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Intercalation and hybrid heterostructure integration of two-dimensional atomic crystals with functional organic semiconductor molecules

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Abstract

Van der Waals (vdW) integration affords semiconductor heterostructures without constrains of lattice matching and opens up a new realm of functional devices by design. A particularly interesting approach is the electrochemical intercalation of two-dimensional (2D) atomic crystal and formation of superlattices, which can provide scalable production of novel vdW heterostructures. However, this approach has been limited to the use of organic cations with non-functional aliphatic chains, therefore failed to take the advantage of the vast potentials in molecular functionalities (electronic, photonic, magnetic, etc.). Here we report the integration of 2D crystal (MoS2, WS2, highly oriented pyrolytic graphite (HOPG), WSe2 as model systems) with electrochemically inert organic molecules that possess semiconducting characteristics (including perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA), pentacene and fullerene), through on-chip electrochemical intercalation. An unprecedented long-range spatial feature of intercalation has been achieved, which allowed facile assembly of a vertical MoS2-PTCDA-Si junction. The intercalated heterostructure shows significant modulation of the lateral transport, and leads to a molecular tunneling characteristic at the vertical direction. The general intercalation of charge neutral and functional molecules defines a versatile platform of inorganic/organic hybrid vdW heterostructures with significantly extended molecular functional building blocks, holding great promise in future design of nano/quantum devices.

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Acknowledgements

M. D. acknowledges the support by the Fundamental Research Funds for the Central Universities in China (No. 020514380224), Natural Science Foundation of Jiangsu Province (No. BK20180321), and instrument/technical support from State Key Lab of Analytical Chemistry for Life Science, and State Key Lab of Coordination Chemistry. P. W. and S. C acknowledge funding from the National Natural Science Foundation of China (No. 11874199), the National Basic Research Program of China, (No. 2015CB654901); X. W. acknowledges funding support by the National Natural Science Foundation of China (Nos. 61734003, 61521001, 51861145202, 61861166001, and 61851401), the National Key Basic Research Program of China (No. 2015CB921600), Strategic Priority Research Program of Chinese Academy of Sciences XDB 30000000, Key Laboratory of Advanced Photonic and Electronic Materials, Collaborative Innovation Center of Solid-State Lighting and Energy-Saving Electronics, and the Fundamental Research Funds for the Central Universities, China. S. H. C. acknowledges the support by the Program A for Outstanding PhD candidate of Nanjing University (No. 201801A013) and Postgraduate Research & Practice Innovation Program of Jiangsu Province (No. KYCX18_0045).

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  1. Wen He, Han Zang, and Songhua Cai contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210093, China

    Wen He, Zhangyan Mu, Cheng Liu & Mengning Ding

  2. National Laboratory of Solid State Microstructures, Nanjing University, Nanjing, 210093, China

    Han Zang, Songhua Cai, Peng Wang & Xinran Wang

  3. School of Electronic Science and Engineering and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, China

    Han Zang & Xinran Wang

  4. Jiangsu Key Laboratory of Artificial Functional Materials, College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, China

    Songhua Cai & Peng Wang

  5. Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, 999077, Kowloon, Hong Kong, China

    Songhua Cai

  6. Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing, 210023, China

    Peng Wang

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  1. Wen He
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Correspondence to Mengning Ding, Peng Wang or Xinran Wang.

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Intercalation and hybrid heterostructure integration of two-dimensional atomic crystals with functional organic semiconductor molecules

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He, W., Zang, H., Cai, S. et al. Intercalation and hybrid heterostructure integration of two-dimensional atomic crystals with functional organic semiconductor molecules. Nano Res. 13, 2917–2924 (2020). https://doi.org/10.1007/s12274-020-2948-9

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