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Understanding resonant charge transport through weakly coupled single-molecule junctions

Author

Listed:
  • James O. Thomas

    (University of Oxford, Chemistry Research Laboratory
    University of Oxford)

  • Bart Limburg

    (University of Oxford, Chemistry Research Laboratory
    University of Oxford)

  • Jakub K. Sowa

    (University of Oxford)

  • Kyle Willick

    (University of Waterloo)

  • Jonathan Baugh

    (University of Waterloo)

  • G. Andrew D. Briggs

    (University of Oxford)

  • Erik M. Gauger

    (Heriot-Watt University)

  • Harry L. Anderson

    (University of Oxford, Chemistry Research Laboratory)

  • Jan A. Mol

    (University of Oxford
    Queen Mary University)

Abstract

Off-resonant charge transport through molecular junctions has been extensively studied since the advent of single-molecule electronics and is now well understood within the framework of the non-interacting Landauer approach. Conversely, gaining a qualitative and quantitative understanding of the resonant transport regime has proven more elusive. Here, we study resonant charge transport through graphene-based zinc-porphyrin junctions. We experimentally demonstrate an inadequacy of non-interacting Landauer theory as well as the conventional single-mode Franck–Condon model. Instead, we model overall charge transport as a sequence of non-adiabatic electron transfers, with rates depending on both outer and inner-sphere vibrational interactions. We show that the transport properties of our molecular junctions are determined by a combination of electron–electron and electron-vibrational coupling, and are sensitive to interactions with the wider local environment. Furthermore, we assess the importance of nuclear tunnelling and examine the suitability of semi-classical Marcus theory as a description of charge transport in molecular devices.

Suggested Citation

  • James O. Thomas & Bart Limburg & Jakub K. Sowa & Kyle Willick & Jonathan Baugh & G. Andrew D. Briggs & Erik M. Gauger & Harry L. Anderson & Jan A. Mol, 2019. "Understanding resonant charge transport through weakly coupled single-molecule junctions," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12625-4
    DOI: 10.1038/s41467-019-12625-4
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    Cited by:

    1. Tian Pei & James O. Thomas & Simen Sopp & Ming-Yee Tsang & Nicola Dotti & Jonathan Baugh & Nicholas F. Chilton & Salvador Cardona-Serra & Alejandro Gaita-Ariño & Harry L. Anderson & Lapo Bogani, 2022. "Exchange-induced spin polarization in a single magnetic molecule junction," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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