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Fabrication of devices featuring covalently linked MoS2–graphene heterostructures

Abstract

The most widespread method for the synthesis of 2D–2D heterostructures is the direct growth of one material on top of the other. Alternatively, flakes of different materials can be manually stacked on top of each other. Both methods typically involve stacking 2D layers through van der Waals forces—such that these materials are often referred to as van der Waals heterostructures—and are stacked one crystal or one device at a time. Here we describe the covalent grafting of 2H-MoS2 flakes onto graphene monolayers embedded in field-effect transistors. A bifunctional molecule featuring a maleimide and a diazonium functional group was used, known to connect to sulfide- and carbon-based materials, respectively. MoS2 flakes were exfoliated, functionalized by reaction with the maleimide moieties and then anchored to graphene by the diazonium groups. This approach enabled the simultaneous functionalization of several devices. The electronic properties of the resulting heterostructure are shown to be dominated by the MoS2–graphene interface.

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Fig. 1: Schematic representation of the preparation of the covalent f-MoS2/CVDG FET heterostructure and characterization of f-MoS2.
Fig. 2: Characterization of the f-MoS2/CVDG heterostructure.
Fig. 3: Electrical properties of the covalent f-MoS2/CVDG heterostructure and equivalent van der Waals heterostructure.

Data availability

The authors declare that all the data that support these findings are available in the manuscript and its Supplementary Information as well as from the corresponding authors on request. Source Data are provided with this paper.

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Acknowledgements

The authors acknowledge European Research Council (ERC-PoC- 842606 (E.M.P.); ERC-AdG-742684 (J. S.) and the MSCA program MSCA-IF-2019-892667 (N.M.S.), MINECO (CTQ2017-86060-P (E.M.P.) and CTQ2016-79419-R), Ministerio de Ciencia e Innovación (RTI2018-096075-A-C22 (E.B.), RYC2019-028429-I (E.B.)) the Comunidad de Madrid (MAD2D-CM S2013/ MIT-3007 (E.M.P.), Y2018/NMT-4783 (A.D.)) and the Programa de Atracción del Talento Investigador 2017-T1/IND-5562 (E.B.)). CzechNanoLab Research Infrastructure supported by MEYS CR (LM2018110) are gratefully acknowledged. IMDEA Nanociencia acknowledges support from the Severo Ochoa Programme for Centres of Excellence in R&D (MINECO, grant no. SEV-2016-0686). The funders had no role in study design, data collection and analysis, decision to publish or preparation of the manuscript.

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Contributions

M.V.S., E.B. and E.M.P. conceived and designed experiments. M.V.S., R.Q.O. and M.V.H. synthesized compound 1. M.V.S. and R.Q.O. exfoliated and functionalized the materials. M.V.S., R.Q.O., N.M.S., M.L.G.J. and I.J.G. carried out the chemical and structural characterization. A.D., L.M.P. and E.B. fabricated the nanodevices and performed the electrical measurements. V.S., J. S., E.B. and E.M.P. supervised research and directed data analysis. M.V.S., E.B. and E.M.P. wrote the manuscript, with contributions from all authors.

Corresponding authors

Correspondence to Enrique Burzurí or Emilio M. Pérez.

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Supplementary Figs. 1–35 and Tables 1–2.

Supplementary Data 1

Statistical source data for Supplementary Fig. 2.

Supplementary Data 2

Statistical source data for Supplementary Fig. 5.

Supplementary Data 3

Statistical source data for Supplementary Fig. 25.

Supplementary Data 4

Statistical source data for Supplementary Fig. 27.

Supplementary Data 5

Statistical source data for Supplementary Fig. 30a.

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Statistical source data for Fig. 2a.

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Vázquez Sulleiro, M., Develioglu, A., Quirós-Ovies, R. et al. Fabrication of devices featuring covalently linked MoS2–graphene heterostructures. Nat. Chem. 14, 695–700 (2022). https://doi.org/10.1038/s41557-022-00924-1

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