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Controlling piezoresistance in single molecules through the isomerisation of bullvalenes

Author

Listed:
  • Jeffrey R. Reimers

    (Shanghai University
    University of Technology Sydney)

  • Tiexin Li

    (Curtin University)

  • André P. Birvé

    (University of Newcastle)

  • Likun Yang

    (Shanghai University)

  • Albert C. Aragonès

    (University of Barcelona
    University of Barcelona)

  • Thomas Fallon

    (University of Newcastle)

  • Daniel S. Kosov

    (James Cook University)

  • Nadim Darwish

    (Curtin University)

Abstract

Nanoscale electro-mechanical systems (NEMS) displaying piezoresistance offer unique measurement opportunities at the sub-cellular level, in detectors and sensors, and in emerging generations of integrated electronic devices. Here, we show a single-molecule NEMS piezoresistor that operates utilising constitutional and conformational isomerisation of individual diaryl-bullvalene molecules and can be switched at 850 Hz. Observations are made using scanning tunnelling microscopy break junction (STMBJ) techniques to characterise piezoresistance, combined with blinking (current-time) experiments that follow single-molecule reactions in real time. A kinetic Monte Carlo methodology (KMC) is developed to simulate isomerisation on the experimental timescale, parameterised using density-functional theory (DFT) combined with non-equilibrium Green’s function (NEGF) calculations. Results indicate that piezoresistance is controlled by both constitutional and conformational isomerisation, occurring at rates that are either fast (equilibrium) or slow (non-equilibrium) compared to the experimental timescale. Two different types of STMBJ traces are observed, one typical of traditional experiments that are interpreted in terms of intramolecular isomerisation occurring on stable tipped-shaped metal-contact junctions, and another attributed to arise from junction‒interface restructuring induced by bullvalene isomerisation.

Suggested Citation

  • Jeffrey R. Reimers & Tiexin Li & André P. Birvé & Likun Yang & Albert C. Aragonès & Thomas Fallon & Daniel S. Kosov & Nadim Darwish, 2023. "Controlling piezoresistance in single molecules through the isomerisation of bullvalenes," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41674-z
    DOI: 10.1038/s41467-023-41674-z
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    References listed on IDEAS

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    1. Christopher Bruot & Julio L. Palma & Limin Xiang & Vladimiro Mujica & Mark A. Ratner & Nongjian Tao, 2015. "Piezoresistivity in single DNA molecules," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    2. Jinshi Li & Pingchuan Shen & Shijie Zhen & Chun Tang & Yiling Ye & Dahai Zhou & Wenjing Hong & Zujin Zhao & Ben Zhong Tang, 2021. "Mechanical single-molecule potentiometers with large switching factors from ortho-pentaphenylene foldamers," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
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