Understanding resonant charge transport through weakly coupled single-molecule junctions

Thomas, Limburg, Sowa, Willick, Baugh, Briggs, Gauger, Anderson, Mol (2019) Understanding resonant charge transport through weakly coupled single-molecule junctions Nat Commun (IF: 16.6) 10(1) 4628

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.

Links

http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6789103
http://www.ncbi.nlm.nih.gov/pubmed/31604934
http://dx.doi.org/10.1038/s41467-019-12625-4

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