Anti-resonance features of destructive quantum interference in single-molecule thiophene junctions achieved by electrochemical gating

Abstract

Controlling the electrical conductance and in particular the occurrence of quantum interference in single-molecule junctions through gating effects has potential for the realization of high-performance functional molecular devices. In this work we used an electrochemically gated, mechanically controllable break junction technique to tune the electronic behaviour of thiophene-based molecular junctions that show destructive quantum interference features. By varying the voltage applied to the electrochemical gate at room temperature, we reached a conductance minimum that provides direct evidence of charge transport controlled by an anti-resonance arising from destructive quantum interference. Our molecular system enables conductance tuning close to two orders of magnitude within the non-faradaic potential region, which is significantly higher than that achieved with molecules not showing destructive quantum interference. Our experimental results, interpreted using quantum transport theory, demonstrate that electrochemical gating is a promising strategy for obtaining improved in situ control over the electrical performance of interference-based molecular devices.

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Fig. 1: Electrochemical gating of 2,4-TP-SAc molecular junctions.
Fig. 2: Conductance–electrode potential and current/conductance–voltage measurements of 2,4-TP-SAc and 2,5-TP-SAc molecular junctions.
Fig. 3: Transport characteristics of 2,4-TP-SMe and 2,5-TP-SMe molecular junctions.
Fig. 4: Transport properties of thiophene core molecular junctions in the absence and presence of HMIPF6.

Data availability

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

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Acknowledgements

This research was supported by the National Key R&D Program of China (2017YFA0204902), the National Natural Science Foundation of China (21722305, 21673195, 21503179 and 21703188), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the Natural Science Foundation of Shanghai (17ZR1447100), the Science and Technology Commission of Shanghai Municipality (14DZ2261000) and the China Postdoctoral Science Foundation (2017M622060) for funding work in Xiamen. It was also supported by EU Horizon 2020 project QuIET under grant agreement no. 767187 and UK EPSRC grants EP/N017188/1 and EP/M014452/1 and Leverhulme Trust (Leverhulme Early Career Fellowships no. ECF-2017-186 and ECF-2018-375) for funding instrumentation used in Lancaster. It was also supported by Hungarian and Czech Academies of Sciences (P2015-107) andHungarian Research Foundation (OTKA 112034) for funding instrumentation used in Hungary. The authors thank Z.-Q. Tian and B.-W. Mao, Xiamen University, for useful discussions.

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W.H. and J.B. conceived the idea and designed the experiments. W.H., C.L. and W.C. co-supervised the project. J.B., W.H., A.D. and S.S. wrote the manuscript with input from all authors. J.B., X.L. and X.H. carried out the break junction experiments and analysed the data. Q.Z. and W.C. synthesized and provided the structural characterization of the molecules. J.B. and S.L. performed the cyclic voltammetry measurements. Y.T., G.M., J.S. and W.H. built the electrical measurement instrument and wrote the software to control the break junction set-up. A.D., S.S., C.L. and H.S. performed the theoretical modelling. Z.T., J.L. and Y.Y. revised the manuscript. All authors discussed the experiments.

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Correspondence to Wenbo Chen or Colin Lambert or Wenjing Hong.

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Supplementary Information

Supplementary Sections 1–5, Supplementary Figures 1–10, Supplementary References 1–21

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Bai, J., Daaoub, A., Sangtarash, S. et al. Anti-resonance features of destructive quantum interference in single-molecule thiophene junctions achieved by electrochemical gating. Nat. Mater. 18, 364–369 (2019). https://doi.org/10.1038/s41563-018-0265-4

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