Issue 33, 2021

Charge transport through extended molecular wires with strongly correlated electrons

Abstract

Electron–electron interactions are at the heart of chemistry and understanding how to control them is crucial for the development of molecular-scale electronic devices. Here, we investigate single-electron tunneling through a redox-active edge-fused porphyrin trimer and demonstrate that its transport behavior is well described by the Hubbard dimer model, providing insights into the role of electron–electron interactions in charge transport. In particular, we empirically determine the molecule's on-site and inter-site electron–electron repulsion energies, which are in good agreement with density functional calculations, and establish the molecular electronic structure within various oxidation states. The gate-dependent rectification behavior confirms the selection rules and state degeneracies deduced from the Hubbard model. We demonstrate that current flow through the molecule is governed by a non-trivial set of vibrationally coupled electronic transitions between various many-body ground and excited states, and experimentally confirm the importance of electron–electron interactions in single-molecule devices.

Graphical abstract: Charge transport through extended molecular wires with strongly correlated electrons

Supplementary files

Article information

Article type
Edge Article
Submitted
06 iyn 2021
Accepted
19 iyl 2021
First published
26 iyl 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2021,12, 11121-11129

Charge transport through extended molecular wires with strongly correlated electrons

J. O. Thomas, J. K. Sowa, B. Limburg, X. Bian, C. Evangeli, J. L. Swett, S. Tewari, J. Baugh, G. C. Schatz, G. A. D. Briggs, H. L. Anderson and J. A. Mol, Chem. Sci., 2021, 12, 11121 DOI: 10.1039/D1SC03050G

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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