Understanding resonant charge transport through weakly coupled single-molecule junctions

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

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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.

Original languageEnglish
Article number4628
JournalNature Communications
Publication statusPublished - 11 Oct 2019

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

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    Thomas, J. O., Limburg, B., Sowa, J. K., Willick, K., Baugh, J., Briggs, G. A. D., Gauger, E. M., Anderson, H. L., & Mol, J. A. (2019). Understanding resonant charge transport through weakly coupled single-molecule junctions. Nature Communications, 10, [4628]. https://doi.org/10.1038/s41467-019-12625-4