Understanding resonant charge transport through weakly coupled single-molecule junctions
| Autor: | Thomas, James O., Limburg, Bart, Sowa, Jakub K., Willick, Kyle, Baugh, Jonathan, Briggs, G. Andrew D., Gauger, Erik M., Anderson, Harry L., Mol, Jan A. |
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| Rok vydání: | 2018 |
| Předmět: | |
| Zdroj: | Nat. Commun. 10, 4628 (2019) |
| Druh dokumentu: | Working Paper |
| DOI: | 10.1038/s41467-019-12625-4 |
| Popis: | Off-resonant charge transport through molecular junctions has been extensively studied since the advent of single-molecule electronics and it 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 the non-interacting Landauer theory as well as the conventional single-mode Franck-Condon model. Instead, we model the overall charge transport as a sequence of non-adiabatic electron transfers, the rates of which depend 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 the 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. Comment: version accepted in Nature Communications; SI available at https://researchportal.hw.ac.uk/en/publications/understanding-resonant-charge-transport-through-weakly-coupled-si |
| Databáze: | arXiv |
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