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Comprehensive suppression of single-molecule conductance using destructive σ-interference

Author

Listed:
  • Marc H. Garner

    (University of Copenhagen)

  • Haixing Li

    (Columbia University
    Columbia University)

  • Yan Chen

    (Shanghai Normal University)

  • Timothy A. Su

    (Columbia University
    University of California, Berkeley)

  • Zhichun Shangguan

    (Shanghai Normal University
    Shanghai Jiao Tong University)

  • Daniel W. Paley

    (Columbia University
    Columbia University)

  • Taifeng Liu

    (Shanghai Normal University)

  • Fay Ng

    (Columbia University)

  • Hexing Li

    (Shanghai Normal University)

  • Shengxiong Xiao

    (Shanghai Normal University)

  • Colin Nuckolls

    (Shanghai Normal University
    Columbia University)

  • Latha Venkataraman

    (Columbia University
    Columbia University)

  • Gemma C. Solomon

    (University of Copenhagen)

Abstract

The tunnelling of electrons through molecules (and through any nanoscale insulating and dielectric material 1 ) shows exponential attenuation with increasing length 2 , a length dependence that is reflected in the ability of the electrons to carry an electrical current. It was recently demonstrated3–5 that coherent tunnelling through a molecular junction can also be suppressed by destructive quantum interference 6 , a mechanism that is not length-dependent. For the carbon-based molecules studied previously, cancelling all transmission channels would involve the suppression of contributions to the current from both the π-orbital and σ-orbital systems. Previous reports of destructive interference have demonstrated a decrease in transmission only through the π-channel. Here we report a saturated silicon-based molecule with a functionalized bicyclo[2.2.2]octasilane moiety that exhibits destructive quantum interference in its σ-system. Although molecular silicon typically forms conducting wires 7 , we use a combination of conductance measurements and ab initio calculations to show that destructive σ-interference, achieved here by locking the silicon–silicon bonds into eclipsed conformations within a bicyclic molecular framework, can yield extremely insulating molecules less than a nanometre in length. Our molecules also exhibit an unusually high thermopower (0.97 millivolts per kelvin), which is a further experimental signature of the suppression of all tunnelling paths by destructive interference: calculations indicate that the central bicyclo[2.2.2]octasilane unit is rendered less conductive than the empty space it occupies. The molecular design presented here provides a proof-of-concept for a quantum-interference-based approach to single-molecule insulators.

Suggested Citation

  • Marc H. Garner & Haixing Li & Yan Chen & Timothy A. Su & Zhichun Shangguan & Daniel W. Paley & Taifeng Liu & Fay Ng & Hexing Li & Shengxiong Xiao & Colin Nuckolls & Latha Venkataraman & Gemma C. Solom, 2018. "Comprehensive suppression of single-molecule conductance using destructive σ-interference," Nature, Nature, vol. 558(7710), pages 415-419, June.
  • Handle: RePEc:nat:nature:v:558:y:2018:i:7710:d:10.1038_s41586-018-0197-9
    DOI: 10.1038/s41586-018-0197-9
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    Cited by:

    1. Leopoldo Mejía & Pilar Cossio & Ignacio Franco, 2023. "Microscopic theory, analysis, and interpretation of conductance histograms in molecular junctions," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Siddhartha Sohoni & Indranil Ghosh & Geoffrey T. Nash & Claire A. Jones & Lawson T. Lloyd & Beiye C. Li & Karen L. Ji & Zitong Wang & Wenbin Lin & Gregory S. Engel, 2024. "Optically accessible long-lived electronic biexcitons at room temperature in strongly coupled H- aggregates," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Shuzhi Liu & Jianmin Zeng & Zhixin Wu & Han Hu & Ao Xu & Xiaohe Huang & Weilin Chen & Qilai Chen & Zhe Yu & Yinyu Zhao & Rong Wang & Tingting Han & Chao Li & Pingqi Gao & Hyunwoo Kim & Seung Jae Baik , 2023. "An ultrasmall organic synapse for neuromorphic computing," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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