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|Title:||A Single-Level Tunnel Model to Account for Electrical Transport through Single Molecule-and Self-Assembled Monolayer-based Junctions||Authors:||Garrigues A.R.
Del Barco E.
|Issue Date:||2016||Publisher:||Nature Publishing Group||Citation:||Garrigues A.R., Yuan L., Wang L., Mucciolo E.R., Thompon D., Del Barco E., Nijhuis C.A. (2016). A Single-Level Tunnel Model to Account for Electrical Transport through Single Molecule-and Self-Assembled Monolayer-based Junctions. Scientific Reports 6 : 26517. ScholarBank@NUS Repository. https://doi.org/10.1038/srep26517||Abstract:||We present a theoretical analysis aimed at understanding electrical conduction in molecular tunnel junctions. We focus on discussing the validity of coherent versus incoherent theoretical formulations for single-level tunneling to explain experimental results obtained under a wide range of experimental conditions, including measurements in individual molecules connecting the leads of electromigrated single-electron transistors and junctions of self-assembled monolayers (SAM) of molecules sandwiched between two macroscopic contacts. We show that the restriction of transport through a single level in solid state junctions (no solvent) makes coherent and incoherent tunneling formalisms indistinguishable when only one level participates in transport. Similar to Marcus relaxation processes in wet electrochemistry, the thermal broadening of the Fermi distribution describing the electronic occupation energies in the electrodes accounts for the exponential dependence of the tunneling current on temperature. We demonstrate that a single-level tunnel model satisfactorily explains experimental results obtained in three different molecular junctions (both single-molecule and SAM-based) formed by ferrocene-based molecules. Among other things, we use the model to map the electrostatic potential profile in EGaIn-based SAM junctions in which the ferrocene unit is placed at different positions within the molecule, and we find that electrical screening gives rise to a strongly non-linear profile across the junction.||Source Title:||Scientific Reports||URI:||https://scholarbank.nus.edu.sg/handle/10635/174960||ISSN:||20452322||DOI:||10.1038/srep26517|
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