengjin Wu
- Xiangdong Guo
- Yanyan Dong
- Xiongzhi Zeng
- Yulin Chen
- Jun Wang
- Huan Wang
- Wei Wei
- Hongyi Yuan
- Hai‐Sheng Su
- Jingyue Wang
Institutions
- University of Science and Technology of China (CN)
- National University of Singapore (SG)
- Dalian Institute of Chemical Physics (CN)
- Shanghai Jiao Tong University (CN)
- Xiamen University (CN)
- Chinese Academy of Sciences (CN)
- Peking University (CN)
- ShanghaiTech University (CN)
- Suzhou Institute of Nano-tech and Nano-bionics (CN)
- Beijing Graphene Institute (CN)
- Beijing National Laboratory for Molecular Sciences (CN)
- Institute for Functional Intelligent Materials (SG)
Publication Details
- Journal
- Advanced Materials
- Published
- 2026-11-02
- DOI
- https://doi.org/10.1002/adma.75580
- Primary Topic
- Graphene research and applications
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Royal Society
- National Natural Science Foundation of China
- Natural Science Foundation of Beijing Municipality
- Beijing Nova Program