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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, Fangsen Li, Minghu Pan, Feng Liu

2024Nature Communications15 citationsDOIOpen Access PDF

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.

Topics & Concepts

GrapheneHeterojunctionMaterials scienceNanotechnologyHighly oriented pyrolytic graphiteGraphitevan der Waals forceMetal-organic frameworkSubstrate (aquarium)OptoelectronicsChemistryScanning tunneling microscopeComposite materialOrganic chemistryMoleculeGeologyAdsorptionOceanographyCovalent Organic Framework ApplicationsGraphene research and applicationsMetal-Organic Frameworks: Synthesis and Applications
Large-scale 2D heterostructures from hydrogen-bonded organic frameworks and graphene with distinct Dirac and flat bands | Litcius