Abstract

Quantum interference can profoundly affect charge transport in single molecules, but experiments can usually measure only the conductance at the Fermi energy. Because, in general, the most pronounced features of the quantum interference are not located at the Fermi energy, it is highly desirable to probe charge transport in a broader energy range. Here, by means of electrochemical gating, we measure the conductance and map the transmission functions of single molecules at and around the Fermi energy, and study signatures associated with constructive and destructive interference. With electrochemical gate control, we tune the quantum interference between the highest occupied molecular orbital and lowest unoccupied molecular orbital, and directly observe anti-resonance, a distinct feature of destructive interference. By tuning the molecule in and out of anti-resonance, we achieve continuous control of the conductance over two orders of magnitude with a subthreshold swing of ~17 mV dec−1, features relevant to high-speed and low-power electronics.

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Code availability

The DFT code CONQUEST is available at http://www.order-n.org and the corresponding module used to calculate the quantum transport properties is available from M.B. upon reasonable request.

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

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Acknowledgements

The authors (N.T. and Y.L.) thank D.N. Beratan and A. Nitzan for stimulating discussions. The authors acknowledge financial support from the National Natural Science Foundation of China (grants nos. 21773117 and 21575062, to H.W., Z.W.), the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan (Grant-in-Aid for Scientific Research on Innovative Areas ‘Molecular Architectonics: Orchestration of Single Molecules for Novel Functions’; grant no. 25110009, to Y.A. and M.B.), the Japan Society for the Promotion of Science (Grant-in-Aid for Young Scientists (Start-up); KAKENHI grant no. 15H06889, to M.B.) and the National Natural Science Foundation of China (grants nos. 21674023 and 51722301, to G.L. and G.Z.).

Author contributions

N.T., Y.L., L.X., G.Z., G.L., Y.A. and M.B. designed the research. G.L. and G.Z. synthesized the studied molecules. Y.L., A.R., H.W. and Z.W. performed and analysed the experiments. M.B., Y.A., D.R.B. and T.M. performed and analysed the DFT and transport calculations. Y.L., N.T., M.B. and G.L. wrote the paper. All authors contributed to revising the manuscript and agreed on its final content.

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Affiliations

  1. Biodesign Center for Bioelectronics and Biosensors, Arizona State University, Tempe, AZ, USA

    • Yueqi Li
    • , Ali Rostamian
    • , Limin Xiang
    •  & Nongjian Tao
  2. Research Center for Computational Design of Advanced Functional Materials (CD-FMat), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, Ibaraki, Japan

    • Marius Buerkle
    •  & Yoshihiro Asai
  3. Laboratory of Advanced Materials, State Key Laboratory of Molecular Engineering of Polymers, Fudan University, Shanghai, China

    • Guangfeng Li
    •  & Gang Zhou
  4. State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China

    • Hui Wang
    • , Zixiao Wang
    •  & Nongjian Tao
  5. London Centre for Nanotechnology and Department of Physics and Astronomy, University College London, London, UK

    • David R. Bowler
  6. International Centre for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS) Tsukuba, Ibaraki, Japan

    • David R. Bowler
    •  & Tsuyoshi Miyazaki

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The authors declare no competing interests.

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Correspondence to Yoshihiro Asai or Gang Zhou or Nongjian Tao.

Supplementary information

  1. Supplementary Information

    Supplementary Figures 1–19, Supplementary Methods: First-principles transport calculations, Supplementary References 1–17

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DOI

https://doi.org/10.1038/s41563-018-0280-5