Large-scale 2D heterostructures from hydrogen-bonded organic frameworks and graphene with distinct Dirac and flat bands

Xin Zhang, Xiaoyin Li, Zhengwang Cheng, Aixi Chen, Pengdong Wang, Xingyue Wang, Xiaoxu Lei, Qi Bian, Shaojian Li, Bingkai Yuan, Jianzhi Gao (), Fang-Sen Li (), Minghu Pan () and Feng Liu ()
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Xin Zhang: Shaanxi Normal University
Xiaoyin Li: University of Utah
Zhengwang Cheng: Hubei University of Technology
Aixi Chen: Chinese Academy of Sciences (CAS)
Pengdong Wang: Chinese Academy of Sciences (CAS)
Xingyue Wang: Shaanxi Normal University
Xiaoxu Lei: Chinese Academy of Sciences (CAS)
Qi Bian: Huazhong University of Science and Technology
Shaojian Li: Huazhong University of Science and Technology
Bingkai Yuan: Chinese Academy of Sciences (CAS)
Jianzhi Gao: Shaanxi Normal University
Fang-Sen Li: Chinese Academy of Sciences (CAS)
Minghu Pan: Shaanxi Normal University
Feng Liu: University of Utah

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract The current strategies for building 2D organic-inorganic heterojunctions involve mostly wet-chemistry processes or exfoliation and transfer, leading to interface contaminations, poor crystallizing, or limited size. Here we show a bottom-up procedure to fabricate 2D large-scale heterostructure with clean interface and highly-crystalline sheets. As a prototypical example, a well-ordered hydrogen-bonded organic framework is self-assembled on the highly-oriented-pyrolytic-graphite substrate. The organic framework adopts a honeycomb lattice with faulted/unfaulted halves in a unit cell, resemble to molecular “graphene”. Interestingly, the topmost layer of substrate is self-lifted by organic framework via strong interlayer coupling, to form effectively a floating organic framework/graphene heterostructure. The individual layer of heterostructure inherits its intrinsic property, exhibiting distinct Dirac bands of graphene and narrow bands of organic framework. Our results demonstrate a promising approach to fabricate 2D organic-inorganic heterostructure with large-scale uniformity and highly-crystalline via the self-lifting effect, which is generally applicable to most of van der Waals materials.

Date: 2024
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DOI: 10.1038/s41467-024-50211-5

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